Diffractive imaging of dissociation and ground-state dynamics in a complex molecule
Abstract
We have investigated the structural dynamics in photoexcited 1,2-diiodotetrafluoroethane molecules $$(C_2F_4I_2)$$ in the gas phase experimentally using ultrafast electron diffraction and theoretically using FOMO-CASCI excited-state dynamics simulations. The molecules are excited by an ultraviolet femtosecond laser pulse to a state characterized by a transition from the iodine $5p⊥$ orbital to a mixed $5p ∥ σ$ hole and $$CF^∙_2$$ antibonding orbital, which results in the cleavage of one of the carbon-iodine bonds. We have observed, with sub-Angstrom resolution, the motion of the nuclear wave packet of the dissociating iodine atom followed by coherent vibrations in the electronic ground state of the $$C_2F_4I_2$$ radical. The radical reaches a stable classical (nonbridged) structure in less than 200 fs.
- Authors:
-
- Univ. of Nebraska, Lincoln, NE (United States). Dept. of Physics and Astronomy
- SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford PULSE Institute, Menlo Park CA (United States); Stanford Univ., CA (United States). Dept. of Chemistry
- SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford PULSE Institute, Menlo Park CA (United States)
- Stanford PULSE Institute, Menlo Park CA (United States)
- Univ. of Nebraska, Lincoln, NE (United States). Dept. of Physics and Astronomy; Univ. of York (United Kingdom). Dept. of Chemistry
- Stanford PULSE Institute, Menlo Park CA (United States); Univ. Potsdam, Potsdam (Germany). Inst. für Physik und Astronomie
- SLAC National Accelerator Lab., Menlo Park, CA (United States)
- Publication Date:
- Research Org.:
- SLAC National Accelerator Lab., Menlo Park, CA (United States); Univ. of Nebraska, Lincoln, NE (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; Volkswagen Foundation
- OSTI Identifier:
- 1560631
- Alternate Identifier(s):
- OSTI ID: 1546834; OSTI ID: 1671786
- Grant/Contract Number:
- AC02-05-CH11231; AC02-76SF00515; SC0014170; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review A
- Additional Journal Information:
- Journal Volume: 100; Journal Issue: 2; Journal ID: ISSN 2469-9926
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 74 ATOMIC AND MOLECULAR PHYSICS
Citation Formats
Wilkin, Kyle J., Parrish, Robert M., Yang, Jie, Wolf, Thomas J. A., Nunes, J. Pedro F., Guehr, Markus, Li, Renkai, Shen, Xiaozhe, Zheng, Qiang, Wang, Xijie, Martinez, Todd J., and Centurion, Martin. Diffractive imaging of dissociation and ground-state dynamics in a complex molecule. United States: N. p., 2019.
Web. doi:10.1103/physreva.100.023402.
Wilkin, Kyle J., Parrish, Robert M., Yang, Jie, Wolf, Thomas J. A., Nunes, J. Pedro F., Guehr, Markus, Li, Renkai, Shen, Xiaozhe, Zheng, Qiang, Wang, Xijie, Martinez, Todd J., & Centurion, Martin. Diffractive imaging of dissociation and ground-state dynamics in a complex molecule. United States. https://doi.org/10.1103/physreva.100.023402
Wilkin, Kyle J., Parrish, Robert M., Yang, Jie, Wolf, Thomas J. A., Nunes, J. Pedro F., Guehr, Markus, Li, Renkai, Shen, Xiaozhe, Zheng, Qiang, Wang, Xijie, Martinez, Todd J., and Centurion, Martin. Fri .
"Diffractive imaging of dissociation and ground-state dynamics in a complex molecule". United States. https://doi.org/10.1103/physreva.100.023402. https://www.osti.gov/servlets/purl/1560631.
@article{osti_1560631,
title = {Diffractive imaging of dissociation and ground-state dynamics in a complex molecule},
author = {Wilkin, Kyle J. and Parrish, Robert M. and Yang, Jie and Wolf, Thomas J. A. and Nunes, J. Pedro F. and Guehr, Markus and Li, Renkai and Shen, Xiaozhe and Zheng, Qiang and Wang, Xijie and Martinez, Todd J. and Centurion, Martin},
abstractNote = {We have investigated the structural dynamics in photoexcited 1,2-diiodotetrafluoroethane molecules $(C_2F_4I_2)$ in the gas phase experimentally using ultrafast electron diffraction and theoretically using FOMO-CASCI excited-state dynamics simulations. The molecules are excited by an ultraviolet femtosecond laser pulse to a state characterized by a transition from the iodine $5p⊥$ orbital to a mixed $5p ∥ σ$ hole and $CF^∙_2$ antibonding orbital, which results in the cleavage of one of the carbon-iodine bonds. We have observed, with sub-Angstrom resolution, the motion of the nuclear wave packet of the dissociating iodine atom followed by coherent vibrations in the electronic ground state of the $C_2F_4I_2$ radical. The radical reaches a stable classical (nonbridged) structure in less than 200 fs.},
doi = {10.1103/physreva.100.023402},
journal = {Physical Review A},
number = 2,
volume = 100,
place = {United States},
year = {2019},
month = {8}
}
Web of Science
Figures / Tables:

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