The hydrogen-terminated Silicon(100)-2x1 surface (H-Si(100)-2x1) provides a promising platform for the development of atom scale devices, with recent work showing their creation through precise desorption of surface hydrogen atoms. While samples with relatively large areas of the hydrogen terminated 2x1 surface are routinely created using an in-situ methodology, surface defects are inevitably formed as well reducing the area available for patterning. Here, we present a catalog of several commonly found defects of the H-Si(100)-2x1 surface. By using a combination of scanning tunneling microscopy (STM) and non-contact atomic force microscopy (nc-AFM), we are able to extract useful information regarding the atomic and electronic structure of these defects. This allowed for the confirmation of literature assignments of several commonly found defects, as well as proposed classification of previously unreported and unassigned defects. By better understanding the structure and origin of these defects, we make the first steps toward enabling the creation of superior surfaces ultimately leading to more consistent and reliable fabrication of atom scale devices.
In this Letter, we present the first non-contact atomic force microscopy (nc-AFM) of a silicene on silver (Ag) surface, obtained by combining non-contact atomic force microscopy (nc-AFM) and scanning tunneling microscopy (STM). STM images over large areas of silicene grown on Ag(111) surface show both (sqrt13xsqrt13)R13.9° and (4x4) superstructures. For the widely observed (4x4) structure, the nc-AFM topography shows an atomic-scale contrast inversion as the tip-surface distance is decreased. At the shortest tip-surface distance, the nc-AFM topography is very similar to the STM one. The observ…
The simultaneous combination of scanning probe methods (tunnelling and force microscopies, STM and AFM) is a unique way to get an information about crystallographic and electronic structure of the studied surface. Here we apply these methods accompanied by the state-of-the-art density functional theory (DFT) calculations to shed a light on the structure and electronic properties of the strongly-corrugated graphene/Rh(111) system. The atomically resolved images are obtained for both STM and AFM modes and compared with the DFT results showing good agreement between theory and experiment.
Here we show scanning tunnelling microscopy (STM), non-contact atomic force microscopy (AFM) and inelastic electron tunnelling spectroscopy (IETS) measurements on organic molecule with a CO- terminated tip at 5K. The high-resolution contrast observed simultaneously in all channels unam- biguously demonstrates the common imaging mechanism in STM/AFM/IETS, related to the lateral bending of the CO-functionalized tip. The IETS spectroscopy reveals that the submolecular con- trast at 5K consists of both renormalization of vibrational frequency and variation of the amplitude of IETS signal. This fin…
Rh-terminated FeRh(001) film is known to be stable in a ferromagnetic (FM) state different from a G-type antiferromagnetic (G-AFM) bulk ground state, while an Fe-terminated FeRh(001) film has the same ground state as the bulk. In this paper, we investigate the magnetic properties of asymmetrically terminated FeRh(001) films: one surface is Fe-terminated and the other is Rh-terminated. Rh surface only ] (RhSO) FM state in asymmetrically terminated FeRh(001) film is identified to exhibit 40% increased perpendicular MCA energy as compare to that of the whole-layer (WL) FM state. This increased MC…
The electronic and crystallographic structure of the graphene/Rh(111) moiré lattice is studied via combination of density-functional theory calculations and scanning tunneling and atomic force microscopy (STM and AFM). Whereas the principal contrast between hills and valleys observed in STM does not depend on the sign of applied bias voltage, the contrast in atomically resolved AFM images strongly depends on the frequency shift of the oscillating AFM tip. The obtained results demonstrate the perspectives of application atomic force microscopy/spectroscopy for the probing of the chemical contra…
Halogen monolayer on a silicon surface is attracting active attention for applications in electronic device fabrication with individual impurities. To create a halogen mask for the impurities incorporation, it is desirable to be able to remove a single halogen atom from the surface. We report the desorption of individual halogen atoms from the Si(100)-2x1-Cl and -Br surfaces in a scanning tunneling microscope (STM). Silicon dangling bonds (DBs) formed on the Si surface after halogen desorption were investigated using STM and the density functional theory. Three charge states: positive, neutral…
The contrast obtained in scanning tunneling microscopy (STM) and atomic force microscopy (AFM) images is determined by the tip termination and symmetry. Functionalizing the tip with a single metal atom, CO molecule or organic species has been shown to provide high spatial resolution and insights into tip-surface interactions. A topic where this concept is utilized is the adsorption of organic molecules at surfaces. With this work we aim to contribute to the growing database of organic molecules that allow assignment by intra-molecular imaging. We investigated the organic molecule para-sexiphen…
