CaltechAUTHORS
Published December 13, 2011 | Version Published + Supplemental Material
Journal Article Open

A fast doubly hybrid density functional method close to chemical accuracy using a local opposite spin ansatz

Creators

  • 1. ROR icon Fudan University
  • 2. ROR icon Xiamen University
  • 3. ROR icon Korea Advanced Institute of Science and Technology
  • 4. ROR icon California Institute of Technology

Abstract

We develop and validate the XYGJ-OS functional, based on the adiabatic connection formalism and Görling-Levy perturbation theory to second order and using the opposite-spin (OS) ansatz combined with locality of electron correlation. XYGJ-OS with local implementation scales as N^3 with an overall accuracy of 1.28 kcal/mol for thermochemistry, bond dissociation energies, reaction barrier heights, and nonbonded interactions, comparable to that of 1.06 kcal/mol for the accurate coupled-cluster based G3 method (scales as N^7) and much better than many popular density functional theory methods: B3LYP (4.98), PBE0 (4.36), and PBE (12.10).

Additional Information

© 2011 by the National Academy of Sciences. Contributed by William A. Goddard III, September 21, 2011 (sent for review April 15, 2011). Published online before print November 23, 2011. X.X. acknowledges the support of NSF of China (91027044, 21133004, 20923004), and the Ministry of Science and Technology of China (2007CB815206, 2011CB808505). Y.J. acknowledges the support of National Research Foundation (NRF) of Korea (2010-0023018, 2010-0029034, and 2010-0029728) by the Ministry of Education, Science and Technology (MEST) of Korea. W.A.G. acknowledges the support of USA National Science Foundation (NSF) (ECS-0609128, CTS-0608889), the Center for Catalytic Hydrocarbon Functionalization (Department of Energy, Basic Energy Sciences Award DE-SC0001298), and Office of Naval Research-Defense Advanced Research Projects Agency [ONR-DARPA_ (PROM N00014-06-1-0938 and N00014-05-1-0778)]. Y.J. and W.A.G. have also been supported by the World Class University (WCU) (NRF R-31-2008-000-10055-0) program funded by the Ministry of Education, Science and Technology. Author contributions: X.X., Y.J., and W.A.G. designed research; I.Y.Z., X.X., and Y.J. performed research; I.Y.Z., X.X., Y.J., and W.A.G. analyzed data; and I.Y.Z., X.X., Y.J., and W.A.G. wrote the paper.

Attached Files

Published - Zhang2011p16645P_Natl_Acad_Sci_Usa.pdf

Supplemental Material - pnas.1115123108_SI.pdf

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pnas.1115123108_SI.pdf

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Additional details

Identifiers

PMCID
PMC3250148
Eprint ID
28676
Resolver ID
CaltechAUTHORS:20120105-121854116

Funding

National Natural Science Foundation of China
91027044
National Natural Science Foundation of China
21133004
National Natural Science Foundation of China
20923004
Ministry of Science and Technology (China)
2007CB815206
Ministry of Science and Technology (China)
2011CB808505
National Research Foundation of Korea
2010-0023018
National Research Foundation of Korea
2010-0029034
National Research Foundation of Korea
2010-0029728
Ministry of Education, Science and Technology (Korea)
NSF
ECS-0609128
NSF
CTS-0608889
Department of Energy (DOE)
DE-SC0001298
Office of Naval Research (ONR)
PROM N00014-06-1-0938
Office of Naval Research (ONR)
PROM N00014-05-1-0778
Ministry of Education, Science and Technology (Korea)
R-31-2008-000-10055-0

Dates

Created
2012-01-05
Created from EPrint's datestamp field
Updated
2021-11-09
Created from EPrint's last_modified field