过渡金属表面石墨烯和硅烯的成核生长机理与相互作用
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摘要
石墨烯和硅烯,两者是具有相似的蜂巢形格子的二维单原子薄膜,它们近年来成为物理、材料、化学等领域的新星材料,吸引了众多科研工作者的研究热情。因独特的线性色散关系,近似无质量的超快费米子存在于这两种材料的狄拉克锥中,这两种材料在未来超快微电子器件和自旋电子器件中大有前途。特别是,由于具有超强的力学性质,独特的光学性质,优良的导热等性质,石墨烯在传感器、探测器、太阳能电池和超级电容器等方面有大量的潜在应用。
基于密度泛函理论和晶体生长理论,我们系统地研究了石墨烯在金属平台和台阶附近的成核生长行为。研究模型为同石墨烯晶格完美匹配的Ni(111)表面和具有较大失配的Rh(111)表面上的碳团簇CN(碳原子数N=1-24)。研究发现平台上最稳定的石墨烯团簇都含有1-3个五元环。并且在N≈10-12处,碳团簇发生了从碳链到碳sp2网格的结构转变,这个转变尺寸在很大的化学势范围内对应碳团簇的成核尺寸。此外,无论在Ni(111)还是Rh(111)表面,金属台阶都有助于稳定六元环并且进一步降低碳团簇形成能。这样,在一定程度的低化学势下,石墨烯优先在台阶处成核生长。此外,在失配较大的Rh(111)台阶处,我们发现了两种饱和碳链的竞争方式以及石墨烯团簇的非线性生长关系。在石墨烯成核生长过程的研究中,四种用以研究的表面Ni(111), Cu(111), Rh(111)和Ru(0001)上都存在一个有趣的超稳定幻数碳团簇C21,这较好地解释了最近实验上在过渡金属表面观察到的均一大小的碳团簇现象。此外,我们系统地研究了在三种过渡金属表面[Cu(111),CO(111)和Ni(111)]上钝化效应对石墨烯边界的影响。与真空中的情况截然不同,纯锯齿形边在所有的过渡金属表面都非常稳定,我们还发现了一个新奇的ac(ad)边在Co(111)和Ni(111)面上是最稳定的扶手椅型朝向边；进一步的研究表明这种奇特的边界结构对石墨烯CVD生长行为具有显著的影响。
作为石墨烯生长工作的延伸,我们系统地计算了Ag(111)表面上的SiN团簇(N≤24)的结构和稳定性,并以此探究硅烯外延生长的初期行为。同时,我们也计算了Ag(111)表面上三种类型的硅烯超结构,与实验STM图像直接对比。分析结果表明硅团簇和银表面存在p-d杂化,并且部分sp2特征存留在SiN@Ag(111)中,硅团簇不具有穹顶形结构。通过Ag(111)和Rh(111)上硅烯热稳定性的分子动力学模拟,确定了Ag(111)表面上硅烯的高稳定性。我们解释了银衬底有助于硅烯生长的优越性,这有助于促进实验提高硅烯合成工艺。
Graphene and silicene, a couple of counterparts of thin atomic monolayers with honeycombed lattices, are the new rising stars in many fields such as physics, materials science and chemistry, causing the great rush of scientific researchers. Based on the linear dispersion, near massless fermions with ultrafast velocity are in their Dirac cone. Therefore, they are the ideal materials for ultrafast microelectronics and spintronics in future. Moreover, due to the excellent mechanical, optical, thermal properties and so on, graphene has many novel applications, e. g. sensor, detection, solar cell and supercapacity.
Based on density functional theory (DFT) calculations and theory of crystal growth, the nucleation of graphene is investigated both on a well matched Ni(111) surface and on a large mismatched Rh(111) by systematically exploring the CN clusters (with size N ranging from1to24) either on a terrace or near a step edge of transition metal (TM) surface. It is surprising that incorporating one to three pentagons into a graphene island on a TM terrace is required to achieve the most stable structure. A ground state structure transformation is found firstly from a C chain to a sp2C network at N-10-12, which is corresponding to the nucleation size at a wide range of carbon chemical potential. Besides, we found that steps of both Ni(111) and Rh(111) can help'to stabilizing the hexagon and reducing the formation energy. Thus, at a relative low carbon chemical potential, the nucleation preferentially occurred along the step. In addition, two competing style of passivation for C chain, as well as the nonlinear growth behaviours were revealed along the large mismatched step of Rh(111) surface. During the research of graphene growth behaviors, a magic carbon cluster C21is intriguingly found at four selected TM surfaces, that is, Ni(111), Cu(111), Rh(111) and Ru(0001), which explained the recent observed uniformed C clusters on TM surfaces. Besides, we investigated the impact of passivation on the graphene edges on three TM surfaces [Cu(111), Co(111), and Ni(111)]. Different from that in vacuum, the pristine zz edge is stable on all TM surface and an undiscovered novel reconstructed ac(ad) edge is high stable on Co(111) and Ni(111) surfaces. Beyond this, the unique edge configuration has a significant impact on the graphene CVD growth behavior.
