Colloidal crystals have been tailored in a format of microspheres to use them as a building block to construct macroscopic photonic surfaces. However, the polycrystalline grains grown from the spherical surface usually exhibit low reflectivity. Although single-crystalline microspheres have been produced, it is difficult to control the crystal orientation. Here, we design spherical microcapsules with density anisotropy that contain single-crystalline grains along the heavy side. The microcapsules spontaneously align to have a heavy side down under the action of gravity and display a bright and uniform reflection color from the entire surface of the grains. Key to the success is the use of gentle centrifugal force to initiate nucleation and grow single-crystalline grains from the heavy side through depletion attraction. The microcapsules have density anisotropy due to the heterogeneity of the shell thickness, which causes them to self-align under centrifugation. At the same time, particles are accumulated on the heavy side, which produces many tiny grains on the heavy side immediately after the centrifugation. With controlled depletion attraction among particles, only a few grains survive during postincubation through Ostwald ripening, and one or a few giant single-crystalline grains are finally produced along the heavy side of each microcapsule.
Keywords: centrifugation; colloidal crystal; colloids; depletion; structural color.