Evolution of the vibrational spectra of single-component solids with pressure: some universalities

TL;DR

This study investigates how the vibrational spectra of single-component solids evolve under pressure, revealing universal behaviors and scaling laws across different potential types and structural forms, supported by numerical, semi-analytical, and experimental data.

Contribution

It uncovers universal scaling laws and behaviors in vibrational spectra evolution under pressure, applicable to various potentials and structures, supported by comprehensive numerical and experimental analysis.

Findings

Average frequency follows a power law with pressure.

Normalized vibrational density of states saturates at high pressure.

Debye frequency and average frequency share the same pressure dependence.

Abstract

We have studied numerically the evolution of the zero temperature vibrational spectra of single-component solids with pressure using various model potentials with power law (type A) or exponential (type B) repulsive part. Based on these data and some semi-analytical calculations our principal results may be summarized as follows. For type A potentials: (i) The average frequency has a power law dependence on the pressure;(ii) The normalized vibrational density of states (NVDOS), with the average frequency as the unit of frequency, will saturate as the pressure keeps increasing. This asymptotic NVDOS is independent of the attractive component of the potential and hence define a universality class; and (iii) At higher pressures the Debye frequency and the average frequency have the same pressure dependence and this dependence is identical for the amorphous form and the two crystalline forms studied (FCC and HCP). For type B potentials, the above phenomenology will hold good to a good approximation over a wide range of intermediate pressures. We suggest a scaling form of the dispersion relations that would explain these observations. Various aspects of the evolution of sound speed with pressure are also studied. In particular we show that the Birch's law prescribing linear relationship between density and sound speed will hold good at very high pressures only in exceptional cases. We have also analyzed the data available in the literature from laboratory experiments and {\it ab initio} calculations and find that there is agreement with our conclusions which are derived from the study of model potentials. We offer explanation for this agreement.