Exciton transport plays a central role in optoelectronic and photonic devices. In quasi-two-dimensional (2D) hybrid organic–inorganic perovskites (HOIPs), tightly bound excitons are found to diffuse within 2D layers rapidly with a non-monotonic temperature dependence. Surprisingly, the interlayer exciton diffusion is quite effective as well despite the large interlayer distance. This is in sharp contrast to electron transport, where the interlayer mobility is several orders of magnitude smaller than the intralayer one. Here, we show that the unusual exciton diffusion behaviors can be systematically modeled via the excitonic band structure arising from a long-range dipolar coupling. Coherent exciton motion is interrupted by scattering of impurities at low temperatures and of acoustic/optical phonons at high temperatures. Acoustic and optical phonons modulate the dipole–dipole distance and the dipole orientation, respectively. The ratio of intralayer and interlayer diffusion constants, Dxx/Dzz, is comparable to az/ax with az and ax being the interlayer and intralayer lattice constants of 2D HOIPs, respectively. The efficient and omnidirectional exciton diffusion suggests a great potential of 2D HOIPs in novel excitonic and polaritonic applications.
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