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Imaging multiphoton ionization dynamics of CH3I at a high repetition rate XUV free-electron laser

Cheng, Yu Chen LU orcid ; Oostenrijk, Bart LU ; Lahl, Jan LU ; MacLot, Sylvain LU ; Augustin, Sven ; Schmid, Georg ; Schnorr, Kirsten ; Meister, Severin ; Rompotis, Dimitrios and Manschwetus, Bastian LU , et al. (2020) In Journal of Physics B: Atomic, Molecular and Optical Physics 54(1).
Abstract

XUV multiphoton ionization of molecules is commonly used in free-electron laser experiments to study charge transfer dynamics. However, molecular dissociation and electron dynamics, such as multiple photon absorption, Auger decay, and charge transfer, often happen on competing time scales, and the contributions of individual processes can be difficult to unravel. We experimentally investigate the Coulomb explosion dynamics of methyl iodide upon core-hole ionization of the shallow inner-shell of iodine (4d) and classically simulate the fragmentation by phenomenologically introducing ionization dynamics and charge transfer. Under our experimental conditions with medium fluence and relatively long XUV pulses (∼75 fs), we find that fast... (More)

XUV multiphoton ionization of molecules is commonly used in free-electron laser experiments to study charge transfer dynamics. However, molecular dissociation and electron dynamics, such as multiple photon absorption, Auger decay, and charge transfer, often happen on competing time scales, and the contributions of individual processes can be difficult to unravel. We experimentally investigate the Coulomb explosion dynamics of methyl iodide upon core-hole ionization of the shallow inner-shell of iodine (4d) and classically simulate the fragmentation by phenomenologically introducing ionization dynamics and charge transfer. Under our experimental conditions with medium fluence and relatively long XUV pulses (∼75 fs), we find that fast Auger decay prior to charge transfer significantly contributes to the charging mechanism, leading to a yield enhancement of higher carbon charge states upon molecular dissociation. Furthermore, we argue for the existence of another charging mechanism for the weak fragmentation channels leading to triply charged carbon atoms. This study shows that classical simulations can be a useful tool to guide the quantum mechanical description of the femtosecond dynamics upon multiphoton absorption in molecular systems.

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organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
Auger decay, charge transfer, methyl iodide dissociation, recoil-ion momentum spectroscopy, sequential ionization
in
Journal of Physics B: Atomic, Molecular and Optical Physics
volume
54
issue
1
article number
014001
publisher
IOP Publishing
external identifiers
  • scopus:85098881073
ISSN
0953-4075
DOI
10.1088/1361-6455/abc6bc
language
English
LU publication?
yes
id
412a2b4f-1e87-40f5-804e-f1e3675b6e31
date added to LUP
2021-01-15 12:20:42
date last changed
2023-11-20 21:16:35
@article{412a2b4f-1e87-40f5-804e-f1e3675b6e31,
  abstract     = {{<p>XUV multiphoton ionization of molecules is commonly used in free-electron laser experiments to study charge transfer dynamics. However, molecular dissociation and electron dynamics, such as multiple photon absorption, Auger decay, and charge transfer, often happen on competing time scales, and the contributions of individual processes can be difficult to unravel. We experimentally investigate the Coulomb explosion dynamics of methyl iodide upon core-hole ionization of the shallow inner-shell of iodine (4d) and classically simulate the fragmentation by phenomenologically introducing ionization dynamics and charge transfer. Under our experimental conditions with medium fluence and relatively long XUV pulses (∼75 fs), we find that fast Auger decay prior to charge transfer significantly contributes to the charging mechanism, leading to a yield enhancement of higher carbon charge states upon molecular dissociation. Furthermore, we argue for the existence of another charging mechanism for the weak fragmentation channels leading to triply charged carbon atoms. This study shows that classical simulations can be a useful tool to guide the quantum mechanical description of the femtosecond dynamics upon multiphoton absorption in molecular systems.</p>}},
  author       = {{Cheng, Yu Chen and Oostenrijk, Bart and Lahl, Jan and MacLot, Sylvain and Augustin, Sven and Schmid, Georg and Schnorr, Kirsten and Meister, Severin and Rompotis, Dimitrios and Manschwetus, Bastian and Redlin, Harald and Bomme, Cédric and Erk, Benjamin and Rolles, Daniel and Boll, Rebecca and Olshin, Pavel and Rudenko, Artem and Meyer, Michael and Johnsson, Per and Moshammer, Robert and Gisselbrecht, Mathieu}},
  issn         = {{0953-4075}},
  keywords     = {{Auger decay; charge transfer; methyl iodide dissociation; recoil-ion momentum spectroscopy; sequential ionization}},
  language     = {{eng}},
  number       = {{1}},
  publisher    = {{IOP Publishing}},
  series       = {{Journal of Physics B: Atomic, Molecular and Optical Physics}},
  title        = {{Imaging multiphoton ionization dynamics of CH<sub>3</sub>I at a high repetition rate XUV free-electron laser}},
  url          = {{http://dx.doi.org/10.1088/1361-6455/abc6bc}},
  doi          = {{10.1088/1361-6455/abc6bc}},
  volume       = {{54}},
  year         = {{2020}},
}