Excitonic enhancement of optical nonlinearities in perovskite CH3NH3PbCl3 single crystals

Abstract

Metal halide perovskites have emerged as versatile photonic device materials because of their outstanding band structure and excellent optical properties. Here, we determined the excitation wavelength dependences of the two-photon absorption coefficient and the Kerr-effect-induced nonlinear refractive index of CH3NH3PbCl3 perovskite single crystals by means of the Z-scan method. From theoretical analysis, we found that the electron-hole interaction, so-called exciton effect, significantly enhances the nonlinear optical responses even for the interband transitions. This interaction explains the universal relation between the exciton reduced mass and the bandgap for lead halide perovskites.