Impact of Reabsorption on the Emission Spectra and Recombination Dynamics of Hybrid Perovskite Single Crystals

Abstract

Understanding the surface properties of organic-inorganic lead-based perovskites is of high importance to improve the device's performance. Here, we have investigated the differences between surface and bulk optical properties of CH₃NH₃PbBr₃ single crystals. Depth-resolved cathodoluminescence was used to probe the near-surface region on a depth of a few microns. In addition, we have studied the transmitted luminescence through thicknesses between 50 and 600 μm. In both experiments, the expected spectral shift due to the reabsorption effect has been precisely calculated. We demonstrate that reabsorption explains the important variations reported for the emission energy of single crystals. Single crystals are partially transparent to their own luminescence, and radiative transport is the dominant mechanism for propagation of the excitation in thick crystals. The transmitted luminescence dynamics are characterized by a long rise time and a lengthening of their decay due to photon recycling and light trapping.