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Journal article
Transition Path Flight Times and Nonadiabatic Electronic Transitions
The journal of physical chemistry letters, Vol.13(30), pp.6966-6974
04/Aug/2022
Abstract
Transition path flight times are studied for scattering on two electronic surfaces with a single crossing. These flight times reveal nontrivial quantum effects such as resonance lifetimes and nonclassical passage times and reveal that nonadiabatic effects often increase flight times. The flight times are computed using numerically exact time propagation and compared with results obtained from the Fewest Switches Surface Hopping (FSSH) method. Comparison of the two methods shows that the FSSH method is reliable for transition path times only when the scattering is classically allowed on the relevant adiabatic surfaces. However, where quantum effects such as tunneling and resonances dominate, the FSSH method is not adequate to accurately predict the correct times and transition probabilities. These results highlight limitations in methods which do not account for quantum interference effects, and suggest that measuring flight times is important for obtaining insights from the time-domain into quantum effects in nonadiabatic scattering.
Details
- Title
- Transition Path Flight Times and Nonadiabatic Electronic Transitions
- Creators
- Xin He - Beijing National Laboratory for Molecular SciencesBaihua Wu - Beijing National Laboratory for Molecular SciencesTom Rivlin - 972WIS_INST___136Jian Liu (Corresponding Author) - Peking UniversityEli Pollak (Corresponding Author) - 972WIS_INST___136
- Resource Type
- Journal article
- Publication Details
- The journal of physical chemistry letters, Vol.13(30), pp.6966-6974; 04/Aug/2022
- Number of pages
- 9
- Publisher
- American Chemical Society
- Language
- English
- DOI
- https://doi.org/10.1021/acs.jpclett.2c01425
- Grant note
- This work has been graciously supported by a joint grant of the National Natural Science Foundation of China (NSFC) and the Israel Science Foundation (ISF), with NSFC Grant No. 21961142017 and ISF Grant No. 2965/19. We acknowledge the High-Performance Computing Platform of Peking University, Beijng PARATERA Tech CO., Ltd., and the Guangzhou Supercomputer Center for providing computational resources. X.H. and B.W. contributed equally to this paper.
- Record Identifier
- 993393884603596
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