Geometry and electronic structure of iridium adsorbed on graphene

We report investigation of the geometry and electronic structure of iridium atoms adsorbed onto graphene through a combined experimental and theoretical study. Ir atoms were deposited onto a flake of graphene on a Pt(111) surface and found to form clusters even at low temperatures. The areal density of the observed clusters on the graphene flake suggests the clusters are most likely pairs of Ir atoms. Theoretical ab initio density functional (DFT) calculations indicate that these Ir dimers are oriented horizontally, near neighboring "bridge" sites of the graphene lattice, as this configuration has the strongest adsorption energy of all high-symmetry configurations for the Ir dimer. A large peak in the local density of states (LDOS) at the Dirac point energy was measured via scanning tunneling spectroscopy, and this result is reproduced by a DFT calculation of the LDOS. The peak at the Dirac point energy is found to be from the Ir s and p states. The LDOS in the monomer case was also calculated, and is found to significantly differ from the experimentally determined data, further supporting the hypothesis of low-temperature clustering

Reversible writing of high-mobility and high-carrier-density doping patterns in two-dimensional van der Waals heterostructures

A key feature of two-dimensional materials is that the sign and concentration of their carriers can be externally controlled with techniques such as electrostatic gating. However, conventional electrostatic gating has limitations, including a maximum carrier density set by the dielectric breakdown, and ionic liquid gating and direct chemical doping also suffer from drawbacks. Here, we show that an electron-beam-induced doping technique can be used to reversibly write high-resolution doping patterns in hexagonal boron nitride-encapsulated graphene and molybdenum disulfide (MoS2) van der Waals heterostructures. The doped MoS2 device exhibits an order of magnitude decrease of subthreshold swing compared with the device before doping, whereas the doped graphene devices demonstrate a previously inaccessible regime of high carrier concentration and high mobility, even at room temperature. We also show that the approach can be used to write high-quality p–n junctions and nanoscale doping patterns, illustrating that the technique can create nanoscale circuitry in van der Waals heterostructures

Single-Atom Gating of Quantum State Superpositions

The ultimate miniaturization of electronic devices will likely require local and coherent control of single electronic wavefunctions. Wavefunctions exist within both physical real space and an abstract state space with a simple geometric interpretation: this state space--or Hilbert space--is spanned by mutually orthogonal state vectors corresponding to the quantized degrees of freedom of the real-space system. Measurement of superpositions is akin to accessing the direction of a vector in Hilbert space, determining an angle of rotation equivalent to quantum phase. Here we show that an individual atom inside a designed quantum corral can control this angle, producing arbitrary coherent superpositions of spatial quantum states. Using scanning tunnelling microscopy and nanostructures assembled atom-by-atom we demonstrate how single spins and quantum mirages can be harnessed to image the superposition of two electronic states. We also present a straightforward method to determine the atom path enacting phase rotations between any desired state vectors. A single atom thus becomes a real space handle for an abstract Hilbert space, providing a simple technique for coherent quantum state manipulation at the spatial limit of condensed matter.Comment: Published online 6 April 2008 in Nature Physics; 17 page manuscript (including 4 figures) + 3 page supplement (including 2 figures); supplementary movies available at http://mota.stanford.ed

