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

verfasst von

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

Abstract

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.

Organisationseinheit(en)

Institut für Quantenoptik
Ultrafast Laser Laboratory
QuantumFrontiers
PhoenixD: Simulation, Fabrikation und Anwendung optischer Systeme

Externe Organisation(en)

Max-Planck-Institut für Kernphysik
Ruprecht-Karls-Universität Heidelberg
Deutsches Elektronen-Synchrotron (DESY)
Helmholtz-Institut Jena
GSI Helmholtzzentrum für Schwerionenforschung GmbH
Universität Hamburg
Kansas State University

Typ

Artikel

Journal

Science advances

Band

9

Anzahl der Seiten

7

ISSN

2375-2548

Publikationsdatum

22.11.2023

Publikationsstatus

Veröffentlicht

Peer-reviewed

Ja

ASJC Scopus Sachgebiete

Allgemein

Elektronische Version(en)

https://doi.org/10.1126/SCIADV.ADK1482 (Zugang: Offen)