Spontaneous Creation of Anisotropic Polymer Crystals with Orientation-Sensitive Birefringence in Liquid Drops

It remains a grand challenge to prepare anisotropic crystal superstructures with sensitive optical properties in polymer science and materials field. This study demonstrates that semicrystalline polymers develop into anisotropic hollow spherulitic crystals spontaneously at interfaces of liquid drops. In contrast to conventional spherulites with centrosymmetric optics and grain boundaries, these anisotropic spherulitic crystals have vanished boundary defects, tunable aspect ratios, and noncentrosymmetric, orientation-sensitive birefringence. The experimental finding is elaborated in poly(l-lactic acid) crystals and is further verified in a broad class of semicrystalline polymers, irrespective of molecular chirality, chemical constitution, or interfacial modification. The facile methods and general mechanism revealed in this study shed light on developing new types of optical microdevices and synthesis of anisotropic semicrystalline particles from liquid emulsions.