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

<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>

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

<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>

Assessment of DFT Approaches in Noble Gas Clathrate-like Clusters: Stability and Thermodynamics

We have assessed the performance and accuracy of different wavefunction-based electronic structure methods, such as DFMP2 and domain-based local pair-natural orbital (DLPNO-CCSD(T)), as well as a variety of density functional...