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

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

doi:10.1039/c7cp01680h

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

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

Department of Physics

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

160 Scopus citations

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.

Original language	English
Pages (from-to)	12452-12465
Number of pages	14
Journal	Physical Chemistry Chemical Physics
Volume	19
Issue number	19
DOIs	https://doi.org/10.1039/c7cp01680h
State	Published - 2017

Bibliographical note

Funding Information:
JMS gratefully acknowledges support from the Engineering and Physical Sciences Research Council (EPSRC) (grant no. EP/K004956/1 and EP/P007821/1). LAB is an International Research Fellow of the Japan Society for the Promotion of Science (JSPS; grant no. 26.04792). AW is grateful for support from the Royal Society and the EPSRC (grant no. EP/M009580/1). Calculations were carried out on the Balena HPC cluster at the University of Bath, which is maintained by Bath University Computing Services, and on the SiSu supercomputer at the IT Center for Science (CSC), Finland, via the Partnership for Advanced Computing in Europe (PRACE) project no. 13DECI0317/IsoSwitch. Some of the calculations were also carried out on the UK national Archer HPC facility, accessed through membership of the UK Materials Chemistry Consortium, which is funded by EPSRC grant no. EP/L000202.

Publisher Copyright:
© 2017 the Owner Societies.

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10.1039/c7cp01680h

Cite this

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title = "Lattice dynamics of the tin sulphides SnS2, SnS and Sn2S3: Vibrational spectra and thermal transport",

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.",

author = "Skelton, {Jonathan M.} and Burton, {Lee A.} and Jackson, {Adam J.} and Fumiyasu Oba and Parker, {Stephen C.} and Aron Walsh",

note = "Funding Information: JMS gratefully acknowledges support from the Engineering and Physical Sciences Research Council (EPSRC) (grant no. EP/K004956/1 and EP/P007821/1). LAB is an International Research Fellow of the Japan Society for the Promotion of Science (JSPS; grant no. 26.04792). AW is grateful for support from the Royal Society and the EPSRC (grant no. EP/M009580/1). Calculations were carried out on the Balena HPC cluster at the University of Bath, which is maintained by Bath University Computing Services, and on the SiSu supercomputer at the IT Center for Science (CSC), Finland, via the Partnership for Advanced Computing in Europe (PRACE) project no. 13DECI0317/IsoSwitch. Some of the calculations were also carried out on the UK national Archer HPC facility, accessed through membership of the UK Materials Chemistry Consortium, which is funded by EPSRC grant no. EP/L000202. Publisher Copyright: {\textcopyright} 2017 the Owner Societies.",

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AU - Walsh, Aron

N1 - Funding Information: JMS gratefully acknowledges support from the Engineering and Physical Sciences Research Council (EPSRC) (grant no. EP/K004956/1 and EP/P007821/1). LAB is an International Research Fellow of the Japan Society for the Promotion of Science (JSPS; grant no. 26.04792). AW is grateful for support from the Royal Society and the EPSRC (grant no. EP/M009580/1). Calculations were carried out on the Balena HPC cluster at the University of Bath, which is maintained by Bath University Computing Services, and on the SiSu supercomputer at the IT Center for Science (CSC), Finland, via the Partnership for Advanced Computing in Europe (PRACE) project no. 13DECI0317/IsoSwitch. Some of the calculations were also carried out on the UK national Archer HPC facility, accessed through membership of the UK Materials Chemistry Consortium, which is funded by EPSRC grant no. EP/L000202. Publisher Copyright: © 2017 the Owner Societies.

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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.

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