Multiphoton-Pumped Highly Polarized Polariton Microlasers from Single Crystals of a Dye-Coordinated Metal–Organic Framework

Room-temperature, low-threshold, photostable, cost-effective, efficient, miniaturized, and all-solid-state lasers are highly desirable in many technological and medicinal applications. Here, an archetypical dye laser is introduced, with the above attributes, based on single-crystalline microplates of a dye-coordinated metal–organic framework (MOF) without an external cavity, holding a potential to be the next-generation laser. With an exciton–polariton lasing mechanism combined with large multiphoton absorption cross sections, the lasing thresholds of the three microplates are in the range from 0.34 to 0.12 µJ cm−2 under various optical pumping schemes. The lasing threshold is observed to be reduced with an increment in the order of optical nonlinearity involved in the pumping scheme. Lasing at an extreme-red region is demonstrated, with a high photostability (with a drop in lasing output as low as 25% after 1.8 × 106 cycles), a large degree of polarization (up to 92%), and an excellent conversion efficiency (up to 12%), thereby realizing a crucial milestone in the field of laser technology.