We introduce the "selPT" perturbative approach, based on ab initio molecular dynamics (AIMD), for computing accurate finite-temperature properties by efficiently using correlated wave-function methods. We demonstrate the power of the method by computing prototypical molecular enthalpies of adsorption in zeolite (CH4 and CO2 on protonated chabazite at 300~K) using the random phase approximation. Results are in excellent agreement with experiment. The improved accuracy provided by selPT represents a crucial step towards the goal of truly quantitative AIMD prediction of experimental observables at finite temperature.
@article{arxiv.1904.05605,
title = {Bridging molecular dynamics and correlated wave-function methods for accurate finite-temperature properties},
author = {Dario Rocca and Anant Dixit and Michael Badawi and Sébastien Lebègue and Tim Gould and Tomáš Bučko},
journal= {arXiv preprint arXiv:1904.05605},
year = {2019}
}