Inelastic Tunneling Research Articles

Cavity Photons as a Probe for Charge Relaxation Resistance and Photon Emission in a Quantum Dot Coupled to Normal and Superconducting Continua

Microwave cavities have been widely used to investigate the behavior of closed few-level systems. Here, we show that they also represent a powerful probe for the dynamics of charge transfer between a discrete electronic level and fermionic continua. We have combined experiment and theory for a carbon nanotube quantum dot coupled to normal metal and superconducting contacts. In equilibrium conditions, where our device behaves as an effective quantum dot-normal metal junction, we approach a universal photon dissipation regime governed by a quantum charge relaxation effect. We observe how photon dissipation is modified when the dot admittance turns from capacitive to inductive. When the fermionic reservoirs are voltage biased, the dot can even cause photon emission due to inelastic tunneling to/from a Bardeen-Cooper-Schrieffer peak in the density of states of the superconducting contact. We can model these numerous effects quantitatively in terms of the charge susceptibility of the quantum dot circuit. This validates an approach that could be used to study a wide class of mesoscopic QED devices.

Four-electron model for singlet and triplet excitation energy transfers with inclusion of coherence memory, inelastic tunneling and nuclear quantum effects

A computational scheme to describe the coherent dynamics of excitation energy transfer (EET) in molecular systems is proposed on the basis of generalized master equations with memory kernels. This formalism takes into account those physical effects in electron-bath coupling system such as the spin symmetry of excitons, the inelastic electron tunneling and the quantum features of nuclear motions, thus providing a theoretical framework to perform an ab initio description of EET through molecular simulations for evaluating the spectral density and the temporal correlation function of electronic coupling. Some test calculations have then been carried out to investigate the dependence of exciton population dynamics on coherence memory, inelastic tunneling correlation time, magnitude of electronic coupling, quantum correction to temporal correlation function, reorganization energy and energy gap.

Nuclear quantum effects of hydrogen bonds probed by tip-enhanced inelastic electron tunneling.

We report the quantitative assessment of nuclear quantum effects on the strength of a single hydrogen bond formed at a water-salt interface, using tip-enhanced inelastic electron tunneling spectroscopy based on a scanning tunneling microscope. The inelastic scattering cross section was resonantly enhanced by "gating" the frontier orbitals of water via a chlorine-terminated tip, so the hydrogen-bonding strength can be determined with high accuracy from the red shift in the oxygen-hydrogen stretching frequency of water. Isotopic substitution experiments combined with quantum simulations reveal that the anharmonic quantum fluctuations of hydrogen nuclei weaken the weak hydrogen bonds and strengthen the relatively strong ones. However, this trend can be completely reversed when a hydrogen bond is strongly coupled to the polar atomic sites of the surface.

Influence of atomic tip structure on the intensity of inelastic tunneling spectroscopy data analyzed by combined scanning tunneling spectroscopy, force microscopy, and density functional theory

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)] such that it is elevated over the substrate strongly diminishes the tip dependence of IETS intensity, showing that an elevated position channels most of the tunneling current through the CO molecule even for multi-atom tips, while a large fraction of the tunneling current bypasses the CO molecule in the case of CO/Cu(111).

Scanning tunneling spectroscopy onSrFe2(As1−xPx)2

We investigated SrFe$\mathrm{_2}$(As$\mathrm{_{1-x}}$P$\mathrm{_x}$)$\mathrm{_2}$ single crystals with four different phosphorus concentrations x in the superconducting phase (x = 0.35, 0.46) and in the magnetic phase (x = 0, 0.2). The superconducting samples display a V-shaped superconducting gap, which suggests nodal superconductivity. Furthermore we determined the superconducting coherence length by measuring the spatially resolved superconducting density of states (DOS). Using inelastic tunneling spectroscopy we investigated excitations in the samples with four different phosphorus concentrations. Inelastic peaks are related to bosonic modes. Phonon and non-phonon mechanism for the origin of these peaks are discussed.

Nanoantenna for Electrical Generation of Surface Plasmon Polaritons.

Light emission by inelastic tunneling has been known for many years. Recently, this technique has been used to generate surface plasmons using a scanning tunneling microscope tip. The emission process suffers from a very low efficiency lower than a photon in 10^{4} electrons. We introduce a resonant plasmonic nanoantenna that allows both enhancing the power conversion to surface plasmon polaritons by more than 2 orders of magnitude and narrowing the emission spectrum. The physics of the emission process is analyzed in terms of local density of states and the efficiency of the nanoantenna to radiate surface plasmon polaritons.

