The effect of electron-electron scattering on the equilibrium properties of few-electron quantum dots is investigated by means of nonequilibrium Green's functions theory. The ground and equilibrium state is self-consistently computed from the Matsubara (imaginary time) Green's function for the spatially inhomogeneous quantum dot system whose constituent charge carriers are treated as spin-polarized. To include correlations, the Dyson equation is solved, starting from a Hartree-Fock reference state, within a conserving (second order) self-energy approximation where direct and exchange contributions to the electron-electron interaction are included on the same footing.
We present results for the zero and finite temperature charge carrier density, the orbital-resolved distribution functions and the self-consistent total energies and spectral functions for isotropic, two-dimensional parabolic confinement as well as for the limit of large anisotropy--quasi-one-dimensional entrapment. For the considered quantum dots with N=2, 3 and 6 electrons, the analysis comprises the crossover from Fermi gas/liquid (at large carrier density) to Wigner molecule or crystal behavior (in the low-density limit).
We develop a mapping of quantum steady-state nonequilibrium to an effective equilibrium and solve the problem using a quantum simulation technique. A systematic implementation of the nonequilibrium boundary condition in steady-state is made in the electronic transport on quantum dot structures. This formulation of quantum manybody problem in nonequilibrium enables the use of existing numerical quantum manybody techniques. The algorithm coherently demonstrates various transport behaviors from phonon-dephasing to I-V staircase and phonon-assisted tunneling.
We extend a perturbative, nonequilibrium renormalization group approach to multi-orbital systems and apply it for studying transport through two parallel quantum dots coupled electrostatically. In general, the conductance shows pronounced Kondoesque peaks at three voltages. One of these peaks disappears if, as in some experiments, one of the dots is decoupled from one of the two leads. For an asymmetric coupling to the leads, also negative differential conductances are possible. This is a genuine nonequilibrium effect, accompanying the Kondoesque peaks. Moreover, a criterion to distinguish spi…
Double quantum dots can provide an experimental realization of the 2 impurity Kondo model which exhibits a non-Fermi liquid quantum critical point (QCP) at a special value of its parameters. We generalize our recent study of double quantum dots in series \cite{Sela08} to a parallel configuration with an Aharonov-Bohm flux. We present an exact universal result for the finite temperature and finite voltage conductance $G[V,T]$ along the crossover from the QCP to the low energy Fermi liquid phase. Compared to the series configuration, here generically $G[V,T] \ne G[-V,T]$, leading to current rect…
We study a pseudo-spin-1/2 quantum dot in the cotunneling regime close to the particle-hole symmetric point. For a generic tunneling matrix we find a generic fixed point with interesting nonequilibrium properties, characterized by effective reservoirs with compensating spin orientation vectors weighted by the polarizations and the tunneling rates. At large bias voltage we study the magnetic field dependence of the dot magnetization and the current. The fixed point can be clearly identified by analyzing the magnetization of the dot. We characterize in detail the universal properties for the cas…
The carrier generation in insulators subjected to strong electric fields is characterized by the Landau-Zener formula for the tunneling probability with a nonperturbative exponent. Despite its long history with diverse applications and extensions, study of nonequilibrium steady states and associated current response in the presence of the generated carriers has been mainly limited to numerical simulations so far. Here, we develop a framework to calculate the nonequilibrium Green's function of generic insulating systems under a DC electric field, in the presence of a fermionic reservoir. Using …
We study a double quantum dot in the regime where each dot carries a spin-1/2. This system is described by the 2-impurity Kondo model, having a non-Fermi liquid fixed point for a critical value of the inter-impurity coupling. The Hamiltonian describing the vicinity of the critical point, including the relevant potential scattering perturbations, can be cast in quadratic form. This allows us to predict a universal scaling function for the finite temperature nonlinear conductance along the crossover from the critical point to the surrounding stable fixed points.
A nonequilibrium Green's functions (NEGF) approach for spatially inhomogeneous, strongly correlated artificial atoms is presented and applied to compute the time-dependent properties while starting from a (correlated) initial few-electron state at finite temperatures. In the regime of moderate to strong coupling, we consider the Kohn mode of a three-electron system in a parabolic confinement excited by a short pulsed classical laser field treated in dipole approximation. In particular, we numerically confirm that this mode is preserved within a conserving (e.g. Hartree-Fock or second Born) the…
We present a theory of zero-bias anomalies and dephasing rates for a Coulomb-blockaded quantum dot, driven out of equilibrium by coupling to voltage biased source and drain leads. We interpret our results in terms of the statistics of voltage fluctuations in the system.
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.
Spin entanglement between two spatially separated electrons can be generated in nonequilibrium interacting quantum dots, coherently coupled to a common lead. In this system entangled two-electron states develop which are Werner states with an imbalance between singlet and triplet probabilities. We propose a multi-terminal, multiply-connected setup for the generation and detection of this imbalance. In particular, we identify a regime in which the formation of spin entanglement leads to a cancellation of Aharonov-Bohm oscillations.
