First Principles Force Field for Metallic Tantalum

TL;DR

This paper introduces a new embedded atom model force field for metallic tantalum, accurately capturing multiple phases, defects, and finite temperature properties based on ab initio calculations, enabling advanced simulations.

Contribution

The paper develops a comprehensive force field for tantalum derived from ab initio data, accurately modeling multiple phases, defects, and thermal properties.

Findings

Force field reproduces QM data for various phases and defects.

Accurately predicts melting temperature and thermal expansion.

Applicable for simulations of defects and high-pressure behavior.

Abstract

We propose a general strategy to develop accurate Force Fields (FF) for metallic systems derived from ab initio quantum mechanical (QM) calculations; we illustrate this approach for tantalum. As input data to the FF we use the linearized augmented plane wave method (LAPW) with the generalized gradient approximation (GGA) to calculate: (i) the zero temperature equation of state (EOS) of Ta for bcc, fcc, and hcp crystal structures for pressures up to ~500 GPa. (ii) Elastic constants. (iii) We use a mixed-basis pseudopotential code to calculate volume relaxed vacancy formation energy also as a function of pressure. In developing the Ta FF we also use previous QM calculations of: (iv) the equation of state for the A15 structure. (v) the surface energy bcc (100). (vi) energetics for shear twinning of the bcc crystal. We find that withappropriate parameters an embedded atom model force field (denoted as qEAM FF) is able to reproduce all this QM data. Thus, the same FF describes with good accuracy the bcc, fcc, hcp and A15 phases of Ta for pressures from ~ -10 GPa to \~ 500 GPa, while also describing the vacancy, surface energy, and shear transformations. The ability of this single FF to describe such a range of systems with a variety of coordinations suggests that it would be accurate for describing defects such as dislocations, grain boundaries, etc. We illustrate the use of the qEAM FF with molecular dynamics to calculate such finite temperature properties as the melting curve up to 300 GPa; we obtain a zero pressure melting temperature of T_{melt}=3150 +/- 50 K in good agreement with experiment (3213-3287 K). We also report on the thermal expansion of Ta in a wide temperature range; our calculated thermal expansivity agrees well with experimental data.