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Kondo Physics and Many-Body Effects in Quantum Dots and Molecular Junctions

David A. Ruiz‐Tijerina

Published Jan 1, 2013• 0 citations
OpenAlex

Abstract

In this document we present a study of the thermodynamic and transport properties of two kinds of quantum impurity systems in the Kondo regime.The first system consists of a spin-1 molecule in which mechanical stretching along the transport axis produces a magnetic anisotropy.We find that a generic coupling between a vibrational mode along this axis and the molecular spin induces a correction to the magnetic anisotropy, driving the ground state of the system into a non-Fermi-liquid phase.A transition into a Fermi-liquid ground state can then be induced by means of stretching, going through an underscreened spin-1 Kondo ground state at zero effective anisotropy.In the second system we study the effects of a charge detector, implemented by a quantum point-contact (QPC), on the Kondo state of a nearby spin-1/2 quantum dot (QD).While making the charge detection possible, the Coulomb interaction between the electrons traversing the QPC and those within the QD contribute to decoherence of the Kondo state.By modeling the QPC as two metallic terminals connected to an intermediate localized level, we can explore three transport regimes of the detector: a zero-conductance regime, a finite-conductance regime in mixed valence, and unitary conductance in a Kondo ground state that has been suggested as an explanation to the "0.7 anomaly" in QPCs.Transitions between these different ground states can be achieved by tuning the strength of a capacitive coupling that parameterizes the electrostatic interaction.