We develop a low-energy nonequilibrium field theory for weakly interacting quantum dots. The theory is based on the Keldysh field integral in the spin channel of the quantum dot described by the single impurity Anderson Hamiltonian. The effective Keldysh action is a functional of the Hubbard-Stratonovich magnetization field decoupling the quantum dot spin channel. We expand this action up to the second order with respect to the magnetization field, which allows to describe nonequilibrium interacting quantum dots at low temperatures and weak electron-electron interactions,up to the contacts-dot…
Nonperturbative dynamic theory has a particular advantage in studying the transport in a quantum impurity system in a steady state. Here, we develop a new approach for obtaining the retarded Green's function expressed in resolvent form. We use the Heisenberg picture to facilitate dynamic theory and propose a new systematic method of collecting the basis vectors spanning the Liouville space, which is the most crucial step in obtaining the resolvent Green's function. We obtain all the linearly independent basis vectors for studying the single-impurity Anderson models with one and two reservoirs.…
We study the spin dynamics in charged quantum dots in the situation where the resident electron is coupled to only about 200 nuclear spins and where the electron spin splitting induced by the Overhauser field does not exceed markedly the spectral broadening. The formation of a dynamical nuclear polarization as well as its subsequent decay by the dipole-dipole interaction is directly resolved in time. Because not limited by intrinsic nonlinearities, almost complete nuclear polarization is achieved, even at elevated temperatures. The data suggest a nonequilibrium mode of nuclear polarization, di…
By nonperturbatively solving the nonequilibrium Anderson two-impurity model with the hierarchical equations of motion approach, we report a robust ferromagnetic (FM) phase in series-coupled double quantum dots, which can suppress the antiferromagnetic (AFM) phase and dominate the phase diagram at finite bias and detuning energy in the strongly correlated limit. The FM exchange interaction origins from the passive parallel spin arrangement caused by the Pauli exclusion principle during the electrons transport. At very low temperature, the Kondo screening of the magnetic moment in the FM phase i…
We report on capacitance-voltage spectroscopy of self-assembled InAs quantum dots under constant illumination. Besides the electronic and excitonic charging peaks in the spectrum reported earlier, we find additional resonances associated with nonequilibrium state tunneling unseen in C(V) measurements before. We derive a master-equation based model to assign the corresponding quantum state tunneling to the observed peaks. C(V) spectroscopy in a magnetic field is used to verify the model-assigned nonequilibrium peaks. The model is able to quantitatively address various experimental findings in C…
We present a unified transport theory of hybrid structures, in which a confined normal state ($N$) sample is sandwiched between two leads each of which can be either a ferromagnet ($F$) or a superconductor ($S$) via tunnel barriers. By introducing a four-dimensional Nambu-spinor space, a general current formula is derived within the Keldysh nonequilibrium Green function formalism, which can be applied to various kinds of hybrid mesoscopic systems with strong correlations even in the nonequilibrium situation. Such a formula is gauge invariant. We also demonstrate analytically for some quantitie…
We develop a theory for charge and spin current between two canted magnetic leads flowing through a quantum dot with an arbitrary local interaction. For a noncollinear magnetic configuration, we calculate equilibrium and nonequilibrium current biased by voltage or temperature difference or pumped by magnetic dynamics. We are able to explicitly separate the equilibrium and nonequilibrium contributions to the current, both of which can be written in terms of the full retarded Green's function on the dot. Taking the specific example of a single-level quantum dot with a large on-site Coulomb inter…
The nonequilibrium spectral properties of the Anderson impurity model with a chemical potential bias are investigated within a numerically exact real time quantum Monte Carlo formalism. The two-time correlation function is computed in a form suitable for nonequilibrium dynamical mean field calculations. Additionally, the evolution of the model's spectral properties are simulated in an alternative representation, defined by a hypothetical but experimentally realizable weakly coupled auxiliary lead. The voltage splitting of the Kondo peak is confirmed and the dynamics of its formation after a co…
We analyze the decoherence of charge states in double quantum dots due to cotunneling. The system is treated using the Bloch-Redfield generalized master equation for the Schrieffer-Wolff transformed Hamiltonian. We show that the decoherence, characterized through a relaxation $τ_{r}$ and a dephasing time $τ_ϕ$, can be controlled through the external voltage and that the optimum point, where these times are maximum, is not necessarily in equilibrium. We outline the mechanism of this nonequilibrium-induced enhancement of lifetime and coherence. We discuss the relevance of our results for recent …
We investigate the transient nonequilibrium dynamics of a molecular junction biased by a finite voltage and strongly coupled to internal vibrational degrees of freedom. Using two different, numerical exact techniques, diagrammatic Monte Carlo and the multilayer multiconfiguration time-dependent Hartree method, we show that the steady state current through the junction may depend sensitively on the initial preparation of the system, thus revealing signatures of bistability. The influence of the bias voltage and the transient dynamics on the phenomenon of bistability is analyzed. Furthermore, a …
We propose schemes for generating spatially-separated spin entanglement in systems of two quantum dots with onsite Coulomb repulsion weakly coupled to a joint electron reservoir. An enhanced probability for the formation of spin entanglement is found in nonequilibrium situations with one extra electron on each dot, either in the transient state after rapid changes of the gate voltage, or in the steady state with applied bias voltage. In both cases so-called Werner states with spin singlet fidelity exceeding 1/2 are generated, which indicates entanglement.
