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  Charge localization in a diamine cation provides a test of energy functionals and self-interaction correction

Cheng, X., Zhang, Y., Jónsson, E., Jónsson, H., & Weber, P. M. (2016). Charge localization in a diamine cation provides a test of energy functionals and self-interaction correction. Nature Communications, 7: 11013. doi:10.1038/ncomms11013.

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Item Permalink: http://hdl.handle.net/11858/00-001M-0000-002B-500B-D Version Permalink: http://hdl.handle.net/11858/00-001M-0000-002B-500C-B
Genre: Journal Article

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http://dx.doi.org/10.1038/ncomms11013 (Publisher version)
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 Creators:
Cheng, Xinxin1, 2, Author              
Zhang, Yao1, Author
Jónsson, Elvar3, Author
Jónsson, Hannes1, 3, 4, Author
Weber, Peter M.1, Author
Affiliations:
1Department of Chemistry, Brown University, 324 Brook Street, Providence, Rhode Island 02912, USA, ou_persistent22              
2Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_1938288              
3COMP, Department of Applied Physics, Aalto University, FIN-00076 Espoo, Finland, ou_persistent22              
4Faculty of Physical Sciences, VR-III, University of Iceland, 107 Reykjavík, Iceland, ou_persistent22              

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Free keywords: Chemical sciences; Physical chemistry
 Abstract: Density functional theory (DFT) is widely applied in calculations of molecules and materials. Yet, it suffers from a well-known over-emphasis on charge delocalization arising from self-interaction error that destabilizes localized states. Here, using the symmetric diamine N,N′-dimethylpiperazine as a model, we have experimentally determined the relative energy of a state with positive charge localized on one of the two nitrogen atoms, and a state with positive charge delocalized over both nitrogen atoms. The charge-localized state was found to be 0.33 (0.04) eV higher in energy than the charge-delocalized state. This provides an important test of theoretical approaches to electronic structure calculations. Calculations with all DFT functionals commonly used today, including hybrid functionals with exact exchange, fail to predict a stable charge-localized state. However, the application of an explicit self-interaction correction to a semi-local functional identifies both states and gives relative energy in excellent agreement with both experiment and CCSD(T) calculations.

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Language(s): eng - English
 Dates: 2016-06-252016-02-102016-03-16
 Publication Status: Published online
 Pages: 6
 Publishing info: -
 Table of Contents: -
 Rev. Method: Peer
 Identifiers: DOI: 10.1038/ncomms11013
PMC: PMC4799366
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Title: Nature Communications
  Abbreviation : Nat. Commun.
Source Genre: Journal
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Publ. Info: London : Nature Publishing Group
Pages: - Volume / Issue: 7 Sequence Number: 11013 Start / End Page: - Identifier: ISSN: 2041-1723
CoNE: /journals/resource/2041-1723