In a semiconductor-based double quantum well (QW) coupled to a degree of freedom with an internal dynamics, we demonstrate that the electronic motion is controllable within femtoseconds by applying appropriately shaped electromagnetic pulses. In particular, we consider a pulse-driven AlxGa1-xAs based symmetric double QW coupled to uniformly distributed or localized vibrational modes and present analytical results for the lowest two levels. These predictions are assessed and generalized by full-fledged numerical simulations showing that localization and time-stabilization of the driven electron dynamics is indeed possible under the conditions identified here, even with a simultaneous excitations of vibrational modes.
We investigate the origin of purported "spin accumulation" signals observed in local "three-terminal" (3T) measurements of ferromagnet/insulator/n-Si tunnel junctions using inelastic electron tunneling spectroscopy (IETS). Voltage bias and magnetic field dependences of the IET spectra were found to account for the dominant contribution to 3T magnetoresistance signals, thus indicating that it arises from inelastic tunneling through impurities and defects at junction interfaces and within the barrier, rather than from spin accumulation due to pure elastic tunneling into bulk Si as has been previ…
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.
Efficient operation of electronic nanodevices at ultrafast speeds requires understanding and control of the currents generated by femtosecond bursts of light. Ultrafast laser-induced currents in metallic nanojunctions can originate from photo-assisted hot electron tunneling or lightwave-induced tunneling. Both processes can drive localized photocurrents inside a scanning tunneling microscope (STM) on femto- to attosecond time scales, enabling ultrafast STM with atomic spatial resolution. Femtosecond laser excitation of a metallic nanojunction, however, also leads to the formation of a transien…
The paper addresses inelastic spin-flip tunneling accompanied by surface spin excitations (magnons) in ferromagnetic junctions. The inelastic tunneling current is proportional to the magnon density of states which is energy-independent for the surface waves and, for this reason, cannot account for the bias-voltage dependence of the observed inelastic tunneling spectra. This paper shows that the bias-voltage dependence of the tunneling spectra can arise from the tunneling matrix elements of the electron-magnon interaction. These matrix elements are derived from the Coulomb exchange interaction …
Gold nanoparticles emit broad-band upconverted luminescence upon irradiation with pulsed infrared laser radiation. Although the phenomenon is widely observed, considerable disagreement still exists concerning the underlying physics - most notably over the applicability of concepts such as multiphoton absorption, inelastic scattering, and interband and intraband electronic transitions. Here, we study single particles and small clusters of particles by employing a spectrally resolved power-law analysis of the irradiation-dependent emission as a sensitive probe of these physical models. Two regim…
A generalized Green's function theory is developed to simulate the inelastic electron tunneling spectroscopy (IETS) of molecular junctions. It has been applied to a realistic molecular junction with an octanedithiolate embedded between two gold contacts in combination with the hybrid density functional theory calculations. The calculated spectra are in excellent agreement with recent experimental results. Strong temperature dependence of the experimental IETS spectra is also reproduced. It is shown that the IETS is extremely sensitive to the intra-molecular conformation and to the molecule-met…
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…
This is a comment on recent paper by T.M. Stace and S.D. Barrett, PRL 92, 136802 (2004). We show that the main result of the paper, absence of the spectral peak for continuous weak measurement of coherent oscillations in a qubit, is incorrect.
