Universität zu Köln

Zhang, Jun and Dolg, Michael ORCID: 0000-0002-0538-0837 (2015). Third-Order Incremental Dual-Basis Set Zero-Buffer Approach for Large High-Spin Open-Shell Systems. J. Chem. Theory Comput., 11 (3). S. 962 - 969. WASHINGTON: AMER CHEMICAL SOC. ISSN 1549-9626

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Abstract

The third-order incremental dual-basis set zero-buffer approach (inc3-db-B0) is an efficient, accurate, and black-box quantum chemical method for obtaining correlation energies of large systems, and it has been successfully applied to many real chemical problems. In this work, we extend this approach to high-spin open-shell systems. In the open-shell approach, we will first decompose the occupied orbitals of a system into several domains by a K-means clustering algorithm. The essential part is that we preserve the active (singly occupied) orbitals in all the calculations of the domain correlation energies. The duplicated contributions of the active orbitals to the correlation energy are subtracted from the incremental expansion. All techniques of truncating the virtual space such as the B0 approximation can be applied. This open-shell inc3-db-B0 approach is combined with the CCSD and CCSD(T) methods and applied to the computations of a singlet-triplet gap and an electron detachment process. Our approach exhibits an accuracy better than 0.6 kcal/mol or 0.3 eV compared with the standard implementation, while it saves a large amount of the computational time and can be efficiently parallelized.

Item Type:	Journal Article
Creators:	Creators Email ORCID ORCID Put Code Zhang, Jun UNSPECIFIED UNSPECIFIED UNSPECIFIED Dolg, Michael UNSPECIFIED orcid.org/0000-0002-0538-0837 UNSPECIFIED
URN:	urn:nbn:de:hbz:38-406124
DOI:	10.1021/ct501052e
Journal or Publication Title:	J. Chem. Theory Comput.
Volume:	11
Number:	3
Page Range:	S. 962 - 969
Date:	2015
Publisher:	AMER CHEMICAL SOC
Place of Publication:	WASHINGTON
ISSN:	1549-9626
Language:	English
Faculty:	Faculty of Mathematics and Natural Sciences
Divisions:	Faculty of Mathematics and Natural Sciences > Department of Chemistry > Institute of Theoretical Chemistry
Subjects:	no entry
Uncontrolled Keywords:	Keywords Language COUPLED-CLUSTER METHOD; LOCAL CORRELATION TREATMENT; GREEN FLUORESCENT PROTEIN; CORRELATION-ENERGY; ELECTRON CORRELATION; CONFIGURATION-INTERACTION; PERTURBATION-THEORY; RELATIVE ENERGIES; EFFICIENT; ACCURATE Multiple languages Chemistry, Physical; Physics, Atomic, Molecular & Chemical Multiple languages
Refereed:	Yes
URI:	http://kups.ub.uni-koeln.de/id/eprint/40612