As an extension of graphene growth work, we investigated the structures and stabilities of SiN clusters (N≤24) on Ag(111)surface as the initial stage of epitaxial growth of silicene and three types of silicene superstructures on Ag(111) surface. Analysis reveals p-d hybridization between Ag and Si as well as sp2characteristics in SiN@Ag(111), without dome-shaped configuration. Molecular dynamic simulation shows high thermal stability of silicene monolayer on Ag(111) surfaces, contrast to that on Rh(111) surface. The superiority of Ag substrate for silicene growth is explained, which would be helpful for improving the experimentally epitaxial growth of silicene.
基于密度泛函理论和晶体生长理论,我们系统地研究了石墨烯在金属平台和台阶附近的成核生长行为。研究模型为同石墨烯晶格完美匹配的Ni(111)表面和具有较大失配的Rh(111)表面上的碳团簇CN(碳原子数N=1-24)。研究发现平台上最稳定的石墨烯团簇都含有1-3个五元环。并且在N≈10-12处,碳团簇发生了从碳链到碳sp2网格的结构转变,这个转变尺寸在很大的化学势范围内对应碳团簇的成核尺寸。此外,无论在Ni(111)还是Rh(111)表面,金属台阶都有助于稳定六元环并且进一步降低碳团簇形成能。这样,在一定程度的低化学势下,石墨烯优先在台阶处成核生长。此外,在失配较大的Rh(111)台阶处,我们发现了两种饱和碳链的竞争方式以及石墨烯团簇的非线性生长关系。在石墨烯成核生长过程的研究中,四种用以研究的表面Ni(111), Cu(111), Rh(111)和Ru(0001)上都存在一个有趣的超稳定幻数碳团簇C21,这较好地解释了最近实验上在过渡金属表面观察到的均一大小的碳团簇现象。此外,我们系统地研究了在三种过渡金属表面[Cu(111),CO(111)和Ni(111)]上钝化效应对石墨烯边界的影响。与真空中的情况截然不同,纯锯齿形边在所有的过渡金属表面都非常稳定,我们还发现了一个新奇的ac(ad)边在Co(111)和Ni(111)面上是最稳定的扶手椅型朝向边；进一步的研究表明这种奇特的边界结构对石墨烯CVD生长行为具有显著的影响。
作为石墨烯生长工作的延伸,我们系统地计算了Ag(111)表面上的SiN团簇(N≤24)的结构和稳定性,并以此探究硅烯外延生长的初期行为。同时,我们也计算了Ag(111)表面上三种类型的硅烯超结构,与实验STM图像直接对比。分析结果表明硅团簇和银表面存在p-d杂化,并且部分sp2特征存留在SiN@Ag(111)中,硅团簇不具有穹顶形结构。通过Ag(111)和Rh(111)上硅烯热稳定性的分子动力学模拟,确定了Ag(111)表面上硅烯的高稳定性。我们解释了银衬底有助于硅烯生长的优越性,这有助于促进实验提高硅烯合成工艺。
Graphene and silicene, a couple of counterparts of thin atomic monolayers with honeycombed lattices, are the new rising stars in many fields such as physics, materials science and chemistry, causing the great rush of scientific researchers. Based on the linear dispersion, near massless fermions with ultrafast velocity are in their Dirac cone. Therefore, they are the ideal materials for ultrafast microelectronics and spintronics in future. Moreover, due to the excellent mechanical, optical, thermal properties and so on, graphene has many novel applications, e. g. sensor, detection, solar cell and supercapacity.
Based on density functional theory (DFT) calculations and theory of crystal growth, the nucleation of graphene is investigated both on a well matched Ni(111) surface and on a large mismatched Rh(111) by systematically exploring the CN clusters (with size N ranging from1to24) either on a terrace or near a step edge of transition metal (TM) surface. It is surprising that incorporating one to three pentagons into a graphene island on a TM terrace is required to achieve the most stable structure. A ground state structure transformation is found firstly from a C chain to a sp2C network at N-10-12, which is corresponding to the nucleation size at a wide range of carbon chemical potential. Besides, we found that steps of both Ni(111) and Rh(111) can help'to stabilizing the hexagon and reducing the formation energy. Thus, at a relative low carbon chemical potential, the nucleation preferentially occurred along the step. In addition, two competing style of passivation for C chain, as well as the nonlinear growth behaviours were revealed along the large mismatched step of Rh(111) surface. During the research of graphene growth behaviors, a magic carbon cluster C21is intriguingly found at four selected TM surfaces, that is, Ni(111), Cu(111), Rh(111) and Ru(0001), which explained the recent observed uniformed C clusters on TM surfaces. Besides, we investigated the impact of passivation on the graphene edges on three TM surfaces [Cu(111), Co(111), and Ni(111)]. Different from that in vacuum, the pristine zz edge is stable on all TM surface and an undiscovered novel reconstructed ac(ad) edge is high stable on Co(111) and Ni(111) surfaces. Beyond this, the unique edge configuration has a significant impact on the graphene CVD growth behavior.
As an extension of graphene growth work, we investigated the structures and stabilities of SiN clusters (N≤24) on Ag(111)surface as the initial stage of epitaxial growth of silicene and three types of silicene superstructures on Ag(111) surface. Analysis reveals p-d hybridization between Ag and Si as well as sp2characteristics in SiN@Ag(111), without dome-shaped configuration. Molecular dynamic simulation shows high thermal stability of silicene monolayer on Ag(111) surfaces, contrast to that on Rh(111) surface. The superiority of Ag substrate for silicene growth is explained, which would be helpful for improving the experimentally epitaxial growth of silicene.
引文
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