Electronic, vibrational, and thermodynamic properties of ZnS (zincblende and rocksalt structure)

TL;DR

This study combines experimental measurements and ab initio calculations to analyze the vibrational, electronic, and thermodynamic properties of ZnS in zincblende and rocksalt structures across a wide temperature range.

Contribution

It provides a comprehensive comparison of experimental specific heat data with ab initio lattice dynamics calculations for different isotopic compositions of ZnS.

Findings

Good agreement between experimental and calculated phonon densities of states.

Identification of the influence of 3d core electrons on band structure and spin-orbit splitting.

Analysis of mode Grueneisen parameters at high symmetry points.

Abstract

We have measured the specific heat of zincblende ZnS for several isotopic compositions and over a broad temperature range (3 to 1100 K). We have compared these results with calculations based on ab initio electronic band structures, performed using both LDA and GGA exchange- correlation functionals. We have compared the lattice dynamics obtained in this manner with experimental data and have calculated the one-phonon and two-phonon densities of states. We have also calculated mode Grueneisen parameters at a number of high symmetry points of the Brillouin zone. The electronic part of our calculations has been used to investigate the effect of the 3d core electrons of zinc on the spin-orbit splitting of the top valence bands. The effect of these core electrons on the band structure of the rock salt modification of ZnS is also discussed.