Computational Prediction and Experimental Realization of Earth-Abundant Transparent Conducting Oxide Ga-Doped ZnSb2O6

Adam J. Jackson; Benjamin J. Parrett; Joe Willis; Alex M. Ganose; W. W. Winnie Leung; Yuhan Liu; Benjamin A.D. Williamson; Timur K. Kim; Moritz Hoesch; Larissa S.I. Veiga; Raman Kalra; Jens Neu; Charles A. Schmuttenmaer; Tien Lin Lee; Anna Regoutz; Tung Chun Lee; Tim D. Veal; Robert G. Palgrave; Robin Perry; David O. Scanlon

doi:10.1021/acsenergylett.2c01961

Computational Prediction and Experimental Realization of Earth-Abundant Transparent Conducting Oxide Ga-Doped ZnSb₂O₆

Adam J. Jackson, Benjamin J. Parrett, Joe Willis, Alex M. Ganose, W. W. Winnie Leung, Yuhan Liu, Benjamin A.D. Williamson, Timur K. Kim, Moritz Hoesch, Larissa S.I. Veiga, Raman Kalra, Jens Neu, Charles A. Schmuttenmaer, Tien Lin Lee, Anna Regoutz, Tung Chun Lee, Tim D. Veal, Robert G. Palgrave, Robin Perry^*, David O. Scanlon^*

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Letter › peer-review

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Abstract

Transparent conducting oxides have become ubiquitous in modern optoelectronics. However, the number of oxides that are transparent to visible light and have the metallic-like conductivity necessary for applications is limited to a handful of systems that have been known for the past 40 years. In this work, we use hybrid density functional theory and defect chemistry analysis to demonstrate that tri-rutile zinc antimonate, ZnSb₂O₆, is an ideal transparent conducting oxide and to identify gallium as the optimal dopant to yield high conductivity and transparency. To validate our computational predictions, we have synthesized both powder samples and single crystals of Ga-doped ZnSb₂O₆which conclusively show behavior consistent with a degenerate transparent conducting oxide. This study demonstrates the possibility of a family of Sb(V)-containing oxides for transparent conducting oxide and power electronics applications.

Original language	English
Pages (from-to)	3807-3816
Number of pages	10
Journal	ACS Energy Letters
Volume	7
Issue number	11
Early online date	10 Oct 2022
DOIs	https://doi.org/10.1021/acsenergylett.2c01961
Publication status	Published - 11 Nov 2022

Bibliographical note

Funding Information:
This work used the ARCHER and ARCHER2 UK National Supercomputing Service ( https://www.archer2.ac.uk ), via our membership of the UK’s HEC Materials Chemistry Consortium, which is funded by the EPSRC (EP/L000202, EP/R029431, and EP/T022213). We are grateful to the UK Materials and Molecular Modelling Hub for computational resources (Thomas and Young), which is partially funded by the EPSRC (EP/P020194/1 and EP/T022213/1). The authors acknowledge the use of the UCL Legion, Myriad, Kathleen, and Thomas High Performance Computing Facilities (Legion@UCL, Myriad@UCL, Kathleen@UCL, Thomas@UCL), and associated support services, in the completion of this work. We acknowledge Diamond Light Source for access to beamline I09 under proposal number SI24449-1. J.W. and D.O.S. acknowledge Diamond Light Source for co-sponsorship of an Eng.D. studentship on the EPSRC Centre for Doctoral Training in Molecular Modelling and Materials Science (EP/L015862/1). A.J.J. and D.O.S. acknowledge support for the EPSRC (grant number EP/N01572X/1). W.W.W.L. acknowledges a Royal Society of Chemistry Researcher Mobility Grant. The authors thank Gavin Stenning at the ISIS material characterization lab for use of XRD and Quantum Design PPMS. We acknowledge useful discussions with Dr. John Buckeridge and Dr. Christoper N. Savory.

Publisher Copyright:
© 2022 American Chemical Society. All rights reserved.

