001     1048820
005     20251203101801.0
024 7 _ |a 10.48550/ARXIV.2511.23001
|2 doi
024 7 _ |a 10.48550/arXiv.2511.23001
|2 doi
037 _ _ |a FZJ-2025-04928
100 1 _ |a Theilen, Marcel
|0 P:(DE-HGF)0
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|e First author
245 _ _ |a Observing the spatial and temporal evolution of exciton wave functions
260 _ _ |c 2025
|b arXiv
336 7 _ |a Preprint
|b preprint
|m preprint
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336 7 _ |a Electronic Article
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336 7 _ |a preprint
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336 7 _ |a ARTICLE
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336 7 _ |a Output Types/Working Paper
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520 _ _ |a Excitons, the correlated electron-hole pairs governing optical and transport properties in organic semiconductors, have long resisted direct experimental access to their full quantum-mechanical wave functions. Here, we use femtosecond time-resolved photoemission orbital tomography (trPOT), combining high-harmonic probe pulses with time- and momentum-resolved photoelectron spectroscopy, to directly image the momentum-space distribution and ultrafast dynamics of excitons in $α$-sexithiophene thin films. We introduce a quantitative model that enables reconstruction of the exciton wave function in real space, including both its spatial extent and its internal phase structure. The reconstructed wave function reveals coherent delocalization across approximately three molecular units and exhibits a characteristic phase modulation, consistent with ab initio calculations within the framework of many-body perturbation theory. Time-resolved measurements further show a $\sim 20$\% contraction of the exciton radius within 400 fs, providing direct evidence of self-trapping driven by exciton-phonon coupling. These results establish trPOT as a general and experimentally accessible approach for resolving exciton wave functions -- with spatial, phase, and temporal sensitivity -- in a broad class of molecular and low-dimensional materials.
536 _ _ |a 5213 - Quantum Nanoscience (POF4-521)
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536 _ _ |a Orbital Cinema - Photoemission Orbital Cinematography: An ultrafast wave function lab (101071259)
|0 G:(EU-Grant)101071259
|c 101071259
|f ERC-2022-SYG
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588 _ _ |a Dataset connected to DataCite
650 _ 7 |a Materials Science (cond-mat.mtrl-sci)
|2 Other
650 _ 7 |a FOS: Physical sciences
|2 Other
700 1 _ |a Kaidisch, Siegfried
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|b 1
700 1 _ |a Stettner, Monja
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700 1 _ |a Zajusch, Sarah
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700 1 _ |a Fackelman, Eric
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700 1 _ |a Adamkiewicz, Alexa
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700 1 _ |a Wallauer, Robert
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700 1 _ |a Windischbacher, Andreas
|0 P:(DE-HGF)0
|b 7
700 1 _ |a Kern, Christian S.
|0 P:(DE-HGF)0
|b 8
700 1 _ |a Ramsey, Michael G.
|0 P:(DE-HGF)0
|b 9
700 1 _ |a Bocquet, François C.
|0 P:(DE-HGF)0
|b 10
700 1 _ |a Soubatch, Serguei
|0 P:(DE-HGF)0
|b 11
700 1 _ |a Tautz, F. Stefan
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700 1 _ |a Höfer, Ulrich
|0 P:(DE-HGF)0
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700 1 _ |a Puschnig, Peter
|0 P:(DE-HGF)0
|b 14
|e Corresponding author
773 _ _ |a 10.48550/arXiv.2511.23001
|y 2025
|t arXiv:2511.23001 [cond-mat.mtrl-sci]
856 4 _ |u https://arxiv.org/abs/2511.23001
910 1 _ |a Forschungszentrum Jülich
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980 _ _ |a preprint
980 _ _ |a EDITORS
980 _ _ |a VDBINPRINT
980 _ _ |a I:(DE-Juel1)PGI-3-20110106
980 _ _ |a UNRESTRICTED


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