Structure Prediction of Atoms Adsorbed on Two-Dimensional Layer Materials: Method and Applications

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• 作者：Bo Gao ; Xuecheng Shao ; Jian Lv ; Yanchao Wang ; Yanming Ma
• 刊名：Journal of Physical Chemistry C
• 出版年：2015
• 出版时间：August 27, 2015
• 年：2015
• 卷：119
• 期：34
• 页码：20111-20118
• 全文大小：541K
• ISSN：1932-7455

文摘

The adsorption of atoms is one of the efficient approaches for functionalizing two-dimensional (2D) layer materials with desirable properties. The structural knowledge of atoms adsorbed on 2D layer materials is crucial for understanding their functional performance. Here we propose a versatile method for predicting the structures of atoms adsorbed on 2D materials via the swarm-intelligence-based CALYPSO structure-prediction method. Several techniques are implemented to improve the efficiency of structure searching, including fixed adsorption sites, constraints of symmetry and distance during structure generation, and the constrained particle swarm-optimization algorithm for structure evolution. The method is successfully applied to investigate the well-studied systems of hydrogenated and oxidized graphene. The energetically most stable structures of single-sided hydrogenated graphene are predicted for different contents of hydrogen; altering the hydrogen content appears to effectively tune the band gap. An energetically most stable phase of fully oxidized graphene is also uncovered. These results provide new structural knowledge on the adsorption of atoms on graphene.