We present a joint experimental and theoretical determination of structures of Ag adatoms on the Ge(111) surface using low energy electron diffraction, low energy electron microscopy, scanning tunneling microscopy, and density functional theory-based calculations, as functions of coverages and temperature. Experimentally for clean Ge(111), c(2X8) and (2X1) phases occur, while Ag overlayers cause (4X4), (V3XV3)R30 and (3X1) surface structural phases. The dependence of the growth behavior of these different phases was examined as a function of temperature, Ag deposition rate and coverage, substrate step density, and history of temperature cycling. First-principles calculations of the electronic and geometric structures and vibrational dynamics show the Ge(111)-c(2X8) configuration with Ge adatoms adsorbed on three-fold hollow (T4) sites to be the energetically most favored phase of the Ge(111) surface, among unreconstructed Ge(111), reconstructed Ge(111)-2X1, and Ge(111)-c(2X8) structures. The Ge(111)-Ag(3X1) overlayer of the system has Ge atoms forming a honeycomb chain on a missing top layer reconstructed surface, with metal at 1/3 ML coverage in channel. The Ge (111)-Ag(V3XV3)R30 overlayer contains one monolayer Ag forming inequivalent Ag triangles in a surface unit cell on the missing top layer reconstructed Ge(111) surface. The Ge(111)-Ag(4X4) overlayer formed at low Ag coverage contains two triangular subunits at different heights: one with six Ag adatoms and the other with three Ge adatoms on the intact double layer Ge(111) surface. The temperature and coverage dependent surface phase diagram, obtained by minimizing the surface free energy, captures the main features of the experimental phase diagram.
Using first-principles calculations, we study the magnetic properties of a Co monolayer on a Pt(111) surface with a capping monolayer of selected $5d$ elements (Re, Os, Ir, Pt and Au). First we determine the tensorial exchange interactions and magnetic anisotropies characterizing the Co monolayer for all considered systems. We find a close relationship between the magnetic moment of the Co atoms and the nearest-neighbor isotropic exchange interaction, which is attributed to the electronic hybridization between the Co and the capping layers, in spirit of the Stoner picture of ferromagnetism. Th…
Density-functional calculations are used to identify one-atom-thick metallic In overlayers on the Si(111) surface, which have long been sought in quest of the ultimate two-dimensional (2D) limit of free-electron-like metallic properties. We predict two metastable single-layer In phases, one $\sqrt{7}\times\sqrt{3}$ phase with a coverage of 1.4 monolayer (ML; here 1 ML refers to one In atom per top Si atom) and the other $\sqrt{7}\times\sqrt{7}$ phase with 1.43 ML, which indeed match well with experimental evidences. Both phases reveal quasi-1D arrangements of protruded In atoms, leading to 2D-…
We present the theoretical study of thermodynamical properties of fcc-Cu(001) substrate covered by iron-cobalt monolayer as well as by incomplete iron layer. The effective two-dimensional Heisenberg Hamiltonian is constructed from first principles and properties of exchange interactions are investigated. The Curie temperatures are estimated using the Monte-Carlo (MC) simulations and compared with a simplified approach using the random-phase approximation (RPA) in connection with the virtual-crystal approach (VCA) to treat randomness in exchange integrals. Calculations indicate a weak maximum o…
Silicon thin films for coverages ($θ$) between 0.3 and 3 monolayers have been grown on rutile \ce{TiO2}(110)-(1x1) at room temperature and studied by x-ray and ultra-violet photoelectron spectroscopies, Auger electron spectroscopy, and low energy electron diffraction (LEED). A clear evidence of a strong \ce{Si}/\ce{TiO2} interaction consistent with the high affinity of O for Si has been found. The Ti cations on the substrate are reduced, while the Si film is oxidized, yielding \ce{SiO2} and a mixture of silicon suboxides. Neutral Si atoms are observed at a coverage of 3 monolayers. At the inte…
