Kominko Yuliia, Sabisch Sebastian, Kanak Andrii, Dubenska Lidiia, Cherniukh Ihor, Klimpel Matthias, Liu Xuqi, Tsarev Sergey, Boehme Simon C, Matt Gebhard J, Rainò Gabriele, Kovalenko Maksym V, Yakunin Sergii
ETH Zürich, Department of Chemistry and Applied Biosciences, Laboratory of Inorganic Chemistry, Vladimir-Prelog-Weg 1, Zürich CH-8093, Switzerland.
Empa-Swiss Federal Laboratories for Materials Science and Technology, Laboratory for Thin Films and Photovoltaics, Überlandstrasse 129, Dübendorf CH-8600, Switzerland.
ACS Nano. 2025 Aug 19;19(32):29216-29227. doi: 10.1021/acsnano.5c03771. Epub 2025 Jul 16.
Semiconductor nanocrystals are widely investigated as tunable quantum emitters due to their composition-, size- and shape-dependent optical properties, and they find applications in various optoelectronic devices, including lasers. However, in compact films, insulating ligands often limit heat and charge transport. Improving the heat management, for example, by removing ligands, can significantly enhance the operational stability at high excitation densities required for laser devices. Here, we report the synthesis, structural characterization, and stable high optical gain of ligand-free nanocrystalline thin films obtained through single-source thermal evaporation of CsPbX (X = Cl, Br). This deposition method is robust, scalable, and compatible with industrial processes. A slow postdeposition crystallization process under nitrogen yields compact, smooth, and optically uniform thin films with nanocrystalline grains with weakly confined optical features and pronounced excitonic resonances. The films show composition-tunable (430-545 nm), low-threshold (. 2 μJ cm) amplified spontaneous emission, with a high net modal gain of 890 cm measured for the pure CsPbBr composition. Due to the enhanced heat dissipation enabled by the optimized film morphology, the operation stability under ambient conditions surpasses 180 million laser shots (.., 5 h of continuous operation), with merely ∼8% degradation, indicating that thermally evaporated perovskite thin films are promising optical gain media for room-temperature lasing applications.
半导体纳米晶体因其与组成、尺寸和形状相关的光学特性而被广泛研究作为可调谐量子发射体,并且它们在包括激光器在内的各种光电器件中得到应用。然而,在致密薄膜中,绝缘配体常常会限制热和电荷传输。例如,通过去除配体来改善热管理,可以显著提高激光器件所需的高激发密度下的运行稳定性。在此,我们报道了通过CsPbX(X = Cl、Br)的单源热蒸发获得的无配体纳米晶薄膜的合成、结构表征以及稳定的高光增益。这种沉积方法坚固耐用、可扩展且与工业工艺兼容。在氮气气氛下缓慢的沉积后结晶过程产生了致密、光滑且光学均匀的薄膜,其纳米晶粒具有弱受限的光学特征和明显的激子共振。这些薄膜显示出组成可调谐(430 - 545 nm)、低阈值(. 2 μJ cm)的放大自发发射,对于纯CsPbBr组成测量得到的净模态增益高达890 cm。由于优化的薄膜形态实现了增强的热耗散,在环境条件下的运行稳定性超过1.8亿次激光脉冲(..,连续运行5小时),仅有约8%的降解,这表明热蒸发钙钛矿薄膜是用于室温激光应用的有前景的光学增益介质。