Embedded Multireference Coupled Cluster Theory

被引:32
作者
Coughtrie, David J. [1 ]
Giereth, Robin [1 ]
Kats, Daniel [1 ]
Werner, Hans Joachim [1 ]
Koehn, Andreas [1 ]
机构
[1] Univ Stuttgart, Inst Theoret Chem, D-70569 Stuttgart, Germany
基金
欧洲研究理事会;
关键词
2ND-ORDER PERTURBATION-THEORY; ELECTRON CORRELATION METHODS; LOCAL CORRELATION TREATMENT; AB-INITIO CALCULATIONS; CU2O2 TORTURE TRACK; WAVE-FUNCTION; BASIS-SETS; CONFIGURATION-INTERACTION; GROUND-STATE; SIMULTANEOUS-OPTIMIZATION;
D O I
10.1021/acs.jctc.7b01144
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
Internally contracted multireference coupled cluster (icMRCC) theory is embedded within multireference perturbation theory (MRPT) to calculate energy differences in large strongly correlated systems. The embedding scheme is based on partitioning the orbital spaces of a complete active space self-consistent field (CASSCF) wave function, with a truncated virtual space constructed by transforming selected projected atomic orbitals (PAOs). MRPT is applied to the environment using a subtractive embedding approach that also allows for multilayer embedding. Benchmark calculations are presented for biradical bond dissociation, spin splitting in a heterocyclic carbene and hydrated Fen, and for the super exchange coupling constant in solid nickel oxide. The method is further applied to two large transition metal complexes with a triple-zeta basis set: an iron complex with 175 atoms and 2939 basis functions, and a nickel complex with 231 atoms, and 4175 basis functions.
引用
收藏
页码:693 / 709
页数:17
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