(Luận án tiến sĩ) nghiên cứu áp dụng một số phương pháp hạt nhân nguyên tử trong phân tích vật liệu tio2 sio2 sử dụng chùm ion từ máy gia tốc

BỘ GIÁO DỤC VÀ ĐÀO TẠO VIỆN HÀN LÂM KHOA HỌC VÀ CÔNG NGHỆ VIỆT NAM HỌC VIỆN KHOA HỌC VÀ CÔNG NGHỆ - TRẦN VĂN PHÚC NGHIÊN CỨU ÁP DỤNG MỘT SỐ PHƯƠNG PHÁP HẠT NHÂN NGUYÊN TỬ TRONG PHÂN TÍCH VẬT LIỆU TIO2/SIO2 SỬ DỤNG CHÙM ION TỪ MÁY GIA TỐC LUẬN ÁN TIẾN SỸ VẬT LÝ NGUYÊN TỬ VÀ HẠT NHÂN Hà Nội - 2023 luan an MINISTRY OF EDUCATION AND TRAINING VIETNAM ACADEMY OF SCIENCE AND TECHNOLOGY GRADUATE UNIVERSITY OF SCIENCE AND TECHNOLOGY - TRẦN VĂN PHÚC STUDY ON APPLICATION OF THE NUCLEAR METHODS FOR ANALYSIS TIO2/SIO2 MATERIAL USING ACCELERATED ION BEAM ATOMIC PHYSICS DOCTORAL THESIS Hanoi – 2023 luan an MINISTRY OF EDUCATION AND TRAINING VIETNAM ACADEMY OF SCIENCE AND TECHNOLOGY GRADUATE UNIVERSITY OF SCIENCE AND TECHNOLOGY - TRẦN VĂN PHÚC STUDY ON APPLICATION OF THE NUCLEAR METHODS FOR ANALYSIS TIO2/SIO2 MATERIAL USING ACCELERATED ION BEAM Major: Atomic Physics Code: 9440106 ATOMIC PHYSICS DOCTORAL THESIS SUPERVISORS: Prof LÊ HỒNG KHIÊM Dr MIROSŁAW KULIK Hanoi - 2023 luan an TÓM TẮT Luận án nghiên cứu chế trộn lẫn nguyên tử TiO2/SiO2 gây chiếu xạ ion tác động liên quan làm biến đổi tính chất quang tính chất hóa học hệ Các mẫu vật liệu chiếu bốn loại ion khí bao gồm Ne+, Ar+, Kr+ Xe+ bốn mức lượng khác 100, 150, 200, 250 keV Phương pháp tán xạ ngược Rutherford (RBS) sử dụng để xác định biến đổi độ dày cấu trúc lớp TiO2, SiO2 vùng chuyển tiến hai lớp trước sau chiếu xạ Theo đó, hình thành lớp trộn lẫn mô tả mức độ trộn lẫn định lượng Kết cho thấy trình trộn lẫn xảy sở dòng thác nguyên tử chuyển dời sinh mặt phân cách TiO2/SiO2 ion mang lượng Các ion có lượng cao bứt dịch chuyển hạt nhân tới vị trí sâu bề mặt phân cách, nguyên tử nặng tương tác với nhiều nguyên tử vùng trộn lẫn, kết mức độ trộn lẫn tăng tuyến tính theo lượng tăng mạnh theo khối lượng ion Các ion tạo nhiều sai hỏng hay nguyên tử bị dịch chuyển sơ cấp TiO2/SiO2 có độ dày lớp mỏng, cấu trúc có mức độ trộn lẫn vượt trội sau chiếu xạ Những biến đổi số quang lớp TiO2/SiO2 trộn lẫn khảo sát phương pháp quang phổ Elip Chỉ số khúc xạ hệ số tắt lớp trộn lẫn tăng lên mẫu chiếu ion có lượng từ 100 đến 200 keV bắt đầu giảm xuống mức lượng 250 keV Sự biến đổi ảnh hưởng trực tiếp việc thay đổi hàm lượng TiO2 vùng chuyển tiếp gây khác biệt mức độ sai hỏng tạo mức lượng ion khác Ngoài ra, biến đổi hàm lượng hợp chất lớp TiO2 gần bề mặt (gồm Ti, TiO, TiO2, Ti2O3) sau cấy khảo sát theo lượng ion tới phương pháp đo phổ quang điện tử tia X (XPS) Hàm lượng TiO2 tăng hợp chất khác giảm theo lượng ion Đồng thời, mát lượng ion TiO2 giảm theo lượng ion tới (tính tốn SRIM), hay mức lượng tương tác ion vùng phân cách cao hơn, dẫn đến mức độ trộn lẫn lớp TiO2 SiO2 lớn hơn, phù hợp với kết đạt phương pháp RBS luan an ABSTRACT In the present dissertation, ion-beam-induced mixing of TiO2/SiO2 and the related effects resulting in variation of optical and chemical properties of this system have been studied The samples were irradiated by four different noble gas ions Ne+, Ar+, Kr+, and Xe+ at four different energies of 100, 150, 200, and 250 keV Using the Rutherford Backscattering Spectrometry method allows to determine changes in thickness structure of TiO2 and SiO2 layers including transition areas between them before and after implantation Accordingly, the formation of mixed layers has been characterized, and the mixing amount has been quantified It was found that the mixing process occurs on the basis of displacement atoms cascade created in TiO2/SiO2 interface by energetic ions Higher energy ions knock deeper target nuclei while heavier ions interact with much more atoms in a mixed area, as a result, mixing amount increase