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

Abstract

In this work, we use an extreme-ultraviolet (XUV) free-electron laser (FEL) to resonantly excite the $\mathrm{I}:4d_{5/2}–{\sigma }^{*}$ transition of a gas-phase di-iodomethane ( ${\mathrm{CH}}_2{\mathrm{I}}_2$) 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 $\mathrm{I}:4d$ 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.

Authors:

Rebholz, Marc ;

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• Search DOE PAGES for ORCID "0000-0002-0035-1412"

Ding, Thomas ;

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• Search DOE PAGES for ORCID "0000-0002-2543-0563"

Despré, Victor ;

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• Search DOE PAGES for ORCID "0000-0001-7364-5625"

Aufleger, Lennart ;

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• Search DOE PAGES for ORCID "0000-0003-4903-3981"

Hartmann, Maximilian ;

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• Search DOE PAGES for ORCID "0000-0002-6494-9368"

Meyer, Kristina; Stooß, Veit ;

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• Search DOE PAGES for ORCID "0000-0003-3165-2741"

Magunia, Alexander; Wachs, David; Birk, Paul ;

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• Search DOE PAGES for ORCID "0000-0002-1405-5155"

Mi, Yonghao ;

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Borisova, Gergana Dimitrova ;

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• Search DOE PAGES for ORCID "0000-0003-3558-3093"

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

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• Search DOE PAGES for ORCID "0000-0002-5519-440X"

Schröter, Claus Dieter; Moshammer, Robert; Loh, Zhi-Heng ;

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• Search DOE PAGES for ORCID "0000-0001-9729-9632"

Attar, Andrew R. more »; Leone, Stephen R. ;

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• Search DOE PAGES for ORCID "0000-0003-1819-1338"

Gaumnitz, Thomas ;

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• Search DOE PAGES for ORCID "0000-0003-2341-7805"

Wörner, Hans Jakob ;

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• Search DOE PAGES for ORCID "0000-0002-8877-0872"

Roling, Sebastian; Butz, Marco; Zacharias, Helmut ;

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• Search DOE PAGES for ORCID "0000-0001-9807-1103"

Düsterer, Stefan ;

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• Search DOE PAGES for ORCID "0000-0003-4379-1327"

Treusch, Rolf ;

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• Search DOE PAGES for ORCID "0000-0001-8479-8862"

Brenner, Günter ;

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• Search DOE PAGES for ORCID "0000-0002-1755-876X"

Vester, Jonas; Kuleff, Alexander I. ;

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• Search DOE PAGES for ORCID "0000-0003-2583-4370"

Ott, Christian ;

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• Search DOE PAGES for ORCID "0000-0003-4110-0916"

Pfeifer, Thomas

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• Search DOE PAGES for ORCID "0000-0002-5312-3747"

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Publication Date:

Thu Jul 01 00:00:00 EDT 2021

Research Org.:

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

Sponsoring Org.:

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)

OSTI Identifier:

1804940

Alternate Identifier(s):

OSTI ID: 1813423; OSTI ID: 1814507

Grant/Contract Number:  

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

Resource Type:

Published Article

Journal Name:

Physical Review. X

Additional Journal Information:

Journal Name: Physical Review. X Journal Volume: 11 Journal Issue: 3; Journal ID: ISSN 2160-3308

Publisher:

American Physical Society

Country of Publication:

United States

Language:

English

Subject:

photodissociation; molecules; transient absorption spectroscopy; 74 ATOMIC AND MOLECULAR PHYSICS