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PHOTOCONDUCTIVITY IN ONE DIMENSIONAL METAL OXIDES NANOSTRUCTURES RAJESH TAMANG NATIONAL UNIVERSITY OF SINGAPORE 2010 PHOTOCONDUCTIVITY IN ONE DIMENSIONAL METAL OXIDES NANOSTRUCTURES RAJESH TAMANG (M.Tech) A THESIS SUBMITTED FOR THE DEGREE OF MASTER OF SCIENCE DEPARTMENT OF PHYSICS NATIONAL UNIVERSITY OF SINGAPORE 2010 ACKNOWLEDGMENTS ACKNOWLEDGMENTS I would like to express my deepest gratitude, respect, and admiration to my supervisor, Assoc. Prof. Sow Chorng Haur. I have been greatly motivated and influenced by him during my course of study. I am thankful for his constant encouragement, support and the freedom for research, he rendered to me. I would like to express my special thanks to Assoc. Prof. TOK Eng Soon for his time and discussion, which helped in completion of the work presented in this thesis. I would like to express deep sense of gratitude to Dr. Binni Varghese, for all the advices, discussions and helping in using focused ion beam (FIB). Special appreciation must be given to Mr. Zheng Minrui, Mr. Lim Zhi Han, Mr. Xie Yilin, Ms. Sharon Lim Xiao Dai, Ms. Deng Suzi, Mr. Bablu Mukherjee, Mr. Rajiv Prabhakar, Ms. Loh Pui Yee, Ms. Tao Ye, Mr. Chang Sheh Lit, Mr. Lee Kian Keat, Mr. Hu Zhibin, Mr. Lu Jun Peng and Mr. Yun Tao for all the help and creating vibrant, cheerful and co-operative environment to work in the laboratory. I would like to thank all the technical staff in the Physics department for all the help I had received. Specially Mr. Chen Gin Seng for helping to rectify instrumental problems. I would like to thank Ms. Foo Eng Tin for assisting with lab suppliers. I would like to thank Mr. Ho Kok Wen for his help in troubleshooting with scanning electron microscope (SEM). I would also like to acknowledge National University of Singapore (NUS) for graduate student scholarships. Finally, I feel I am indebted to my parents for their unconditional support, love and understanding. To my brother and sister who have been always supportive and encouraging, i ACKNOWLEDGMENTS definitely, I wouldn’t have finished this thesis without them. It gives me immense pleasure in dedicating this work to them. ii TABLE OF CONTENTS TABLE OF CONTENTS • ACKNOWLEDGEMENTS • TABLE OF CONTENTS iii • ABSTRACT vi • LIST OF PUBLICATIONS • LIST OF TABLES • LIST OF FIGURES i viii ix x Chapter 1: Introduction and Motivation 1.1 Introduction 1 1.2 Motivation 3 1.3 Brief outline of the present work 4 References 6 Chapter 2: Photoconductivity in one-dimensional nanostructures 2.1 Introduction 8 2.2 Concepts in Photoconductivity 9 2.2.1 Steady-state Photoconductivity 2.3 Photoconductivity in one-dimensional metal-oxide nanowires 11 12 2.4 Factors contributing to photoresponse in one-dimensional metal-oxide nanowires 2.4.1 Surface effects 13 2.4.2 Photoresponse in dry and wet air 14 2.4.3 Electrical contacts 15 References 18 Chapter 3: Fabrication and Characterization Techniques 3.1 Niobium and vanadium oxide nanomaterials synthesis techniques 3.1.1 Cleaning of substrate/metal foil 22 3.1.2 Thermal oxidation techniques for the synthesis of Nb 2 O 5 nanowires 22 3.1.3 Hotplate techniques for the synthesis of V 2 O 5 nanowires 24 iii TABLE OF CONTENTS 3.2 Characterization Methods and Techniques 3.2.1 X-Ray Diffraction (XRD) Analysis 25 3.2.2 Raman Spectroscopy 26 3.2.3 Scanning Electron Microscope (SEM) 27 3.3 Nano-device fabrication Techniques 3.3.1 Photolithography techniques 29 3.3.2 Single nanowire device fabrication 31 3.4 Electrical Characterization of Single Nanowire 32 3.5 Photoconductivity Measurement Techniques 3.5.1 Global irradiation techniques 32 3.5.2 Localized irradiation techniques 33 References 34 Chapter 4: Photoconductivity of Individual Nb 2 O 5 Nanowire 4.1 Introduction 35 4.2 Experimental Section 36 4.2.1 Characterization of Nanostructure 37 4.3 Nb 2 O 5 nano-device fabrication and electrical characterization 39 4.4 Photoconductivity study 41 4.4.1 Photoresponse of individual Nb 2 O 5 NW to global irradiation (a) Time characteristics analysis for global irradiation 4.4.2 Photoresponse of individual Nb 2 O 5 NW with focused laser 43 45 48 (a) Time characteristics analysis for focused laser beam 52 (b) Zero bias photocurrent with focused laser beam 53 4.5 Conclusion 58 References 59 Chapter 5: Photoconductivity of Individual V 2 O 5 Nanowire 5.1 Introduction 61 5.2 Experimental Section 62 5.3 V 2 O 5 nano-device fabrication 64 iv TABLE OF CONTENTS 5.4 Electrical characterization and photoconductivity of individual V 2 O 5 NW 65 5.5 Time characteristics analysis 73 5.6 Conclusion 75 References 77 Chapter 6: Conclusions and Future Works v 79 ABSTRACT ABSTRACT With recent development in individual nanowire (NW) characterization and device fabrication, study of photoconductivity of individual NWs has been proven to be an efficient approach in probing their electronic and surface related properties. In this work, systematic studies were carried out to investigate the photoconductivity of individual Nb 2 O 5 and V 2 O 5 NWs. The synthesized Nb 2 O 5 and V 2 O 5 NWs were characterized using various characterization techniques. Global and focused laser beam irradiation techniques were used as experimental approach for photoresponse study. The focused laser beam irradiation with spot size < 1 µm had the advantage of probing the desired section of isolated NW along the NW-Pt interface. We observed, fast and prominent photoresponse from individual Nb 2 O 5 NW towards visible and infrared laser irradiation under various conditions. The global irradiation on Nb 2 O 5 NW showed multiple photocurrent contribution from defect level excitations, surface states and thermal heating effects. Significant photoresponse was observed in vacuum condition. The time characteristic of the observed photoresponse was further analysed and revealed characteristic response time in the photoresponse of the NW to laser irradiation. Interestingly, the photoresponse with focused laser beam showed large enhancement compared to global irradiation at relatively low applied bias. We found that NW-Pt contact played a major role in the photoresponse of the sample. This envisioned in developing better insight into the photoresponse of the NW, particularly along the metal-NW interface. The mechanisms to account for the observed photocurrent were proposed. We proposed that Schottky barrier formation and photoinduced thermoelectric effects are key carrier transport mechanisms for photocurrent generation, at the NW-Pt interface at zero bias. While at applied bias, the thermoelectric effect was observed vi ABSTRACT to be less significant, and most photoresponse was likely from defect and surface state excitations. V 2 O 5 NW showed rapid photoresponse at vacuum condition and very small photocurrent (~1 nA) in ambient condition at applied bias. The electrical properties were investigated at various pressure conditions and with varying laser power. From the time characteristics analysis, photocurrents in V 2 O 5 NW were mostly attributed to thermal heating. The NW device was modelled as metal-semiconductor-metal structure composed of two Schottky diode connected back-to-back in series. Quantitative analysis was carried out and the carrier density and mobility of V 2 O 5 NW were determined. vii LIST OF PUBLICATIONS LIST OF PUBLICATIONS • R. Tamang, B. Varghese, S. G. Mahaisalkar, E. S. Tok, C. H. Sow; Probing the photoresponse of individual Nb 2 O 5 nanowires with global and localized laser beam irradiation; Nanotechnology 22(2011) 115202 • B. Varghese, R. Tamang, E. S. Tok, S. G. Mahaisalkar, C. H Sow; Photothermoelectric Effects in Localized Photocurrent of Individual VO 2 Nanowires; Journal of Physical Chemistry C 114(2010) 15149 • Y. L. Xie, F. C. Cheong, Y. W. Zhu, B. Varghese, R. Tamang, et al; Rainbow–like MoO 3 Nanobelts Fashioned via AFM Micromachining; Journal of Physical Chemistry C 114 (2010) 120 Conferences • R. Tamang, B. Varghese, S. G. Mahaisalkar, E. S. Tok, C. H. Sow; Systematic studies of photo – response of individual Nb 2 O 5 Nanowires; 4th MRS–S Conference on Advanced materials, Singapore (2010)-Poster presentation. viii LIST OF TABLES LIST OF TABLES Table 4.1: Time characteristics analysis in vacuum and ambient condition. Table 4.2: Rising time characteristic analysis to localized irradiation along the NW. ix LIST OF FIGURES LIST OF FIGURES Figure 2.1 Schematic diagram showing intrinsic and extrinsic phenomena involved in photoconductivity. Figure 2.2 schematic diagrams representing (a) metal-nanowire-metal contact nano device structure on SiO 2 /Si substrate. (b) Two Schottky barrier modeled as back-to-back diode connected in series. (c) Energy band diagram of metal-semiconductor-metal structure at equilibrium. Figure 3.1 Schematic diagram of tube furnace set up with all its necessary components for the growth of nanostructures. Figure 3.2 Hotplate for the growth of V 2 O 5 nanowires on SiN substrate. Figure 3.3 The relationship between atomic planes, incident X-rays and reflected X-rays in XRD analysis. Figure 3.4 (a) Schematic diagram representing the steps for photolithography process, (b) Au finger electrodes on SiO 2 /Si substrate. Figure 3.5 Schematic diagram of single nanowire device with Pt contact between the NW and the Au electrodes. Figure 3.6 (a) Schematic diagram of individual nanowire device with global irradiation (spot size larger than the electrodes gap). (b) Schematic diagram of individual nanowire device inside the vacuum chamber for photocurrent measurements in vacuum environment with global irradiation. Figure 3.7 Schematic experimental setup of localized photoconductivity techniques probed at individual nanowire device. Figure 4.1 FE-SEM image of Nb 2 O 5 nanowires grown in Nb-metal foil with thermal oxidation techniques at 900 oC. Figure 4.2 XRD spectrum of Nb 2 O 5 nanowires grown in Nb-metal foil with thermal oxidation techniques at 900 oC. Figure 4.3 Raman spectrum of as grown Nb 2 O 5 nanostructures. Figure 4.4 SEM image of individual Nb 2 O 5 nanowire device fabricated in Au electrodes with Pt- contacts on both ends of the NW. Figure 4.5 Typical I-V characteristics of individual Nb 2 O 5 nanowire measured at room temperature. x LIST OF FIGURES Figure 4.6 Schematic representation of individual nanowire device for photoconductivity measurements with (a) global and (b) localized irradiation. Figure 4.7 (a) Photocurrent measured at zero bias, under ambient condition. (b) Photocurrent measured at applied bias of 3V, under ambient and vacuum environment, (808nm wavelength, power ~170mW). Figure 4.8 (a) Rising and (b) Decaying time response analysis (808nm wavelength, power ~ 170mW) at ambient and vacuum conditions (solid lines are the exponential fitted curves). Figure 4.9 (a) Schematic representation of photocurrent measurements with focused laser beam irradiation on NW. (b) Schematic diagram of focused laser beam locally irradiated on (i) high terminal NW-Pt interface (ii) middle of NW (ii) low terminal NW-Pt interface. (c) I-V characteristics with/without focused laser beam irradiation on NW-Pt contacts at sweeping voltage -2V to +2V. (d) Photoresponse at applied bias 0 . 5 Vwith laser (λ=532 nm, power ~80 µW) irradiated on the low terminal NW-Pt contacts, middle of the NW and on the high terminal NW-Pt contacts respectively. Schematic representation of band bending diagram with corresponding electron-hole transfer at Pt-NW interface when laser irradiated at (e) forward and (f) reverse applied bias. Figure 4.10 Time response analysis curve (a) rising and (b) decay, when the focused laser (λ=532 nm) beam irradiated at the forward bias NW-Pt interface, middle of the NW, and at reverse biased NW-Pt contact (solid lines are the fitted curves). Figure 4.11 (a) Photoresponse at zero bias with varying laser power (λ=532 nm, 125 µW, 260 µW and 324 µW respectively) when focused laser irradiated on the low terminal NW-Pt contacts, middle of NW and the high NW-Pt contact. (b) Schematic representation of band diagram with corresponding electron-hole transfer at two ends of the Pt-NW due to localized heating, resulting photocurrent due to thermoelectric effect with focused laser beam irradiated at the Pt-NW interface at zero bias. Figure 4.13 Photocurrent responses with global irradiation on Nb 2 O 5 NW with (a) 808 nm laser (power ~ 50 mW) (b) 1064 nm (power ~108 mW) under ambient condition with applied bias voltage of 3V. (c) and (d) represents photocurrent responses from Nb 2 O 5 NW with localized laser beam irradiation (λ=1064 nm) at applied bias 0.1V (laser power ~ 120 µW) and at zero bias (laser power ~ 160 µW) respectively. Figure 4.12 Photoresponse at zero bias when focused laser (48 mW, λ=808 nm) irradiated on the low terminal NW-Pt contacts, middle of NW and the high terminal NW-Pt contacts. Figure 5.1 SEM images of V 2 O 5 nanowires on (a) SiN substrate, (b) and (c) are images of suspended V 2 O 5 nanowire on the edge of the SiN substrate. Figure 5.2 Raman spectrums of V 2 O 5 nanowires. xi LIST OF FIGURES Figure 5.3 SEM image of individual V 2 O 5 NW, NW ends are connected to the Au finger electrodes on Si/SiO 2 substrate with Pt deposition. Figure 5.4 (a) Schematic diagram of experimental setup used for the study of photoresponse of V 2 O 5 NW. (b) I-V curve of V 2 O 5 NW at ambient. (c) I-V curves with/without light illumination at ambient. (d) I-V curves with light illumination at ambient and at different vacuum condition. Figure 5.5 (a) I-V results of individual V 2 O 5 NW measured at vacuum (~5 x 10-5 Torr) irradiated by different laser (λ=808) power. (b) Experimental and fitted plot of laser (λ=808 nm) power vs photocurrent at fixed applied bias of 1.5V. Figure 5.6 Experimental and fitted ln(I) vs V plot for V 2 O 5 on linear regime of I-V curve shown in Figure 5.4 (b). Figure 5.7 The response curve under laser (λ=808nm, power ~165 mW) at an ambient and vacuum (~8.3 x 10-3Torr, 4.2 x 10-5Torr) environment. Figure 5.8 Power dependent I-V characteristic curves on irradiation of laser (λ=1064 nm) at vacuum environment (~ 4 x 10-5Torr). (b) Experimental and fitted plot of current with respect to dark current versus the laser power (1064 nm) at fixed biased 1.5V. Figure 5.9 Photoresponse of individual V 2 O 5 NW on irradiation of laser (λ=1064 nm, power ~230 mW) measured at applied bias 0.5V (a) in ambient and vacuum (~ 4 x 10-5Torr). (b) Power dependent photoresponse at vacuum (~ 4 x 10-5Torr). Figure 5.10 Experimental and fitted exponential time characteristics curves obtained from Figure 5.7 (λ=808 nm) and Figure 5.9 (λ=1064 nm): (a) Rising time (b) Decay time for λ=808 nm laser irradiation. (c) Rising time (b) Decay time for λ=1064 nm laser irradiation. Figure 5.11 Photocurrent responses from individual V 2 O 5 NW (different NW device then the above results) on irradiation of 808 nm laser (power ~ 130 mW) at applied bias of 0.5 V. xii Chapter 1 Introduction and Motivation Chapter 1 Introduction and Motivation 1.1 Introduction With unique and controlled optical and electrical properties, nanowires (NWs) are ideal for applications in optoelectronics, photovoltics, and biological and chemical sensing.1-10 With the recent development in individual NW characterization and device fabrication, study of photoresponse of individual NWs has emerged as an efficient tool in understanding their electronic and surface related properties. The photoresponse of NWs is determined by several factors including its light absorption efficiency, carrier photogeneration, carrier trappingdetrapping mechanism and recombination process.11-15 In addition change in large surface-tovolume ratio in nanostructures, its electrical transport properties strongly influenced by the surrounding environment and not dependent only on the intrinsic properties of the nanowire material. In addition, the nature of