All-XUV Pump-Probe Transient Absorption Spectroscopy of the Structural Molecular Dynamics of Di-iodomethane
In this work, we use an extreme-ultraviolet (XUV) free-electron laser (FEL) to resonantly excite the I: 4d_{5/2}–σ^{*} transition of a gas-phase di-iodomethane (CH_{2}I_{2}) target. This site-specific excitation generates a 4d core hole located at an iodine site, which leaves the molecule in a well-...
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American Physical Society
2021
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oai:doaj.org-article:64b424a18119400eb2c7746afff63f502021-12-02T17:09:54ZAll-XUV Pump-Probe Transient Absorption Spectroscopy of the Structural Molecular Dynamics of Di-iodomethane10.1103/PhysRevX.11.0310012160-3308https://doaj.org/article/64b424a18119400eb2c7746afff63f502021-07-01T00:00:00Zhttp://doi.org/10.1103/PhysRevX.11.031001http://doi.org/10.1103/PhysRevX.11.031001https://doaj.org/toc/2160-3308In this work, we use an extreme-ultraviolet (XUV) free-electron laser (FEL) to resonantly excite the I: 4d_{5/2}–σ^{*} transition of a gas-phase di-iodomethane (CH_{2}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 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.Marc RebholzThomas DingVictor DespréLennart AuflegerMaximilian HartmannKristina MeyerVeit StooßAlexander MaguniaDavid WachsPaul BirkYonghao MiGergana Dimitrova BorisovaCarina da Costa CastanheiraPatrick RupprechtGeorg SchmidKirsten SchnorrClaus Dieter SchröterRobert MoshammerZhi-Heng LohAndrew R. AttarStephen R. LeoneThomas GaumnitzHans Jakob WörnerSebastian RolingMarco ButzHelmut ZachariasStefan DüstererRolf TreuschGünter BrennerJonas VesterAlexander I. KuleffChristian OttThomas PfeiferAmerican Physical SocietyarticlePhysicsQC1-999ENPhysical Review X, Vol 11, Iss 3, p 031001 (2021) |
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DOAJ |
| language |
EN |
| topic |
Physics QC1-999 |
| spellingShingle |
Physics QC1-999 Marc Rebholz Thomas Ding Victor Despré Lennart Aufleger Maximilian Hartmann Kristina Meyer Veit Stooß Alexander Magunia David Wachs Paul Birk Yonghao Mi Gergana Dimitrova Borisova Carina da Costa Castanheira Patrick Rupprecht Georg Schmid Kirsten Schnorr Claus Dieter Schröter Robert Moshammer Zhi-Heng Loh Andrew R. Attar Stephen R. Leone Thomas Gaumnitz Hans Jakob Wörner Sebastian Roling Marco Butz Helmut Zacharias Stefan Düsterer Rolf Treusch Günter Brenner Jonas Vester Alexander I. Kuleff Christian Ott Thomas Pfeifer All-XUV Pump-Probe Transient Absorption Spectroscopy of the Structural Molecular Dynamics of Di-iodomethane |
| description |
In this work, we use an extreme-ultraviolet (XUV) free-electron laser (FEL) to resonantly excite the I: 4d_{5/2}–σ^{*} transition of a gas-phase di-iodomethane (CH_{2}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 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. |
| format |
article |
| author |
Marc Rebholz Thomas Ding Victor Despré Lennart Aufleger Maximilian Hartmann Kristina Meyer Veit Stooß Alexander Magunia David Wachs Paul Birk Yonghao Mi Gergana Dimitrova Borisova Carina da Costa Castanheira Patrick Rupprecht Georg Schmid Kirsten Schnorr Claus Dieter Schröter Robert Moshammer Zhi-Heng Loh Andrew R. Attar Stephen R. Leone Thomas Gaumnitz Hans Jakob Wörner Sebastian Roling Marco Butz Helmut Zacharias Stefan Düsterer Rolf Treusch Günter Brenner Jonas Vester Alexander I. Kuleff Christian Ott Thomas Pfeifer |
| author_facet |
Marc Rebholz Thomas Ding Victor Despré Lennart Aufleger Maximilian Hartmann Kristina Meyer Veit Stooß Alexander Magunia David Wachs Paul Birk Yonghao Mi Gergana Dimitrova Borisova Carina da Costa Castanheira Patrick Rupprecht Georg Schmid Kirsten Schnorr Claus Dieter Schröter Robert Moshammer Zhi-Heng Loh Andrew R. Attar Stephen R. Leone Thomas Gaumnitz Hans Jakob Wörner Sebastian Roling Marco Butz Helmut Zacharias Stefan Düsterer Rolf Treusch Günter Brenner Jonas Vester Alexander I. Kuleff Christian Ott Thomas Pfeifer |
| author_sort |
Marc Rebholz |
| title |
All-XUV Pump-Probe Transient Absorption Spectroscopy of the Structural Molecular Dynamics of Di-iodomethane |
| title_short |
All-XUV Pump-Probe Transient Absorption Spectroscopy of the Structural Molecular Dynamics of Di-iodomethane |
| title_full |
All-XUV Pump-Probe Transient Absorption Spectroscopy of the Structural Molecular Dynamics of Di-iodomethane |
| title_fullStr |
All-XUV Pump-Probe Transient Absorption Spectroscopy of the Structural Molecular Dynamics of Di-iodomethane |
| title_full_unstemmed |
All-XUV Pump-Probe Transient Absorption Spectroscopy of the Structural Molecular Dynamics of Di-iodomethane |
| title_sort |
all-xuv pump-probe transient absorption spectroscopy of the structural molecular dynamics of di-iodomethane |
| publisher |
American Physical Society |
| publishDate |
2021 |
| url |
https://doaj.org/article/64b424a18119400eb2c7746afff63f50 |
| work_keys_str_mv |
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| _version_ |
1718381500667265024 |