Sequential‐Stimuli Induced Stepwise‐Response of Pyridylpyrenes

Abstract Stimuli‐responsive materials, especially multi‐stimuli‐responsive materials, can sense external stimuli such as light, heat, and force, have shown great potential in drug delivery, data storage, encryption, energy‐harvesting, and artificial intelligence. Conventional multi‐stimuli‐responsive materials are sensitive to each independent stimulus, causing losses in the diversity and accuracy of the identification for practical application. Herein, a unique phenomenon of sequential‐stimuli induced stepwise‐response generated from elaborately designed single‐component organic materials is reported, which shows large bathochromic shifts up to 5800 cm⁻¹ under sequential stimuli of force and light. In contrast to multi‐stimuli‐responsive materials, the response of these materials strictly relies on the sequence of stimuli, allowing logicality, rigidity, and accuracy to be integrated into one single‐component material. The molecular keypad lock is built based on these materials, pointing promising to a future for this logical response in significant practical applications. This breakthrough gives a new drive to classical stimuli‐responsiveness and provides a fundamental design strategy for new generations of high‐performance stimuli‐responsive materials.