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•Jan 1, 2011•0 citations
In this document we present a study of the thermodynamic and transport properties of two kinds of quantum impurity systems in the Kondo regime.The first system consists of a spin-1 molecule in which mechanical stretching along the transport axis produces a magnetic anisotropy.We find that a generic coupling between a vibrational mode along this axis and the molecular spin induces a correction to the magnetic anisotropy, driving the ground state of the system into a non-Fermi-liquid phase.A transition into a Fermi-liquid ground state can then be induced by means of stretching, going through an underscreened spin-1 Kondo ground state at zero effective anisotropy.In the second system we study the effects of a charge detector, implemented by a quantum point-contact (QPC), on the Kondo state of a nearby spin-1/2 quantum dot (QD).While making the charge detection possible, the Coulomb interaction between the electrons traversing the QPC and those within the QD contribute to decoherence of the Kondo state.By modeling the QPC as two metallic terminals connected to an intermediate localized level, we can explore three transport regimes of the detector: a zero-conductance regime, a finite-conductance regime in mixed valence, and unitary conductance in a Kondo ground state that has been suggested as an explanation to the "0.7 anomaly" in QPCs.Transitions between these different ground states can be achieved by tuning the strength of a capacitive coupling that parameterizes the electrostatic interaction.
We present a study of the correlated transport regimes of a double quantum impurity system with mutual capacitive interactions. Such system can be implemented by a double quantum dot arrangement or by a quantum dot and nearby quantum point contact, with independently connected sets of metallic terminals. Many-body spin correlations arising within each dot-lead subsystem give rise to the Kondo effect under appropriate conditions. The otherwise independent Kondo ground states may be modified by the capacitive coupling, decisively modifying the ground state of the double quantum impurity system. We analyze this coupled system through variational methods and the numerical renormalization group technique. Our results reveal a strong dependence of the coupled system ground state on the electron-hole asymmetries of the individual subsystems, as well as on their hybridization strengths to the respective reservoirs. The electrostatic repulsion produced by the capacitive coupling produces an effective shift of the individual energy levels toward higher energies, with a stronger effect on the ``shallower'' subsystem (that closer to resonance with the Fermi level), potentially pushing it out of the Kondo regime and dramatically changing the transport properties of the system. The effective remote gating that this entails is found to depend nonlinearly on the capacitive coupling strength, as well as on the independent subsystem levels. The analysis we present here of this mutual interaction should be important to fully characterize transport through such coupled systems.
We study correlated two-level quantum dots, coupled in effective one-channel fashion to metallic leads, with electron interactions including on-level and interlevel Coulomb repulsions, as well as the interorbital Hund's rule exchange favoring the spin-1 state in the relevant sector of the free dot. For arbitrary dot occupancy, the underlying phases, quantum phase transitions (QPTs), thermodynamics, single-particle dynamics, and electronic transport properties are considered, and direct comparison is made to conductance experiments on lateral quantum dots. Two distinct phases arise generically, one characterized by a normal Fermi liquid fixed point (FP) and the other by an underscreened (USC) spin-1 FP. Associated QPTs, which occur in general in a mixed valent regime of nonintegral dot charge, are found to consist of continuous lines of Kosterlitz-Thouless transitions, separated by first-order level-crossing transitions at high symmetry points. A ``Friedel-Luttinger sum rule'' is derived and, together with a deduced generalization of Luttinger's theorem to the USC phase (a singular Fermi liquid), is used to obtain a general result for the T=0T=0T=0 zero-bias conductance, expressed solely in terms of the dot occupancy and applicable to both phases. Relatedly, dynamical signatures of the QPT show two broad classes of behavior, corresponding to the collapse of either a Kondo resonance, or antiresonance, as the transition is approached from the Fermi liquid phase, the latter behavior being apparent in experimental differential conductance maps. The problem is studied using the numerical renormalization group method, combined with analytical arguments.
This thesis contributes to the understanding of impurity models. It is divided into two main parts, with a general introduction given in Part I and the research related to it presented in Part II, with the second part being subdivided into two main projects. In the first project, the influence of two many-body effects, the Kondo effect and the Fermi edge singularity, on the absorption and emission spectra of self-assembled quantum dots (QDs) is examined. Whereas the Kondo effect so far was always examined with transport experiments, we show that it has been observed with optical methods for the first time, by comparing experimental data for the absorption line shapes of QDs to calculations with the numerical renormalization group. We continue by examining a QD with strong optical coupling of the energy levels. The resulting interplay of Rabi-oscillations and Kondo effect leads to a new many-body state, a secondary, outer Kondo effect, with Kondo-like correlations between the spin-Kondo and the trion state. The last work regarding optics at QDs addresses the Fermi edge singularity. We show that for QDs this phenomenon can be described numerically on a quantitative level. The second project concerns transport properties of impurity models. First, we present a comprehensive study of the Kondo effect for an InAs-nanowire QD, a system for which the Kondo effect was observed only a few years ago. The second study regarding transport concerns the Kondo effect in bulk metals with magnetic impurities. Although nowadays the Kondo effect is often studied with QDs, it was discovered for iron impurities in noble metals like gold and silver. However, it was unknown for a long time which exact realization of Kondo model describes these systems. We identify the model by comparing numerical calculations for the magnetoresistivity and the dephasing rate for different models to experimental results. The third work about transport concerns the phenomenon that for a fixed type of Kondo model quantities like the magnetoresistivity or the conductivity, respectively, can be scaled onto a universal curve for different parameters, when energies are rescaled with the the Kondo temperature TKT_KTK​, since it is the only relevant low energy scale of the problem. For finite bandwidth, however, different definitions of TKT_KTK​ (which coincide in the limit of infinite bandwidth) lead to different TKT_KTK​-values. We show that with a very common definition of TKT_KTK​, finite bandwidth, which is always present at numerical calculations, can deteriorate the universality of rescaled curves, and we offer an alternative definition of TKT_KTK​ which ensures proper scaling. In the last study presented in this thesis we calculate the Fermi-liquid coefficients for fully screened multi-channel Kondo models. For temperatures below TKT_KTK​, these models show Fermi-liquid behavior, and the impurity density of states and certain quantities which depend on it, like resistivity, show quadratic dependencies on parameters like temperature or magnetic field, described by the Fermi-liquid coefficients. We calculate these coefficients both analytically and numerically.
