Kondo-transport spectroscopy of single molecule magnets

We demonstrate that in a single molecule magnet strongly coupled to electrodes the Kondo effect involves all magnetic excitations. This Kondo effect is induced by the quantum tunneling of the magnetic moment. Importantly, the Kondo temperature TK can be much larger than the magnetic splittings. We find a strong modulation of the Kondo effect as a function of the transverse anisotropy parameter or a longitudinal magnetic field. Both for integer and half-integer spin this can be used for an accurate transport spectroscopy of the magnetic states in low magnetic fields on the order of the easy-axis anisotropy parameter. We set up a relationship between the Kondo effects for successive integer and half-integer spins.     

Quantum-tunneling-induced Kondo effect in single molecular magnets

We consider transport through a single-molecule magnet strongly coupled to metallic electrodes. We demonstrate that, for a half-integer spin of the molecule, electron and spin tunneling cooperate to produce both quantum tunneling of the magnetic moment and a Kondo effect in the linear conductance. The Kondo temperature depends sensitively on the ratio of the transverse and easy-axis anisotropies in a nonmonotonic way. The magnetic symmetry of the transverse anisotropy imposes a selection rule on the total spin for the occurrence of the Kondo effect which deviates from the usual even-odd alternation.     

Phonon-assisted thermoelectric effects in strongly interacting quantum dot

The joint effects of the electron-phonon interaction and Kondo effect on the charge and heat transport through a single molecule transistor are investigated by applying the improved canonical transformation and noncrossing approximation technique. We find that the electron-phonon interaction decreases the conductance, thermopower and the Wiedemann-Franz law in the Kondo regime due to the splitting and the decreasing of the main Kondo peak. However, the thermoelectric figure of merit achieves enhancement with the electron-phonon coupling strength increasing. In addition, the dip value of the thermopower at the Kondo temperature for the different electron-phonon coupling strength can give a straightforward reliable estimate of the electron-phonon coupling strength.     

Study of the interaction of a palladium nanocontact with a hydrogen molecule

The interaction of a palladium nanocontact with a hydrogen molecule has been studied using molecular static method. The influence of impurity on the atomic structure and mechanical properties of the palladium nanocontact has been demonstrated. The characteristic interatomic distance has been determined in this contact. It has been found that the hydrogen molecule dissociates by interaction with nanocontact atoms.     

Intra- and inter-shell Kondo effects in carbon nanotube quantum dots

The linear response transport properties of carbon nanotube quantum dot in the strongly correlated regime are discussed. The finite-U mean field slave boson approach is used to study many-body effects. Magnetic field can rebuilt Kondo correlations, which are destroyed by the effect of spin-orbit interaction or valley mixing. Apart from the field induced revivals of SU(2) Kondo effects of different types: spin, valley or spin-valley, also more exotic phenomena appear, such as SU(3) Kondo effect. Threefold degeneracy occurs due to the effective intervalley exchange induced by short-range part of Coulomb interaction or due to the intershell mixing. In narrow gap nanotubes the full spin-orbital degeneracy might be recovered in the absence of magnetic field opening the condition for a formation of SU(4) Kondo resonance.     

Universal scaling in nonequilibrium transport through a single channel Kondo dot

Scaling laws and universality play an important role in our understanding of critical phenomena and the Kondo effect. We present measurements of nonequilibrium transport through a single-channel Kondo quantum dot at low temperature and bias. We find that the low-energy Kondo conductance is consistent with universality between temperature and bias and is characterized by a quadratic scaling exponent, as expected for the spin-1/2 Kondo effect. We show that the nonequilibrium Kondo transport measurements are well described by a universal scaling function with two scaling parameters.     

通过单分子化学调控单个离子磁性--单分子"手术"开启分子磁性"开关"

报道了如何通过改变单个磁性离子的化学环境来调控其白旋性质．利用扫描隧道显微镜，对吸附于Au（111）表面的单个钴酞菁分子进行化学修饰，通过在针尖上施加一定的电压脉冲，将分子配合体外层的8个氢原子“剪裁”掉，使其与金衬底形成稳定的化学键合．在这个新的人造分子结构中，其中心钴离子的电子态在费米面上出现强烈的共振峰；通过理论的模拟和分析，发现出现这一共振峰的原因是，脱氢和与衬底的化学结合使中心钴离子自旋性质发生改变，从而导致了输运特性中近藤效应（Kondo effect）的出现．     

Kondo effect of an adsorbed cobalt phthalocyanine (CoPc) molecule: the role of quantum interference

It has been shown that by distorting a CoPc molecule adsorbed on a Au(111) surface a Kondo effect is induced with a temperature higher than 200 K. We examine a model in which an atom with strong Coulomb repulsion (Co) is surrounded by four atoms on a square (molecule lobes), with two atoms above and below it representing the apex of the STM tip and an atom on the gold surface (all with a single atomic orbital). The Hamiltonian is solved exactly for the isolated cluster, and, after connecting the leads, the conductance is calculated by standard techniques. Quantum interference prevents the existence of the Kondo effect when the orbitals on the square do not interact (undistorted molecule); the Kondo resonance shows up after switching on that interaction. The weight of the Kondo resonance is controlled by the interplay of couplings to the STM tip and the gold surface and between the molecule lobes.     

