Ultrafast Random Lasing in MAPbI₃ Halide Perovskite Single Crystals

Abstract

Halide perovskites are a promising optical gain media for lasers. In this work, the phenomenon of random lasing is studied in the halide perovskite MAPbI3 single crystal at a temperature of 4 K and pico- or femtosecond pulsed optical pumping. Spectral, temporal, polarimetric, and threshold measurements facilitate isolating random lasing from the photoluminescence background. Spectral localization of the lasing lines points to defect-related states emission as the lasing origin. Time-resolved photoluminescence study shows that the random lasing is emitted as an ultrashort pulse with a duration below 10 ps, and the photoluminescence background as a long 100 ps afterglow. The mechanism of lasing in MAPbI3 halide perovskite is determined, which is ultrafast radiation from states associated with defects. The obtained information will make it possible to increase the efficiency of lasing in halide perovskites by controlled introduction of radiating states in the material transparency region.

Discrete Donor–Acceptor Pair Transitions in CH3NH3PbI3 Perovskite Single Crystals

“…Interestingly, understanding the nature of defect‐related states is also relevant to application in lasing since these states are implied in the mechanism of lasing in HPs. [ 83 ]…”

White lasing – materials, design and applications

“…Moreover, they are known for light amplification. 84,85 The observed fluorescence color of perovskites is subject to several factors, such as chemical composition, crystal structure, and nanoparticle size. A noteworthy attribute of perovskites is their capacity to exhibit different light colors, which is commonly known as multicolor tunability.…”

Free Exciton and Defect-Related States in CH3NH3PbCl3 Perovskite Single Crystal

“…These states are generally undesirable in most cases; however, it has been reported that they are essential for lasing in halide perovskites. 12,13 In the PL spectra of MAPbCl 3 , the presence of many narrow lines in the region of defect-related states was reported. However, there are conflicting interpretations of these spectral lines in the literature.…”

“…Despite its high applicability potential and the highest stability among other MA-based perovskites, there is a significant knowledge gap in the fundamental properties of this material, particularly regarding defect-related states. These states are generally undesirable in most cases; however, it has been reported that they are essential for lasing in halide perovskites. , …”