Regional Embedding Enables High-Level Quantum Chemistry for Surface Science

Compared to common density functionals, ab initio wave function methods can provide greater reliability and accuracy, which could prove useful when modeling adsorbates or 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.

This document is the Accepted Manuscript version of a Published Work that appeared in final form in The Journal of Physical Chemistry Letters, copyright © 2021 American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see


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Work Title Regional Embedding Enables High-Level Quantum Chemistry for Surface Science
Open Access
  1. Bryan T. G. Lau
  2. Gerald Knizia
  3. Timothy C. Berkelbach
License In Copyright (Rights Reserved)
Work Type Article
  1. American Chemical Society (ACS)
Publication Date January 21, 2021
Publisher Identifier (DOI)
  1. 10.1021/acs.jpclett.0c03274
  1. The Journal of Physical Chemistry Letters
Deposited May 27, 2022




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Work History

Version 1

  • Created
  • Added main-a-1.pdf
  • Added Creator Bryan T. G. Lau
  • Added Creator Gerald Knizia
  • Added Creator Timothy C. Berkelbach
  • Published