Layer-Dependent Coherent Acoustic Phonons in Two-Dimensional Ruddlesden-Popper Perovskite Crystals

By combining femtosecond transient reflectance (TR) spectroscopy and density functional theory (DFT) calculations, we reveal the impact of the length of the organic linkers (HOC₂H₄NH₃⁺ and C₆H₅C₂H₄NH₃⁺) and the number of inorganic layers (n = 1-3) on the hot carrier relaxation dynamics and coherent acoustic phonons in 2D Ruddlesden-Popper (RP) perovskites. We find that the interplay between the hot carriers and the coherent longitudinal acoustic phonons (CLAPs) can extend the oscillation of the TR kinetics to nanoseconds, which could lead to the higher thermal conductivities of 2D RP perovskites. Moreover, we find that the frequency of the acoustic phonon oscillation and phonon velocity decreases with the increasing number of layers due to the increased mass of the inorganic layers and reduced electron-phonon coupling. This finding provides new physical insights into how the organic spacers and number of inorganic layers control the overall carrier dynamics of 2D perovskite materials.