In this work, systematic constant-bias, variable-current scanning tunneling microscopy (STM) measurements and STM simulations from density-functional theory are made, yielding critical insights into the spatial structure of electrons in graphene. A foundational comparison is drawn between graphene and graphite, showing the surface charge density of graphene to be 300 percent that of graphite. Furthermore, simulated STM images reveal that high-current STM better resolves graphenes honeycomb bonding structure because of a retraction which occurs in the topmost dangling bond orbitals.
This lecture has been given at the 45th Spring School: Computing Solids: Models, Ab-initio Methods and Supercomputing organized at the Forschungszentrum Jülich. The goal of this manuscript is to review the basics behind the theory accompanying Scanning Tunneling Microscopy.
This review covers recent experimental progress in probing the electronic properties of graphene and how they are influenced by various substrates, by the presence of a magnetic field and by the proximity to a superconductor. The focus is on results obtained using scanning tunneling microscopy, spectroscopy, transport and magneto-transport techniques.
We consider scanning gate microscopy imaging of the double slit interference for a pair of quantum point contacts (QPCs) defined within the two-dimensional electron gas. The interference is clearly present in the scattered electron wave functions for each of the incident subbands. Nevertheless, we find that the interference is generally missing in the experimentally accessible conductance maps for many incident subbands. We explain this finding on the basis of the Landauer approach. A setup geometry allowing for observation of the double slit interference by the scanning gate microscopy is pro…
We have performed low-temperature scanning tunneling spectroscopy measurements on suspended single-wall carbon nanotubes with a gate electrode allowing three-terminal spectroscopy measurements. These measurements show well-defined Coulomb diamonds as well as side peaks from phonon-assisted tunneling. The side peaks have the same gate voltage dependence as the main Coulomb peaks, directly proving that they are excitations of these states.
Acquisition and analysis is described for scanning tunneling spectroscopy data acquired from a monolayer of WSe$_2$ grown on epitaxial graphene on SiC. Curve fitting of the data is performed, in order to deduce band-edge energies. In addition to describing the details of the theoretical curves used for the fitting, the acquisition and analysis methods are also discussed within the larger context of the historical development of scanning tunneling spectroscopy techniques.
Systematic displacement measurements of freestanding graphene as a function of applied bias voltage and tunneling current setpoint using scanning tunneling microscopy (STM) are presented. When the bias voltage is increased the graphene approaches the STM tip, while, on the other hand, when the tunneling current is increased the graphene contracts from the STM tip. To understand the role of the bias voltage, we quantitatively model the attractive force between the tip and the sample using electrostatics. For the tunneling current, we qualitatively model the contraction of the graphene using ent…
Correlated electron states in high mobility two-dimensional electron systems (2DESs), including charge density waves and microemulsion phases intermediate between a Fermi liquid and Wigner crystal, are predicted to exhibit complex local charge order. Existing experimental studies, however, have mainly probed these systems at micron to millimeter scales rather than directly mapping spatial organization. Scanning probes should be well-suited to study the spatial structure of these states, but high mobility 2DESs are found at buried semiconductor interfaces, beyond the reach of conventional scann…
We report low temperature high magnetic field scanning tunneling microscopy and spectroscopy of graphene flakes on graphite that exhibit the structural and electronic properties of graphene decoupled from the substrate. Pronounced peaks in the tunneling spectra develop with field revealing a Landau level sequence that provides a direct way to identify graphene and to determine the degree of its coupling to the substrate. The Fermi velocity and quasiparticle lifetime, obtained from the positions and width of the peaks, provide access to the electron-phonon and electron-electron interactions.