linearly with ion energy and is strongly enhanced with rising of ion mass It was also found that the ions produced a more significant number of displacement per atom for thinner-layers TiO2/SiO2 leading to greater mixing of this system Alteration of optical constants of TiO2/SiO2 mixed layers were evaluated based on the Ellipsometry Spectroscopy method The refractive index and extinction coefficient of the mixed layers grow for ion energy of 100 to 200 keV, then reduce for energy of 250 keV This effect is associated with variation in TiO2 concentration at mixed areas due to changes amount of created defects In addition, the variation in the chemical composition of implanted TiO2 near-surface layers including Ti, TiO, TiO2, and Ti2O3 was surveyed as a function of ion energy by mean of the X-ray Photoelectron Spectroscopy method Concentration of TiO2 increases with ion energy while the other compounds show the opposite Reducing in energy loss of ion in TiO2 (obtained by SRIM simulation) refer to enhancement of mixing amount that also found by the RBS method luan an ACKNOWLEDGMENTS First and foremost, I would like to express my sincerest thanks to Professor Le Hong Khiem for giving me the opportunity to get into science He was patient, trusted, and encouraged me to overcome the initial difficulties and helped me step by step to complete this thesis These results I want to dedicate as gratitude for his concern and help I would like to deeply thank my supervisor, Dr Miroslaw Kulik, for his thorough guidance, support, his patience, and generosity I have been very happy to work with him who always demonstrates cheerfulness, is never run out of ideas, highly respected my idea, and continuously develops encouragement Thanks for the cakes at lunch times, for the conversations, and I am indebted to him for the success of my Ph.D My thanks also go to my Dear friends and colleagues for the nice working atmosphere, the constructive discussion, especially for the great lunch and coffee breaks I would like to thank Prof Alexander Pavlovich Kobzev, Phan Luong Tuan, Aleksandr Doroshkevic, Afag Madadzada, T.Y Zelenyak, and the technician staff in EG-5 group Frank Laboratory of Neutron Physics, JINR, Dubna I am also grateful to the colleagues I had the honor to work with The numerous collaborations with different characterization techniques, implantation techniques and research fields made my research more interesting and gave me the nice feeling that my work was useful and appreciated In particular, I would like to mention Marcin Turek, Dorota Kołodyńska, and Krzysztof Siemek While studying at the Graduate University of Science and Technology, I gained a lot of knowledge and research experience I want to extend my profound gratitude to all the teachers and administrators who enabled me to accomplish this thesis by teaching, encouraging, and supporting me in every way possible This work was funded by Vingroup Joint Stock Company and supported by the Domestic Master/ Ph.D Scholarship Programme of Vingroup Innovation Foundation (VINIF), Vingroup Big Data Institute (VINBIGDATA), code VINIF.2020.TS.22 Last but not least, I would like to thank my Family for their patience, their entire and unconditional support luan an Dedicated to my Parents! luan an TABLE OF CONTENTS ACKNOWLEDGMENTS TABLE OF CONTENTS LIST OF ABBREVIATIONS LIST OF TABLES LIST OF FIGURES INTRODUCTION 12 CHAPTER 1: THEORETICAL BACKGROUND 16 1.1 Literature review 16 1.2 Concept of ion beam mixing 20 1.3 Atomic collisions in solids 22 1.3.1 Kinematic of elastic collisions 22 1.3.2 Differential cross-section 24 1.3.3 Energy loss process 25 1.4 Low-energy ion modification of solids and IBM process 27 1.4.1 Recoil mixing 29 1.4.2 Cascade mixing 