A Rhodamine‐Spiropyran Conjugate Empowering Tunable Mechanochromism in Polymers under Multiple Stimuli

Abstract Mechanochromic functionality realized via the force‐responsive mechanophores in polymers has great potential for damage sensing and information storage. Mechanophores with the ability to recognize multiple stimuli for tunable chromic characteristics are highly sought after for versatile sensing ability and color programmability. Nevertheless, the majority of mechanophores are based on single‐component chromophores with limited sensitivity, or require additional fabrication technology for multi‐modal chromism. Here, we report a novel multifunctional mechanophore capable of vividly detectable and tunable mechanochromism in polymers. This synergistic optical coupling relies on strategically fusing rhodamine and spiropyran (Rh−SP), and tethering polymer chains on both subunits. The mechanochromic behaviors of the Rh−SP‐linked polymers under sonication and compression are thoroughly evaluated in response to changes in force and the light‐controlled relaxation process. Non‐sequential ring‐opening of the two subunits under force is identified, endowing high‐contrast mechanochromism. Light‐induced differential ring‐closing reactions of the two subunits, together with the acidichromism of the SP moiety, are employed to engineer elastomers with programmable and wide‐spectrum colors. Our work presents an effective strategy for highly appreciable and regulable mechanochromic functionality, and also provides new insights into the rupture mechanisms of π‐fused mechanophores, as well as how the stimuli history controls stress accumulation in polymers.