We demonstrate the emergence of classical features in electronic quantum transport for the scanning gate microscopy response in a cavity defined by a quantum point contact and a micron-sized circular reflector. The branches in electronic flow characteristic of a quantum point contact opening on a two-dimensional electron gas with weak disorder are folded by the reflector, yielding a complex spatial pattern. Considering the deflection of classical trajectories by the scanning gate tip allows to establish simple relationships of the scanning pattern, which are in agreement with recent experiment…
In scanning tunneling experiments on semiconductor surfaces, the energy scale within the tunneling junction is usually unknown due to tip-induced band bending. Here, we experimentally recover the zero point of the energy scale by combining scanning tunneling microscopy with Kelvin probe force spectroscopy. With this technique, we revisit shallow acceptors buried in GaAs. Enhanced acceptor-related conductance is observed in negative, zero, and positive band-bending regimes. An Anderson-Hubbard model is used to rationalize our findings, capturing the crossover between the acceptor state being pa…
We have developed a fabrication process for incorporating a gate electrode into suspended single-walled carbon nanotube structures for scanning tunneling spectroscopy studies. The nanotubes are synthesized by chemical vapor deposition directly on a metal surface. The high temperature ~800 C involved in the growth process poses challenging issues such as surface roughness and integrity of the structure which are addressed in this work. We demonstrate the effectiveness of the gate on the freestanding part of the nanotubes by performing tunneling spectroscopy that reveals Coulomb blockade diamond…
Achieving a high intensity in inelastic scanning tunneling spectroscopy (IETS) is important for precise measurements. The intensity of the IETS signal can vary up to a factor three for various tips without an apparent reason accessible by scanning tunneling microscopy (STM) alone. Here, we show that combining STM and IETS with atomic force microscopy enables carbon monoxide front atom identification, revealing that high IETS intensities for CO/Cu(111) are obtained for single atom tips, while the intensity drops sharply for multi-atom tips. Adsorbing the CO molecule on a Cu adatom [CO/Cu/Cu(111…
Scanning tunneling images of carbon nanotubes frequently show electron distributions which break the local sixfold symmetry of the graphene sheet. We present a theory of these images which relates these anisotropies to the off diagonal correlations in the single particle density matrix, and allows one to extract these correlations from the observed images. The theory is applied to images of the low energy states reflected at the end of a tube or by point defects, and to states propagating on defect free semiconducting tubes. The latter exhibit a novel switching of the anisotropy in the tunneli…
A scanning tunneling microscopy based potentiometry technique for the measurements of the local surface electric potential is presented and illustrated by experiments performed on current-carrying thin tungsten films. The obtained results demonstrate a sub-millivolt resolution in the measured surface potential. The application of this potentiometry technique to the local sensing of the spin Hall effect is outlined and some experimental results are reported.
We show that scanning gate microscopy can be used for probing electron-electron interactions inside a nanostructure. We assume a simple model made of two non-interacting strips attached to an interacting nanosystem. In one of the strips, the electrostatic potential can be locally varied by a charged tip. This change induces corrections upon the nanosystem Hartree-Fock self-energies which enhance the fringes spaced by half the Fermi wavelength in the images giving the quantum conductance as a function of the tip position.
We perform scanning-gate microscopy on a quantum-point contact. It is defined in a high-mobility two-dimensional electron gas of an AlGaAs/GaAs heterostructure, giving rise to a weak disorder potential. The lever arm of the scanning tip is significantly smaller than that of the split gates defining the conducting channel of the quantum-point contact. We are able to observe that the conducting channel is shifted in real space when asymmetric gate voltages are applied. The observed shifts are consistent with transport data and numerical estimations.
A theoretical description of scanning tunneling potentoimetry (STP) measurement is presented to address the increasing need for a basis to interpret experiments on macrscopic samples. Based on a heuristic understanding of STP provided to facilitate theoretical understanding, the total tunneling current related to the density matrix of the sample is derived within the general framework of quantum transport. The measured potentiometric voltage is determined implicitly as the voltage necessary to null the tunneling current. Explicit expressions of measured voltages are presented under certain ass…
We study electronic and topographic properties of the Si(335) surface, containing Au wires parallel to the steps. We use scanning tunneling microscopy (STM) supplemented by reflection of high energy electron diffraction (RHEED) technique. The STM data show the space and voltage dependent oscillations of the distance between STM tip and the surface which can be explained within one band tight binding Hubbard model. We calculate the STM current using nonequilibrium Keldysh Green function formalism.
We perform scanning gate microscopy on individual suspended carbon nanotube quantum dots. The size and position of the quantum dots can be visually identified from the concentric high conductance rings. For the ultra clean devices used in this study, two new effects are clearly identified. Electrostatic screening creates non-overlapping multiple sets of Coulomb rings from a single quantum dot. In double quantum dots, by changing the tip voltage, the interactions between the quantum dots can be tuned from the weak to strong coupling regime.
