Bioinspired Dynamic Remodeling of Excited-State Pathways for High-Performance Stimuli-Responsive Materials.

Abstract

Artificial stimuli-responsive systems play a pivotal role in driving rapid advances at the frontiers of science and technology. However, existing systems are commonly constrained by "single fixed reaction pathways", making it difficult to replicate the synergistic integration of low-energy activation, multistable states, and excellent cycling reversibility of biological processes. Inspired by the precise regulation of water in biological photoreceptors, this study introduces a "water-assisted excited-state pathway remodeling" (WEPR) mechanism. By designing photoswitchable molecules that functionally mimic rhodopsin chromophores, we employ environmentally benign water as a dynamic regulatory factor to achieve intelligent switching of reaction pathways between high- and low-barrier channels. Materials developed based on this mechanism exhibit exceptional bistability (>7 days), excellent cycling reversibility (>100 cycles), and remarkable long-term stability (>2 years). These properties make it a compelling candidate for technologies such as dynamic information encryption and sustainable displays featuring on-demand visualization and instant erasure. Furthermore, leveraging the multiscale similarities between our molecular switch system and biological visual pigments, the potential role of water in visual perception is discussed. This work not only provides a bioinspired paradigm for developing novel intelligent materials but also offers new insights into the fundamental mechanisms of color perception.