We report a detailed study of tunneling spectra measured on 2H-Ta$_x$Nb$_{1-x}$Se$_2$ ($x=0\sim 0.1$) single crystals using a low-temperature scanning tunneling microscope. The prominent gap-like feature unintelligible for a long time was found to be accompanied by some "in-gap" fine structures. By investigating the second-derivative spectra and their temperature and magnetic field dependencies, we were able to prove that inelastic electron tunneling is the origin of these features and obtain the Eliashberg function of 2H-Ta$_x$Nb$_{1-x}$Se$_2$ at atomic scale, providing a potential way to study the local Eliashberg function and phonon spectra of the related transition-metal dichalcogenides.
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.
Amorphous silica deforms viscoplastically at elevated temperatures, as is common for brittle glasses. The key mechanism of viscoplastic deformation involves interatomic bond switching, which is known to be a thermally activated process. In this study, through systematic in-situ compression tests by scanning electron microscopy, the viscoplastic deformation of amorphous silica is observed without thermal activation. Furthermore, ductility does not increase monotonically with acceleration voltage and current density of the SEM e-beam but is maximized by a factor of three at a specific accelerati…
We have combined scanning tunneling microscopy with inelastic electron tunneling spectroscopy (IETS) and density functional theory (DFT) to study a tetracyanoethylene monolayer on Ag(100). Images show that the molecules arrange in locally ordered patterns with three non-equivalent, but undeterminable, adsorption sites. While scanning tunneling spectroscopy only shows subtle variations of the local electronic structure at the three different positions, we find that vibrational modes are very sensitive to the local atomic environment. IETS detects sizeable mode frequency shifts of the molecules …
We investigated the localized electronic properties of nanoporous gold films by using an ultra-high vacuum scanning tunneling microscope at low temperature (4.2 K). Second derivative scanning tunneling spectroscopy shows the plasmon peaks of the nanoporous gold films, which are excited by inelastic tunneling electrons. We propose that the nanorod model is appropriate for nanoporous gold studies at the nanometer-scale. These results are supported by a 3D electron tomography analysis and theoretical calculations of nanoporous gold with ellipsoid shape.
We report real space imaging measurements of inelastic Friedel oscillations. The inelastic electron tunneling spectroscopy, using scanning tunneling microscopy, around dimers of dichlorobenze adsorbates on Au(111) surface display clear spatial modulations that we attribute to inelastic scattering at the molecular sites caused by molecular vibrations. Due to local interactions between the adsorbate and the surface states, the molecular vibrations generate a redistribution of the charge density at energies in a narrow range around the inelastic mode. Our experimental findings are supported by th…
Local electronic structures of nanometer-sized patches of epitaxial graphene and its interface layer with SiC(0001) have been studied by atomically resolved scanning tunneling microscopy and spectroscopy. Localized states belonging to the interface layer of a graphene/SiC system show to have an essential influence on the electronic structure of graphene. Giant enhancement of inelastic tunneling, reaching 50% of the total tunneling current, has been observed at the localized states on a nanometer-sized graphene monolayer surrounded by defects.
The reconstruction on Ge(001) surface is locally and reversibly changed between c(4x2) and p(2x2) by controlling the bias voltage of a scanning tunneling microscope (STM) at 80K. It is c(4x2) with the sample bias voltage V_b =< -0.7V. This structure can be kept with V_b =< 0.6V. When V_b is higher than 0.8V during the scanning, the structure changes to p(2x2). This structure is then maintained with V_b >= - 0.6V. The observed local change of the reconstruction with hysteresis is ascribed to inelastic scattering during the electron tunneling in the electric field under the STM-tip.
