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Living organisms are molecular systems with self-sustained dynamics viaenergy conversion through molecular cooperation, resulting in highly complexmacroscopic behaviors. Construction of such autonomous macroscopic dynamics ata molecular system level remains one of the central challenges in the field ofchemistry. Looking further ahead, constructing motile systems that can receiveexternal information and adapt their autonomous behavior represents the nextfrontier towards newly functional molecular devices such as microrobots. Inthis study, we focused on a light-driven self-oscillatory crystal that exhibitscontinuous flipping motion under constant light irradiation. We experimentallyevaluated the oscillation frequency of the crystal under polarized light andconfirmed the validity of our previously proposed mechanism, and clarified therequirements for self-oscillation. Based on this mechanism, we constructed amathematical model that demonstrates the motion of the crystal itself. Themodel revealed that diverse oscillatory behaviors at the macroscopic level canemerge due to small differences in conditions even when the underlyingmolecular-level processes are identical. Furthermore, we found that theoscillatory behavior depended on the state generated by the previously appliedlight. This suggests that a memory effect contributes to the complex motion ofthe crystal.

Emergent Complexity in a Light-Driven Self-Oscillatory Crystal: A Molecular Perspective on Autonomous Behavior and Stimulus-Modulated Motion