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

Rebholz, Marc; Ding, Thomas; Despré, Victor; Aufleger, Lennart; Hartmann, Maximilian; Meyer, Kristina; Stooß, Veit; Magunia, Alexander; Wachs, David; Birk, Paul; Mi, Yonghao; Borisova, Gergana Dimitrova; Castanheira, Carina da Costa; Rupprecht, Patrick; Schmid, Georg; Schnorr, Kirsten; Schröter, Claus Dieter; Moshammer, Robert; Loh, Zhi-Heng; Attar, Andrew R.; Leone, Stephen R.; Gaumnitz, Thomas; Wörner, Hans Jakob; Roling, Sebastian; Butz, Marco; Zacharias, Helmut; Düsterer, Stefan; Treusch, Rolf; Brenner, Günter; Vester, Jonas; Kuleff, Alexander I.; Ott, Christian; Pfeifer, Thomas

doi:10.1103/PhysRevX.11.031001

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

Journal Article · Thu Jul 01 00:00:00 EDT 2021 · Physical Review. X

DOI:https://doi.org/10.1103/PhysRevX.11.031001· OSTI ID:1804940

;

; Meyer, Kristina;

; Magunia, Alexander; Wachs, David;

;

; Castanheira, Carina da Costa; Rupprecht, Patrick; Schmid, Georg;

; Schröter, Claus Dieter; Moshammer, Robert;

; Attar, Andrew R. more »

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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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; European Research Council (ERC); Ministry of Education, Singapore; German Research Foundation (DFG); National Science Foundation (NSF); German Federal Ministry of Education and Research (BMBF)

Grant/Contract Number:: AC02-05CH11231; X-MuSiC-616783; RG105/17; RG1/20; CHE-1660417; 05K13PM2

OSTI ID:: 1804940

Alternate ID(s):: OSTI ID: 1813423; OSTI ID: 1814507

Journal Information:: Physical Review. X, Journal Name: Physical Review. X Vol. 11 Journal Issue: 3; ISSN 2160-3308

Publisher:: American Physical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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