30 CHAPTER 2: THE EXPERIMENTAL METHODS 33 2.2 Ion implantation 34 2.3 SRIM calculation 39 2.4 Rutherford Backscattering Spectrometry (RBS) – an IBA method 41 2.5 Ellipsometry Spectroscopy (ES) method 46 2.5.1 Light & Materials 47 2.5.2 Interaction of Light and Materials 48 2.5.3 Ellipsometry Measurements 50 2.6 X-ray Photoelectron Spectroscopy (XPS) method 53 CHAPTER 3: RESULTS AND DISCUSSION 59 3.1 Influence of ion energy and mass on mixing of TiO2/SiO2 structures with different thickness 59 luan an 3.1.1 Characterization of samples and the mixing process 59 3.1.2 Dependence of mixing degree on energy of incident ions 66 3.1.3 Dependence of mixing degree on mass of the incident ions 74 3.1.4 Study on mixing of TiO2/SiO2 systems with different thicknesses 78 3.2 Influence of the ion energy on chemical composition of TiO2 near surface layers, and its effect to mixing of TiO2/SiO2 systems 83 3.3 The optical property of the TiO2/SiO2 mixed layers obtained by Spectroscopy Ellipsometry 86 3.3.1 Calculation thickness and components of the TiO2/SiO2 mixed layers 87 3.3.2 Variation of refractive index (n) and extinction coefficient (k) with ion energy 90 3.3.3 Variation of optical energy gap (Eg) of TiO2/SiO2 mixed area with ion energy 91 CONCLUSIONS AND FUTURE SCOPE 94 REFERENCES 98 luan an LIST OF ABBREVIATIONS Abbreviations Meaning ARC Antireflection Coating DPA Displacements per Atom EMA Effective Medium Approximation IBA Ion Beam Analysis IBM Ion Beam Mixing JINR Joint Institute for Nuclear Research MAIE Multiple-Angle-of-Incidence Ellipsometry NRA Nuclear Reaction Analysis PKA Primary Knock-on Atom PME Phase Modulation RBS Rutherford Backscattering Spectrometry RAE Rotating Analyzer Ellipsometer RCE Rotating Compensator Ellipsometer RPE Rotating Polarizer Ellipsometer ES Ellipsometry Spectroscopy SRIM Stopping and Range of Ions in Matter TRIM Transport of Ions in Matter MCSU Maria Curie-Skłodowska University XPS X-Ray Photoelectron Spectroscopy luan an 91 composition of the transition layer Fig 3.17 also demonstrates that the virgin sample has the lowest refractive index and extinction coefficient at any given wavelength These values for irradiated samples increase with Xe+ ion energy up to 200 keV before abruptly decreasing at 250 keV The incident Xe+ ions produce atom displacements resulting in enhancement absorption of the TiO2-SiO2 system and change the light propagation in the mixed layers The number of displaced atoms, however, decline for ion energy of 250 keV, which is associated with a drop in the TiO2 component of the mixed layer (see Table 8) This behavior probably explains why the 𝒏 and 𝒌 values suddenly dropped as shown in Fig 3.17 Moreover, the existence of Xe atoms, which remains in the examined system especially in the mixed layer, may have an impact on light absorption Whereas the projected range of 100-keV Xe+ ions is extremely close to the thickness of the TiO2 layer, the projected range of 250-keV Xe+ ions is far beyond the TiO2/SiO2 interface Therefore, the low values of 𝒏 and 𝒌 for 250-keV irradiation, which are nearly the same as those of 100 keV, are probably caused by the absence of Xe atoms in transition layers and a low number of atom displacements 0.6 Virgin E = 100 E = 150 E = 200 E = 250 2.0 extinction coefficient k refractive index n 2.1 1.9 1.8 1.7 1.6 Virgin E = 100 E = 150 E = 200 E = 250 0.5 0.4 0.3 0.2 0.1 a) b) 400 600 800 1000  [nm] 0.0 300 400 500  [nm] 600 700 Fig 3.17 The refractive index 𝑛 (a) and extinction coefficient 𝑘 (b) for the transition layers of un-irradiated and irradiated TiO2/SiO2 systems as a function of wavelength 3.3.3 Variation of optical energy gap (Eg) of TiO2/SiO2 mixed area with ion energy The optical absorption can be