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001     1041609
005     20250424202216.0
024 7 _ |a 10.48550/ARXIV.2010.02599
|2 doi
037 _ _ |a FZJ-2025-02343
100 1 _ |a Wallauer, Robert
|0 P:(DE-HGF)0
|b 0
245 _ _ |a Tracing orbital images on ultrafast time scales
260 _ _ |c 2020
|b arXiv
336 7 _ |a Preprint
|b preprint
|m preprint
|0 PUB:(DE-HGF)25
|s 1745495498_9276
|2 PUB:(DE-HGF)
336 7 _ |a WORKING_PAPER
|2 ORCID
336 7 _ |a Electronic Article
|0 28
|2 EndNote
336 7 _ |a preprint
|2 DRIVER
336 7 _ |a ARTICLE
|2 BibTeX
336 7 _ |a Output Types/Working Paper
|2 DataCite
520 _ _ |a Frontier orbitals, i.e., the highest occupied and lowest unoccupied orbitals of a molecule, generally determine molecular properties, such as chemical bonding and reactivities. Consequently, there has been a lot of interest in measuring them, despite the fact that, strictly speaking, they are not quantum-mechanical observables. Yet, with photoemission tomography a powerful technique has recently been introduced by which the electron distribution in orbitals of molecules adsorbed at surfaces can be imaged in momentum space. This has even been used for the identification of reaction intermediates in surface reactions. However, so far it has been impossible to follow an orbital's momentum-space dynamics in time, for example through an excitation process or a chemical reaction. Here, we report a key step in this direction: we combine time-resolved photoemission employing high laser harmonics and a recently developed momentum microscope to establish a tomographic, femtosecond pump-probe experiment of unoccupied molecular orbitals. Specifically, we measure the full momentum-space distribution of transiently excited electrons. Because in molecules this momentum-space distribution is closely linked to orbital shapes, our experiment offers the extraordinary possibility to observe ultrafast electron motion in time and space. This enables us to connect their excited states dynamics to specific real-space excitation pathways.
536 _ _ |a 5213 - Quantum Nanoscience (POF4-521)
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588 _ _ |a Dataset connected to DataCite
650 _ 7 |a Chemical Physics (physics.chem-ph)
|2 Other
650 _ 7 |a Mesoscale and Nanoscale Physics (cond-mat.mes-hall)
|2 Other
650 _ 7 |a Other Condensed Matter (cond-mat.other)
|2 Other
650 _ 7 |a FOS: Physical sciences
|2 Other
700 1 _ |a Raths, Miriam
|0 P:(DE-Juel1)172607
|b 1
700 1 _ |a Stallberg, Klaus
|0 P:(DE-HGF)0
|b 2
700 1 _ |a Münster, Lasse
|0 P:(DE-HGF)0
|b 3
700 1 _ |a Brandstetter, Dominik
|0 P:(DE-HGF)0
|b 4
700 1 _ |a Yang, Xiaosheng
|0 P:(DE-Juel1)165181
|b 5
700 1 _ |a Güdde, Jens
|0 P:(DE-HGF)0
|b 6
700 1 _ |a Puschnig, Peter
|0 P:(DE-HGF)0
|b 7
700 1 _ |a Soubatch, Serguei
|0 P:(DE-HGF)0
|b 8
700 1 _ |a Kumpf, Christian
|0 P:(DE-Juel1)128774
|b 9
|u fzj
700 1 _ |a Bocquet, Francois C.
|0 P:(DE-HGF)0
|b 10
700 1 _ |a Tautz, Frank Stefan
|0 P:(DE-Juel1)128791
|b 11
|e Corresponding author
|u fzj
700 1 _ |a Höfer, Ulrich
|0 P:(DE-HGF)0
|b 12
773 _ _ |a 10.48550/ARXIV.2010.02599
856 4 _ |u https://arxiv.org/abs/2010.02599
909 C O |o oai:juser.fz-juelich.de:1041609
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910 1 _ |a Forschungszentrum Jülich
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910 1 _ |a Forschungszentrum Jülich
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913 1 _ |a DE-HGF
|b Key Technologies
|l Natural, Artificial and Cognitive Information Processing
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920 1 _ |0 I:(DE-Juel1)PGI-3-20110106
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980 _ _ |a preprint
980 _ _ |a VDB
980 _ _ |a I:(DE-Juel1)PGI-3-20110106
980 _ _ |a UNRESTRICTED

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