Analytic Linear Vibronic Coupling Method for First-Principles Spin-Dynamics Calculations in Single-Molecule Magnets.

ABSTRACT: Accurate modeling of vibronically driven magnetic relaxation from ab initio calculations is of paramount importance to the design of next-generation single-molecule magnets (SMMs). Previous theoretical studies have been relying on numerical differentiation to obtain spin-phonon couplings in the form of derivatives of spin Hamiltonian parameters. In this work, we introduce a novel approach to obtain these derivatives fully analytically by combining the linear vibronic coupling (LVC) approach with analytic complete active space self-consistent field derivatives and nonadiabatic couplings computed at the equilibrium geometry with a single electronic structure calculation. We apply our analytic approach to the computation of Orbach and Raman relaxation rates for a bis-cyclobutadienyl Dy(III) s

SUBMITTER: Staab JK 

PROVIDER: S-EPMC9648194 | biostudies-literature | 2022 Nov

REPOSITORIES: biostudies-literature