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Title: Single- and multi-photon-induced ultraviolet excitation and photodissociation of CH3I probed by coincident ion momentum imaging

Abstract

The UV-induced photodissociation dynamics of iodomethane (CH3I) in its A-band are investigated by time-resolved coincident ion momentum imaging using strong-field ionization as a probe. The delay-dependent kinetic energy distribution of the photofragments resulting from double ionization of the molecule maps the cleavage of the carbon–iodine bond and shows how the existence of a potential well in the di-cationic potential energy surfaces shapes the observed distribution at small pump–probe delays. Furthermore, the competition between single- and multi-photon excitation and ionization of the molecule is studied as a function of the intensity of the UV-pump laser pulse. Two-photon excitation to Rydberg states is identified by tracking the transformation of the delay-dependent singly-charged iodomethane yield from a pure Gaussian distribution at low intensity to a Gaussian with an exponentially decaying tail at higher intensities. In conclusion, dissociative ionization induced by absorption of three UV photons is resolved as an additional delay-dependent feature in the kinetic energy of the fragment ions detected in coincidence.

Authors:
ORCiD logo [1];  [1]; ORCiD logo [2]; ORCiD logo [3];  [1];  [1];  [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Kansas State Univ., Manhattan, KS (United States)
  2. SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
  3. Kansas State Univ., Manhattan, KS (United States); School of Quantum Technology, Pune (India)
Publication Date:
Research Org.:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); USDOE
OSTI Identifier:
2006863
Alternate Identifier(s):
OSTI ID: 1963331
Grant/Contract Number:  
AC02-76SF00515; FG02-86ER13491
Resource Type:
Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP
Additional Journal Information:
Journal Volume: 25; Journal Issue: 14; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; UV-induced photodissociation; strong-field ionization; Coulomb explosion imaging; coincident ion momentum imaging; femtosecond dynamics

Citation Formats

Ziaee, Farzaneh, Borne, Kurtis, Forbes, Ruaridh, P., Kanaka Raju, Malakar, Yubaraj, Kaderiya, Balram, Severt, Travis, Ben-Itzhak, Itzik, Rudenko, Artem, and Rolles, Daniel. Single- and multi-photon-induced ultraviolet excitation and photodissociation of CH3I probed by coincident ion momentum imaging. United States: N. p., 2023. Web. doi:10.1039/d3cp00498h.
Ziaee, Farzaneh, Borne, Kurtis, Forbes, Ruaridh, P., Kanaka Raju, Malakar, Yubaraj, Kaderiya, Balram, Severt, Travis, Ben-Itzhak, Itzik, Rudenko, Artem, & Rolles, Daniel. Single- and multi-photon-induced ultraviolet excitation and photodissociation of CH3I probed by coincident ion momentum imaging. United States. https://doi.org/10.1039/d3cp00498h
Ziaee, Farzaneh, Borne, Kurtis, Forbes, Ruaridh, P., Kanaka Raju, Malakar, Yubaraj, Kaderiya, Balram, Severt, Travis, Ben-Itzhak, Itzik, Rudenko, Artem, and Rolles, Daniel. Thu . "Single- and multi-photon-induced ultraviolet excitation and photodissociation of CH3I probed by coincident ion momentum imaging". United States. https://doi.org/10.1039/d3cp00498h. https://www.osti.gov/servlets/purl/2006863.
@article{osti_2006863,
title = {Single- and multi-photon-induced ultraviolet excitation and photodissociation of CH3I probed by coincident ion momentum imaging},
author = {Ziaee, Farzaneh and Borne, Kurtis and Forbes, Ruaridh and P., Kanaka Raju and Malakar, Yubaraj and Kaderiya, Balram and Severt, Travis and Ben-Itzhak, Itzik and Rudenko, Artem and Rolles, Daniel},
abstractNote = {The UV-induced photodissociation dynamics of iodomethane (CH3I) in its A-band are investigated by time-resolved coincident ion momentum imaging using strong-field ionization as a probe. The delay-dependent kinetic energy distribution of the photofragments resulting from double ionization of the molecule maps the cleavage of the carbon–iodine bond and shows how the existence of a potential well in the di-cationic potential energy surfaces shapes the observed distribution at small pump–probe delays. Furthermore, the competition between single- and multi-photon excitation and ionization of the molecule is studied as a function of the intensity of the UV-pump laser pulse. Two-photon excitation to Rydberg states is identified by tracking the transformation of the delay-dependent singly-charged iodomethane yield from a pure Gaussian distribution at low intensity to a Gaussian with an exponentially decaying tail at higher intensities. In conclusion, dissociative ionization induced by absorption of three UV photons is resolved as an additional delay-dependent feature in the kinetic energy of the fragment ions detected in coincidence.},
doi = {10.1039/d3cp00498h},
journal = {Physical Chemistry Chemical Physics. PCCP},
number = 14,
volume = 25,
place = {United States},
year = {Thu Mar 16 00:00:00 EDT 2023},
month = {Thu Mar 16 00:00:00 EDT 2023}
}

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