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…
Coupling a quantum system to a bosonic environment always give rise to inelastic processes, which reduce the coherency of the system. We measure energy dependent rates for inelastic tunneling processes in a fully controllable two-level system of a double quantum dot. The emission and absorption rates are well repro-duced by Einstein's coefficients, which relate to the spontaneous emission rate. The inelastic tunneling rate can be comparable to the elastic tunneling rate if the boson occupation number becomes large. In the specific semiconductor double dot, the energy dependence of the inelasti…
Inelastic electron tunneling provides a low-energy pathway for the excitation of surface plasmons and light emission. We theoretically investigate tunnel junctions based on metals and graphene. We show that graphene is potentially a highly efficient material for tunneling excitation of plasmons because of its narrow plasmon linewidths, strong emission, and large tunability in the midinfrared wavelength regime. Compared to gold and silver, the enhancement can be up to 10 times for similar wavelengths and up to 5 orders at their respective plasmon operating wavelengths. Tunneling excitation of g…
We study inelastic electron tunneling through a molecular junction using the non-equilibrium Green function (NEGF) formalism. The effect of the mutual influence between the phonon and the electron subsystems on the electron tunneling process is considered within a general self-consistent scheme. Results of this calculation are compared to those obtained from the simpler Born approximation and the simplest perturbation theory approaches, and some shortcomings of the latter are pointed out. The self-consistent calculation allows also for evaluating other related quantities such as the power loss…
The recent experimental conductance measurements taken on magnetic impurities on metallic surfaces, using scanning tunneling microscopy technique and suggesting occurrence of inelastic scattering processes, are theoretically addressed. We argue that the observed conductance signatures are caused by transitions between the spin states which have opened due to e.g. exchange coupling between the local spins and the tunneling electrons, and are directly interpretable in terms of inelastic transitions energies. Feasible measurements using spin-polarized scanning tunneling microscopy that would enab…
A theoretical analysis of inelastic electron tunneling spectroscopy (IETS) experiments conducted on molecular junctions are presented, where the second derivative of the current with respect to voltage is usually plotted as a function of applied bias. Within the nonperturbative computational scheme, adequate for arbitrary parameters of the model, we consider the virtual conduction process in the off-resonance region. Here we study the influence of few crucial factors on the IETS spectra: the strength of the vibronic coupling, the phonon energy, and the device working temperature. It was also s…
We study pentanedithiol molecular junctions formed by means of the break-junction technique with a scanning tunneling microscope at low temperatures. Using inelastic electron tunneling spectroscopy and first-principles calculations, the response of the junction to elastic deformation is examined. We show that this procedure makes a detailed characterization of the molecular junction possible. In particular, our results indicate that tunneling takes place through just a single molecule.
We present a first principles method for calculating the inelastic electron tunneling spectroscopy (IETS) on gated graphene. We reproduce experiments on pristine graphene and point out the importance of including several phonon modes to correctly estimate the local doping from IETS. We demonstrate how the IETS of typical imperfections in graphene can yield characteristic fingerprints revealing e.g. adsorbate species or local buckling. Our results show how care is needed when interpreting STM images of defects due to suppression of the elastic tunneling on graphene.
We address quantum invisibility in the context of electronics in nanoscale quantum structures. We make use of the freedom of design that quantum corrals provide and show that quantum mechanical objects can be hidden inside the corral, with respect to inelastic electron scattering spectroscopy in combination with scanning tunneling microscopy, and we propose a design strategy. A simple illustration of the invisibility is given in terms of an elliptic quantum corral containing a molecule, with a local vibrational mode, at one of the foci. Our work has implications to quantum information technolo…