NW-metal electrode interface also sensitively contributes to the individual NW photoconductivity. This is typically due to formation of rectifying Schottky barrier. In order to realize NW functional devices, an insight of the underlying mechanism of photogeneration and transport of charge carriers in NWs contacted with metal electrodes is critical. Currently, many reports on the studies of photoconductivity of nanowires focus on the effect of broad beam illumination on the electrical conductivity of thin films of nanowires contacted on both ends with conducting electrode.13-16 Naturally the observed photoresponse of these sample depends on the interplay between the intrinsic response of the NWs, NW-NW and the NW-electrode contact barriers. Given the wide variety of contributing factors to the 1 Chapter 1 Introduction and Motivation experimentally observed results in a typical photoconductivity experiment, interpretation of the observed results could prove to be challenging. The effects of Schottky barriers at the metal-semiconductor interface are often encountered in the studies of semiconductor NWs. UV response in ZnO nanowire nanosensor was improved with Schottky contact in device fabrication where its sensitivity enhanced by four orders of magnitude, and significant decreased in reset time.17 In recent studies of photoconductivity in individual NWs, scanning photocurrent microscopy has been a valuable tool for the investigation of these effects with the help of focused laser beam techniques. In this technique the individual NW can be locally probed to locate NW-electrode interface and the desired segment of the NW body along its length. It is well know that, devices fabricated using semiconducting NWs form non-Ohmic contacts with metal electrodes. Thus it is more likely that their contact properties play a crucial role in understanding the overall performance of the nanodevices. Thus, the locally probe techniques is highly desirable for investigating the contact properties and understanding the device physics mechanism in the region of interface. The electrical measurements for metallic single-walled carbon nanotube (SWCNT), at both ends of the contact generated short-circuit current manifesting an offset photovoltage.18 Mapping the electronic band structures by scanning photocurrent microscopy, could probe the origin of photocurrent. At zero bias the enhanced photocurrent response was observed close to the metal contacts in CNT.19 Investigation of localized photoresponse in Si NWs showed paolarization-sensitive, and high-resolution photodetector in the visible range. On locally probing the NWs with laser on the two ends near the contact interface, the Si NWs observed positive photoresponse at one end and negative on the other end at zero bias. Such phenomena have been explained as due to built in electric field near the contacts.20 However for such effect 2 Chapter 1 Introduction and Motivation the thermoelectric or thermal effects caused by the laser cannot be ruled out, which is one of the key findings in our experiment using focused laser beam technique for photocurrent measurements. Near-field scanning optical microscope (NSOM) has also been used for photocurrent measurement by allowing local illumination along the length of metal-NW-metal in CdS NW, and in the contact region.21 But then this technique could have limitation on power/intensity of the illumination of light used onto the NWs. Photocurrent generated at the Schottky contacts between the GaAs NW and the metal electrodes, interpreted that the photoconductance due to band bending effects caused by surface states on the NW surface.11 In controlled fabrication of Schottky and Ohmic electrical contacts in single CdS NWs, the localized photocourrent measurements for Schottky-barrier devices, found highly localized electric field in the contact region. And the photogenerated carriers diffuse from the nanowire channel region into the space-charge region or the Schottky-barrier region, where they were collected. In contrast, for the Ohmic device, both drift and diffusion were seen in different portions of the channel region. Under biased condition scanning photocurrent microscopy images and the transport characteristics were found to be similar for Schottky diodes, and those of Schottky-barrier (Ohmic) devices.22 Thus it is important to investigate the various mechanism and contributing factors to photocurrent in single NW devices for better device performance in various nano-electronics and nano-optoelectronics. 1.2 Motivation One-dimensional nanostructures are ideal system for exploring a large number of novel phenomena at the nano-scale with wide range of device applicability. Nanostructures as photodetectors are useful for applications such as binary switches in imaging techniques and 3 Chapter 1 Introduction and Motivation light-wave communication as well as in future storage and optoelectronic circuits. In metal-oxide nanostructures, the role of oxygen vacancies is predominant for the electronic properties similar to the bulk system. Considering various nanostructures, nanowires represents the smallest dimension for efficient transport of electrons and excitons, and thus can be used as interconnects and critical devices in future nano-electronics and nano-optoelectronics. In comparison to the film Photodetectors, one-dimensional metal-oxide nanostructures have several advantages as: (i) large surface-to-volume ratio with the carrier and photon confinement in two-dimension, (ii) superior stability owing to high order of crystallinity, and (iii) possible for surface functionalization with target-specific receptor series and FET configuration that allow the use of gate potentials controlling the sensitivity selectively. Considering the photocurrent measurement in single nanowires in our present work, it was our interest to see the possible mechanism and main contributing factors to photoresponse of metal oxide nanowires. The localized photocurrent measurements could provide insight into the photoresponse of NWs, including in the region of interface. 1.3 Brief outline of the present work In the present work, we investigated the studies of photocurrent in individual and isolated metal-oxide NWs (Nb 2 O 5 and V 2 O 5 ) by using global (spot size much larger than the length of the NWs) and localized focused laser beam irradiation in the visible and infrared region. Photoresponse of these NWs were investigated under different environmental conditions. Using focused laser beam techniques in our experiments, we can direct the laser beam locally in the region of NW-electrode (Pt) interface or the main body of the NW. This allows us to develop 4 Chapter 1 Introduction and Motivation better insight into the photoresponse of the NW. The photoresponse of metal-oxide NWs (with and without bias) towards visible and infrared laser irradiation was studied. Particularly, it was found that NW-Pt contact played a major role in the photoresponse of the nanowire device. The present work of photoconductivity studies in individual NW under local irradiation near the interface of NW-Pt contacts facilitate better understanding of photocurrent transport mechanism in nano-devices with light irradiation. This also highlighted the importance of localized photoconductivity techniques, so as to have better insight of nanowire based devices. Its importance could lie in the development of NW optoelectronic, and sensing devices with better performance control, knowing the role of contact contribution in NW devices. In this chapter motivation and brief outline of the present work is presented. In chapter 2 brief reviews on photoconductivity concepts, photoconductivity in one-dimensional nanostructures (nanowires) and some of the mechanism involved for photorespone in NWs are summarized. Chapter 3 deals with the experimental techniques. Chapter 4 and chapter 5 presents detailed study of photoconductivity in single Nb 2 O 5 and V 2 O 5 NWs, respectively. Finally, chapter 6 summarizes with some future works of this thesis. 5 Chapter 1 Introduction and Motivation References: 1 B. Tian, X. Zheng, T. J. Kempa, Y. Fang, N. Yu, G. Yu et. al, Nature (2007) 449, 885 2 R. Yan, D. Gragas, P. Yang, Nature (2009) 3, 569 3 Y. Li, F. Qian, J. Xiang, C. M. Lieber, Materials today (2006) 9, 18 4 L. Cao, J. S. White, J. S. Park, J. A. Schuller et. al, Nature materials (2009) 8, 643 5 J. Wang, M. S. Gudiksen, Xiangfeng Duan, Yi Cui, C. M. Lieber, Science (2001) 293, 1455 6 M. D. Kezenberg, B. Daniel, T. Evans, B. M. Kayes, M. A. Filler, M. C. Putnam, N. S. Lewis, H. A. Atwater, Nano. Lett (2008) 8, 710 7 Y. Cui, Q. Wei, H. Park, C. M. Lieber, Science (2001) 293, 1289 8 M. W. Ahn, K. S. park, J. H. Heo, D. W. Kim et. al, Senssors and Actuators B (2009) 138, 168 9 Y. H. Ahn and Jiwoong Park, Appl. Phys. Lett. (2007) 91, 162102 10 Q. H. Li, Y. X. Liang, Q. Wan, and T. H. Wang, Appl. Phys. Lett. (2004) 85, 6389 11 S. Thunich, L. Prechtel, D. Spirkoska, G. Abstreiter et. al, Appl. Phys. Lett. (2009) 95, 083111 12 H. Pettersson, J. Tragardh, A. I. Persson, L. Landin e.t al, Nano. Lett. (2006) 6, 2, 229 13 C. Soci, A. Zhang, B. Xiang, S. A. Dayeh, D. P. R. Aplin, J. Park, X. Y. Bao, Y. H. Lo, D. Wang, Nano. Lett. (2007) 7, 1003 14 Z. M. Liao, Y. Lu, J. Xu, J. M. Zhang, D. P. Yu, Appl. Phys. A (2009) 95, 363 15 T. Zhai, X. Fang, M. Liao, X. Xu, H. Zeng, B. Yoshio, D. Golberg, Sensors (2009) 9, 6504 16 S. P. Mondal, S. K. Ray, App. Phys. Lett. (2009) 94, 223119 17 J. Zhou, Y. Gu, Y. Hu, W. Mai, P. H. Yeh, G. Bao et. al, Appl. Phys. Lett. (2009) 94, 191103 18 K. Balasubramanian, M. Burghard, K. Kern, M. Scolari, A. Mews, Nano Letts. (2005) 5, 507 19 E. J. H. Lee, K. balasubramanian, J. Dofmüller R. Vogelgesang et.al, Small (2007) 3, 2038 20 Y. Ahn, J. Dunning, and J. Park, Nano Letts (2005) 5, 1367 6 Chapter 1 Introduction and Motivation 21 Y. Gu, E. S kwak, J. L. Lehsch, J. E Allen et. al. Appl. Phys. Letts. (2005) 87, 043111 22 Y. Gu, J. P. Romankiewicz, J. K. David et. al. J. Vac. Sci. Technol. B (2006) 24, 2172 7 Chapter 2 Photoconductivity in one-dimensional nanostructures Chapter 2 Photoconductivity in one-dimensional nanostructure 2.1 Introduction With extensive research in the synthesis techniques of various one-dimensional or quasione-dimensional nanostructures (nanowires) for the last few decades, there has been tremendous exploration on its fundamental nano-scale physical properties, with special attentions on their nano-electronics and nano-devices applications. To realize these nanostructures for future applications in electronics, optoelectronics and semiconductors, study of photoconductivity of these nanomaterials is one of the most important investigations embarked by researchers worldwide. Photoconductivity is widely studied property of materials, started with thin-film to presently in nanostructures. The photoconductivity of individual or a network of nanowires (randomly or aligned along preferred direction) is generally measured on placing/dispersing them on an insulating substrate (mostly Si/SiO 2 substrate), under external bias applied either in two probe or three probe (with back gate) metal electrodes configuration. Upon irradiation with light on the NW/NWs the electrical conductivity changes, thus providing light-sensing capabilities. The unique properties of individual or array of NW photoconductors such as light polarization sensitivity, light absorption enhancement, and internal photoconductivity gain, could be utilized for the realization of efficient and highly integrated optical, electronic and sensing devices.1-6 In this chapter some of the basic concepts of photoconductivity of metal-oxide NW are reviewed, highlighting some of the mechanism involved in photoconductivity of NWs, such as surface effect and contacts effects which are crucial in low dimensional nano-devices. 8 Chapter 2 Photoconductivity in one-dimensional nanostructures 2.2 Concepts in photoconductivity Photoconductivity is an important property of semiconductors in which the electrical conductivity changes on irradiation of incident light. Photoconductivity phenomena can be mainly described with electron activity in semiconductors. Photoconductivity involves the following mechanisms: absorption of the incident light, carrier photo-generation, carrier and transport including carrier trapping, de-trapping and recombination process. Thus, it can be divided into (a) intrinsic: band to band conduction or (b) extrinsic: excitation of electrons from defect or imperfect state (Figure 2.1). The extrinsic contribution to photoconductivity usually involves two step processes: (i) recombination with a carrier of opposite type, or (ii) be thermally excitation to the nearest energy band before recombination. The imperfection or defect state is referred to as trap, and the capture and release processes are called trapping and de-trapping.7-9 Figure 2.1 Schematic diagram showing intrinsic and extrinsic phenomena involved in photoconductivity. 9 Chapter 2 Photoconductivity in one-dimensional nanostructures Photoelectric phenomena involves, the concepts of optical absorption by which free carriers are created. These free carriers contribute to electrical transport and electrical conductivity of the material. The capture of free carriers leads to either recombination or trapping. Thus most photoconductivity effects are due to intrinsic or extrinsic optical absorption.9 The intrinsic conductivity of a semiconductor is given by; σ = enµ (2.1) Where e is the electronic charge, n is the charge carrier density, and μ is the carrier mobility. In the presence of applied electric field F=V/L. Where V is the voltage applied across a NW with length L. The current density is given by; J = σF = enυ (2.2) Where υ = µF is the carrier drift velocity. Under irradiation of light, we have a change in conductivity ∆n (carrier photo-generation) or a change in the carrier mobility ∆µ: ∆σ = σ light − σ dark = e( µ∆n + n∆µ ) (2.3) In general; J PC (t ) = [ µ (t )∆n(t ) + n(t )∆µ (t )]eF (2.4) Where J PC is the photocurrent, mobility and carrier density are time dependent. As in many semiconductor ∆n >>∆µ, thus the time dependence of the mobility can be neglected. Therefore the expression for the photocurrent density reduces to the form: J PC (t ) = ∆σF = eµ∆n(t ) F (2.5) The absorption properties of semiconducting NWs are strongly dependent on the polarization of the incident light.10-13 The main explanation for such phenomena are: (i) the modification of energy spectrum by size quantization of carriers, (ii) the dielectric confinement of the optical electric field due to the difference in the dielectric constants of the NW (ϵ) and the 10 Chapter 2 Photoconductivity in one-dimensional nanostructures environment (ϵ o ). The ratio of absorption coefficient for light polarization parallel and perpendicular to the NW axis is given by:10 ε + εo = k⊥ 2ε o k || 2 (2.6) Polarization dependent photoconductivity in single NW with light irradiation has been reported in many NW material systems.3,14,15 2.2.1 Steady-state photoconductivity When the light is illuminated on NWs, the optical absorption causes carrier generation and inter band excitation. Light absorption process can be described by: dI = −αI dx (2.7) ⇒ I ( x ) = I o e −α x (2.8) Where α is the absorption coefficient, I o intensity of incident photons and x is the direction along which absorption occurs. The steady-state photoconductivity under constant light irradiation directly depends on the majority carrier (electrons or holes) life time: ∆n=Gτ (2.9) Here, G is the photo-excitation rate and τ is the carrier’s lifetime. Thus, the photoconductivity equation and the total steady-state photocurrent density in NW: Thus, ∆σ=Ge(µτ) (2.10) J pc =∆σF (2.11) 11 Chapter 2 Photoconductivity in one-dimensional nanostructures Due to