Vibrational spectra and lattice thermal conductivity of kesterite-structured Cu2ZnSnS4 and Cu2ZnSnSe4

Jonathan M. Skelton; Adam J. Jackson; Mirjana Dimitrievska; Suzanne K. Wallace; Aron Walsh

doi:10.1063/1.4917044

Vibrational spectra and lattice thermal conductivity of kesterite-structured Cu₂ZnSnS₄ and Cu₂ZnSnSe₄

Jonathan M. Skelton, Adam J. Jackson, Mirjana Dimitrievska, Suzanne K. Wallace, Aron Walsh

Department of Physics

Research output: Contribution to journal › Review article › peer-review

71 Scopus citations

Abstract

Cu₂ZnSnS₄ (CZTS) is a promising material for photovoltaic and thermoelectric applications. Issues with quaternary semiconductors include chemical disorder (e.g., Cu-Zn antisites) and disproportionation into secondary phases (e.g., ZnS and Cu₂SnS₃). To provide a reference for the pure kesterite structure, we report the vibrational spectra - including both infra-red and Raman intensities - from lattice-dynamics calculations using first-principles force constants. Three-phonon interactions are used to estimate phonon lifetimes (spectral linewidths) and thermal conductivity. CZTS exhibits a remarkably low lattice thermal conductivity, competitive with high-performance thermoelectric materials. Transition from the sulfide to selenide (Cu₂ZnSnSe₄) results in softening of the phonon modes and an increase in phonon lifetimes.

Original language	English
Article number	041102
Journal	APL Materials
Volume	3
Issue number	4
DOIs	https://doi.org/10.1063/1.4917044
State	Published - Apr 2015

Bibliographical note

Funding Information:
We thank A. Togo for discussions on phonon theory and access to Phono3py. We acknowledge membership of the UK’s HPC Materials Chemistry Consortium, which is funded by EPSRC Grant No. EP/L000202. J.M.S. is funded by an EPSRC Programme Grant (No. EP/K004956/1). A.J.J. and S.K.W. are funded by the EPSRC Doctoral Training Centre in Sustainable Chemical Technologies (Nos. EP/G03768X/1 and EP/L016354/1). M.D. has received funding from the People Program (Marie Curie Actions) of the European Union’s Seventh Framework Program under REA Grant Agreement No. 316488 (KESTCELLS). A.W. acknowledges support from the Royal Society and the ERC (Grant No. 277757).

Publisher Copyright:
© 2015 Author(s).

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10.1063/1.4917044

Cite this

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title = "Vibrational spectra and lattice thermal conductivity of kesterite-structured Cu2ZnSnS4 and Cu2ZnSnSe4",

abstract = "Cu2ZnSnS4 (CZTS) is a promising material for photovoltaic and thermoelectric applications. Issues with quaternary semiconductors include chemical disorder (e.g., Cu-Zn antisites) and disproportionation into secondary phases (e.g., ZnS and Cu2SnS3). To provide a reference for the pure kesterite structure, we report the vibrational spectra - including both infra-red and Raman intensities - from lattice-dynamics calculations using first-principles force constants. Three-phonon interactions are used to estimate phonon lifetimes (spectral linewidths) and thermal conductivity. CZTS exhibits a remarkably low lattice thermal conductivity, competitive with high-performance thermoelectric materials. Transition from the sulfide to selenide (Cu2ZnSnSe4) results in softening of the phonon modes and an increase in phonon lifetimes.",

author = "Skelton, {Jonathan M.} and Jackson, {Adam J.} and Mirjana Dimitrievska and Wallace, {Suzanne K.} and Aron Walsh",

note = "Funding Information: We thank A. Togo for discussions on phonon theory and access to Phono3py. We acknowledge membership of the UK{\textquoteright}s HPC Materials Chemistry Consortium, which is funded by EPSRC Grant No. EP/L000202. J.M.S. is funded by an EPSRC Programme Grant (No. EP/K004956/1). A.J.J. and S.K.W. are funded by the EPSRC Doctoral Training Centre in Sustainable Chemical Technologies (Nos. EP/G03768X/1 and EP/L016354/1). M.D. has received funding from the People Program (Marie Curie Actions) of the European Union{\textquoteright}s Seventh Framework Program under REA Grant Agreement No. 316488 (KESTCELLS). A.W. acknowledges support from the Royal Society and the ERC (Grant No. 277757). Publisher Copyright: {\textcopyright} 2015 Author(s).",

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AU - Wallace, Suzanne K.

AU - Walsh, Aron

N1 - Funding Information: We thank A. Togo for discussions on phonon theory and access to Phono3py. We acknowledge membership of the UK’s HPC Materials Chemistry Consortium, which is funded by EPSRC Grant No. EP/L000202. J.M.S. is funded by an EPSRC Programme Grant (No. EP/K004956/1). A.J.J. and S.K.W. are funded by the EPSRC Doctoral Training Centre in Sustainable Chemical Technologies (Nos. EP/G03768X/1 and EP/L016354/1). M.D. has received funding from the People Program (Marie Curie Actions) of the European Union’s Seventh Framework Program under REA Grant Agreement No. 316488 (KESTCELLS). A.W. acknowledges support from the Royal Society and the ERC (Grant No. 277757). Publisher Copyright: © 2015 Author(s).

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N2 - Cu2ZnSnS4 (CZTS) is a promising material for photovoltaic and thermoelectric applications. Issues with quaternary semiconductors include chemical disorder (e.g., Cu-Zn antisites) and disproportionation into secondary phases (e.g., ZnS and Cu2SnS3). To provide a reference for the pure kesterite structure, we report the vibrational spectra - including both infra-red and Raman intensities - from lattice-dynamics calculations using first-principles force constants. Three-phonon interactions are used to estimate phonon lifetimes (spectral linewidths) and thermal conductivity. CZTS exhibits a remarkably low lattice thermal conductivity, competitive with high-performance thermoelectric materials. Transition from the sulfide to selenide (Cu2ZnSnSe4) results in softening of the phonon modes and an increase in phonon lifetimes.

AB - Cu2ZnSnS4 (CZTS) is a promising material for photovoltaic and thermoelectric applications. Issues with quaternary semiconductors include chemical disorder (e.g., Cu-Zn antisites) and disproportionation into secondary phases (e.g., ZnS and Cu2SnS3). To provide a reference for the pure kesterite structure, we report the vibrational spectra - including both infra-red and Raman intensities - from lattice-dynamics calculations using first-principles force constants. Three-phonon interactions are used to estimate phonon lifetimes (spectral linewidths) and thermal conductivity. CZTS exhibits a remarkably low lattice thermal conductivity, competitive with high-performance thermoelectric materials. Transition from the sulfide to selenide (Cu2ZnSnSe4) results in softening of the phonon modes and an increase in phonon lifetimes.

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