Power-like corrections to the conductivity of Mo-C nanocomposites

The evolution of the electron transport character in thin films of Mo‐C nanocomposites is studied over the metal concentration range 0.14 ‐ 0.3 at temperatures from 4.2 to 400 K. It is shown that conductivity of the Mo‐C nanocomposites demonstrates the distinct power-like behavior in the two temperature intervals separated at 20 ‐ 25 K. The concentration dependences of the power exponent in both temperature intervals are characterized by the expressed minimum at Mo content close to 0.2 varying over the range 0.25 ‐ 1.0. The experimental data are discussed and simulated in the model of inelastic tunneling of the electrons in amorphous dielectrics in the framework of the effective medium approximation.

Controllable dissociations of PH3 molecules on Si(001)

We demonstrate for the first time to our knowledge that controllable dissociation of PH3 adsorption products PHx (x = 2, 1) can be realized by STM (scanning tunneling microscope) manipulation techniques at room temperature. Five dissociative products and their geometric structures are identified via combining STM experiments and first-principle calculations and simulations. In total we realize nine kinds of controllable dissociations by applying a voltage pulse among the PH3-related structures on Si(001). The dissociation rates of the five most common reactions are measured by the I–t spectrum method as a function of voltage. The suddenly increased dissociation rate at 3.3 V indicates a transition from multivibrational excitation to single-step excitation induced by inelastic tunneling electrons. Our studies prove that selectively breaking the chemical bonds of a single molecule on semiconductor surface by STM manipulation technique is feasible.

Coupling to real and virtual phonons in tunneling spectroscopy of superconductors

Fine structures in the tunneling spectra of superconductors have been widely used to identify fingerprints of the interaction responsible for Cooper pairing. Here we show that for scanning tunneling microscopy (STM) of Pb, the inclusion of inelastic tunneling processes is crucial for the proper interpretation of these fine structures. For STM the usual McMillan inversion algorithm of tunneling spectra must therefore be modified to include inelastic tunneling events, an insight that is crucial for the identification of the pairing glue in conventional and unconventional superconductors alike.

Observing spin excitations in3dtransition-metal adatoms on Pt(111) with inelastic scanning tunneling spectroscopy: A first-principles perspective

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. 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. 114, 106807 (2015)]. Utilizing time-dependent density functional theory in combination with many-body perturbation theory, we demonstrate that, although inelastic spin excitations are possible for Cr, Mn, Fe, and Co adatoms, their efficiency differs. While the excitation signature is less pronounced for Mn and Co adatoms, it is larger for Cr and Fe adatoms. We find that the tunneling matrix elements or the tunneling cross-section related to the nature and symmetry of the relevant electronic states are more favorable for triggering the spin excitations in Fe than in Co. An enhancement of the tunneling and of the inelastic spectra is possible by attaching hydrogen to the adatom at the appropriate position.

Direct Observation of Photoinduced Tautomerization in Single Molecules at a Metal Surface.

Molecular switches are of fundamental importance in nature, and light is an important stimulus to selectively drive the switching process. However, the local dynamics of a conformational change in these molecules remain far from being completely understood at the single-molecule level. Here, we report the direct observation of photoinduced tautomerization in single porphycene molecules on a Cu(111) surface by using a combination of low-temperature scanning tunneling microscopy and laser excitation in the near-infrared to ultraviolet regime. It is found that the thermodynamically stable trans configuration of porphycene can be converted to the metastable cis configuration in a unidirectional fashion by photoirradiation. The wavelength dependence of the tautomerization cross section exhibits a steep increase around 2 eV and demonstrates that excitation of the Cu d-band electrons and the resulting hot carriers play a dominant role in the photochemical process. Additionally, a pronounced isotope effect in the cross section (∼100) is observed when the transferred hydrogen atoms are substituted with deuterium, indicating a significant contribution of zero-point energy in the reaction. Combined with the study of inelastic tunneling electron-induced tautomerization with the STM, we propose that tautomerization occurs via excitation of molecular vibrations after photoexcitation. Interestingly, the observed cross section of ∼10(-19) cm(2) in the visible-ultraviolet region is much higher than that of previously studied molecular switches on a metal surface, for example, azobenzene derivatives (10(-23)-10(-22) cm(2)). Furthermore, we examined a local environmental impact on the photoinduced tautomerization by varying molecular density on the surface and find substantial changes in the cross section and quenching of the process due to the intermolecular interaction at high density.

