Control of Imine Exchange Kinetics with Photoswitches to Modulate Self‐Healing in Polysiloxane Networks by Light Illumination

Various aldehyde‐containing photoswitches have been developed whose reactivity toward amines can be controlled externally. A thermally stable bifunctional diarylethene, which in its ring‐closed form exhibits imine formation accelerated by one order of magnitude, was used as a photoswitchable crosslinker and mixed with a commercially available amino‐functionalized polysiloxane to yield a rubbery material with viscoelastic and self‐healing properties that can be reversibly tuned by irradiation.