Litcius/Paper detail

A zeroth-order active-space frozen-orbital embedding scheme for multireference calculations

Nan He, Francesco A. Evangelista

2020The Journal of Chemical Physics20 citationsDOIOpen Access PDF

Abstract

Multireference computations of large-scale chemical systems are typically limited by the computational cost of quantum chemistry methods. In this work, we develop a zeroth-order active space embedding theory [ASET(0)], a simple and automatic approach for embedding any multireference dynamical correlation method based on a frozen-orbital treatment of the environment. ASET(0) is combined with the second-order multireference driven similarity renormalization group and tested on several benchmark problems, including the excitation energy of 1-octene and bond-breaking in ethane and pentyldiazene. Finally, we apply ASET(0) to study the singlet-triplet gap of p-benzyne and 9,10-anthracyne diradicals adsorbed on a NaCl surface. Our results show that despite its simplicity, ASET(0) is a powerful and sufficiently accurate embedding scheme applicable when the coupling between the fragment and the environment is in the weak to medium regime.

Topics & Concepts

Multireference configuration interactionEmbeddingCoupled clusterComputational chemistrySinglet stateChemistryComplete active spacePhysicsQuantum mechanicsConfiguration interactionMolecular orbitalComputer scienceMoleculeExcited stateArtificial intelligenceAdvanced Chemical Physics StudiesSpectroscopy and Quantum Chemical StudiesAdvanced NMR Techniques and Applications