Surfaces of classical spherical liquid droplets are isotropic, promoting the random distribution of surface-adsorbed molecules¹. Here we demonstrate a counterintuitive temperature-controlled self-assembly of well-defined and highly ordered patterns of surface-adsorbed fluorescent molecules on the surfaces of water-suspended spherical oil droplets. These patterns are induced by precisely self-positioned, topology-dictated structural defects in a crystalline monolayer covering these droplets’ surfaces over a wide temperature range. We elucidate the pattern formation mechanism, visualize the defects’ positions and map the stress fields within the surface crystal. The observed phenomena provide insights into the interfacial freezing effect on curved surfaces, enable precise positioning of functional ligands on droplets for their self-assembly into higher-hierarchy structures^2,3,4,5,6 and may also play an important role in vital protein positioning on cell membranes⁷ and morphogenesis^8,9,10,11,12.

经典球形液滴的表面是各向同性的，促进表面吸附分子的随机分布¹. 在这里，我们展示了水悬浮球形油滴表面上定义明确且高度有序的表面吸附荧光分子图案的违反直觉的温度控制自组装。这些图案是由在很宽的温度范围内覆盖这些液滴表面的结晶单层中的精确自定位、拓扑决定的结构缺陷引起的。我们阐明了图案形成机制，可视化缺陷的位置并绘制表面晶体内的应力场。观察到的现象提供了对曲面上界面冻结效应的见解，使功能配体能够精确定位在液滴上，以便它们自组装成更高层次的结构^2,3,4,5,6并且还可能在细胞膜上的重要蛋白质定位⁷和形态发生^8,9,10,11,12中发挥重要作用。