Quantum Holographic Encoding in a Two-dimensional Electron Gas

The advent of bottom-up atomic manipulation heralded a new horizon for attainable information density, as it allowed a bit of information to be represented by a single atom. The discrete spacing between atoms in condensed matter has thus set a rigid limit on the maximum possible information density. While modern technologies are still far from this scale, all theoretical downscaling of devices terminates at this spatial limit. Here, however, we break this barrier with electronic quantum encoding scaled to subatomic densities. We use atomic manipulation to first construct open nanostructures--"molecular holograms"--which in turn concentrate information into a medium free of lattice constraints: the quantum states of a two-dimensional degenerate Fermi gas of electrons. The information embedded in the holograms is transcoded at even smaller length scales into an atomically uniform area of a copper surface, where it is densely projected into both two spatial degrees of freedom and a third holographic dimension mapped to energy. In analogy to optical volume holography, this requires precise amplitude and phase engineering of electron wavefunctions to assemble pages of information volumetrically. This data is read out by mapping the energy-resolved electron density of states with a scanning tunnelling microscope. As the projection and readout are both extremely near-field, and because we use native quantum states rather than an external beam, we are not limited by lensing or collimation and can create electronically projected objects with features as small as ~0.3 nm. These techniques reach unprecedented densities exceeding 20 bits/nm2 and place tens of bits into a single fermionic state.Comment: Published online 25 January 2009 in Nature Nanotechnology; 12 page manuscript (including 4 figures) + 2 page supplement (including 1 figure); supplementary movie available at http://mota.stanford.ed

Strong correlations and orbital texture in single-layer 1T-TaSe2

Strong electron correlation can induce Mott insulating behaviour and produce intriguing states of matter such as unconventional superconductivity and quantum spin liquids. Recent advances in van der Waals material synthesis enable the exploration of Mott systems in the two-dimensional limit. Here we report characterization of the local electronic properties of single- and few-layer 1T-TaSe2 via spatial- and momentum-resolved spectroscopy involving scanning tunnelling microscopy and angle-resolved photoemission. Our results indicate that electron correlation induces a robust Mott insulator state in single-layer 1T-TaSe2 that is accompanied by unusual orbital texture. Interlayer coupling weakens the insulating phase, as shown by reduction of the energy gap and quenching of the correlation-driven orbital texture in bilayer and trilayer 1T-TaSe2. This establishes single-layer 1T-TaSe2 as a useful platform for investigating strong correlation physics in two dimensions

Topological Surface States Protected From Backscattering by Chiral Spin Texture

Topological insulators are a new class of insulators in which a bulk gap for electronic excitations is generated by strong spin orbit coupling. These novel materials are distinguished from ordinary insulators by the presence of gapless metallic boundary states, akin to the chiral edge modes in quantum Hall systems, but with unconventional spin textures. Recently, experiments and theoretical efforts have provided strong evidence for both two- and three-dimensional topological insulators and their novel edge and surface states in semiconductor quantum well structures and several Bi-based compounds. A key characteristic of these spin-textured boundary states is their insensitivity to spin-independent scattering, which protects them from backscattering and localization. These chiral states are potentially useful for spin-based electronics, in which long spin coherence is critical, and also for quantum computing applications, where topological protection can enable fault-tolerant information processing. Here we use a scanning tunneling microscope (STM) to visualize the gapless surface states of the three-dimensional topological insulator BiSb and to examine their scattering behavior from disorder caused by random alloying in this compound. Combining STM and angle-resolved photoemission spectroscopy, we show that despite strong atomic scale disorder, backscattering between states of opposite momentum and opposite spin is absent. Our observation of spin-selective scattering demonstrates that the chiral nature of these states protects the spin of the carriers; they therefore have the potential to be used for coherent spin transport in spintronic devices.Comment: to be appear in Nature on August 9, 200

Quasi-particle interference and superconducting gap in a high-temperature superconductor Ca2-xNaxCuO2Cl2

High-transition-temperature (high-Tc) superconductivity is ubiquitous in the cuprates containing CuO2 planes but each cuprate has its own character. The study of the material dependence of the d-wave superconducting gap (SG) should provide important insights into the mechanism of high-Tc. However, because of the 'pseudogap' phenomenon, it is often unclear whether the energy gaps observed by spectroscopic techniques really represent the SG. Here, we report spectroscopic imaging scanning tunneling microscopy (SI-STM) studies of nearly-optimally-doped Ca2-xNaxCuO2Cl2 (Na-CCOC) with Tc = 25 ~ 28 K. They enable us to observe the quasi-particle interference (QPI) effect in this material, through which unambiguous new information on the SG is obtained. The analysis of QPI in Na-CCOC reveals that the SG dispersion near the gap node is almost identical to that of Bi2Sr2CaCu2Oy (Bi2212) at the same doping level, while Tc of Bi2212 is 3 times higher than that of Na-CCOC. We also find that SG in Na-CCOC is confined in narrower energy and momentum ranges than Bi2212. This explains at least in part the remarkable material dependence of TcComment: 13pages, 4fig

