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Study of Germanium Carbide and Zirconium Nitride As an Absorber Material for Hot Carrier Solar Cells

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Study of Germanium Carbide and Zirconium Nitride As an Absorber Material for Hot Carrier Solar Cells Study of Germanium carbide and Zirconium nitride as an absorber material for Hot Carrier Solar Cells A thesis in fulfilment of the requirements for the degree of Doctor of Philosophy by Neeti Gupta The School of Photovoltaic and Renewable Energy Engineering The University of New South Wales Sydney, Australia August 2016 PLEASE TYPE THE UNIVERSITY OF NEW SOUTH WALES Thesis/Dissertation Sheet Surname or Family name: Gupta First name: Neeti Other name/s: Abbreviation for degree as given in the University calendar: School: Photovoltaic and Renewable Energy Faculty: Engineering Title: Study of Germanium Carbide and Zirconium Nitride as an absorber material for Hot Carrier Solar Cells Abstract 350 words maximum: (PLEASE TYPE) Hot Carrier Solar Cell {HC-SC) is one of the advanced photovoltaic technologies. The two main building blocks of a HC-SC are: the absorber, where electrons- holes pairs are photo generated by absorbing the incoming photons, and the energy selective contacts, which allow extraction of these carriers to the external circuit in a narrow range of energies. HC-SCs offer the possibility of operating at very high efficiencies (Limiting efficiency above 65% for un-concentrated light) with structure of reduced complexity. An ideal HC-SC operates at very high efficiency by absorbing wide range of photon energies and extracting the photo-generated carriers at elevated temperatures before they thermalize to the band-edge of the absorber material. The finding of suitable absorber material and its fabrication along with characterisation are the initial steps to implement the HC-SC with a better efficiency. Germanium Carbide {Gee) and Zirconium nitride (ZrN) have a large mass difference between their consecutive elements and exhibit a large phonon band gap sufficient to block the dominant carrier cooling mechanism by Klemens decay route. In this thesis, Gee and ZrN have been studied to investigate their suitability as absorbers for HC-SCs. These material have been fabricated using sputtering and characterised using an array of techniques such as X-ray photoelectron spectroscopy, transmission microscopy, X-ray diffraction, Raman spectroscopy, Atomic Force Microscopy and optical absorption spectroscopy to study structural, compositional and optical properties. Transient absorption spectroscopy was used to study the carrier dynamics. Nano-crystalline Gee has been fabricated which may be suitable for photovoltaic application. Germanium carbide with the record of 15.5 % Gee has been demonstrated. Growth of ZrN have been demonstrated in the range of process parameters. Epitaxial growth of ZrN on MgO substrate has been achieved with DC sputtering at 500°C. Carrier dynamics in ZRN film have been investigated with Ultrafast transient absorption measurements which have indicated a long relaxation time of order of hundreds of picoseconds. The finding in the thesis provide initial insight into the properties of Gee and ZrN and show the possibilities of these materials as an absorber for the HC-SC. Declaration relating to disposition of project thesis/dissertation I hereby grant to the University of New South Wales or its agents the right to archive and to make available my thesis or dissertation in whole or in part in th·e University libraries in all forms of media, now or here after known, subject to the provisions of the Copyright Act 1968. I retain all property rights, such as patent rights. I also retain the right to use in future works (such as articles or books) all or part of this thesis or dissertation. I also authorise University Microfilms to use the 350 word abstract of my thesis in Dissertation Abstracts International (this is applicable to doctoral theses only). Signature Witness Signature Date The University recognises that there may be exceptional circumstances requiring restrictions on copying or conditions on use. Requests for restriction for a period of up to 2 years must be made in writing. Requests for a longer period of restriction may be considered in exceptional circumstances and require the aooroval of the Dean of Graduate Research. FOR OFFICE USE ONLY Date of completion of requirements for Award: ORIGINALITY STATEMENT 'I hereby declare that this submission is my own work and to the best of my knowledge it contains no materials previously published or written by another person, or substantial proportions of material which have been accepted for the award of any other degree or diploma at UNSW or any other educational institution, except where due acknowledgement is made in the thesis. Any contribution made to the research by others, with whom I have worked at UNSW or elsewhere, is explicitly acknowledged in the thesis. I also declare that the intellectual content of this thesis is the product of my own work, except to the extent that assistance from others in the project's design and