Realization of Single-Crystal Dye Lasers by Taming Charge Transfer in Molecular Self-Assemblies

The large library of organic dye molecules offers almost infinite possibilities for laser design, but still faces a great challenge in achieving pure dye aggregate lasers due to intermolecular quenching. Here, we report a kinetically controlled molecular self-assembly strategy to synthesize unconventional dye microcrystals for lasing. By increasing temperature, the dye self-assembly is transformed from thermodynamic to kinetic control. Unlike the thermodynamic microcrystal products incapable of lasing due to intermolecular charge-transfer-mediated excimer formation, the kinetic dye microcrystals have large intermolecular distances and weak intermolecular interactions, supporting highly efficient intramolecular charge-transfer monomer emission and low-threshold lasing. This work demonstrates single-crystal dye lasers, promising to unleash the full potential of laser dyes in solid-state lasers.