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Magnetic field processing is promising for directing and enhancing self-assembly of diamagnetic block copolymers (BCPs) via domain alignment, but is typically limited to high field strengths and few polymer chemistries. Herein, a novel magnetic field-induced ordering mechanism distinct from domain alignment is demonstrated in aqueous, spherical BCP micelles. Here, low-intensity magnetic fields (B< 0.5 T) induce an anomalous disorder-to-order transition, accompanied by a several order-of-magnitude increase in shear modulus-- effectively transforming a low viscosity liquid into an ordered soft solid. The induced moduli are orders of magnitude larger than those resulting from thermally-induced ordering. Further magnetization induces cubic-to-cylinder order-to-order transitions. Comprehensive characterization via magnetorheology, small- and wide-angle X-ray scattering, differential scanning calorimetry, and vibrational spectroscopy reveals a significant reduction in micelle size and aggregation number relative to zero-field temperature- or concentration-induced ordering, suggesting that B-fields strongly alter polymer-solvent interactions. This extraordinary BCP ordering strategy enables discovery of structures and d-spacings inaccessible via traditional processing routes, thus providing a new platform for developing advanced materials with precisely-controlled features. 

Abstract Natural materials are highly organized, frequently possessing intricate and sophisticated hierarchical structures from which superior properties emerge. In the wake of biomimicry, there is a growing interest in designing architected materials in the laboratory as such structures could enable myriad functionalities in engineering. Yet, their fabrication remains challenging despite recent progress in additive manufacturing. In particular, soft materials are typically poorly suited to form the requisite structures consisting of regular geometries. Here, a new frugal methodology is reported to fabricate pixelated soft materials. This approach is conceptually analogous to the watershed transform used in image analysis and allows the passive assembly of complex geometries through the capillary‐mediated flow of curable elastomers in confined geometries. Emerging from sources distributed across a Hele–Shaw cell consisting of two parallel flat plates separated by an infinitesimally small gap, these flows eventually meet at the “dividing lines” thereby forming Voronoi tesselations. After curing is complete, these structures turn into composite elastic sheets. Rationalizing the fluid mechanics at play allows the structural geometry of the newly formed sheets to be tailored and thereby their local material properties to be tuned.