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

authored by

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.

Organisation(s)

Institute of Quantum Optics
Ultrafast Laser Laboratory
QuantumFrontiers
PhoenixD: Photonics, Optics, and Engineering - Innovation Across Disciplines

External Organisation(s)

Max Planck Institute for Nuclear Physics
Heidelberg University
Deutsches Elektronen-Synchrotron (DESY)
Helmholtz Institute Jena
GSI Helmholtz Centre for Heavy Ion Research
Universität Hamburg
Kansas State University

Type

Article

Journal

Science advances

Volume

9

No. of pages

7

ISSN

2375-2548

Publication date

22.11.2023

Publication status

Published

Peer reviewed

Yes

ASJC Scopus subject areas

General

Electronic version(s)

https://doi.org/10.1126/SCIADV.ADK1482 (Access: Open)