We propose a new method for atomic-scale imaging of spatial current patterns in nanoscopic quantum networks by using scanning tunneling microscopy (STM). By measuring the current flowing from the STM tip into one of the leads attached to the network as a function of tip position, one obtains an atomically resolved spatial image of "current riverbeds" whose spatial structure reflects the coherent flow of electrons out of equilibrium. We show that this method can be successfully applied in variety of network topologies, and is robust against dephasing effects.
We study interfacial water trapped between a sheet of graphene and a muscovite (mica) surface using Raman spectroscopy and ultra-high vacuum scanning tunneling microscopy (UHV-STM) at room temperature. We are able to image the graphene-water interface with atomic resolution, revealing a layered network of water trapped underneath the graphene. We identify water layer numbers with a carbon nanotube height reference. Under normal scanning conditions, the water structures remain stable. However, at greater electron energies, we are able to locally manipulate the water using the STM tip.
Graphene flakes are prepared on freshly cleaved mica by exfoliation and studied by scanning tunneling microscopy in ultra high vacuum. On few-layer graphene, a triangular network of partial dislocations separating ABC stacked and ABA stacked graphene was found similar to the networks occasionally visible on freshly cleaved HOPG. We found differences in the electronic structure of ABC and ABA stacked areas by scanning tunneling spectroscopy, i.e., a pronounced peak at 0.25 eV above the Fermi level exclusively in the ABA areas, which is shown to be responsible for the different apparent heights …
We use low-temperature scanning gate microscopy (SGM) to investigate the breakdown of the quantum Hall regime in an exfoliated bilayer graphene flake. SGM images captured during breakdown exhibit intricate patterns of "hotspots" where the conductance is strongly affected by the presence of the tip. Our results are well described by a model based on quantum percolation which relates the points of high responsivity to tip-induced scattering between localized Landau levels.
A technique to locally generate mechanical vibrations in freestanding graphene using scanning tunneling microscopy (STM) is presented. The frequency of the mechanical vibrations is tuned over nearly four decades and is centered around 10 Hz. The amplitude of the vibrations also changes over nearly three decades centered on 1 nm. The oscillating motion is generated in two ways: first, by scanning the STM tip on the surface and second, by scanning the bias voltage on the STM tip. The frequency and amplitude of the displaced freestanding graphene is quantitatively transformed to the frequency and…
We present a multi-tip scanning tunneling potentiometry technique that can be implemented into existing multi-tip scanning tunneling microscopes without hardware changes. The resulting setup allows flexible in situ contacting of samples under UHV conditions and subsequent measurement of the sample topography and local electric potential with resolution down to Å and μV, respectively. The performance of the potentiometry feedback is demonstrated by thermovoltage measurements on the Ag/Si$(111)-(\sqrt3\times\sqrt3)\rm R30^{\circ}$ surface by resolving a standing wave pattern. Subsequently, the a…
This paper presents a brief review of scanning-gate microscopy applied to the imaging of electron transport in buried semiconductor quantum structures. After an introduction to the technique and to some of its practical issues, we summarise a selection of its successful achievements found in the literature, including our own research. The latter focuses on the imaging of GaInAs-based quantum rings both in the low magnetic field Aharonov-Bohm regime and in the high-field quantum Hall regime. Based on our own experience, we then discuss in detail some of the limitations of scanning-gate microsco…
We propose a novel probe technique capable of performing local low-temperature spectroscopy on a 2D electron system (2DES) in a semiconductor heterostructure. Motivated by predicted spatially-structured electron phases, the probe uses a charged metal tip to induce electrons to tunnel locally, directly below the tip, from a "probe" 2DES to a "subject" 2DES of interest. We test this concept with large-area (non-scanning) tunneling measurements, and predict a high spatial resolution and spectroscopic capability, with minimal influence on the physics in the subject 2DES.
The electroluminescence of a polythiophene wire suspended between two metallic electrodes is probed using a scanning tunneling microscope. Under positive sample voltage, the spectral and voltage dependencies of the emitted light are consistent with the fluorescence of the wire junction mediated by localized plasmons. This emission is strongly attenuated for the opposite polarity. Both emission mechanism and polarity dependence are similar to what occurs in organic light emitting diodes (OLED) but at the level of a single molecular wire.
