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

Research output: Contribution to journalArticleResearchpeer review

Authors

  • 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

External Research Organisations

  • 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
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Details

Original languageEnglish
Article numbereadk1482
Number of pages7
JournalScience advances
Volume9
Issue number47
Publication statusPublished - 22 Nov 2023

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.

ASJC Scopus subject areas

Cite this

Time-resolving state-specific molecular dissociation with XUV broadband absorption spectroscopy. / Magunia, Alexander; Rebholz, Marc; Appi, Elisa et al.
In: Science advances, Vol. 9, No. 47, eadk1482, 22.11.2023.

Research output: Contribution to journalArticleResearchpeer review

Magunia, A, Rebholz, M, Appi, E, Papadopoulou, CC, Lindenblatt, H, Trost, F, Meister, S, Ding, T, Straub, M, Borisova, GD, Lee, J, Jin, R, von der Dellen, A, Kaiser, C, Braune, M, Düsterer, S, Ališauskas, S, Lang, T, Heyl, C, Manschwetus, B, Grunewald, S, Frühling, U, Tajalli, A, Wahid, AB, Silletti, L, Calegari, F, Mosel, P, Morgner, U, Kovacev, M, Thumm, U, Hartl, I, Treusch, R, Moshammer, R, Ott, C & Pfeifer, T 2023, 'Time-resolving state-specific molecular dissociation with XUV broadband absorption spectroscopy', Science advances, vol. 9, no. 47, eadk1482. https://doi.org/10.1126/SCIADV.ADK1482
Magunia, A., Rebholz, M., Appi, E., Papadopoulou, C. C., Lindenblatt, H., Trost, F., Meister, S., Ding, T., Straub, M., Borisova, G. D., Lee, J., Jin, R., von der Dellen, A., Kaiser, C., Braune, M., Düsterer, S., Ališauskas, S., Lang, T., Heyl, C., ... Pfeifer, T. (2023). Time-resolving state-specific molecular dissociation with XUV broadband absorption spectroscopy. Science advances, 9(47), Article eadk1482. https://doi.org/10.1126/SCIADV.ADK1482
Magunia A, Rebholz M, Appi E, Papadopoulou CC, Lindenblatt H, Trost F et al. Time-resolving state-specific molecular dissociation with XUV broadband absorption spectroscopy. Science advances. 2023 Nov 22;9(47):eadk1482. doi: 10.1126/SCIADV.ADK1482
Magunia, Alexander ; Rebholz, Marc ; Appi, Elisa et al. / Time-resolving state-specific molecular dissociation with XUV broadband absorption spectroscopy. In: Science advances. 2023 ; Vol. 9, No. 47.
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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.",
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T1 - Time-resolving state-specific molecular dissociation with XUV broadband absorption spectroscopy

AU - Magunia, Alexander

AU - Rebholz, Marc

AU - Appi, Elisa

AU - Papadopoulou, Christina C.

AU - Lindenblatt, Hannes

AU - Trost, Florian

AU - Meister, Severin

AU - Ding, Thomas

AU - Straub, Michael

AU - Borisova, Gergana D.

AU - Lee, Junhee

AU - Jin, Rui

AU - von der Dellen, Alexander

AU - Kaiser, Christian

AU - Braune, Markus

AU - Düsterer, Stefan

AU - Ališauskas, Skirmantas

AU - Lang, Tino

AU - Heyl, Christoph

AU - Manschwetus, Bastian

AU - Grunewald, Sören

AU - Frühling, Ulrike

AU - Tajalli, Ayhan

AU - Wahid, Ammar Bin

AU - Silletti, Laura

AU - Calegari, Francesca

AU - Mosel, Philip

AU - Morgner, Uwe

AU - Kovacev, Milutin

AU - Thumm, Uwe

AU - Hartl, Ingmar

AU - Treusch, Rolf

AU - Moshammer, Robert

AU - Ott, Christian

AU - Pfeifer, Thomas

N1 - Funding Information: This work was supported by theDeutscheForschungsgemeinschaft(DFG,GermanResearchFoundation), Germany’sExcellenceStrategy EXC2181/1390900948(the HeidelbergSTRUCTURESExcellenceCluster) (to T.P.);EuropeanResearch Council(grant no. X-MuSiC616783)(to T.P.); DeutscheForschungsgemeinschaft (DFG, GermanResearch Foundation), Germany’sExcellenceStrategyEXC 2122 (PhoenixD- 390833453,EXC-2123,QuantumFrontiers390837967)(to M.K.);DeutscheForschungsgemeinschaft(DFG,GermanResearchFoundation), Germany’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.).

PY - 2023/11/22

Y1 - 2023/11/22

N2 - 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.

AB - 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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DO - 10.1126/SCIADV.ADK1482

M3 - Article

C2 - 37992169

AN - SCOPUS:85177875947

VL - 9

JO - Science advances

JF - Science advances

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