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Atomic Layer Deposition of Thin Film Indium Oxysulfide - a Non- Toxic Electron Transport Layer for Chalcogenide Solar Cells

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Atomic Layer Deposition of Thin Film Indium Oxysulfide - a Non- Toxic Electron Transport Layer for Chalcogenide Solar Cells Atomic Layer Deposition of Thin Film Indium Oxysulfide - A Non- Toxic Electron Transport Layer for Chalcogenide Solar Cells The Harvard community has made this article openly available. Please share how this access benefits you. Your story matters Citation Jayaraman, Ashwin. 2018. Atomic Layer Deposition of Thin Film Indium Oxysulfide - A Non-Toxic Electron Transport Layer for Chalcogenide Solar Cells. Doctoral dissertation, Harvard University, Graduate School of Arts & Sciences. Citable link http://nrs.harvard.edu/urn-3:HUL.InstRepos:41129213 Terms of Use This article was downloaded from Harvard University’s DASH repository, and is made available under the terms and conditions applicable to Other Posted Material, as set forth at http:// nrs.harvard.edu/urn-3:HUL.InstRepos:dash.current.terms-of- use#LAA Atomic Layer Deposition of Thin Film Indium Oxysulfide - A Non-Toxic Electron Transport Layer for Chalcogenide Solar Cells A dissertation presented by by Ashwin Jayaraman to The Harvard John A. Paulson School of Engineering and Applied Sciences in partial fulfillment of the requirements for the degree of Doctor of Philosophy in the subject of Engineering Sciences Harvard University Cambridge, Massachusetts April 2018 © 2018 by Ashwin Jayaraman All rights reserved. Dissertation Advisor: Professor Roy G. Gordon Ashwin Jayaraman Atomic Layer Deposition of Thin Film Indium Oxysulfide - A Non-Toxic Electron Transport Layer for Chalcogenide Solar Cells Abstract CZT(S,Se) (Cu2ZnSn(SxSe1-x)4) has emerged as an earth-abundant, non-toxic alternative to thin-film photovoltaic technologies based on CIG(S,Se) (Cu(In,Ga)(S,Se)2) and CdTe. Devices employing CZT(S,Se), however, suffer from poor voltage extraction, reaching only 60 % of the Shockley-Queisser limit. The low photovoltage results primarily from interfacial recombination at the absorber-electron conductor junction, owing to mismatch in conduction band energies, lack of conformality, unpassivated defects, and elemental interdiffusion. The best existing heterojunction devices employ CdS as the electron transport layer. We have explored In2(O,S)3 films prepared by atomic layer deposition (ALD) as an electron transport layer for CZT(S,Se). The motivation for this thesis was to tune the bands of In2(O,S)3 by controlling the S:O ratio. This would result in higher collection of photo-generated electrons and higher open circuit voltage on coupling In2(O,S)3 with CZT(S,Se). We initially 3+ 2+ selected In2S3 on grounds that In ion possibly has lower diffusivity than Cd which should limit elemental interdiffusion. It has been previously established in literature by solution deposition that incorporation of oxygen into In2S3 allows us to obtain band positions at the p-n iii junction that should enable good minority carrier extraction. Oxygen incorporation also increases the band gap and therefore the optical transparence. Unfortunately, solution-based methods leave a large number of uncontrollable hydroxyl groups in the film, which affords poor control over electrical properties of the film. We now report that atomic layer deposition (ALD) using alternate cycles of tris(N,N'- diisopropylformamidinato) indium(III) (indium formamidinate), water, and hydrogen sulfide at o 200 C results in growth of a pure In2(O,S)3 film (free of halides, carbon) with close control in- situ over sulfur to oxygen ratio. We arrived at conditions for growth of In2(O,S)3 by studying ALD of binaries In2S3 and In2O3 independently. The choice of precursor for growing In2(O,S)3 was made on the basis of kinetics of the growth process of the aforementioned binaries. As we use water as the oxygen source, there is incorporation of adventitious hydroxyl groups. We are able to control the content of hydroxyl groups in the In2(O,S)3 film though, by varying number of water containing sub-cycles. In2(O,S)3 films exhibited an indirect band gap higher than In2S3 which minimizes absorption losses in the electron transport layer. A reasonably high mobility was obtained with wide and tunable range of carrier concentrations over 5 orders of magnitude. To limit recombination, fewer charge carriers are targeted in In2(O,S)3 close to its junction with absorber while more carriers are targeted adjacent the transparent conducting oxide in the solar cell. Band offset measurements of In2(O,S)3 with reference to CZT(S,Se) by x-ray photoelectron spectroscopy indicate that oxygen incorporation (and resultant decrease in S:O ratio) increases conduction band offset relative to the pure sulfide. We identify In2(O,S)3 with oxygen contents between 4-33 at. % as the optimal composition in combination with CZT(S,Se), to potentially boost the open circuit voltage of the solar cells. iv Acknowledgements