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Harnessing the optoelectronic response of organic semiconductors requires athorough understanding of the fundamental light-matter interaction that isdominated by the excitation of correlated electron-hole pairs, i.e. excitons.The nature of these excitons would be fully captured by knowing thequantum-mechanical wavefunction, which, however, is difficult to access boththeoretically and experimentally. Here, we use femtosecond photoemissionorbital tomography in combination with many-body perturbation theory to gainaccess to exciton wavefunctions in organic semiconductors. We find that thecoherent sum of multiple electron-hole pair contributions that typically makeup a single exciton can be experimentally evidenced by photoelectronspectroscopy. For the prototypical organic semiconductor buckminsterfullerene(C$_{60}$), we show how to disentangle such multiorbital contributions andthereby access key properties of the exciton wavefunctions includinglocalization, charge-transfer character, and ultrafast exciton formation andrelaxation dynamics.

Multiorbital exciton formation in an organic semiconductor