The functionality of many biological systems depends on reliable electron transfer with minimal heating. Unlike man-made electric circuits, nature realizes electron transport via insulating chiral molecules. Here we include spin into the analysis of tunneling through these molecules, and demonstrate its importance for efficient transport. We show that the helical geometry induces robust spin filtering accompanied by, and intimately related to, strongly enhanced transmission. Thus, we resolve two key questions posed by transport measurements through organic molecules, demonstrating their common origin.
We measure electron tunneling in single-molecule transistors made from C_{140}, a molecule with a mass-spring-mass geometry chosen as a model system to study electron-vibration coupling. We observe vibration-assisted tunneling at an energy corresponding to the stretching mode of C_{140}. Molecular modeling provides explanations for why this mode couples more strongly to electron tunneling than the other internal modes of the molecule. We make comparisons between the observed tunneling rates and those expected from the Franck-Condon model.
Magnetization measurements of a truly axial symmetry Mn12-tBuAc molecular nanomagnet with a spin ground state of S = 10 show resonance tunneling. This compound has the same magnetic anisotropy as Mn12-Ac but the molecules are better isolated and the crystals have less disorder and a higher symmetry. Hysteresis loop measurements at several temperatures reveal a well-resolved step fine-structure which is due to level crossings of excited states. All step positions can be modeled by a simple spin Hamiltonian. The crossover between thermally assisted and pure quantum tunneling can be investigated …
The transport properties of a metal core/semiconductor shell quantum dot molecule (QDM) embedded in a matrix connected to metallic electrodes are theoretically studied in the framework of Keldysh Green function technique. The effects of the electron plasmon interactions (EPIs) on the tunneling current spectra of QDM are examined. The energy levels of the QDs, intradot and interdot Coulomb interactions, electron interdot hopping strengths, and tunneling rates of QDs are renormalized by the EPIs. The differential conductance spectra show peaks arising from the plasmon assisted tunneling process,…
Coherent state path integrals are shown in general to contain instantons with jumps at the boundaries, i.e., with boundary points lying outside classical parameter or phase space. As an example, the magnetic molecule Fe_8 is studied using a realistic Hamiltonian, and instanons with jumps are shown to dominate beyond a certain external magnetic field. An approximate formula is found for the fields where ground state tunneling is quenched in this molecule.
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.
The equal-interval splitting of quantum tunneling observed in simple-Ising-model systems of Ni$_{4}$ (3D) and Mn$_3$ (2D) single-molecule magnets (SMMs) is reported. The splitting is due to the identical exchange coupling in the SMMs, and is simply determined by the difference between the two numbers of the spin-down $n_{\downarrow}$ and spin-up $n_{\uparrow}$ molecules neighboring to the tunneling molecule. The splitting may be presented as $(n_{\downarrow}-n_{\uparrow})JS/{gμ_{0}μ_{B}}$, and the number of the splittings follows $n+1$ where $n=n_{\downarrow}+n_{\uparrow}$ is the coordination …
The symmetry of magnetic quantum tunneling has been studied in the prototype single molecule magnet Mn$_{12}$-acetate using a micro-Hall effect magnetometer and superconducting high field vector magnet system. An average crystal fourfold symmetry is shown to be due to local molecular environments of twofold symmetry that are rotated by 90$^o$ with respect to one another, confirming that disorder which lowers the molecule symmetry is at important to magnetic quantum tunneling. We have studied a subset of these lower (twofold) site symmetry molecules and present evidence for a Berry phase effect…
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…
We theoretically study the effects of bias-controlled interdot tunneling in vertically coupled quantum dots on the emission properties of spin excitons in various bias-controlled tunneling regimes. As a main result, for strongly coupled dots we predict substantial reduction of optical fine structure splitting without any drop in the optical oscillator strength. This special reduction diminishes the distinguibility of polarized decay paths in cascade emission processes suggesting the use of stacked quantum dot molecules as entangled photon-pair sources.
