Journal Article PUBDB-2021-03434

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A localized view on molecular dissociation via electron-ion partial covariance

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2022
Macmillan Publishers Limited, part of Springer Nature [London]

Communications chemistry 5(1), 42 () [10.1038/s42004-022-00656-w]
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Abstract: Inner-shell photoelectron spectroscopy provides an element-specific probe of molecular structure, as core-electron binding energies are sensitive to the chemical environment. Short-wavelength femtosecond light sources, such as Free-Electron Lasers (FELs), even enable time-resolved site-specific investigations of molecular photochemistry. Here, we study the ultraviolet photodissociation of chiral (R/S)-1-iodo-2-methylbutane, probed by XUV pulses from the Free-electron LASer in Hamburg (FLASH) through the ultrafast evolution of the iodine 4d binding energy. Methodologically, we introduce electron-ion partial covariance imaging as a technique to isolate otherwise elusive features in a two-dimensional photoelectron spectrum arising from different photofragmentation pathways. The experimental and theoretical results for the time-resolved electron spectra of the 4d$_{3/2}$ and 4d$_{5/2}$ atomic and molecular levels that are disentangled by this method provide a key step towards studying structural and chemical changes from a specific spectator site. We thus pave the way for approaching femto-stereochemistry with FELs.

Classification:

Contributing Institute(s):
  1. FLASH Photonen-Diagnose und Steuerungen (FS-FLASH-D)
  2. FS-CFEL-3 (CFEL-DESYT)
  3. FLASH Wissenschaftlicher Nutzerbetrieb (FS-FLASH-O)
  4. Experimentebetreuung FLASH (FS-FL)
  5. DOOR-User (DOOR ; HAS-User)
  6. Biomoleküle in Gasphase (FS-BIG)
  7. CFEL-Theory (FS-CFEL-3)
  8. Laser Forschung und Entwicklung (FS-LA)
Research Program(s):
  1. 631 - Matter – Dynamics, Mechanisms and Control (POF4-631) (POF4-631)
  2. 6G2 - FLASH (DESY) (POF4-6G2) (POF4-6G2)
  3. FS-Proposal: F-20171078 (F-20171078) (F-20171078)
  4. DFG project 328961117 - SFB 1319: Extremes Licht zur Analyse und Kontrolle molekularer Chiralität (ELCH) (328961117) (328961117)
  5. SFB 755 B03 - Untersuchung ultraschneller Dynamik chemischer Reaktionen mit Femtosekunden-Röntgenpulsen (B03) (50499717) (50499717)
  6. VH-NG-1104 - Structure and dynamics of gas-phase biomolecules studied by photon-induced ionization and dissociation (2007_IVF-VH-NG-1104) (2007_IVF-VH-NG-1104)
Experiment(s):
  1. FLASH Beamline BL1 (FLASH)

Appears in the scientific report 2022
Database coverage:
Medline ; Creative Commons Attribution CC BY 4.0 ; DOAJ ; OpenAccess ; Article Processing Charges ; Clarivate Analytics Master Journal List ; Current Contents - Physical, Chemical and Earth Sciences ; DOAJ Seal ; Essential Science Indicators ; Fees ; IF < 5 ; IF >= 5 ; JCR ; SCOPUS ; Science Citation Index Expanded ; Web of Science Core Collection
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The record appears in these collections:
Private Collections > >CFEL > >FS-CFEL > CFEL-DESYT
Private Collections > >Extern > >HAS-User > HAS-User
Private Collections > >DESY > >FS > FS-FLASH-D
Private Collections > >DESY > >FS > FS-FLASH-O
Private Collections > >DESY > >FS > FS-CFEL-3
Private Collections > >DESY > >FS > FS-BIG
Private Collections > >DESY > >FS > FS-LA
Private Collections > >DESY > >FS > FS-FL
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 Record created 2021-08-19, last modified 2025-07-15


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