Ramp-edge junctions between superconducting Nd1.85Ce0.15CuO4 and La1.85Sr0.15CuO4

We have fabricated in-plane ramp-edge junctions between Nd1.85Ce0.15CuO4 (NCCO) and La1.85Sr0.15CuO4 (LSCO) where both layers are superconducting. At the interface, we find an insulating barrier in electronic transport. The barrier is shown to be a tunneling barrier with a combination of inelastic and elastic tunneling, the former is indicated by the appearance of the LSCO phonon density of states in measurements and the latter is inferred from the temperature dependence of the conductance. The energy scale of the barrier is smaller than would be expected from band alignment found by considering the cuprates as degenerate semiconductors. It is closest to the scenario where hybridization of the O 2p valence band states dictate band alignment. Additional experiments with overdoped interlayers of Nd1.8Ce0.2CuO4 and La1.75Sr0.25CuO4 show that the origin of the barrier is most likely a combination of electronic depletion mainly in the NCCO and a strain effect in the LSCO.

Current-Driven Hydrogen Desorption from Graphene: Experiment and Theory.

Electron-stimulated desorption of hydrogen from the graphene/SiC(0001) surface at room temperature was investigated with ultrahigh vacuum scanning tunneling microscopy and ab initio calculations in order to elucidate the desorption mechanisms and pathways. Two different desorption processes were observed. In the high electron energy regime (4-8 eV), the desorption yield is independent of both voltage and current, which is attributed to the direct electronic excitation of the C-H bond. In the low electron energy regime (2-4 eV), however, the desorption yield exhibits a threshold dependence on voltage, which is explained by the vibrational excitation of the C-H bond via transient ionization induced by inelastic tunneling electrons. The observed current independence of the desorption yield suggests that the vibrational excitation is a single-electron process. We also observed that the curvature of graphene dramatically affects hydrogen desorption. Desorption from concave regions was measured to be much more probable than desorption from convex regions in the low electron energy regime (∼2 eV), as would be expected from the identified desorption mechanism.

Correlated Cooper pair transport and microwave photon emission in the dynamical Coulomb blockade

We study theoretically electromagnetic radiation emitted by inelastic Cooper-pair tunneling. We consider a dc-voltage-biased superconducting transmission line terminated by a Josephson junction. We show that the generated continuous-mode electromagnetic field can be expressed as a function of the time-dependent current across the Josephson junction. The leading-order expansion in the tunneling coupling, similar to the "$P(E)$-theory", has previously been used to investigate the photon emission statistics in the limit of sequential (independent) Cooper-pair tunneling. By explicitly evaluating the system characteristics up to the fourth-order in the tunneling coupling, we account for dynamics between consecutively tunneling Cooper pairs. Within this approach we investigate how temporal correlations in the charge transport can be seen in the first- and second-order coherences of the emitted microwave radiation.

Engineering the emission of light from a scanning tunneling microscope using the plasmonic modes of a nanoparticle

The inelastic tunnel current in the junction formed between the tip of a scanning tunneling microscope (STM) and the sample can electrically generate optical signals. This phenomenon is potentially of great importance for nano-optoelectronic devices. In practice, however, the properties of the emitted light are difficult to control because of the strong influence of the STM tip. In this work, we show both theoretically and experimentally that the sought-after, well-controlled emission of light from an STM tunnel junction may be achieved using a nonplasmonic STM tip and a plasmonic nanoparticle on a transparent substrate. We demonstrate that the native plasmon modes of the nanoparticle may be used to engineer the light emitted in the substrate. Both the angular distribution and intensity of the emitted light may be varied in a predictable way by choosing the excitation position of the STM tip on the particle.

Excitation of plasmonic nanoantennas by nonresonant and resonant electron tunnelling.

A rigorous theory of photon emission generated by inelastic electron tunnelling inside the gap of plasmonic nanoantennas is developed. The disappointingly low efficiency of the electrical excitation of surface plasmon polaritons in these structures can be increased by orders of magnitude when a resonant tunnelling structure is incorporated inside the gap. A resonant tunnelling assisted surface plasmon emitter may become a key element in future electrically-driven plasmonic nanocircuits.

A scanning tunneling microscopy study of the electronic and spin states of bis(phthalocyaninato)terbium(iii) (TbPc2) molecules on Ag(111).