An application of impedance measurement technique (IMT) for a detection of quantum tunneling in molecular structures is investigated. A charged particle which tunnels in a two-well potential is electrically coupled to a high-quality superconducting LC-circuit(tank) that makes possible a measurement of the electric susceptibility of the molecule at the resonant frequency of the tank. The real part of this susceptibility bears information about the tunneling rate through a measurable parameter - a phase angle between the tank voltage and a bias current applied to the tank. It is shown that the p…
We report spin-pair tunneling observed in Mn$_3$ single-molecule magnet, which is a crystal with 2D network of identical exchange coupling. We observed a series of extra quantum tunnelings by the ac susceptibility measurements, and demonstrated these are concerted tunnelings of two spins taking place from the same initial state to the same final state simultaneously. The resonant field of spin-pair tunneling can be expressed as $H_z=lD/gμ_{0}μ_{B}+(n_{\downarrow}-n_{\uparrow})JS/2{gμ_{0}μ_{B}}$, and the splitting interval ($|J|S/{gμ_{0}μ_{B}}$) is half of that of the single-spin tunneling ($2|…
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…
Tunneling between the two lowest energy levels of single molecule magnets with Ising type anisotropy, accompanied by the emission or absorption of phonons, is considered. Quantitatively accurate calculations of the rates for such tunneling are performed for a model Hamiltonian especially relevant to the best studied example, \Fe8. Two different methods are used: high-order perturbation theory in the spin-phonon interaction and the non-Ising-symmetric parts of the spin Hamiltonian, and a novel semiclassical approach based on spin-coherent-state-path-integral instantons. The methods are found to…
We theoretically investigate quantum transport through single-molecule magnet (SMM) junctions with ferromagnetic and normal-metal leads in the sequential regime. The current obtained by means of the rate-equation gives rise to the tunneling anisotropic magnetoresistance (TAMR), which varies with the angle between the magnetization direction of ferromagnetic lead and the easy axis of SMM. The angular dependence of TAMR can serve as a probe to determine experimentally the easy axis of SMM. Moreover, it is demonstrated that both the magnitude and sign of TAMR are tunable by the bias voltage, sugg…
We present a theory of tunneling spectroscopy of spin-selective Aharonov-Bohm oscillations in a lateral triple quantum dot molecule. The theory combines exact treatment of an isolated many-body system with the rate equation approach when the quantum dot molecule is weakly connected to the leads subject to arbitrary source-drain bias. The tunneling spectroscopy of the many-body complex is analyzed using the spectral functions of the system and applied to holes in a quantum dot molecule. Negative differential conductance is predicted and explained as a result of the redistribution of the spectra…
Chiral tunneling through a harmonically driven potential barrier in graphene monolayer is considered in this work. Since the quasiparticles in this system are chiral in nature, tunneling is highly anisotropic, we determine the transmission probabilities for the central and sidebands as the incident angle of the electron beam is changed . Furthermore, we investigate how the transmission probabilities change as the width, amplitude and frequency of the oscillating barrier is changed. An interesting result of our study is that perfect transmission for normal incidence that has been reported for a…
We present low temperature magnetometry measurements on a new Mn3 single-molecule magnet (SMM) in which the quantum tunneling of magnetization (QTM) displays clear evidence for quantum mechanical selection rules. A QTM resonance appearing only at elevated temperatures demonstrates tunneling between excited states with spin projections differing by a multiple of three: this is dictated by the C3 symmetry of the molecule, which forbids pure tunneling from the lowest metastable state. Resonances forbidden by the molecular symmetry are explained by correctly orienting the Jahn-Teller axes of the i…
We consider electrical transport through single molecules coupled to metal electrodes via tunneling barriers. Approximating the molecule by the Anderson impurity model as the simplest model which includes Coulomb charging effects, we extend the ``orthodox'' theory to expand current and shot noise systematically order by order in the tunnel couplings. In particular, we show that a combined measurement of current and shot noise reveals detailed information of the system even in the weak-coupling limit, such as the ratio of the tunnel-coupling strengths of the molecule to the left and right elect…
We investigate the topological quenching of spin tunneling in Mn_12-acetate molecules with an applied magnetic field along the hard axis. The model Hamiltonian describing this system has a fourth-order term due to the tetragonal anisotropy. We treat this model using the discrete phase integral formalism in which the Schrodinger equation corresponding to the Hamiltonian becomes a nine-term recursion relation. We solve this recursion relation and find that the tunnel splitting is quenched at certain values of the applied field. We also present a qualitative treatment based on the instanton appro…
We demonstrate theoretically that it is possible to use Rabi oscillations to coherently control the electron tunneling in an asymmetric double quantum dot system, a quantum dot molecule. By applying an optical pump pulse we can excite an electron in one of the dots, which can in turn tunnel to the second dot, as controlled by an external voltage. Varying the intensity of the pulse one can suppress or enhance the tunneling between the dots for given level resonance conditions. This approach allows substantial flexibility in the control of the quantum mechanical state of the system.