The magnetic properties of BaFe$_{2}$As$_{2}$(001) surface have been studied by using first-principles electronic structure calculations. We find that for As-terminated surface the magnetic ground state of the top-layer FeAs is in the staggered dimer antiferromagnetic (AFM) order, while for Ba-terminated surface the collinear (single stripe) AFM order is the most stable. When a certain coverage of Ba or K atoms are deposited onto the As-terminated surface, the calculated energy differences among different AFM orders for the top-layer FeAs on BaFe$_{2}$As$_{2}$(001) can be much reduced, indicat…
Perovskite oxides attract increasing attention due to their broad potential in many applications. Understanding their surfaces is challenging, though, because the ternary composition of the bulk allows for multiple stable surface terminations. We demonstrate a simple procedure for preparing the bulk-terminated (001) surface of SrTiO3, a prototypical cubic perovskite. Controlled application of strain on a SrTiO3 single crystal results in a flat cleavage with micrometer-size domains of SrO and TiO2. Distribution of these two terminations is dictated by ferroelectric domains induced by strain dur…
CrSb is a layered antiferromagnet (AFM) with perpendicular magnetic anisotropy, a high Néel temperature, and large spin-orbit coupling (SOC), which makes it interesting for AFM spintronic applications. To elucidate the various mechanisms of Néel vector control, the effects of strain, band filling, and electric field on the magnetic anisotropy energy (MAE) of bulk and thin-film CrSb are determined and analysed using density functional theory. The MAE of the bulk crystal is large (1.2 meV per unit cell). Due to the significant ionic nature of the Cr-Sb bond, finite slabs are strongly affected by…
We have investigated electronic and magnetic properties of ultrathin SrRuO$_{3}$ (SRO) film grown on (111) SrTiO$_{3}$ substrate using the {\it ab initio} electronic structure calculations. Ru-terminated SRO (111) film suffers from strong surface atomic relaxations, while SrO$_{3}$-terminated one preserves the surface structure of ideal perovskites. Both Ru- and SrO$_{3}$-terminated SRO (111) film show unexpected interlayer antiferromagnetic (AFM) structure at the surface, but with different characters and mechanisms. The AFM structure for the former results from the large surface atomic relax…
By the first-principles electronic structure calculations, we find that energetically the most favorable cleaved $A$Fe$_2$As$_2$(001) surface ($A$=Ba, Sr, or Ca) is $A$-terminated with a $(\sqrt{2}\times \sqrt{2})R45^{\circ}$ or $(1\times 2)$ order. The $(1\times 2)$ ordered structure yields a $(1\times 2)$ dimerized STM image, in agreement with the experimental observation. The $A$ atoms are found to diffuse on the surface with a small energy barrier so that the cleaving process may destroy the $A$ atoms ordering. At the very low temperatures this may result in an As-terminated surface with t…
BaFe2As2 exhibits properties characteristic of the parent compounds of the newly discovered iron (Fe)-based high-TC superconductors. By combining the real space imaging of scanning tunneling microscopy/spectroscopy (STM/S) with momentum space quantitative Low Energy Electron Diffraction (LEED) we have identified the surface plane of cleaved BaFe2As2 crystals as the As terminated Fe-As layer - the plane where superconductivity occurs. LEED and STM/S data on the BaFe2As2(001) surface indicate an ordered arsenic (As) - terminated metallic surface without reconstruction or lattice distortion. It i…
Photoexcited Hole States at the SrTiO3(001) Surface Imaged with Noncontact AFM
TU Wien（维也纳工业大学）；University of Vienna（维也纳大学）；Charles University（查理大学）；Jagiellonian University（雅盖隆大学）；CNR-SPIN, c/o Department of Physical and Chemical Sciences, University of L’Aquila（拉奎拉大学物理与化学科学系附属意大利国家研究委员会自旋中心）
We compare STM investigations on two hexaboride compounds, SmB$_6$ and EuB$_6$, in an effort to provide a comprehensive picture of their surface structural properties. The latter is of particular importance for studying the nature of the surface states in SmB$_6$ by surface-sensitive tools. Beyond the often encountered atomically rough surface topographies of {\it in situ}, low-temperature cleaved samples, differently reconstructed as well as B-terminated and, more rarely, rare-earth terminated areas could be found. With all the different surface topographies observed on both hexaborides, a re…
The relative thermodynamic stability of surface reconstructions including vacancies, adatoms and additional layers on both CaO and MnO$_{2}$ terminations is calculated to predict the surface phase diagram of ($\sqrt{2}\times\sqrt{2}$)$\it{R}$45$^{\circ}$ CaMnO$_{3}$ (001) using $\it{ab}$ $\it{initio}$ thermodynamics. Stoichiometric and nonstoichiometric reconstructions are considered. A set of boundary conditions driven by the binary and ternary sub-phases from CaMnO$_{3}$ defines its bulk stability region, enclosing the stable surface reconstructions that can be in equilibrium with the bulk. …
