Study of low refractive index homogeneous thin film for application on metamaterial

VIETNAM NATIONAL UNIVERSITY OF HANOI VIETNAM JAPAN UNIVERSITY PHAM DINH DAT STUDY OF LOW REFRACTIVE INDEX HOMOGENEOUS THIN FILM FOR APPLICATION ON METAMATERIAL MASTER’S THESIS HANOI, 2019 VIETNAM NATIONAL UNIVERSITY OF HANOI VIETNAM JAPAN UNIVERSITY PHAM DINH DAT STUDY OF LOW REFRACTIVE INDEX HOMOGENEOUS THIN FILM FOR APPLICATION ON METAMATERIAL MAJOR: NANOTECHNOLOGY CODE: PILOT RESEARCH SUPERVISOR: Ph.D PHAM TIEN THANH HANOI, 2019 Acknowledgement First and foremost, I want to express my appreciation to my supervisor, Pham Tien Thanh Ph.D for his patient guidance and encouragement during my study and research at Vietnam Japan University I would like to thank Prof Kajikawa Kotaro and his students at Kajikawa Lab, Faculty of Electrical and Electronics Engineering, Tokyo Institute of Technology who helped us facilities to perform calculation, experiments and measurements I also would like to send my sincere thanks to the lecturers of Nanotechnology Program, Vietnam Japan University, who have taught and interested me over the past two years Besides, I am grateful to my family and my friends who are always there to share their experiences that help me overcome the obstacles of student’s life Hanoi, 17 June, 2019 Author Pham Dinh Dat i TABLE OF CONTENT Acknowledgement LIST OF FIGURES, SCHEMES LIST OF ABBREVIATIONS CHAPTER 1: INTRODUCTION 1.1Metamaterial 1.2Optical material relate to refractive index CHAPTER 2: FUNDAMENTAL THEORY 2.1Effective Medium Theory 2.1.1Effective medium 2.1.2Permittivity calculation 2.2Transfer Matrix for multilayer optics 2.3Finite Difference Time Domain (FDTD) CHAPTER 3: EXPERIMENTS 3.1Silver nanoparticles synthesis 3.1.1Chemicals 3.1.2Process 3.2Thin films fabrication 3.2.1Chemicals 3.2.2Process 3.3Optical properties determination 3.4Thin films thickness determination CHAPTER 4: RESULTS AND DISCUSSION 4.1Calculation results ii 4.1.1 Index of refraction and index of extinction depend on element of particles 22 4.1.2 Index of refraction and index of extinction depend on volume fill fraction of silver nanoparticles on polymer matrix 25 4.1.3 Calculation for thin film following EMT using TMM 28 4.1.4 Calculation for thin film using FDTD method 31 4.1.5 Neighbor particles interaction 34 4.2 Experiment results 37 4.2.1 Properties of silver nanoparticles 37 4.2.2 Properties of thin films 40 CONCLUSION 45 iii LIST OF FIGURES, SCHEMES Fig 1.1: Multilayer structure and nanowires embedded structure metamaterial (A: metal-dielectric layered, B: wires in dielectric host) Fig 2.1: A material model of UEM Fig 2.2:Three simple model of UEM material classified following topology _ Fig 2.3: A simple model for assumption limitation of volume fill fraction _ Fig 2.4: Considered system of TMM problem 11 Fig 2.5: The arrangement of electric- and magnetic-field nodes in space and time 17 Fig 4.1: The index of refraction of PVP including 3% volume fill fraction of silver, gold and copper 22 Fig 4.2: The index of extinction of PVP including 3% volume fill fraction of silver, gold and copper 23 Fig 4.3: The index of refraction of PVA including 3% volume fill fraction of silver, gold and copper 24 Fig 4.4: The index of extinction of PVA including 3% volume fill fraction of silver, gold and copper 24 Fig 4.5: The index of refraction of PVP including 2%, 3%, 4% and 5% volume fill fraction of silver _ 25 Fig 4.6: The index of refraction of PVA including 2%, 3%, 4% and 5% volume fill fraction of silver _ 26 Fig 4.7: The index of extinction of silver and PVP including 2%, 3%, 4% and 5% volume fill fraction of silver 27 Fig 4.8: The index of extinction of silver and PVA including 2%, 3%, 4% and 5% volume fill fraction of silver 27 Fig 4.9: Transmittance spectrum of 30 nm PVP-based films corresponding to different Ag fill fraction _ 28 Fig 4.10: Transmittance spectrum of 30 nm PVA-based films corresponding to different Ag fill fraction _ 29 Fig 4.11: The calculated transmittance spectrum of 200 nm PVP-based films corresponding to different Ag fill fraction using TMM _ 30 iv Fig 4.12: The calculated transmittance spectrum of 200 nm PVA-based films corresponding to different Ag fill fraction using TMM _ 31 Fig 4.13: The FDTD domain for calculation of 200nm film by x, y, z direction and 3D visions 32 Fig 4.14: The calculated