large surface to volume ratio, NWs contains extremely high density of surface states. Thus the surface potential and Fermi energy pinning at the surface strongly depends on the geometry of the NWs. These factors strongly influence the performance of NWs as photodectector devices.16 2.3 Photoconductivity in one-dimensional metal-oxide nanowires As material system with wide range of band gap energy, metal-oxide NWs are extremely important and attractive class of photoconductors. In addition, due to unique surface chemistry and photoconducting properties, metal-oxide NWs are suitable choices as biological, chemical and gas sensing devices.2,17 Among all, ZnO is the widely studied metal-oxide semiconducting NW. Its photoconductivity alone is vastly studied. Due to wide bandgap (3.34 eV at room temperature) and large excitonic binding energy (60 meV), ZnO NW finds applications as UV photodetectors.18-20 Single NW or networks (randomly or vertically oriented) arrays of ZnO NWs photodetectors have been extensively investigated.21 Literature reported 4 to 6 orders of decrease in magnitude of resistivity in ZnO on exposure to UV light (365 nm).9 The extremely long photocurrent relaxation time, relates to carrier trapping. Defect states played significant role in photocurrent response as well.20 The photoconductivity in ZnO NWs is mainly governed by a charge-trapping mechanism mediated by oxygen adsorption and desorption at the surface.7,19,22,23 Besides ZnO, variety of other metal-oxide semiconducting NW photodetectors have also been investigated, some of them are SnO 2 , β-Ga 2 O 3, In 2 O 3, Cu 2 O and V 2 O 5 NWs. SnO 2 nanostructured materials (bandgap = 3.6 eV) are ideal as transparent conducting electrodes for organic light emitting diodes and solar cells.24, 25 It has also been used as chemical sensors for environmental and industrial applications. Cu 2 O is a p-type direct band gap semiconductor. It 12 Chapter 2 Photoconductivity in one-dimensional nanostructures found applications as field-effect transistors, photovoltaic devices, sensors, and photo-electrodes in high-efficiency photo-electrochemical cells.26, 27 Cu 2 O is sensitive to blue light (488 nm) laser irradiation in air and at room temperature.26 Monoclinic gallium oxide (β-Ga 2 O 3 ) has wide bandgap of 4.9 eV,28, 29 it is chemically and thermally stable and has been widely used as an insulating oxide layer in gallium-based electrical devices. β-Ga 2 O 3 is an n-type semiconductor, which finds applications in high temperature gas sensing, solar cells, flat-panel displays and optical limiters for UV irradiation.30 β-Ga 2 O 3 NWs are sensitive to 254 nm wavelength and is a promising material for solar photodeterctor.31 In 2 O 3 NWs (direct bandgap of ~3.6 eV, and indirect bandgap ~ 2.5 eV) are reported as UV Photodetectors. It is highly responsive to 254 nm UV light, due to excitation of electrons from valance band to conduction band (excitation energy (4.9 eV) greater than the direct bandgap).32 And its sensitivity to 365 nm light is attributed to transition in indirect bandgap.32 V 2 O 5 NWs showed a week temperature dependent photocurrent upon exposure to white light, and its photoconductivity has been explained in terms of hopping-mediated transport.33 2.4 Factors contributing to photoresponse in one-dimensional metal-oxide nanowires 2.4.1 Surface effects In one-dimension nanostructures, it is possible that the surface approaches the bulk, and the defects segregate on the surface leaving a high quality bulk devoid of defects, thereby producing large difference in properties.34 Due to high surface-to-volume ratio in one dimensional nanostructure materials, study of interfacial properties is vital for photoconductivity in NWs.35, 36 13 Chapter 2 Photoconductivity in one-dimensional nanostructures From the literature, the photoconductivity in ZnO NWs is mainly attributed to surface states.37-39 The photoconductivity in NWs is highly dependent on surface absorbed oxygen molecules.35,39,40 The effect of water vapor, and other gas species also plays vital role in photoresponse in NWs.39-41 Due to the effect of water vapor and gas species, the shortening of the current decay in photoresponse has been reported.39-41 However, the mechanism of water interaction with surface of metal oxide NWs is still a subject of fundamental interest.42, 43 2.4.2 Photoresponse in dry and wet air The photoresponse of NWs in dry air, are generally governed by adsorption of oxygen molecules on the surface of the NWs.35-42 The presence of oxygen molecules adsorbed at the surface of NWs decrease the carrier density in NWs in dark, by trapping free electrons [O 2 ( g ) + e − → O2− (ad )] in n-type semiconducting NWs. This decreases the mobility of the remaining carriers by creating depletion layers near the surface, and leads to band bending near the surface.39 Because of large surface-to-volume ratio in NWs, the adsorption of O 2 molecules significantly decreases the conductivity in the NWs. On irradiation of light on NWs, electronhole pairs are generated [hν → e − + h + ] . This results increase in photoconductivity, because of increased carrier densities in NWs. In the process, holes migrate to the surface along the potential slope created by the band bending and the recombine with the O 2 -trapped electrons, thus releasing O2− from the surface [O2− (ad ) + h + →O 2 ( g )] . The remaining unpaired electrons become the major carriers that would contribute to the current, unless they are trapped again by re-adsorbed O 2 on the surface. The unpaired electrons accumulate gradually with time until the de-sorption and re-adsorption of O 2 reach an equilibrium state, resulting in a gradual rise in current until saturation during light irradiation. At the end of the illumination, the hole density is 14 Chapter 2 Photoconductivity in one-dimensional nanostructures much lower than electron density. Although holes recombine quickly with electrons upon turning off the irradiated light, there would still be lot of electrons left in the NWs. O 2 molecules gradually re-adsorb on the surface and capture these electrons, which results in a slow current decay.44 Photoresponse is also greatly affected by surrounding wet air, with the presence of water molecule. Under dark condition, the water molecules probably replace the previously adsorbed and ionized oxygen, releasing electrons from the ionized oxygen molecules, partially annihilating the depletion layer resulting rise in conductivity.45 Water molecules from the atmosphere can be physisorbed followed by chemisorbed that can capture electrons onto the surface of the NWs.41 2.4.3. Electrical contacts For the measurements of transport properties in semiconducting materials including in nanoelectronics, it is ordinarily necessary to make electrical contacts to the material, usually with metallic contacts. However, when it comes to making electrical contacts in nanostructures, it might not be easy and straightforward. Thus it becomes an important issue in understanding the electrical properties in NW-metal electrodes. Nevertheless, with advances in technology, many techniques such as optical lithography, electron beam lithography and focused ion beam techniques are utilized as a tool for fabricating electrical contacts in nano-devices and nanoelectronics. When metal-semiconductor contact is made, it can either be an Ohmic or Schottky barrier depending on the Fermi surface alignment and the nature of the interface between the metal and the semiconducting nanowire. The ohmic contact can likely to be treated as Schottky barrier having zero barrier height. Thus the metal-semiconductor-metal (metal-nanowire-metal) 15 Chapter 2 Photoconductivity in one-dimensional nanostructures structure can be modeled as two Schottky barrier connected back to back, in series with semiconductor having resistance as shown in Figure 2.2. Figure 2.2 Schematic diagrams representing (a) metalnanowire-metal contact nano device structure on SiO2/Si substrate. (b) Two Schottky barrier modeled as back-to-back diode connected in series. (c) Energy band diagram of metalsemiconductor-metal structure at equilibrium. To study the intrinsic properties of NWs a good electrical contact is highly desired. But the ideal contacts may not be realized. Most of the semiconducting NWs measured follow nonlinear I-V characteristics. The literature reports on transport properties of NWs have demonstrated influence on contact between metal electrodes and semiconducting NWs.45-49 Several important factors, including dimensionality-dependent Schottky barriers, oxidation of metal electrodes and/or NWs, fringing field effects, interfacial trap states, and others have been demonstrated.47,50-52 Carriers in many oxide materials typically originates from defect level states including oxygen vacancies (n-type) and cation vacancies (p-type).53 Stoichiometry at the interface should affect significantly the carrier injection from electrodes/metal to oxide NWs. 16 Chapter 2 Photoconductivity in one-dimensional nanostructures With the aid of photoconductivity as experimental techniques, the studies of NW-electrode interface is possible. Recent studies of photoconductivity of individual NW using field optical microscopy or localized focused beam techniques have been reported, where one can direct the laser beam towards the NW-electrode interface or the main body of the NW and thus develop a better insight into the photoresponse of the NW3, 54, 55 Photoconductivity in single NWs could also be affected by thermoelectric effect, a subjective of our investigation in this work. 17 Chapter 2 Photoconductivity in one-dimensional nanostructures References: 1 Y. Li, F. Qian, J. Xiang, C. M. Lieber, Materials Today (2006) 9, 18 2 Y. Cui, Q. Wei, H. Park, C. M. Liber, Science (2001) 293, 1289 3 Y. H. Ahn, J. Park, Apl. Phy. Letts. (2007) 91, 161202 4 L.Cao, J. S. White, J. S. Park, J. A. Schuller, B. M. Clemens, Nature Mat. (2009) 8, 642 5 B. Tian, X. Zheng, T. J. Kempa, Y. Fang, N. Yu, G. Yu, J. Huang, C. M. Lieber, Nature (2007) 449, 885 6 R. Yan, D. Gargas, P. 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Z. W. Liu, S. P. Ringer, Y. Bando, D. Golberg, ACS Nano (2008) 2, 107. 29 P. Feng, X. Y. Xue, G. Y. Liu, Q. Wan, T. H. Wang, Appl. Phys. Lett. (2006) 89, 112114 30 Y. Huang, Z. L. Wang, Q. Wang, C. Z. GU, C. C. Tang, Y. Bando, D. Golberg, Phys. Chem. C. (2009) 113, 1980. 31 P. Feng, Y. J. Zhang, Q. H. Li, T. H. Wang, Appl. Phys. Lett. (2006) 88, 153207. 32 D. Zhang, C. Li, S. Han, X. Liu, T. Tang, W. Jin, C. W. Zhou, Appl. Phys. A (2003) 77, 163 33 J. Park, E. Lee, K. W. Lee, C. E. Lee, Appl. Phys. Lett. (2006) 89, 183114. 34 J. S. Jie, W. J. Zhang, Y. Jiang, X. M. Meng, Y. Q. Li, S. T. Lee, Nano Lett. (2006) 6, 1887 35 C. Soci, A. Zhang, B. Xiang, S. A. Sayeh, D. P. R. Aplin, J. Park, X. Y. Bao, Y. H. Lo, D. Wang, Nano Lett. (2007) 7, 1003. 36 A. Bera, D. Basak, Appl. Phys. Lett. (2008) 93, 053102 19 Chapter 2 Photoconductivity in one-dimensional nanostructures 37 Z. M. Liao, K. J. Liu, J. M. Zhang, J. Xu, D. P. Yu, Phys. Lett. A (2007) 367, 207 38 Z. M. Liao, H. Z. Zhang, Y. B. Zhou, J. Xu, J.M. Zhang, D. P. Yu, Phys. Lett. A (2008) 372, 4505 39 Q. H. Li, T. Gao, Y. G. Wang, T. H. Wang, Appl. Phys. Lett. (2005) 86, 123117. 40 J. B. K. Law, J. T. L. Tong. Appl. Phys. Lett. (2006) 88, 133114 41 X. Xie, F. C. Cheong, B. Varghese, Y. W. Zhu, R. Mahendrian, C. H. Sow, Sens. Actuators B (2010) in press. 42 S. Suzuki, K. Fukui, H. Onishi, Y. Iwasawa, Phys. Rev. Lett. (2000) 84, 2156 43 C. Wӧll, Prog. Surf. Sci. (2007) 82, 55 44 A. Bera, D. Basak, Appl. Phys. Lett. (2009) 94, 163119 45 Z. Chen, C. Lu, Sens. Lett. (2005) 3, 274 46 Z. Zhang, K. Yao, Y. Liu, C. Jin, X. Liang, Q. Chen, L. M. Peng, Adv. Funct. Mater. (2007) 17, 2478 47 Y. Gu, L. J. Lauhon, Appl. Phys. Lett. (2006) 89, 143102 48 Z. R. Wang, G. Zhang, K. L. Pey, C. H. Tung, G. Q. Lo, J. Appl. Phys. (2009) 105,09458 49 Y. F. Lin, W. B. Jian, Nano. Lett. (2008) 8, 3146 50 B. S. Simpkins, M. A. Mastro, C. R. Eddy, Jr, P. E. Pehrsson, J. Appl. Phys. (2008) 103, 104313 51 J. Hu, Y. Liu, C. Z. Ning, R. Dutton, S. M. Kang, Appl. Phys. Lett. (2008) 92, 083503 52 K. Nagashima, T. Yanagida, A. Klamchuen, M. Kanai, K. Oka, S. Seki, T. Kawai, Appl, Phys. Lett. (2010) 073110 53 A. K. Singh, A. Janotti, M. Scheffler, C. G. Van de Walle, Phys. Rev. Lett. (2008) 101, 055502 20 Chapter 2 Photoconductivity in one-dimensional nanostructures 54 Y. Gu, E. S. Kwak, J. L. Lensch, J. E. Allen, T. W. Odom, L. J. Lauhon, Appl. Phys. Lett. (2005) 87, 043111 55 S. Thunich, L. Prechtel, D. Spirkoska, G. Abstreiter, A. F. Morral, A. W. Holleitner, Appl. Phys. Lett. (2009) 95, 083111 21 Chapter 3 Fabrication and Characterization Techniques Chapter 3 Fabrication and Characterization Techniques In this chapter, the synthesis of metal-oxide and the characterization techniques used are detailed. Niobium and Vanadium oxide nanomaterials were synthesised using thermal oxide and hotplate techniques, and investigated with various characterization techniques. The electrical characterization techniques for transport properties of individual nanowire device and the home built experimental setup for photoconducting studies are also provided. 3.1 Niobium and vanadium oxide nanomaterials synthesis techniques 3.1.1 Cleaning of substrate/metal foil The substrate/metal foil (Niobium or Vanadium foil) purchased from Sigma-Aldrich was cut into pieces typically of about 0.5 cm square. The substrate/metal foil was then polished with sand paper to remove the dust particles and stain. After which the foil was put in ultrasonic bath in deionised water, followed by acetone each for about 15 minutes and then finally again ultrasonicated with deionised water, so as to have clean and smooth foil. Finally the foil was dried using nitrogen gas. 3.1.2 Thermal oxidation techniques for the synthesis of Nb 2 O 5 nanowires A horizontal tube furnace from Carbolite was used for the controlled synthesis of Nb 2 O 5 nanostructures by thermal oxidation techniques. The main component of the tube furnace contained a ceramic tube of diameter ~10 cm with both ends vacuum sealed using O-rings. One end of the ceramic tube was connected to a rotary pump and the lowest achievable pressure of 22 Chapter 3 Fabrication and Characterization Techniques this set-up was ~ 2 x 10-2 mbar. While different gases can be introduced from the other end of the tube controllably by mass flow controller. The cleaned Nb-metal foil (purchased from SigmaAldrich 0.25mm thick, 99.8%) was placed in small quartz tube of smaller diameter ~ 2.5 cm. This small tube was then carefully placed inside the big ceramic tube so that the location of Nb foil was exactly at the hottest region of the tube furnace set at 900 oC. The system was then evacuated to a base pressure of ~ 2 x 10-2 mbar. This was then followed with the flow of argon (Ar) gas at the rate of 25 standard cubic centimetre per minute (sccm) and pressure maintained at 1Torr. The temperature of the furnace was the raised at the rate of 20 oC/minute. After reaching the required temperature the growth process for 2 hour was further initiated with the flow of oxygen gas at the rate of 25 sccm. After the growth, the oxygen flow was terminated and the system was left to cool down room temperature while Ar gas was kept flowing.1 A schematic of the entire system is shown in Figure 3.1. Figure 3.1 Schematic diagram of tube furnace set up with all its necessary components for the growth of nanostructures. 