Theoretical prediction of magnetic exchange coupling constants from broken-symmetry coupled cluster calculations

Henry F Schurkus; Garnet Kin-Lic Chan; Dian-Teng Chen; Hai-Ping Cheng; John F Stanton

doi:10.1063/1.5144696

Theoretical prediction of magnetic exchange coupling constants from broken-symmetry coupled cluster calculations

J Chem Phys. 2020 Jun 21;152(23):234115. doi: 10.1063/1.5144696.

Authors

Henry F Schurkus¹, Garnet Kin-Lic Chan¹, Dian-Teng Chen², Hai-Ping Cheng², John F Stanton³

Affiliations

¹ Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, California 91125, USA.
² Department of Physics, University of Florida, Gainesville, Florida 32611, USA.
³ Department of Chemistry, University of Florida, Gainesville, Florida 32611, USA.

PMID: 32571049
DOI: 10.1063/1.5144696

Abstract

Exchange coupling constants (J) are fundamental to the understanding of spin spectra of magnetic systems. Here, we investigate the broken-symmetry (BS) approaches of Noodleman and Yamaguchi in conjunction with coupled cluster (CC) methods to obtain exchange couplings. J values calculated from CC in this fashion converge smoothly toward the full configuration interaction result with increasing level of CC excitation. We compare this BS-CC scheme to the complementary equation-of-motion CC approach on a selection of bridged molecular cases and give results from a few other methodologies for context.