Cu2SiSe3 as a promising solar absorber: harnessing cation dissimilarity to avoid killer antisites

Adair Nicolson; Seán R. Kavanagh; Christopher N. Savory; Graeme W. Watson; David O. Scanlon

doi:10.1039/D3TA02429F

Cu₂SiSe₃ as a promising solar absorber: harnessing cation dissimilarity to avoid killer antisites

Adair Nicolson, Seán R. Kavanagh, Christopher N. Savory, Graeme W. Watson, David O. Scanlon^*

^*Corresponding author for this work

Chemistry

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Abstract

Copper-chalcogenides are promising candidates for thin film photovoltaics due to their ideal electronic structure and potential for defect tolerance. To this end, we have theoretically investigated the optoelectronic properties of Cu₂SiSe₃, due to its simple ternary composition, and the favourable difference in charge and size between the cation species, limiting antisite defects and cation disorder. We find it to have an ideal, direct bandgap of 1.52 eV and a maximum efficiency of 30% for a 1.5 μm-thick film at the radiative limit. Using hybrid density functional theory, the formation energies of all intrinsic defects are calculated, revealing the p-type copper vacancy as the dominant defect species, which forms a perturbed host state. Overall, defect concentrations are predicted to be low and have limited impact on non-radiative recombination, as a consequence of the p–d coupling and antibonding character at the valence band maxima. Therefore, we propose that Cu₂SiSe₃ should be investigated further as a potential defect-tolerant photovoltaic absorber.

Original language	English
Pages (from-to)	14833-14839
Number of pages	7
Journal	Journal of Materials Chemistry A
Volume	11
Issue number	27
Early online date	19 Jun 2023
DOIs	https://doi.org/10.1039/D3TA02429F
Publication status	Published - 21 Jul 2023

Bibliographical note

Acknowledgements:
We acknowledge Bodoo Batnaran for sharing data which was useful for comparisons in the early stages of this project. A. N and S. R. K acknowledge the EPSRC and SFI Centre for Doctoral Training in Advanced Characterisation of Materials (EP/S023259/1) for funding a PhD studentship. C. N. S. is grateful to the Department of Chemistry at UCL and the Ramsay Memorial Fellowship Trust for the funding of a Ramsay Fellowship. The authors acknowledge the use of the UCL Kathleen and Thomas High Performance Computing Facility. Via membership of the UK's HEC Materials Chemistry Consortium, which is funded by the EPSRC (EP/L000202, EP/R029431, EP/T022213), this work used the ARCHER2 UK National Supercomputing Service (http://www.archer2.ac.uk/) and the UK Materials and Molecular Modelling (MMM) Hub (Thomas – EP/P020194 & Young – EP/T022213).

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Cite this

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title = "Cu2SiSe3 as a promising solar absorber: harnessing cation dissimilarity to avoid killer antisites",

abstract = "Copper-chalcogenides are promising candidates for thin film photovoltaics due to their ideal electronic structure and potential for defect tolerance. To this end, we have theoretically investigated the optoelectronic properties of Cu2SiSe3, due to its simple ternary composition, and the favourable difference in charge and size between the cation species, limiting antisite defects and cation disorder. We find it to have an ideal, direct bandgap of 1.52 eV and a maximum efficiency of 30% for a 1.5 μm-thick film at the radiative limit. Using hybrid density functional theory, the formation energies of all intrinsic defects are calculated, revealing the p-type copper vacancy as the dominant defect species, which forms a perturbed host state. Overall, defect concentrations are predicted to be low and have limited impact on non-radiative recombination, as a consequence of the p–d coupling and antibonding character at the valence band maxima. Therefore, we propose that Cu2SiSe3 should be investigated further as a potential defect-tolerant photovoltaic absorber.",

author = "Adair Nicolson and Kavanagh, {Se{\'a}n R.} and Savory, {Christopher N.} and Watson, {Graeme W.} and Scanlon, {David O.}",

note = "Acknowledgements: We acknowledge Bodoo Batnaran for sharing data which was useful for comparisons in the early stages of this project. A. N and S. R. K acknowledge the EPSRC and SFI Centre for Doctoral Training in Advanced Characterisation of Materials (EP/S023259/1) for funding a PhD studentship. C. N. S. is grateful to the Department of Chemistry at UCL and the Ramsay Memorial Fellowship Trust for the funding of a Ramsay Fellowship. The authors acknowledge the use of the UCL Kathleen and Thomas High Performance Computing Facility. Via membership of the UK's HEC Materials Chemistry Consortium, which is funded by the EPSRC (EP/L000202, EP/R029431, EP/T022213), this work used the ARCHER2 UK National Supercomputing Service (http://www.archer2.ac.uk/) and the UK Materials and Molecular Modelling (MMM) Hub (Thomas – EP/P020194 & Young – EP/T022213).",

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AU - Nicolson, Adair

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AU - Watson, Graeme W.

AU - Scanlon, David O.

N1 - Acknowledgements: We acknowledge Bodoo Batnaran for sharing data which was useful for comparisons in the early stages of this project. A. N and S. R. K acknowledge the EPSRC and SFI Centre for Doctoral Training in Advanced Characterisation of Materials (EP/S023259/1) for funding a PhD studentship. C. N. S. is grateful to the Department of Chemistry at UCL and the Ramsay Memorial Fellowship Trust for the funding of a Ramsay Fellowship. The authors acknowledge the use of the UCL Kathleen and Thomas High Performance Computing Facility. Via membership of the UK's HEC Materials Chemistry Consortium, which is funded by the EPSRC (EP/L000202, EP/R029431, EP/T022213), this work used the ARCHER2 UK National Supercomputing Service (http://www.archer2.ac.uk/) and the UK Materials and Molecular Modelling (MMM) Hub (Thomas – EP/P020194 & Young – EP/T022213).

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N2 - Copper-chalcogenides are promising candidates for thin film photovoltaics due to their ideal electronic structure and potential for defect tolerance. To this end, we have theoretically investigated the optoelectronic properties of Cu2SiSe3, due to its simple ternary composition, and the favourable difference in charge and size between the cation species, limiting antisite defects and cation disorder. We find it to have an ideal, direct bandgap of 1.52 eV and a maximum efficiency of 30% for a 1.5 μm-thick film at the radiative limit. Using hybrid density functional theory, the formation energies of all intrinsic defects are calculated, revealing the p-type copper vacancy as the dominant defect species, which forms a perturbed host state. Overall, defect concentrations are predicted to be low and have limited impact on non-radiative recombination, as a consequence of the p–d coupling and antibonding character at the valence band maxima. Therefore, we propose that Cu2SiSe3 should be investigated further as a potential defect-tolerant photovoltaic absorber.

AB - Copper-chalcogenides are promising candidates for thin film photovoltaics due to their ideal electronic structure and potential for defect tolerance. To this end, we have theoretically investigated the optoelectronic properties of Cu2SiSe3, due to its simple ternary composition, and the favourable difference in charge and size between the cation species, limiting antisite defects and cation disorder. We find it to have an ideal, direct bandgap of 1.52 eV and a maximum efficiency of 30% for a 1.5 μm-thick film at the radiative limit. Using hybrid density functional theory, the formation energies of all intrinsic defects are calculated, revealing the p-type copper vacancy as the dominant defect species, which forms a perturbed host state. Overall, defect concentrations are predicted to be low and have limited impact on non-radiative recombination, as a consequence of the p–d coupling and antibonding character at the valence band maxima. Therefore, we propose that Cu2SiSe3 should be investigated further as a potential defect-tolerant photovoltaic absorber.

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