ASJC Scopus subject areas

Chemistry (miscellaneous)
Renewable Energy, Sustainability and the Environment
Fuel Technology
Energy Engineering and Power Technology
Materials Chemistry

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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Cite this

Jackson, A. J., Parrett, B. J., Willis, J., Ganose, A. M., Leung, W. W. W., Liu, Y., Williamson, B. A. D., Kim, T. K., Hoesch, M., Veiga, L. S. I., Kalra, R., Neu, J., Schmuttenmaer, C. A., Lee, T. L., Regoutz, A., Lee, T. C., Veal, T. D., Palgrave, R. G., Perry, R., & Scanlon, D. O. (2022). Computational Prediction and Experimental Realization of Earth-Abundant Transparent Conducting Oxide Ga-Doped ZnSb₂O₆. ACS Energy Letters, 7(11), 3807-3816. https://doi.org/10.1021/acsenergylett.2c01961

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title = "Computational Prediction and Experimental Realization of Earth-Abundant Transparent Conducting Oxide Ga-Doped ZnSb2O6",

abstract = "Transparent conducting oxides have become ubiquitous in modern optoelectronics. However, the number of oxides that are transparent to visible light and have the metallic-like conductivity necessary for applications is limited to a handful of systems that have been known for the past 40 years. In this work, we use hybrid density functional theory and defect chemistry analysis to demonstrate that tri-rutile zinc antimonate, ZnSb2O6, is an ideal transparent conducting oxide and to identify gallium as the optimal dopant to yield high conductivity and transparency. To validate our computational predictions, we have synthesized both powder samples and single crystals of Ga-doped ZnSb2O6which conclusively show behavior consistent with a degenerate transparent conducting oxide. This study demonstrates the possibility of a family of Sb(V)-containing oxides for transparent conducting oxide and power electronics applications.",

author = "Jackson, {Adam J.} and Parrett, {Benjamin J.} and Joe Willis and Ganose, {Alex M.} and Leung, {W. W. Winnie} and Yuhan Liu and Williamson, {Benjamin A.D.} and Kim, {Timur K.} and Moritz Hoesch and Veiga, {Larissa S.I.} and Raman Kalra and Jens Neu and Schmuttenmaer, {Charles A.} and Lee, {Tien Lin} and Anna Regoutz and Lee, {Tung Chun} and Veal, {Tim D.} and Palgrave, {Robert G.} and Robin Perry and Scanlon, {David O.}",

note = "Funding Information: This work used the ARCHER and ARCHER2 UK National Supercomputing Service ( https://www.archer2.ac.uk ), via our membership of the UK{\textquoteright}s HEC Materials Chemistry Consortium, which is funded by the EPSRC (EP/L000202, EP/R029431, and EP/T022213). We are grateful to the UK Materials and Molecular Modelling Hub for computational resources (Thomas and Young), which is partially funded by the EPSRC (EP/P020194/1 and EP/T022213/1). The authors acknowledge the use of the UCL Legion, Myriad, Kathleen, and Thomas High Performance Computing Facilities (Legion@UCL, Myriad@UCL, Kathleen@UCL, Thomas@UCL), and associated support services, in the completion of this work. We acknowledge Diamond Light Source for access to beamline I09 under proposal number SI24449-1. J.W. and D.O.S. acknowledge Diamond Light Source for co-sponsorship of an Eng.D. studentship on the EPSRC Centre for Doctoral Training in Molecular Modelling and Materials Science (EP/L015862/1). A.J.J. and D.O.S. acknowledge support for the EPSRC (grant number EP/N01572X/1). W.W.W.L. acknowledges a Royal Society of Chemistry Researcher Mobility Grant. The authors thank Gavin Stenning at the ISIS material characterization lab for use of XRD and Quantum Design PPMS. We acknowledge useful discussions with Dr. John Buckeridge and Dr. Christoper N. Savory. Publisher Copyright: {\textcopyright} 2022 American Chemical Society. All rights reserved.",

year = "2022",

month = nov,

day = "11",

doi = "10.1021/acsenergylett.2c01961",

language = "English",

volume = "7",

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Jackson, AJ, Parrett, BJ, Willis, J, Ganose, AM, Leung, WWW, Liu, Y, Williamson, BAD, Kim, TK, Hoesch, M, Veiga, LSI, Kalra, R, Neu, J, Schmuttenmaer, CA, Lee, TL, Regoutz, A, Lee, TC, Veal, TD, Palgrave, RG, Perry, R & Scanlon, DO 2022, 'Computational Prediction and Experimental Realization of Earth-Abundant Transparent Conducting Oxide Ga-Doped ZnSb₂O₆', ACS Energy Letters, vol. 7, no. 11, pp. 3807-3816. https://doi.org/10.1021/acsenergylett.2c01961

TY - JOUR

T1 - Computational Prediction and Experimental Realization of Earth-Abundant Transparent Conducting Oxide Ga-Doped ZnSb2O6

AU - Jackson, Adam J.

