Energy-dependent timescales in the dissociation of diiodothiophene dication
(2023) In Physical Chemistry Chemical Physics 25(7). p.5795-5807- Abstract
Photodissociation molecular dynamics of gas-phase 2,5-diiodothiophene molecules was studied in an electron-energy-resolved electron-multi-ion coincidence experiment performed at the FinEstBeAMS beamline of MAX IV synchrotron. Following the photoionization of the iodine 4d subshell and the Auger decay, the dissociation landscape of the molecular dication was investigated as a function of the Auger electron energy. Concentrating on an major dissociation pathway, C4H2I2S2+ → C4H2S+ + I+ + I, and accessing the timescales of the process via ion momentum correlation analysis, it was revealed how this three-body process changes depending on the available internal energy. Using a generalized secondary dissociation model, the process was shown... (More)
Photodissociation molecular dynamics of gas-phase 2,5-diiodothiophene molecules was studied in an electron-energy-resolved electron-multi-ion coincidence experiment performed at the FinEstBeAMS beamline of MAX IV synchrotron. Following the photoionization of the iodine 4d subshell and the Auger decay, the dissociation landscape of the molecular dication was investigated as a function of the Auger electron energy. Concentrating on an major dissociation pathway, C4H2I2S2+ → C4H2S+ + I+ + I, and accessing the timescales of the process via ion momentum correlation analysis, it was revealed how this three-body process changes depending on the available internal energy. Using a generalized secondary dissociation model, the process was shown to evolve from secondary dissociation regime towards concerted dissociation as the available energy increased, with the secondary dissociation time constant changing from 1.5 ps to 129 fs. The experimental results were compared with simulations using a stochastic charge-hopping molecular mechanics model. It represented the observed trend and also gave a fair quantitative agreement with the experiment.
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- author
- Kukk, Edwin ; Pihlava, Lassi ; Kooser, Kuno ; Stråhlman, Christian LU ; MacLot, Sylvain LU and Kivimäki, Antti LU
- organization
- publishing date
- 2023
- type
- Contribution to journal
- publication status
- published
- subject
- in
- Physical Chemistry Chemical Physics
- volume
- 25
- issue
- 7
- pages
- 13 pages
- publisher
- Royal Society of Chemistry
- external identifiers
-
- pmid:36744651
- scopus:85148250482
- ISSN
- 1463-9076
- DOI
- 10.1039/d2cp05309h
- language
- English
- LU publication?
- yes
- id
- 3c1b1371-9204-4a35-a4e9-bde2905a363a
- date added to LUP
- 2023-03-03 15:14:13
- date last changed
- 2024-04-18 19:19:40
@article{3c1b1371-9204-4a35-a4e9-bde2905a363a, abstract = {{<p>Photodissociation molecular dynamics of gas-phase 2,5-diiodothiophene molecules was studied in an electron-energy-resolved electron-multi-ion coincidence experiment performed at the FinEstBeAMS beamline of MAX IV synchrotron. Following the photoionization of the iodine 4d subshell and the Auger decay, the dissociation landscape of the molecular dication was investigated as a function of the Auger electron energy. Concentrating on an major dissociation pathway, C4H2I2S2+ → C4H2S+ + I+ + I, and accessing the timescales of the process via ion momentum correlation analysis, it was revealed how this three-body process changes depending on the available internal energy. Using a generalized secondary dissociation model, the process was shown to evolve from secondary dissociation regime towards concerted dissociation as the available energy increased, with the secondary dissociation time constant changing from 1.5 ps to 129 fs. The experimental results were compared with simulations using a stochastic charge-hopping molecular mechanics model. It represented the observed trend and also gave a fair quantitative agreement with the experiment.</p>}}, author = {{Kukk, Edwin and Pihlava, Lassi and Kooser, Kuno and Stråhlman, Christian and MacLot, Sylvain and Kivimäki, Antti}}, issn = {{1463-9076}}, language = {{eng}}, number = {{7}}, pages = {{5795--5807}}, publisher = {{Royal Society of Chemistry}}, series = {{Physical Chemistry Chemical Physics}}, title = {{Energy-dependent timescales in the dissociation of diiodothiophene dication}}, url = {{http://dx.doi.org/10.1039/d2cp05309h}}, doi = {{10.1039/d2cp05309h}}, volume = {{25}}, year = {{2023}}, }