Journal
SCIENCE
Volume 371, Issue 6533, Pages 1056-+Publisher
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.abf3286
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Funding
- Deutsche Forschungsgemeinschaft (DFG) [223848855SFB 1083]
- Austrian Science Fund (FWF) [I3731]
- DFG [396769409]
- Austrian Science Fund (FWF) [I3731] Funding Source: Austrian Science Fund (FWF)
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This study combined high laser harmonics and a momentum microscope to establish tomographic, femtosecond pump-probe experiment of unoccupied molecular orbitals, providing the possibility of observing ultrafast electron motion in time and space in the future.
Frontier orbitals determine fundamental molecular properties such as chemical reactivities. Although electron distributions of occupied orbitals can be imaged in momentum space by photoemission tomography, it has so far been impossible to follow the momentum-space dynamics of a molecular orbital in time, for example, through an excitation or a chemical reaction. Here, we combined time-resolved photoemission using high laser harmonics and a momentum microscope to establish a tomographic, femtosecond pump-probe experiment of unoccupied molecular orbitals. We measured the full momentum-space distribution of transiently excited electrons, connecting their excited-state dynamics to real-space excitation pathways. Because in molecules this distribution is closely linked to orbital shapes, our experiment may, in the future, offer the possibility of observing ultrafast electron motion in time and space.
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