“…To date, photoswitchable adhesives have been developed by utilizing a variety of photoresponsive systems including large structural changes of azobenzenes, − conjugation changes of diarylethenes, , dimerization of anthracenes, − photothermal effects of supramolecular motifs and dyes, − and other reactions. − Reversibly switchable polymer adhesives are particularly attractive because of their strong adhesion and recyclability. Similarly, large polarity changes in the photoisomerization between noncharged spiropyran (SP) and zwitterionic merocyanine (MC) seem highly suitable for photocontrol of adhesion (Figure a) , because molecular polarity and related interactions between adhesives and substrate surfaces are dominant factors to generate adhesion force. − The dipole moment (μ) drastically changes between 4–6 D for SP and 14–18 D for MC. , However, to the best of our knowledge, SP has been only used as additives in polymer adhesives ,, or as low-molecular-weight adhesives . In the additive approach, there is a concern about phase separation between a polymer matrix and SP small molecules particularly after isomerization to MC due to the large difference in the polarity between them, which degrades the performance and undermines the reliability.…”