We theoretically investigate the effect of transverse magnetic anisotropy on spin-flip assisted tunneling through atomic spin chains. Using a phenomenological approach and first-order perturbation theory, we analytically calculate the inelastic tunneling current, differential conductance and atomic spin transition rates. We predict the appearance of additional steps in the differential conductance and a pronounced increase in the spin-flip transition rate which at low voltages scale quadratically with the ratio of the transverse anisotropy energy and the sum of the longitudinal anisotropy ener…
Recent work shows that inelastic electron scanning tunneling microscope (STM) probes the elementary spin excitations of a single and a few magnetic atoms in a thin insulating layer. Here I show that this new type of spectroscopy is described using a phenomenological spin-assisted tunneling Hamiltonian. Within this formalism, the inelastic $dI/dV$ lineshape is related to the spin spectral weight of the probed magnetic atom. This accounts for the spin selection rules observed experimentally. The theory agrees well with existing STM experiments for single Fe and Mn atoms as well as linear chains …
Our objective is to study resonant tunneling of an electron in the presence of inelastic scattering by optical phonons. Using a recently developed technique, based on exact mapping of a many-body problem onto a one-body problem, we compute transmission through a single site at finite temperatures. We also compute current through a single site at finite temperatures and an arbitrary strength of the potential drop over the tunneling region. Transmission vs. incident electron energy at finite temperatures displays additional peaks due to phonon absorption processes. Current at a voltage bias smal…
Probing topological Floquet states in graphene with ultrafast terahertz scanning tunneling microscopy
University of Bremen（不来梅大学）；Max Planck Institute for the Structure and Dynamics of Matter（马普物质结构与动力学研究所）；Paul Scherrer Institute（保罗谢尔研究所）；University of Fribourg（弗里堡大学）；The Flatiron Institute（_flatiron研究所）；Fritz Haber Institute of the Max Planck Society（马克斯·普朗克学会弗里茨·哈伯研究所）
The theory of inelastic electron tunneling spectroscopy (IETS) and motions of single adsorbed atoms and molecules on metal surfaces induced by vibrational excitation with a scanning tunneling microscope (STM) is reviewed. The theory of STM-IETS is described using the adsorbate-induced resonance model. Elementary processes of how an adsorbate overcomes the potential barrier along the reaction coordinate (RC) by inelastic tunneling current are described with a focus on direct excitation of the RC mode by coherent and incoherent vibrational ladder climbing and an indirect one through anharmonic c…
The role of the tip in inelastic electron tunneling spectroscopy (IETS) performed with scanning tunneling microscopes (STM) is theoretically addressed via first-principles simulations of vibrational spectra of single carbon monoxide (CO) molecules adsorbed on Cu(111). We show how chemically functionalized STM tips modify the IETS intensity corresponding to adsorbate modes on the sample side. The underlying propensity rules are explained using symmetry considerations for both the vibrational modes and the molecular orbitals of the tip and sample. This suggests that single-molecule IETS can be o…
Using the closed-time path integral approach, we nonperturbatively study inelastic tunneling of electrons via magnetic impurities in the barrier accompanied by phonon emission in a magnetic tunnel junction. The spectrum density of phonon emission is found to show a power-law infrared singularity $\simω^{-(1-g)}$ with $g$ the dimensionless electron-phonon coupling. As a consequence, the tunneling conductance $G(V)$ increases with bias voltage $| V|$ as $G(V)-G(0)\sim| V|^{2g}$, exhibiting a discontinuity in slope at V=0 for $g\le 0.5$. This theory can reproduce both cusp-like and non-cusp-like …
For a non-superconducting system, the electronic tunneling current through an insulating barrier is calculated, including interaction effects. The exact Hamiltonian of the full system is projected onto the subspaces of the "left" and "right" leads. In the weak tunneling limit the well-known tunneling Hamiltonian is recovered, along with an additional term. This additional term originates from the projection of the electron-electron interaction onto each subsystem and corresponds to correlated tunneling. It is shown that the tunneling current is determined by---in addition to the single-particl…
We reply to a comment by Averin and Korotkov http://uk.arxiv.org/abs/cond-mat/0404549 on Stace and Barrett, PRL 92, 136802 (2004) http://link.aps.org/abstract/PRL/v92/e136802, showing that their specific criticisms are unfounded, and clarifying some of our results.
