Atom-Based Bootstrap Embedding For Molecules
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be_atombased.pdf
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Author(s)
Ye, Hongzhou
Van Voorhis, Troy
Date Issued
October 2019
Journal
Journal of Physical Chemistry Letters
Publisher
American Chemical Society (ACS)
Citation
Ye, Hongzhou and Troy Van Voorhis. "Atom-Based Bootstrap Embedding For Molecules." Journal of Physical Chemistry Letters 10, 20 (October 2019): 6368–6374 © 2019 American Chemical Society
Version
Author's final manuscript
Abstract
Recent developments in quantum embedding have offered an attractive approach to describing electron correlation in molecules. However, previous methods such as density matrix embedding theory (DMET) require rigid partitioning of the system into fragments, which creates significant ambiguity for molecules. Bootstrap embedding (BE) is more flexible because it allows overlapping fragments, but when done on an orbital-by-orbital basis, BE introduces ambiguity in defining the connectivity of the orbitals. In this Letter, we present an atom-based fragment definition that significantly augments BE’s performance in molecules. The resulting method, which we term atom-based BE, is very effective at recovering valence electron correlation in moderate-sized bases and delivers near-chemical-accuracy results using extrapolation. We anticipate atom-based BE may lead to a low-scaling and highly accurate approach to electron correlation in large molecules.
MIT Department
Massachusetts Institute of Technology. Department of Chemistry
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Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use.
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DOI of Published Version
https://doi.org/10.1021/acs.jpclett.9b02479