The detection of fluorescence with submolecular resolution enables the exploration of spatially varying photon yields and vibronic properties at the single-molecule level. By placing individual polycyclic aromatic hydrocarbon molecules into the plasmon cavity formed by the tip of a scanning tunneling microscope and a NaCl-covered Ag(111) surface, molecular light emission spectra are obtained that unravel vibrational progression. In addition, light spectra unveil a signature of the molecule even when the tunneling current is injected well separated from the molecular emitter. This signature exh…
We show that the interplay between chiral tunneling and spin-momentum locking of helical surface states leads to spin amplification and filtering in a 3D Topological Insulator (TI). Chiral tunneling across a TI pn junction allows normally incident electrons to transmit, while the rest are reflected with their spins flipped due to spin-momentum locking. The net result is that the spin current is enhanced while the dissipative charge current is simultaneously suppressed, leading to an extremely large, gate tunable spin to charge current ratio (~20) at the reflected end. At the transmitted end, t…
Magnetic adsorbates on superconductors induce a Kondo resonance outside and Yu-Shiba-Rusinov (YSR) bound states inside the superconducting energy gap. When probed by scanning tunneling spectroscopy, the associated differential-conductance spectra frequently exhibit characteristic bias-voltage asymmetries. Here, we observe correlated variations of Kondo and YSR asymmetries across an Fe-porphyrin molecule adsorbed on Pb(111). We show that both asymmetries originate in interfering tunneling paths via a spin-carrying orbital and the highest occupied molecular orbital (HOMO). Strong evidence for th…
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.
We study the influence of the phonon environment on the electron dynamics in a doped quantum dot molecule. A non-perturbative quantum kinetic theory based on correlation expansion is used in order to describe both diagonal and off-diagonal electron-phonon couplings representing real and virtual processes with relevant acoustic phonons. We show that the relaxation is dominated by phonon-assisted electron tunneling between constituent quantum dots and occurs on a picosecond time scale. The dependence of the time evolution of the quantum dot occupation probabilities on the energy mismatch between…
Magnons can generate a spin current, and the standard generating mechanism requires at least one external field. Since this mechanism is often applied to a multilayer system including a magnet and a paramagnetic metal, the system can possess not only the charge current induced by the spin current but also the charge current induced by the external field. The latter is an unnecessary accompaniment. Here we show that the tunneling of a magnon pair between chiral magnets can generate a spin current even without external fields. This phenomenon originates from a phase difference between magnon pai…
The junction of a scanning tunneling microscope (STM) operating in the tunneling regime was irradiated with femtosecond laser pulses. A photo-excited hot electron in the STM tip resonantly tunnels into an excited state of a single molecule on the surface, converting it from the neutral to the anion. The electron transfer rate depends quadratically on the incident laser power, suggesting a two-photon excitation process. This nonlinear optical process is further confirmed by the polarization measurement. Spatial dependence of the electron transfer rate exhibits atomic-scale variations. A two-pul…
A key step towards building single molecule machines is to control the rotation of molecules and nanostructures step by step on a surface. Here, we used the tunneling electrons coming from the tip of a scanning tunneling microscope to achieve the controlled directed rotation of complex o-MeO-DMBI molecules. We studied the adsorption of single o-MeO-DMBI molecules on Au(111) by scanning tunneling microscopy at low temperature. The enantiomeric form of the molecule on the surface can be determined by imaging the molecule by STM at high bias voltage. We observed by lateral manipulation experiment…
The electronic transport properties in magnetically doped ultra-thin films of topological-insulators is investigated by using Landauer-buttiker formalism. The chiral selective tunneling is addressed in such systems which leads to transport gap and as a consequence current blocking. This quantum blocking of transport occurs when the magnetic states with opposite chirality are aligned energetically. This can be obsereved when an electron tunnels through a barrier or well of magnetic potential induced by the exchange field. It is proved and demonstrated that this chiral transition rule fails when…