Several aspects of intermolecular effects in molecular conduction have been studied in recent years. These experimental and theoretical studies, made on several setups of molecular conduction junctions, have focused on the current-voltage characteristic that is usually dominated by the elastic transmission properties of such junctions. In this paper we address cooperative intermolecular effects in the inelastic tunneling signal calculated for simple generic models of such systems. We find that peaks heights in the inelasticspectrum may be affected by such cooperative effects even when direct i…
We demonstrate that a suspended nanowire forming a weak link between two superconductors can be cooled to its motional ground state by a supercurrent flow. The predicted cooling mechanism has its origins in magnetic field induced inelastic tunneling of the macroscopic superconducting phase associated with the junction. Furthermore, we show the voltage-drop over the junction is proportional to the average population of the vibrational modes in the stationary regime, a phenomena which can be used to probe the level of cooling.
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…
In single-molecule transistors, we observe inelastic cotunneling features that correspond energetically to vibrational excitations of the molecule, as determined by Raman and infrared spectroscopy. This is a form of inelastic electron tunneling spectroscopy of single molecules, with the transistor geometry allowing in-situ tuning of the electronic states via a gate electrode. The vibrational features shift and change shape as the electronic levels are tuned near resonance, indicating significant modification of the vibrational states. When the molecule contains an unpaired electron, we also ob…
Resonant electron transport through a mesoscopic region (quantum dot or single molecule) with electron-phonon interaction is considered at finite voltage. In this case the standard Landauer-Büttiker approach cannot be applied. Using the nonequilibrium Green function method we show that due to a nonequilibrium distribution function of electrons in the mesoscopic region, the inelastic scattering rate and spectral function of the dot become functions of the voltage and have to be calculated self-consistently.
The excitation of the spin degrees of freedom of an adsorbed atom by tunneling electrons is computed using a strong coupling theory. The excitation process is shown to be a sudden switch between the initial state determined by the environmental anisotropy to an intermediate state given by the coupling to the tunnelling electron. This explains the observed large inelastic currents. Application is presented for Fe and Mn adsorbates on CuN monolayers on Cu(100). First-principles calculations show the dominance of one collisional channel, leading to a quantitative agreement with the experiment.
In a recent experiment, Hirjibehedin {\it et al.} [Science {\bf 317}, 1199 (2007)] performed inelastic tunneling spectroscopy of a single iron atom absorbed on a nonmagnetic substrate. The observed steps in the differential conductance marked the spin excitation energies. In this Letter, we explain observed nonmonotonicities in the differential conductance by a nonequilibrium population of the atom spin states. Furthermore, we predict super-Poissonian current noise due to this nonequilibrium situation. By introducing an anisotropic relaxation channel we are also able to explain the remarkable …
Detection of a single nuclear spin constitutes an outstanding problem in different fields of physics such as quantum computing or magnetic imaging. Here we show that the energy levels of a single nuclear spin can be measured by means of inelastic electron tunneling spectroscopy (IETS). We consider two different systems, a magnetic adatom probed with STM and a single Bi dopant in a Silicon nanotransistor. We find that the hyperfine coupling opens new transport channels which can be resolved at experimentally accessible temperatures. Our simulations evince that IETS yield information about the o…
Recent experimental conductance measurements performed on paramagnetic molecular adsorbates on a superconducting surface, using superconducting scanning tunneling microscopy techniques, are theoretically investigated. For low temperatures, we demonstrate that tunneling current assisted excitations of the local magnetic moment cannot occur for voltage biases smaller than the superconducting gap of the scanning tunneling microscope. The magnetic moment is only excited for voltages corresponding to the sum of the superconducting gap and the spin excitation energies. In excellent agreement with ex…
The influence of structural asymmetries (barrier height and exchange splitting), as well as inelastic scattering (magnons and phonons) on the bias dependence of the spin transfer torque in a magnetic tunnel junction is studied theoretically using the free electron model. We show that they modify the "conventional" bias dependence of the spin transfer torque, together with the bias dependence of the conductance. In particular, both structural asymmetries and bulk (inelastic) scattering add {\em antisymmetric} terms to the perpendicular torque ($\propto V$ and $\propto j_e|V|$), while the interf…
Spin excitations in atomic-scale nanostructures have been investigated with inelastic scanning tunneling spectroscopy, sometimes with conflicting results. In this work we present a theoretical viewpoint on a recent experimental controversy regarding the spin excitations of Co adatoms on Pt(111). While one group [Balashov et al., Phys. Rev. Lett. \textbf{102}, 257203 (2009)] claims to have detected them, another group reported their observation only after the hydrogenation of the Co adatom [Dubout et al., Phys. Rev. Lett. \textbf{114}, 106807 (2015)]. Utilizing time-dependent density functional…
We show that a properly dc-biased Josephson junction in series with two microwave resonators of different frequencies emits photon pairs in the resonators. By measuring auto- and inter-correlations of the power leaking out of the resonators, we demonstrate two-mode amplitude squeezing below the classical limit. This non-classical microwave light emission is found to be in quantitative agreement with our theoretical predictions, up to an emission rate of 2 billion photon pairs per second.
