Methodological Choices for the Spin-Crossover Energy: Mn(taa) as an Example

ORAL

Abstract

Systematic prediction of the spin-crossover (SCO) energy for both an isolated molecule and its condensed aggregates poses a challenge to current density functional approximations, DFAs [1]. With Mn(taa) as the example, we discuss the effects of DFA choice, dispersion corrections, whether and how to use Hubbard U corrections, and technical and procedural sensitivities and subtleties. We show that, with one exception (r2SCAN [2]), no comparatively simple, non-empirical DFA provides predictive accuracy. Systematic procedures to calculate U fail with popular DFAs. User-driven tuning of U becomes a diagnostic of DFA appropriateness. It confirms the suitability of r2SCAN [2]. In conjunction with structural calculation using r2SCAN-L [3], a rapid procedure for assessing SCO becomes possible.

[1] B. J. Houghton, and R. J. Deeth, Eur. J. Inorg. Chem. 2014, 4573 (2014).
[2] J. W. Furness, A. D. Kaplan, J. Ning, J. P. Perdew, and J. Sun, J. Phys. Chem. Lett. 11, 8208 (2020).
[3] D. Mejia-Rodriguez, and S.B. Trickey, Phys. Rev. B 102, 121109(R) (2020).

*Supported by U.S. Dept. of Energy Frontier Research Center grant DE-SC 0019330

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Presenters

  • Angel Albavera Mata

    • Department of Materials Science and Engineering, University of Florida
    • University of Florida

Authors

  • Angel Albavera Mata

    • Department of Materials Science and Engineering, University of Florida
    • University of Florida

  • Daniel Mejia-Rodriguez

    • University of Florida
    • Department of Physics, University of Florida

  • Eric Fonseca

    • Department of Materials Science and Engineering, University of Florida

  • Dianteng Cheng

    • Department of Physics, University of Florida

  • H-P. Cheng

    • University of Florida
    • Department of Physics, University of Florida
    • Center for Molecular Magnetic Quantum Materials, University of Florida

  • Samuel Trickey

    • University of Florida
    • Department of Physics, University of Florida
    • Center for Molecular Magnetic Quantum Materials, University of Florida

  • Richard Hennig

    • University of Florida
    • Department of Materials Science and Engineering, University of Florida
    • Materials Science and Engineering, University of Florida