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Title: 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:
; ; ;  [1];  [2]; ;  [3]
  1. Key Laboratory of Theoretical and Computational Photochemistry, Ministry of Education, College of Chemistry, Beijing Normal University, Beijing 100875 (China)
  2. Guizhou Provincial Key Laboratory of Computational Nano-material Science, Guizhou Normal College, Guiyang 550018 (China)
  3. Department of Physics, Beijing Normal University, Beijing 100875 (China)
Publication Date:
OSTI Identifier:
22493247
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 143; Journal Issue: 19; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
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, E-mail: fangwh@bnu.edu.cn, 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, E-mail: fangwh@bnu.edu.cn, 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. doi:10.1063/1.4935800.
Xie, Binbin, Liu, Lihong, Cui, Ganglong, Fang, Wei-Hai, E-mail: fangwh@bnu.edu.cn, Cao, Jun, Feng, Wei, and Li, Xin-qi. Sat . "Ab initio implementation of quantum trajectory mean-field approach and dynamical simulation of the N{sub 2}CO photodissociation". United States. doi: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, E-mail: fangwh@bnu.edu.cn 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},
journal = {Journal of Chemical Physics},
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}
}