Lattice dynamics of the tin sulphides SnS2, SnS and Sn2S3: vibrational spectra and thermal transport

Jonathan M. Skelton, Lee A. Burton, Adam Jackson, Fumiyasu Oba, Stephen C. Parker, Aron Walsh

Research output: Contribution to journalArticle

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Abstract

We present an in-depth first-principles study of the lattice dynamics of the tin sulphides SnS2, Pnma and π-cubic SnS and Sn2S3. An analysis of the harmonic phonon dispersion and vibrational density of states reveals phonon bandgaps between low- and high-frequency modes consisting of Sn and S motion, respectively, and evidences a bond-strength hierarchy in the low-dimensional SnS2, Pnma SnS and Sn2S3 crystals. We model and perform a complete characterisation of the infrared and Raman spectra, including temperature-dependent anharmonic linewidths calculated using many-body perturbation theory. We illustrate how vibrational spectroscopy could be used to identify and characterise phase impurities in tin sulphide samples. The spectral linewidths are used to model the thermal transport, and the calculations indicate that the low-dimensional Sn2S3 has a very low lattice thermal conductivity, potentially giving it superior performance to SnS as a candidate thermoelectric material.

LanguageEnglish
Pages12452-12465
Number of pages14
JournalPhysical Chemistry Chemical Physics
Volume19
Issue number19
DOIs
StatusPublished - 21 May 2017

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Lattice vibrations
Vibrational spectra
Linewidth
vibrational spectra
sulfides
tin
Vibrational spectroscopy
thermoelectric materials
hierarchies
Raman scattering
Thermal conductivity
Energy gap
thermal conductivity
infrared spectra
perturbation theory
Impurities
Raman spectra
low frequencies
Infrared radiation
harmonics

ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

Cite this

Lattice dynamics of the tin sulphides SnS2, SnS and Sn2S3 : vibrational spectra and thermal transport. / Skelton, Jonathan M.; Burton, Lee A.; Jackson, Adam; Oba, Fumiyasu; Parker, Stephen C.; Walsh, Aron.

In: Physical Chemistry Chemical Physics , Vol. 19, No. 19, 21.05.2017, p. 12452-12465.

Research output: Contribution to journalArticle

Skelton, Jonathan M. ; Burton, Lee A. ; Jackson, Adam ; Oba, Fumiyasu ; Parker, Stephen C. ; Walsh, Aron. / Lattice dynamics of the tin sulphides SnS2, SnS and Sn2S3 : vibrational spectra and thermal transport. In: Physical Chemistry Chemical Physics . 2017 ; Vol. 19, No. 19. pp. 12452-12465
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