Abstract
We present first-principles calculations of the thermal and thermal transport properties of that combine an ab initio molecular dynamics (AIMD) approach to calculate interatomic force constants (IFCs) along with a full iterative solution of the Peierls-Boltzmann transport equation for phonons. The newly developed AIMD approach allows determination of harmonic and anharmonic interatomic forces at each temperature, which is particularly appropriate for highly anharmonic materials such as . The calculated phonon dispersions, heat capacity, and thermal expansion coefficient are found to be in good agreement with measured data. The lattice thermal conductivity, , calculated using the AIMD approach nicely matches measured values, showing better agreement than the obtained using temperature-independent IFCs. A significant contribution to from optic phonon modes is found. Already at room temperature, the phonon line shapes show a notable broadening and onset of satellite peaks reflecting the underlying strong anharmonicity.
2 More- Received 24 August 2014
- Revised 26 September 2014
- Corrected 24 October 2014
DOI:https://doi.org/10.1103/PhysRevB.90.134309
©2014 American Physical Society
Corrections
24 October 2014