transmittance spectrum of 200 nm PVP-based films corresponding to different Ag fill fraction using FDTD method 33 Fig 4.15: The calculated transmittance spectrum of 200 nm PVA-based films corresponding different Ag fill fraction using FDTD method 33 Fig 4.16: The simple model for consider neighbor-particles interaction 35 Fig 4.17: Calculated extinction spectra of two neighbor-particles with distance equal 3nm in medium that has refractive index equal 1.5 using FDTD 36 Fig 4.18: Calculated extinction spectra of neighbor-particles with distance equal 3nm in medium that has refractive index equal 1.5 using DDA _ 37 Fig 4.19: The images of silver nanoparticles solution after synthesis(a), after centrifugation(b) and after re-disperse on water(c) _ 38 Fig 4.20: SEM image of self-synthesis silver nanoparticles 39 Fig 4.21: Transmittance spectrum of self-synthesis and commercial silver nanoparticles solution _ 39 Fig 4.22: Molecular formula of PVP and PVA 40 Fig 4.23: Transmittance spectrum of PVA, PVP solution with and without existence of silver nanoparticles _ 41 Fig 4.24: Transmittance spectrum of drop-coating PVP, PVA films corresponding 3% fill fraction of silver nanoparticles 42 Fig 4.25: Transmittance spectrum of PVP-based films different fill fraction of silver nanoparticles 43 Fig 4.26: Transmittance spectrum of PVA-based films different fill fraction of silver nanoparticles 44 v LIST OF ABBREVIATIONS DDA: Discrete Dipole Approximation EMT: Effective Medium Theory EM: Effective Medium E-field: Electric field LSPR: Localized Surface Plasmon Resonance MGG: Maxwell Garnet geometry MGT: Maxwell Garnett theory FDTD: Finite Different Time Domain H-field: Magnetic field PVP: Poly Vinyl Pyrrolydone PVA: Poly Vinyl Alcohol PML: Perfect Match Layer SPR: Surface Plasmon Resonance TMM: Transfer Matrix Method UEM: Uniform Effective Medium vi CHAPTER 1: INTRODUCTION 1.1 Metamaterial Electromagnetic metamaterial is a class of material using for engineering electromagnetic space and controlling light propagation Metamaterials have shown their promise for the next generation optical materials with electromagnetic behaviors almost can’t be obtained in any conventional materials They have a plenty of application including cloaking [11,15,26], imagining [12,29,41], sensing [18,23,36], wave guiding [13,22,38], absorber [5], etc The metamaterial is fabricated based on the composite structures including inclusions that have sub-wavelength structures The inclusions have designed structure They can be totally artifact or emulate based on nature structure The inclusions are arranged on a host medium that is normally dielectric Due to the small size and distance of inclusion, the metamaterials can be considered as the homogeneous mediums The properties of material are represented through permittivity and permeability By changing shape and size of inclusion, permittivity and permeability of metamaterial can be adjusted to very high or low (even negative) value Under the consideration for permittivity and permeability, the material can be classified into groups [31] They are epsilon-negative material (ENG), mu-negative material (MNG), double positive material (DPS) and double negative material (DNG) The metamaterial is in class of ENG, MNG and DNG materials Besides that, the metamaterial includes band gap material but it will not be considered in this research The three classes ENG, MNG and DNG of metamaterial show the noticeable of negative permittivity and permeability For example, the index of refraction of materials can become small than with structure like in Fig 1.1 It makes the refraction of light becomes very different when comparing with the original materials Fig 1.1: Multilayer structure and nanowires embedded structure metamaterial (A: metal-dielectric layered, B: wires in dielectric host) The metamaterials structuring as in Fig are called as hyperbolic metamaterial In this class of metamaterial, the refractive indexes and arrangement of components play a significant role to properties of metamaterial The below equations is used to calculate the anisotropic dielectric function of layered metamaterial ϵ ϵ with ϵ and ϵ are dielectric function following directions those are parallel and perpendicular with surface of multilayer structure; d d and dm are thickness; and are dielectric function of dielectric material