The Special “Morse Code” between Solvent Polarity and Morphology Flexibility in a POSS–Dendrimer Supramolecular System

An amazing phenomenon of the relative magnitude of modulus of two liquid‐crystal (LC) gels is found inverted under/above their phase transition temperature T LC‐iso , which is further proved to be caused by their diverse morphology flexibility. By testing the polarity of two LCs, gelator POSS‐G1‐Boc (POSS=polyhedral oligomeric silsesquioxane) was discovered to self‐assemble into more flexible structures in a relatively low polar LC, whereas more rigid ones are formed in higher polar LC. Hence, a fitting function to connect morphology flexibility with solvent polarity was established, which can even be generalized to a number of common solvents. Experimental observations and coarse‐grained molecular dynamics simulations revealed that solvent polarity mirrors a “Morse code”, with each “code” corresponding to a specific morphology flexibility.