High-Resolution Scanning Tunneling Microscope and its Adaptation for Local Thermopower Measurements in 2D Materials
Jose D. Bermúdez-Perez, Edwin Herrera-Vasco, Javier Casas-Salgado, Hector A. Castelblanco, Karen Vega-Bustos, Gabriel Cardenas-Chirivi, Oscar L. Herrera-Sandova… 展开作者
Jose D. Bermúdez-Perez, Edwin Herrera-Vasco, Javier Casas-Salgado, Hector A. Castelblanco, Karen Vega-Bustos, Gabriel Cardenas-Chirivi, Oscar L. Herrera-Sandoval, Hermann Suderow, Paula Giraldo-Gallo, Jose A. Galvis
We present the design, fabrication and discuss the performance of a new combined high-resolution Scanning Tunneling and thermopower Microscope (STM/SThEM). We also describe the development of the electronic control, the user interface, the vacuum system, and arrangements to reduce acoustical noise and vibrations. We demonstrate the microscope performance with atomic-resolution topographic images of Highly oriented pyrolytic graphite (HOPG) and local thermopower measurements in the semimetal Bi2Te3 sample. Our system offers a tool to investigate the relationship between electronic structure and thermoelectric properties at the nanoscale.
The design, fabrication, and predicted performance of a new type of magnetic scanning probe microscope based on the newly discovered phenomenon of extraordinary magnetoresistance (EMR) is described. It is shown that the new probe should advance the state of the art of both sensitivity and spatial resolution by an order of magnitude or more.
A novel phenomenon of anomalous contrast in scanning electron microscope when the instrument is used to observe an insulator specimen with a wolfram probe, we called double imaging, is reported in this article. We give a detail analysis of this phenomenon in its occurrence, and discuss the influence of the added probe to internal electric field which lead to the occurrence of double imaging.
Iron diantimonide is a material with the highest known thermoelectric power. By combining scanning transmission electron microscope study with electronic transport neutron, X-ray scattering and first principle calculation we identify atomic defects that control colossal thermopower magnitude and nanoprecipitate clusters with Sb vacancy ordering which induce additional phonon scattering and substantially reduce thermal conductivity. Defects are found to cause rather weak but important monoclinic distortion of the unit cell Pnnm to Pm. The absence of Sb along [010] for high defect concentration …
Ultraviolet and visible radiation is observed from the contacts of a scanning tunneling microscope with Si(100) and (111) wafers. This luminescence relies on the presence of hot electrons in silicon, which are supplied, at positive bias on n- and p-type samples, through the injection from the tip, or, at negative bias on p-samples, by Zener tunneling. Measured spectra reveal a contribution of direct optical transitions in Si bulk. The necessary holes well below the valence band edge are injected from the tip or generated by Auger processes.
We report a novel atom extraction mechanism from the native substrate by means of a scanning tunneling microscope tip-crash on a Ag(111) surface at 5 K. Individual atoms are scattered on the surface when a silver coated tip is dipped into the substrate at low tunneling biases. Quantitative analyses reveal that the mechanical energy supplied by the tip-crash dominates the atom extraction process. Application of this procedure is demonstrated by constructing quantum structures using the extracted atoms on an atom-by-atom basis.
Semiconductor dopant profiling using secondary electron imaging in a scanning electron microscope (SEM) has been developed in recent years. In this paper, we show that the mechanism behind it also allows mapping of the electric potential of undoped regions. By using an unbiased GaAs/AlGaAs heterostructure, this article demonstrates the direct observation of the electrostatic potential variation inside a 90nm wide undoped GaAs channel surrounded by ionized dopants. The secondary electron emission intensities are compared with two-dimensional numerical solutions of the electric potential.
We describe near-field imaging of sample sheet resistance via frequency shifts in a resonant coaxial scanning microwave microscope. The frequency shifts are related to local sample properties, such as surface resistance and dielectric constant. We use a feedback circuit to track a given resonant frequency, allowing measurements with a sensitivity to frequency shifts as small as one parts in 50000 for a 30 ms sampling time. The frequency shifts can be converted to sheet resistance based on a simple model of the system.
