Low Threshold and Ultrastability of One-Step Air-Processed All-Inorganic CsPbX3 Thin Films toward Full-Color Visible Amplified Spontaneous Emission

ACS Appl Mater Interfaces. 2022 May 31. doi: 10.1021/acsami.2c02577. Online ahead of print.

Abstract

All-inorganic perovskites (CsPbX3) with the merits of high stability and remarkable optical gain property are attractive for achieving on-chip coherent light sources. Unfortunately, traditional solution-processed CsPbX3 films suffer from inevitable poor surface integrity and pinhole defects, severely hindering their optical properties. Here, from the perspective of precursor solution chemistry, we use an ionic liquid solvent methylammonium acetate (MAAc) to fabricate compact, pinhole-free, and smooth CsPbX3 thin films in a one-step air process without antisolvent treatment. Optically pumped amplified spontaneous emission (ASE) with a straightforward visible spectral tunability (418-725 nm) is achieved under both nanosecond and femtosecond laser excitation. For the representative CsPbBr3 films, the threshold reaches down to 11.4 μJ cm-2 under nanosecond laser pumping, which is comparable to the value under one-photon femtosecond pumping. The long gain lifetime up to 258.2 ps is revealed by transient absorption spectroscopy. Most importantly, the films show excellent optical stability and humidity stability with no obvious degradation under the pulsed laser irradiation for more than 210 min, stable ASE output under 95% high humidity, and conspicuous ASE after 1000 h of storage in air condition without encapsulation. These results demonstrate that the method of fabricating inorganic perovskite films with an ionic liquid solvent is promising in developing high-performance full-color visible lasers.

Keywords: amplified spontaneous emission; cesium lead halide perovskites; ionic liquid solvent; nanosecond laser pumping; wavelength-tunable.