considered as an effective approach for acquiring information about the structure and bandgap The absorption coefficient, which indicates the amount of light that a medium absorbs, is defined by the fraction of incident radiation luan an 92 absorbed per thickness of the absorber [105] From the extinction coefficient 𝑘 and wavelength , the absorption coefficient of thin films can be determined by: 4𝜋𝑘 𝛼=  (3.15) The relationship between absorption coefficient 𝛼 and the photon energy can be expressed by 𝐾(ℎ − 𝐸𝑔 )𝑚 (3.16) 𝛼= , ℎ where 𝐾 is a constant which inversely proportional to amorphicity, ℎ is the incident photon energy (eV), and 𝑚 is a number that characterizes the transition process Depending on the material and the kind of optical transitions that occur during the absorption process, whether they are direct or indirect, 𝑚 may take the values (1/2, 3/2, 2, or 3) It is well known that SiO2 has a direct bandgap, and TiO2 has direct and indirect bandgaps [106] As a result, for the allowed direct and indirect transitions of TiO2-SiO2, 𝑚 takes the values of 1/2 and 2, respectively 0.07 [eV/cm]1/2 0.015 Vir 100 keV 150 keV 200 keV 250 keV hu)1/2 hu)2 [eV/cm]2 0.020 0.010 0.005 0.06 0.05 Virgin 100 keV 150 keV 200 keV 250 keV 0.04 0.03 0.02 0.01 a) 0.000 3.5 4.0 4.5 5.0 incident photon energy hu [eV] b) 0.00 3.0 3.5 4.0 4.5 5.0 incident photon energy hu [eV] Fig 3.18 Plot of (αhν)2 (a) and (αhν)1/2 (b) as a function of photon energy, the bandgap is deduced from the extrapolation of the straight line to (αhν)2 = and (αhν)1/2 = luan an 93 Energy gap value [eV] 4.2 4.1 4.0 Eg-direct Eg-indirect 3.9 3.8 3.7 3.6 3.5 50 100 150 200 250 Energy of irradiating ion [keV] Fig 3.19 Energy gap values as a function of incident ion energy for Xe-implanted TiO2/SiO2 mixed layers From Figs 3.18a and b, the optical energy gap is determined by plotting Tauc equation and taking the extrapolation of the linear portion of the (𝛼ℎ)2 and (𝛼ℎ)1/2 as a function of (ℎ) curve to (𝛼=0), respectively The extracted Eg values of the five samples which are virgin, and implanted by Xe 100, 150, 200 and 250 keV are shown in Fig 3.19 It is evident that the mixed layers of the implanted samples have smaller Eg compare with that of the virgin one Eg decrease with growing of ion energy up to 200 keV, and then increase with ion energy of 250 keV It should be noted that due to scattering losses, the thickness of the films increases the absorbance Also, as film thickness increases, there are significant changes in the optical edge of the films The optical absorption edge of the film is shifted as a result of film thickness, changing the band structure of the films It is found that as ion energy increases, the optical absorption edge changes This demonstrates that defects in thin films can be generated when there are not enough atoms, leading to the formation of unsaturated bonds during the broadening of the films [107] Certain defects in the films are formed as a result of these bonds, and these defects result in localized states in the films Increasing defects widen localized states in the optical band gap, which has the opposite consequence of reducing the optical absorption edge The optical band gaps enhancement therefore can be attributed to the changes in mixed layer thickness and concentration of TiO2 in this area due to variation of produced defects luan an 94 CONCLUSIONS AND FUTURE SCOPE In the present dissertation, the ion-induced mixing of TiO2/SiO2 bilayers was characterized and quantified using RBS method The oxide/oxide samples were irradiated by the noble gas ions Ne+, Ar+, Kr+, and Xe+ at four different energies of 100, 150, 200, and 250 keV Mixing process is associated with shifting of the RBS spectra borders, thus