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NAST: Nonadiabatic Statistical Theory Package for Predicting Kinetics of Spin-Dependent Processes

Topics in Current Chemistry volume 380, Article number: 15 (2022) Cite this article

Abstract

We present a nonadiabatic statistical theory (NAST) package for predicting kinetics of spin-dependent processes, such as intersystem crossings, spin-forbidden unimolecular reactions, and spin crossovers. The NAST package can calculate the probabilities and rates of transitions between the electronic states of different spin multiplicities. Both the microcanonical (energy-dependent) and canonical (temperature-dependent) rate constants can be obtained. Quantum effects, including tunneling, zero-point vibrational energy, and reaction path interference, can be accounted for. In the limit of an adiabatic unimolecular reaction proceeding on a single electronic state, NAST reduces to the traditional transition state theory. Because NAST requires molecular properties at only a few points on potential energy surfaces, it can be applied to large molecular systems, used with accurate high-level electronic structure methods, and employed to study slow nonadiabatic processes. The essential NAST input data include the nuclear Hessian at the reactant minimum, as well as the nuclear Hessians, energy gradients, and spin–orbit coupling at the minimum energy crossing point (MECP) between two states. The additional computational tools included in the NAST package can be used to extract the required input data from the output files of electronic structure packages, calculate the effective Hessian at the MECP, and fit the reaction coordinate for more advanced NAST calculations. We describe the theory, its implementation, and three examples of application to different molecular systems.

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Availability of data and material

The input files for the electronic structure, NAST and MESMER calculations discussed in the main text are available in the SI.

Code availability

The source code of the NAST package is available free of charge at https://github.com/svarganov/NAST.

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Acknowledgements

This work was supported by the National Science Foundation through a CAREER Award (CHE-1654547). We acknowledge Dr. Ryan Zaari for his contributions to the earlier version of the NAST package and thank Drs. Danil Kaliakin and Saikat Mukherjee for fruitful discussions.

Funding

This work was supported by the National Science Foundation through a CAREER Award (CHE 1654547).

Author information

Author notes

  1. Aleksandr O. Lykhin

    Present address: Department of Chemistry, The University of Chicago, Chicago, IL, 60637, USA

Authors and Affiliations

  1. Department of Chemistry, University of Nevada, Reno, 1664 N. Virginia Street, Reno, NV, 89557-0216, USA

    Vsevolod D. Dergachev, Mitra Rooein, Ilya D. Dergachev, Aleksandr O. Lykhin, Robert C. Mauban & Sergey A. Varganov

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  1. Vsevolod D. Dergachev
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Contributions

S.A.V. supervised the NAST package development. V.D.D., M.R., I.D.D., A.O.L. and R.C.M. wrote different parts of the code. V.D.D, M.R. and I.D.D. performed the electronic structure and kinetics calculations. All authors contributed to the preparation of the manuscript.

Corresponding author

Correspondence to Sergey A. Varganov.

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This article is part of the Topical Collection “New Horizon in Computational Chemistry Software”; edited by Michael Filatov, Cheol H. Choi, and Massimo Olivucci.

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Dergachev, V.D., Rooein, M., Dergachev, I.D. et al. NAST: Nonadiabatic Statistical Theory Package for Predicting Kinetics of Spin-Dependent Processes. Top Curr Chem (Z) 380, 15 (2022). https://doi.org/10.1007/s41061-022-00366-w

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