Implicit solvation model for density-functional study of nanocrystal surfaces and reaction pathways
Implicit solvation model for density-functional study of nanocrystal surfaces and reaction pathways
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DOI：
10.1063/1.4865107
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发表时间：
2014-02-28
影响因子：
4.4
通讯作者：
Hennig, Richard G.
中科院分区：
文献类型：
--
作者：
Mathew, Kiran;Sundararaman, Ravishankar;Hennig, Richard G.
固液界面是许多现代技术的核心，并对许多材料模拟方法提出了挑战。对此类系统进行现实的第一原理计算研究需要考虑溶剂效应。在这项工作中，我们实现了一个隐式溶剂化模型，该模型为广泛使用的密度函数代码 Vienna ab initio 软件包奠定了坚实的理论基础。隐式溶剂化模型遵循联合密度泛函理论的框架。我们描述了小分子系统的框架、算法和实现以及基准。我们应用溶剂化模型来研究半导体和金属纳米晶体不同面的表面能以及S(N)2 反应途径。我们发现溶剂化降低了纳米晶体的表面能，尤其是半导体纳米晶体的表面能，并增加了 S(N)2 反应的能垒。 (C) 2014 AIP 出版有限责任公司。
Solid-liquid interfaces are at the heart of many modern-day technologies and provide a challenge to many materials simulation methods. A realistic first-principles computational study of such systems entails the inclusion of solvent effects. In this work, we implement an implicit solvation model that has a firm theoretical foundation into the widely used density-functional code Vienna ab initio Software Package. The implicit solvation model follows the framework of joint density functional theory. We describe the framework, our algorithm and implementation, and benchmarks for small molecular systems. We apply the solvation model to study the surface energies of different facets of semiconducting and metallic nanocrystals and the S(N)2 reaction pathway. We find that solvation reduces the surface energies of the nanocrystals, especially for the semiconducting ones and increases the energy barrier of the S(N)2 reaction. (C) 2014 AIP Publishing LLC.