This thesis came to fruition because of the kind help and support of many individuals. At the outset I would like to extend my sincerest thanks to my research advisor Professor Roy Gordon for keeping me extremely motivated throughout the duration of graduate research. I like and admire his ability to perform application-oriented research no end. I deeply appreciate his help in my choice of the research topic and related projects. It was an amazing experience to learn the art of well-directed, innovative and improvised scientific research from him. This work would not have been possible without the invaluable collaboration opportunities that Professor Roy Gordon provided with centers of learning like IBM Thomas J Watson labs and Massachusetts institute of technology. I would like to acknowledge the generous financial support by my advisor during my time at Harvard. Simply put, I could not have had a nicer guide and I cannot thank him enough for all the academic support and help with finalizing my career going forward. I sincerely thank my defense committee members Professor Michael Aziz and Professor Frans Spaepen. Professor Aziz also served on my qualification committee and asked me interesting questions on my research direction. I am ever so thankful to have learnt from esteemed professors like him and express my gratitude for all his guidance. I thoroughly enjoyed the “Energy Technology” course conducted by him. Professor Spaepen who was also on my qualification committee was an amazing mentor to me at Harvard. His course on “Kinetics of condensed phase processes”, I felt was the best class that I took at Harvard. I am simply amazed by his ability to communicate complex ideas in v very simple terms. I am very thankful for his generous contribution of time and efforts to make sure my concepts are clear. I am also grateful to Professor David Clarke and Professor Shriram Ramanathan (Now at Purdue University) for mentoring me in my 1st year at Harvard. I learnt immensely from the studies on thermal conductivity variations with pore geometry that I conducted with Professor Clarke. I also benefitted no end from Professor Ramanathan’s knowledge of functional oxide thin films. I would like to thank Professor Ramanathan for giving me the opportunity to serve as his teaching assistant for his course “Electrical, Optical and Magnetic Properties of Materials” I take this opportunity to thank my undergraduate research advisor Professor Upadrasta Ramamurty who was very influential in my choice to do a PhD. His work ethics and quest for excellence I felt were second to none and I feel blessed to have been given a chance to work with him. This work would not have been possible without the unconditional support and mentorship of 2 individuals in the Gordon group, Dr. Sang Bok Kim and Dr. Luke Davis. Dr. Sang Bok Kim synthesized precursors for growth of indium based thin films and I am very grateful for the opportunity to work with him. I sincerely feel that his knowledge in synthetic chemistry and design of novel experiments is unparalleled. I was very impressed by Dr. Luke Davis for his amazing breadth of knowledge in all fields of science and thank him for his suggestions to improve the quality of my work. I would like to thank all Gordon group members who I have been associated with and befriended during my tenure at Harvard. I had a great time getting to know them and learning from them. I extend my humble thanks to current group members who worked with me on solar cells namely Danny Chua, Robert Gustafson, Xizhu Zhao and Lauren Hartle. I closely vi collaborated with Danny Chua and Xizhu Zhao for the electrical and optical measurements respectively done in this work. I specially thank Robert Gustafson for his time and expertise in designing the valve control set up for the atomic layer deposition reactor that was used in this work for the deposition of thin films. I thank other current group members Christina Chang, Aykut Aydin, Xian Gong, Dr. Yunlong Ji, Dr. Yan Jing, Emily Kerr, Dan Pollack, Lu Sun, Dr. Liuchuan Tong and Dr. Marc-Antoni Goulet. I found the research of every group member equally fascinating. I would also like to thank our lab administrator, Teri Howard for being very supportive during my stay at Harvard. I take this opportunity to thank former Gordon group members; Prof. Jaeyeong Heo, Dr. Yeung (Billy) Au, Prof. Sang Woon Lee, Dr. Norifusa Satoh, Dr. Eugene Beh, Dr. Xudong Chen, Prof. Xinwei Wang, Dr. Bin Xi, Dr. Prasert Sinsermsuksakul, Dr. Jing Yang, Dr. Leizhi Sun, Michael Vogel, Dr. Kecheng Li, Dr. Jun Feng, Dr. Kaixiang Lin, Dr. Rachel Heasley, Dr. Tamara Powers and Dr. Michael Marshak. I will fondly remember Dr. Helen Hejin Park who I collaborated with on solar cell buffer layers. Also many thanks are due to Dr. Xiabing Lou for helping me with transmission electron microscopy studies and analysis. I would like to express my gratitude to Professor Sunghwan Lee, a visiting professor in the Gordon lab who collaborated with us on the indium oxide project.
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