Unveiling the mixed nature of polaritonic transport: From enhanced diffusion to ballistic motion approaching the speed of light (2205.06683v1)

Abstract: In recent years it has become clear that the transport of excitons and charge carriers in molecular systems can be enhanced by coherent coupling with photons, giving rise to the formation of hybrid excitations known as polaritons. Such enhancement has far-reaching technological implications, however, the enhancement mechanism and the transport nature of these composite light-matter excitations in such systems still remain elusive. Here we map the ultrafast spatiotemporal dynamics of surface-bound optical waves strongly coupled to a self-assembled molecular layer and fully resolve them in energy/momentum space. Our studies reveal intricate behavior which stems from the hybrid nature of polaritons. We find that the balance between the molecular disorder and long-range correlations induced by the coherent mixing between light and matter leads to a mobility transition between diffusive and ballistic transport, which can be controlled by varying the light-matter composition of the polaritons. Furthermore, we directly demonstrate that the coupling with light can enhance the diffusion coefficient of molecular excitons by six orders of magnitude and even lead to ballistic flow at two-thirds the speed of light.