23 Chapter 3 Fabrication and Characterization Techniques 3.1.3 Hot plate techniques for the synthesis of V 2 O 5 nanowires Hotplate techniques are easy and cost effective techniques developed for synthesis of various metal-oxide nanostructures in our group. The hotplate from Barnstead/Thermolyne, can be set to desirable temperature with digital display on it. Vanadium foils (99.98%) purchased from Sigma-Aldrich were cleaned and dried as described above. The foil was then placed on the hotplate, and a SiN substrate was placed on top of the foil. The hotplate was heated to a temperature of ~540 oC and maintained at this temperature for 3 days.2 This technique allowed the growth of V 2 O 5 nanowires on the SiN substrate. The SiN substrate used was 200 nm thick SiN film with hollow microholes. The film was framed by a 300 µm thick frame. Figure 3.2 shows the hotplate used to fabricate V 2 O 5 nanowires. Figure 3.2 Hotplate for the growth of V2O5 nanowires on SiN substrate. 24 Chapter 3 Fabrication and Characterization Techniques 3.2 Characterization Methods and Techniques 3.2.1 X-Ray Diffraction (XRD) Analysis X-Ray diffraction (XRD) is a well known tool for determining the crystal structure, grain size and internal strain of crystalline materials. XRD is a non destructive technique. In this method, structural information such as crystalline order of the nanostructure is determined through Braggs Law. Also, accurate values of the d spacing are determined by X-ray diffraction. In all crystalline materials the atoms are oriented in a regular way (Figure 3.3). This arrangement of atoms forms different planes of the crystal. When X-ray falls on a crystalline material it reflects from different planes. According to Bragg, the reflected X-rays will create a diffraction pattern, when the inter-planar distance (d hkl ) satisfies the relation 2d hkl sinθ hkl =nλ (3.1) Where θ is the angle of incidence of the X-ray beam, λ is the wavelength of the X-ray radiation used, (hkl) are Miller indices of a particular crystal plane and n is the order of diffraction. This equation can be used to calculate the d-spacing of different crystal planes. The direction of the reflected beams are determined by the orientation and spacing of the crystal planes. 25 Chapter 3 Fabrication and Characterization Techniques Incident rays Reflected rays θ N θ Lattice plane d Figure 3.3 The relationship between atomic planes, incident X-rays and reflected X-rays in XRD analysis. The metal foil with nanostructures on the surface was used for recording XRD spectrum o using Philips X’PERT MRD (Cu-Kα (1.542 A ) radiation) system. Due to large penetration length of the X-ray, the XRD spectrum comprises peaks that correspond to the supporting metal foil in addition to the peaks that originate from the oxide nanostructures. 3.2.2 Raman Spectroscopy Raman spectroscopy is a non-destructive technique and requires no contacts to the sample. Raman spectroscopy is based on Raman effect, in which the inelastic scattering of electromagnetic waves due to the photon-photon interaction within the material. Most oxides nanostructures can be characterized by Raman spectroscopy. In a typical set-up, the laser is incident on the sample and the shift in wavelengths of the scattered light are collected, analysed and matched to known wavelengths for identification. Various properties of the sample can be characterized. Its composition and size can be determined. Raman spectroscopy is sensitive to 26 Chapter 3 Fabrication and Characterization Techniques crystal structure. The nanostructures fabricated on the metal foil, as such was used for recording Raman spectrum using a Renishaw system2000 micro-Raman system. In this Raman system, the polarized diode laser of wavelength 514 nm was focused on the nanowires using 50x objective lense (NA: 0.9) microscope. The spectrum data was collected by the computer system for further analysis. 3.2.3 Scanning Electron Microscope (SEM) An electron microscope utilizes an electron beam (e-beam) to produce a magnified image of the sample. There are three principle types of electron microscopes; scanning, transmission, and emission. In the scanning and transmission electron microscope, an electron beam incident on sample produces an image. SEM is similar to light microscopy with the exception that electrons are used instead of photons and the image is formed in a different manner. The use of electrons has two main advantages over optical microscopes: much larger magnification is possible since electron wavelengths are much smaller than photon wavelengths and the depth of field is much higher. The electron wavelength λ e depends on the electron velocity v or the accelerating voltage V as λe = h h 1.22 = = (nm) mυ 2qmV V 3.2 The wavelength is 0.012 nm for V = 10kV; a wavelength significantly below the wavelength range of visible light (400nm to 700 nm), making the resolution of SEM much better than that of an optical microscope. The image in SEM is produced by scanning the sample with focused electron beam and detecting the secondary and or/backscattered electrons. Secondary 27 Chapter 3 Fabrication and Characterization Techniques electrons form the conventional SEM image. Basic components of a SEM are an electron gun, a magnetic lens system, scanning coils, an electron collector and a cathode ray tube for viewing the image. The electron gun provides a stable source of electrons, which are accelerated to the operating voltage of the microscope by an anode plate. The condenser and the objective lenses focus the beam into a fine spot, the diameter of which ultimately determines the resolution of the microscope. To prevent the impact of the electrons with molecules in the environment, the column is kept at a vacuum of 10-7 Torr or better. Some of the electrons escaping from each impact point at the surface are collected, and the intensity of this signal is used to modulate the brightness of the viewing screen. The electrons vary in energy from a few eV to keV, and their collective behaviour and intensity are strongly influenced by the surface topography and chemical makeup of the sample. Scanning coils deflect the spot in a television-like raster over the surface of the sample. These are controlled by a saw tooth waveform that also drives the X-Y input of the viewing screen, so that the rastering on the sample is identical point-by-point to that being traced on the Cathode Ray Tube. Though identical in shape, the traces are considerably different in size. In fact, it is the ratio of trace length on the imaging screen to that on the sample that determines the magnification of the microscope. Probe electrons that scatter within the solid and eventually escape through the surface are called backscattered electrons. The efficiency on backscattering process improves with the increasing atomic number of atoms in the solid. It is also possible for electrons within the shells of target atoms to gain enough energy in a collision to break away and escape for detection. These are secondary electrons. Secondary electron emission intensity is particularly sensitive to the chemical make-up of the sample and the surface work function. Intensity variations are the basis for contrast in imaging roughness, thin films, and hillocks and etch pits, as well as particles and contaminations. In this work, morphologies of 28 Chapter 3 Fabrication and Characterization Techniques the Nb 2 O 5 and V 2 O 5 were envisioned by the field-emission scanning electron microscope (FESEM, JEOL JSM-6700F). The typical acceleration voltage for electron used for the imaging was in the range 5-10 kV and the emission current 5-20 µA. 3.3 Nano-device Fabrication Techniques 3.3.1 Photolithographic techniques A photolithographic technique was used to pattern gold (Au) finger electrodes with the gap of about ~ 10 μm. The standard steps for the photolithography process is shown in the figure 3.4. Heavily n-doped Si substrates (Resistivity ~1-10 Ohm.cm) with 100 nm thick insulating oxide layer were used as the supporting substrate for the patterned electrodes. The clean Si/SiO 2 (cleaned as described above for Nb metal foil) substrate was spin coated with photoresist at the rate of 1500 rotation per minute (rpm) for 30 seconds and the baked in a hot plate for ~15 minutes at 100 oC. The substrate was then masked and exposed to ultra violet (UV) irradiation for 2 seconds. After which it was rinsed in a microresist developer. After development, the substrate was sputtered with Au (~ 100 nm thickness). Finally it was put in acetone for one night for lift up. 29 Chapter 3 Fabrication and Characterization Techniques Figure 3.4 (a) Schematic diagram representing the steps for photolithography process, (b) Au finger electrodes on SiO2/Si substrate. 30 Chapter 3 Fabrication and Characterization Techniques 3.3.2 Single nanowire(NW) device fabrication The single NW devices were fabricated by transferring individual NW from the growth substrates to the patterned Au electrode SiO 2 /Si substrates, with the aid of tungsten needle probes (tip size ~75 nm) attached to a micro-positioner under an optical microscope (CascadeTM Microtech). The NW was first electrostatically attached to the tungsten probes by direct contact, and then transferred to the SiO 2 /Si substrate by exploiting the Van der Waals force between the substrate and the NW. The ends of these NW were then electrically connected to the Au electrodes by depositing Pt (300nm in thickness) using a dual beam focused ion beam system (Quanta 200-3D FIB-SEM, FEI Company, Ga+ ion beam operated at 30 kV, 50 pA). The schematic diagram of the device is shown in the Figure 3.5. Figure 3.5 Schematic diagram of single nanowire device with Pt contact between the NW and the Au electrodes. 31 Chapter 3 Fabrication and Characterization Techniques 3.4 Electrical Characterization of Single Nanowire The single nanowire device prepared as shown in Figure 3.5 was employed for electrical transport measurements. The two point electrical measurements was carried out in either ambient or vacuum (~ 10-6 torr) environment at room temperature. Keithley 6430 sub-femto amp remote source meter was connected to the external leads from the nano-device for current-voltage and photoresponse measurements. 3.5 Photoconductivity Measurement Techniques Two different methodologies were employed as photoconductivity measurement techniques for individual nanowire devices; (i) global irradiation and (ii) localized irradiation. 3.5.1 Global irradiation technique Figure 3.6(a) below represents the schematic diagram of individual nanowire device with global irradiation (spot size of laser beam larger than the gap between the electrodes). The diameter of the laser is about ~ 3 mm, this would obviously means that the irradiation includes the contact region of the electrodes too. Thus such irradiation approach was denoted as broad beam/global irradiation approach. Figure 3.6(b) represents the schematic diagram for experimental set-up of nano-device in vacumm environment with global irradiation. 32 Chapter 3 Fabrication and Characterization Techniques Figure 3.6 (a) Schematic diagram of individual nanowire device with global irradiation (spot size larger than the electrodes gap). (b) Schematic diagram of individual nanowire device inside the vacuum chamber for photocurrent measurements in vacuum environment with global irradiation. 3.5.2 Localized irradiation technique Schematic home built experimental set-up for photoconductivity with focused laser irradiation of laser beam is shown in Figure 3.7. The laser beam can be focused to a diffraction limited spot size of ~1 µm using 100X objective lens (Leica, NA ~0.75) of the microscope with our set-up in nanomaterial research laboratory. Thus the irradiation of focused laser beam facilitates localized photoresponse studies along different parts of the NW. The laser beam is focused after passing through the microscopic objective lense. This technique was used for the study of photo-response from the contact points and middle of the individual nanowire devices. 33 Chapter 3 Fabrication and Characterization Techniques Figure 3.7 Schematic experimental setup of localized photoconductivity techniques probed at individual nanowire device. Reference 1 B. Varghese, C. H. Sow, C. T. Lim, J. Phys. Chem. C (2008) 112, 10008 2 Y. Zhu, Y. Zhang, L. Dai, F. C Cheong, V. Tan, C. H. Sow, C. T Lim, Acta Materilaia (2010) 55, 415 34 Chapter 4 Photoconductivity of Individual Nb2O5 Nanowire Chapter 4 Photoconductivity of Individual Nb 2O5 Nanowire 4.1 Introduction Niobium oxide is known to occur in many forms such as NbO, NbO 2 , Nb 2 O 3 and Nb 2 O 5 . Among all the Niobium oxide, Nb 2 O 5 is oxygen-rich and thermodynamically the most stable phase. Crystalline Nb 2 O 5 can be obtained by oxidation of metallic niobium by heating the metallic niobium foil up about 800-1000 oC. Amorphous Nb 2 O 5 can be formed by heating niobium powder between 260 oC and 350 oC or by dehydration of niobium hydrous oxides. The temperature and treatment time are the critical conditions for various crystalline modifications. Nearly all the phase changes are irreversible.1,2 Niobium oxide (NbO) has a unique structure, which gives each metal atom a square coordination. Nb 2 O 5 has molecular weight MW=265.82 g/mol and a melting point MP=1495oC. Among the different polymorphs, H-Nb 2 O 5 which crystallized at temperature > 1000 oC with monoclinic structure is the thermodynamically most stable form.3 The Nb 2 O 5 formed at temperature range 800-1000 oC is normally labelled as M-Nb 2 O 5 with tetragonal or monoclinic structure. Nb 2 O 5 formed at a temperature range 700-800 oC crystallizes in orthorhombic structure and known as T-Nb 2 O 5 . The least stable polymorph of Nb 2 O 5 is the TT-Nb 2 O 5 , which crystallises at a temperature < 700 oC with pseudo-hexagonal structure. Many of these forms are metastable under normal conditions, and some of them are structurally quite similar. They can be easily converted to the most stable H-Nb 2 O 5 structure by heating to high temperatures. Thus the 35 Chapter 4 Photoconductivity of Individual Nb2O5 Nanowire phase transformation of niobium oxide strongly depends on the preparation method of the compound and the heat treatment. Traditionally, niobium pentoxide is used in metallurgy for the production of hard materials. In optics it is used as an additive to molten glass to prevent the devitrification and to control the properties such as refractive index and light absorption of special glasses. Nb 2 O 5 is an intrinsic n-type semiconductor material with wide band gap of ~ 3.4 eV.4 There are only a few research work carried out on Nb 2 O 5 nanostructures and its functional properties.5-10 Nb 2 O 5 nanostructures have found applications in field emission,7 gas sensing,8,9 as electrochromic materials10 and catalysis.11 It also shows potential in nano-electronics and nano-mechanical devices.12 As a wide band gap material, photoconductivity of these nanowires would be of great interest. In this chapter, studies of photocurrent of individual and isolated Nb 2 O 5 NW by using global (spot size much larger than the length of the NWs) and localized focused laser beam irradiation is presented. 4.2 Experimental Section Nb 2 O 5 NWs were synthesized by thermal oxidation of Nb foils purchased from SigmaAldrich (0.25mm thick, 99.8%), in a horizontal tube furnace at 900 oC with the parameters as described in section 3.1.2. The morphology and characterization of as grown nanostructures were obtained using field emission scanning electron microscope (FE-SEM, JEOL JSM-6700F), X-ray diffraction (XRD, X’PERT, Cu-K α (1.542 nm) radiation) and micro Raman spectroscopy (Renishaw system 200, excitation wavelength 532 nm). 