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@ARTICLE{Theilen:1048820,
author = {Theilen, Marcel and Kaidisch, Siegfried and Stettner, Monja
and Zajusch, Sarah and Fackelman, Eric and Adamkiewicz,
Alexa and Wallauer, Robert and Windischbacher, Andreas and
Kern, Christian S. and Ramsey, Michael G. and Bocquet,
François C. and Soubatch, Serguei and Tautz, F. Stefan and
Höfer, Ulrich and Puschnig, Peter},
title = {{O}bserving the spatial and temporal evolution of exciton
wave functions},
journal = {arXiv:2511.23001 [cond-mat.mtrl-sci]},
publisher = {arXiv},
reportid = {FZJ-2025-04928},
year = {2025},
abstract = {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.},
keywords = {Materials Science (cond-mat.mtrl-sci) (Other) / FOS:
Physical sciences (Other)},
cin = {PGI-3},
cid = {I:(DE-Juel1)PGI-3-20110106},
pnm = {5213 - Quantum Nanoscience (POF4-521) / Orbital Cinema -
Photoemission Orbital Cinematography: An ultrafast wave
function lab (101071259)},
pid = {G:(DE-HGF)POF4-5213 / G:(EU-Grant)101071259},
typ = {PUB:(DE-HGF)25},
doi = {10.48550/arXiv.2511.23001},
url = {https://juser.fz-juelich.de/record/1048820},
}