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Computationally driven discovery of layered quinary oxychalcogenides: Potential p-type transparent conductors?

Computationally driven discovery of layered quinary oxychalcogenides: Potential p-type transparent conductors?
Computationally driven discovery of layered quinary oxychalcogenides: Potential p-type transparent conductors?

Summary: n-type transparent conductors (TCs) are key materials in the modern optoelectronics industry. Despite years of research, the development of a high-performance p-type TC has lagged far behind that of its n-type counterparts, delaying the advent of “transparent electronics”-based p-n junctions. Here, we propose the layered oxysulfide [Cu 2S 2][Sr 3Sc 2O 5] as a structural motif for discovering p-type TCs. We have used density functional theory to screen 24 compositions based on this motif in terms of their thermodynamic and dynamic stability and their electronic structure, thus predicting two p-type TCs and eight other stable systems with semiconductor properties. Following our predictions, we have successfully synthesized our best candidate p-type TC, [Cu 2S 2][Ba 3Sc 2O 5], which displays structural and optical properties that validate our computational models. It is expected that the design principles emanating from this analysis will move the field closer to the realization of a high figure-of-merit p-type TC.

Progress and Potential: This work has predicted and experimentally realized the p-type transparent conductor [Cu 2S 2][Ba 3Sc 2O 5], and at the same time has developed design principles for layered oxychalcogenide materials of this structure type. The layered oxychalcogenide materials offer a large configurational space of potentially stable compounds with tunable functional properties for a wide range of applications. The longer-term ambitions of the research are to use the combined methods of density functional theory and experiments to search for and understand further layered oxychalcogenide structure types and configurations for different semiconductor applications. This research has the potential to affect the types of electronic devices by bringing us closer to the realism of transparent electronics. The research presented will also further the development of applications for which transparent conductors are essential, such as solar cells.

Abstract: The realization of transparent electronics is hindered by the lack of a suitable high-mobility p-type transparent conductor (TC). This work used ab initio simulations to search for a p-type TC based on the layered oxychalcogenide [Cu 2S 2][A 3M 2O 5] structure. The main result of this study was the discovery of the optimum p-type oxychalcogenide TC, [Cu 2S 2][Ba 3Sc 2O 5], predicted to have a higher optical band gap, better hole mobility, and greater stability than its parent compound [Cu 2S 2][Ba 3Sc 2O 5]; this was verified experimentally.

DFT, MAP2: Benchmark, inorganic, layered compounds, materials prediction, mixed anion semiconductors, oxychalcogenides, p-type, photocatalysts, photovoltaics, transparent conductors
2590-2393
759-781
Williamson, Benjamin
ed9fcfca-1cfc-44c3-b4af-dca0b60c8a04
Limburn, Gregory James
afd49e4c-1afa-4c37-b608-fa0581d380f7
Watson, Graeme
77d94716-378e-4546-b773-7d9bc02e116e
Hyett, Geoffrey
4f292fc9-2198-4b18-99b9-3c74e7dfed8d
Scanlon, David O.
23dbcc36-0b42-40dc-a3af-64c8bad7beb3
Williamson, Benjamin
ed9fcfca-1cfc-44c3-b4af-dca0b60c8a04
Limburn, Gregory James
afd49e4c-1afa-4c37-b608-fa0581d380f7
Watson, Graeme
77d94716-378e-4546-b773-7d9bc02e116e
Hyett, Geoffrey
4f292fc9-2198-4b18-99b9-3c74e7dfed8d
Scanlon, David O.
23dbcc36-0b42-40dc-a3af-64c8bad7beb3

Williamson, Benjamin, Limburn, Gregory James, Watson, Graeme, Hyett, Geoffrey and Scanlon, David O. (2020) Computationally driven discovery of layered quinary oxychalcogenides: Potential p-type transparent conductors? Matter, 3 (3), 759-781. (doi:10.1016/j.matt.2020.05.020).

Record type: Article

Abstract

Summary: n-type transparent conductors (TCs) are key materials in the modern optoelectronics industry. Despite years of research, the development of a high-performance p-type TC has lagged far behind that of its n-type counterparts, delaying the advent of “transparent electronics”-based p-n junctions. Here, we propose the layered oxysulfide [Cu 2S 2][Sr 3Sc 2O 5] as a structural motif for discovering p-type TCs. We have used density functional theory to screen 24 compositions based on this motif in terms of their thermodynamic and dynamic stability and their electronic structure, thus predicting two p-type TCs and eight other stable systems with semiconductor properties. Following our predictions, we have successfully synthesized our best candidate p-type TC, [Cu 2S 2][Ba 3Sc 2O 5], which displays structural and optical properties that validate our computational models. It is expected that the design principles emanating from this analysis will move the field closer to the realization of a high figure-of-merit p-type TC.

Progress and Potential: This work has predicted and experimentally realized the p-type transparent conductor [Cu 2S 2][Ba 3Sc 2O 5], and at the same time has developed design principles for layered oxychalcogenide materials of this structure type. The layered oxychalcogenide materials offer a large configurational space of potentially stable compounds with tunable functional properties for a wide range of applications. The longer-term ambitions of the research are to use the combined methods of density functional theory and experiments to search for and understand further layered oxychalcogenide structure types and configurations for different semiconductor applications. This research has the potential to affect the types of electronic devices by bringing us closer to the realism of transparent electronics. The research presented will also further the development of applications for which transparent conductors are essential, such as solar cells.

Abstract: The realization of transparent electronics is hindered by the lack of a suitable high-mobility p-type transparent conductor (TC). This work used ab initio simulations to search for a p-type TC based on the layered oxychalcogenide [Cu 2S 2][A 3M 2O 5] structure. The main result of this study was the discovery of the optimum p-type oxychalcogenide TC, [Cu 2S 2][Ba 3Sc 2O 5], predicted to have a higher optical band gap, better hole mobility, and greater stability than its parent compound [Cu 2S 2][Ba 3Sc 2O 5]; this was verified experimentally.

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Accepted/In Press date: 20 May 2020
e-pub ahead of print date: 23 June 2020
Published date: 2 September 2020
Keywords: DFT, MAP2: Benchmark, inorganic, layered compounds, materials prediction, mixed anion semiconductors, oxychalcogenides, p-type, photocatalysts, photovoltaics, transparent conductors

Identifiers

Local EPrints ID: 442290
URI: http://eprints.soton.ac.uk/id/eprint/442290
ISSN: 2590-2393
PURE UUID: fe4e03e7-c41f-43d2-832b-9d835c4e1f16
ORCID for Geoffrey Hyett: ORCID iD orcid.org/0000-0001-9302-9723

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Date deposited: 10 Jul 2020 16:41
Last modified: 28 Apr 2022 06:13

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Contributors

Author: Benjamin Williamson
Author: Gregory James Limburn
Author: Graeme Watson
Author: Geoffrey Hyett ORCID iD
Author: David O. Scanlon

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