Integrating Molecular Motions in Ternary Cocrystals for NIR‐II Photothermal Conversion

Organic photothermal conversion materials hold immense promise for various applications owing to their structural flexibility. Recent research has focused on enhancing near‐infrared (NIR) absorption and mitigating radiative transition processes. In this study, we have developed a viable approach to the design of photothermal conversion materials through the construction of ternary organic cocrystals, by introducing a third component as a molecular blocker and motion unit into a binary donor–acceptor system. Superstructural and photophysical properties of the ternary cocrystals were characterized using various spectroscopic techniques. The role of the molecular blocker in radical stabilization and photothermal conversion were demonstrated. Intriguingly, the motions of the entire pyrene molecules in the cocrystal have been observed by variable temperature single‐crystal X‐ray diffraction results. The excellent performance of ternary cocrystal as a photothermal material was validated through efficient NIR‐II photothermal and solar‐driven water evaporation experiments. The efficiency of water evaporation reached 88.7 %, with a corresponding evaporation rate of 1.29 kg m−2 h−1, representing excellent performance among pure organic small molecular photothermal conversion materials. Our research underscores the introduction of molecular blockers and motion units to stabilize radicals and produce outstanding photothermal conversion materials, offering new pathways for developing efficient and stable photothermal conversion materials.