Nies Cara-Lena, Nolan Michael
Tyndall National Institute, University College Cork, Lee Maltings, Dyke Parade, Cork, T12 R5CP, Ireland.
NIBEC, School of Engineering, University of Ulster at Jordanstown BT37 0QB, United Kingdom.
Beilstein J Nanotechnol. 2021 Jul 14;12:704-724. doi: 10.3762/bjnano.12.56. eCollection 2021.
Layered materials, such as MoS, have a wide range of potential applications due to the properties of a single layer, which often differ from the bulk material. They are of particular interest as ultrathin diffusion barriers in semiconductor device interconnects and as supports for low-dimensional metal catalysts. Understanding the interaction between metals and the MoS monolayer is of great importance when selecting systems for specific applications. In previous studies the focus has been largely on the strength of the interaction between a single atom or a nanoparticle of a range of metals, which has created a significant knowledge gap in understanding thin film nucleation on 2D materials. In this paper, we present a density functional theory (DFT) study of the adsorption of small Co and Ru structures, with up to four atoms, on a monolayer of MoS. We explore how the metal-substrate and metal-metal interactions contribute to the stability of metal clusters on MoS, and how these interactions change in the presence of a sulfur vacancy, to develop insight to allow for a prediction of thin film morphology. The strength of interaction between the metals and MoS is in the order Co Ru. The competition between metal-substrate and metal-metal interaction allows us to conclude that 2D structures should be preferred for Co on MoS, while Ru prefers 3D structures on MoS. However, the presence of a sulfur vacancy decreases the metal-metal interaction, indicating that with controlled surface modification 2D Ru structures could be achieved. Based on this understanding, we propose Co on MoS as a suitable candidate for advanced interconnects, while Ru on MoS is more suited to catalysis applications.
诸如二硫化钼（MoS）之类的层状材料，由于其单层特性（通常与块体材料不同）而具有广泛的潜在应用。它们作为半导体器件互连中的超薄扩散阻挡层以及低维金属催化剂的载体尤其受到关注。在为特定应用选择系统时，了解金属与二硫化钼单层之间的相互作用非常重要。在先前的研究中，重点主要集中在一系列金属的单个原子或纳米颗粒之间相互作用的强度上，这在理解二维材料上的薄膜成核方面造成了重大的知识空白。在本文中，我们展示了一项密度泛函理论（DFT）研究，该研究针对含有多达四个原子的小钴（Co）和钌（Ru）结构在二硫化钼单层上的吸附情况。我们探究了金属 - 衬底和金属 - 金属相互作用如何有助于二硫化钼上金属簇的稳定性，以及在存在硫空位的情况下这些相互作用如何变化，以深入了解从而能够预测薄膜形态。金属与二硫化钼之间相互作用的强度顺序为钴 钌。金属 - 衬底和金属 - 金属相互作用之间的竞争使我们得出结论，对于二硫化钼上的钴，二维结构应该更受青睐，而钌在二硫化钼上更倾向于三维结构。然而，硫空位的存在会降低金属 - 金属相互作用，这表明通过可控的表面改性可以实现二维钌结构。基于这种理解，我们提出二硫化钼上的钴作为先进互连的合适候选材料，而二硫化钼上的钌更适合催化应用。
