Skip to main content

Research Repository

Advanced Search

Steering the outcome of a photochemical reaction - an in silico experiment on the H2CSO sulfine using few-femtosecond dump pulses

Mignolet, Benoit; Curchod, Basile FE

Steering the outcome of a photochemical reaction - an in silico experiment on the H2CSO sulfine using few-femtosecond dump pulses Thumbnail


Authors

Benoit Mignolet



Abstract

We propose a pump-dump control scheme using sub-10 fs pulses to enhance the photochemical formation of the three-membered C–S–O ring oxathiirane from the parent H2CSO sulfine molecule. The ultrashort nature of the pulses is essential to promptly alter the photoinduced dynamics, e.g., while a bond is elongating, which is key to selectively form the oxathiirane by radiative dumping. We carried out an in silico pump-dump experiment with excited-state dynamics simulations that include the interaction with electric field of the pump and dump pulses. By applying the dump pulse when the CS bond is elongating, the population transferred to the ground state will form the oxathiirane with a branching ratio of 4, much higher than the one solely due to nonradiative relaxation (0.66). The overall oxathiirane yield can be increased by up to 17% when the 6 fs IR dump pulse is applied at a delay time of 47 fs.

Citation

Mignolet, B., & Curchod, B. F. (2019). Steering the outcome of a photochemical reaction - an in silico experiment on the H2CSO sulfine using few-femtosecond dump pulses. The Journal of Chemical Physics, 150(10), Article 101101. https://doi.org/10.1063/1.5089124

Journal Article Type Article
Acceptance Date Feb 25, 2019
Online Publication Date Mar 12, 2019
Publication Date Mar 14, 2019
Deposit Date Feb 25, 2019
Publicly Available Date Mar 12, 2020
Journal Journal of Chemical Physics
Print ISSN 0021-9606
Electronic ISSN 1089-7690
Publisher American Institute of Physics
Peer Reviewed Peer Reviewed
Volume 150
Issue 10
Article Number 101101
DOI https://doi.org/10.1063/1.5089124

Files


Accepted Journal Article (1.1 Mb)
PDF

Copyright Statement
© 2019 American Institute of Physics. This article may be downloaded for personal use only. Any other use requires prior permission of the author and the American Institute of Physics. The following article appeared in Mignolet, Benoit & Curchod, Basile F E (2019). Steering the outcome of a photochemical reaction - an in silico experiment on the H2CSO sulfine using few-femtosecond dump pulses. Journal of Chemical Physics and may be found at https://doi.org/10.1063/1.5089124




You might also like



Downloadable Citations