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Organic semiconductor crystals stand out as an efficient, cheap and diverseplatform for realising optoelectronic applications. The optical response ofthese crystals is governed by a rich tapestry of exciton physics. So far,little is known on the phonon-driven singlet exciton dynamics in this class ofmaterials. In this joint theory-experiment work, we combine the fabrication ofa high-quality oligoacene semiconductor crystal and characterization viaphotoluminescence measurements with a sophisticated approach to the microscopicmodeling in these crystals. This allows us to investigate singlet excitonoptics and dynamics. We predict phonon-bottleneck effects in pentacenecrystals, where we find dark excitons acting as crucial phonon-mediatedrelaxation scattering channels. While the efficient singlet fission inpentacene crystals hampers the experimental observation of this bottleneckeffect, we reveal both in theory and experiment a distinct polarisation- andtemperature-dependence in absorption and photoluminescence spectra of tetracenecrystals, including microscopic origin of exciton linewidths, the activation ofthe higher Davydov states at large temperatures, and polarisation-dependentquenching of specific exciton resonances. Our joint theory-experiment studyrepresents a significant advance in microscopic understanding of singletexciton optics and dynamics in oligoacene crystals.

Singlet exciton optics and phonon-mediated dynamics in oligoacene semiconductor crystals