Bootstrap Embedding for Molecules
Name
acs.jctc.9b00529.pdf
Description
Published version
Size
1.93 MB
Format
Adobe PDF
Checksum (MD5)
758bc2a553639412771496aecaec1d17
Author(s)
Ye, Hongzhou
Ricke, Nathan Darrell
Tran, Henry K.
Van Voorhis, Troy
Date Issued
July 2019
Journal
Journal of Chemical Theory and Computation
Publisher
American Chemical Society (ACS)
Citation
Ye, Hong-Zhou et al. "Bootstrap Embedding for Molecules." Journal of Chemical Theory and Computing 15, 8 (July 2019): 4497-4506 © 2019 American Chemical Society
Version
Final published version
Abstract
Fragment embedding is one way to circumvent the high computational scaling of accurate electron correlation methods. The challenge of applying fragment embedding to molecular systems primarily lies in the strong entanglement and correlation that prevent accurate fragmentation across chemical bonds. Recently, Schmidt decomposition has been shown effective for embedding fragments that are strongly coupled to a bath in several model systems. In this work, we extend a recently developed quantum embedding scheme, bootstrap embedding (BE), to molecular systems. The resulting method utilizes the matching conditions naturally arising from using overlapping fragments to optimize the embedding. Numerical simulation suggests that the accuracy of the embedding improves rapidly with fragment size for small molecules, whereas larger fragments that include orbitals from different atoms may be needed for larger molecules. BE scales linearly with system size (apart from an integral transform) and hence can potentially be useful for large-scale calculations.
MIT Department
Massachusetts Institute of Technology. Department of Chemistry
Terms of Use
Creative Commons Attribution-NonCommercial-NoDerivs License
Persistent DSpace Link
DOI of Published Version
https://doi.org/10.1021/acs.jctc.9b00529