Site-specific kondo effect at ambient temperatures in iron-based molecules

Kondo resonances are a very precise measure of spin-polarized transport through magnetic impurities. However, the Kondo temperature, indicating the thermal range of stability of the magnetic properties, is very low. By contrast, we find for iron phthalocyanine a Kondo temperature in spectroscopic measurements which is well above room temperature. It is also shown that the signal of the resonance depends strongly on the adsorption site of the molecule on a gold surface. Experimental data are verified by extensive numerical simulations, which establish that the coupling between iron states and states of the substrate depends strongly on the adsorption configuration.     

Chiral splitting of Kondo peak in triangular triple quantum dot

New characteristics of the Kondo effect, arising from spin chirality induced by the Berry phase in the equilibrium state, are investigated. The analysis is based on the hierarchical equations of motion (HEOM) approach in a triangular triple quantum-dot (TTQD) structure. In the absence of magnetic field, TTQD has four-fold degenerate chiral ground states with degenerate spin chirality. When a perpendicular magnetic field is applied, the chiral interaction is induced by the magnetic flux threading through TTQD and the four-fold degenerate states split into two chiral state pairs. The chiral excited states manifest as chiral splitting of the Kondo peak in the spectral function. The theoretical analysis is confirmed by the numerical computations. Furthermore, under a Zeeman magnetic field B, the chiral Kondo peak splits into four peaks, owing to the splitting of spin freedom. The influence of spin chirality on the Kondo effect signifies an important role of the phase factor. This work provides insight into the quantum transport of strongly correlated electronic systems.     

Conductance through atomic point contacts between fcc(100) electrodes of gold

Electrical conductance through various nanocontacts between gold electrodes is studied by using the density functional theory, scalar-relativistic pseudopotentials, generalized gradient approximation for the exchange-correlation energy and the recursion-transfer-matrix method along with channel decomposition. The nanocontact is modeled with pyramidal fcc(100) tips and 1 to 5 gold atoms between the tips. Upon elongation of the contact by adding gold atoms between the tips, the conductance at Fermi energy E_F evolves from G ≈ 3G₀ to G ≈ 1G₀ (G₀ = 2e/h²). Formation of a true one-atom point contact, with G ≈ 1G₀ and only one open channel, requires at least one atom with coordination number 2 in the wire. Tips that share a common vertex atom or tips with touching vertex atoms have three partially open conductance channels at E_F, and the symmetries of the channels are governed by the wave functions of the tips. The long 5-atom contact develops conductance oscillations and conductance gaps in the studied energy range -3 ≤ E-E_F ≤ 5 eV, which reflects oscillations in the local density of electron states in the 5-atom linear “gold molecule" between the electrodes, and a weak coupling of this “molecule" to the tips.     

Magnetic-field probing of an SU(4) Kondo resonance in a single-atom transistor

Semiconductor devices have been scaled to the point that transport can be dominated by only a single dopant atom. As a result, in a Si fin-type field effect transistor Kondo physics can govern transport when one electron is bound to the single dopant. Orbital (valley) degrees of freedom, apart from the standard spin, strongly modify the Kondo effect in such systems. Owing to the small size and the s-like orbital symmetry of the ground state of the dopant, these orbital degrees of freedom do not couple to external magnetic fields which allows us to tune the symmetry of the Kondo effect. Here we study this tunable Kondo effect and demonstrate experimentally a symmetry crossover from an SU(4) ground state to a pure orbital SU(2) ground state as a function of magnetic field. Our claim is supported by theoretical calculations that unambiguously show that the SU(2) symmetric case corresponds to a pure valley Kondo effect of fully polarized electrons.     

Kondo resonance assisted thermoelectric transport through strongly correlated quantum dots

We theoretically studied the thermoelectric transport properties of a strongly correlated quantum dot system in the presence of the Kondo effect based on accurate numerical evaluations using the hierarchical equations of motion approach. The thermocurrent versus gate voltage shows a distinct sawtooth line-shape at high temperatures. In particular, the current changes from positive(hole charge) to negative(particle charge) in the electron number N = 1 region due to the Coulomb blockade effect. However,at low temperatures, where the Kondo effect occurs, the thermocurrent's charge polarity reverses, along with a significantly enhanced magnitude. As anticipated, the current sign can be analyzed by the occupation difference between particle and hole.Moreover, the characteristic turnover temperature can be further defined at which the influences of the Coulomb blockade and Kondo resonance are in an effective balance. Remarkably, the identified characteristic turnover temperature, as a function of the Coulomb interaction and dot-lead coupling, possessed a much higher value than the Kondo temperature. When a magnetic field is applied, a spin-polarized thermocurrent can be obtained, which could be tested in future experiments.     

