Crystal structure prediction using ab initio evolutionary techniques: principles and applications

TL;DR

This paper introduces a new ab initio evolutionary algorithm for crystal structure prediction that accurately identifies stable and metastable structures across various compounds and conditions, advancing high-pressure crystallography.

Contribution

The paper presents a novel, efficient methodology combining ab initio calculations with evolutionary algorithms for crystal structure prediction without experimental input.

Findings

High success rate in predicting structures for diverse compounds

Resolved important high-pressure crystallography problems

Discovered new high-pressure crystal structures

Abstract

We have developed an efficient and reliable methodology for crystal structure prediction, merging ab initio total-energy calculations and a specifically devised evolutionary algorithm. This method allows one to predict the most stable crystal structure and a number of low-energy metastable structures for a given compound at any P-T conditions without requiring any experimental input. Extremely high success rate has been observed in a few tens of tests done so far, including ionic, covalent, metallic, and molecular structures with up to 40 atoms in the unit cell. We have been able to resolve some important problems in high-pressure crystallography and report a number of new high-pressure crystal structures. Physical reasons for the success of this methodology are discussed.