TY  - EJOUR
AU  - Theilen, Marcel
AU  - Kaidisch, Siegfried
AU  - Stettner, Monja
AU  - Zajusch, Sarah
AU  - Fackelman, Eric
AU  - Adamkiewicz, Alexa
AU  - Wallauer, Robert
AU  - Windischbacher, Andreas
AU  - Kern, Christian S.
AU  - Ramsey, Michael G.
AU  - Bocquet, François C.
AU  - Soubatch, Serguei
AU  - Tautz, F. Stefan
AU  - Höfer, Ulrich
AU  - Puschnig, Peter
TI  - Observing the spatial and temporal evolution of exciton wave functions
JO  -  arXiv:2511.23001 [cond-mat.mtrl-sci]
PB  - arXiv
M1  - FZJ-2025-04928
PY  - 2025
AB  - 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.
KW  - Materials Science (cond-mat.mtrl-sci) (Other)
KW  - FOS: Physical sciences (Other)
LB  - PUB:(DE-HGF)25
DO  - DOI:10.48550/arXiv.2511.23001
UR  - https://juser.fz-juelich.de/record/1048820
ER  -