Organic Crystals with Response to Multiple Stimuli: Mechanical Bending, Acid‐Induced Bending and Heating‐Induced Jumping

Multiple stimuli-responsive molecular crystals are attracting extensive attentions due to their potential as smart materials, such as molecular machines, actuators, and sensors. However, the task of giving a single crystal multiple stimuli-responsive properties remains extremely challenging. Herein, we found two polymorphs (Form O and Form R) of a Schiff base compound, which could respond to multiple stimuli (external force, acid, heat). Form O and Form R have different elastic deformability, which can be attributed to the differences in the molecular conformation, structural packing and intermolecular interactions. Moreover, both polymorphs exhibit reversible bending driven by volatile acid vapor, which we hypothesize is caused by reversible protonation reaction of imines with formic acid. In addition, jumping can be triggered by heating due to the significant anisotropic expansion. The integration of reversible bending and jumping into one single crystal expands the application scope of stimuli-responsive crystalline materials.