the mixing amount has been usually determined by variation in FWHM of the peaks of over layers This method, however, did not fully quantify mixing for the oxide/oxide systems This work utilized evaluating the degree of variation in relative thickness of TiO2/SiO2 transition layers as a new approach to survey mixing amount Broadening thickness of these mixed area was investigated as a function of ion energy and mass In the energy range of 100 - 250 keV, the interactions occur due to diffusion controlled by cascade mixing With increasing ion energy, mixing amount enhances associating with changes in atomic transport process The dependence of mixing on energy has been observed as a simple linear function for all ion species Ne+, Ar+, Kr+, and Xe+ Mixing degree is not proportional to the defect concentration, whereas the ion energy transfers to the target atoms creating deeper damage play a crucial role in broadening of TiO2/SiO2 mixed area, in other words, the inward mixing process is dominant Since the heavier ions lose energy more intensively and are closer to the interface than the light ions, the mixing amount shows a strong dependence on ion mass The chemical compounds including Ti, TiO2, TiO, and Ti2O3 for 10 nm thickness of un-irradiated and irradiated TiO2 surface layers have been identified using XPS method Concentration of TiO, Ti2O3 increase while concentrations of Ti and TiO2 decrease with the growth of incident ion energy Besides, energy loss of Ne ions linearly reduces with ion energy, and the ions lose most of their energy in TiO2 Accordingly, reducing TiO2 concentration, which enhances energy deposited at the TiO2/SiO2 mixed layers, is considered one of the reasons for mixing amount enhancement as also found by RBS method luan an 95 Using ES method, the thickness of layers, chemical compounds and optical parameters of the TiO2/SiO2 mixed layers before and after irradiation have been obtained The variation of the refractive index 𝑛 and extinction coefficient (𝑘) does not depend on the irradiation as a function of wavelength, while 𝑛 and 𝑘 values vary with ion energy The 𝑛 and 𝑘 of the irradiated samples increase as the Xe+ ion energy rises from 100 to 200 keV At 250 keV, both these parameters decrease to almost the same as those corresponding to the energy of 100 keV A similar relation has also been observed for changes in the optical energy gap of the TiO2/SiO2 mixed layers These effects are attributed to changes in TiO2 amount due to varying created defects concentration in mixed areas It is worth mentioning that the calculating results for thickness of TiO2/SiO2 mixed layers obtained by ES and RBS methods are in good agreement The results of the present work are useful in extending the understanding influence of ions on an oxide/oxide material system Although the experimental observations and the conclusions have been given, there are still restrictions For the structural modification, in this thesis, we focus mainly on the kinetics transportation of ion-solid interactions within the mixing phenomena caused by low-energy ions Some other effects such as amorphization, phase formation, or adhesion of layers have not been investigated Thus, more detailed studies on these effects are recommended with a broader range of ion energy for both bilayer and multilayer systems Also, the ion fluence dependence needs to be surveyed so that the mixing rate could be estimated Regarding the material properties modification, for an ARC, refractive index should be constant over time, and absorption in materials at interfaces should remain as low as possible In our work, the results obtained from the ES method thus predict a degradation for irradiated solar cells However, conclusions cannot