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

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

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
Publication status	Published - 7 Apr 2015

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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.",

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T1 - Vibrational spectra and lattice thermal conductivity of kesterite-structured Cu2ZnSnS4 and Cu2ZnSnSe4

AU - Skelton, Jonathan M.

AU - Jackson, Adam J.

AU - Dimitrievska, Mirjana

AU - Wallace, Suzanne K.

AU - Walsh, Aron

PY - 2015/4/7

Y1 - 2015/4/7

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

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