TY - JOUR
T1 - Lattice dynamics of the tin sulphides SnS2, SnS and Sn2S3
T2 - Vibrational spectra and thermal transport
AU - Skelton, Jonathan M.
AU - Burton, Lee A.
AU - Jackson, Adam J.
AU - Oba, Fumiyasu
AU - Parker, Stephen C.
AU - Walsh, Aron
N1 - Publisher Copyright:
© 2017 the Owner Societies.
PY - 2017
Y1 - 2017
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85024387770&partnerID=8YFLogxK
U2 - 10.1039/c7cp01680h
DO - 10.1039/c7cp01680h
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C2 - 28470289
AN - SCOPUS:85024387770
SN - 1463-9076
VL - 19
SP - 12452
EP - 12465
JO - Physical Chemistry Chemical Physics
JF - Physical Chemistry Chemical Physics
IS - 19
ER -