36 Chapter 4 Photoconductivity of Individual Nb2O5 Nanowire 4.2.1 Characterization of Nanostructure (a) Morphology: The Figure 4.1 shows the FE-SEM image of the Nb 2 O 5 nanowires grown on niobium metal foil after thermal heating at temperature ~900 oC for 2 hours in vacuum as described in section 3.1.2. The morphology in Figure 4.1 shows that the nanowires are vertically free standing and uniformly grown. The length of the nanowires falls in the range of 10-30 μm, and the tip of the nanowires are sharp with a tip size of ~10-50 nm. Morpholoy of Nb 2 O 5 nanostructure is very much dependent on growth temperature. (b) X-ray diffraction (XRD): XRD spectrum of the nanostructures fabricated at temperature 900 oC supported on the Nb foil is displayed in Figure 4.2. The peak observed at 47.6o is from Nb substrate. All the peaks can be indexed to tetragonal Nb 2 O 5 (JCPDS: 74-1484) phase structure. Figure 4.1 FE-SEM image of Nb2O5 nanowires grown in Nb-metal foil with thermal oxidation techniques at 900 oC. 37 Photoconductivity of Individual Nb2O5 Nanowire 20 40 50 60 (15 0 1) (14 8 0) (303) (15 4 1) (433) (14 4 0) (11 3 2 ) (222)(941) (11 3 0) (10 6 0) (532) (10 5 1) (11 4 1) (13 1 0) (12 3 1 ) (002) 30 (770) (640) (431) (521) (800) (541) (701) (440) (600) (321) (301) Intensity (a.u) (101) Chapter 4 70 80 2θ (degrees) Figure 4.2 XRD spectrum of Nb2O5 nanowires grown in Nb-metal foil with thermal oxidation techniques at 900 oC. (c) Micro Raman spectroscopy: The micro-Raman spectrum of the Nb 2 O 5 nanostructure on heated Nb-foil at 900 oC, were collected in back scattering configuration at room temperature. The Renishaw system2000 micro-Raman system used a diode laser that emits laser beam with a wavelength of 514 nm that was focused by a 50x objective lens for irradiation of the sample. Figure 4.3 shows the micro-Raman spectrum collected from the Nb 2 O 5 nanostructures sample. From the spectrum, the A 1g bands observed in the 700-1000 cm-1 region corresponded to the longitudinal optical (LO) modes of the Nb-O stretching associated with NbO 6 octahedral and NbO 4 tetrahedral. The spectra in the range 600-700 cm-1 corresponds to transverse optical (TO) modes E g . The shoulder peak in this region may be due to overlap from the T 1u bands. The weak bands observed in the 300-560 cm-1 were assigned to be T 2g mode. The strongest peak observed 38 Chapter 4 Photoconductivity of Individual Nb2O5 Nanowire in 200-300 cm-1 are assigned to the T 2u modes. These results are consistent with the previous studies on Nb 2 O 5 single and nanocrystalline powder.6,13 Intensity (a. u.) A1g 0 T2u T2u E2g E2g T2g T2g 200 T2g A1g 400 600 800 A1g -1 1000 1200 Raman Shift (cm ) Figure 4.3 Raman spectrum of as grown Nb2O5 nanostructures. 4.3 Nb 2 O 5 nano-device fabrication and electrical characterization Heavily n-doped Si substrates (Resistivity ~1-10 Ohm-cm) with a thick insulating oxide layer (100 nm) were used to construct single NW devices. These substrates were pre-patterned with gold (Au) electrodes in two-probe configurations using standard photolithography as discussed in section 3.3. The gap between the two Au finger electrodes was 10 µm. The single NW devices were fabricated by transferring individual NW from the growth substrates to the patterned Au electrode SiO 2 /Si substrates, with the aid of tungsten needle probes (tip size ~75 nm) attached to a micro-positioner under an optical microscope (CascadeTM Microtech). The NW was first electrostatically attached to the tungsten probes by direct contact, and then transferred 39 Chapter 4 Photoconductivity of Individual Nb2O5 Nanowire to the SiO 2 /Si substrate by exploiting the Van der Waals force between the substrate and the NW. The ends of these NW were then electrically connected to the Au electrodes by depositing Pt (300nm in thickness) using a dual beam focused ion beam system (Quanta 200-3D FIB-SEM, FEI Company, Ga+ ion beam operated at 30 kV, 50 pA). The SEM image of the individual Nb 2 O 5 nanowire fabricated is as shown in Figure 4.4. Figure 4.4 SEM image of individual Nb2O5 nanowire device fabricated in Au electrodes with Pt contacts on both ends of the NW. We examined the transport properties of as fabricated NW device under ambient environment at room temperature. Figure 4.5 displays a typical nonlinear I-V characteristic of a semiconducting Nb 2 O 5 NW. A typical SEM image of the fabricated device is displayed in the Figure 4.4. The I-V characteristic showed symmetrical and nonlinear response in positive and negative bias condition. The NW connected with high work function metal electrodes at both ends can be generally modeled as a circuit containing two Schottky junctions connected back-toback.14 When external bias was applied, one of these Schottky junction became forward biased 40 Chapter 4 Photoconductivity of Individual Nb2O5 Nanowire and the other became reversely biased. The current through such NW circuit was mainly controlled and limited by the response of the reversely biased Schottky junction. Figure 4.5 Typical I-V characteristics of individual Nb2O5 nanowire measured at room temperature. 4.4 Photoconductivity study The photoconductivity measurements of single NW were carried out by irradiating the NW with laser beam from continuous wave diode lasers. As mentioned in section 3.5 two approaches were implemented for the measurements of photoconductivity: the traditional approach where the laser was irradiated as (i) broad beam or global (spot size was much larger than the length of the NW) irradiation to the NW devices with the laser spot size of ~3 mm, and in the other (ii) focused laser beam approach where the laser beam was focused to a diffraction limited spot size of < 1µm using 100x objective lens (Leica, NA ~0.75) of an optical microscope. 41 Chapter 4 Photoconductivity of Individual Nb2O5 Nanowire Figure 4.6 represents the schematic irradiation of laser on NW with the above mentioned approaches (global and localized irradiation). Figure 4.6 Schematic representation of individual nanowire device for photoconductivity measurements with (a) global and (b) localized irradiation. The electrical measurements were carried out using Keithley 6430 source meter under zero and applied external bias conditions. Unlike the photoconductivity with global irradiation, the focused laser beam irradiated (with area of < 1µm) had the advantage of probing the Nb 2 O 5 NWs selectively along the length of the NW so that we can specifically target NW-Pt interface region for the photoresponse. The measurements carried out in these individual NWs had consistent and reproducible results. With the global irradiation the photoconductivity were measured in an ambient as well as in vacuum condition (~10-6 Torr). The schematic diagram for photoconductivity under vacuum condition with global irradiation is represented in Figure 3.6(b). The laser was irradiated from the top of the vacuum chamber through a transparent glass 42 Chapter 4 Photoconductivity of Individual Nb2O5 Nanowire window. The device was electrically connected through the external leads of the chamber to the source meter. 4.4.1 Photoresponse of individual Nb 2 O 5 NW to global irradiation The global irradiation to individual NW was subjected with a laser spot size of ~ 3 mm. The laser system used in this case emits laser beam with a wavelength 808 nm and adjustable power (maximum power of 200 mW). Here, the presence of laser irradiation shall be denoted as the “on” state. We made use of a card to block the laser beam from irradiating the nanowire and this shall be denoted as “off” state. Photocurrent experiments were carried out by measuring the current passing through the NWs as a function of time subjecting to the presence (on) and absence (off) of the laser beam. Figure 4.7(a) represents the on/off photocurrent response corresponding to the laser irradiation (λ=808nm, power=170mW) at zero bias under ambient condition. Figure 4.7(b) represents the photocurrent response at an applied external bias of 3V in ambient and vacuum (~10-6 torr) conditions respectively. For the photocurrent measurements in vacuum environment, the laser was allowed to globally irradiate on the NW device from top of the vacuum chamber through a transparent window (see Figure 3.6(b)). In both cases the laser power was maintained at ~ 170 mW. At zero bias, sharp and prominent photocurrent response was observed with the on/off of laser irradiation. While at external applied bias, the photoresponses comprised of a rapid and a slow varying components with on/off of laser irradiation. The photocurrent measured under vacuum environment (~ 10-6 Torr) at room temperature increased by ~ 41% ( (∆I Vacuum − ∆I Ambient ) ∆I Ambient × 100% ) compared to that measured at ambient condition. 43 Chapter 4 Photoconductivity of Individual Nb2O5 Nanowire Figure 4.7 (a) Photocurrent measured at zero bias, under ambient condition. (b) Photocurrent measured at applied bias of 3V, under ambient and vacuum environment, (808nm wavelength, power ~ 170mW). The energy of the laser photon used is less than the band gap energy of the Nb 2 O 5 NWs. The NWs are likely to have many defect level states8,9, which probably lies near mid band energy. Thus when the laser was irradiated on the NW, free electrons (or holes) are likely to be excited to/from the defect level state. Under the biased condition, these charge carriers can be separated and motion of these carriers led to the detected photocurrent. Notably at the NW-Pt contact (Schottky contact), the presence of localized electric field could further enhance the magnitude of the photocurrent. These contributions are mainly responsible for the observed rapid photocurrent effect. In addition, laser induced thermal heating of the NW, carrier thermalization trapping at the NW and interaction of the surface states of the NWs with the laser irradiation are possible contributors to the measured photocurrent as well. These factors tend to introduce a slower photoresponse in the NW. Hence the photocurrent from these contributions exhibits different characteristic time scales with distinct rapid and slowly varying components as evident in Figure 4.7(b). Probing the detail nature of the defects in the Nb 2 O 5 nanowires is a challenging 44 Chapter 4 Photoconductivity of Individual Nb2O5 Nanowire task. Rosenfeld et al.8 proposed oxygen vacancies as major contributing factors with respect to the electrical properties of Nb 2 O 5 thin film. They proposed that extrinsic impurities may associate to form complex defects that give rise to oxygen vacancies with trapped electrons. In addition, they argued for the presence of surface electron traps that are associated with chemisorbed oxygen that is able to diffuse into the bulk of the material. These trapped electrons at the oxygen-related surface or defect states could be freed upon laser irradiation and/or laser induced thermal heating of the NW, giving rise to the observed strong photocurrent. The additional increase in photocurrent at vacuum environment could be attributed to heightened thermal effect and desorption of molecular species from the surface of the NW. In the ambient environment, the presence of air helped to dissipate some of the heat generated and suppress desorption at the same time. In vacuum condition, these impeding factors were reduced significantly and as a consequence, additional increase in photocurrent was observed. In the off state, the photocurrent is seen to decay to a level comparable to its dark level under ambient condition and this can be attributable to the absence of photo-excitation, cooling of the NWs and the trapping of charge carriers into various defect states. In the case of experiment carried out in vacuum condition, the tailing of photocurrent in off state did not return to its dark level (Figure 4.7(b)) prior to laser irradiation. Such a difference is indicated by the symbol δ, in Figure 4.7(b). In fact there is an increasing trend of δ with every cycle of laser onoff irradiation. This observation is attributed to the suppression of re-absorption charge trapping molecular species onto the nanowire in the vacuum environment [15-19]. At zero bias, the photocurrent transition is sharp but the magnitude of the photocurrent is ~ 600 times smaller than that observed under biased condition. We attribute this observation to the contribution from the NW-Pt contact. With laser irradiation globally onto the nanowire, it is 45 Chapter 4 Photoconductivity of Individual Nb2O5 Nanowire not straightforward to draw such a deduction from the results shown in Figure 4.7 (a). In fact, such a deduction was arrived at from the results of our studies using focused laser beam. A further detail of the statement is elaborated in Section 4.4.2 where the results for localized laser irradiation are presented. (a)Time characteristic analysis for global irradiation From the basic concepts of photoconductivity, the increase in photocurrent upon laser irradiation is characterized by a time constant associated with the increase in photocurrent towards its steady state (rising time). Likewise, there is a time constant associated with the decrease of photocurrent to its dark current value when the laser irradiation is turned off (decaying time). The simplest rate equation is given by:20 dI (t ) = − I /τ dt (4.1) Thus, equation (4.1) gives I (t ) = I s (1 − e − t /τ ) for the rising curve and I (t ) = I s e − t / τ for the decay curve, where I s = Gτ, G being the photoexcitation rate and τ as the carrier’s lifetime. The experimentally obtained rising and decaying photocurrents were found to fit well within this simple model. The fitted equation takes the following form for the decaying time and rising time respectively:21,22 I (t ) = I o + Ae − (t − t o ) / τ (4.2) I (t ) = I o + A(1 − e − (t − t o ) / τ ) (4.3) Here t o and t are the initial and final response time, τ is the characteristic time constant, related to slow photoresponse process observed. I o is the dark current and A is the current amplitude. The fitted data for both ambient and vacuum was extracted from the response curves (Figure 4.7(b)) 46 Chapter 4 Photoconductivity of Individual Nb2O5 Nanowire in the regime of slowly varying photocurrent. Figure 4.8(a) shows the rising curve, while Figure 4.8(b) shows the decaying curve fitting using data shown in Figure 4.7(b). The simple time characteristic functions (equations (4.1)-(4.3)) provide a good exponential fit to the data. From the analysis, the amplitudes and the characteristic response times at vacuum and ambient conditions are summarized in Table 4.1. Figure 4.8 (a) Rising and (b) Decaying time response analysis (808nm wavelength, power ~ 170mW) at ambient and vacuum conditions (solid lines are the exponential fitted curves). Table 4.1: Time characteristics analysis in vacuum and ambient condition Vacuum condition Ambient condition Response |A| τ (s) |A| τ (s) Rising 2.99 x 10-8 51 1.06 x 10-8 54 Decay 1.84 x 10-6 32 7.64 x 10-7 34 47 Chapter 4 Photoconductivity of Individual Nb2O5 Nanowire The rising and decaying response time obtained from the curve fitting for data obtained under vacuum conditions are ~51 sec and ~32 sec respectively (Table 4.1). Such a slow photoresponse time observed in the Nb 2 O 5 NW consistent with presence of the deep trap states23 associated with oxygen-related surface or defects in the system. Moreover, the difference in time constants indicates that the time taken to free the trapped-charges thermally is longer than that when it actually gets trapped. Similarly, the rising and decaying time constant to photocurrent measured under ambient conditions were ~ 54 sec and ~ 34 sec (Table 4.1). These values are similar to those obtained under vacuum condition and suggest that similar processes took place in ambient conditions. 