Ultrafast THz Probe of Photoinduced Polarons in Lead-Halide Perovskites

Abstract

We study the nature of photoexcited charge carriers in CsPbBr_{3} nanocrystal thin films by ultrafast optical pump-THz probe spectroscopy. We observe a deviation from a pure Drude dispersion of the THz dielectric response that is ascribed to the polaronic nature of carriers; a transient blueshift of observed phonon frequencies is indicative of the coupling between photogenerated charges and stretching-bending modes of the deformed inorganic sublattice, as confirmed by DFT calculations.