期刊
JOURNAL OF CHEMICAL PHYSICS
卷 135, 期 19, 页码 -出版社
AMER INST PHYSICS
DOI: 10.1063/1.3651370
关键词
diffusion; entropy; free energy; Monte Carlo methods; phase diagrams; quasicrystals
资金
- U.S. Air Force Office of Scientific Research under Multidisciplinary University Research Initiative [FA9550-06-1-0337, 444286-P061716]
- DOD/DDRE [N00244-09-1-0062]
- Deutsche Forschungsgemeinschaft
- University of Michigan
Advancements in the synthesis of faceted nanoparticles and colloids have spurred interest in the phase behavior of polyhedral shapes. Regular tetrahedra have attracted particular attention because they prefer local symmetries that are incompatible with periodicity. Two dense phases of regular tetrahedra have been reported recently. The densest known tetrahedron packing is achieved in a crystal of triangular bipyramids (dimers) with a packing density of 4000/4671 approximate to 85.63%. In simulation a dodecagonal quasicrystal is observed; its approximant, with periodic tiling (3.4.3(2).4), can be compressed to a packing fraction of 85.03%. Here, we show that the quasicrystal approximant is more stable than the dimer crystal for packing densities below 84% using Monte Carlo computer simulations and free energy calculations. To carry out the free energy calculations, we use a variation of the Frenkel-Ladd method for anisotropic shapes and thermodynamic integration. The enhanced stability of the approximant can be attributed to a network substructure, which maximizes the free volume (and hence the wiggle room) available to the particles and facilitates correlated motion of particles, which further contributes to entropy and leads to diffusion for packing densities below 65%. The existence of a solid-solid transition between structurally distinct phases not related by symmetry breaking - the approximant and the dimer crystal - is unusual for hard particle systems. (C) 2011 American Institute of Physics. [doi: 10.1063/1.3651370]
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据