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The energy landscapes of bidisperse particle assemblies on a sphere
Soft Matter ( IF 2.9 ) Pub Date : 2021-09-15 , DOI: 10.1039/d1sm01140e Alexander F Ballard 1 , Jack R Panter 1 , David J Wales 1
Soft Matter ( IF 2.9 ) Pub Date : 2021-09-15 , DOI: 10.1039/d1sm01140e Alexander F Ballard 1 , Jack R Panter 1 , David J Wales 1
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The interplay between crystalline ordering, curvature, and size dispersity make the packing of bidisperse mixtures of particles on a sphere a varied and complex phenomenon. These structures have functional significance in a broad range of systems, such as cellular organisation in spherical epithelia, catalytic activity in binary colloidosomes, and chemical activity in heterofullerenes. In this contribution, we elucidate the potential energy landscapes for systems of repulsive, bidisperse particles confined to the surface of a sphere. It is commonly asserted that particle size dispersity destroys ordered arrangements, leading to glassy landscapes. Surprisingly, across a range of compositions, we find highly ordered global minima. Moreover, a minority of small particles is able to passivate defects, stabilising bidisperse global minima relative to monodisperse systems. However, our landscape analysis also reveals that bidispersity introduces numerous defective, low-lying states that are expected to cause broken ergodicity in corresponding experimental and computational systems. Probing the global minimum structures further, particle segregation is energetically preferred at intermediate compositions, contrasting with the approximate icosahedral global packing at either end of the composition range. Finally, changing the composition has a dramatic effect on the heat capacity: systems with low-symmetry global minima have melting temperatures an order of magnitude lower than monodisperse or high-symmetry systems. This observation may provide a further example of the principle of maximum symmetry: higher symmetry global minima exhibit a larger energy separation from the minima that define the high-entropy phase-like region of configuration space, raising the transition temperature.
中文翻译：
球体上双分散粒子组件的能量景观
晶体有序性、曲率和尺寸分散性之间的相互作用使双分散颗粒混合物在球体上的堆积成为一种多样而复杂的现象。这些结构在广泛的系统中具有功能意义，例如球形上皮的细胞组织、二元胶体的催化活性和异富勒烯的化学活性。在这个贡献中，我们阐明了限制在球体表面的排斥性双分散粒子系统的潜在能量景观。人们普遍认为，粒度分散会破坏有序排列，导致玻璃状景观。令人惊讶的是，在一系列组合中，我们发现了高度有序的全局最小值。此外，少数小颗粒能够钝化缺陷，相对于单分散系统稳定双分散全局最小值。然而，我们的景观分析还表明，双分散性引入了许多有缺陷的低洼状态，预计会在相应的实验和计算系统中导致破坏遍历性。进一步探索全局最小结构，粒子分离在中间组成中是能量上优选的，与在组成范围两端的近似二十面体全局堆积形成对比。最后，改变成分对热容量有显着影响：具有低对称性全局最小值的系统的熔化温度比单分散或高对称性系统低一个数量级。这个观察结果可以提供最大对称原理的另一个例子：
更新日期：2021-09-20
中文翻译：
球体上双分散粒子组件的能量景观
晶体有序性、曲率和尺寸分散性之间的相互作用使双分散颗粒混合物在球体上的堆积成为一种多样而复杂的现象。这些结构在广泛的系统中具有功能意义，例如球形上皮的细胞组织、二元胶体的催化活性和异富勒烯的化学活性。在这个贡献中，我们阐明了限制在球体表面的排斥性双分散粒子系统的潜在能量景观。人们普遍认为，粒度分散会破坏有序排列，导致玻璃状景观。令人惊讶的是，在一系列组合中，我们发现了高度有序的全局最小值。此外，少数小颗粒能够钝化缺陷，相对于单分散系统稳定双分散全局最小值。然而，我们的景观分析还表明，双分散性引入了许多有缺陷的低洼状态，预计会在相应的实验和计算系统中导致破坏遍历性。进一步探索全局最小结构，粒子分离在中间组成中是能量上优选的，与在组成范围两端的近似二十面体全局堆积形成对比。最后，改变成分对热容量有显着影响：具有低对称性全局最小值的系统的熔化温度比单分散或高对称性系统低一个数量级。这个观察结果可以提供最大对称原理的另一个例子：
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