One-dimensional Topological Edge States of Bismuth Bilayers

The hallmark of a time-reversal symmetry protected topologically insulating state of matter in two-dimensions (2D) is the existence of chiral edge modes propagating along the perimeter of the system. To date, evidence for such electronic modes has come from experiments on semiconducting heterostructures in the topological phase which showed approximately quantized values of the overall conductance as well as edge-dominated current flow. However, there have not been any spectroscopic measurements to demonstrate the one-dimensional (1D) nature of the edge modes. Among the first systems predicted to be a 2D topological insulator are bilayers of bismuth (Bi) and there have been recent experimental indications of possible topological boundary states at their edges. However, the experiments on such bilayers suffered from irregular structure of their edges or the coupling of the edge states to substrate's bulk states. Here we report scanning tunneling microscopy (STM) experiments which show that a subset of the predicted Bi-bilayers' edge states are decoupled from states of Bi substrate and provide direct spectroscopic evidence of their 1D nature. Moreover, by visualizing the quantum interference of edge mode quasi-particles in confined geometries, we demonstrate their remarkable coherent propagation along the edge with scattering properties that are consistent with strong suppression of backscattering as predicted for the propagating topological edge states.Comment: 15 pages, 5 figures, and supplementary materia

Anisotropic behaviors of massless Dirac fermions in graphene under periodic potential

Charge carriers of graphene show neutrino-like linear energy dispersions as well as chiral behavior near the Dirac point. Here we report highly unusual and unexpected behaviors of these carriers in applied external periodic potentials, i.e., in graphene superlattices. The group velocity renormalizes highly anisotropically even to a degree that it is not changed at all for states with wavevector in one direction but is reduced to zero in another, implying the possibility that one can make nanoscale electronic circuits out of graphene not by cutting it but by drawing on it in a non-destructive way. Also, the type of charge carrier species (e.g. electron, hole or open orbit) and their density of states vary drastically with the Fermi energy, enabling one to tune the Fermi surface-dominant properties significantly with gate voltage. These results address the fundamental question of how chiral massless Dirac fermions propagate in periodic potentials and point to a new possible path for nanoscale electronics.Comment: 10 pages, 9 figure

Polarons and confinement of electronic motion to two dimensions in a layered transition metal oxide

A very remarkable feature of the layered transition metal oxides (TMOs), whose most famous members are the high-temperature superconductors (HTSs), is that even though they are prepared as bulk three-dimensional single crystals, they display hugely anisotropic electrical and optical properties, seeming to be insulating perpendicular to the layers and metallic within them. This is the phenomenon of confinement, a concept at odds with the conventional theory of solids and recognized as due to magnetic and electron-lattice interactions in the layers which must be overcome at a substantial energy cost if electrons are to be transferred between layers. The associated energy gap or 'pseudogap' is particularly obvious in experiments where charge is moved perpendicular to the planes, most notably scanning tunneling microscopy (STM) and polarized infrared spectroscopy. Here, using the same experimental tools, we show that there is a second family of TMOs - the layered manganites La2-2xSr1+2xMn2O7 (LSMO) - with even more extreme confinement and pseudogap effects. The data, which are the first to resolve atoms in any metallic manganite, demonstrate quantitatively that because they are attached to polarons - lattice and spin textures within the planes -, it is equally difficult to remove carriers from the planes via vacuum tunneling into a conventional metallic tip, as it is for them to move between Mn-rich layers within the material itself