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Polyion complex (PIC) formation is an attractive method for obtaining molecular assemblies owing to their facile fabrication process in aqueous media, but more insights are required in order to control the higher‐dimensional structures of polypeptide‐based PICs. Herein, the PIC formation behavior of oppositely charged homochiral polypeptides, poly‐l‐lysine and poly(ethylene glycol)‐b‐poly(l‐glutamate)...
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