Spin-Dependent Stereochemistry: A Nonadiabatic Quantum Dynamics Case Study of S + H2 → SH + H Reaction

Bian, Xuezhi; Subotnik, Joseph E.

doi:10.1021/acs.jpclett.3c03344

Title: Spin-Dependent Stereochemistry: A Nonadiabatic Quantum Dynamics Case Study of S + H₂ → SH + H Reaction

Journal Article · 19 March 2024 · Journal of Physical Chemistry Letters

DOI: https://doi.org/10.1021/acs.jpclett.3c03344 · OSTI ID:2510489

^[1]; Subotnik, Joseph E. ^[1]

University of Pennsylvania, Philadelphia, PA (United States)

We study the spin-dependent stereodynamics of the S + H₂ → SH + H reaction by using full-dimensional quantum dynamics calculations with zero total nuclear angular momentum along the triplet ³A" states and singlet ¹A' states. We find that the interplay between the electronic spin direction and the molecular geometry has a measurable influence on the singlet–triplet intersystem crossing reaction probabilities. Our results show that for some incident scattering angles in the body-fixed frame, the relative difference in intersystem crossing reaction probabilities (as determined between spin up and spin down initial states) can be as large as 15%. Furthermore, our findings are an ab initio demonstration of spin-dependent nonadiabatic dynamics, which we hope will shine light as far as understanding the chiral-induced spin selectivity effect.

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Research Organization:: University of Pennsylvania, Philadelphia, PA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0019397

OSTI ID:: 2510489

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 12 Vol. 15; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Spin-Dependent Stereochemistry: A Nonadiabatic Quantum Dynamics Case Study of S + H2 → SH + H Reaction

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Title: Spin-Dependent Stereochemistry: A Nonadiabatic Quantum Dynamics Case Study of S + H₂ → SH + H Reaction