Finite temperature elastic constants of paramagnetic materials within the disordered local moment picture from ab initio molecular dynamics calculations

TL;DR

This paper introduces a new ab initio molecular dynamics approach combining disordered local moments and symmetry-imposed force constants to accurately compute the elastic constants of paramagnetic materials at high temperatures, exemplified by CrN.

Contribution

The study develops a novel theoretical scheme integrating DLM-MD and SIFC-TDEP methods for calculating elastic properties of magnetic materials in the paramagnetic state.

Findings

Elastic constants of CrN match experimental data at 300 K.

Young's modulus decreases by ~14% from 300 K to 1200 K.

CrN becomes more isotropic with increasing temperature.

Abstract

We present a theoretical scheme to calculate the elastic constants of magnetic materials in the high-temperature paramagnetic state. Our approach is based on a combination of disordered local moments picture and ab initio molecular dynamics (DLM-MD). Moreover, we investigate a possibility to enhance the efficiency of the simulations of elastic properties using recently introduced method: symmetry imposed force constant temperature dependent effective potential (SIFC-TDEP). We have chosen cubic paramagnetic CrN as a model system. This is done due to its technological importance and its demonstrated strong coupling between magnetic and lattice degrees of freedom. We have studied the temperature dependent single-crystal and polycrystalline elastic constants of paramagentic CrN up to 1200 K. The obtained results at T= 300 K agree well with the experimental values of polycrystalline elastic constants as well as Poisson ratio at room temperature. We observe that the Young's modulus is strongly dependent on temperature, decreasing by ~14% from T=300 K to 1200 K. In addition we have studied the elastic anisotropy of CrN as a function of temperature and we observe that CrN becomes substantially more isotropic as the temperature increases. We demonstrate that the use of Birch law may lead to substantial errors for calculations of temperature induced changes of elastic moduli. The proposed methodology can be used for accurate predictions of mechanical properties of magnetic materials at temperatures above their magnetic order-disorder phase transition.