Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 12, Issue 3, Pages 1104-1109Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.0c03274
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Funding
- NSF CAREER program [CHE-1945276]
- NSF Cyberinfrastructure for Sustained Scientific Innovation program [OAC-1931321]
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This paper introduces a regional embedding approach that allows for correlated wave function treatments of target fragments through small, fragment-localized orbital spaces. Applications show that regional embedding combined with focal-point corrections can provide converged CCSD(T) adsorption energies with very small fragment sizes.
Compared to common density functionals, ab initio wave function methods can provide greater reliability and accuracy, which could prove useful when modeling adsorbates or A defects of otherwise periodic systems. However, the breaking of translational symmetry necessitates large supercells that are often prohibitive for correlated wave function methods. As an alternative, this paper introduces the regional embedding approach, which enables correlated wave function treatments of only a target fragment of interest through small, fragment-localized orbital spaces constructed using a simple overlap criterion. Applications to the adsorption of water on lithium hydride, hexagonal boron nitride, and graphene substrates show that regional embedding combined with focal-point corrections can provide converged CCSD(T) (coupled-cluster) adsorption energies with very small fragment sizes.
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