Photophysical Properties, Stability and Microstructures of Temperature-Dependent Evolution of Methylammonium Lead Bromide Perovskite

Organic/inorganic hybrid perovskite materials, such as CH3NH3PbX3 (X = I, Br), have attracted the attention of the scientific community due to their excellent properties such as a widely tunable bandgap, high optical absorption coefficient, excellent power conversion efficiency, etc. The exposure of perovskite solar cells and photovoltaic devices to heat can significantly degrade their performance. Therefore, elucidating their temperature-dependent optical properties is essential for performance optimization of perovskite solar cells. We synthesized CH3NH3PbBr3 (MAPbBr3) single crystals through the polymer-controlled nucleation route and investigated the optical properties and molecular structure evolution of them with temperature. Through temperature evolution photoluminescence (PL) spectroscopy, we found that the fluorescence intensity was greatly affected by increasing the temperature, with an asymmetric PL profile suggesting that more captured excitons undergo radiative complexation. The optical photographs showed that the color of MAPbBr3 single crystals faded. Raman spectroscopy revealed that during the heating process, the structure of MAPbBr3 was still preserved at 90 °C since all of the Raman bands were very clear. When the temperature increased to 120 °C, the Raman bands of the internal modes became very weak. On further heating, the inorganic framework on sample’s surface started to disintegrate above 210 °C. During the heating process, the PL spectra exhibited significant changes in spectral intensity, peak position and Full Width Half Maximum (FWHM). The PL spectral intensity decreased abruptly with increasing temperature. The peak position was blue shifted with increasing temperature, and the peak shape showed an obvious asymmetry. The FMWH of the PL spectra was gradually broadened with the increase in the temperature, and there was a sharp increase from 270 °C to 300 °C. These variations in the PL spectra with temperature indicate that the optical properties of MAPbBr3 are greatly affected by temperature, which in turn affects the application of MAPbBr3 in fields such as optical devices. These results may be instructive for the application of MAPbBr3.