Comparison of Density-Matrix Corrections to Density Functional Theory

被引:14
|
作者
Gibney, Daniel [1 ,2 ]
Boyn, Jan-Niklas [1 ,2 ]
Mazziotti, David A. [1 ,2 ]
机构
[1] Univ Chicago, Dept Chem, Chicago, IL 60637 USA
[2] Univ Chicago, James Franck Inst, Chicago, IL 60637 USA
基金
美国国家科学基金会;
关键词
SELF-INTERACTION ERROR; CONFIGURATION-INTERACTION; ENERGY; THERMOCHEMISTRY; STATES;
D O I
10.1021/acs.jctc.2c00625
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Density functional theory (DFT), one of the most widely utilized methods available to computational chemistry, fails to describe systems with statically correlated electrons. To address this shortcoming, in previous work, we transformed DFT into a one-electron reduced density matrix theory (1-RDMFT) via the inclusion of a quadratic one-electron reduced density matrix (1-RDM) correction. Here, we combine our 1-RDMFT approach with different DFT functionals as well as Hartree-Fock to elucidate the method's dependence on the underlying functional selection. Furthermore, we generalize the information density matrix functional theory (iDMFT), recently developed as a correction to the Hartree-Fock method, by incorporating density functionals in place of the Hartree-Fock functional. We relate iDMFT mathematically to our approach and benchmark the two with a common set of functionals and systems.
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页码:6600 / 6607
页数:8
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