Abstract Last decade has witnessed a surge of research pertaining to ultrathin oxide films grown on metal substrate due to their unique physical properties that cannot be derived from their bulk counterparts. One prototype example is two-dimensional (2D) SiO2 or silica, which has attracted considerable interest from physics/chemistry and materials science communities. Here, by systematic first-principles calculations, we investigate the structural and electronic properties of SiO2/Ru(0 0 0 1) interface influenced by Al doping. We demonstrate that Al doping transforms the original van der Waals interaction to strong chemical bonding between SiO2 and Ru(0 0 0 1), originating from the pronounced charge transfer that leads to enhanced electrostatic interaction. Interestingly, interfacial Al doping enhances the stabilization of single Au/Pt atoms adsorbed on SiO2/Ru(0 0 0 1) and effectively tunes the charging state of the metal species, a great benefit for the realization of single-atom catalyst. These results show the great promise of chemical doping in manipulating the physical/chemical properties of supported oxide ultrathin films for practical applications.

中文翻译：

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金属衬底上负载的二维二氧化硅的界面掺杂调制结构和电子特性

摘要 过去十年见证了关于在金属衬底上生长的超薄氧化膜的研究激增，因为它们具有独特的物理特性，而这些物理特性无法从它们的大块对应物获得。一个原型示例是二维 (2D) SiO2 或二氧化硅，它引起了物理/化学和材料科学界的极大兴趣。在这里，通过系统的第一性原理计算，我们研究了受 Al 掺杂影响的 SiO2/Ru(0 0 0 1) 界面的结构和电子特性。我们证明了 Al 掺杂将原始范德华相互作用转化为 SiO2 和 Ru(0 0 0 1) 之间的强化学键，源于显着的电荷转移，导致静电相互作用增强。有趣的是，界面 Al 掺杂增强了吸附在 SiO2/Ru(0 0 0 1) 上的单个 Au/Pt 原子的稳定性，并有效地调整了金属物种的充电状态，对实现单原子催化剂有很大的好处。这些结果表明，化学掺杂在操纵负载氧化物超薄膜的物理/化学性质方面具有巨大的潜力，可用于实际应用。