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Density-based errors in mixed-basis mean-field electronic structure, with implications for embedding and QM/MM methods

Lee, Sebastian J. R. and Miyamoto, Kaito and Ding, Feizhi and Manby, Frederick R. and Miller, Thomas F., III (2017) Density-based errors in mixed-basis mean-field electronic structure, with implications for embedding and QM/MM methods. Chemical Physics Letters, 683 . pp. 375-382. ISSN 0009-2614. http://resolver.caltech.edu/CaltechAUTHORS:20170508-080116014

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Abstract

We consider mean-field electronic structure calculations with subsystems that employ different atomic-orbital basis sets. A major source of error arises in charge-manifestation reactions (including ionization, electron attachment, or deprotonation) due to electronic density artifacts at the subsystem interface. The underlying errors in the electronic density can be largely eliminated with Fock-matrix corrections or by avoiding the use of a minimal basis set in the low-level region. These corrections succeed by balancing the electronegativity of atoms at the subsystem interface, much as link-atoms in QM/MM calculations rely upon balancing the electronegativity of atoms in the truncated QM region.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1016/j.cplett.2017.04.059DOIArticle
http://www.sciencedirect.com/science/article/pii/S0009261417303913PublisherArticle
ORCID:
AuthorORCID
Manby, Frederick R.0000-0001-7611-714X
Miller, Thomas F., III0000-0002-1882-5380
Additional Information:© 2017 Published by Elsevier B.V. Received 28 February 2017, Accepted 18 April 2017, Available online 19 April 2017. This material is based upon work performed by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the U.S. Department of Energy under Award Number DE-SC0004993. The work was also supported by the U.S. Army Research Laboratory under Grant No. W911NF-12-2-0023. S.J.R.L. acknowledges a fellowship from the Caltech Resnick Institute, K.M. acknowledges financial support for his PhD research from Toyota Central R&D Labs, Inc., F.R.M. is grateful for financial support from the Engineering and Physical Sciences Research Council (EP/M013111/1), and T.F.M. acknowledges support from a Camille Dreyfus Teacher-Scholar Award.
Group:Resnick Sustainability Institute
Funders:
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0004993
Army Research Office (ARO)W911NF-12-2-0023
Resnick Sustainability InstituteUNSPECIFIED
Toyota Central R&D Labs, Inc.UNSPECIFIED
Engineering and Physical Sciences Research Council (EPSRC)EP/M013111/1
Camille and Henry Dreyfus FoundationUNSPECIFIED
Subject Keywords:Mixed basis; Embedding; DFT; QM/MM; Embedded mean-field theory
Record Number:CaltechAUTHORS:20170508-080116014
Persistent URL:http://resolver.caltech.edu/CaltechAUTHORS:20170508-080116014
Official Citation:Sebastian J.R. Lee, Kaito Miyamoto, Feizhi Ding, Frederick R. Manby, Thomas F. Miller, Density-based errors in mixed-basis mean-field electronic structure, with implications for embedding and QM/MM methods, Chemical Physics Letters, Volume 683, 2017, Pages 375-382, ISSN 0009-2614, http://dx.doi.org/10.1016/j.cplett.2017.04.059. (http://www.sciencedirect.com/science/article/pii/S0009261417303913)
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:77248
Collection:CaltechAUTHORS
Deposited By: Ruth Sustaita
Deposited On:08 May 2017 20:10
Last Modified:19 Sep 2017 16:34

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