We report inelastic electron tunneling spectroscopy (IETS) of multilayer molecular junctions with and without incorporated metal nano-particles. The incorporation of metal nanoparticles into our devices leads to enhanced IET intensity and a modified line-shape for some vibrational modes. The enhancement and line-shape modification are both the result of a low lying hybrid metal nanoparticle-molecule electronic level. These observations explain the apparent discrepancy between earlier IETS measurements of alkane thiolate junctions by Kushmerick \emph{et al.} [Nano Lett. \textbf{4}, 639 (2004)] …
We study the light emission from a Ag(111) surface when the bias voltage on a scanning tunneling microscope (STM) junction is ramped into the field emission regime. Above the vacuum level, scanning tunneling spectroscopy (STS) shows a series of well defined resonances associated with the image states of the surface, which are Stark shifted due to the electric field provided by the STM tip. We present photon--energy resolved measurements that unambiguously show that the mechanism for light emission is the radiative decay of surface localized plasmons excited by the electrons that tunnel inelast…
In this paper we analyze different contributions to the magnetoresistance of magnetic tunneling junctions at low voltages. A substantial fraction of the resistance drop with voltage can be ascribed to variations of the density of states and the barrier transmission with the bias. However, we found that the anomaly observed at zero bias and the magnetoresistance behavior at very small voltages, point to the contribution of inelastic magnon-assisted tunneling. The latter is described by a transfer parameter $T^{J}$, which is one or two orders of magnitude smaller than $T^{d}$, the direct transmi…
We present an extension of the tunneling theory for scanning tunneling microcopy (STM) to include different types of vibrational-electronic couplings responsible for inelastic contributions to the tunnel current in the strong-coupling limit. It allows for a better understanding of more complex scanning tunneling spectra of molecules on a metallic substrate in separating elastic and inelastic contributions. The starting point is the exact solution of the spectral functions for the electronic active local orbitals in the absence of the STM tip. This includes electron-phonon coupling in the coupl…
In this paper we study in detail the effect of the rotational alignment between a hexagonal boron nitride (hBN) slab and the graphene layers in the vertical current of a a graphene-hBN-graphene device. We show how for small rotational angles, the transference of momentum by the hBN crystal lattice leads to multiple peaks in the I-V curve of the device, giving origin to multiple regions displaying negative differential conductance. We also study the effect of scattering by phonons in the vertical current an see how the opening up of inelastic tunneling events allowed by spontaneous emission of …
We consider the transport spectroscopy of a quantum dot with an even number of electrons at finite bias voltage within the Coulomb blockade diamond. We calculate the tunneling current due to the elastic and inelastic co-tunneling processes associated with the spin-singlet ground state and the spin-triplet first excited state. We find a step in the differential conductance at a bias voltage equal to the excitation energy with a peak at the step edge. This may explain the recently observed sharp features in finite bias spectroscopy of semi-conductor quantum dots and carbon nanotubes. Two limitin…
We demonstrate that a quantum spin Hall current, spontaneously generated at the edge of a two-dimensional topological insulator, acts as a source of spin-pumping for a magnetic impurity with uniaxial anisotropy. One can then manipulate the impurity spin direction by means of an electrical current without using either magnetic electrodes or an external magnetic field. Furthermore we show that the unique properties of the quantum spin Hall topological state have profound effects on the inelastic electron tunneling spectrum of the impurity. For low current densities inelastic spin-flip events do …