Atomic-scale topography of epitaxial multilayer graphene grown on 4H-SiC(0001) was investigated using scanning tunneling microscopy (STM). Bunched nano-ridges ten times smaller than previously recorded were observed throughout the surface, the morphology of which was systematically altered using a relatively new technique called electrostatic-manipulation scanning tunneling microscopy. Transformed graphene formations sometimes spontaneously returned to their original morphology, while others permanently changed. Using an electrostatic model, we calculate that a force up to ~5 nN was exerted by…
We present a method capable of calculating elastic scanning tunneling microscopy (STM) currents from localized atomic orbital density functional theory (DFT). To overcome the poor accuracy of the localized orbital description of the wave functions far away from the atoms, we propagate the wave functions, using the total DFT potential. From the propagated wave functions, the Bardeen's perturbative approach provides the tunneling current. To illustrate the method we investigate carbon monoxide adsorbed on a Cu(111) surface and recover the depression/protrusion observed experimentally with normal…
Indium arsenide nanowires grown by selective-area vapor phase epitaxy are used as tips for scanning tunneling microscopy (STM). The STM tips are realized by positioning the wires manually on the corner of a double cleaved gallium arsenide wafer with submicrometer precision and contacting them lithographically, which is fully compatible with further integrated circuitry on the GaAs wafer. STM images show a z-noise of 2 pm and a lateral stability of, at least, 0.5 nm on a Au(111) surface. I(z) spectroscopy reveals an exponential decay indicating tunneling through vacuum. Subsequent electron micr…
Temperature imaging of nanoscale systems is a fundamental problem which has myriad potential technological applications. For example, nanoscopic cold spots can be used for spot cooling electronic components while hot spots could be used for precise activation of chemical or biological reactions. More fundamentally, imaging the temperature fields in quantum coherent conductors can provide a wealth of information on heat flow and dissipation at the smallest scales. However, despite significant technological advances, the spatial resolution of temperature imaging remains in the few nanometers ran…
Using the non-equilibrium Keldysh formalism, we investigate the spatial relation between the electro-chemical potential measured in scanning tunneling spectroscopy, and local current patterns over the entire range from the quantum to the classical transport regime. These quantities show similar spatial patterns near the quantum limit, but are related by Ohm's law only in the classical regime. We demonstrate that defects induce a Landauer residual resistivity dipole in the electro-chemical potential with the concomitant spatial current pattern representing the field lines of the dipole.
Spin-momentum locking in the surface mode of topological insulators (TI) leads to the surface accumulation of spin-polarized electrons caused by bias current flows through TI samples. Here, we demonstrate that scanning tunneling microscopy can be used to sense this surface spin-polarized electron accumulation. We present experimental results of this sensing for Sn-doped Bi$_2$Se$_3$ samples by employing Fe-coated W tips as well as non-magnetic W tips. We observe a linear increase in the spin-accumulation as a function of bias current through TI samples.
An extension of the direct-current, double-lamella drop-off technique for electrochemically etching tungsten scanning-tunneling-microscope tips is presented. The key fabrication step introduced here is the use of an etch stop as a simple but accurate way to optimize the contact area between the etchant and the wire. By restricting the etching process, the final cone angle of the tips can be made sharp and mechanically stable without a lot of finesse from the STM tip maker.
We investigate the correlations of mutual positions of charge density waves nodes in side-by-side placed InAs nanowires in presence of a conductive atomic force microscope tip served as a mobile gate at helium temperatures. Scanning gate microscopy scans demonstrate mutual correlation of positions of charge density waves nodes of two wires. A general mutual shift of the nodes positions and "crystal lattice mismatch" defect were observed. These observations demonstrate the crucial role of Coulomb interaction in formation of charge density waves in InAs nanowires.