We describe the use of a near-field scanning microwave microscope to image the permittivity and tunability of bulk and thin film dielectric samples on a length scale of about 1 micron. The microscope is sensitive to the linear permittivity, as well as to nonlinear dielectric terms, which can be measured as a function of an applied electric field. We introduce a versatile finite element model for the system, which allows quantitative results to be obtained. We demonstrate use of the microscope at 7.2 GHz with a 370 nm thick barium strontium titanate thin film on a lanthanum aluminate substrate.…
Electron-electron interactions and excitons in carbon nanotubes are locally measured by combining Scanning tunneling spectroscopy and optical absorption in bundles of nanotubes. The largest gap deduced from measurements at the top of the bundle is found to be related to the intrinsic quasi-particle gap. From the difference with optical transitions, we deduced exciton binding energies of 0.4 eV for the gap and 0.7 eV for the second Van Hove singularity. This provides the first experimental evidence of substrate-induced gap renormalization on SWNTs.
We discuss the local cutting of single-walled carbon nanotubes by a voltage pulse to the tip of a scanning tunneling microscope. The tip voltage ($\mid V \mid \ge $~3.8 eV) is the key physical quantity in the cutting process. After reviewing several possible physical mechanisms we conclude that the cutting process relies on the weakening of the carbon-carbon bonds through a combination of localized particle-hole excitations induced by inelastically tunneling electrons and elastic deformation due to the electric field between tip and sample. The carbon network releases part of the induced mecha…
We demonstrate that the sub-atomically focused beam of a scanning transmission electron microscope (STEM) can be used to controllably manipulate individual dopant atoms in a 2D graphene lattice. We demonstrate the manipulation of adsorbed source materials and the graphene lattice with the electron beam such that individual vacancy defects can be controllably passivated by Si substitutional atoms. We further demonstrate that these Si defects may be directed through the lattice via e-beam control or modified (as yet, uncontrollably) to form new defects which can incorporate new atoms into the gr…
We present a method for extracting high-spatial resolution dielectric constant data at microwave frequencies. A scanning near field microwave microscope probes a sample and acquires data in the form of the frequency and quality factor shifts of a resonant cavity coupled to the sample. The approach reported here is to calculate the electromagnetic fields by the finite element method in both static and time-dependent modes. Cavity perturbation theory connects the measured frequency shifts to changes in the computed energy stored in the electromagnetic field. In this way, the complex permittivity…
Double ring formation on Co2MnSi (CMS) films is observed at electrical breakdown voltage during local anodic oxidation (LAO) using atomic force microscope (AFM). Corona effect and segregation of cobalt in the vicinity of the rings is studied using magnetic force microscopy and energy dispersive spectroscopy. Double ring forma-tion is attributed to the interaction of ablated material with the induced magnetic field during LAO. Steepness of forward bias transport characteristics from the unperturbed region of the CMS film suggest a non equilibrium spin contribution. Such mesoscopic textures in m…
A first principles theory of inelastic tunneling between a model probe tip and an atom adsorbed on a surface is presented, extending the elastic tunneling theory of Tersoff and Hamann. The inelastic current is proportional to the change in the local density of states at the center of the tip due to the addition of the adsorbate. We use the theory to investigate the vibrational heating of an adsorbate below an STM tip. We calculate the desorption rate of H from Si(100)-H(2$\times$1) as function of the sample bias and tunnel current, and find excellent agreement with recent experimental data.
We present the design and experimental results of a near-field scanning microwave microscope (NSMM) working at a frequency of 1GHz. Our microscope is unique in that the sensing probe is separated from the excitation electrode to significantly suppress the common-mode signal. Coplanar waveguides were patterned onto a silicon nitride cantilever interchangeable with atomic force microscope (AFM) tips, which are robust for high speed scanning. In the contact mode that we are currently using, the numerical analysis shows that contrast comes from both the variation in local dielectric properties and…
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.
Scanning tunneling microscope (STM) is a powerful tool for studying the structural and electronic properties of materials at the atomic scale. The combination of low temperature and high magnetic field for STM and related spectroscopy techniques allows us to investigate the novel physical properties of materials at these extreme conditions with high energy resolution. Here, we present the construction and the performance of an ultrahigh vacuum 3He fridge-based STM system with a 7 Tesla superconducting magnet. It features a double deck sample stage on the STM head so we can clean the tip by fie…
We have developed scanning near-field microwave microscopes which can image electrodynamic properties of superconducting materials on length scales down to about 2 $μ$m. The microscopes are capable of quantitative imaging of sheet resistance of thin films, and surface topography. We demonstrate the utility of the microscopes through images of the sheet resistance of a YBa2Cu3O7-d thin film wafer, images of bulk Nb surfaces, and spatially resolved measurements of Tc of a YBa2Cu3O7-d thin film. We also discuss some of the limitations of the microscope and conclude with a summary of its present c…
We report a new technique of scanning capacitance microscopy at microwave frequencies. A near field scanning microwave microscope probe is kept at a constant height of about 1nm above the samplewith the help of Scanning Tunneling Microscope (STM) feedback. The microwaves are incident onto the sample through a coaxial resonator that is terminated at one end with a sharp tip (the same tip is used to conduct STM), and capacitively coupled to a feedback circuit and microwave source at the other end. The feedback circuit keeps the source locked onto the resonance frequency of the resonator and outp…
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.