be reached due to some experimental limitations in the framework of the thesis Therefore, determining variation of optical constants for the ARC system induced by ions, and how it affects to efficiency of the solar systems need to be considered in the forthcoming studies luan an 96 LIST OF PUBLICATIONS Tran Van Phuc, M Kulik, A P Kobzev, Le Hong Khiem, Study of MOS structures using nuclear analytical methods, Communications in Physics, Vol 27, No (2017), pp 279-289 https://doi.org/10.15625/0868-3166/27/4/10825 T.V Phuc, M Kulik, A P Kobzev, L H Khiem, Study of elemental depth distribution in the material TiO2/SiO2/Si by Rutherford Backscattering Spectrometry (RBS), Communications in Physics, Vol 29, No 3SI (2019), pp 393-400 http://dx.doi.org/10.15625/0868-3166/29/3/14328 T.V Phuc, M Kulik, D Kołodyńska, L.H Khiem, P.L Tuan, J Zuk, M Turek, Investigations of elemental depth distribution and chemical compositions in the TiO2/SiO2/Si structures after ion irradiation, Surface & Coatings Technology, 387 (2020), 125494 http://dx.doi.org/10.1016/j.surfcoat.2020.125494 P.L Tuan, M Kulik, J Nowicka-Scheibe, J Żuk, P Horodek, L.H Khiem, T.V Phuc, Nguyen Ngoc Anh, M Turek, Investigations of chemical and atomic composition of native oxide layers covering SI GaAs implanted with Xe ions, Surface and Coatings Technology, Volume 394, 25 July (2020), 12587 http://dx.doi.org/10.1016/j.surfcoat.2020.125871 Tran Van Phuc, Miroslaw Kulik, Le Hong Khiem, Afag Madadzada, Marcin Turek, Dorota Kołodyńska, Phan Luong Tuan, Nguyen Ngoc Anh, Mai Quynh Anh, Nguyen Van Tiep, Krzysztof Siemek, Variation of TiO2/SiO2 mixed layers induced by Xe+ ion irradiation with energies from 100 to 250 keV, Materials Science and Engineering: B, Volume 277, (2022), 115566 https://doi.org/10.1016/j.mseb.2021.115566 P.L Tuan, M Kulik, T.V Phuc, A.I Madadzada, T.Yu Zelenyak, M Turek, J Zuk, C Mita, A Stanculescu, A.S Doroshkevich, B Jasinska, L.H Khiem, N.N Anh, N.T Bao My, Pseudo-dielectric function spectra of the near surface layer of GaAs implanted with various fluence of Xe+ ions, Thin Solid Films 756 (2022) 139376 https://doi.org/10.1016/j.tsf.2022.139376 luan an 97 SCIENTIFIC CONTRIBUTIONS Time Contributions XII-th International Conference ”Ion Implantation 2018 And Other Applications Of Ions And Electrons”, Kazimierz Dolny, Poland International Conference on Surface Modification of 25-30/8/2019 Materials by Ion Beams (SMMIB-2019), Tomsk, Russia PNPI Winter School on Condensed Matter Physics, 16-21/3/2020 Saint-Petersburg, Russia 28 International Seminar on Interaction of Neutrons with Nuclei: Fundamental Interactions & Neutrons, 24-28/5/ 2021 Nuclear Structure, Ultracold Neutrons, Related Topics 3rd International Conference on Solar Technologies & Hybrid Mini Grids to improve energy access, 15-17/9/2021 Mallorca, Spain, at the University of Balearic Islands (UIB) New Trends in Nuclear Physics Detectors (NTNPD25-27/10/ 2021), Heavy Ion Laboratory, University of Warsaw, 2021 Warsaw, Poland Presentation Poster Oral Poster Oral Oral Oral AWARDS RECEIVED FOR THE SCIENTIFIC CONTRIBUTIONS Award Second prize in the competition “Scientific research, methods and applications of FLNP”, 2017 Outstanding Ph.D student Scholarship, 2019 Domestic Ph.D student Sponsorship, 2020 Organizations Frank 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TÓM TẮT Luận án nghiên cứu chế trộn lẫn nguyên tử TiO2/ SiO2 gây chiếu xạ ion tác động liên quan làm biến đổi tính chất quang tính chất hóa học hệ Các mẫu vật liệu chiếu bốn loại ion khí bao gồm... tác ion vùng phân cách cao hơn, dẫn đến mức độ trộn lẫn lớp TiO2 SiO2 lớn hơn, phù hợp với kết đạt phương pháp RBS luan an ABSTRACT In the present dissertation, ion- beam-induced mixing of TiO2/ SiO2