In this article, we investigate a single molecule magnet bis(phthalocyaninato)terbium(iii) (TbPc2) molecule film by using low temperature STM. In order to investigate the effect of molecule-substrate interaction on the electronic and spin properties of the adsorbed molecule, we tune the molecule-substrate coupling by switching the substrate between Au(111) and Ag(111), the latter of which provides stronger interaction with the molecule than the former. Despite the enhanced chemical reactivity of the Ag(111) surface compared with Au(111), a well-organized pseudo-square film is formed. In addition, a checker-board type contrast variation is identified, which is well explained by the existence of two types of molecules whose rotational angle between the top and bottom Pc is θ = 45° (bright molecule) and θ = 30° (dark molecule). The expected stronger molecule-substrate interaction, however, appears as an intriguing dI/dV mapping image which reveals the spatial distribution of the density of states (DOS). We identify the contrast reversal in the dI/dV mapping for the molecules of θ = 45° and θ = 30° at the sample voltages of V = 0.7 eV and 1.1 eV. Combined with the density functional theory (DFT) calculation, we attribute this change to the shift of an electronic state due to the rotation of the mutual angle between the top and bottom Pc. For the spin behavior, we previously observed a Kondo resonance for the TbPc2 molecule adsorbed on the Au(111) surface. On the Ag(111) surface, the Kondo resonance is hardly observed, which is due to the annihilation of the π radical spin by the charge transfer from the substrate to the molecule. Instead we observe a Kondo peak for the molecule on the second layer, for which the spin recovers due to the reduction of the coupling with the substrate. In addition, when a magnetic field of 2 T normal to the surface is applied, the second layer molecule shows a sharp dip at the Fermi level. We attribute this to the inelastic tunneling feature caused by the spin flipping. This feature is not observed for the TbPc2/Au(111) system, suggesting that the decoupling between the TbPc2 molecule and Ag(111) by the presence of the first layer produces an inelastic feature in the tunneling spectra.

Tunneling in graphene–topological insulator hybrid devices

Hybrid graphene-topological insulator (TI) devices were fabricated using a mechanical transfer method and studied via electronic transport. Devices consisting of bilayer graphene (BLG) under the TI Bi$_2$Se$_3$ exhibit differential conductance characteristics which appear to be dominated by tunneling, roughly reproducing the Bi$_2$Se$_3$ density of states. Similar results were obtained for BLG on top of Bi$_2$Se$_3$, with 10-fold greater conductance consistent with a larger contact area due to better surface conformity. The devices further show evidence of inelastic phonon-assisted tunneling processes involving both Bi$_2$Se$_3$ and graphene phonons. These processes favor phonons which compensate for momentum mismatch between the TI $\Gamma$ and graphene $K, K'$ points. Finally, the utility of these tunnel junctions is demonstrated on a density-tunable BLG device, where the charge-neutrality point is traced along the energy-density trajectory. This trajectory is used as a measure of the ground-state density of states.

Effective action theory of Andreev level spectroscopy

With the aid of the Keldysh effective action technique we develop a microscopic theory describing Andreev level spectroscopy experiments in nontunnel superconducting contacts. We derive an effective impedance of such contacts which accounts for the presence of Andreev levels in the system. At subgap bias voltages and low temperatures, inelastic Cooper pair tunneling is accompanied by transitions between these levels resulting in a set of sharp current peaks. We evaluate the intensities of such peaks, establish their dependence on the external magnetic flux piercing the structure and estimate the thermal broadening of these peaks. We also specifically address the effect of capacitance renormalization in a nontunnel superconducting contact and its impact on both the positions and heights of the current peaks. At overgap bias voltages, the $I\ensuremath{-}V$ curve is determined by quasiparticle tunneling and contains current steps related to the presence of discrete Andreev states in our system.

Vibrational Properties of h-BN and h-BN-Graphene Heterostructures Probed by Inelastic Electron Tunneling Spectroscopy.

Inelastic electron tunneling spectroscopy is a powerful technique for investigating lattice dynamics of nanoscale systems including graphene and small molecules, but establishing a stable tunnel junction is considered as a major hurdle in expanding the scope of tunneling experiments. Hexagonal boron nitride is a pivotal component in two-dimensional Van der Waals heterostructures as a high-quality insulating material due to its large energy gap and chemical-mechanical stability. Here we present planar graphene/h-BN-heterostructure tunneling devices utilizing thin h-BN as a tunneling insulator. With much improved h-BN-tunneling-junction stability, we are able to probe all possible phonon modes of h-BN and graphite/graphene at Γ and K high symmetry points by inelastic tunneling spectroscopy. Additionally, we observe that low-frequency out-of-plane vibrations of h-BN and graphene lattices are significantly modified at heterostructure interfaces. Equipped with an external back gate, we can also detect high-order coupling phenomena between phonons and plasmons, demonstrating that h-BN-based tunneling device is a wonderful playground for investigating electron-phonon couplings in low-dimensional systems.