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Representation of diabatic potential energy matrices for multiconfiguration time-dependent hartree treatments of high-dimensional nonadiabatic photodissociation dynamics

Conventional quantum mechanical characterization of photodissociation dynamics is restricted by steep scaling laws with respect to the dimensionality of the system. In this work, we examine the applicability of the multi-configurational time-dependent Hartree (MCTDH) method in treating nonadiabatic...

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Main Authors: Han, Shanyu (Author) , Schröder, Markus (Author) , Gatti, Fabien (Author) , Meyer, Hans-Dieter (Author) , Lauvergnat, David (Author) , Yarkony, David R. (Author) , Guo, Hua (Author)
Format: Article (Journal)
Language:English
Published: July15, 2022
In: Journal of chemical theory and computation
Year: 2022, Volume: 18, Issue: 8, Pages: 4627-4638
ISSN:1549-9626
DOI:10.1021/acs.jctc.2c00370
Online Access:Resolving-System, lizenzpflichtig, Volltext: https://doi.org/10.1021/acs.jctc.2c00370
Verlag, lizenzpflichtig, Volltext: https://pubs.acs.org/doi/10.1021/acs.jctc.2c00370
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Author Notes:Shanyu Han, Markus Schröder, Fabien Gatti, Hans-Dieter Meyer, David Lauvergnat, David R. Yarkony, and Hua Guo
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Summary:Conventional quantum mechanical characterization of photodissociation dynamics is restricted by steep scaling laws with respect to the dimensionality of the system. In this work, we examine the applicability of the multi-configurational time-dependent Hartree (MCTDH) method in treating nonadiabatic photodissociation dynamics in two prototypical systems, taking advantage of its favorable scaling laws. To conform to the sum-of-product form, elements of the ab initio diabatic potential energy matrix (DPEM) are re-expressed using the recently proposed Monte Carlo canonical polyadic decomposition method, with enforcement of proper symmetry. The MCTDH absorption spectra and product branching ratios are shown to compare well with those calculated using conventional grid-based methods, demonstrating its promise for treating high-dimensional nonadiabatic photodissociation problems.
Item Description:Gesehen am 15.11.2022
Physical Description:Online Resource
ISSN:1549-9626
DOI:10.1021/acs.jctc.2c00370

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