Understanding the mechanisms of spin-dependent processes, including intersystem crossing transitions in photochemistry, spin-forbidden chemical reactions, and spin-crossovers in materials, is important for  the design of novel photosensitizers, single-molecule magnets, qubits, quantum sensors, and spintronic devices. Predicting the rates of spin-dependent processes is critical for developing the means to control these processes. We will present our implementation of the nonadiabatic statistical theory (NAST) to predict the rates of the spin-orbit-coupling-mediated transitions between the pairs of electronic states with different spin multiplicities in various molecular systems. In addition, the NAST software package can be used to calculate the rates of adiabatic unimolecular reactions proceeding on a single potential energy surface. The NAST package capabilities, modular structure, and the ways to generate the NAST input files from the electronic structure calculations will be described. Finally, several examples of NAST applications, including the adiabatic isomerization of propylene oxide to acetone and propanal, and the T<sub>1</sub>→S<sub>0</sub> relaxation in cyclopropene via intersystem crossing, will be presented.

Implementation of the nonadiabatic statistical theory to predict the rates of spin-dependent processes

ACS Spring 2022

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