We report our detailed investigation of high-resolution imaging using secondary electrons (SE) with a subnanometer probe in an aberration-corrected transmission electron microscope, Hitachi HD2700C. This instrument also allows us to acquire the corresponding annular-dark-field (ADF) images simultaneously and separately. We demonstrate that atomic SE imaging is achievable for a wide range of elements, from uranium to carbon. Using the ADF images as a reference, we study the SE image intensity and contrast as a function of applied bias, atomic number, crystal tilt and thickness to shed light on …
We describe a technique for extracting topographic information using a scanning near-field microwave microscope. By monitoring the shift of the system's resonant frequency, we obtain quantitative topographic images of uniformly conducting metal surfaces. At a frequency of 9.572 GHz, our technique allows for a height discrimination of about 55 nm at a separation of 30 microns. We present topographic images of uneven, conducting samples and compare the height response and sensitivity of the system with theoretical expectations.
Measurements of light emission from a scanning tunneling microscope probing a Na overlayer on the (111) surface of Cu are reported along with results of a model calculation that essentially agree with the experimental ones. The observed light emission spectra show two characteristic features depending on the bias voltage. When the bias voltage is smaller than the energy of the second quantum well state formed outside the Na overlayer the light emission is due to a plasmon-mediated process, while for larger biases light emission is mainly caused by quantum well transitions between the two level…
We present a Scanning Hall Probe Microscope operating in ambient conditions. One of the unique features of this microscope is the use of the same stepper motors for both sample positioning as well as scanning, which makes it possible to have a large scan range (few mm) in x and y directions, with a scan resolution of 0.1 $μ$m. Protocols have been implemented to enable scanning at different heights from the sample surface. The z range is 35 mm. Microstructured Hall probes of size 1-5 $μ$m have been developed. A minimum probe-sample distance \textless{} 2 $μ$m has been obtained by the combinatio…
We present the main features of a home-built scanning tunneling microscope that has been attached to the mixing chamber of a dilution refrigerator. It allows scanning tunneling microscopy and spectroscopy measurements down to the base temperature of the cryostat, T approx. 30mK, and in applied magnetic fields up to 13T. The topography of both highly-ordered pyrolytic graphite (HOPG) and the dichalcogenide superconductor NbSe2 have been imaged with atomic resolution down to T approx. 50mK as determined from a resistance thermometer adjacent to the sample. As a test for a successful operation in…
We investigate atomistic details of a single atom extraction process realized by using scanning tunneling microscope (STM) tip-cluster interaction on a Ag(111) surface at 6 K. Single atoms are extracted from a silver cluster one atom at a time using small tunneling biases less than 35 mV and a threshold tunneling resistance of 47 kOhm. A combination of total energy calculations and molecular dynamics simulations shows a lowering of the atom extraction barrier upon approaching the tip to the cluster. Thus, a mere tuning of the proximity between the tip and the cluster governs the extraction pro…
Time resolution is one of the most severe limitations of scanning probe microscopies (SPMs), since the typical image acquisition times are in the order of several seconds or even few minutes. As a consequence, the characterization of dynamical processes occurring at surfaces (e.g. surface diffusion, film growth, self-assembly and chemical reactions) cannot be thoroughly addressed by conventional SPMs. To overcome this limitation, several years ago we developed a first prototype of the FAST module, an add-on instrument capable of driving a commercial scanning tunneling microscope (STM) at and b…
We report the destabilization of the charge ordered insulating (COI) state in a localized region of Pr_0.63Ca_0.37MnO_3 single crystal by current injection using a scanning tunneling microscope tip. This leads to controlled phase separation and formation of localized metallic nanoislands in the COI matrix which have been detected by local tunneling conductance mapping. The metallic regions thus created persist even after reducing the injected current to lower values. The original conductance state can be restored by injecting a current of similar magnitude but of opposite polarity. We thus ach…
