Nonlinear optical response, theoretical efficiencies, and high photosensitivity of CH3NH3PbI3-xClxthin films for photonic applications

Abstract

In this paper, we have investigated the nonlinear optical response and theoretical efficiency of CH3NH3PbI3-xClx thin films from the optical transmission and reflection measurements. The dispersion of the complex refractive index is evaluated using the Wemple-DiDomenico single oscillator model. The oscillator energy (E0) of CH3NH3PbI3-xClx follows by an empirical relationship with optical bandgap (Eg) as E0 ≈ 2.41 Eg for chemical dip coating, spray, and E0 ≈ 1.63 Eg for dipping deposited samples, respectively. The long wavelength refractive index, average oscillator wavelength, and oscillator strength are also determined using the Sellmeier oscillator equation. The estimated third-order nonlinear optical susceptibility is found to be the order of 10-12 esu. The incident photon and charge carrier interaction in CH3NH3PbI3-xClx is studied from the dielectric response of the samples. The charge carrier excitation is found higher at lower wavelength and experienced bulk excitation in volume while surface excitation on the surface region. The optical conductivity of CH3NH3PbI3-xClx is notably high, which leads to an increase in carrier transfer through the extrinsic halide perovskite material expedient for higher conversion efficiency. The highest theoretical efficiency of CH3NH3PbI3-xClx is estimated to be 17.4%, which is in excellent agreement with the experimental report. From photosensitivity study, it is confirmed that CH3NH3PbI3-xClx films are highly photosensitive. All these results comprehend that CH3NH3PbI3-xClx is a potential candidate for photonic applications.