AU - Parrett, Benjamin J.

AU - Willis, Joe

AU - Ganose, Alex M.

AU - Leung, W. W. Winnie

AU - Liu, Yuhan

AU - Williamson, Benjamin A.D.

AU - Kim, Timur K.

AU - Hoesch, Moritz

AU - Veiga, Larissa S.I.

AU - Kalra, Raman

AU - Neu, Jens

AU - Schmuttenmaer, Charles A.

AU - Lee, Tien Lin

AU - Regoutz, Anna

AU - Lee, Tung Chun

AU - Veal, Tim D.

AU - Palgrave, Robert G.

AU - Perry, Robin

AU - Scanlon, David O.

N1 - Funding Information: This work used the ARCHER and ARCHER2 UK National Supercomputing Service ( https://www.archer2.ac.uk ), via our membership of the UK’s HEC Materials Chemistry Consortium, which is funded by the EPSRC (EP/L000202, EP/R029431, and EP/T022213). We are grateful to the UK Materials and Molecular Modelling Hub for computational resources (Thomas and Young), which is partially funded by the EPSRC (EP/P020194/1 and EP/T022213/1). The authors acknowledge the use of the UCL Legion, Myriad, Kathleen, and Thomas High Performance Computing Facilities (Legion@UCL, Myriad@UCL, Kathleen@UCL, Thomas@UCL), and associated support services, in the completion of this work. We acknowledge Diamond Light Source for access to beamline I09 under proposal number SI24449-1. J.W. and D.O.S. acknowledge Diamond Light Source for co-sponsorship of an Eng.D. studentship on the EPSRC Centre for Doctoral Training in Molecular Modelling and Materials Science (EP/L015862/1). A.J.J. and D.O.S. acknowledge support for the EPSRC (grant number EP/N01572X/1). W.W.W.L. acknowledges a Royal Society of Chemistry Researcher Mobility Grant. The authors thank Gavin Stenning at the ISIS material characterization lab for use of XRD and Quantum Design PPMS. We acknowledge useful discussions with Dr. John Buckeridge and Dr. Christoper N. Savory. Publisher Copyright: © 2022 American Chemical Society. All rights reserved.

PY - 2022/11/11

Y1 - 2022/11/11

N2 - Transparent conducting oxides have become ubiquitous in modern optoelectronics. However, the number of oxides that are transparent to visible light and have the metallic-like conductivity necessary for applications is limited to a handful of systems that have been known for the past 40 years. In this work, we use hybrid density functional theory and defect chemistry analysis to demonstrate that tri-rutile zinc antimonate, ZnSb2O6, is an ideal transparent conducting oxide and to identify gallium as the optimal dopant to yield high conductivity and transparency. To validate our computational predictions, we have synthesized both powder samples and single crystals of Ga-doped ZnSb2O6which conclusively show behavior consistent with a degenerate transparent conducting oxide. This study demonstrates the possibility of a family of Sb(V)-containing oxides for transparent conducting oxide and power electronics applications.

AB - Transparent conducting oxides have become ubiquitous in modern optoelectronics. However, the number of oxides that are transparent to visible light and have the metallic-like conductivity necessary for applications is limited to a handful of systems that have been known for the past 40 years. In this work, we use hybrid density functional theory and defect chemistry analysis to demonstrate that tri-rutile zinc antimonate, ZnSb2O6, is an ideal transparent conducting oxide and to identify gallium as the optimal dopant to yield high conductivity and transparency. To validate our computational predictions, we have synthesized both powder samples and single crystals of Ga-doped ZnSb2O6which conclusively show behavior consistent with a degenerate transparent conducting oxide. This study demonstrates the possibility of a family of Sb(V)-containing oxides for transparent conducting oxide and power electronics applications.

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DO - 10.1021/acsenergylett.2c01961

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JO - ACS Energy Letters

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