Bilayer (BL) MoSe2 films grown by molecular-beam epitaxy (MBE) are studied by scanning tunneling microscopy and spectroscopy (STM/S). Similar to monolayer (ML) films, networks of inversion domain boundary (DB) defects are observed both in the top and bottom layers of BL MoSe2, and often they are seen spatially correlated such that one is on top of the other. There are also isolated ones in the bottom layer without companion in the top-layer and are detected by STM/S through quantum tunneling of the defect states through the barrier of the MoSe2 ML. Comparing the DB states in BL MoSe2 with that…
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…
The inelastic lifetimes of electrons in image-potential states at Cu(100) that are Stark-shifted by the electrostatic tip-sample interaction in the scanning tunneling microscope are calculated using the many-body GW approximation. The results demonstrate that in typical tunneling conditions the image state lifetimes are significantly reduced from their field-free values. The Stark-shift to higher energies increases the number of inelastic scattering channels that are available for decay, with field-induced changes in the image state wave function increasing the efficiency of the inelastic scat…
A scanning tunneling microscope (STM) can probe the inelastic spin excitations of single magnetic atoms in a surface via spin-flip assisted tunneling. A particular and intriguing case is the Mn dimer case. We show here that the existing theories for inelastic transport spectroscopy do not explain the observed spin transitions when both atoms are equally coupled to the STM tip and the substrate. The hyperfine coupling to the nuclear spins is shown to lead to a finite excitation amplitude, but the physical mechanism leading to the large inelastic signal observed is still unknown. We discuss some…
Sykes {\it et al.} [Proc. Natl. Acad. Sci. {\bf 102}, 17907 (2005)] have reported how electrons injected from a scanning tunneling microscope modify the diffusion rates of H buried beneath Pd(111). A key point in that experiment is the symmetry between positive and negative voltages for H extraction, which is difficult to explain in view of the large asymmetry in Pd between the electron and hole densities of states. Combining concepts from the theory of ballistic electron microscopy and electron-phonon scattering we show that H diffusion is driven by the $s$-band electrons only, which explains…
We have carried out a computational study of the inelastic electron tunneling spectrum (IETS) of the two vibrational modes of a single hydrogen atom on a Cu(100) surface in a scanning tunneling microscopy (STM) junction. This study addresses key issues about vibrational assignment and line shape of observed peaks in IETS within the framework of density functional theory calculations and the Lorente-Persson theory for STM-IETS. We argue that the observation of only a single, broad peak in the STM-IETS [L.J. Lauhon and W. Ho, Phys. Rev. Lett. 85, 4566 (2000)] is not caused by any symmetry restri…
Circular dichroism spectroscopy is an essential technique for understanding molecular structure and magnetic materials, but spatial resolution is limited by the wavelength of light, and sensitivity sufficient for single-molecule spectroscopy is challenging. We demonstrate that electrons can efficiently measure the interaction between circularly polarized light and chiral materials with deeply sub-wavelength resolution. By scanning a nanometer-sized focused electron beam across an optically-excited chiral nanostructure and measuring the electron energy spectrum at each probe position, we produc…
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 …
Karlsruhe Institute of Technology（卡尔斯鲁厄理工学院）；Jiangsu University（江苏大学）；Forschungszentrum Jülich GmbH（于利希研究中心有限公司）；Johannes Gutenberg-University Mainz（美因茨约翰内斯·古腾堡大学）
The honeycomb lattice of graphene is a unique two-dimensional (2D) system where the quantum mechanics of electrons is equivalent to that of relativistic Dirac fermions. Novel nanometer-scale behavior in this material, including electronic scattering, spin-based phenomena, and collective excitations, is predicted to be sensitive to charge carrier density. In order to probe local, carrier-density dependent properties in graphene we have performed atomically-resolved scanning tunneling spectroscopy measurements on mechanically cleaved graphene flake devices equipped with tunable back-gate electro…
A low-temperature scanning tunneling microscope is employed to build a junction comprising a Co atom bridging a copper-coated tip and a Cu(100) surface. An Abrikosov-Suhl-Kondo resonance is evidenced in the differential conductance and its width is shown to vary exponentially with the ballistic conductance regardless of the tip structure. Using a theoretical description based on the Anderson model, we show that the Kondo effect and the conductance are related through the atomic relaxations affecting the environment of the Co atom.
