Time-resolving state-specific molecular dissociation with XUV broadband absorption spectroscopy

The electronic and nuclear dynamics inside molecules are essential for chemical reactions, where different pathways typically unfold on ultrafast timescales. Extreme ultraviolet (XUV) light pulses generated by free-electron lasers (FELs) allow atomic-site and electronic-state selectivity, triggering...

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Hauptverfasser: Magunia, Alexander (VerfasserIn) , Rebholz, Marc (VerfasserIn) , Appi, Elisa (VerfasserIn) , Papadopoulou, Christina C. (VerfasserIn) , Lindenblatt, Hannes (VerfasserIn) , Trost, Florian (VerfasserIn) , Meister, Severin (VerfasserIn) , Ding, Thomas (VerfasserIn) , Straub, Michael (VerfasserIn) , Borisova, Gergana D. (VerfasserIn) , Lee, Junhee (VerfasserIn) , Jin, Rui (VerfasserIn) , von der Dellen, Alexander (VerfasserIn) , Kaiser, Christian (VerfasserIn) , Braune, Markus (VerfasserIn) , Düsterer, Stefan (VerfasserIn) , Ališauskas, Skirmantas (VerfasserIn) , Lang, Tino (VerfasserIn) , Heyl, Christoph (VerfasserIn) , Manschwetus, Bastian (VerfasserIn) , Grunewald, Sören (VerfasserIn) , Frühling, Ulrike (VerfasserIn) , Tajalli, Ayhan (VerfasserIn) , Wahid, Ammar Bin (VerfasserIn) , Silletti, Laura (VerfasserIn) , Calegari, Francesca (VerfasserIn) , Mosel, Philip (VerfasserIn) , Morgner, Uwe (VerfasserIn) , Kovacev, Milutin (VerfasserIn) , Thumm, Uwe (VerfasserIn) , Hartl, Ingmar (VerfasserIn) , Treusch, Rolf (VerfasserIn) , Moshammer, Robert (VerfasserIn) , Ott, Christian (VerfasserIn) , Pfeifer, Thomas (VerfasserIn)
Dokumenttyp: Article (Journal)
Sprache:Englisch
Veröffentlicht: Nov 2023
In: Science advances
Year: 2023, Jahrgang: 9, Heft: 47, Pages: 1-7
ISSN:2375-2548
DOI:10.1126/sciadv.adk1482
Online-Zugang:Verlag, kostenfrei, Volltext: https://doi.org/10.1126/sciadv.adk1482
Verlag, kostenfrei, Volltext: https://www.science.org/doi/10.1126/sciadv.adk1482
Volltext
Verfasserangaben:Alexander Magunia, Marc Rebholz, Elisa Appi, Christina C. Papadopoulou, Hannes Lindenblatt, Florian Trost, Severin Meister, Thomas Ding, Michael Straub, Gergana D. Borisova, Junhee Lee, Rui Jin, Alexander von der Dellen, Christian Kaiser, Markus Braune, Stefan Düsterer, Skirmantas Ališauskas, Tino Lang, Christoph Heyl, Bastian Manschwetus, Sören Grunewald, Ulrike Frühling, Ayhan Tajalli, Ammar Bin Wahid, Laura Silletti, Francesca Calegari, Philip Mosel, Uwe Morgner, Milutin Kovacev, Uwe Thumm, Ingmar Hartl, Rolf Treusch, Robert Moshammer, Christian Ott, Thomas Pfeifer

MARC

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520 |a The electronic and nuclear dynamics inside molecules are essential for chemical reactions, where different pathways typically unfold on ultrafast timescales. Extreme ultraviolet (XUV) light pulses generated by free-electron lasers (FELs) allow atomic-site and electronic-state selectivity, triggering specific molecular dynamics while providing femtosecond resolution. Yet, time-resolved experiments are either blind to neutral fragments or limited by the spectral bandwidth of FEL pulses. Here, we combine a broadband XUV probe pulse from high-order harmonic generation with an FEL pump pulse to observe dissociation pathways leading to fragments in different quantum states. We temporally resolve the dissociation of a specific O2+ state into two competing channels by measuring the resonances of ionic and neutral fragments. This scheme can be applied to investigate convoluted dynamics in larger molecules relevant to diverse science fields. 
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