We have carried out first-principles based DFT calculation on electronic properties of silicene monolayer on various (111) semi-conducting surfaces. We find that the relative stability and other properties of the silicene overlayer depends sensitively on whether the interacting top layer of the substrate is metal or non-metal terminated. The nature of silicene-monolayer on the metal termi- nated surface can be metallic or even magnetic, depending upon the choice of the substrate. The silicene overlayer undergoes n-type doping on metal terminated surface while it undergoes p-type doping on non …
We present detailed ab initio study of structural and magnetic stability of a Fe-monolayer on the fcc(001) surface of iridium. The Fe-monolayer has a strong tendency to order antiferromagnetically for the true relaxed geometry. On the contrary an unrelaxed Fe/Ir(001) sample has a ferromagnetic ground state. The antiferromagnetism is thus stabilized by the decreased Fe-Ir layer spacing in striking contrast to the recently experimentally observed antiferromagnetism of the Fe/W(001) system which exists also for an ideal bulk-truncated, unrelaxed geometry. The calculated layer relaxations for Fe/I…
We present a new approach to study the magnetic phase stability of magnetic overlayers on nonmagnetic substrates. The exchange integrals among magnetic atoms in the overlayer are estimated in the framework of the adiabatic approximation and used to construct the effective classical two-dimensional Heisenberg Hamiltonian. Its stability is then studied with respect to a large number of collinear and non-collinear magnetic arrangements which include, as special cases, not only ferromagnetic and various antiferromagnetic configurations, but also possible incommensurate spin-spiral structures. This…
The total energy distributions (TEDs) of the emission currents in field emission and surface photofield emission and the overlayer-induced modifications in the surface electronic structures from the technologically important W surfaces with the commensurate W(100)/Na c(2x2), W(110)/Na (2x2) and W(111)/Na (1x1) overlayers are calculated. The TEDs obtained by our recent numerical method that extends the full-potential linear augmented plane wave method for the electronic structures to the study of field and photofield emission are used to interpret the shifts of the peaks in the experimental TED…
In this work we investigate the Fe$_3$O$_4$(001) surface/water interface by combining several theoretical approaches, ranging from a hybrid functional method (HSE06) to density-functional tight-binding (DFTB) to molecular mechanics (MM). First, we assess the accuracy of the DFTB method to reproduce correctly HSE06 results on structural details and energetics and available experimental data for the adsorption of isolated water, dimers, trimers, etc. up to a water monolayer. Secondly, we build two possible configurations of a second and a third overlayer and perform molecular dynamics simulation…
The electronic structure of a single Na monolayer on the surface of single-crystal HfSe$_2$ is investigated using angle-resolved photoemission spectroscopy. We find that this system exhibits an almost perfect "nearly-free-electron" behavior with an extracted effective mass of $\sim\!1m_e$, in contrast to heavier masses found previously for alkali metal monolayers on other substrates. Our density-functional-theory calculations indicate that this is due to the large lattice constant, causing both exchange and correlation interactions to be suppressed, and to the weak hybridization between the ov…
Systematic studies of the two high-temperature monolayer oxygen structures that exist on the (110) tungsten surface were performed using low-energy electron microscopy and diffraction measurements. Our work questions the commonly accepted interpretation from the literature that striped oxygen superstructures arise from alternating site-exchanged (S-E) domains. We postulate that the superstructures originate from a misfit between tungsten and oxygen lattices while the striped appearance corresponds to a moiré pattern. Moreover, we show that the two structures, indicated as 113- and 337-phases d…
We present density functional theory (DFT) calculations for 6H-SiC$\{0001\}$ surfaces with different surface stackings and terminations. We compare the relative stability of different $(0001)$ and $(000\bar1)$ surfaces in terms of their surface free energies. Removing surface and subsurface Si atoms, we simulate the formation of graphene and graphene-like overlayers by Si evaporation. We find that overlayers with a different nature of bonding are preferred at the two non-equivalent surface orientations. At $(0001)$, a chemically bonded, highly strained and buckled film is predicted. At $(000\b…
