Nuclear quantum effects in ab initio dynamics: theory and experiments for lithium imide

TL;DR

This paper demonstrates a cost-effective stochastic method to include nuclear quantum effects in ab initio simulations, validated by experiments on lithium imide for hydrogen storage.

Contribution

It introduces a novel stochastic scheme for efficiently incorporating nuclear quantum effects in first principles calculations.

Findings

Good agreement between theory and inelastic neutron scattering experiments

The method accurately predicts proton momentum distribution in lithium imide

Shows potential for improved modeling of hydrogen-containing materials

Abstract

Owing to their small mass, hydrogen atoms exhibit strong quantum behavior even at room temperature. Including these effects in first principles calculations is challenging, because of the huge computational effort required by conventional techniques. Here we present the first ab-initio application of a recently-developed stochastic scheme, which allows to approximate nuclear quantum effects inexpensively. The proton momentum distribution of lithium imide, a material of interest for hydrogen storage, was experimentally measured by inelastic neutron scattering experiments and compared with the outcome of quantum thermostatted ab initio dynamics. We obtain favorable agreement between theory and experiments for this purely quantum mechanical property, thereby demonstrating that it is possible to improve the modelling of complex hydrogen-containing materials without additional computational effort.