Realization of Single-Crystal Dye Lasers by Taming Charge Transfer in Molecular Self-Assemblies
Wanting Dong, Chunhuan Zhang, Haiyun Dong, Zhonghao Zhou, Jiannian Yao, Yong Sheng Zhao
Abstract
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.