Strong multiple scattering of the probe in scanning transmission electron microscopy (STEM) means image simulations are usually required for quantitative interpretation and analysis of elemental maps produced by electron energy-loss spectroscopy (EELS). These simulations require a full quantum-mechanical treatment of multiple scattering of the electron beam, both before and after a core-level inelastic transition. Current algorithms scale quadratically and can take up to a week to calculate on desktop machines even for simple crystal unit cells and do not scale well to the nano-scale heterogen…
Non-equilibrium Effects in Vibrational Modes Pumped by Inelastic Tunneling
State Key Laboratory of Micro-nano Engineering Science, Tsung-Dao Lee Institute & School of Physics and Astronomy, Shanghai Jiao Tong University（上海交通大学物理与天文学院、李政道研究所微纳工程科学国家重点实验室）；SUPA, School of Physics and Astronomy, University of St Andrews（圣安德鲁斯大学物理与天文学院）；Department of Physics, King’s College London（伦敦国王学院物理系）；Max Planck Institute for Chemical Physics of Solids（马克斯·普朗克固体化学物理研究所）；Physikalisches Institut, Universität Bonn（波恩大学物理研究所）
Here we introduce a new approach to compute the finite temperature lattice dynamics from first-principles via the newly developed slave mode expansion. We study PbTe where inelastic neutron scattering (INS) reveals strong signatures of nonlinearity as evidenced by anomalous features which emerge in the phonon spectra at finite temperature. Using our slave mode expansion in the classical limit, we compute the vibrational spectra and show remarkable agreement with temperature dependent INS measurements. Furthermore, we resolve experimental controversy by showing that there are no appreciable loc…
Inelastic tunneling spectroscopy of Pb islands on Cu(111) obtained by scanning tunneling microscopy below 1K provides a direct access to the local Eliashberg function of the islands with high energy resolution. The Eliashberg function describes the electron-phonon interaction causing conventional superconductivity. The measured Eliashberg function strongly depends on the local thickness of the Pb nanostructures and shows a sharp maximum when quantum well states of the Pb islands come close to the Fermi energy. Ab initio calculations reveal that this is related to enhanced electron-phonon coupl…
We have performed low temperature scanning tunnelling spectroscopy (STS) measurements on graphene epitaxially grown on Ru(0001). An inelastic feature, related to the excitation of a vibrational breathing mode of the graphene lattice, was found at 360 meV. The change in the differential electrical conductance produced by this inelastic feature, which is associated with the electron-phonon interaction strength, varies spatially from one position to other of the graphene supercell. This inhomogeneity in the electronic properties of graphene on Ru(0001) results from local variations of the carbon-…
We present a study of charge density wave (CDW) ordering in CeTe$_3$ at room temperature using a scanning tunneling microscope and Raman spectroscopy. Two characteristic CDW ordering wavevectors obtained from the Fourier analysis are assessed to be $|{\bf \textbf{c}}^\ast-{\bf q}|=4.19\,{\rm nm}^{-1}$ and $|{\bf q}|=10.26\,{\rm nm}^{-1}$ where $|{\bf c}^\ast| = 2π/c$ is the reciprocal lattice vector. The scanning tunneling spectroscopy measurements, along with inelastic light (Raman) scattering measurements, show a CDW gap $Δ_{\rm max}$ of approximately 0.37 eV. In addition to the CDW modulati…
A new type of excitations by highly focused electron beams in scanning transmission electron microscopes is predicted for nanoparticles. The calculated electron energy loss spectra of metallic (silver) and insulating (SiO(sub2)) nanoplatelets reveal dramatic enhancement of radiative electromagnetic modes within the light cone, allowed by the breakdown of momentum conservation in the inelastic scattering event. These modes can be accessed with e-beams in the vacuum far-field zone, similarly to the recently developed far-field optics based on surface plasmon resonances.
Scanning tunneling spectroscopy of p(2x2) Cs and Na ordered overlayers on Cu(111) reveals similar line widths of quasi two-dimensional quantum well states despite largely different binding energies. Detailed calculations show that 50% of the line widths are due to electron-phonon scattering while inelastic electron-electron scattering is negligible. A frequently ignored mechanism for ordered structures, i.e., enhanced elastic scattering due to Brillouin zone back folding, contributes the remaining width.
We have performed single-atom magnetization curve (SAMC) measurements and inelastic scanning tunneling spectroscopy (ISTS) on individual Fe atoms on a Cu(111) surface. The SAMCs show a broad distribution of magnetic moments with $\unit[3.5]{μ_{\rm B}}$ being the mean value. ISTS reveals a magnetization excitation with a lifetime of $\unit[200]{fsec}$ which decreases by a factor of two upon application of a magnetic field of $\unit[12]{T}$. The experimental observations are quantitatively explained by the decay of the magnetization excitation into Stoner modes of the itinerant electron system a…
