Projector-Based Quantum Embedding for Molecular Systems: An Investigation of Three Partitioning Approaches Waldrop, Jonathan Windus, Theresa Govind, Niranjan
dc.contributor.department Ames National Laboratory
dc.contributor.department Chemistry 2021-08-05T17:40:58.000 2021-08-14T03:02:55Z 2021-08-14T03:02:55Z Fri Jan 01 00:00:00 UTC 2021 2021-07-29
dc.description.abstract <p>Projector-based embedding is a relatively recent addition to the collection of methods that seek to utilize chemical locality to provide improved computational efficiency. This work considers the interactions between the different proposed procedures for this method and their effects on the accuracy of the results. The interplay between the embedded background, projector type, partitioning scheme, and level of atomic orbital (AO) truncation are investigated on a selection of reactions from the literature. The Huzinaga projection approach proves to be more reliable than the level-shift projection when paired with other procedural options. Active subsystem partitioning from the subsystem projected AO decomposition (SPADE) procedure proves slightly better than the combination of Pipek–Mezey localization and Mulliken population screening (PMM). Along with these two options, a new partitioning criteria is proposed based on subsystem von Neumann entropy and the related subsystem orbital occupancy. This new method overlaps with the previous PMM method, but the screening process is computationally simpler. Finally, AO truncation proves to be a robust option for the tested systems when paired with the Huzinaga projection, with satisfactory results being acquired at even the most severe truncation level.</p>
dc.description.comments <p>This document is the unedited Author’s version of a Submitted Work that was subsequently accepted for publication in the <em>Journal of Physical Chemistry A</em>, copyright © American Chemical Society after peer review. To access the final edited and published work see DOI: <a href="" target="_blank">10.1021/acs.jpca.1c03821</a>. Posted with permission.</p>
dc.format.mimetype application/pdf
dc.identifier archive/
dc.identifier.articleid 2323
dc.identifier.contextkey 24197524
dc.identifier.s3bucket isulib-bepress-aws-west
dc.identifier.submissionpath chem_pubs/1318
dc.language.iso en
dc.source.bitstream archive/|||Fri Jan 14 19:46:19 UTC 2022
dc.source.uri 10.1021/acs.jpca.1c03821
dc.subject.disciplines Physical Chemistry
dc.subject.keywords Algorithms
dc.subject.keywords Embedding
dc.subject.keywords Energy
dc.subject.keywords Chemical calculations
dc.subject.keywords Density functional theory
dc.title Projector-Based Quantum Embedding for Molecular Systems: An Investigation of Three Partitioning Approaches
dc.type article
dc.type.genre article
dspace.entity.type Publication
relation.isAuthorOfPublication 97c1485c-99ca-4fbe-969a-e970c6251814
relation.isOrgUnitOfPublication 25913818-6714-4be5-89a6-f70c8facdf7e
relation.isOrgUnitOfPublication 42864f6e-7a3d-4be3-8b5a-0ae3c3830a11
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