A quantitative structural investigation is reported, aimed at resolving the issue of whether substrate adatoms are incorporated into the monolayers formed by strong molecular electron acceptors deposited onto metallic electrodes. A combination of normal-incidence X-ray standing waves, low energy electron diffraction, scanning tunnelling microscopy and X-ray photoelectron spectroscopy measurements demonstrate that the systems TCNQ and F4TCNQ on Ag(100) lie at the boundary between these two possibilities and thus represent ideal model systems with which to study this effect. A room-temperature c…
While the phenomenon of metal substrate adatom incorporation into molecular overlayers is generally believed to occur in several systems, the experimental evidence for this relies on the interpretation of scanning tunnelling microscopy (STM) images, which can be ambiguous and provides no quantitative structural information. We show that surface X-ray diffraction (SXRD) uniquely provides unambiguous identification of these metal adatoms. We present the results of a detailed structural study of the Au(111)-F4TCNQ system, combining surface characterisation by STM, low energy electron diffraction …
The magnetic properties of materials based on two-dimensional transition-metal dichalcogenides (TMDC) have been investigated by means of first-principles DFT calculations, namely Fe-intercalated bulk Fe$_{1/4}$TaS$_2$ compounds as well as TMDC monolayers with deposited Fe films. Changing the structure and the composition of systems consisting of Fe overlayers on top of a TMDC monolayers resulted in considerable variations of their physical properties. For the considered systems the Dzyaloshinskii-Moriya (DM) interaction has been determined and used for the subsequent investigation of their mag…
We have investigated the magnetic ordering in the ultrathin c(10$\times$2) CoO(111) film supported on Ir(100) on the basis of ab-initio calculations. We find a close relationship between the local structural properties of the oxide film and the induced magnetic order, leading to alternating ferromagnetically and anti-ferromagnetically ordered segments. While the local magnetic order is directly related to the geometric position of the Co atoms, the mismatch between the CoO film and the Ir substrate leads to a complex long-range order of the oxide.
Liquid phase epitaxy of an 18 nm thick Yttrium Iron garnet (YIG) film is achieved. Its magnetic properties are investigated in the 100 -- 400 K temperature range, as well as the influence of a 3 nm thick Pt overlayer on them. The saturation magnetization and the magnetocrystalline cubic anisotropy of the bare YIG film behave similarly to bulk YIG. A damping parameter of only a few $10^{-4}$ is measured, together with a low inhomogeneous contribution to the ferromagnetic resonance linewidth. The magnetic relaxation increases upon decreasing temperature, which can be partly ascribed to impurity …
The novel electronic properties emerging at interfaces between transition metal oxides, and in particular the discovery of conductivity in heterostructures composed of LaAlO$_3$ (LAO) and SrTiO$_3$ (STO) band insulators, have generated new challenges and opportunities in condensed matter physics. Although the interface conductivity is stabilized when LAO matches or exceeds a critical thickness of 4 unit cells (u.c.), other phenomena such as a universal metallic state found on the bare surface of STO single crystals and persistent photon-triggered conductivity in otherwise insulating STO-based …
We investigate the spin-valley polarization in MoTe$_2$ monolayer on (111) and (001) surfaces of ferromagnetic semiconductor EuO based on first-principles calculations. We consider surface reconstructions for EuO(111). We find that there is no direct chemical bonding between the reconstructed EuO(111) and the MoTe$_2$ overlayer, in contrast to the case of the ideal EuO(111). However, there is a strong hybridization between the states of MoTe$_2$ and the substrate states, which has a substantial impact on the valleys. The valley polarization due to the magnetic proximity effect is dependent on …
