Bridging molecular dynamics and correlated wave-function methods for accurate finite-temperature properties

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 a prototypical molecular enthalpy of adsorption in zeolite (CH₄ 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.