TY - JOUR
T1 - All-XUV Pump-Probe Transient Absorption Spectroscopy of the Structural Molecular Dynamics of Di-iodomethane
AU - Rebholz, Marc
AU - Ding, Thomas
AU - Despré, Victor
AU - Aufleger, Lennart
AU - Hartmann, Maximilian
AU - Meyer, Kristina
AU - Stooß, Veit
AU - Magunia, Alexander
AU - Wachs, David
AU - Birk, Paul
AU - Mi, Yonghao
AU - Borisova, Gergana Dimitrova
AU - Castanheira, Carina Da Costa
AU - Rupprecht, Patrick
AU - Schmid, Georg
AU - Schnorr, Kirsten
AU - Schröter, Claus Dieter
AU - Moshammer, Robert
AU - Loh, Zhi Heng
AU - Attar, Andrew R.
AU - Leone, Stephen R.
AU - Gaumnitz, Thomas
AU - Wörner, Hans Jakob
AU - Roling, Sebastian
AU - Butz, Marco
AU - Zacharias, Helmut
AU - Düsterer, Stefan
AU - Treusch, Rolf
AU - Brenner, Günter
AU - Vester, Jonas
AU - Kuleff, Alexander I.
AU - Ott, Christian
AU - Pfeifer, Thomas
N1 - Publisher Copyright:
© 2021 authors. Published by the American Physical Society. Published by the American Physical Society under the terms of the "https://creativecommons.org/licenses/by/4.0/"Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI. Open access publication funded by the Max Planck Society.
PY - 2021/9
Y1 - 2021/9
N2 - In this work, we use an extreme-ultraviolet (XUV) free-electron laser (FEL) to resonantly excite the I: 4d5/2-σ∗ transition of a gas-phase di-iodomethane (CH2I2) target. This site-specific excitation generates a 4d 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: 4d 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.
AB - In this work, we use an extreme-ultraviolet (XUV) free-electron laser (FEL) to resonantly excite the I: 4d5/2-σ∗ transition of a gas-phase di-iodomethane (CH2I2) target. This site-specific excitation generates a 4d 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: 4d 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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U2 - 10.1103/PhysRevX.11.031001
DO - 10.1103/PhysRevX.11.031001
M3 - Article
AN - SCOPUS:85110547820
SN - 2160-3308
VL - 11
JO - Physical Review X
JF - Physical Review X
IS - 3
M1 - 031001
ER -