Near Kohn anomalies in the phonon dispersion relations of lead chalcogenides

TL;DR

This paper presents ab-initio phonon dispersion calculations for lead chalcogenides, revealing a near Kohn anomaly at the L point that explains observed dips in optical phonon branches.

Contribution

It is the first to identify a near Kohn anomaly in lead chalcogenides, linking phonon dispersion features to their electronic structure.

Findings

Good agreement with experimental phonon data

Identification of a near Kohn anomaly at the L point

Persistence of the dip in pure lead chalcogenides

Abstract

We present ab-initio phonon dispersion relations for the three lead chalcogenides PbS, PbSe, and PbTe. The acoustic branches are in very good agreement with inelastic neutron-scattering data and calculations of the specific heat give good agreement with experimental data. The pronounced minimum of the transverse optical branch at Gamma due to the near-ferroelectricity of the lead chalcogenides is qualitatively reproduced. In addition, we find a pronounced dip in the longitudinal optical branch at Gamma. This dip was previously explained as the effect of "free carriers" (due to the presence of impurities). The calculations demonstrate that it persists also in the case of pure lead chalcogenides. We explain the dip as a "near Kohn anomaly" which is associated with the small electronic band-gap at the high-symmetry point L.