conception or in style, presentation and linguistic expression is acknowledged.' Signed Date COPYRIGHT STATEMENT ‘I hereby grant the University of New South Wales or its agents the right to archive and to make available my thesis or dissertation in whole or part in the University libraries in all forms of media, now or here after known, subject to the provisions of the Copyright Act 1968. I retain all proprietary rights, such as patent rights. I also retain the right to use in future works (such as articles or books) all or part of this thesis or dissertation. I also authorise University Microfilms to use the 350 word abstract of my thesis in Dissertation Abstract International (this is applicable to doctoral theses only). I have either used no substantial portions of copyright material in my thesis or I have obtained permission to use copyright material; where permission has not been granted I have applied/will apply for a partial restriction of the digital copy of my thesis or dissertation.' Signed Date AUTHENTICITY STATEMENT ‘I certify that the Library deposit digital copy is a direct equivalent of the final officially approved version of my thesis. No emendation of content has occurred and if there are any minor variations in formatting, they are the result of the conversion to digital format.’ Signed Date ii THESIS ABSTRACT Hot Carrier Solar Cell (HC-SC) is one of the advanced photovoltaic technologies. The two main building blocks of a HC‐SC are: the absorber, where electrons‐ holes pairs are photo generated by absorbing the incoming photons, and the energy selective contacts, which allow extraction of these carriers to the external circuit in a narrow range of energies. HC‐SCs offer the possibility of operating at very high efficiencies (Limiting efficiency above 65% for un-concentrated light) with structure of reduced complexity. An ideal HC‐SC operates at very high efficiency by absorbing wide range of photon energies and extracting the photo‐generated carriers at elevated temperatures before they thermalize to the band‐edge of the absorber material. The finding of suitable absorber material and its fabrication along with characterisation are the initial steps to implement the HC-SC with a better efficiency. Germanium Carbide (GeC) and Zirconium nitride (ZrN) have a large mass difference between their consecutive elements and exhibit a large phonon band gap sufficient to block the dominant carrier cooling mechanism by Klemens decay route. In this thesis, GeC and ZrN have been studied to investigate their suitability as absorbers for HC-SCs. These material have been fabricated using sputtering and characterised using an array of techniques such as X-ray photoelectron spectroscopy, transmission microscopy, X-ray diffraction, Raman spectroscopy, Atomic Force Microscopy and optical absorption spectroscopy to study structural, compositional and optical properties. Transient absorption spectroscopy was used to study the carrier dynamics. Nano-crystalline GeC has been fabricated which may be suitable for photovoltaic application. Germanium carbide with the record of 15.5 % GeC has been demonstrated. Growth of ZrN have been demonstrated in the range of process parameters. Epitaxial growth of ZrN on MgO substrate has been achieved with DC sputtering at 500oC. Carrier dynamics in ZRN film have been investigated with ultrafast transient absorption measurements which have indicated a long relaxation time of order of hundreds of picoseconds. The finding in the thesis provide initial insight into the properties of GeC and ZrN and show the possibilities of these materials as an absorber for the HC-SC. iii Acknowledgements This work has been supported by many people. It is now my great pleasure to express my gratitude to them. I would like to express my deepest gratitude to my supervisors, Dr. Santosh Shrestha for allowing me to work on this challenging and exciting project. I am grateful for his trust and guidance that he gave me throughout the duration of this project. This allowed me to investigate aspects of the project that interested me the most, keeping my curiosity always at high levels. I very much appreciate his helpful discussions, suggestions, encouragements and efforts relating to my research work. I would like to thank my co-supervisor Professor Gavin Conibeer for his precious advices, useful suggestions and discussions. I am also grateful to him for his scientific and punctual guidance during the crucial moments of my research. It has been great honour to one of his student. A special thank goes to Hongze Xia. I appreciated his great help for the computation of numerical results, presented in the third and fifth chapter of this thesis. I thank Dr. Pasquale Aliberti and Dr. Binesh Putthen Vettill for the series of very helpful discussions on the characterization results. Special Thanks to Dr Shujuan Huang for the discussion on XRD and TEM results. Great thanks to Dr. Bill Gong for the XPS measurements. I am also thankful to the entire LDOT team of the SPREE for being so efficient in keeping the laboratories in such an amazing working order.
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