Solid-liquid work of adhesion of coarse-grained models of n-hexane on graphene layers derived from the conditional reversible work method
Solid-liquid work of adhesion of coarse-grained models of n-hexane on graphene layers derived from the conditional reversible work method
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DOI：
10.1063/1.4936253
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发表时间：
2015-12-28
影响因子：
4.4
通讯作者：
Leroy, Frederic
中科院分区：
文献类型：
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作者：
Ardham, Vikram Reddy;Deichmann, Gregor;Leroy, Frederic
我们讨论了减少自由度如何改变非均相固-液体系的界面热力学性质的问题。我们考虑了正己烷与多层石墨烯相互作用的例子，我们用全原子化和粗粒度(CG)模型进行了模拟。利用条件可逆功(CRW)方法得到了CG模型。这些模型的界面热力学以分子动力学模拟的干表面方法计算的固液粘附功W-SL为表征。我们发现，CRW势导致W-SL的值大于原子势。通过对W-SL的能量和熵成分的详细研究，阐明了表面附近正己烷的结构与W-SL之间的关系。我们强调了固液能量涨落所起的关键作用。我们的方法建议，CG势的设计应该保持固-液相互作用能的范围，但也要保持它们的涨落，以便保持W-SL的参考原子值。因此，我们的研究打开了获得CG相互作用势的前景，该相互作用势保持了固-液接触的热力学，并将在旨在解决由界面驱动的材料的研究中得到应用。(C)2015 AIP出版有限责任公司。
We address the question of how reducing the number of degrees of freedom modifies the interfacial thermodynamic properties of heterogeneous solid-liquid systems. We consider the example of n-hexane interacting with multi-layer graphene which we model both with fully atomistic and coarse-grained (CG) models. The CG models are obtained by means of the conditional reversible work (CRW) method. The interfacial thermodynamics of these models is characterized by the solid-liquid work of adhesion W-SL calculated by means of the dry-surface methodology through molecular dynamics simulations. We find that the CRW potentials lead to values of W-SL that are larger than the atomistic ones. Clear understanding of the relationship between the structure of n-hexane in the vicinity of the surface and W-SL is elucidated through a detailed study of the energy and entropy components of W-SL. We highlight the crucial role played by the solid-liquid energy fluctuations. Our approach suggests that CG potentials should be designed in such a way that they preserve the range of solid-liquid interaction energies, but also their fluctuations in order to preserve the reference atomistic value of W-SL. Our study thus opens perspectives into deriving CG interaction potentials that preserve the thermodynamics of solid-liquid contacts and will find application in studies that intend to address materials driven by interfaces. (C) 2015 AIP Publishing LLC.