In this paper the early stages of the self-catalyzed Vapor-Liquid-Solid (VLS) growth of GaAs nanowires on epi-ready Si substrates by Molecular Beam Epitaxy (MBE) are studied. The interaction of Ga nano-droplets (NDs) with the silica overlayer is investigated by X-ray Photoemission Spectroscopy (XPS) and Atomic Force Microscopy (AFM). We show how Ga NDs drill the silica overlayer and make contact with bulk Si to allow GaAs nanowires (NWs) epitaxial growth by studying each of the three steps of the NW growth process sequentially: Ga NDs pre-deposition, post-deposition annealing to reach the NW g…
We propose the design of low strained and energetically favourable mono and bilayer graphene overlayer on anatase TiO$_2$ (001) surface and examined the electronic structure of the interface with the aid of first principle calculations. In the absence of hybridization between surface TiO$_2$ and graphene states, dipolar fluctuations govern the minor charge transfer across the interface. As a result, both the substrate and the overlayer retain their pristine electronic structure. The interface with the monolayer graphene retains its gapless linear band dispersion irrespective of the induced epi…
Our first-principles study has revealed unexpected spin polarization of the Pd(001) substrate in contact with antiferromagnetic CoO overlayers. We give an evidence that the ferromagnetism of Pd is caused by the zigzag positions of Co atoms with respect to the Pd interface, resulted from the lattice-mismatch driven structural relaxation. Thanks to the itinerant nature of its 4d electrons, we see that the ferromagnetic properties of Pd are highly sensitive to the local environment and can be enhanced further by increasing the thickness of CoO overlayer film or/and by applying an additional uniax…
We present a detailed ab initio study of the electronic structure and magnetic order of an Fe monolayer on the Ir(001) surface covered by adsorbed oxygen and hydrogen. The results are compared to the clean Fe/Ir(001) system, where recent intensive studies indicated a strong tendency towards an antiferromagnetic order and complex magnetic structures. The adsorption of an oxygen overlayer significantly increases interlayer distance between the Fe layer and the Ir substrate, while the effect of hydrogen is much weaker. We show that the adsorption of oxygen (and also of hydrogen) leads to a p(2$\t…
The formation of Ni(Pt)silicides on a Si(001) surface is investigated using an ab initio approach. After deposition of a Ni overlayer alloyed with Pt, the calculations reveal fast diffusion of Ni atoms into the Si lattice, which leads initially to the formation of Ni2Si. At the same time Si atoms are found to diffuse into the metallic overlayer. The transformation of Ni2Si into NiSi is likely to proceed via a vacancy-assisted diffusion mechanism. Silicon atoms are the main diffusing species in this transformation, migrating from the Si substrate through the growing NiSi layer into the Ni2Si. P…
Honeycomb structures of group IV elements can host massless Dirac fermions with non-trivial Berry phases. Their potential for electronic applications has attracted great interest and spurred a broad search for new Dirac materials especially in monolayer structures. We present a detailed investigation of the β12 boron sheet, which is a borophene structure that can form spontaneously on a Ag(111) surface. Our tight-binding analysis revealed that the lattice of the β12-sheet could be decomposed into two triangular sublattices in a way similar to that for a honeycomb lattice, thereby hosting Dirac…
Auger Electron Spectroscopy, Low Energy Electron Diffraction and Scanning Tunneling Microscopy have been used to study the atomic structure of a Zn monolayer deposited on Ag(111) and Ag(110) substrates at room temperature. On both faces, there is formation of a close packed monolayer of Zn covering the entire substrate surface and giving rise to specific Moir{é} patterns. From a comprehensive LEED and STM data analysis, we deduce that the Zn monolayer adopts a (111) structure equivalent to a pure Zn layer rotated with respect to the silver substrate, of about $1.5^\circ$ on the Ag(111) face an…
