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

Igor Ying Zhang; Xin Xu; Yousung Jung; William A. Goddard

doi:10.1073/pnas.1115123108

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

Igor Ying Zhang, Xin Xu, Yousung Jung, William A. Goddard

Research output: Contribution to journal › Article › peer-review

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).

Original language	English
Pages (from-to)	19896-19900
Number of pages	5
Journal	Proceedings of the National Academy of Sciences of the United States of America
Volume	108
Issue number	50
DOIs	https://doi.org/10.1073/pnas.1115123108
Publication status	Published - 13 Dec 2011
Externally published	Yes

Keywords

ACM
DHDF
GGA
LDA
MAD

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10.1073/pnas.1115123108

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

abstract = "We develop and validate the XYGJ-OS functional, based on the adiabatic connection formalism and G{\"o}rling-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).",

keywords = "ACM, DHDF, GGA, LDA, MAD",

author = "Zhang, \{Igor Ying\} and Xin Xu and Yousung Jung and Goddard, \{William A.\}",

year = "2011",

month = dec,

day = "13",

doi = "10.1073/pnas.1115123108",

language = "English",

volume = "108",

pages = "19896--19900",

journal = "Proceedings of the National Academy of Sciences of the United States of America",

issn = "0027-8424",

number = "50",

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TY - JOUR

T1 - A fast doubly hybrid density functional method close to chemical accuracy using a local opposite spin ansatz

AU - Zhang, Igor Ying

AU - Xu, Xin

AU - Jung, Yousung

AU - Goddard, William A.

PY - 2011/12/13

Y1 - 2011/12/13

N2 - 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).

AB - 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).

KW - ACM

KW - DHDF

KW - GGA

KW - LDA

KW - MAD

U2 - 10.1073/pnas.1115123108

DO - 10.1073/pnas.1115123108

M3 - Article

AN - SCOPUS:84055200893

SN - 0027-8424

VL - 108

SP - 19896

EP - 19900

JO - Proceedings of the National Academy of Sciences of the United States of America

JF - Proceedings of the National Academy of Sciences of the United States of America

IS - 50

ER -

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

Abstract

Keywords

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