# Zero-Field Splitting Calculations by Multiconfiguration Pair-Density Functional Theory br

JOURNAL OF CHEMICAL THEORY AND COMPUTATION（2022）

Abstract

Zero-field splitting (ZFS) is a fundamental molecular property that is especially relevant for single-molecule magnets (SMMs), electron paramagneticresonance spectra, and quantum computing. Developing a method that can accuratelypredict ZFS parameters can be very powerful for designing new SMMs. One of thechallenges is to include external correlation in an inherently multiconfigurationalopen-shell species for the accurate prediction of magnetic properties. Previouslyavailable methods depend on expensive multireference perturbation theorycalculations to include external correlation. In this paper, we present spin-orbit-inclusive multiconfiguration and multistate pair-density functional theory (MC-PDFT) calculations of ZFSs; these calculations have a cost comparable to complete-active-space self-consistentfield (CASSCF) theory, but they include correlation external to the active space. We found that combining a multistate formulation of MC-PDFT, namely, compressed-state multistate pair-density functional theory, with orbitals optimized by weighted-state-averaged CASSCF, yields reasonably accurate ZFS results

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Key words

zero-field,pair-density

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