Ab initio implementation of quantum trajectory mean-field approach and dynamical simulation of the N{sub 2}CO photodissociation
Abstract
In this work, the recently introduced quantum trajectory mean-field (QTMF) approach is implemented and employed to explore photodissociation dynamics of diazirinone (N{sub 2}CO), which are based on the high-level ab initio calculation. For comparison, the photodissociation process has been simulated as well with the fewest-switches surface hopping (FSSH) and the ab initio multiple spawning (AIMS) methods. Overall, the dynamical behavior predicted by the three methods is consistent. The N{sub 2}CO photodissociation at λ > 335 nm is an ultrafast process and the two C—N bonds are broken in a stepwise way, giving birth to CO and N{sub 2} as the final products in the ground state. Meanwhile, some noticeable differences were found in the QTMF, FSSH, and AIMS simulated time constants for fission of the C—N bonds, excited-state lifetime, and nonadiabatic transition ratios in different intersection regions. These have been discussed in detail. The present study provides a clear evidence that direct ab initio QTMF approach is one of the reliable tools for simulating nonadiabatic dynamics processes.
- Authors:
-
- Key Laboratory of Theoretical and Computational Photochemistry, Ministry of Education, College of Chemistry, Beijing Normal University, Beijing 100875 (China)
- Guizhou Provincial Key Laboratory of Computational Nano-material Science, Guizhou Normal College, Guiyang 550018 (China)
- Department of Physics, Beijing Normal University, Beijing 100875 (China)
- Publication Date:
- OSTI Identifier:
- 22493247
- Resource Type:
- Journal Article
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 143; Journal Issue: 19; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0021-9606
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; CARBON MONOXIDE; CHEMICAL BONDS; COMPARATIVE EVALUATIONS; COMPUTERIZED SIMULATION; DISSOCIATION; EXCITED STATES; GROUND STATES; IMPLEMENTATION; LIFETIME; MEAN-FIELD THEORY; NITROGEN; NITROGEN COMPOUNDS; PHOTOLYSIS; SURFACES
Citation Formats
Xie, Binbin, Liu, Lihong, Cui, Ganglong, Fang, Wei-Hai, Cao, Jun, Feng, Wei, and Li, Xin-qi. Ab initio implementation of quantum trajectory mean-field approach and dynamical simulation of the N{sub 2}CO photodissociation. United States: N. p., 2015.
Web. doi:10.1063/1.4935800.
Xie, Binbin, Liu, Lihong, Cui, Ganglong, Fang, Wei-Hai, Cao, Jun, Feng, Wei, & Li, Xin-qi. Ab initio implementation of quantum trajectory mean-field approach and dynamical simulation of the N{sub 2}CO photodissociation. United States. https://doi.org/10.1063/1.4935800
Xie, Binbin, Liu, Lihong, Cui, Ganglong, Fang, Wei-Hai, Cao, Jun, Feng, Wei, and Li, Xin-qi. 2015.
"Ab initio implementation of quantum trajectory mean-field approach and dynamical simulation of the N{sub 2}CO photodissociation". United States. https://doi.org/10.1063/1.4935800.
@article{osti_22493247,
title = {Ab initio implementation of quantum trajectory mean-field approach and dynamical simulation of the N{sub 2}CO photodissociation},
author = {Xie, Binbin and Liu, Lihong and Cui, Ganglong and Fang, Wei-Hai and Cao, Jun and Feng, Wei and Li, Xin-qi},
abstractNote = {In this work, the recently introduced quantum trajectory mean-field (QTMF) approach is implemented and employed to explore photodissociation dynamics of diazirinone (N{sub 2}CO), which are based on the high-level ab initio calculation. For comparison, the photodissociation process has been simulated as well with the fewest-switches surface hopping (FSSH) and the ab initio multiple spawning (AIMS) methods. Overall, the dynamical behavior predicted by the three methods is consistent. The N{sub 2}CO photodissociation at λ > 335 nm is an ultrafast process and the two C—N bonds are broken in a stepwise way, giving birth to CO and N{sub 2} as the final products in the ground state. Meanwhile, some noticeable differences were found in the QTMF, FSSH, and AIMS simulated time constants for fission of the C—N bonds, excited-state lifetime, and nonadiabatic transition ratios in different intersection regions. These have been discussed in detail. The present study provides a clear evidence that direct ab initio QTMF approach is one of the reliable tools for simulating nonadiabatic dynamics processes.},
doi = {10.1063/1.4935800},
url = {https://www.osti.gov/biblio/22493247},
journal = {Journal of Chemical Physics},
issn = {0021-9606},
number = 19,
volume = 143,
place = {United States},
year = {Sat Nov 21 00:00:00 EST 2015},
month = {Sat Nov 21 00:00:00 EST 2015}
}