Michael Wassermair, Gerhard Kahl, Roland Roth, Andrew J Archer
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引用次数: 0
摘要
我们利用蒙特卡罗(MC)计算机模拟和经典密度泛函理论(DFT)研究了二维核壳粒子系统的相序(模式形成)。粒子通过具有硬核和斥性方肩的对势能相互作用。我们的模拟结果表明,在冷却过程中,液态结构越来越多地表现为长波长密度调制,并在进一步冷却过程中形成各种其他相,包括簇状相、条状相和其他图案相。在 DFT 中,使用基本量度理论或简单的局部密度近似来处理势的硬核部分,而使用随机相近似来处理软肩。我们利用大规模大规范数模转换和吉布斯集合数模转换模拟对不同的 DFT 进行了基准测试,以证明它们的预测能力和不足之处。我们发现,拥有波长 k 的液态静态结构因子 S(k) 就足以确定液相和固相的傅立叶模式。这使我们能够从更容易获得的液态数据中识别出与周期相相关的波数,并大致预测出这些模式相在相图中的位置。
Fingerprints of ordered self-assembled structures in the liquid phase of a hard-core, square-shoulder system.
We investigate the phase ordering (pattern formation) of systems of two-dimensional core-shell particles using Monte Carlo (MC) computer simulations and classical density functional theory (DFT). The particles interact via a pair potential having a hard core and a repulsive square shoulder. Our simulations show that on cooling, the liquid state structure becomes increasingly characterized by long wavelength density modulations and on further cooling forms a variety of other phases, including clustered, striped, and other patterned phases. In DFT, the hard core part of the potential is treated using either fundamental measure theory or a simple local density approximation, whereas the soft shoulder is treated using the random phase approximation. The different DFTs are benchmarked using large-scale grand-canonical-MC and Gibbs-ensemble-MC simulations, demonstrating their predictive capabilities and shortcomings. We find that having the liquid state static structure factor S(k) for wavenumber k is sufficient to identify the Fourier modes governing both the liquid and solid phases. This allows us to identify from easier-to-obtain liquid state data the wavenumbers relevant to the periodic phases and to predict roughly where in the phase diagram these patterned phases arise.
期刊介绍:
The Journal of Chemical Physics publishes quantitative and rigorous science of long-lasting value in methods and applications of chemical physics. The Journal also publishes brief Communications of significant new findings, Perspectives on the latest advances in the field, and Special Topic issues. The Journal focuses on innovative research in experimental and theoretical areas of chemical physics, including spectroscopy, dynamics, kinetics, statistical mechanics, and quantum mechanics. In addition, topical areas such as polymers, soft matter, materials, surfaces/interfaces, and systems of biological relevance are of increasing importance.
Topical coverage includes:
Theoretical Methods and Algorithms
Advanced Experimental Techniques
Atoms, Molecules, and Clusters
Liquids, Glasses, and Crystals
Surfaces, Interfaces, and Materials
Polymers and Soft Matter
Biological Molecules and Networks.