All Hands on Deck: Accelerating Ab Initio Thermochemistry via Wavefunction Approximations

Abstract

<div>We accelerate the G4(MP2) composite model by fine-tuning the individual steps using resolution-of-identity and domain‐based local pair‐natural orbitals. The new variant, G4(MP2)-XP, has a low prediction error when tested on 1694 benchmark molecules. To showcase the method's relevance for large molecules, we determine and present a new reference value for the standard formation enthalpy of buckminsterfullerene. We expect G4(MP2)-XP to become the <i>de facto</i> method for rapid and accurate production of thermochemistry big data.</div>