Two‐Photon Pumped Single‐Mode Lasing in CsPbBr3 Perovskite Microwire

Abstract Achieving high‐quality, frequency‐upconversion single‐mode lasing output is an important requirement for developing new nonlinear optoelectronic devices, such as on‐chip optical communication, nonlinear optical switches, and optical parametric amplifiers. Here, an individual CsPbBr 3 microwire prepared by the anti‐solvent method is served as both gain media and microresonator to achieve two‐photon pumped frequency upconversion single‐mode lasing with the side‐mode suppression ratio of 18 dB. Meanwhile, the refractive index of orthorhombic perovskite is theoretically calculated based on first principles, and determining its square whispering‐gallery oscillation type by combining with the plane wave model and the steady‐state oscillation conditions of laser. The extracted exciton binding energy of 33.15 meV higher than the thermal ionization energy of room temperature (≈26 meV) suggests that the as‐grown CsPbBr 3 microwires possess the capacity to achieve two‐photon pumped lasing output, as well further gaining deeper insights into the role of exciton‐phonon coupling in light emission.