Phonon anharmonicity and negative thermal expansion in SnSe

Journal Article (Journal Article)

The anharmonic phonon properties of SnSe in the Pnma phase were investigated with a combination of experiments and first-principles simulations. Using inelastic neutron scattering (INS) and nuclear resonant inelastic X-ray scattering (NRIXS), we have measured the phonon dispersions and density of states (DOS) and their temperature dependence, which revealed a strong, inhomogeneous shift and broadening of the spectrum on warming. First-principles simulations were performed to rationalize these measurements, and to explain the previously reported anisotropic thermal expansion, in particular the negative thermal expansion within the Sn-Se bilayers. Including the anisotropic strain dependence of the phonon free energy, in addition to the electronic ground state energy, is essential to reproduce the negative thermal expansion. From the phonon DOS obtained with INS and additional calorimetry measurements, we quantify the harmonic, dilational, and anharmonic components of the phonon entropy, heat capacity, and free energy. The origin of the anharmonic phonon thermodynamics is linked to the electronic structure.

Full Text

Duke Authors

Cited Authors

  • Bansal, D; Hong, J; Li, CW; May, AF; Porter, W; Hu, MY; Abernathy, DL; Delaire, O

Published Date

  • August 9, 2016

Published In

Volume / Issue

  • 94 / 5

Electronic International Standard Serial Number (EISSN)

  • 2469-9969

International Standard Serial Number (ISSN)

  • 2469-9950

Digital Object Identifier (DOI)

  • 10.1103/PhysRevB.94.054307

Citation Source

  • Scopus