Using combined low temperature scanning tunneling microscopy (STM) and atomic force microscopy (AFM), we demonstrate hydrogen passivation of individual, selected dangling bonds (DBs) on a hydrogen-passivated Si(100)-2$\times$1 surface (H-Si) by atom manipulation. This method allows erasing of DBs and thus provides an error-correction scheme for hydrogen lithography. Si-terminated tips (Si tips) for hydrogen desorption and H-terminated tips (H tips) for hydrogen passivation are both created by deliberate contact to the H-Si surface and are assigned by their characteristic contrast in AFM. DB pa…
The combination of the surface science techniques (STM, XPS, ARPES) and density-functional theory calculations was used to study the decoupling of graphene from Ni(111) by oxygen intercalation. The formation of the antiferromagnetic (AFM) NiO layer at the interface between graphene and ferromagnetic (FM) Ni is found, where graphene protects the underlying AFM/FM sandwich system. It is found that graphene is fully decoupled in this system and strongly $p$-doped via charge transfer with a position of the Dirac point of $(0.69\pm0.02)$ eV above the Fermi level. Our theoretical analysis confirms a…
A new technique for the fabrication of highly sensitive qPlus sensor for atomic force microscopy (AFM) is described. Focused ion beam was used to cut then weld onto a bare quartz tuning fork a sharp micro-tip from an electrochemically etched tungsten wire. The resulting qPlus sensor exhibits high resonance frequency and quality factor allowing increased force gradient sensitivity. Its spring constant can be determined precisely which allows accurate quantitative AFM measurements. The sensor is shown to be very stable and could undergo usual UHV tip cleaning including e-beam and field evaporati…
We have studied the surface of pure and oxidized Pt$_3$Zr(0001) by scanning tunneling microscopy (STM), Auger electron microscopy, and density functional theory (DFT). The well-annealed alloy surface shows perfect long-range chemical order. Occasional domain boundaries are probably caused by nonstoichiometry. Pt$_3$Zr exhibits ABAC stacking along [0001]; only the A-terminated surfaces are seen by STM, in agreement with DFT results showing a lower surface energy for the A termination. DFT further predicts a stronger inward relaxation of the surface Zr than for Pt, in spite of the larger atomic …
Si dangling bonds without H termination at the interface of quasi-free standing monolayer graphene (QFMLG) are known scattering centers that can severely affect carrier mobility. In this report, we study the atomic and electronic structure of Si dangling bonds in QFMLG using low-temperature scanning tunneling microscopy/spectroscopy (STM/STS), atomic force microscopy (AFM), and density functional theory (DFT) calculations. Two types of defects with different contrast were observed on a flat terrace by STM and AFM. Their STM contrast varies with bias voltage. In STS, they showed characteristic …
Ultra-wide bandgap and the absence of shallow dopants are the major challenges in realizing diamond based electronics. However, the surface functionalization offers an excellent alternative to tune electronic structure of diamonds. Herein, we report on tuning the surface electronic properties of hydrogenated polycrystalline diamond films through oxygen functionalization. The hydrogenated diamond (HD) surface transforms from hydrophobic to hydrophilic nature and the sheet resistance increases from ~ 8 kohms/sq. to over 10 Gohms/sq. with progressive ozonation. The conductive atomic force microsc…
Hidden order in URu$_2$Si$_2$ has remained a mystery now entering its 4th decade. The importance of resolving the nature of the hidden order has stimulated extensive research. Here we present a detailed characterization of different surface terminations in URu$_2$Si$_2$ by angle-resolved photoemission spectroscopy, in conjunction with scanning tunneling spectroscopy and DMFT calculations that may unveil a new piece of this puzzle. The U-terminated surface is characterized by an electron-like band around the $\bar{X}$ point, while a hole-like band for the Si-terminated surface. We also investig…
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 have studied the incommensurate moiré structure of epitaxial graphene grown on iridium(111) by dynamic low energy electron diffraction [LEED-I(V)] and non-contact atomic force microscopy (AFM) with a CO terminated tip. Our LEED-I(V) results yield the average positions of all the atoms in the surface unit cell and are in qualitative agreement with the structure obtained from density functional theory (DFT). The AFM experiments reveal local variations of the moiré structure: the corrugation varies smoothly over several moiré unit cells between 42 and 56 pm. We attribute these variations to th…
