Outstanding nonlinear optical properties of methylammonium- and Cs-PbX3 (X = Br, I, and Br–I) perovskites: Polycrystalline thin films and nanoparticles

Abstract

Metal Halide Perovskites (MHPs) have arisen as promising materials to construct cost-effective photovoltaic and light emission devices. The study of nonlinear optical properties of MHPs is necessary to get similar success in nonlinear photonic devices, which is practically absent in the literature. The determination of the third order nonlinear coefficients is typically done by the Z-scan technique, which is limited by the scattering of polycrystalline thin films. In this work, we have studied nonlinear optical properties of polycrystalline CH3NH3PbX3 (MAPbX3) thin films and colloidal CsPbX3 nanoparticles with three different bandgaps (X3 = I3, Br3, and Br1.5I1.5). Their bright generation of photoluminescence under infrared illumination demonstrates an excellent efficiency of multiphoton absorption. The nonlinear absorption coefficient (β) was studied by analyzing the transmitted light through the samples, observing the expected Eg−3 dependence with values as high as β = 1500 cm/GW. In addition, we proposed the use of a modified Z-scan technique with imaging processing to analyze the nonlinear refraction coefficient (n2) under the laser damage threshold. Our experimental data agree quite well with theoretical predictions, demonstrating the accuracy of the method and potential applications to other thin films. Moreover, n2 parameter reaches values of 3.5 cm2/GW, indicating the suitability of MHPs for nonlinear photonics.