4.4.2 Photocurrent on individual Nb 2 O 5 NW with focused laser beam In order to gain better insights into the major contributing factors to the photocurrent, we carried out photocurrent measurement with localized focused laser irradiation. The efforts here were to study the photocurrent effect with focussed laser beam (spot size < 1µm) that can be locally directed at specific location such as the NW-Pt interface. Figure 4.9(a) represents the schematic diagram of focused laser beam irradiation on individual NW. The NW device was mounted on a precision movable stage so that focused laser beam can be irradiated along the body of the NW. Figure 4.9(b) shows schematics of localized irradiation on (i) NW-Pt interface at forward bias (high terminal), (ii) middle of the NW and (iii) NW-Pt interface at reverse biased (low terminal). From here on, we shall use the labels “(i)”, “(ii)” and “(iii)” to denote the experimental results obtained from the three different cases as depicted in Figure 4.9(b). Figure 4.9(c) shows the I-V characteristics of individual Nb 2 O 5 NW measured at ambient environment with focused laser beam (diode laser, λ=532nm, power ~80 μW) irradiation for the three 48 Chapter 4 Photoconductivity of Individual Nb2O5 Nanowire different cases at sweeping voltage of -2V to +2V. Figure 4.9(d) represents the photocurrent response at an applied bias of 0.5V corresponding to the three different conditions. Evidently the magnitude of the photocurrent in the case of laser beam irradiated on the NW-Pt interface at low terminal (case (iii)) is higher compared to response at NW-Pt interface at high terminal (case (i)). The photocurrent measured with laser irradiating at the middle of the NW (case (ii)) is comparatively less than the other two cases. The same observation can also be made from the I-V characteristics shown in Figure 4.9(c) for these three cases. The magnitudes of photocurrent increased with the increased in applied bias and the laser power. 49 Chapter 4 Photoconductivity of Individual Nb2O5 Nanowire Figure 4.9 (a) Schematic representation of photocurrent measurements with focused laser beam irradiation on NW. (b) Schematic diagram of focused laser beam locally irradiated on (i) high terminal NW-Pt interface (ii) middle of NW (ii) low terminal NW-Pt interface. (c) I-V characteristics with/without focused laser beam irradiation on NW-Pt contacts at sweeping voltage -2V to +2V. (d) Photoresponse at applied bias 0.5V with laser (λ = 532 nm, power ~80 µW) irradiated on the low terminal NW-Pt contacts, middle of the NW and on the high terminal NW-Pt contacts respectively. Schematic representation of band bending diagram with corresponding electron-hole transfer at Pt-NW interface when laser irradiated at (e) forward and (f) reverse applied bias. 50 Chapter 4 Photoconductivity of Individual Nb2O5 Nanowire The observed properties of the photocurrent at applied bias can be interpreted by considering the NW system as back-to-back Schottky diode model.24 Figures 4.9(e) and 4.9(f) illustrate the mechanism of photocurrent-generation at the NW-Pt interface under an applied external bias. The work function of Pt is slightly higher than that of Nb 2 O 5 . Upon contact, Schottky barrier formed and the barrier height is the difference in metal work function and the electron affinity of the semiconductor. Applying an external bias result in band bending as illustrated in the schematic Figures 4.9(e)-(f). When the laser irradiated was directed near the NW-Pt contact at reverse-biased (Figure 4.9(f)), photogenerated electrons and holes are separated by the strong local electric field. The holes move towards the Pt contact and the photogenerated electrons, experiencing a large barrier height at the contact, diffuse across the NW and followed by collection at the forward-biased contact. On the other hand, when the laser was irradiated near Pt-NW interface at forward bias contacts (Figure 4.9(e)), the photogenerated electrons are readily collected and the photogenerated holes diffuse across the NWs and followed by collection at the reverse-biased contact. Thus there is unidirectional current flow at applied biased conditions irrespective to where the focused laser is directed. In addition the NW being ntype semiconductor and possibly due to asymmetry in the construction of the NW-Pt contact there is excess of electrons flow when laser is irradiated on reversed bias. Moreover, holes may have lower mobility than electrons in Nb 2 O 5 and holes diffusion may lead to greater carrier loss than for electron diffusion. Consequently, higher photocurrent appeared when the laser was focused on the reverse-biased contact. In the case of laser irradiation directed at the middle of NWs (case (ii)), presence of a potential drop maintained by the applied bias resulted in the flow of photogenerated electrons and holes and give rise to the photocurrent. However, more efficient recombination reduced the magnitude of the photocurrent. 51 Chapter 4 Photoconductivity of Individual Nb2O5 Nanowire (a) Time characteristics analysis for focused laser beam Photocurrent time response analysis was carried out for the current response with focused laser beam (λ=532nm) irradiation at the ends of the NW-Pt interface and middle of NW. The time response curve for rising and decaying photocurrent with focused laser irradiation is shown in the Figure 4.10(a) and 4.10(b). Similar to section 4.4.1 (a) analysis was carried out using equations (4.1-4.4). The rising and decaying time response characteristic obtained from the cure fitting are shown in Table 4.2. The time constant τ falls in the range of ~ 4-7 sec on irradiation at the interface of Pt-NW, and the middle of the NW. On the other hand, decay response characteristic in the off state for the three cases was found to be comparably similar (~ 8-9 sec) as shown in Table 4.2, suggesting the recovery mechanism for the NW in the off state is similar. It is noted that the time constants for rising or decay are faster than the global illumination results. The slower tailing in time response in the case of broad beam illumination could possibly be attributed to multiple factors that include carrier diffusion and thermalization across the NW along with Schottky contacts in NW. Figure 4.10 Time response analysis curve (a) rising and (b) decay, when the focused laser (λ= 532 nm) beam irradiated at the forward bias NW-Pt interface, middle of the NW, and at reverse biased NW-Pt contact (solid lines are the fitted curves). 52 Chapter 4 Photoconductivity of Individual Nb2O5 Nanowire Table 4.2: Rising time and decay characteristics with localized irradiation LT Pt-NW interface Response Rising Decay |A| Middle of NW |A| τ(s) -6 1.07 x10 1.53 x 10-5 ~7 ~9 -7 3.22 x 10 9.97 x 10-5 HR Pt-NW interface τ(s) |A| τ(s) ~6 ~7 1.23 x 10-5 5.18 x 10-5 ~4 ~8 (b) Zero bias photocurrent with focused laser beam When the photocurrent experiments were repeated with zero applied bias, surprising results were observed. Figure 4.11(a) shows the photocurrent response measured at zero bias with varying laser power when the focused laser was irradiated at different regions of the NW (see Figure 4.9(b)). The wavelength of the laser beam is 532 nm and the laser powers studied are 125 µW, 260 µW and 324 µW respectively. Similar to the experiment conducted with applied bias, the focused laser beam was locally directed on the NW-Pt interfaces and middle of the NW for photocurrent measurements. It is observed that the photocurrent responses exhibited opposite trend to each other when the laser beam was focused at two different ends of NW-Pt junctions (Figure 4.11(a)). No photocurrent was observed when the focused laser beam was directed at the middle of the NW. It should be noted that the behaviour of the photocurrent obtained at zero bias is in contrast to the trend observed at applied bias (Figure 4.9(d)). In addition, the magnitude of the photocurrent under zero bias is much smaller than the photocurrent observed under biased condition. It is also interesting to note that similar result has been reported before for Si NW using scanning photocurrent measurement setup by Ahn et. al.25 The interesting behaviour of the photocurrent at zero bias can be explained by the process as illustrated in Figure 4.11(b). The Figure 11.4(b) illustrates the flow of electron direction in the Pt-NW interface with corresponding laser irradiation. 53 Chapter 4 Photoconductivity of Individual Nb2O5 Nanowire Figure 4.11 (a) Photoresponse at zero bias with varying laser power (λ = 532 nm, 125 µW, 260 µW and 324 µW respectively) when focused laser irradiated on the low terminal NW-Pt contacts, middle of NW and the high NW-Pt contact. (b) Schematic representation of band diagram with corresponding electron-hole transfer at two ends of the Pt-NW due to localized heating, resulting photocurrent due to thermoelectric effect with focused laser beam irradiated at the Pt-NW interface at zero bias. The increase in photogenerated charge carriers density upon irradiation can modify the barrier width and resulting in a narrow Schottky barrier. This may facilitates an increase in the tunnelling of photogenerated electrons from NW to Pt through the modified Schottky barrier. In addition, the localized thermal heating within the focused laser irradiated region resulted in 54 Chapter 4 Photoconductivity of Individual Nb2O5 Nanowire thermoelectric effects at the NW-Pt interface.26 This gives rise to a temperature gradient between the NW-Pt contacts. The thermalization increased the energy of the electrons in NW, which gained greater velocities than those in metal (Pt) contact region. Consequently this resulted in a net increase in diffusion of electrons from NW to metal electrode at the NW-Pt junction. Both processes would result in a net increase in the flow charge carriers during localised laser irradiation. As the flow of electron are opposite in direction at two different ends of the NW, the observed flow of photocurrent is opposite in direction. When the laser was irradiated on the middle NW, electrons need to diffuse across the length of NW to travel near to the NW-Pt contact region. At zero bias, not all electrons are energetic enough to travel this distance and results in lost due to recombination and scattering along the NW before reaching the NW-Pt interface. Thus the photo-response with laser irradiated on the middle of NW was found to be negligible compared to that on the NW-Pt junctions. Notably there was a clear difference in the magnitude of the opposing photocurrents. This was attributed to physical differences between the two NW-Pt contacts (contact area, thickness of Pt etc) and difference in the relative position of the laser spot to the NW-Pt contact during the measurement. 55 Chapter 4 Photoconductivity of Individual Nb2O5 Nanowire Figure 4.12 Photoresponse at zero bias when focused laser (48 mW, λ = 808 nm) irradiated on the low terminal NW-Pt contacts, middle of NW and the high terminal NW-Pt contacts. Figure 4.12 shows the photoresponse at zero bias with a different laser source (λ=808nm, power = 48 mW), when at the interface and middle of NW. The photoresponse is similar to that obtained with laser irradiation (λ=532nm in Figure 4.11(a)). However the magnitude of the photocurrent is smaller and this is attributed to the laser being less energetic. The photo-response on irradiation at the middle body of the NW at zero bias (λ=808 nm) is not negligible. This could possibly due to the fact that the position of the probing laser irradiation was not exactly at the middle of the NW, but slightly shifted towards negatively bias region from the middle of NW, resulting in slight photo-response. Similar result has been reported before for CdS NW using near-field scanning optical microscope (NSOM) techniques by Lauhon et al.15 At this point it is worthwhile to relate the results shown in Figure 4.12 with the results shown in Figure 4.7(a). i.e. Comparison of the photocurrent of global and localized irradiation in ambient condition and at 56 Chapter 4 Photoconductivity of Individual Nb2O5 Nanowire zero biased. Combining the opposing photocurrent in Figure 4.12, we would obtain a “net” positive photocurrent with a magnitude of tens of pA, this is very similar to the photocurrent for global irradiation shown in Figure 4.7(a). Hence we argue that in the case of Figure 4.7 (a), despite the fact that we have used a broad laser beam illumination, the contribution to photocurrent was largely due to the photoresponse of the NW-Pt contacts. Thus, both with global and localized laser beam irradiation on individual Nb 2 O 5 NWs, the results tested for about 8-10 NWs showed to be consistent. All of the above results with global and localized irradiation photocurrent response on Nb 2 O 5 were carefully taken with same NW, so that we could analyse the results qualitatively. At the end, we would like to display in Figure 4.13, the photocurrent response extracted with other Nb 2 O 5 NW devices under global and localized irradiation of laser beam at applied and zero bias conditions to show the consistency in our results. However, the magnitudes of the photocurrent response depend on the laser power, length of the NWs, contacts, etc. The uneven response of photocurrent at zero bias on irradiation at the middle of the NW (Figure 4.13(d)) is possibly due to uneven distribution of contact area, including that the laser not irradiating exactly at middle of the NW. 57 Chapter 4 Photoconductivity of Individual Nb2O5 Nanowire Figure 4.13 Photocurrent responses with global irradiation on Nb2O5 NW with (a) 808 nm laser (power ~ 50 mW) (b) 1064 nm (power ~108 mW) under ambient condition with applied bias voltage of 3V. (c) and (d) represents photocurrent responses from Nb2O5 NW with localized laser beam irradiation (λ=1064 nm) at applied bias 0.1V (laser power ~ 120 µW) and at zero bias (laser power ~ 160 µW) respectively. 