Tailoring the Energy Levels and Cavity Structures toward Organic Cocrystal Microlasers

Organic cocrystals with unique energy-level structures are potentially a new class of materials for the development of versatile solid-state lasers. However, till now, the stimulated emission in cocrystal materials remains a big challenge possibly because of the nonradiative charge-transfer (CT) transitions. Here, for the first time, we report organic cocrystal microlasers constructed by simultaneously tailoring the energy levels and cavity structures based on the intermolecular halogen-bonding interactions. The intermolecular interactions triggered different self-assembly processes, resulting in distinct types of high-quality resonant microcavities. More importantly, the halogen-bonding interactions alleviated intermolecular CT and thus brought about a favorable four-level energy structure for the population inversion and tunable lasing in the cocrystals.