Chemistry and Physics of Materials Unit, Jawaharlal Nehru Centre for Advanced Scientific Research, Bangalore 560064, India.
Department of Physics, Indian Institute of Science, Bangalore 560012, India.
Proc Natl Acad Sci U S A. 2022 Aug 9;119(32):e2206470119. doi: 10.1073/pnas.2206470119. Epub 2022 Aug 3.
Melting in two-dimensional flat space is typically two-step and via the hexatic phase. How melting proceeds on a curved surface, however, is not known. Topology mandates that crystalline particle assemblies on these surfaces harbor a finite density of defects, which itself can be ordered, like the icosahedral ordering of 5-coordinated disclination defects on a sphere. Thus, melting even on a sphere, the simplest closed surface, involves the loss of both crystalline and defect order. Probing the interplay of these two forms of order, however, requires a system in which melting can be performed in situ, and this has not been achieved hitherto. Here, by tuning interparticle interactions in situ, we report an observation of an intermediate hexatic phase during the melting of colloidal crystals on a sphere. Remarkably, we observed a precipitous drop in icosahedral defect order in the hexatic phase where the shear modulus is expected to vanish. Furthermore, unlike in flat space, where disorder can fundamentally alter the nature of the melting process, on the sphere, we observed the signature characteristics of ideal melting. Our findings have profound implications for understanding, for instance, the self-assembly and maturation dynamics of viral capsids and also phase transitions on curved surfaces.
在二维平面空间中,熔融通常是分两步进行的,且经过六方相。然而,在曲面上熔融是如何进行的还不得而知。拓扑学要求这些表面上的晶体颗粒组装体具有有限密度的缺陷,这些缺陷本身可以像五配位的扭结缺陷在球体上的二十面体有序排列一样有序。因此,即使在最简单的封闭表面球体上熔融也涉及到晶体和缺陷有序的丧失。然而,要探究这两种有序形式的相互作用,需要一个可以原位进行熔融的系统,而这迄今尚未实现。在这里,通过原位调整颗粒间相互作用,我们报告了在球体上胶体晶体熔融过程中观察到中间六方相的情况。值得注意的是,我们观察到在剪切模量预计为零的六方相中二十面体缺陷有序的急剧下降。此外,与在平面空间中无序可以从根本上改变熔融过程的性质不同,在球面上,我们观察到了理想熔融的特征。我们的发现对理解例如病毒衣壳的自组装和成熟动力学以及曲面相变具有深远的意义。