001048820 001__ 1048820
001048820 005__ 20251203101801.0
001048820 0247_ $$2doi$$a10.48550/ARXIV.2511.23001
001048820 0247_ $$2doi$$a10.48550/arXiv.2511.23001
001048820 037__ $$aFZJ-2025-04928
001048820 1001_ $$0P:(DE-HGF)0$$aTheilen, Marcel$$b0$$eFirst author
001048820 245__ $$aObserving the spatial and temporal evolution of exciton wave functions
001048820 260__ $$barXiv$$c2025
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001048820 520__ $$aExcitons, the correlated electron-hole pairs governing optical and transport properties in organic semiconductors, have long resisted direct experimental access to their full quantum-mechanical wave functions. Here, we use femtosecond time-resolved photoemission orbital tomography (trPOT), combining high-harmonic probe pulses with time- and momentum-resolved photoelectron spectroscopy, to directly image the momentum-space distribution and ultrafast dynamics of excitons in $α$-sexithiophene thin films. We introduce a quantitative model that enables reconstruction of the exciton wave function in real space, including both its spatial extent and its internal phase structure. The reconstructed wave function reveals coherent delocalization across approximately three molecular units and exhibits a characteristic phase modulation, consistent with ab initio calculations within the framework of many-body perturbation theory. Time-resolved measurements further show a $\sim 20$\% contraction of the exciton radius within 400 fs, providing direct evidence of self-trapping driven by exciton-phonon coupling. These results establish trPOT as a general and experimentally accessible approach for resolving exciton wave functions -- with spatial, phase, and temporal sensitivity -- in a broad class of molecular and low-dimensional materials.
001048820 536__ $$0G:(DE-HGF)POF4-5213$$a5213 - Quantum Nanoscience (POF4-521)$$cPOF4-521$$fPOF IV$$x0
001048820 536__ $$0G:(EU-Grant)101071259$$aOrbital Cinema - Photoemission Orbital Cinematography: An ultrafast wave function lab (101071259)$$c101071259$$fERC-2022-SYG$$x1
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001048820 650_7 $$2Other$$aMaterials Science (cond-mat.mtrl-sci)
001048820 650_7 $$2Other$$aFOS: Physical sciences
001048820 7001_ $$0P:(DE-HGF)0$$aKaidisch, Siegfried$$b1
001048820 7001_ $$0P:(DE-Juel1)190627$$aStettner, Monja$$b2$$ufzj
001048820 7001_ $$0P:(DE-HGF)0$$aZajusch, Sarah$$b3
001048820 7001_ $$0P:(DE-Juel1)201937$$aFackelman, Eric$$b4$$ufzj
001048820 7001_ $$0P:(DE-HGF)0$$aAdamkiewicz, Alexa$$b5
001048820 7001_ $$0P:(DE-HGF)0$$aWallauer, Robert$$b6
001048820 7001_ $$0P:(DE-HGF)0$$aWindischbacher, Andreas$$b7
001048820 7001_ $$0P:(DE-HGF)0$$aKern, Christian S.$$b8
001048820 7001_ $$0P:(DE-HGF)0$$aRamsey, Michael G.$$b9
001048820 7001_ $$0P:(DE-HGF)0$$aBocquet, François C.$$b10
001048820 7001_ $$0P:(DE-HGF)0$$aSoubatch, Serguei$$b11
001048820 7001_ $$0P:(DE-Juel1)128791$$aTautz, F. Stefan$$b12$$ufzj
001048820 7001_ $$0P:(DE-HGF)0$$aHöfer, Ulrich$$b13
001048820 7001_ $$0P:(DE-HGF)0$$aPuschnig, Peter$$b14$$eCorresponding author
001048820 773__ $$a10.48550/arXiv.2511.23001$$t arXiv:2511.23001 [cond-mat.mtrl-sci]$$y2025
001048820 8564_ $$uhttps://arxiv.org/abs/2511.23001
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