Near-Infrared Microlasers from Self-Assembled Spiropyrane-Based Microsphercial Caps

Near-infrared (NIR) microlasers play a significant role in telecommunication and biomedical tissue imaging. However, it remains a big challenge to realize NIR microlasers because of the difficulty in preparing highly efficient NIR luminescent materials and perfect optical resonators. Here, we propose a molecular design strategy to creatively realize the first spiropyrane (SP)-based NIR microlasers with low threshold from self-assembled microsphercial caps. The tetraphenylethylene (TPE) moiety with a highly twisted conformation provides a large free volume to facilitate the photoisomerization process of SP and enhance NIR emission of merocyanine in the solid state. Moreover, self-assembled TPE–SP microsphercial caps simultaneously serve as gain media and resonant microcavities, providing optical gain and feedback for NIR laser oscillations with a low threshold (3.68 μJ/cm 2 ). These results are beneficial for deeply understanding the SP microstructures-lasing emission characteristic relationship and provide a useful guideline for the rational molecular design of NIR microlasers with special functionalities.