Single molecule scanning tunneling spectroscopy (STS), with dephasing due to elastic and inelastic scattering, is of some current interest. Motivated by this, we report an extended Huckel theory (EHT) based mean-field Non-equilibrium Green's function (NEGF) transport model with electron-phonon scattering treated within the self-consistent Born approximation (SCBA). Furthermore, a procedure based on EHT basis set modification is described. We use this model to study the effect of the temperature dependent dephasing, due to low lying modes in far-infrared range for which hw<<kT, on the resonant …
We study the effect of chiral-tunneling in Bernal and Rombhohedral stacked trilayer-graphene (3LG). Based on the chirality of the electronic bands, at the K-point, (Rombhohedral) Bernal-3LG exhibits 100% (50%) transparency across a heterojunction. Utilizing this property, we further investigate the effect of electron collimation in 3LG. Due to the difference in the Berry's phase, we show that, Rombhohedral-3LG is a better electron collimator, compared to monolayer and Bernal-bilayer graphene. Since, Bernal-3LG can be decomposed into two separate channels consisting of a monolayer and a modifie…
We study the elementary processes behind one of the pioneering works on STM controlled reactions of single molecules [Stipe et al., Phys. Rev. Lett. 81, 1263 (1998)]. Using the Keldysh-Green function approach for the vibrational generation rate in combination with DFT calculations to obtain realistic parameters we reproduce the experimental rotation rate of an acetylene molecule on a Cu(100) surface as a function of bias voltage and tunneling current. This combined approach allows us to identify the reaction coordinate mode of the acetylene rotation and its anharmonic coupling with the C-H str…
We explore theoretically the scanning tunneling microscopy of single molecules on substrates using a framework of two local probes. This framework is appropriate for studying electron flow in tip/molecule/substrate systems where a thin insulating layer between the molecule and a conducting substrate transmits electrons non-uniformly and thus confines electron transmission between the molecule and substrate laterally to a nanoscale region significantly smaller in size than the molecule. The tip-molecule coupling and molecule-substrate coupling are treated on the same footing, as local probes to…
The symmetry of magnetic quantum tunneling (MQT) in the single molecule magnet Mn12-acetate has been determined by sensitive low-temperature magnetic measurements in the pure quantum tunneling regime and high frequency EPR spectroscopy in the presence of large transverse magnetic fields. The combined data set definitely establishes the transverse anisotropy terms responsible for the low temperature quantum dynamics. MQT is due to a disorder induced locally varying quadratic transverse anisotropy associated with rhombic distortions in the molecular environment (2nd order in the spin-operators).…
Electronic devices composed of single molecules constitute the ultimate limit in the continued downscaling of electronic components. A key challenge for single-molecule electronics is to control the temperature of these junctions. Controlling heating and cooling effects in individual vibrational modes, can in principle, be utilized to increase stability of single-molecule junctions under bias, to pump energy into particular vibrational modes to perform current-induced reactions or to increase the resolution in inelastic electron tunneling spectroscopy by controlling the life-times of phonons i…
We employ ultrafast pump-probe spectroscopy to directly monitor electron tunneling between discrete orbital states in a pair of spatially separated quantum dots. Immediately after excitation, several peaks are observed in the pump-probe spectrum due to Coulomb interactions between the photo-generated charge carriers. By tuning the relative energy of the orbital states in the two dots and monitoring the temporal evolution of the pump-probe spectra the electron and hole tunneling times are separately measured and resonant tunneling between the two dots is shown to be mediated both by elastic and…
We have studied the crossover between thermally assisted and pure quantum tunneling in single crystals of high spin (S=10) uniaxial single molecule magnet Mn12-acetate using micro-Hall effect magnetometry. Magnetic hysteresis experiments have been used toinvestigate the energy levels that determine the magnetization reversal as a function of magnetic field and temperature. These experiments demonstrate that the crossover occurs in a narrow (~0.1 K) or broad (~1 K) temperature interval depending on the magnitude and direction of the applied field. For low external fields applied parallel to the…
