Accelerated Carrier Relaxation through Reduced Coulomb Screening in 2D Halide Perovskite Nanoplatelets

Abstract: For high-speed optoelectronic applications relying on fast relaxation or energy transfer mechanisms, understanding of carrier relaxation and recombination dynamics is critical. Here, we compare the differences in photoexcited carrier dynamics in 2D and quasi-3D colloidal methylammonium lead iodide perovskite nanoplatelets via differential transmission spectroscopy. We find that the cooling of excited electron-hole pairs by phonon emission progresses much faster and is intensity-independent in the 2D-case. This is due to the low dielectric surrounding of the thin perovskite layers, for which the Fr\"ohlich interaction is screened less efficiently leading to higher and less density dependent carrier-phonon scattering rates. In addition, rapid dissipation of heat into the surrounding occurs due to the high surface-to-volume ratio. Furthermore, we observe a sub-picosecond dissociation of resonantly excited 1s excitons in the quasi-3D case, an effect which is suppressed in the 2D nanoplatelets due to their large exciton binding energies. The results highlight the importance of the surrounding environment of the inorganic nanoplatelets on their relaxation dynamics. Moreover, this 2D material with relaxation times in the sub-picosecond regime shows great potential for realizing devices such as photodetectors or all-optical switches operating at THz frequencies.