A first-principles study on remote van der Waals epitaxy through a graphene monolayer on semiconductor substrates

To investigate the mechanism of remote epitaxy, where the overlayer can follow the same crystalline structure as the underlying semiconductor substrate through a thin two-dimensional interlayer, we systematically study the potential fluctuations of graphene covered Si, Ga As, and Ga N substrates from first-principles. We find that the uneven semiconductor surface, the distorted graphene, and the non-uniform interface charge transfer make significant contributions to the potential fluctuation. The semiconductor substrate with different surface reconstructions and orientations will generate different potential fluctuations through the graphene interlayer. We also calculate and compare the adsorption of adatoms on graphene covered substrates. The adsorption energies of adatoms not only depend on their distances to the underlying semiconductor surface, but are also sensitive to the direction of the charge transfer at the graphene/substrate interface. Changing the semiconductor reconstruction or orientation could even reverse the order of the adsorption energies of cation and anion adatoms by reversing the interface charge transfer direction, leading to a change in the growth orientation of the overlayer.Our study improves the understanding of the mechanism of remote epitaxy, and reveals that it is possible to control the initial nucleation and orientation of overlayers by changing the semiconductor reconstructions and/or orientations in remote epitaxy.

Antiferromagnetic ferromagnetic transition in zigzag graphene nanoribbons induced by substitutional doping

Using first-principles calculations based on density functional theory, we show that the ground state of zigzag-edged graphene nanoribbons（ZGNRs） can be transformed from antiferromagnetic（AFM） order to ferromagnetic（FM） order by changing the substitutional sites of N or B dopants. This AFM–FM transition induced by substitutional sites is found to be a consequence of the competition between the edge and bulk states. The energy sequence of the edge and bulk states near the Fermi level is reversed in the AFM and FM configurations. When the dopant is substituted near the edge of the ribbon, the extra charge from the dopant is energetically favorable to occupy the edge states in AFM configuration. When the dopant is substituted near the center, the extra charge is energetically favorable to occupy the bulk states in FM configuration. Proper substrate with weak interaction is necessary to maintain the magnetic properties of the doped ZGNRs. Our study can serve as a guide to synthesize graphene nanostructures with stable FM order for future applications to spintronic devices.

Uniaxial strain-modulated electronic structures of CdX(X-S,Se,Te)from first-principles calculations:A comparison between bulk and nanowires

sing first-principles calculations based on density functional theory, we systematically study the structural deformation and electronic properties of wurtzite CdX（X = S, Se, Te） bulk and nanowires（NWs） under uniaxial [0001] strain. Due to the intrinsic shrinking strain induced by surface contraction, large NWs with {10ˉ10} facets have heavy hole（HH）-like valence band maximum（VBM） states, while NWs with {11ˉ20} facets have crystal hole（CH）-like VBM states. The external uniaxial strain induces an HH–CH band crossing at a critical strain for both bulk and NWs, resulting in nonlinear variations in band gap and hole effective mass at VBM. Unlike the bulk phase, the critical strain of NWs highly depends on the character of the VBM state in the unstrained case, which is closely related to the size and facet of NWs. The critical strain of bulk is at compressive range, while the critical strain of NWs with HH-like and CH-like VBM appears at compressive and tensile strain, respectively. Due to the HH–CH band crossing, the charge distribution of the VBM state in NWs can also be tuned by the external uniaxial strain. Despite the complication of the VBM state, the electron effective mass at conduction band minimum（CBM） of NWs shows a linear relation with the CBM–HH energy difference, the same as the bulk material.

Bi- and Au-Induced Reconstructions on GaAs（001）-2 × 4 Surface

Submonolayer Bi and Au adsorptions on the GaAs（001）-2× 4 surface are investigated by scanning tunnelling microscopy, low energy electron diffraction and first-principles calculations. The 1 ×4 and 3 × 4 reconstructed surface induced by Bi and Au, respectively, are revealed and their structural models are proposed based on experiments and first-principles calculations. Moreover, the validity of the recently proposed generalized electron counting （GEC） model [Phys. Rev. Lett. 97 （2006） 126103] is examined in detail by using the two surfaces. The GEC model perfectly explains the structural features, such Bi-1 × 4 surface and the 3x arrangement of four-atom Au as the characteristic short double-line structure in the clusters.

First-principles study on improvement of two-dimensional hole gas concentration and confinement in AlN/GaN superlattices

Using first-principles calculations based on density functional theory,we have systematically studied the influence of in-plane lattice constant and thickness of slabs on the concentration and distribution of two-dimensional hole gas(2 DHG)in AlN/GaN superlattices.We show that the increase of in-plane lattice constant would increase the concentration of 2 DHG at interfaces and decrease the valence band offset,which may lead to a leak of current.Increasing the thickness of AlN and/or decreasing the thickness of GaN would remarkably strengthen the internal field in GaN layer,resulting in better confinement of 2 DHG at AlN/GaN interfaces.Therefore,a moderate larger in-plane lattice constant and thicker AlN layer could improve the concentration and confinement of 2 DHG at AlN/GaN interfaces.Our study could serve as a guide to control the properties of 2 DHG at Ⅲ-nitride interfaces and help to optimize the performance of p-type nitride-based devices.

N-Doped Zigzag Graphene Nanoribbons on Si(001):a First-Principles Calculation

The structural and electronic properties of N-doped zigzag graphene nanoribbons （N-ZGNRs） adsorbed on Si（001） substrates are investigated with first-principles density functional cMculations. Compared with the free-standing N-ZGNRs, the energy difference between the substitutional doping at the edge and the inner sites is significantly decreased on the Si substrate. The distribution of the extra charge induced by the N substitutional .dopant keeps the Friedel oscillation feature, and is a main effect that influences the C-Si bonding strength. When N is doped in regions with high C-Si bond densities, the strain induced by the dopant also plays an important role in determining the C-Si bonding interactions. Similar to the undoped case, the strong N-ZGNR/Si interaction destroys the antiferromagnetic coupling of the edge states in N-ZGNR, leading to a non-magnetic ground state for the N-ZGNR/Si heterostructures.

Structural and Electronic Properties of Zigzag Graphene Nanoribbons on Si(001)Substrates

We study the adsorption of zigzag graphene nanoribbons （GNRs） on Si（001） substrates using the first-principles density functional theory, exploring the effects of the interface interaction on the structurM and electronic prop- erties of both GNRs and the substrate. By comparing the adsorption structures predicted by the local density approximation, the generalized gradient approximation, and the DFT-D2 approach, we confirm that both edge and inner C atoms of GNRs can form covalent bonds with the substrate. The GNR/substrate interaction destroys the antiferromagnetic coupling of the edge states in GNB.s. The charge transfer from the substrate to GNRs exhibits a complicated pattern and is mainly localized near the C-Si bonds. We also observe a strong perturbation of the surface states and a surface reconstruction transition induced by the GNR adsorption.

钙覆盖的富勒烯作为高存储容量的储氢材料

文章从理论上研究了轻碱土金属覆盖的富勒烯作为储氢介质的可行性.基于第一性原理密度泛函理论计算,文章作者发现Ca和Sr在C60表面的吸附很强,并且倾向于形成单层覆盖.这种强吸附归因于这类金属元素未占据的d轨道参与的一种独特的电荷转移机制.电荷的重新分布在金属覆盖的富勒烯表面附近产生强电场,使得金属-富勒烯复合物成为理想的氢分子吸附中心.Ca32C60复合物的理论储氢质量百分比达到8.4wt%,因此,在富勒烯+金属体系的储氢介质研究中,Ca优于目前提出的所有覆盖富勒烯的金属元素.