We present high-frequency angle-dependent EPR data for crystals of [NixZn1-x(hmp)(t-BuEtOH)Cl]4 (x = 1 and 0.02). The x = 1 complex behaves as a single-molecule magnet at low temperatures, displaying hysteresis and exceptionally fast magnetization tunneling. We show that this behavior is related to a 4th-order transverse crystal-field interaction, which produces a significant tunnel-splitting (~10 MHz) of the ground state of this S = 4 system. The magnitude of the 4th-order anisotropy, and the dominant axial term (D), can be related to the single-ion interactions (Di and Ei) at the individual …
The Majorana fermion can be described by a real wave function with only two phases (0 and π) which provide a controllable degree of freedom. We propose a strategy to regulate the phase of the chiral Majorana state by coupling with a scanning tunneling microscope tip in a system consisting of quantum anomalous Hall insulator coupled with a superconductor. With the change of the chemical potential, the chiral Majorana state can be tuned alternately between 0 and π, in which, correspondingly, the perfect normal tunneling and perfect crossed Andreev reflection appear. The perfect crossed Andreev r…
Electrons in graphene follow unconventional trajectories at PN junctions, driven by their pseudospintronic degree of freedom. Significant is the prominent angular dependence of transmission, capturing the chiral nature of the electrons and culminating in unit transmission at normal incidence (Klein tunneling). We theoretically show that such chiral tunneling can be directly observed from the junction resistance of a tilted interface probed with separate split gates. The junction resistance is shown to increase with tilt in agreement with recent experimental evidence. The tilt dependence arises…
A quantum effect at ambient conditions is presented. A benzene dithiol (BDT) molecule or a tetrahydrofuran (THF) molecule is used as a barrier molecule bridging the gold electrodes from a Mechanically Controllable Break junction. It has been known for a long time that the environment of a junction couples to the conduction. With a microscopic layer of fluid it is actually possible to influence this coupling. The electrode-molecule-electrode configuration is lined with a microscopic layer of THF fluid, also known as the partially wet phase. This is effectively decoupling the electrode-molecule-…
EPR studies of a Ni4 single-molecule magnet yield the zero-field-splitting (zfs) parameters, D, B40 and B44, based on a giant spin approximation (GSA) with S = 4. Experiments on an isostructural Ni-doped Zn4 crystal establish the Ni(II) ion zfs parameters. The 4th-order zfs parameters in the GSA arise from the interplay between the Heisenberg interaction, Js1.s2, and the 2nd-order single-ion anisotropy, giving rise to mixing of higher lying states into the S = 4 state. Consequently, J directly influences the zfs in the ground state, enabling its direct determination by EPR.
We explore theoretically the electroluminescence of single molecules. We adopt a local-electrode framework that is appropriate for scanning tunneling microscopy (STM) experiments where electroluminescence originates from individual molecules of moderate size on complex substrates: Couplings between the STM tip and molecule and between the molecule and multiple substrate sites are treated on the same footing, as local electrodes contacting the molecule. Electron flow is modelled with the Lippmann-Schwinger Green function scattering technique. The evolution of the electronic energy levels of the…
A new approach is used that allows to describe the magnetic molecules main properties in a direct and simple way. Results obtained for the Fe8 cluster show good agreement with the experimental data.
We analyze how functionality could be obtained within single-molecule devices by using a combination of non-equilibrium Green's functions and ab-initio calculations to study the inelastic transport properties of single-molecule junctions. First we apply a full non-equilibrium Green's function technique to a model system with electron-vibration coupling. We show that the features in the inelastic electron tunneling spectra (IETS) of the molecular junctions are virtually independent of the nature of the molecule-lead contacts. Since the contacts are not easily reproducible from one device to ano…
Based on numerical calculations it is shown that the antiferromagnetic grid molecule Mn-[3 x 3] is a very promising candidate to experimentally detect the phenomenon of quantum tunneling of the Neel vector.