Digital image correlation of laser-ablated platinum nanoparticles on the surface of a polycrystalline metal (nickel-based superalloy Rene 88DT) was used to obtain the local strain behavior from an in situ scanning electron microscope tensile experiment at room temperature. By fusing this information with crystallographic orientations from EBSD, a subsequent analysis shows that the average maximum shear strain tends to increase with increasing Schmid factor. Additionally, the range of the extreme values for the maximum shear strain also increases closer to the grain boundary, signifying that gr…
Scanning tunneling spectroscopy (STS) allows to image single molecules decoupled from the supporting substrate. The obtained images are routinely interpreted as the square moduli of molecular orbitals, dressed by the mean-field electron-electron interaction. Here we demonstrate that the effect of electron correlation beyond mean field qualitatively alters the uncorrelated STS images. Our evidence is based on the ab-initio many-body calculation of STS images of planar molecules with metal centers. We find that many-body correlations alter significantly the image spectral weight close to the met…
Silicon can be isotopically enriched, allowing for the fabrication of highly coherent semiconductor spin qubits. However, the conduction band of bulk Si exhibits a six-fold valley degeneracy, which may adversely impact the performance of silicon quantum devices. To date, the spatial characterization of valley states in Si remains limited. Moreover, techniques for probing valley states in functional electronic devices are needed. We describe here a cryogen-free scanning gate microscope for the characterization of Si/Si$_{0.7}$Ge$_{0.3}$ quantum devices at mK temperatures. The microscope is base…
We fabricate and characterize carbon-fiber tips for their use in combined scanning tunneling and force microscopy based on piezoelectric quartz tuning fork force sensors. An electrochemical fabrication procedure to etch the tips is used to yield reproducible sub-100-nm apex. We also study electron transport through single-molecule junctions formed by a single octanethiol molecule bonded by the thiol anchoring group to a gold electrode and linked to a carbon tip by the methyl group. We observe the presence of conductance plateaus during the stretching of the molecular bridge, which is the signa…
We describe the design and performance of a scanning tunneling microscope (STM) which operates at a base temperature of 30 mK in a vector magnetic field. The cryogenics is based on an ultra-high vacuum (UHV) top-loading wet dilution refrigerator that contains a vector magnet allowing for fields up to 9 T perpendicular and 4 T parallel to the sample. The STM is placed in a multi-chamber UHV system, which allows in-situ preparation and exchange of samples and tips. The entire system rests on a 150-ton concrete block suspended by pneumatic isolators, which is housed in an acoustically isolated an…
We describe quantitative imaging of the sheet resistance of metallic thin films by monitoring frequency shift and quality factor in a resonant scanning near-field microwave microscope. This technique allows fast acquisition of images at approximately 10 ms per pixel over a frequency range from 0.1 to 50 GHz. In its current configuration, the system can resolve changes in sheet resistance as small as 0.6 Ohms/sq for 100 Ohms/sq films. We demonstrate its use at 7.5 GHz by generating a quantitative sheet resistance image of a YBa2Cu3O7 (YBCO) thin film on a 5 cm-diameter sapphire wafer.
We constructed a dilution-refrigerator (DR) based ultra-low temperature scanning tunneling microscope (ULT-STM) which works at temperatures down to 30 mK, in magnetic fields up to 6 T and in ultrahigh vacuum (UHV). Besides these extreme operation conditions, this STM has several unique features not available in other DR based ULT-STMs. One can load STM tips as well as samples with clean surfaces prepared in a UHV environment to an STM head keeping low temperature and UHV conditions. After then, the system can be cooled back to near the base temperature within 3 hours. Due to these capabilities…
We summarize our new scanning magnetic 3-D imaging system. This scanning system uses optically detected magnetic resonance in a single nitrogen vacancy center in a diamond nanocrystal. The theoretical analysis and the first experimental demonstrations have proved that this method has single spin sensitivity and a sub-nanoscale spatial resolution at room temperature.
