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A localized view on molecular dissociation via electron-ion partial covariance
Allum, F. (Corresponding author)Extern* ; Music, V. ; Inhester, L. (Corresponding author)CFEL*Extern*XFEL.EU*DESY* ; Boll, R.XFEL.EU* ; Erk, B.XFEL.EU*DESY* ; Schmidt, P. ; Baumann, T. M.XFEL.EU* ; Brenner, G.DESY* ; Burt, M. ; Demekhin, P. V. ; Dörner, S.Extern*XFEL.EU* ; Ehresmann, A. ; Galler, A.XFEL.EU* ; Grychtol, P.XFEL.EU* ; Heathcote, D. ; Kargin, D. ; Larsson, M.Extern* ; Lee, J. W. L. ; Li, Z. ; Manschwetus, B.Extern*DESY* ; Marder, L. ; Mason, R.Extern* ; Meyer, M. ; Otto, H.Extern* ; Passow, C.XFEL.EU*DESY* ; Pietschnig, R. ; Ramm, D.DESY* ; Schubert, K.XFEL.EU*DESY* ; Schwob, L.XFEL.EU*DESY* ; Thomas, R. D. ; Vallance, C. ; Vidanović, I.Extern* ; von Korff Schmising, C.Extern* ; Wagner, R.XFEL.EU* ; Walter, P. ; Zhaunerchyk, V.Extern*EMBL* ; Rolles, D.Extern* ; Bari, S.DESY* ; Brouard, M. ; Ilchen, M. (Corresponding author)XFEL.EU*DESY*
2022
Macmillan Publishers Limited, part of Springer Nature
[London]
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Please use a persistent id in citations: doi:10.1038/s42004-022-00656-w doi:10.3204/PUBDB-2021-03434
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.
Contributing Institute(s):
- FLASH Photonen-Diagnose und Steuerungen (FS-FLASH-D)
- FS-CFEL-3 (CFEL-DESYT)
- FLASH Wissenschaftlicher Nutzerbetrieb (FS-FLASH-O)
- Experimentebetreuung FLASH (FS-FL)
- DOOR-User (DOOR ; HAS-User)
- Biomoleküle in Gasphase (FS-BIG)
- CFEL-Theory (FS-CFEL-3)
- Laser Forschung und Entwicklung (FS-LA)
Research Program(s):
- 631 - Matter – Dynamics, Mechanisms and Control (POF4-631) (POF4-631)
- 6G2 - FLASH (DESY) (POF4-6G2) (POF4-6G2)
- FS-Proposal: F-20171078 (F-20171078) (F-20171078)
- DFG project 328961117 - SFB 1319: Extremes Licht zur Analyse und Kontrolle molekularer Chiralität (ELCH) (328961117) (328961117)
- SFB 755 B03 - Untersuchung ultraschneller Dynamik chemischer Reaktionen mit Femtosekunden-Röntgenpulsen (B03) (50499717) (50499717)
- 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):
- FLASH Beamline BL1 (FLASH)
Appears in the scientific report
2022
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