We report on experimental verification of the rotational sense and type of homogeneous chiral spin spiral order in a Mn monolayer on a W(110) substrate using spin-polarized scanning tunneling microscopy. We found that the magnetic contrast due to the spin spiral order almost vanishes with a magnetic tip magnetized normal to the (001) plane, indicating that the spin spiral rotates in the plane. From a shift in the most-contrasted sites by changing the tip magnetization direction within the rotating plane, we reveal that the rotational sense is left-handed, consistent with the previous results p…
Recent advances in scanning probe techniques rely on the chemical functionalization of the probe-tip termination by a single molecule. The success of this approach opens the tantalizing prospect of introducing spin sensitivity through the functionalization by a magnetic molecule. Here, we use a nickelocene-terminated tip (Nc-tip), which offers the possibility of producing spin excitations on the tip apex of a scanning tunneling microscope (STM). We show that when the Nc-tip is a hundred pm away from point contact with a surface-supported object, magnetic effects may be probed through changes i…
Electron Spin Resonance-Scanning Tunneling Microscopy (ESR-STM) of C60 radical ion on graphene is a first demonstration on radical ions. ESR-STM signal at g=2.00 was measured in accordance with macroscopic ESR of fullerene radical ion. The ESR-STM signal was bias voltage dependent, as it reflects the charge state of the molecule. The signal appears in the bias voltage which enables the ionization of the lowest unoccupied molecular orbital (LUMO) (creation of radical anion) and the highest occupied molecular orbital (HOMO (creation of a radical cation) of the C60 molecule when it deposited on g…
Understanding how the mechanism of charge transport through molecular tunnel junctions depends on temperature is crucial to control electronic function in molecular electronic devices. With just a few systems investigated as a function of bias and temperature so far, thermal effects in molecular tunnel junctions remain poorly understood. Here we report a detailed charge transport study of an individual redox-active ferrocene-based molecule over a wide range of temperatures and applied potentials. The results show the temperature dependence of the current to vary strongly as a function of the g…
Polyalanine molecules (PA) with an α-helix conformation gathered recently a lot of interest as the propagation of electrons through the chiral backbone structure comes along with spin polarization of the transmitted electrons. By means of scanning tunneling microscopy and spectroscopy at ambient conditions, PA molecules adsorbed on surfaces of epitaxial magnetic Al2O3/Pt/Au/Co/Au nanostructures with perpendicular anisotropy were studied. Thereby, a correlation between the PA molecules ordering at the surface with the electron tunneling across this hybrid system as a function of the substrate m…
We present electronic transport measurements through thiolated C$_{60}$ molecules in liquid environment. The molecules were placed within a mechanically controllable break junction using a single anchoring group per molecule. When varying the electrode separation of the C$_{60}$-modified junctions, we observed a peak in the conductance traces. The shape of the curves is strongly influenced by the environment of the junction as shown by measurements in two distinct solvents. In the framework of a simple resonant tunneling model, we can extract the electronic tunneling rates governing the transp…
The so-called Klein paradox - unimpeded penetration of relativistic particles through high and wide potential barriers - is one of the most exotic and counterintuitive consequences of quantum electrodynamics (QED). The phenomenon is discussed in many contexts in particle, nuclear and astro- physics but direct tests of the Klein paradox using elementary particles have so far proved impossible. Here we show that the effect can be tested in a conceptually simple condensed-matter experiment by using electrostatic barriers in single- and bi-layer graphene. Due to the chiral nature of their quasipar…
By a polaronic energy shift, the effective charging energy of molecules can become negative, favoring ground states with even numbers of electrons. Here, we show that charge transport through such molecules near ground-state degeneracies is dominated by tunneling of electron pairs which coexists with (featureless) single-electron cotunneling. Due to the restricted phase space for pair tunneling, the current-voltage characteristics exhibits striking differences from the conventional Coulomb blockade. In asymmetric junctions, pair tunneling can be used for gate-controlled current rectification a…
Achieving a high intensity in inelastic scanning tunneling spectroscopy (IETS) is important for precise measurements. The intensity of the IETS signal can vary up to a factor three for various tips without an apparent reason accessible by scanning tunneling microscopy (STM) alone. Here, we show that combining STM and IETS with atomic force microscopy enables carbon monoxide front atom identification, revealing that high IETS intensities for CO/Cu(111) are obtained for single atom tips, while the intensity drops sharply for multi-atom tips. Adsorbing the CO molecule on a Cu adatom [CO/Cu/Cu(111…
Scanning tunneling microscopy (STM) has been a fundamental tool to characterize many-body effects in condensed matter systems, from extended solids to quantum dots. STM of molecules decoupled from the supporting conductive substrate has the potential to extend STM characterization of many body effects to the molecular world as well. In this article, we describe a many-body tunneling theory for molecules decoupled from the STM substrate, and we report on the use of standard quantum chemical methods to calculate the quantities necessary to provide the 'correlated' STM molecular image. The develo…
Inelastic tunneling through magnetically anisotropic molecules is studied theoretically in the presence of a strong magnetic field. Since the molecular orientation is not well controlled in tunneling experiments, we consider arbitrary angles between easy axis and field. This destroys all conservation laws except that of charge, leading to a rich fine structure in the differential conductance. Besides single molecules we also study monolayers of molecules with either aligned or random easy axes. We show that detailed information on the molecular transitions and orientations can be obtained from…
