Two‐Photon Pumped CH₃NH₃PbBr₃ Perovskite Microwire Lasers

Abstract

Solution‐processed lead halide perovskites have shown good applicability in both solar cells and microlasers. Very recently, the nonlinear properties of perovskites have attracted considerable research attention. Second harmonic generation and two‐photon absorption have been successfully demonstrated. However, perovskite devices based on these nonlinear properties, such as micro‐ and nanolasers have thus far not been fabricated. Here we demonstrate two‐photon pumped microlasers from CH3NH3PbBr3 perovskite microwires. These CH3NH3PbBr3 perovskite microwires are synthesized through a one‐step solution precipitation method and dispersed on a glass substrate. Under optical excitation at 800 nm, two‐photon pumped lasing action with periodic peaks is successfully observed at around 546 nm. The obtained quality (Q) factors of the two‐photon pumped microlasers are around 682, and the corresponding thresholds are about 674 µJ cm‐2. Both the Q factors and thresholds are comparable to conventional whispering‐gallery modes in two‐dimensional polygon microplates. This work is the first demonstration of two‐photon pumped microlasers in CH3NH3PbBr3 perovskite microwires. We believe our finding will significantly expand the application of perovskites in low‐cost nonlinear optical devices, such as optical limiters, optical switches, and biomedical imaging devices.

Room temperature three-photon pumped CH3NH3PbBr3 perovskite microlasers

“…For the wavelength range above 550 nm, the linearly material absorption is negligibly small. All these experimental observations are consistent with the previous reports very well131420. The situation changed dramatically when the sample was illuminated with ultrashort laser pulses (100 fs, 1 KHz, see Figure S2 in supplemental information).…”

“…Within past two years, a number of nonlinear effects have been experimentally demonstrated, e.g. two-photon absorption8910, two-photon pumped photoluminescence (PL)8, two-photon pumped amplified spontaneous emission (ASE)13, and two-photon pumped lasers14. Very recently, three-photon pumped PL and amplifications have also been reported15.…”

Colloidal lead halide perovskite nanocrystals: synthesis, optical properties and applications

“…High PLQY is one of the main advantages of the colloidal perovskite NCs, prompting researchers to perform intensive investigations for their use as optical gain media for lasing. 13,34,36,37,[106][107][108] Zhu et al 13 have demonstrated wavelengthtunable lasing from single-crystalline organic-inorganic lead perovskite NWs with low thresholds (~220 nJ cm − 2 ) and high quality factors of Q~3600 (Figures 9a-c). The narrowing of the FWHM in the PL spectra by two orders of magnitude above an excitation fluence threshold presented a clear sign of lasing (Figure 9b).…”

“…Other morphologies of hybrid perovskites such as microdisks have also been shown to produce efficient optical gain. 107,109 All-inorganic perovskite NCs, with high PLQYs and greater stability, have also been explored as a potential optical gain medium. Kovalenko and colleagues 37 demonstrated wavelength tunable low-threshold ASE and lasing from colloidal caesium lead halide perovskite NCs at room temperature (Figures 9d-g).…”

Acoustic-optical phonon up-conversion and hot-phonon bottleneck in lead-halide perovskites

“…A strong phonon bottleneck effect is helpful to establish a long-lived hot carrier population, which is critical to achieve a working hot carrier photovoltaic device161718 and break the Shockley–Queisser limit19 for photovoltaic energy conversion. Hot carrier properties of materials are also important in photodetection20, photocatalysis21 and light emission2223 to improve the power efficiency and carrier dynamics, especially in high-power optoelectronic applications such as lasing242526.…”