We demonstrate theoretically that charge transport across a Josephson junction, voltage-biased through a resistive environment, produces antibunched photons. We develop a continuous-mode description of the emitted radiation field in a semi-infinite transmission line terminated by the Josephson junction. Within a perturbative treatment in powers of the tunneling coupling across the Josephson junction, we capture effects originating in charging dynamics of consecutively tunneling Cooper pairs. We find that within a feasible experimental setup the Coulomb blockade provided by high zero-frequency …
We report the observation of two fundamental sub-gap transport processes through a quantum dot (QD) with a superconducting contact. The device consists of a carbon nanotube contacted by a Nb superconducting and a normal metal contact. First, we find a single resonance with position, shape and amplitude consistent with the theoretically predicted resonant Andreev tunneling (AT) through a single QD level. Second, we observe a series of discrete replicas of resonant AT at a separation of $\sim145\,μ$eV, with a gate, bias and temperature dependence characteristic for boson-assisted, inelastic AT, …
Nature sets fundamental limits regarding how accurate the amplification of analog signals may be. For instance, a linear amplifier unavoidably adds some noise which amounts to half a photon at best. While for most applications much higher noise levels are acceptable, the readout of microwave quantum systems, such as spin or superconducting qubits, requires noise as close as possible to this ultimate limit. To date, it is approached only by parametric amplifiers exploiting non-linearities in superconducting circuits and driven by a strong microwave pump tone. However, this microwave drive makes…
We address local inelastic scattering from vibrational impurity adsorbed onto graphene and the evolution of the local density of electron states near the impurity from weak to strong coupling regime. For weak coupling the local electronic structure is distorted by inelastic scattering developing peaks/dips and steps. These features should be detectable in the inelastic electron tunneling spectroscopy, $d^2I/dV^2$, using local probing techniques. Inelastic Friedel oscillations distort the spectral density at energies close to the inelastic mode. In the strong coupling limit, a local negative $U…
Analogous to radio- and microwave antennas, optical nanoantennas are devices that receive and emit radiation at optical frequencies. Until recently, the realization of electrically driven optical antennas was an outstanding challenge in nanophotonics. In this review we discuss and analyze recent reports in which quantum tunneling-specifically inelastic electron tunneling-is harnessed as a means to convert electrical energy into photons, mediated by optical antennas. To aid this analysis we introduce the fundamentals of optical antennas and inelastic electron tunneling. Our discussion is focuse…
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…
The interaction between propagating microwave fields and Cooper-pair tunneling across a DC voltage-biased Josephson junction can be highly nonlinear. We show theoretically that this nonlinearity can be used to convert an incoming single microwave photon into an outgoing $n$-photon Fock state in a different mode. In this process, the electrostatic energy released in a Cooper-pair tunneling event is transferred to the outgoing Fock state, providing energy gain. The created multi-photon Fock state is frequency entangled and highly bunched. The conversion can be made reflectionless (impedance-matc…
We examine theoretically the effects of the bonding geometries at the gold-thiol interfaces on the inelastic tunneling spectra of propanedithiolate (PDT) molecules bridging gold electrodes and show that inelastic tunneling spectroscopy combined with theory can be used to determine these bonding geometries experimentally. With the help of density functional theory, we calculate the relaxed geometries and vibrational modes of extended molecules each consisting of one or two PDT molecules connecting two gold nanoclusters. We formulate a perturbative theory of inelastic tunneling through molecules…
