Work

Density Matrix Embedding Theory-Based Multiconfigurational Quantum Chemistry Approach to Lanthanide Single-Ion Magnets

Year: 2025

Type: article

Abstract: 2022, 13, 10627), we now extend the DMET + CASSCF-SO approach to lanthanide SIM systems and further consider the dynamical correlation via multireference perturbation theory within the embedded cluster space. We provide a detailed formulation of the regularized direct inversion of iterative subspace (R-DIIS) algorithm, which ensures obtaining physically correct restricted open-shell Hartree-Fock (ROHF) wave functions, a critical factor for the effectiveness of DMET. Additionally, we introduce the subspace R-DIIS (sR-DIIS) algorithm, which proves to be more efficient and robust for lanthanide systems. Using several representative lanthanide single-ion magnets (4f-SIMs) as test cases, we demonstrate the performance of these new algorithms and highlight the exceptional accuracy of the DMET treatment, with respect to its all-electron counterpart. We anticipate that this enhanced DMET-based multiconfigurational quantum chemistry methodology will significantly advance large-scale theoretical investigations of complex lanthanide systems.

Source: Journal of Chemical Theory and Computation

DOI: 10.1021/acs.jctc.5c01336

Authors: Yuhang Ai, Ze-Wei Li, Zhe-Bin Guan, Hong Jiang

Institutions: Peking University, Beijing National Laboratory for Molecular Sciences

Language: English

Topic: Advanced Chemical Physics Studies

Subfield: Atomic and Molecular Physics, and Optics

Field: Physics and Astronomy

Domain: Physical Sciences

Open Access status: green

Funder: National Natural Science Foundation of China

Awards: G1399844993, 针对分子磁性材料的第一性原理方法发展与理论研究