Quantum defect-assisted multiphonon Raman scattering in metal halide perovskites.

ABSTRACT

Quantum defects are essential to understand the non-radiative recombination processes in metal halide perovskites-based photovoltaic devices, in which Huang-Rhys factor, reflecting the coupling strength between the charge carrier and optical phonons, plays a key role in determining the non-radiative recombination via multiphonon processes. Herein, we theoretically present multiphonon Raman scattering intermediated by defects arising from the charge carrier of defect coupled with the longitudinal optical (LO) phonon in the deformation potential and Fröhlich mechanisms, respectively. We find that the Raman scattering shows multiple LO phonon overtones at equal interval LO phonons, where Huang-Rhys factor could be evaluated by the order of the strongest overtone. Meanwhile, we give the combinational multiphonon scattering between two mechanisms. Different types of the combinational modes with the weak scattering intensities provide a possible explanation for the long non-radiative charges-carrier lifetimes in metal halide perovskites.