Nonaffine lattice dynamics with the Ewald method reveals strongly nonaffine elasticity of {\alpha}-quartz

TL;DR

This paper develops a nonaffine lattice dynamical formalism incorporating the Ewald method to accurately compute elastic constants in non-centrosymmetric crystals like { extalpha}-quartz, revealing significant nonaffine softening effects.

Contribution

It introduces a novel framework for calculating elastic constants that accounts for long-range interactions and nonaffine responses in non-centrosymmetric crystals, improving accuracy and efficiency.

Findings

Nonaffine corrections significantly reduce elastic constants in { extalpha}-quartz.

The framework achieves excellent agreement with experimental data.

Nonaffine effects are 3-4 times larger than affine estimates.

Abstract

A lattice dynamical formalism based on nonaffine response theory is derived for non-centrosymmetric crystals, accounting for long-range interatomic interactions using the Ewald method. The framework takes equilibrated static configurations as input to compute the elastic constants in excellent agreement with both experimental data and calculations under strain. Besides this methodological improvement, which enables faster evaluation of elastic constants without the need of explicitly simulating the deformation process, the framework provides insights into the nonaffine contribution to the elastic constants of {\alpha}-quartz. It turns out that, due to the non-centrosymmetric lattice structure, the nonaffine (softening) correction to the elastic constants is very large, such that the overall elastic constants are at least 3-4 times smaller than the affine Born-Huang estimat