Large-scale surface reconstruction energetics of Pt(100) and Au(100) by all-electron density functional theory
Large-scale surface reconstruction energetics of Pt(100) and Au(100) by all-electron density functional theory
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DOI：
10.1103/physrevb.82.161418
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发表时间：
2010-10-25
影响因子：
3.7
通讯作者：
Scheffler, Matthias
中科院分区：
文献类型：
--
作者：
Havu, Paula;Blum, Volker;Scheffler, Matthias
Au和Pt的低折射率表面都倾向于重建，这一事实在许多纳米结构、催化和电化学应用中至关重要。值得注意的是，即使在今天，关于它们的结构能的一些重要问题仍然存在，特别是对于大规模的准六边形重构（100）曲面：在现有的实验中，Au和Pt的重构能相当不同，实验和理论与Pt不匹配。我们在这里通过全电子密度泛函理论表明，只有足够大的“（5XN）”近似超级电池才能捕获Au（100）和Pt（100）之间的定性重构能趋势，与理论文献中经常做的相反。因此，它们的大小实际上与Pt（100）的测量值相似且更接近；我们的计算与已知的几何特征非常吻合，为电子重构驱动力提供了直接证据。
The low-index surfaces of Au and Pt all tend to reconstruct, a fact that is of key importance in many nanostructure, catalytic, and electrochemical applications. Remarkably, some significant questions regarding their structural energies remain even today, specifically for the large-scale quasihexagonally reconstructed (100) surfaces: rather dissimilar reconstruction energies for Au and Pt in available experiments and experiment and theory do not match for Pt. We here show by all-electron density functional theory that only large enough "(5XN)" approximant supercells capture the qualitative reconstruction energy trend between Au(100) and Pt(100), in contrast to what is often done in the theoretical literature. Their magnitudes are then in fact similar and closer to the measured value for Pt(100); our calculations achieve excellent agreement with known geometric characteristics and provide direct evidence for the electronic reconstruction driving force.