Dimension Tailoring of Quasi-2D Perovskite Films Based on Atmosphere Control Toward Enhanced Amplified Spontaneous Emission

Quasi-two-dimensional (Q2D) perovskite films have garnered significant attention as novel gain media for lasers due to their tunable bandgap, narrow linewidth, and solution processability. Q2D perovskites endowed with intrinsic quantum well structures demonstrate remarkable potential as gain media for cost-effective miniaturized lasers, owing to their superior ambient stability and enhanced photon confinement capabilities. However, the mixed-phase distribution within Q2D films constitutes a critical determinant of their optical properties, exhibiting pronounced sensitivity to specific fabrication protocols and processing parameters, including annealing temperature, duration, antisolvent volume, injection timing, and dosing rate. These factors frequently lead to broad phase distribution in Q2D perovskite films, thereby inducing incomplete exciton energy transfer and multiple emission peaks, while simultaneously making the fabrication processes intricate and reducing reproducibility. Here, we report a novel annealing-free and antisolvent-free method for the preparation of Q2D perovskite films fabricated in ambient atmosphere. By constructing a tailored mixed-solvent vapor atmosphere and systematically investigating its regulatory effects on the nucleation and growth processes of film via in situ photoluminescence spectra, we successfully achieved the fabrication of Q2D perovskite films with large n narrow phase distribution characteristics. Due to the reduced content of small n domains, the incomplete energy transfer from small n to large n phases and the carriers’ accumulation in small n can be greatly suppressed, thereby suppressing the trap-assistant nonradiative recombination and Auger recombination. Ultimately, the Q2D perovskite film showed a single emission peak at 519 nm with the narrow full width at half maximum (FWHM) of 21.5 nm and high photoluminescence quantum yield (PLQY) of 83%. And based on the optimized Q2D film, we achieved an amplified spontaneous emission (ASE) with a low threshold of 29 μJ·cm⁻², which was approximately 60% lower than the 69 μJ·cm⁻² of the control film.