Coherent epitaxial growth allows to produce crystalline films with strained structures which are unstable in the bulk. Thereby, the relationship between the lattice parameters of the overlayer in the interface plane, $(a,b)$, and its minimum-energy out-of-plane lattice parameter, $c_{\text{min}}(a,b)$, need not be continuous. This general statement is proven by examples of total energy calculations. As a consequence, $c_{\text{min}}$, which is determined by the choice of the substrate, and $c_{\text{min}}$-dependent intrinsic properties of the overlayer cannot always be tuned in a continuous w…
Electronic structure of S-C6H5 self-assembled monolayers on Cu(111) and Au(111) substrates
采用第一性原理密度泛函理论计算了苯硫醇（S-C $_6$ H $_5$）在Cu（111）和Au（111）衬底上的自组装单分子层（SAM）的电子结构.我们发现了SAM分子态的显着横向分散，并讨论了其对分子线阵列输运性质的影响。计算了Cu（111）表面自组装膜的双光子光电子能谱和功函数，并与已有的实验数据进行了比较。我们的研究结果被用来讨论所观察到的光谱数据的分配和产量预测新的电子状态，由于单层尚未访问实验。
The substrate contribution to the magnetic anisotropy energy (MAE) of supported nanostructures can be quantified by a site-selective manipulation of the spin-orbit coupling (SOC) and the effective exchange field B_ex. A systematic study of Co adatoms and Co monolayers on the (111) surfaces of Cu, Ag, Au, Pd and Pt is performed to study common trends in this class of materials. It is found that for adatoms, the substrate contribution is relatively small (10-30% of the MAE) while for monolayers, the substrate contribution can be substantial. The contribution from the SOC is much more important t…
The growth of up to 10 monolayer-thick Fe films on a Au(001) surface was investigated during deposition at room temperature and during annealing using low-energy electron diffraction and x-ray photoemission spectroscopy as well as locally with low-energy electron microscopy and photoemission electron microscopy. The growth proceeds with a submonolayer of Au segregating to the surface of Fe, which is in agreement with previous studies. Annealing was found to be critical for the presence of Au on the Fe surface. Our findings show that Au segregation proceeds by the formation of cracks in the Fe …
Sub-monolayer physical layer deposition of Zn on Ag(111) substrate at room temperature is investigated using Auger electron spectroscopy, low energy electron diffraction and scanning tunneling microscopy. We identified an original Zn highly-anisotropic structure in the shape of finger-like inserted dendrite in front of Zn monolayer growth. On the basis of STM observations, a mechanism of inserted dendritic growth and a mechanism of its transition to layered growth are proposed.
Monolayers (ML) of Group-6 transition-metal dichalcogenides (TMDs) are semiconducting two-dimensional materials with direct bandgap, showing promising applications in various fields of science and technology, such as nanoelectronics and optoelectronics. These monolayers can undergo strong elastic deformations, up to about 10\%, without any bond breaking. Moreover, the electronic structure and transport properties, which define the performance of these TMDs monolayers in nanoelectronic devices, can be strongly affected by the presence of point defects, which are often present in the synthetic s…
Graphene monolayers supported on oxide substrates have been demonstrated with superior charge mobility and thermal transport for potential device applications. Morphological corrugation can strongly influence the transport properties of the supported graphene. In this paper, we theoretically analyze the morphological stability of a graphene monolayer on an oxide substrate, subject to van der Waals interactions and in-plane mismatch strains. First, we define the equilibrium separation and the interfacial adhesion energy as the two key parameters that characterize the van der Waals interaction b…
In this Letter, we theoretically propose for the first time that graphene monolayers can be used for superscatterer designs. We show that the scattering cross section of the bare deep-subwavelength dielectric cylinder is markedly enhanced by six orders of magnitude due to the excitation of the first-order resonance of graphene plamons. By utilizing the tunability of the plasmonic resonance through tuning graphene's chemical potential, the graphene superscatterer works in a wide range of frequencies from several terahertz to tens of terahertz.