and metal Following it, the very low refractive index n = √ can be achieved by this way [38] The problem is that the fabrication is very complex and expensive The distance between wires, the thickness of each layer must be very precise Here, we can see some issues of the metamaterial Firstly, the properties of metamaterial depend on not only structures but also nature of hosts and inclusions It suggests that along with structural changes, developing materials as host or inclusion also contribute to the metamaterials Most of the researches about the affected by the decreasing dielectric constant of overall medium due to effect from them The existence of silver nanoparticles decreases index of 43 refraction Then this decrease makes blue shift of LSPR signal For consider this phenomena, the range of particles fill fraction will be expanded later Transmittance (unit) 1.02 1.015 1.01 1.005 0.995 0.99 0.985 0.98 0.975 0.3 Fig 4.26: Transmittance spectrum of PVA-based films different fill fraction of silver nanoparticles On wavelength region about 310nm to 400nm, the transmittance of PVAbased films with silver particles (≥ 98.5%) is higher than calculated transmittance of films without particles ( ≥96%) It suggests that the index of refraction of PVA including silver is lower than bare PVA’s and higher than in this wavelength region of light This trend of index of refraction is quite similar as predicted index by EMT So, the decrease of index of extinction due to the nanoparticles is confirmed for PVA thin film As an initial research, this research phase can be considered as completed The next phase will focus to optimize the calculation approximation and to determine precisely both of index of refraction and index of extinction of material 44 CONCLUSION In conclusion, the initial study about the low refractive index and low loss material based on PVP and PVA including silver nanoparticles has conducted The numerical calculation was run using Wolfram Mathematica software and FullWAVE software Applying the approximation following Maxwell Garnett topology for uniform effective medium, the index of refraction and index of extinction of materials was calculated The silver is predicted to be a better element of inclusion for object material compare with gold and copper The suitable size of using silver particles is 20 nm diameter The suitable fill fraction of silver nanoparticles is about 3% to less than 5% Theoretically, the indexes of refraction of those materials are lower than in region of wavelength about 380 to 400 nm The transmittance of thin films based on two types of material was calculated using two methods those are TMM apply refractive index predicted by EMT and FDTD method They verify the existence of LSPR signal at wavelength about 400 nm The predicted extinction is stronger than in real samples The FDTD method also introduces the problem of neighbor-particles interaction affect to transmittance of films It illustrates the picture that should be nearly similar as in real films The experiments focused on determining transmittance of real thin films The PVP-based material is easy to prepare but hard to fabricate and maintain The PVAbased material is harder to prepare but more stable The signal of LSPR of silver nanoparticles is investigated for case of PVA-based films The decrease of index of refraction is also confirmed through transmittance of PVA including silver nanoparticles thin films Here, it is possible to conclude that PVA and silver nanoparticle are promising host and inclusion to fabricate low index of refraction and low loss material The future research will focus to optimize the approximation for prediction and investigate precisely optical properties of materials 45 REFERENCES [1] Abdellatif, S., Sharifi, P., Kirah, K., Ghannam, R., Khalil, A S G., Erni, D., & Marlow, F (2018a) Refractive index and scattering of porous TiO films Microporous and Mesoporous Materials, 264, 84–91 https://doi.org/10.1016/j.micromeso.2018.01.011 [2] Acquaroli, L.N., Urteaga, R., & Koropecki, R R (2010b) Innovative design for optical porous silicon gas sensor Sensors and Actuators B: Chemical, 149(1), 189–193 https://doi.org/10.1016/j.snb.2010.05.065 [3] Acquaroli, Leandro N., Urteaga, R., Berli, C L A., & Koropecki, R R (2011c) Capillary Filling in 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