Details
| Original language | English |
|---|---|
| Article number | eadk1482 |
| Number of pages | 7 |
| Journal | Science advances |
| Volume | 9 |
| Issue number | 47 |
| Publication status | Published - 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.
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In: Science advances, Vol. 9, No. 47, eadk1482, 22.11.2023.
Research output: Contribution to journal › Article › Research › peer review
}
TY - JOUR
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.
UR - http://www.scopus.com/inward/record.url?scp=85177875947&partnerID=8YFLogxK
U2 - 10.1126/SCIADV.ADK1482
DO - 10.1126/SCIADV.ADK1482
M3 - Article
C2 - 37992169
AN - SCOPUS:85177875947
VL - 9
JO - Science advances
JF - Science advances
SN - 2375-2548
IS - 47
M1 - eadk1482
ER -