4.8 Article

Binary icosahedral clusters of hard spheres in spherical confinement

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NATURE PHYSICS
卷 17, 期 1, 页码 -

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NATURE RESEARCH
DOI: 10.1038/s41567-020-1003-9

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资金

  1. European Research Council under the European Union/ERC [291667 HierarSACol]
  2. Netherlands Organization for Scientific Research (NWO) [13CSER025]
  3. Shell Global Solutions International BV
  4. NWO
  5. ERC [815128 REALNANO]
  6. Research Foundation Flanders (FWO, Belgium)
  7. Office of Naval Research Multidisciplinary University Research Initiative [ONR N00014-18-1-2497]

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The influence of geometry on the local and global packing of particles is crucial, with binary mixtures of hard-sphere-like nanoparticles crystallizing into icosahedral clusters in bulk. The local structure of a significant portion of particles is similar to the MgCu(2)Laves phase, which has potential applications in photonics. The nucleation of icosahedral clusters is observed away from the spherical boundary, providing new insights into particle-level studies of binary crystallization.
The influence of geometry on the local and global packing of particles is important to many fundamental and applied research themes, such as the structure and stability of liquids, crystals and glasses. Here we show by experiments and simulations that a binary mixture of hard-sphere-like nanoparticles crystallizing into a MgZn(2)Laves phase in bulk spontaneously forms icosahedral clusters in slowly drying droplets. Using advanced electron tomography, we are able to obtain the real-space coordinates of all the spheres in the icosahedral clusters of up to about 10,000 particles. The local structure of 70-80% of the particles became similar to that of the MgCu(2)Laves phase. These observations are important for photonic applications. In addition, we observed in simulations that the icosahedral clusters nucleated away from the spherical boundary, which is distinctly different from that of the single species clusters. Our findings open the way for particle-level studies of nucleation and growth of icosahedral clusters, and of binary crystallization. The authors investigate out-of-equilibrium crystallization of a binary mixture of sphere-like nanoparticles in small droplets. They observe the spontaneous formation of an icosahedral structure with stable MgCu(2)phases, which are promising for photonic applications.

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