The adsorption of CO molecules at the Ca3Ru2O7(001) surface was studied using low-temperature scanning tunneling microscopy (STM) and density functional theory (DFT). Ca3Ru2O7 can be easily cleaved along the (001) plane, yielding a smooth, CaO-terminated surface. The STM shows a characteristic pattern with alternating dark and bright stripes, resulting from the tilting of the RuO$_6$ octahedra. At 78,K, CO adsorbs at an apical surface O at the channel edge with a predicted binding energy of $E_{ads} = -0.85$eV. After annealing at room temperature, the CO forms a strong bond ($E_{ads}= -2.04$eV…
Many new material systems are being explored to enable smaller, more capable and energy efficient devices. These bottom up approaches for atomic and molecular electronics, quantum computation, and data storage all rely on a well-developed understanding of materials at the atomic scale. Here, we report a versatile scanning tunneling microscope (STM) charge characterization technique, which reduces the influence of the typically perturbative STM tip field, to develop this understanding even further. Using this technique, we can now observe single molecule binding events to atomically defined rea…
Alkane chains are the most commonly used molecules for monolayer fabrication. Long chains are used for their strong van der Waals interactions inducing good layer organization. Amine function-terminated alkyl chains are of great interest and are widely used for further surface functionalization. Since it is mandatory that such layers be organized to provide amine moieties at the surface, the present study deals with exploring amine-terminated SAM formation as an alternative to the usual aminopropylalkylsilane SAM. Additionally, using a long NH2terminated alkyl chain allows the formation of hyd…
Using a non-contact atomic force microscope (nc-AFM), we examine continuous DB wire structures on the hydrogen-terminated silicon (100) 2x1 surface. By probing the DB structures at varying energies, we identify the formation of previously unobserved ionic charge distributions correlated to the net charge of DB wires and their predicted lattice distortion. Performing spectroscopic analysis, we identify higher energy configurations corresponding to alternative lattice distortions as well as tip-induced charging effects. By varying the length and orientation of these DB structures, we further hig…
Epitaxial graphene grown on transition metal surfaces typically exhibits a moiré pattern due to the lattice mismatch between graphene and the underlying metal surface. We use both scanning tunneling microscopy (STM) and atomic force microscopy (AFM) experiments to probe the electronic and topographic contrast of the graphene moiré on the Ir(111) surface. While STM topography is influenced by the local density of states close to the Fermi energy and the local tunneling barrier height, AFM is capable of yielding the 'true' surface topography once the background force arising from the van der Waa…
Atomic-scale characteristics of surfaces dictate the principles governing numerous scientific phenomena ranging from catalysis to friction. Despite this fact, our ability to visualize and alter surfaces on the atomic scale is severely hampered by the strict conditions under which the related methods are operated to achieve high spatial resolution. In particular, the two prominent methods utilized to achieve atomic-resolution imaging - scanning tunneling microscopy (STM) and noncontact atomic force microscopy (NC-AFM) - are typically performed under ultrahigh vacuum (UHV) and often at low tempe…
Bi(0001) films with thicknesses up to several bilayers (BLs) are grown on Se-terminated Bi$_2$Se$_3$(0001) surfaces, and low energy electron diffraction (LEED), low energy ion scattering (LEIS) and atomic force microscopy (AFM) are used to investigate the surface composition, topography and atomic structure. For a single deposited Bi BL, the lattice constant matches that of the substrate and the Bi atoms adjacent to the uppermost Se atoms are located at fcc-like sites. When a 2nd Bi bilayer is deposited, it is incommensurate with the substrate. As the thickness of the deposited Bi film increas…
Silicon carbide (SiC) is an excellent substrate for growth and manipulation of large scale, high quality epitaxial graphene. On the carbon face (the ($\bar{1}\bar{1}\bar{1}$) or $(000\bar{1}$) face, depending on the polytype), the onset of graphene growth is intertwined with the formation of several competing surface phases, among them a (3$\times$3) precursor phase suspected to hinder the onset of controlled, near-equilibrium growth of graphene. Despite more than two decades of research, the precise atomic structure of this phase is still unclear. We present a new model of the (3$\times$3)-Si…