Graphene is a truly two-dimensional material with exceptional electronic, mechanical, and optical properties. As such, it consists of surface only and can be probed by the well developed surface-science techniques as, e.g., scanning tunneling microscopy. This method bridges the gap between the surface science community and the electronic device community and might lead to novel combined approaches. Here, I review some of the scanning tunneling microscopy (STM) and spectroscopy (STS) experiments on monolayer graphene samples. I will concentrate on graphene samples deposited on insulating substr…
Atomic scale characterization and manipulation with scanning probe microscopy rely upon the use of an atomically sharp probe. Here we present automated methods based on machine learning to automatically detect and recondition the quality of the probe of a scanning tunneling microscope. As a model system, we employ these techniques on the technologically relevant hydrogen-terminated silicon surface, training the network to recognize abnormalities in the appearance of surface dangling bonds. Of the machine learning methods tested, a convolutional neural network yielded the greatest accuracy, ach…
The miniaturization of semiconductor devices to the scales where small numbers of dopants can control device properties requires the development of new techniques capable of characterizing their dynamics. Investigating single dopants requires sub-nanometer spatial resolution which motivates the use of scanning tunneling microscopy (STM), however, conventional STM is limited to millisecond temporal resolution. Several methods have been developed to overcome this shortcoming. Among them is all-electronic time-resolved STM, which is used in this work to study dopant dynamics in silicon with nanos…
We consider conductance mapping of systems based on the two-dimensional electron gas with scanning gate microscopy using two and more tips of the atomic force microscope. The paper contains results of numerical simulations for a model tip potential with a proposal of a few procedures for extraction and manipulation the ballistic transport properties. In particular, we demonstrate that the multi-tip techniques can be used for readout of the Fermi wavelength, detection of potential defects, filtering specific transverse modes, tuning the system into resonant conditions under which a stable map o…
Electronic transport in semiconducting single-wall carbon nanotubes is studied by combined scanning gate microscopy and scanning impedance microscopy (SIM). Depending on the probe potential, SIM can be performed in both invasive and non-invasive mode. High-resolution imaging of the defects is achieved when the probe acts as a local gate and simultaneously an electrostatic probe of local potential. A class of weak defects becomes observable even if they are located in the vicinity of strong defects. The imaging mechanism of tip-gating scanning impedance microscopy is discussed.
Graphene nanopatterning on highly oriented pyrolytic graphite (HOPG) has previously been shown using both atomic force microscopy (AFM) and scanning tunneling microscopy (STM) based techniques, including folding of intrinsic step edges and electrochemical etching or cutting in graphene layers. We here report development of a new technique, combining electrochemical etching and folding using mechanical STM manipulation. Our technique shows unprecedented control of nanoscale folding of graphene in multiple folding steps and could be a route towards STM study of magic angle graphene with in-situ …
The Scanning Tunneling Microscope is a powerful tool for studying the electronic properties at the atomic level, however it's relatively small scanning range and the fact that it can only operate on conducting samples prevents its application to study heterogeneous samples consisting on conducting and insulating regions. Here we present a long-range scanning tunneling microscope capable of detecting conducting micro and nanostructures on insulating substrates using a technique based on the capacitance between the tip and the sample and performing STM studies.
We present a method to identify distinct tunneling modes in tunable superconducting tunnel junction composed of superconducting tip and sample in scanning tunneling microscope. Combining the measurement of the relative decay constant of tunneling current extracted from I-V-z spectroscopy with its statistical analysis over the atomic disorders in the sample surface, we identified the crossover of tunneling modes between single quasiparticle tunneling, multiple Andreev reflection, and Josephson tunneling with respect to the bias voltage. The method enables one to determine the particular tunneli…
Nanoscale lithography on SrRuO3 (SRO) thin film surfaces has been performed by scanning tunneling microscopy under ambient conditions. The depth of etched lines increases with increasing bias voltage but it does not change significantly by increasing the tunneling current. The dependence of line width on bias voltage from experimental data is in agreement with theoretical calculation based on field-induced evaporation. Moreover, a three-square nanostructure was successfully created, showing the capability of fabricating nanodevices in SRO thin films.
The integration of a scanning tunneling microscope chamber with a sample growth facility using non-custom, commercially available parts is described. The facility also features a newly-designed magnetic wobble stick to increase the reliability of sample transfer in a cost-effective manner.
