Journal Article PUBDB-2021-02850

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All-XUV Pump-Probe Transient Absorption Spectroscopy of the Structural Molecular Dynamics of Di-iodomethane

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2021
APS College Park, Md.

Physical review / X 11(3), 031001 (1-9) () [10.1103/PhysRevX.11.031001]
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Abstract: In this work, we use an extreme-ultraviolet (XUV) free-electron laser (FEL) to resonantly excite the I: 4$d_{5/2}–σ^∗$ transition of a gas-phase di-iodomethane (CH$_2$I$_2$) target. This site-specific excitation generates a 4$d$ core hole located at an iodine site, which leaves the molecule in a well-defined excited state. We subsequently measure the time-dependent absorption change of the molecule with the FEL probe spectrum centered on the same I: 4$_d$ resonance. Using ab initio calculations of absorption spectra of a transient isomerization pathway observed in earlier studies, our time-resolved measurements allow us to assign the timescales of the previously reported direct and indirect dissociation pathways. The presented method is thus sensitive to excited-state molecular geometries in a time-resolved manner, following a core-resonant site-specific trigger.

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Contributing Institute(s):
  1. DOOR-User (DOOR ; HAS-User)
  2. FLASH Wissenschaftlicher Nutzerbetrieb (FS-FLASH-O)
  3. FLASH Photonen-Strahlführungen und Optiken (FS-FLASH-B)
  4. FLASH Photonen-Diagnose und Steuerungen (FS-FLASH-D)
Research Program(s):
  1. 631 - Matter – Dynamics, Mechanisms and Control (POF4-631) (POF4-631)
  2. 6G2 - FLASH (DESY) (POF4-6G2) (POF4-6G2)
Experiment(s):
  1. FLASH Beamline BL2 (FLASH)

Appears in the scientific report 2021
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 Record created 2021-07-01, last modified 2025-07-16


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