We present theoretically the electronic structure of antiferromagnetic (AFM) FeSe monolayer on TiO$_{2}$ terminated SrTiO$_{3}$(001) surface. It is revealed that the striking disappearance of the Fermi surface around the Brillouin zone (BZ) center can be well explained by the antiferromatnetic (AFM) phase. We show that the system has a considerable charge transfer from SrTiO$_{3}$(001) substrate to FeSe monolayer, and so has a self-constructed electric field. The FeSe monolayer band structure near the BZ center is sensitive to charge doping, and the spin-resolved energy bands at BZ corner are …
We combined in-situ scanning tunneling microscopy (STM) with the conventional growth characterization methods of atomic force microscopy (AFM) and reflection high energy electron diffraction (RHEED) to simultaneously assess atomic-scale impurities and the larger-scale surface morphology of molecular beam epitaxy (MBE) grown homoepitaxial InAs(111)A. By keeping a constant substrate temperature and indium flux while increasing the As$_2$ flux, we find two differing MBE growth parameter regions for optimized surface roughness on the macro and atomic scale. In particular, we show that a pure step-…
Structural defects in 2D materials offer an effective way to engineer new material functionalities beyond conventional doping in semiconductors. Specifically, deep in-gap defect states of chalcogen vacancies have been associated with intriguing phenomena in monolayer transition metal dichalcogenides (TMDs). Here, we report the direct experimental correlation of the atomic and electronic structure of a sulfur vacancy in monolayer WS2 by a combination of CO-tip noncontact atomic force microscopy (nc-AFM) and scanning tunneling microscopy (STM). Sulfur vacancies, which are absent in as-grown samp…
We report the study of single dangling bonds (DB) on the hydrogen terminated silicon (100) surface using a low temperature scanning tunneling microscope (LT-STM). By investigating samples prepared with different annealing temperatures, we establish the critical role of subsurface arsenic dopants on the DB electronic properties. We show that when the near surface concentration of dopants is depleted as a result of $1250°C$ flash anneals, a single DB exhibits a sharp conduction step in its I(V) spectroscopy that is not due to a density of states effect but rather corresponds to a DB charge state…
The layered MnBi2nTe3n+1 family represents the first intrinsic antiferromagnetic topological insulator (AFM TI, protected by a combination symmetry ) ever discovered, providing an ideal platform to explore novel physics such as quantum anomalous Hall effect at elevated temperature and axion electrodynamics. Recent angle-resolved photoemission spectroscopy (ARPES) experiments on this family have revealed that all terminations exhibit (nearly) gapless topological surface states (TSSs) within the AFM state, violating the definition of the AFM TI, as the surfaces being studied should be -breaking …
Based on first-principles calculations and symmetry analysis, we propose that EuIn$_2$As$_2$ is a long awaited axion insulator with antiferromagnetic (AFM) long range order. Characterized by the parity-based invariant $\mathbb Z_4=2$, the topological magneto-electric effect is quantized with $θ=π$ in the bulk, with a band gap as large as 0.1 eV. When the staggered magnetic moment of the AFM phase is along $a/b$ axis, it's also a TCI phase. Gapless surface states emerge on (100), (010) and (001) surfaces, protected by mirror symmetries (nonzero mirror Chern numbers). When the magnetic moment is…
Quasi free standing monolayer graphene (QFMLG) grown on SiC by selective Si evaporation from the Si-rich SiC(0001) face and H intercalation displays irregularities in STM and AFM analysis, appearing as localized features, which we previously identified as vacancies in the H layer coverage [Y Murata, et al. Nano Res, in press, DOI: 10.1007/s12274-017-1697-x]. The size, shape, brightness, location, and concentration of these features, however, are variable, depending on the hydrogenation conditions. In order to shed light on the nature of these features, in this work we perform a systematic Dens…
The non-centrosymmetric semiconductor BiTeI exhibits two distinct surface terminations that support spin-split Rashba surface states. Their ambipolarity can be exploited for creating spin-polarized $p$-$n$ junctions at the boundaries between domains with different surface terminations. We use scanning tunneling microscopy/spectroscopy (STM/STS) to locate such junctions and investigate their atomic and electronic properties. The Te- and I-terminated surfaces are identified owing to their distinct chemical reactivity, and an apparent height mismatch of electronic origin. The Rashba surface state…
Graphene, consisting of an inert, thermally stable material with an atomically flat, dangling bond-free surface is by essence an ideal template layer for van der Waals heteroepitaxy of two-dimensional materials such as silicene. However, depending on the synthesis method and growth parameters, graphene (Gr) substrates could exhibit, on a single sample, various surface structures, thicknesses, defects, and step heights. These structures noticeably affect the growth mode of epitaxial layers, e.g. turning the layer-by-layer growth into the Volmer-Weber growth promoted by defect-assisted nucleatio…
