Picosecond Random Lasing Based on Three-Photon Absorption in Organometallic Halide CH₃NH₃PbBr₃ Perovskite Thin Films

Abstract

Organometallic halide perovskites have been demonstrated to be very promising for nonlinear optics and practical frequency upconversion devices in integrated photonics. In this work, high quality organometallic halide CH 3 NH 3 PbBr 3 perovskite thin films were synthesized through a solution-based one-step spin-coating method. With femtosecond optical pumping at 1300 nm, frequency-upconverted random lasing (RL) from the bromide perovskite films were achieved via three-photon (3P) absorption processes. The RL spectra show no spikes due to the large scattering mean-free path in the perovskite crystals, meaning the incoherent RL emission with incoherent feedback. In comparison with the one-photon pumped situation, it is found that both the two-photon and 3P excitations are more effective in reducing the RL threshold, despite the low conversion efficiency of their nonlinear multiphoton schemes. Moreover, the time-and spectralresolved lasing characteristics of the laser pulses were systematically explored by time-resolved photoluminescence based on an optical Kerr-gate method. The measured ultrashort 3.1 ps output pulse is the shortest one that has been observed so far in bromide perovskite random lasers, without any postprocessing. In addition, wavelength dependence of the pulse width and delay time of the RL pulses were clearly demonstrated, and could be unravelled by intraband carrier relaxation dynamics, which is an important physical mechanism in ultrafast lasers. Our results demonstrate that organometallic halide perovskites are excellent gain medium for high-performance frequency upconversion random lasers and have great potential for use in gain-switched semiconductor lasers with ultrashort output pulses and tunable emission wavelengths across the entire visible spectrum.

Giant Nonlinear Optical Response in Triple Cation Halide Mixed Perovskite Films

“…Overall, the β values of TCMHP film are significantly higher than those of MAPbI 3 film and an order of magnitude higher near to the peak intensity of 35 GW cm −2 . While we could not observe the 3PA response for MAPbI 3 film, the obtained γ values of TCMHP film for each intensity are much larger than those of other perovskite film, micro‐/nanocrystals, and single crystal 15,16,56–60. The β and γ values of various types of perovskite materials reported in previous literatures and current study are summarized in Table 1 .…”

2D Layered Materials: Synthesis, Nonlinear Optical Properties, and Device Applications

“…Third‐order optical nonlinearity plays a key role in nonlinear photonic devices . In this section, we will briefly discuss two important nonlinear properties of layered materials, namely Kerr effect and nonlinear absorption, and review their recent research history.…”

Lead-Free Perovskites for Lighting and Lasing Applications: A Minireview

“…The main burst in this scientific area of utilizing the perovskite materials in lightning and lasing applications was caused by the synthesis of highly luminescent perovskite materials with QY above 80% [61,87]. At the present moment, the lasing perovskite materials possess wide range of morphology, including thin films [82,84,88,89,90,91,92], microstructures such as cubes [83,93,94,95,96,97], plates [81,98,99,100], wires [99,101,102,103,104], spheres [85,95,105], pyramids [97], nanosheets [106,107], microdisks [108,109], and quantum confined materials such as 2D R-P [110,111,112,113] and NCs [114,115,116,117], including NCs in glasses [118] and polymers [119]. Also, for the enhancement of the device performance, the perovskite materials can be patterned by ion beam lithography [109], laser ablation [108], or imprinting methods [89,120], and can be applied on the initially patterned substrates [81,90].…”