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 journalReview article

38 Citations (Scopus)

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 languageEnglish
Article number041102
JournalAPL Materials
Volume3
Issue number4
DOIs
Publication statusPublished - 2015 Jan 1

Fingerprint

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

All Science Journal Classification (ASJC) codes

  • Materials Science(all)
  • Engineering(all)

Cite this

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{da4c0b38d0ab4efc8e2a78c3b0251314,
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",
year = "2015",
month = "1",
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",

}

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, 01.01.2015.

Research output: Contribution to journalReview article

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 - 2015/1/1

Y1 - 2015/1/1

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 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.

UR - http://www.scopus.com/inward/record.url?scp=84945267009&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84945267009&partnerID=8YFLogxK

U2 - 10.1063/1.4917044

DO - 10.1063/1.4917044

M3 - Review article

AN - SCOPUS:84945267009

VL - 3

JO - APL Materials

JF - APL Materials

SN - 2166-532X

IS - 4

M1 - 041102

ER -