We show scanning probe microscopy measurements of metallic nanocontacts between controlled electromigration cycles. The nanowires used for the thinning process are fabricated by shadow evaporation. The highest resolution obtained using scanning force microscopy is about 3 nm. During the first few electromigration cycles the overall slit structure of the nanocontact is formed. The slit first passes along grain boundaries and then at a later stage vertically splits grains in the course of consuming them. We find that first the whole wire is heated and later during the thinning process as the sli…
The scanning-tunneling-microscope-induced luminescence emerges recently as an incisive tool to measure the molecular properties down to the single-molecule level. The rapid experimental progress is far ahead of the theoretical effort to understand the observed phenomena. Such incompetence leads to a significant difficulty in quantitatively assigning the observed feature of the fluorescence spectrum to the structure and dynamics of a single molecule. This letter is devoted to reveal the microscopic origin of the molecular excitation via inelastic scattering of the tunneling electrons in scannin…
We describe software that simulates the hardware of a scanning force microscope. The essential feature of the software is its real-time response, which is critical for mimicking the behavior of real scanning probe hardware. The simulator runs on an open-source real time Linux kernel, and can be used to test scanning probe microscope control software as well as theoretical models of different types of scanning probe microscopes. We describe the implementation of a tuning-fork based atomic force microscope and a dc electrostatic force microscope, and present representative images obtained from t…
In scanning gate microscopy, where the tip of a scanning force microscope is used as a movable gate to study electronic transport in nanostructures, the shape and magnitude of the tip-induced potential are important for the resolution and interpretation of the measurements. Contaminations picked up during topography scans may significantly alter this potential. We present an in situ high-field treatment of the tip that improves the tip-induced potential. A quantum dot was used to measure the tip-induced potential.
We demonstrate high resolution scanning fluorescence resonance energy transfer 10 microscopy between a single nitrogen-vacancy center as donor and graphene as acceptor. 11 Images with few nanometer resolution of single and multilayer graphene structures were 12 attained. An energy transfer efficiency of 30% at distances of 10nm between a single 13 defect and graphene was measured. Further the energy transfer distance dependence of 14 the nitrogen-vacancy center to graphene was measured to show the predicted d-4 15 dependence. Our studies pave the way towards a diamond defect center based versa…
We demonstrate rotational excitation spectroscopy with the scanning tunneling microscope for physisorbed hydrogen and its isotopes hydrogen-deuterid and deuterium. The observed excitation energies are very close to the gas phase values and show the expected scaling with moment of inertia. Since these energies are characteristic for the molecular nuclear spin states we are able to identify the para and ortho species of hydrogen and deuterium, respectively. We thereby demonstrate nuclear spin sensitivity with unprecedented spatial resolution.
We report the fabrication and the characterization of carbon fibre tips for their use in combined scanning tunnelling and force microscopy based on piezoelectric quartz tuning fork force sensors. We find that the use of carbon fibre tips results in a minimum impact on the dynamics of quartz tuning fork force sensors yielding a high quality factor and consequently a high force gradient sensitivity. This high force sensitivity in combination with high electrical conductivity and oxidation resistance of carbon fibre tips make them very convenient for combined and simultaneous scanning tunnelling …
Nickel islands are grown on W(110) at elevated temperatures. Islands with a thickness of two layers are investigated with scanning tunneling microscopy. Spectroscopic measurements reveal that nanometer sized areas of the islands exhibit distinctly different apparent heights and dI/dV spectra. Spin polarized and paramagnetic band structure calculations indicate that the spectral features are due to fcc(111) and bcc(110) orientations of the Ni film, respectively.
Au-induced atomic wires on the Ge(001) surface were recently claimed to be an ideal 1D metal and their tunneling spectra were analyzed as the manifestation of a Tomonaga-Luttinger liquid (TLL) state. We reinvestigate this system for atomically well-ordered areas of the surface with high resolution scanning tunneling microscopy and spectroscopy (STS). The local density-of-states maps do not provide any evidence of a metallic 1D electron channel along the wires. Moreover, the atomically resolved tunneling spectra near the Fermi energy are dominated by local density-of-states features, deviating …
The qPlus sensor allows simultaneous measurements of scanning tunneling microscopy (STM) and atomic force microscopy (AFM). Its design for use in frequency modulation AFM (FM-AFM) involves separate electrodes, applied on an oscillating quartz cantilever, for the detection of an electronic tunneling current and the deflection signal. Cable resistance and capacities in the electronic setup can induce cross talk phenomena. We report a tunneling current-induced cross coupling observed in a combined STM/AFM setup which uses the qPlus sensor. This cross coupling can induce a positive or negative cha…
