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 journalArticle

  • 27 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 Cu2 SnS 3). 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.
LanguageEnglish
Article number041102
JournalAPL Materials
Volume3
Issue number4
DOIs
StatusPublished - 1 Apr 2015

Fingerprint

Vibrational spectra
Thermal conductivity
Lattice vibrations
Sulfides
Linewidth
Semiconductor materials
Infrared radiation
Cu2ZnSnS4

Cite this

Vibrational spectra and lattice thermal conductivity of kesterite-structured Cu2ZnSnS4 and Cu2ZnSnSe4. / Skelton, Jonathan M.; Jackson, Adam J.; Dimitrievska, Mirjana; Wallace, Suzanne K.; Walsh, Aron.

In: APL Materials, Vol. 3, No. 4, 041102, 01.04.2015.

Research output: Contribution to journalArticle

Skelton JM, Jackson AJ, Dimitrievska M, Wallace SK, Walsh A. Vibrational spectra and lattice thermal conductivity of kesterite-structured Cu2ZnSnS4 and Cu2ZnSnSe4. APL Materials. 2015 Apr 1;3(4). 041102. Available from, DOI: 10.1063/1.4917044
Skelton, Jonathan M. ; Jackson, Adam J. ; Dimitrievska, Mirjana ; Wallace, Suzanne K. ; Walsh, Aron. / Vibrational spectra and lattice thermal conductivity of kesterite-structured Cu2ZnSnS4 and Cu2ZnSnSe4. In: APL Materials. 2015 ; Vol. 3, No. 4.
@article{df8ef952f3f748179190238883ca9721,
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 Cu2 SnS 3). 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",
year = "2015",
month = "4",
day = "1",
doi = "10.1063/1.4917044",
language = "English",
volume = "3",
journal = "APL Materials",
issn = "2166-532X",
publisher = "American Institute of Physics Publising LLC",
number = "4",

}

TY - JOUR

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 - 2015/4/1

Y1 - 2015/4/1

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 Cu2 SnS 3). 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 Cu2 SnS 3). 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.

UR - http://dx.doi.org/10.1063/1.4917044

U2 - 10.1063/1.4917044

DO - 10.1063/1.4917044

M3 - Article

VL - 3

JO - APL Materials

T2 - APL Materials

JF - APL Materials

SN - 2166-532X

IS - 4

M1 - 041102

ER -