We present a detailed modeling and characterization of our scalable microwave nanoprobe, which is a micro-fabricated cantilever-based scanning microwave probe with separated excitation and sensing electrodes. Using finite-element analysis, the tip-sample interaction is modeled as small impedance changes between the tip electrode and the ground at our working frequencies near 1GHz. The equivalent lumped elements of the cantilever can be determined by transmission line simulation of the matching network, which routes the cantilever signals to 50 Ohm feed lines. In the microwave electronics, the …
Pacific Northwest National Laboratory（太平洋西北国家实验室）；Washington State University – Tri-Cities（华盛顿州立大学三城分校）
Artificial intelligence (AI) promises to reshape scientific inquiry and enable breakthrough discoveries in areas such as energy storage, quantum computing, and biomedicine. Scanning transmission electron microscopy (STEM), a cornerstone of the study of chemical and materials systems, stands to benefit greatly from AI-driven automation. However, present barriers to low-level instrument control, as well as generalizable and interpretable feature detection, make truly automated microscopy impractical. Here, we discuss the design of a closed-loop instrument control platform guided by emerging spar…
Scanning tunneling microscopy and spectroscopy have been used to investigate the femtosecond dynamics of Dirac fermions in the topological insulator Bi$_2$Se$_3$ ultrathin films. At two-dimensional limit, bulk electrons becomes quantized and the quantization can be controlled by film thickness at single quintuple layer level. By studying the spatial decay of standing waves (quasiparticle interference patterns) off steps, we measure directly the energy and film thickness dependence of phase relaxation length $l_ϕ$ and inelastic scattering lifetime $τ$ of topological surface-state electrons. We …
Scanning tunneling microscopy (STM) images are obtained for the first time on few layer and twisted multilayer epitaxial graphene states synthesized on n+ 6H-SiC a-plane non-polar surface. The twisted graphene is determined to have a rotation angle of 5.4° between the top two layers, by comparing moiré patterns from stick and ball models of bilayer graphene to experimentally obtained images. Furthermore, the experimental moiré pattern shows dynamic behavior, continuously shuffling between two stable surface arrangements one bond length apart. The moiré pattern shifts by more than 1 nm, making …
ANTARES beamline (BL), a new soft X-ray scanning photoemission microscope located at the SOLEIL synchrotron storage ring has been recently designed, built and commissioned. The implemented interferometer control allows the accurate measurement of the transverse position of the Fresnel zone plate (FZP) relative to the sample. An effective sample position feedback has been achieved during experiments in static mode, with a fixed FZP position required to perform nano Angle-Resolved Photoelectron Spectroscopy (Nano-ARPES) measurements. Likewise, long-term stability has been attained for the FZP po…
We report the construction and performance of a low temperature, high field scanning tunneling microscope (STM) operating down to 350mK and in magnetic fields up to 9T, with thin film deposition and in-situ cleaving capabilities. The main focus lies on the simple design of STM head allowing top loading of the sample and innovative sample holder design that allows us to get spectroscopic data on superconducting thin films grown in-situ on insulating substrates. Other design details on sample transport, chamber and vibration isolation scheme are also described. We demonstrate the capability of o…
Electron paramagnetic resonance (EPR) spectroscopy is widely employed to characterize paramagnetic complexes. Recently, EPR combined with scanning tunneling microscopy (STM) achieved single-spin sensitivity with sub-angstrom spatial resolution. The excitation mechanism of EPR in STM, however, is broadly debated, raising concerns about widespread application of this technique. Here, we present an extensive experimental study and modelling of EPR-STM of Fe and hydrogenated Ti atoms on an MgO surface. Our results support a piezoelectric coupling mechanism, in which the EPR species oscillate adiab…
We have developed a noncontact method for measurement of the interline capacitance in Cu/low-k interconnect. It is based on a miniature test vehicle with net capacitance of a few femto-Farads formed by two 20-μm-long parallel wires (lines) with widths and spacings the same as those of the interconnect wires of interest. Each line is connected to a small test pad. The vehicle impedance is measured at 4 GHz by a near-field microwave probe with 10 μm probe size via capacitive coupling of the probe to the vehicle's test pads. Full 3D finite element modeling at 4 GHz confirms that the microwave rad…
Integration of Scanning Probe Microscope with High-Performance Computing: fixed-policy and reward-driven workflows implementation
University of Tennessee（田纳西大学）；Oxford Instruments Asylum Research（牛津仪器庇护研究公司）；Pacific Northwest National Laboratory（太平洋西北国家实验室）；National Cheng Kung University（国立成功大学）；the Pennsylvania State University（宾夕法尼亚州立大学）
