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We report on the exciton formation and relaxation dynamics followingphotocarrier injection in a single-layer two-dimensional lead-iodideperovskite. We probe the time evolution of four distinct exciton resonances bymeans of time-resolved photoluminescence and transient absorptionspectroscopies, and find that at 5\,K a subset of excitons form on a $\lesssim$1-ps timescale, and that these relax subsequently to lower-energy excitons on$\sim$ 5--10\,ps with a marked temperature dependence over $<$ 100\,K. Weimplement a mode projection analysis that determines the relative contributionof all observed phonons with frequency $\leq$50\,cm$^{-1}$ to inter-excitonnonadiabatic coupling, which in turn determines the rate of exciton relaxation.This analysis ranks the relative contribution of the phonons that participatein polaronic lattice distortions to the exciton inter-conversion dynamics andthus establishes their role in the nonadiabatic mixing of exciton states, andthis in the exciton relaxation rate.

Electron-phonon couplings inherent in polarons drive exciton dynamics in two-dimensional metal-halide perovskites