Document Type
Article
Publication Date
2023
Publisher
American Chemical Society
Source Publication
Journal of Physical Chemistry Letters
Source ISSN
1948-7185
Original Item ID
DOI: 10.1021/acs.jpclett.3c02887
Abstract
The phenomena of propensity and inverse propensity are explored using time-dependent mixed quantum classical theory, MQCT, in which the rotational motion of the molecule is treated quantum mechanically, whereas the scattering process is described classically. Good agreement with the results of accurate full-quantum calculations is reported for a closed shell approximation to the NO + Ar system. It is shown that MQCT reproduces both phenomena in a broad range of the final states of the molecule and for various initial rotational states, offering a unique time-dependent insight. It permits seeing that both propensity and inverse propensity occur due to efficient depopulation of some states at the early postcollisional stage of the scattering process, when the molecule exists in a coherent superposition of many excited states that span a very broad range of angular momentum quantum numbers, populated by an efficient stepladder process of many consecutive transitions with small Δj.
Recommended Citation
Imanzi, Kayla; Bostan, Dulat; McCrea, Max; Featherstone, Josh; Brouard, Mark; and Babikov, Dmitri, "Symmetry Breaking: A Classic Example of Quantum Interference Captured by Mixed Quantum/Classical Theory" (2023). Chemistry Faculty Research and Publications. 1074.
https://epublications.marquette.edu/chem_fac/1074
Comments
Accepted version. The Journal of Physical Chemistry Letters, Vol. 14, No. 47 (2023): 10617-10623. DOI. © 2023 American Chemical Society. Used with permission.