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)

BibTeX

@article{23ec758a36494c929323bb7760aa534b,
title = "Time-resolving state-specific molecular dissociation with XUV broadband absorption spectroscopy",
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.",
author = "Alexander Magunia and Marc Rebholz and Elisa Appi and Papadopoulou, {Christina C.} and Hannes Lindenblatt and Florian Trost and Severin Meister and Thomas Ding and Michael Straub and Borisova, {Gergana D.} and Junhee Lee and Rui Jin and {von der Dellen}, Alexander and Christian Kaiser and Markus Braune and Stefan D{\"u}sterer and Skirmantas Ali{\v s}auskas and Tino Lang and Christoph Heyl and Bastian Manschwetus and S{\"o}ren Grunewald and Ulrike Fr{\"u}hling and Ayhan Tajalli and Wahid, {Ammar Bin} and Laura Silletti and Francesca Calegari and Philip Mosel and Uwe Morgner and Milutin Kovacev and Uwe Thumm and Ingmar Hartl and Rolf Treusch and Robert Moshammer and Christian Ott and Thomas Pfeifer",
note = "Funding Information: This work was supported by theDeutscheForschungsgemeinschaft(DFG,GermanResearchFoundation), Germany{\textquoteright}sExcellenceStrategy EXC2181/1390900948(the HeidelbergSTRUCTURESExcellenceCluster) (to T.P.);EuropeanResearch Council(grant no. X-MuSiC616783)(to T.P.); DeutscheForschungsgemeinschaft (DFG, GermanResearch Foundation), Germany{\textquoteright}sExcellenceStrategyEXC 2122 (PhoenixD- 390833453,EXC-2123,QuantumFrontiers390837967)(to M.K.);DeutscheForschungsgemeinschaft(DFG,GermanResearchFoundation), Germany{\textquoteright}sExcellenceStrategy Cluster of ExcellenceAdvancedImagingof Matter–AIM (to F.C.); HelmholtzAssociation (HIRS-0018)(to C.C.P., M.B., S.D., S.A., T.L., C.H., B.M., S.G., U.F., A.T., I.H., and R.T.);ChemicalSciences,Geosciences,and BiosciencesDivision,Officeof Basic EnergySciences,Officeof Science,U.S. Departmentof Energy, award no. DEFG02-86ER13491(strong fielddynamicsof small molecules)(to U.T.); and NSF grant no. PHY 2110633(numericalmodeldevelopment)(to U.T.). ",
year = "2023",
month = nov,
day = "22",
doi = "10.1126/SCIADV.ADK1482",
language = "English",
volume = "9",
journal = "Science advances",
issn = "2375-2548",
publisher = "American Association for the Advancement of Science",
number = "47",
}