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The efficiency of two-dimensional Dion-Jacobson-type materials relies on thecomplex interplay between electronic and lattice dynamics; however, questionsremain about the functional role of exciton-phonon interactions. This studyestablishes the robust polaronic nature of the excitons in these materials atroom temperature by combining ultrafast spectroscopy and electronic structuralcalculations. We show that polaronic distortion is associated withlow-frequency (30-60 cm-1) lead iodide octahedral lattice motions. Moreimportantly, we discover how targeted ligand modification of thistwo-dimensional perovskite structure controls exciton-phonon coupling,exciton-polaron population, and carrier cooling. At high excitation density,stronger exciton-phonon coupling increases the hot carrier lifetime, forming ahot-phonon bottleneck. Our study provides detailed insight into theexciton-phonon coupling and its role in carrier cooling in two-dimensionalperovskites relevant for developing emerging hybrid semiconductor materialswith tailored properties.

Exciton-phonon Coupling Controls Exciton-polaron Formation and Hot Carrier Relaxation in Rigid Dion-Jacobson Type Two-Dimensional Perovskites