Dataset generated from the work "Unraveling Pathway Complexity in Photoreversible Supramolecular Hydrogels: Real-Time Visualization and Sub-Micrometric Photopatterning"

Figure 1. a, Scheme of the instrumentation employed to orthogonally induce the phototriggered isomerization while capturing the emission from the probe. The absorption spectra of an aqueous solution of Z-AAP (green), E-AAP (purple), and the absorption (light orange) and emission (dark orange) spectrum of the probe AQui in DMSO are depicted in the inset, with the corresponding chemical structure of the probe and the gelators’ both isomers. b and c, Phototriggered disassembly and reassembly of a GdL-prepared AAP hydrogel dyed with AQui (50µM, λex 561nm). b, Disassembly irradiation time-lapse [c.a. 5’]. c, Reassembly irradiation time-lapse [total irradiation time 45’. The last frame was irradiated a total of 15’ without interruption to check for scar disappearance.] For both rows, the section irradiated with 375 nm or 450 nm is highlighted with a colored square. Figure 2. Photopatterning of the University of Granada acronym (UGR) inside the gel matrix employing a 375 nm laser-light source. AAP hydrogel sample was prepared by GdL acidification and visualized by dying with AQui (50µM, λex 561nm). Figure 3. FLIM imaging of AQui (50µM, lex = 561nm) in a HCl-prepared AAP gel, during (a) phototriggered disassembly and (b) reassembly. Every frame was taken after 3’of irradiation with the corresponding 375 nm or 450 nm light source. The pseudocolor scale indicates the average τf of AQui and its relationship with the environment polarity is indicated for clarity. (c) Decay time distributions computed from the irradiated square (highlighted in dashed colored lines) over the whole cycle of disassembly and reassembly. Figure 4. Molecular Dynamics simulations on polarity evolution of Z-AAP and E-AAP aggregates. a-d, Selected supramolecular clusters generated during the molecular dynamics simulation of the self-assembly of systems composed of different proportions of E-AAP and Z-AAP isomers (a: 100% E-AAP, b: 80% E-AAP / 20% Z-AAP, c: 20% E-AAP / 80% Z-AAP, d: 100% Z-AAP) and one molecule of AQui. e, Selected structures extracted from the first and last stages of the MD simulation performed over a portion of the crystalline structure of AAP in water. f and g, Boxplots (Boxes represent the interquartile range (25th to 75th percentiles). The horizontal full line indicates the median, while the white rhomboid represents the mean. Whiskers extend to the maximum and minimum data points within 1.5 times the interquartile range. Outliers’ data points lying beyond this range are plotted individually) computed from the total dipole moment calculated during the MD simulation of a crystalline portion in water (f) and from simulations over systems with increase proportion of the Z-AAP isomer (g). Figure 5. SAXS during AAP hydrogel photoreversion. Scatterers radius (R), and fractal correlation length (ξ) parameters obtained from modeled SAXS data of disassembled gel (sol state) during a complete reassembly-disassembly-reassembly cycle. Time intervals during bulk, 520 nm irradiation are back-shaded in green, whereas the time interval with bulk, 365 nm -irradiation is back-shaded in purple. Figure S1. Confocal images of AQui (50µM, lex = 561nm) in a HCl-prepared AAP hydrogel, during (a) phototriggered disassembly and (b) reassembly. Every frame was taken after 3’of irradiation with the corresponding 375 nm or 450 nm light source. Figure S2. SAXS during pH-induced supramolecular polymerization. Scatterers radius (R), fractal correlation length (ξ) and fractal dimension (DFr) parameters obtained from modeled SAXS data for a GdL-prepared AAP hydrogel during supramolecular polymerization.