Amplified Spontaneous Emission and Random Lasing in MAPbBr₃ Halide Perovskite Single Crystals

Abstract

Halide perovskites are a promising optical gain medium with high tunability and simple solution synthesis. In this study, two gain regimes, namely, amplified spontaneous emission and random lasing, are demonstrated in the same MAPbBr3 halide perovskite single crystal. For this, photoluminescence is measured at a temperature of 4 K with pulsed femtosecond pumping by UV light with an 80 MHz repetition rate. Random lasing is observed in areas of the sample where a random resonator is formed due to cracks and crystal imperfections. In more homogeneous regions of the sample, the dominant regime is amplified spontaneous emission. These two regimes are reliably distinguished by the line width, the mode structure, the growth of the intensity after the threshold, and the degree of polarization of the radiation. The spectral localization of the stimulated emission well below the bound exciton resonance raises a question concerning the origin of the emission in halide perovskite lasers.

Photoluminescence Excitation Spectroscopy of Defect‐Related States in MAPbI3 Perovskite Single Crystals

“…Nevertheless, this tail state plays an important role in lasing phenomenon, as it was demonstrated that the laser gain spectral region is located well below the BE resonance. [5] In this study, we demonstrate that the PL from defect-related states can be revealed by the careful and precise selection of the excitation energy (E ex ). We use the micro-photoluminescence excitation (PLE) spectroscopy to study the MAPbI 3 single crystals at 5 K temperature.…”

“…Nevertheless, this tail state plays an important role in lasing phenomenon, as it was demonstrated that the laser gain spectral region is located well below the BE resonance. [ 5 ]…”

“…Halide perovskite semiconductors are novel optical materials, which have found their perspective applications as an active medium in many optoelectronic devices: solar cells, [1] lightemitting diodes, [2] microlasers, [3][4][5][6][7] electromagnetic radiation detectors, [8] and others. In all these photophysical applications, the defect states, which are energy levels located within the bandgap of material, play a crucial role being either an undesired obstacle, or a mean of the material functionalization.…”

Tunable Plasmonic Random Laser Based on Emitters Coupled to Plasmonic Resonant Nanocavities of Silver Nanorod Arrays

“…[ 12 ] Nevertheless, controlling the emission wavelength of random lasers is still challenging due to the absence of optical cavity, which limits their applications in some fields such as medical detection, [ 13 ] photonic crystals, [ 14,15 ] and high‐precision sensors. [ 16,17 ] Therefore, emission characteristics of random lasers, especially the control strategies of the emission wavelengths, have attracted increasing attention, so far, various optical structures have been reported, including liquid crystals, [ 18 ] quantum dots, [ 19,20 ] graphene/semiconductor heterostructures, [ 21 ] polymer films, [ 22 ] disordered photonic crystal platform, [ 23 ] perovskite single crystals, [ 24 ] fibers, [ 5,25,26 ] and fiber gratings. [ 27 ] For example, Perumbiavil et al.…”

Substrate Effects on the Random Lasing Performance of Solution-Processed Hybrid-Perovskite Multicrystal Film

“…The green-emitting CH 3 NH 3 PbBr 3 (MAPbBr 3 ) is one of the most popular HOIP materials for investigations on lasing devices [18][19][20] because of its high emission efficiency, excellent stability, and easy synthesizing and processing advantages. MAPbBr 3 is a directbandgap material with a bandgap energy of about 2.3 eV, which may be excited to produce green light emission.…”