Computing energy barriers for rare events from hybrid quantum/classical simulations through the virtual work principle

Abstract

Hybrid quantum/classical techniques can flexibly couple ab initio simulations to an empirical or elastic medium to model materials systems that cannot be contained in small periodic supercells. However, due to electronic nonlocality, a total energy cannot be defined, meaning energy barriers cannot be calculated. We provide a general solution using the principle of virtual work in a modified nudged elastic band algorithm. Our method enables ab initio calculations of the kink formation energy for (100) edge dislocations in molybdenum and lattice trapping barriers to brittle fracture in silicon.