Cut-off nonlinearities in the low-temperature vibrations of glasses and crystals

TL;DR

This study reveals that truncating interaction potentials in simulations causes persistent low-temperature nonlinearities affecting vibrational modes and elastic properties, challenging the harmonic approximation in glasses and crystals.

Contribution

It demonstrates that cut-off nonlinearities are a general feature in systems with truncated potentials, significantly impacting low-temperature vibrational and elastic properties.

Findings

Cut-off nonlinearities persist at very low temperatures.

Elastic moduli are sensitive to eigen vectors affected by these nonlinearities.

Vibrational density of states remains largely unaffected.

Abstract

We present a computer simulation study of glassy and crystalline states using the standard Lennard-Jones interaction potential that is truncated at a finite cut-off distance, as is typical of many computer simulations. We demonstrate that the discontinuity at the cut-off distance in the first derivative of the potential (corresponding to the interparticle force) leads to the appearance of cut-off nonlinearities. These cut-off nonlinearities persist into the very-low-temperature regime thereby affecting low-temperature thermal vibrations, which leads to a breakdown of the harmonic approximation for many eigen modes, particularly for low-frequency vibrational modes. Furthermore, while expansion nonlinearities which are due to higher order terms in the Taylor expansion of the interaction potential are usually ignored at low temperatures and show up as the temperature increases, cut-off nonlinearities can become most significant at the lowest temperatures. Anharmonic effects readily show up in the elastic moduli which not only depend on the eigen frequencies, but are crucially sensitive to the eigen vectors of the normal modes. Whereas, those observables that rely mainly on static structural information or just the eigen frequencies, such as the vibrational density of states, total potential energy, and specific heat, show negligible dependence on the presence of the cut-off. Similar aspects of nonlinear behavior have recently been reported in model granular materials, where the constituent particles interact through finite-range, purely-repulsive potentials. These nonlinearities have been ascribed to the nature of the sudden cut-off at contact in the force-law, thus we demonstrate that cut-off nonlinearities emerge as a general feature of ordered and disordered solid state systems interacting through truncated potentials.