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We have investigated PLLA crystallization in lamellae-forming PS-b-PLLAconfined to straight cylindrical nanopores under weak confinement (nanoporediameter D / equilibrium PS-b-PLLA period L0 larger than 4.8). Molten PS-b-PLLApredominantly forms concentric lamellae along the nanopores, but intertwinedhelices occur even for D/L0 = 7.3. Quenching PS-b-PLLA melts below TG(PS)results in PLLA cold crystallization strictly confined by the vitrified PSdomains. Above TG(PS), PLLA crystallization is templated by the PS-b-PLLA meltdomain structure in the nanopore centers, while adsorption on the nanoporewalls stabilizes the outermost cylindrical PS-b-PLLA shell. In between, thenanoscopic PS-b-PLLA melt domain structure apparently ripens to reducefrustrations transmitted from the outermost immobilized PS-b-PLLA layer. Theonset of PLLA crystallization catalyzes the ripening while transient ripeningstates are arrested by advancing PLLA crystallization. Certain helicalstructure motifs persist PLLA crystallization even if PS is soft. The directionof fastest PLLA crystal growth is preferentially aligned with the nanopore axesto the same degree as for PLLA homopolymer, independent of whether PS isvitreous or soft.

Semicrystalline block copolymers in rigid confining nanopores