Angular Momentum Transfer between a Molecular System and a Continuous Circularly Polarized Light Field within a Semiclassical Born-Oppenheimer Surface Hopping Framework

We simulate semiclassically angular momentum transfer for a molecular system subject to a circularly polarized light (CPL) field either moving along a single Born-Oppenheimer (BO) surface or moving along multiple BO surfaces. Both sets of simulations are able to conserve the total angular momentum a...

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Veröffentlicht in:Journal of chemical theory and computation Jg. 20; H. 15; S. 6442
Hauptverfasser: Bian, Xuezhi, Subotnik, Joseph E
Format: Journal Article
Sprache:Englisch
Veröffentlicht: United States 13.08.2024
ISSN:1549-9626, 1549-9626
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Zusammenfassung:We simulate semiclassically angular momentum transfer for a molecular system subject to a circularly polarized light (CPL) field either moving along a single Born-Oppenheimer (BO) surface or moving along multiple BO surfaces. Both sets of simulations are able to conserve the total angular momentum around the propagation direction of the CPL field, the former requiring a Berry force and the latter requiring a surface parametrized by both nuclear position and momentum (a so-called phase-space approach). Our results provide new insight into the nature of semiclassical nonadiabatic dynamics methods and further demonstrate the power of such methods to capture angular momentum transfer between different media, highlighting the need for accurate algorithms that conserve the total angular momentum.
Bibliographie:ObjectType-Article-1
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ISSN:1549-9626
1549-9626
DOI:10.1021/acs.jctc.4c00225