4.5 Conclusion We have studied the photoconductivity of individual Nb 2 O 5 NW devices with Pt contact electrodes through global and localized laser irradiation. The photocurrent response was found to be sensitive to the adsorbed ambient molecules as a larger photocurrent was generated in vacuum 58 Chapter 4 Photoconductivity of Individual Nb2O5 Nanowire than in air. The photocurrent also shows different time characteristics with rapid and slow varying components arising from defect level excitations, thermal heating effect, surface states and NW-Pt contacts. Results from localized irradiation, revealed that the measured photocurrent of single NW device (with and without applied bias) depended sensitively on the photoresponse at the NW-Pt contacts. At applied bias, unidirectional photocurrent was observed and higher photocurrent was achieved with localized laser irradiation at reverse biased NW-Pt contact. At zero bias, opposite polarity of photocurrents were detected. We attributed this behaviour to the presence of a reduced Schottky barrier/width resulting from an increase in charge carriers generated by laser irradiation and also thermoelectric electric effects arising from the localized thermal heating. Comparison of photocurrents generated upon global and localized irradiation showed that the main contribution to photocurrent was largely due to the photoresponse of the NW-Pt contacts. References 1 H. Schäfer, R. Gruhn, F. Schulter, Angew. Chem. (1966)78, 28 2 H. Schäfer, A. Durkop, M. Jori, Z. Anorg. Allg. Chem. (1954) 275, 289 3 J. M Jehng, I.E Wachs, Chem. Mater. (1991) 3, 100 4 N Özer, D. G. Chen, C. M. Lampert, Thin Solid Films (1996) 177, 162 5 P. George, V. G. Pol, A. Gedanken, Nanoscale Res. Lett. (2007) 2, 17 6 M. Mozetic, U. Cvelbar, M. K. Sunkara, S. Vaddiraju, Adv. Mater (2005) 17, 2138 7 B. Varghese, C. H. Sow, C. T. Lim, J. Phys. Chem. C (2008) 112, 10008 8 D. Rosenfeld, P.E. Schmid, S. Széles, F. Lévy, V. Demarne et. al, Sens. Actua. B (1996) 37, 83 9 U. Cvelbar, K. Ostrikov, A. Drenik, and M. Mozetic, Appl. Phys. Lett. (2008) 92, 133505 59 Chapter 4 Photoconductivity of Individual Nb2O5 Nanowire 10 N. Özer, Din-Guo Chen, Carl M. Lampert, Thin Solid Films (1996) 277, 162 11 K. Taanabe, Catal. Today (2003) 78, 65 12 B. Varghese, Y. Zhang, Y. P. Feng, C. T. Lim, C. H. Sow, Phy. Rev. B (2009) 7,9115419 13 A. A. McConnel, J. S. Anderson, C. N. R. Rao, Specteochimica. Acta. A (1976) 32, 1067 14 Y. Gu, E. S kwak, T. W Odom, L. J. Lauhon, Appl. Phys. Lett. (2005) 87, 043111 15 C. Scoi, A. Ahang, B. Xiang, S. A. Dayeh, D. P. R. Aplin, J. Park, X. Y. Bao, Y. H. Lo, D. Wang, Nano Lett. (2007) 7, 1003 16 A. Bera, D. Basak, Appl. Phys. Lett. (2009) 94, 163119 17 Y. Xie, F. C. Cheong, B. Varghese, Y. W. Zhu, R. Mahendiran, C. H. Sow, Sensors Actuators B (2010) 115, 320 18 S. Hullavarad, N. Hullavarad, Nanoscale Res. Lett. (2009) 4, 1421 19 L. Ping, J. L. Zhai, D. J. Wang, P. Wang, Y. Zhang, S. Pang, T. F. Xie, Chem. Phys. Lett. (2008) 156, 231 20 Richard H. Bube, photoelectronic properties of semiconductor, Cambridge University press (1992) 21 C. Soci, A. Zhang, X. Y. Bao, H. Kim, Y. Lo, D. Wang, J. Nano Science and Nanotechnology (2010) 10, 1 22 A. Bera, D. Basak, Appl. Phys. Lett. (2008) 93, 053102 23 J. A. Hornbeck, J. R. Haynes, Phys. Rev. (1955) 97, 311 24 Y. Gu, E. S. kwak, T. W. Odom, L. J. Lauhon, Appl. Phys. Lett. (2005) 87, 043111 25 Y. Ahn, J. Dunning, J. Park, Nano Lett. (2005) 5, 1367 26 B. Varghese, R. Tamang, E. S. Tok , S. G. Mhaisalkar, C. H. Sow, J. Phys. Chem. C. (2010) 114, 15149 60 Chapter 5 Photoconductivity of Individual V2O5 Nanowire Chapter 5 Photoconductivity of Individual V 2O 5 Nanowire 5.1 Introduction In the past decade, several methods have been used to prepare V 2 O 5 nanostructures such as; nanowires, nanoribbons, nanosheets, and nanotubes. These techniques include hydrothermal syntheses, sol-gel techniques, electrodeposition, and vapour transport. Recently, Vanadium oxide NWs have been intensively studied for use as lithium-ion batteries, electrochromic devices, gas sensors, and also have found application in the photographic industry as antistatic coatings.1-7 V 2 O 5 in simple orthorhombic crystalline structure comprises layers of square pyramids sharing edges and corners. These layers are weakly bound by electrostatic forces along the caxis, as indicated by the long V-O distance of 0.279 nm,8 which provides abundant sites for the facile intercalation of various guest species. The layered structure and mixed valance of vanadium (V5+ and V4) in V 2 O 5 makes this material an attractive candidate for electrochemical energy storage via the intercalation and de-intercalation of Li-ions.4,6,9 Probing the intrinsic properties of nanostructures is critical to assess their possible role and functionality nanoscale devices. In this regard CNT and ZnO have been investigated in great detail.10-14 Thus there is a need to explore the potential of other nanostructure materials for better device performance. This chapter details the systematic study of electrical transport and photocurrent measurements of V 2 O 5 individual NWs, with the aim for better understanding of these NWs for their applicability in nano-devices, such as optoelectronics and photodetectors. 61 Chapter 5 Photoconductivity of Individual V 2O5 Nanowire 5.2 Experimental Section Vanadium metal foil (99.98%) purchased from Sigma-Aldrich was cleaned, dried and mounted on a hotplate and on top of it a SiN substrate (with grid pattern) was placed. The hotplate was set to temperature ~ 540oC for 3 days for the growth of V 2 O 5 nanostructures (NWs) in an ambient environment.15 Hotplate technique for the growth of V 2 O 5 nanostructures is detailed in Section 3.1.3. Figure 5.1 shows the SEM image of the V 2 O 5 nanowires grown on SiN substrate. The nanowires ranged the length of ~ 10-30 μm, with diameter ~ 50-150 nm. Figures 5.1(b) and (c) show the V 2 O 5 NWs grown at the edge of the substrate, with one end anchored to the growth substrate. Figure 5.1 SEM images of V2O5 nanowires on (a) SiN substrate, (b) and (c) are images of suspended V2O5 nanowire on the edge of the SiN substrate. 62 Chapter 5 Photoconductivity of Individual V 2O5 Nanowire Figure 5.2 shows the micro-Raman spectrum collected from the V 2 O 5 nanostructures sample. The micro-Raman spectrum of the V 2 O 5 nanowires grown on SiN by placing Vanadium metal foil on top of it at temperature 540oC, were collected in back scattering configuration at room temperature. The Renishaw system2000 micro-Raman system used a diode laser that emits laser beam with a wavelength of 514 nm that was focused by a 50x objective lens. The Raman peaks are located at 213, 373, 621, 838, 896 and 952 cm-1 as shown in Figure 5.2. Among all peaks, peak at 952 cm-1 corresponds to stretching mode of V-O group, the peaks at 213 and 373 cm-1 are caused by V-O bending vibration. The peaks at about 621, 838 and 896 cm-1 are attributed to the streaching modes of V 2 -O and V 3 -O. All of these peaks were observed from 896 838 621 373 213 Intensity (a. u) 952 vapor-deposited V 2 O 5 films and NWs, but with shifts.16-18 200 400 600 800 1000 Raman shift (cm-1) Figure 5.2 Raman spectrums of V2O5 nanowires. 63 Chapter 5 Photoconductivity of Individual V 2O5 Nanowire 5.3 V 2 O 5 nano-device fabrication The single V 2 O 5 NW devices were fabricated by transferring individual NW from the growth substrate (SiN) to the patterned Au electrodes SiO 2 /Si substrate, with the aid of tungsten needle probes (tip size ~75 nm) attached to a micro-positioner under an optical microscope (CascadeTM Microtech). The NW was first electrostatically attached to the tungsten probes by direct contact from the growth substrate, and then transferred to the SiO 2 /Si substrate by exploiting Van der Waals force between the substrate and the NW. The ends of these NW were then electrically connected to the Au electrodes by depositing Pt (300nm in thickness) using a dual beam focused ion beam system. Figure 5.3 shows the SEM image of an individual V 2 O 5 NW (length ~15 µm, diameter ~100 nm) device fabricated. Figure 5.3 SEM image of individual V2O5 NW, NW ends are connected to the Au finger electrodes on Si/SiO2 substrate with Pt deposition. 64 Chapter 5 Photoconductivity of Individual V 2O5 Nanowire 5.4 Electrical characterization and photoconductivity of individual V 2 O 5 NW The electrical transport measurements were performed in an individual V 2 O 5 nanowire device fabricated (Figure 5.3) in two-point probe configuration, using Keithley 6430 current source meter. Figure 5.4(a) represents the schematic diagram of the experimental setup with nano-device inside. The nano-device was electrically connected to the leads inside the vacuum chamber. This leads were then externally connected to the current source meter unit (Figure 5.4(a)). Notably, the chamber comprises of a transparent window. The device was placed in its face up position at the middle of the visible transparent window of the vacuum chamber. The laser was irradiated on the sample through this transparent glass window. The I-V response with laser irradiation was studied with continuous laser irradiation, while the time dependent photoresponse were recorded with blockage of laser (on/off state) at equal time interval. All the measurements were performed with same experimental setup. Figure 5.4(b) shows the typical I-V characteristics of individual V 2 O 5 NW measured at ambient and room temperature with sweeping voltage from -4V to +4V. Figure 5.4(c) shows the I-V measured as dark current and on illumination of laser (808 nm-200 mW EOIN, diode laser) at ambient environment. Figure 5.4(d) shows the I-V characteristics when laser was irradiated at different pressure (ambient, ~5 x 10-3 torr, and ~5 x 10-5 torr). The current response increased in high vacuum. 65 Chapter 5 Photoconductivity of Individual V 2O5 Nanowire Figure 5.4 (a) Schematic diagram of experimental setup used for the study of photoresponse of V2O5 NW. (b) I-V curve of V2O5 NW at ambient. (c) I-V curves with/without light illumination at ambient. (d) I-V curves with light illumination at ambient and at different vacuum condition. Figure 5.5(a) represents the varying dependent I-V curves of V 2 O 5 NWs upon laser irradiation (λ=808nm) at vacuum condition (~5 x 10-5torr). All the electrical transport measurements were performed at room temperature. Thus Figure 5.4(b)-(d) and Figure 5.5(a) shows that the individual V 2 O 5 nanowire device exhibited nonlinear and almost symmetric I-V 66 Chapter 5 Photoconductivity of Individual V 2O5 Nanowire characteristics at various sweeping voltage. The dark current measured was as low as 2.5 nA (Figure 5.4(c)) at biasing voltage -1.5V to +1.5V. It is well established that a Schottky barrier is formed at the metal-semiconductor (M-S) interface, and Schottky barrier plays a crucial role in the electrical transport in the M-S-M structure including semiconducting nanowires. The nonlinearity in I-V characteristics could be due to Schottky barrier formation between the nanowire and the metal electrodes (Pt) in nanowire devices. Platinum (Pt) is a high work function material and a Schottky contact forms when Pt connected with most semiconductor materials unless Pt is doped to reduce its work function value.19-21 Figure 5.5(b) show that the photocurrent versus laser power at a bias voltage of 1.5V, varies almost lineary. Figure 5.5 (a) I-V results of individual V2O5 NW measured at vacuum (~5 x 10-5 Torr) irradiated by different laser (λ=808) power. (b) Experimental and fitted plot of laser (λ = 808 nm) power vs photocurrent at fixed applied bias of 1.5V. 67 Chapter 5 Photoconductivity of Individual V 2O5 Nanowire At very low bias, the current passing through the NW is very small and the total voltage is distributed mainly on the two Schottky barriers. On the other hand, at large bias, the contribution from the two Schottky barriers become less significant and the potential drop is mainly contributed by the potential difference across the NW. Thus at the region of larger bias regime, the resistance of the NW can be obtained on differentiated I-V characteristics (R ≈ ∆V/∆I). Thus, the resistance of the NW obtained was R=130 MΩ for Figure 5.4(b). Other parameters can also be extracted from the I-V curves in the intermediate bias regime where the reverse-biased Schottky barrier dominated the total current I 19,20 1   q  + ln J s ln I = ln(SJ ) + V  −  kT Eo   qE  Eo = Eoo coth oo   kT   N  Eoo =  * d  2  mnε sε o  1 (5.1) (5.2) 2 (5.3) Where J is the current density through the Schottky barrier, S is the contact area associated with the barrier. E o depends on the carriers density corresponding to E oo , and J s is a slowly varying function of the applied bias. Thus, logarithmic plot of the current I as a function of the bias voltage V gives approximately a straight line of slope q/(kT) – 1/E o , and the plot is shown in Figure 5.6. From this plot, the electronic concentration n can then be obtained via E o and the electron mobility can be calculated using the relation µ=1/(nqρ), with ρ (ρ=RA/L) being the resistivity of the NW. Thus, applying the procedure to I-V curve in Figure 5.4(b), plot of In(I) versus the bias voltage at higher regime is shown in the Figure 5.6. From the linear fitting we get slope = 0.814, from which we can extract E o =26.43 mV, and further calculation applying equations (5.2) and (5.3) and taking the ε o =3.389 as reported for the thin film,22 gives N d =n ≈ 68 Chapter 5 Photoconductivity of Individual V 2O5 Nanowire 1.7 x 1017 /cm3. For NW in Figure 5.2 with diameter ≈110 nm and length ( L) ≈15 µm, the resistivity ρ ≈8.23 Ω cm, and thus putting these values in equation, we get mobility µ=4.47 cm2/V s. Figure 5.6 Experimental and fitted ln(I) vs V plot for V2O5 on linear regime of I-V curve shown in Figure 5.4 (b) The current increased slightly on illumination of laser (λ=808nm) because of the photon generated excess carriers due to excitation from defect level states (Figure 5.4(c)). The photocurrent measurement at vacuum showed significant increase in current compared to that in an ambient environment, attributable to desorption of oxygen/water at surface of NW or enhanced thermal effect in vacuum condition (Figure 5.4(d)). Photon generated increased on increasing the laser power, leading to increase in photocurrent (Figure 5.5(a)). Transport 69 Chapter 5 Photoconductivity of Individual V 2O5 Nanowire mechanism in V 2 O 5 NW involves contribution from thermal effects. This can be seen from the power dependent transport measurements curves indicated in Figure 5.5(a). V 2 O 5 is an n-type semiconductor material. Nano-device on exposure to air, there is a strong possibility of water molecules and oxygen becoming trapped on the surface of the nanowire. The oxygen molecules that are chemisorbed can capture electrons while water molecules from the atmosphere can be physisorbed followed by chemisorbed onto the surface of the nanowire. When the laser was irradiated onto the NWs, the originally adsorbed negatively charged oxygen ions combined with the holes generated from the optical absorption and subsequently desorbed, reducing the electron depletion layer thickness to increase the electron flow channel width, resulting increase in overall photoresponse.23 The photoresponse recorded under different environmental conditions on V 2 O 5 NWdevice at a fixed biased at 0.5V are shown in Figure 5.7. In these cases, the NW was illuminated by the laser beam at a regular interval of about 240 seconds. At an ambient condition, there was only a small (~pA) photoresponse to on/off state of laser. However under vacuum conditions (~8.3 x 10-3 torr and ~4.2 x 10-4 torr), the photocurrent is significantly enhanced. Upon illumination of laser beam, large enhancement of ~ 415% ( (∆I Vacuum − ∆I Ambient ) ∆I Ambient × 100% ) from ambient to vacuum was observed. The current dropped when the laser was blocked (off state). The recovery process is slow and shows an apparent tailing, slightly above the original starting current. The off state tailing, not reaching to the original current value suggests that the laser irradiation under vacuum condition likely to be modified the surface states of NW. The slow response in photocurrent could be attributed to the contribution from thermal effect. Temperature increases due to laser irradiation, which causes resistance R in NW to decrease and thus gives rise to higher current. The change in temperature is more significant in vacuum as 70 Chapter 5 Photoconductivity of Individual V 2O5 Nanowire cooling effect from environmental air is suppressed; i.e the NW becomes even hotter and resulted in more significant change in photocurrent. Figure 5.7 The response curve under laser (λ=808nm, power ~165 mW) at an ambient and vacuum (~8.3 x 10-3Torr, 4.2 x 10-5Torr) environment. The laser power dependent I-V characteristics, and photoresponse at an applied bias of 0.5V were also measured using near-infrared laser (λ=1064 nm) as shown in Figure 5.8 and Figure 5.9. Figure 5.8(b) shows the linear dependent nature of photocurrent with the laser power, at vacuum condition. Notably the higher current on 1064 nm laser irradiation as compared with 808 nm laser, the significance of thermal contribution in transport mechanism. The I-V curves showed non-linear and almost symmetric trend similar to the results obtained with 808 nm laser irradiation. The photocurrent measurements show laser intensity dependent response (Figure 5.9) 71 Chapter 5 Photoconductivity of Individual V 2O5 Nanowire measured at applied bias 0.5V. Thus one of the possible applications of V 2 O 5 NW can be in visible-infrared range photosensing and photodetectors devices. Figure 5.8 Power dependent I-V characteristic curves on irradiation of laser (λ=1064 nm) at vacuum environment (~ 4 x 10-5torr). (b) Experimental and fitted plot of current with respect to dark current versus the laser (1064 nm) power at fixed biased 1.5V. Figure 5.9 Photoresponse of individual V2O5 NW on irradiation of laser (λ=1064 nm, power ~230 mW) measured at applied bias 0.5V (a) in ambient and vacuum (~ 4 72 x 10-5Torr). (b) Power dependent photoresponse at vacuum (~ 4 x 10-5Torr). Chapter 5 Photoconductivity of Individual V 2O5 Nanowire 5.5 Time characteristics analysis From the photoresponse obtained in Figure 5.7 and Figure 5.9(a) for λ=808 nm and λ=1064nm irradiation respectively, the characteristic time associated with the increase in photoconductivity to its steady state value on laser irradiation (rising time) at on-state, and the characteristic time associated with the decrease of photoconductivity to its dark current value when the laser irradiation is at off-state (decay time) can be calculated with fitted exponential curves as shown in Figure 5.10(a)-(d), which very well fits to the exponential curve. The simplest rate equation is a function of current with time given by: And, dI (t ) = − I /τ dt (5.4) I (t ) = I o + Ae − t / τ (5.5) Here t is the response time interval, τ the relaxation time constant associated to the thermal effect. I o is the dark current and A is the current amplitude on response to on/off of laser irradiation. Thus the characteristic time obtained for λ=808 nm irradiation for rising and decay was calculated to be ~ 102 sec and ~ 37 sec (Figure 5.10(a)-(b)). And for λ=1064 nm it was ~ 99 sec and 32 sec respectively (Figure 5.10(c)-(d). Thus the response times are similar in these cases (i.e thermal effect similar). However on irradiation of green laser (λ=532 nm) there was no observation of any photoresponse, which also suggests that the photoresponse due to thermal effects with IR (λ=1064 nm) and near IR (λ=808 nm) laser irradiation. 