Efficient Implementation of the Random Phase Approximation with Domain-Based Local Pair Natural Orbitals

被引:0
|
作者
Liang, Yu Hsuan [1 ]
Zhang, Xing [2 ]
Chan, Garnet Kin-Lic [2 ]
Berkelbach, Timothy C. [1 ,3 ]
Ye, Hong-Zhou [4 ,5 ]
机构
[1] Columbia Univ, Dept Chem, New York, NY 10027 USA
[2] CALTECH, Div Chem & Chem Engn, Pasadena, CA 91125 USA
[3] Flatiron Inst, Initiat Computat Catalysis, New York, NY 10010 USA
[4] Univ Maryland, Dept Chem & Biochem, College Pk, MD 20742 USA
[5] Univ Maryland, Inst Phys Sci & Technol, College Pk, MD 20742 USA
基金
美国国家科学基金会;
关键词
QUANTUM MONTE-CARLO; ELECTRON CORRELATION; CORRELATION-ENERGY; ADSORPTION ENERGIES; EXCHANGE; BENCHMARK; SURFACE; THERMOCHEMISTRY; DEPENDENCE; CHEMISTRY;
D O I
10.1021/acs.jctc.4c01540
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
We present an efficient implementation of the direct random phase approximation (RPA) for molecular systems within the domain-based local pair natural orbital (DLPNO) framework. With recommended loose, normal, and tight parameter settings, DLPNO-RPA achieves approximately 99.7-99.95% accuracy in the total correlation energy compared to a canonical implementation, enabling highly accurate reaction energies and potential energy surfaces to be computed while substantially reducing computational costs. As an application, we demonstrate the capability of DLPNO-RPA to efficiently calculate basis set-converged binding energies for a set of large molecules, with results showing excellent agreement with high-level reference data from both coupled cluster and diffusion Monte Carlo. This development paves the way for the routine use of RPA-based methods in molecular quantum chemistry.
引用
收藏
页码:2918 / 2927
页数:10
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