Kondo effect in the presence of itinerant-electron ferromagnetism studied with the numerical renormalization group method

The Kondo effect in quantum dots (QDs)-artificial magnetic impurities-attached to ferromagnetic leads is studied with the numerical renormalization group method. It is shown that the QD level is spin split due to the presence of ferromagnetic electrodes, leading to a suppression of the Kondo effect. We find that the Kondo effect can be restored by compensating this splitting with a magnetic field. Although the resulting Kondo resonance then has an unusual spin asymmetry with a reduced Kondo temperature, the ground state is still a locally screened state, describable by Fermi liquid theory and a generalized Friedel sum rule, and transport at zero temperature is spin independent.     

Phase transition and charge transport through a triple dot device beyond the Kondo regime

Semiconductor quantum dot structure provides a promising basis for quantum information processing, within which to reveal the quantum phase and charge transport is one of the most important issues. In this paper, by means of the numerical renormalization group technique, we study the quantum phase transition and the charge transport for a parallel triple dot device in the strongly correlated limit, focusing on the effect of inter-dot hopping t beyond the Kondo regime. We find the quantum behaviors depend closely on the initial electron number on the dots, and the present model may map to single,double, and side-coupled impurity models in different parameter spaces. An orbital spin-1/2 Kondo effect between the conduction leads and the bonding orbital, and several magnetic-frustration phases are demonstrated when t is adjusted to different regimes. To understand these phenomena, a canonical transformation of the energy levels is given, and important physical quantities with respect to increasing t and necessary theoretical discussions are shown.     

Kondo effect in a deformed molecule coupled asymmetrically to ferromagnetic electrodes

The nonequilibrium Kondo effect is studied in a molecule quantum dot coupled asymmetrically to two ferromagnetic electrodes by employing the nonequilibrium Green function technique. The current-induced deformation of the molecule is taken into account, modeled as interactions with a phonon system, and phonon-assisted Kondo satellites arise on both sides of the usual main Kondo peak. In the antiparallel electrode configuration, the Kondo satellites can be split only for the asymmetric dot-lead couplings, distinguished from the parallel configuration where splitting also exists, even though it is for symmetric case. We also analyze how to compensate the splitting and restore the suppressed zero-bias Kondo resonance. It is shown that one can change the TMR ratio significantly from a negative dip to a positive peak only by slightly modulating a local external magnetic field, whose value is greatly dependent on the electron--phonon coupling strength.     

Spin-flip transport through an interacting quantum dot

The spin-flip associated transport based on the Anderson model is studied. It is found that the electrons are scattered due to spin-flip effect via the normal, mixed and Kondo channels. The spin-flip scattering via Kondo channel enhances the Kondo resonance peak and causes a slight blue shift. The conductance is suppressed by the spin-flip scattering. This is attributed to the reason that electrons with energy near Fermi level are scattered by Kondo channel.     

Imaginary-time formulation of steady-state nonequilibrium: application to strongly correlated transport

We extend the imaginary-time formulation of the equilibrium quantum many-body theory to steady-state nonequilibrium with an application to strongly correlated transport. By introducing the Matsubara voltage, we maintain the finite chemical potential shifts in the Fermi-Dirac function, in agreement with the Keldysh formulation. The formulation is applied to strongly correlated transport in the Kondo regime using the quantum Monte Carlo method.     

Many-body effects on the transport properties of single-molecule devices

The conductance through a molecular device including electron-electron and electron-phonon interactions is calculated using the numerical renormalization group method. At low temperatures and weak electron-phonon coupling the properties of the conductance can be explained in terms of the standard Kondo model with renormalized parameters. At large electron-phonon coupling a charge analog of the Kondo effect takes place that can be mapped into an anisotropic Kondo model. In this regime the molecule is strongly polarized by a gate voltage which leads to rectification in the current-voltage characteristics of the molecular junction.     

Splitting and Restoration of Kondo Peak in a Deformed Molecule Quantum Dot Coupled to Ferromagnetic Electrodes

We adopt the nonequilibrium Green＇s function method to theoretically study the Kondo effect in a deformed molecule, which is treated as an electron-phonon interaction （EPI） system. The self-energy for phonon part is calculated in the standard many-body diagrammatic expansion up to the second order in EPI strength. We find that the multiple phonon-assisted Kondo satellites arise besides the usual Kondo resonance. In the antiparallel magnetic configuration the splitting of main Kondo peak and phonon-assisted satellites only happen for asymmetrical dot-lead couplings, but it is free from the symmetry for the parallel magnetic configuration. The EPI strength and vibrational frequency can enhance the spin splitting of both main Kondo and satellites. It is shown that the suppressed zero-bias Kondo resonance can be restored by applying an external magnetic field, whose magnitude is dependent on the phononic effect remarkably. Although the asymmetry in tunnel coupling has no contribution to the restoration of spin splitting of Kondo peak, it can shrink the external field needed to switch tunneling magnetoresistance ratio between large negative dip and large positive peak.