Accurate Surface Chemistry beyond the Generalized Gradient Approximation: Illustrations for Graphene Adatoms

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• 作者：Benjamin G. Janesko ; Veronica Barone ; Edward N. Brothers
• 刊名：Journal of Chemical Theory and Computation
• 出版年：2013
• 出版时间：November 12, 2013
• 年：2013
• 卷：9
• 期：11
• 页码：4853-4859
• 全文大小：335K
• 年卷期：v.9,no.11(November 12, 2013)
• ISSN：1549-9626

文摘

Simulations of surface chemistry often use density functional theory with generalized gradient approximations (GGAs) for the exchange-correlation functional. GGAs have well-known limitations for gas-phase chemistry, including underestimated reaction barriers, and are largely superseded by meta-GGAs and hybrids. Our simulations of O and Li adatoms on graphene add to a growing body of evidence that GGAs have similar limitations on surfaces and that meta-GGAs and screened hybrids are computationally feasible for such systems. Meta-GGAs and screened hybrids systematically improve accuracy, just as they do for gas-phase chemistry, motivating their continued exploration in surface chemistry.