The numerical renormalization group is employed to study a double quantum (DQD) dot system consisting of two equivalent single-level dots, each coupled to its own lead and with a mutual capacitive coupling embodied in an interdot interaction U', in addition to the intradot Coulomb interaction U. We focus on the regime with two electrons on the DQD, and the evolution of the system on increasing U'/U. The spin-Kondo effect arising for U'=0 (SU(2) x SU(2)) is found to persist robustly with increasing U'/U, before a rapid but continuous crossover to (a) the SU(4) point U'=U where charge and spin degrees of freedom are entangled and the Kondo scale strongly enhanced; and then (b) a charge-Kondo state, in which a charge-pseudospin is quenched on coupling to the leads/conduction channels. A quantum phase transition of Kosterlitz-Thouless type then occurs from this Fermi liquid, strong coupling (SC) phase, to a broken symmetry, non-Fermi liquid charge ordered (CO) phase at a critical U'_c. Our emphasis in this paper is on the structure, stability and flows between the underlying RG fixed points, on the overall phase diagram in the (U,U')-plane and evolution of the characteristic low-energy Kondo scale inherent to the SC phase; and on static physical properties such as spin- and charge-susceptibilities (staggered and uniform), including universality and scaling behaviour in the strongly correlated regime. Some exact results for associated Wilson ratios are also obtained.
Abstract. The numerical renormalization group is employed to study a double quantum (DQD) dot system consisting of two equivalent single-level dots, each coupled to its own lead and with a mutual capacitive coupling embodied in an interdot interaction U ′, in addition to the intradot Coulomb interaction U. We focus on the regime with two electrons on the DQD, and the evolution of the system on increasing U ′/U. The spin-Kondo effect arising for U ′ = 0 (SU(2) × SU(2)) is found to persist robustly with increasing U ′/U, before a rapid but continuous crossover to (a) the SU(4) point U ′ = U where charge and spin degrees of freedom are entangled and the Kondo scale strongly enhanced; and then (b) a charge-Kondo state, in which a charge-pseudospin is quenched on coupling to the leads/conduction channels. A quantum phase transition of Kosterlitz-Thouless type then occurs from this Fermi liquid, strong coupling (SC) phase, to a broken symmetry, non-Fermi liquid charge ordered (CO) phase at a critical U ′ c. Our emphasis in this paper is on the structure, stability and flows between the underlying RG fixed points, on the overall phase diagram in the (U, U ′)-plane and evolution of the characteristic low-energy Kondo scale inherent to the SC phase; and on static physical properties such as spin- and charge-susceptibilities (staggered and uniform), including universality and scaling behaviour in the strongly correlated regime. Some exact results for associated Wilson ratios are also obtained.
The first topic of this thesis is the study of many-body effects in an one-dimensional strongly correlated electronic system - the Kondo lattice model. This system is tackled numerically by means of the density matrix renormalization group, since analytic method, i.e., perturbation the- ory fail due to competing coupling constants. The Kondo lattice model consists of a conduction band of electrons which couple via a spin exchange coupling to a localized spin lattice. We study the spectral properties of the one-dimensional Kondo lattice model as a function of the exchange coupling, the band filling, and the quasimomentum in the ferromagnetic and paramagnetic phases. We compute the dispersion relation of the quasiparticles, their lifetimes, and the Z factor. The exact ground state and the quasiparticle-dispersion relation of the Kondo lattice model with one conduction electron are well known. The quasiparticle could be identified as the spin polaron. Our calculations of the dispersion relation for partial band fillings give a result similar to the one-electron case, which suggests that the quasiparticle in both cases is the spin polaron. We find that the quasiparticle lifetime differs by orders of magnitude between the ferromagnetic and paramagnetic phases and depends strongly on the quasimomentum. Further- more, we study the effects of the Coulomb interaction on the phase diagram, the static magnetic susceptibility and electron spin relaxation. We show that onsite Coulomb interaction supports ferromagnetic order and nearest neighbor Coulomb interaction drives, depending on the elec- tron filling, either a paramagnetic or ferromagnetic order. Furthermore, we calculate electron quasiparticle life times, which can be related to electron spin relaxation and decoherence times, and explain their dependence on the strength of interactions and the electron filling in order to find the sweet spot of parameters where the relaxation time is maximized. We find that effective exchange processes between the electrons dominate the spin relaxation and decoherence rate. In the second topic of this thesis, we numerically calculate the electron transport through carbon nanotube based quantum dot devices. We use a master equation’s approach in first order of the tunneling rate to the leads and an extended constant interaction model to model the carbon nanotube system. This work has been done in collaboration with two experimental groups and we compare their respective experimentally obtained data to our numerical calculations. In both collaborations striking similarity between the numerical data and the experimental data is found. In the first collaboration transport through a carbon nanotube peapod, i.e, a carbon nanotube filled with fullerenes, has been measured. We identify a small hybridization between a fullerene molecule and the surrounding carbon nanotube to be of crucial importance for the understanding of the transport data. In the second collaboration, electron transport through a carbon nanotube rope, i.e., a bundle of carbon nanotubes has been measured. Also here, hybridization between the different nanotubes plays a crucial role. Furthermore, an external magnetic field is applied, which enables the identification of specific spin states of the compound quantum dot system. This might be important for future applications of such devices in spin-dependent electronics.