Please use this identifier to cite or link to this item: http://dx.doi.org/10.14279/depositonce-14801
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Main Title: Real-time observation of photoionization-induced water migration dynamics in 4-methylformanilide–water by picosecond time-resolved infrared spectroscopy and ab initio molecular dynamics simulations
Author(s): Miyazaki, Mitsuhiko
Kamiya, Tairiku
Wohlgemuth, Matthias
Chatterjee, Kuntal
Mitrić, Roland
Dopfer, Otto
Fujii, Masaaki
Type: Article
URI: https://depositonce.tu-berlin.de/handle/11303/16027
http://dx.doi.org/10.14279/depositonce-14801
License: https://creativecommons.org/licenses/by/3.0/
Abstract: A novel time-resolved pump-probe spectroscopic approach that enables to keep high resolution in both the time and energy domain, nanosecond excitation-picosecond ionization-picosecond infrared probe (ns-ps-ps TRIR) spectroscopy, has been applied to the trans-4-methylformanilide-water (4MetFA-W) cluster. Water migration dynamics from the CO to the NH binding site in a peptide linkage triggered by photoionization of 4MetFA-W is directly monitored by the ps time evolution of IR spectra, and the presence of an intermediate state is revealed. The time evolution is analyzed by rate equations based on a four-state model of the migration dynamics. Time constants for the initial to the intermediate and hot product and to the final product are obtained. The acceleration of the dynamics by methyl substitution and the strong contribution of intracluster vibrational energy redistribution in the termination of the solvation dynamics is suggested. This picture is well confirmed by the ab initio on-the-fly molecular dynamics simulations. Vibrational assignments of 4MetFA and 4MetFA-W in the neutral (S-0 and S-1) and ionic (D-0) electronic states measured by ns IR dip and electron-impact IR photodissociation spectroscopy are also discussed prior to the results of time-resolved spectroscopy.
Subject(s): water migration
spectroscopy
trans-4MeFA
4MeFA–W
Issue Date: 1-Oct-2021
Date Available: 30-Dec-2021
Language Code: en
DDC Class: 530 Physik
Sponsor/Funder: TU Berlin, Open-Access-Mittel – 2021
Journal Title: Physical Chemistry Chemical Physics
Publisher: Royal Society of Chemistry (RSC)
Volume: 24
Issue: 1
Publisher DOI: 10.1039/d1cp03327a
Page Start: 73
Page End: 85
EISSN: 1463-9084
ISSN: 1463-9076
TU Affiliation(s): Fak. 2 Mathematik und Naturwissenschaften » Inst. Optik und Atomare Physik » FG Lasermolekülspektroskopie und Umweltphysik
Appears in Collections:Technische Universität Berlin » Publications

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