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Formative period in the x-ray-induced photodissociation of organic molecules

Kukk, E. ; Fukuzawa, H. ; Niskanen, J. ; Nagaya, K. ; Kooser, K. ; You, D. ; Peschel, J. LU ; Maclot, S. LU ; Niozu, A. and Saito, S. , et al. (2021) In Physical Review Research 3(1).
Abstract
Absorption of x-ray photons by atomic inner shells of light-element organics and biomolecules often leads to formation of dicationic electronic states and to molecular fragmentation. We investigated the x-ray-induced dissociation landscape of a representative medium-sized organic molecule, thiophene, by femtosecond x-ray pulses from the Super Photon Ring-8 GeV (SPring-8) Angstrom Compact Free-Electron Laser (SACLA). Holes, created in the sulfur 2p orbital by photoemission, were filled by the Auger process that created dicationic molecular states within a broad range of internal energies—a starting point particular to x-ray-induced dynamics. The evolution of the ionized molecules was monitored by a pump-probe experiment using... (More)
Absorption of x-ray photons by atomic inner shells of light-element organics and biomolecules often leads to formation of dicationic electronic states and to molecular fragmentation. We investigated the x-ray-induced dissociation landscape of a representative medium-sized organic molecule, thiophene, by femtosecond x-ray pulses from the Super Photon Ring-8 GeV (SPring-8) Angstrom Compact Free-Electron Laser (SACLA). Holes, created in the sulfur 2p orbital by photoemission, were filled by the Auger process that created dicationic molecular states within a broad range of internal energies—a starting point particular to x-ray-induced dynamics. The evolution of the ionized molecules was monitored by a pump-probe experiment using a near-infrared (800 nm) laser pulse. Ion-ion coincidence and ion momentum analysis reveals enhanced yields of ionic fragments from multibody breakup of the ring, attributed to additional ionization of the highly excited fraction of the dicationic parent molecular states. The transient nature of the enhancement and its decay with about a 160-fs time constant indicate formation of an open-ring parent geometry and the statistical survival time of the parent species before the dissociation events. By probing specific Auger final states of transient, highly excited nature by near-infrared light, we demonstrate how pump-probe signatures can be related to the key features in dynamics during the early period of the x-ray-induced damage of organic molecules and biomolecules. (Less)
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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Physical Review Research
volume
3
issue
1
article number
013221
pages
12 pages
publisher
American Physical Society
external identifiers
  • scopus:85112091228
ISSN
2643-1564
DOI
10.1103/PhysRevResearch.3.013221
language
English
LU publication?
yes
id
b4f2970f-922b-48d5-9406-7750562f2d77
date added to LUP
2021-04-02 12:11:10
date last changed
2022-04-27 01:14:57
@article{b4f2970f-922b-48d5-9406-7750562f2d77,
  abstract     = {{Absorption of x-ray photons by atomic inner shells of light-element organics and biomolecules often leads to formation of dicationic electronic states and to molecular fragmentation. We investigated the x-ray-induced dissociation landscape of a representative medium-sized organic molecule, thiophene, by femtosecond x-ray pulses from the Super Photon Ring-8 GeV (SPring-8) Angstrom Compact Free-Electron Laser (SACLA). Holes, created in the sulfur <b>2<i>p</i></b> orbital by photoemission, were filled by the Auger process that created dicationic molecular states within a broad range of internal energies—a starting point particular to x-ray-induced dynamics. The evolution of the ionized molecules was monitored by a pump-probe experiment using a near-infrared (800 nm) laser pulse. Ion-ion coincidence and ion momentum analysis reveals enhanced yields of ionic fragments from multibody breakup of the ring, attributed to additional ionization of the highly excited fraction of the dicationic parent molecular states. The transient nature of the enhancement and its decay with about a 160-fs time constant indicate formation of an open-ring parent geometry and the statistical survival time of the parent species before the dissociation events. By probing specific Auger final states of transient, highly excited nature by near-infrared light, we demonstrate how pump-probe signatures can be related to the key features in dynamics during the early period of the x-ray-induced damage of organic molecules and biomolecules.}},
  author       = {{Kukk, E. and Fukuzawa, H. and Niskanen, J. and Nagaya, K. and Kooser, K. and You, D. and Peschel, J. and Maclot, S. and Niozu, A. and Saito, S. and Luo, Y. and Pelimanni, E. and Itälä, E. and Bozek, J. D. and Takanashi, T and Berholts, M. and Johnsson, P. and Ueda, K.}},
  issn         = {{2643-1564}},
  language     = {{eng}},
  number       = {{1}},
  publisher    = {{American Physical Society}},
  series       = {{Physical Review Research}},
  title        = {{Formative period in the x-ray-induced photodissociation of organic molecules}},
  url          = {{http://dx.doi.org/10.1103/PhysRevResearch.3.013221}},
  doi          = {{10.1103/PhysRevResearch.3.013221}},
  volume       = {{3}},
  year         = {{2021}},
}