73 Chapter 5 Photoconductivity of Individual V 2O5 Nanowire Figure 5.10 Experimental and fitted exponential time characteristics curves obtained from Figure 5.7 (λ=808 nm) and Figure 5.9 (λ=1064 nm): (a) Rising time (b) Decay time for λ=808 nm laser irradiation. (c) Rising time (b) Decay time for λ=1064 nm laser irradiation. Finally, It has been observed that the above results of photoresponse in single V 2 O 5 NWs were consistent (such photoresponse with other V 2 O 5 NW device has been displayed in Figure 5.1). However, the photocurrent responses from the NWs also depended on the irradiated laser power, dimension of the NWs, etc. 74 Chapter 5 Photoconductivity of Individual V 2O5 Nanowire Figure 5.11 Photocurrent responses from individual V2O5 NW (different NW device then the above results) on irradiation of 808 nm laser (power ~ 130 mW) at applied bias of 0.5 V. 5.6 Conclusion The photoconductivity of individual V 2 O 5 NW device with global laser irradiation was studied systematically. The I-V characteristics on different laser power showed a linear photocurrent response. This increase in photoresponse with laser power suggests the significant attribution of thermal effects. The Schottky effects near contact electrodes-NW junction also contribute to photoresponse of V 2 O 5 NW. The photocurrent measurements at ambient and vacuum are very significantly different. The thermal heating of NW is significant in vacuum as the cooling effect from air is reduced. The photoresponse of V 2 O 5 NW at ambient with λ=808 nm irradiation was ~ 1nA and with λ=1064 nm irradiation was ~ 0.8nA. At applied bias 0.5V the photoresponse showed more responsive to red laser (λ=808 nm) compared to infrared (λ=1064 75 Chapter 5 Photoconductivity of Individual V 2O5 Nanowire nm) under vacuum environment. This could be because of higher energy of red laser compared to infrared. The photocurrent is sensitive to the intensity of laser. Thus, this study of photoresponse in individual V 2 O 5 NW could enrich the study of one-dimensional metal-oxide NWs, with its potential applications in nano-optoelectronics, photodetectors and next generation NW based electronic devices. The localized laser beam experiment for photocurrent measurements could not be performed on V 2 O 5 NW owing to some technical difficulties: The focused laser beam set-up for our experiments has a very short working distance (~2-5 mm), which means that the sample/device should be very close to the microscope objective lens. Thus at this situation the measurements can be performed only in an ambient condition presently. And the V 2 O 5 NWs showed no much significant photoresponse in ambient condition, it was anticipated that no response could be seen with focused laser beam too at ambient. Due to these difficulties as mentioned above, the contribution of photocurrent from Pt-NW junction could not be extracted; however we would like to develop our experimental setup for localized photocurrent for future studies. 76 Chapter 5 Photoconductivity of Individual V 2O5 Nanowire References: 1 F. Zhou, X. Zhao, C. Yuan, L. Li, Crystal Growth & Design, (2008) 8, 723 2 C. Xiong, A. E. Aliev, B. 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(2009) 94, 023110 78 Chapter 6 Conclusions and Future Works Chapter 6 Conclusions and Future Work The one-dimensional nanostructures (nanowires) were synthesized using tube furnace and hotplate techniques. Nb 2 O 5 and V 2 O 5 NWs were fabricated using these techniques. These nanostructures were characterized using XRD, SEM and micro-Raman as characterizing tool. Following which photoconductivity studies were carried out on these nanostructures. The single NW devices were fabricated by transferring individual NW from the growth substrates to the SiO 2 /Si substrates with pre-patterned Au electrodes of ~10 µm gap. These electrodes were fabricated using standard photolithographic technique. With the aid of tungsten needle probes (tip size ~75 nm) attached to a micropositioner under an optical microscope (CascadeTM Microtech), the NW was first attached to the tungsten probes by direct contact, and then transferred to the SiO 2 /Si substrate by exploiting the Van der Waals force between the substrate and the NW. The ends of these NW were then electrically connected to the Au electrodes by depositing Pt (300nm in thickness) using a dual beam focused ion beam system (Quanta 200-3D FIB-SEM, FEI Company, Ga+ ion beam operated at 30 kV, 50 pA). The systematic studies of photocurrent of these nano-devices were conducted under different environmental conditions upon irradiation of green (λ=532 nm), near-infrared (λ = 808) nm and infrared (λ=1064 nm) laser beam. Global laser irradiation on the isolated Nb 2 O 5 and V 2 O 5 NWs showed multiple photocurrent contribution from defect level excitations, surface states and thermal heating effect. In another approach of photoconductivity study, the focused laser beam techniques with spot size < 1 µm was used on individual Nb 2 O 5 NW. This technique 79 Chapter 6 Conclusions and Future Works ensured local probing along the desired section of NW and to develop better insight into the photoresponse of the NW and at the Pt-NW interface region. The fast and prominent photocurrent response from Nb 2 O 5 NW towards visible and Infar-red wavelengths with focused laser beam was demonstrated. The individual Nb 2 O 5 showed distinct photoresponse when the laser was irradiated globally and locally, especially at the PtNW interface on local irradiation. The photocurrent measurements on Nb 2 O 5 NW with focused beam revealed the predominant contribution from the Pt-NW contacts, when the device was operated both under a bias as well as at zero bias conditions. The polarity of the photocurrent generated at zero bias near Nb 2 O 5 Pt-NW interface suggests Schottky barrier and thermoelectric effects playing significant role in the carrier transport mechanism on irradiation of laser. Hence we suggest the Schottky barrier response and thermoelectric effect as the key for transport mechanism resulting to photocurrent response at zero bias. While at applied bias, the photocurrent response was unidirectional when the focused laser beam irradiated onto different segments (two ends of Pt-NW interface and middle of the NW) of NW. Most significant photocurrent was observed when laser irradiated at reversed bias contact. Global irradiation showed photoresponse ~ 41% at vacuum compared to an ambient in Nb 2 O 5 NW. The time characteristic analysis showed slow rising time and fast decay time, and significant response with focused laser beam irradiation. The I-V characteristics on varying laser power showed increased in the photocurrent response from V 2 O 5 NW. This increased current-response is attributed to thermal effects. The Schottky barrier effects and contact electrodes also contributes to transport properties in V 2 O 5 NW. The thermal heating of NW was significant in vacuum as the cooling effect from air is reduced. The photoresponse of V 2 O 5 NW at ambient upon irradiation of laser (λ=808 nm and 80 Chapter 6 Conclusions and Future Works λ=1064 nm) was ~1nA. At applied bias of 0.5V the photoresponse measured showed significant responsive to red laser (λ=808 nm) compared to infrared (λ=1064 nm) under vacuum environment. This is because of higher band energy of red laser compared to infrared. The observed photocurrent was sensitive to the laser intensity. The localized laser beam technique for photocurrent measurements could not be implemented on V 2 O 5 NW owing to some technical difficulties: The focused laser beam setup developed in our laboratory has a very short working distance (~ 2-5 mm). Therefore the nanodevice for photocurrent measurement should be kept very close to the microscope objective lens. This presented restriction in vacuum photocurrent measurements using focused laser beam irradiation. And as the V 2 O 5 NW showed no significant photoresponse in ambient condition, it was anticipated that no response could be seen with focused laser beam too at ambient. Thus at present situation one of the main challenge is to develop the focused laser beam technique for vacuum measurements. For the experiments conducted in vacuum, many additional experiments can be carried out. These include refilling the vacuum chamber with specific gaseous species to investigate the effect of different gaseous species on the photoconductivity of the NWs. So far all the experiments presented in this work were carried out at room temperature. It would be worthwhile to conduct future experiments with the NW devices placed on a heating stage. In this way, we could investigate the temperature dependence of the individual NWs. Certainly a combination of the environmental control as well as temperature control will be an interesting area of investigation to be conducted in the future. Our focus in this work can also be extended to other type of metal electrodes such as Au, Al and etc. Since each of these metals has different workfunctions, the behavior of the NW-metal contact would be different. 81 Chapter 6 Conclusions and Future Works Henceforth, with better understanding in device physics extracted specially from the metal-nanowire interface region of the device using focused laser beam technique, our approach presented on photocurrent in individual metal-oxide nanowire could have better implication in photodetectors, nano-optoelectronics, and next generation NW based electronic devices. 82 [...]... Chapter 2 Photoconductivity in one- dimensional nanostructures 2.2 Concepts in photoconductivity Photoconductivity is an important property of semiconductors in which the electrical conductivity changes on irradiation of incident light Photoconductivity phenomena can be mainly described with electron activity in semiconductors Photoconductivity involves the following mechanisms: absorption of the incident... potentials controlling the sensitivity selectively Considering the photocurrent measurement in single nanowires in our present work, it was our interest to see the possible mechanism and main contributing factors to photoresponse of metal oxide nanowires The localized photocurrent measurements could provide insight into the photoresponse of NWs, including in the region of interface 1.3 Brief outline of the... trappingdetrapping mechanism and recombination process.11-15 In addition change in large surface-tovolume ratio in nanostructures, its electrical transport properties strongly influenced by the surrounding environment and not dependent only on the intrinsic properties of the nanowire material In addition, the nature of NW -metal electrode interface also sensitively contributes to the individual NW photoconductivity. .. the nearest energy band before recombination The imperfection or defect state is referred to as trap, and the capture and release processes are called trapping and de-trapping.7-9 Figure 2.1 Schematic diagram showing intrinsic and extrinsic phenomena involved in photoconductivity 9 Chapter 2 Photoconductivity in one- dimensional nanostructures Photoelectric phenomena involves, the concepts of optical absorption... properties.34 Due to high surface-to-volume ratio in one dimensional nanostructure materials, study of interfacial properties is vital for photoconductivity in NWs.35, 36 13 Chapter 2 Photoconductivity in one- dimensional nanostructures From the literature, the photoconductivity in ZnO NWs is mainly attributed to surface states.37-39 The photoconductivity in NWs is highly dependent on surface absorbed... its photoconductivity has been explained in terms of hopping-mediated transport.33 2.4 Factors contributing to photoresponse in one- dimensional metal- oxide nanowires 2.4.1 Surface effects In one- dimension nanostructures, it is possible that the surface approaches the bulk, and the defects segregate on the surface leaving a high quality bulk devoid of defects, thereby producing large difference in properties.34... lie in the development of NW optoelectronic, and sensing devices with better performance control, knowing the role of contact contribution in NW devices In this chapter motivation and brief outline of the present work is presented In chapter 2 brief reviews on photoconductivity concepts, photoconductivity in one- dimensional nanostructures (nanowires) and some of the mechanism involved for photorespone... enhancement, and internal photoconductivity gain, could be utilized for the realization of efficient and highly integrated optical, electronic and sensing devices.1-6 In this chapter some of the basic concepts of photoconductivity of metal- oxide NW are reviewed, highlighting some of the mechanism involved in photoconductivity of NWs, such as surface effect and contacts effects which are crucial in low dimensional. .. Chapter 2 Photoconductivity in one- dimensional nanostructures Due to large surface to volume ratio, NWs contains extremely high density of surface states Thus the surface potential and Fermi energy pinning at the surface strongly depends on the geometry of the NWs These factors strongly influence the performance of NWs as photodectector devices.16 2.3 Photoconductivity in one- dimensional metal- oxide... one can direct the laser beam towards the NW-electrode interface or the main body of the NW and thus develop a better insight into the photoresponse of the NW3, 54, 55 Photoconductivity in single NWs could also be affected by thermoelectric effect, a subjective of our investigation in this work 17 Chapter 2 Photoconductivity in one- dimensional nanostructures References: 1 Y Li, F Qian, J Xiang, C M ... Concepts in Photoconductivity 2.2.1 Steady-state Photoconductivity 2.3 Photoconductivity in one- dimensional metal- oxide nanowires 11 12 2.4 Factors contributing to photoresponse in one- dimensional metal- oxide... (2006) 24, 2172 Chapter Photoconductivity in one- dimensional nanostructures Chapter Photoconductivity in one- dimensional nanostructure 2.1 Introduction With extensive research in the synthesis techniques... Figure 2.1 Schematic diagram showing intrinsic and extrinsic phenomena involved in photoconductivity Figure 2.2 schematic diagrams representing (a) metal- nanowire -metal contact nano device structure

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