“…12,13 These factors, together with the large photo-induced structural change, determine the specific application profile for, e.g., tailored surface functionalisation, light-induced material deformation, surface-relief formation, nonlinear optics, or charge separation in organic photovoltaic and ferroelectric materials. 7,[14][15][16][17][18][19] DR1 is of particular practical interest because of its hydroxy group, which can be employed as a covalent linker, for example by functionalizing it with a methacrylate group for embedding in a polybutylmethacrylate (PBMA) matrix. 20 In contrast to plain AB, where the photoisomerisation mechanism is well studied, [21][22][23][24][25][26][27][28][29][30][31] the molecular dynamics of DR1 and related push-pull substituted ABs following excitation in the strong visible ππ*-type absorption band still remains controversial, despite several spectroscopic 32,33 and time-resolved 10,11,34,35 experimental studies and theoretical calculations.…”