We have derived a variational principle that defines the nonequilibrium steady-state transport across a correlated impurity mimicking, e.g., a quantum dot coupled to biased leads. This variational principle has been specialized to a Gutzwiller's variational space, and applied to the study of the simple single-orbital Anderson impurity model at half filling, finding a good qualitative accord with the observed behavior in quantum dots for the expected regime of values of the bias. Beyond the purely theoretical interest in the formal definition of a variational principle in a nonequilibrium probl…
The optically induced polarization of localized electron spins in an ensemble of quantum dots (QDs) dephases due to the interaction with the surrounding nuclear spins. Despite this dephasing, the spins in the QDs can be controlled to respond coherently by applying periodic laser pulses, leading to a revival of the spin polarization before each pulse. This effect, known as spin mode locking, strongly depends on an emerging selection of certain polarizations of the nuclear spin bath which is driven to a steady state far from equilibrium. We investigate the influence of the nuclear composition in…
We develop a nonperturbative dynamical theory (NDT) to calculate the retarded Green's function under nonequilibrium conditions. The NDT is particularly useful for treating nonequilibrium transport problems in systems with strong correlation. We apply our NDT to the well-known single-impurity Anderson model at equilibrium to determine its feasibility. We then apply it to a nonequilibrium transport problem in a system with Kondo coupling. An Anderson model with two metallic reservoirs is studied to understand the phenomenon of Kondo-peak splitting in a single-electron transistor of mesoscopic si…
We introduce diagrammatic technique for Hubbard nonequilibrium Green functions (NEGF). The formulation is an extension of equilibrium considerations for strongly correlated lattice models to description of current carrying molecular junctions. Within the technique intra-system interactions are taken into account exactly, while molecular coupling to contacts is used as a small parameter in perturbative expansion. We demonstrate the viability of the approach with numerical simulations for a generic junction model of quantum dot coupled to two electron reservoirs.
We theoretically investigate the full time evolution of a nonequilibrium double quantum dot structure from initial conditions corresponding to different product states (no entanglement between dot and lead) to a nonequilibrium steady state. The structure is described by a two-level spinless Anderson model where the levels are coupled to two leads held at different chemical potentials. The problem is solved by a numerically exact hierarchical master equation technique and the results are compared to approximate ones obtained from Born-Markov theory. The methods allow us to study the time evolut…
Stationary electric transport in semiconductor nanostructures is studied by the method of nonequilibrium Green functions. In the case of sequential tunneling the results are compared with density matrix theory, providing almost identical results. Nevertheless, the method of Green functions is easier to handle due to the availability of an absolute energy scale. It is demonstrated, that the transport in complicated structures, like quantum cascade lasers, can be described in reasonable agreement with experiment.
We present a formulation of a nonequilibrium Green's function method for thermal current in nanojunction atomic systems with nonlinear interactions. This first-principle approach is applied to the calculation of the thermal conductance in carbon nanotube junctions. It is shown that nonlinearity already becomes important at low temperatures. Nonlinear interactions greatly suppress phonon transmission at room temperature. The peak of thermal conductance is found to be around 400K, in good agreement with experiments. High-order phonon scattering processes are important for diffusive heat transpor…
We investigate the effects of alternating voltage on nonequilibrium quantum systems with localised phonon modes. Nonequilibrium Green's functions are utilised, with electron-phonon coupling being considered with the $GD$ approximation (self-consistent Born approximation). Using a Floquet approach, we assume periodicity of the dynamics. This approach allows us to investigate the influence of the driven electronic component on the nonequilibrium occupation of the vibrations. It was found that signatures of inelastic transport gained photon-assisted peaks. A simplistic model was proposed and foun…
In this paper, spin-dependent transport through a spin diode composed of a quantum dot coupled to a normal metal and a ferromagnetic lead is studied. The current polarization and the spin accumulation are analyzed using the equations of motion method within the nonequilibrium Green's function formalism. We present a suitable method for computing Green's function without carrying out any self-consistent calculation. The influence of coupling strength and magnetic field on the spin current is studied and observed that this device cannot work as a spin diode under certain conditions.
A generalized Landauer formula, derived with the methods due to Keldysh, and Baym and Kadanoff, is gaining widespread use in the modeling of transport in a large number of different mesoscopic systems. We review some of the recent developments, including transport in semiconductor superlattices, calculation of noise, and nanoelectromechanical systems.
An open quantum system consists of leads connected to a device of interest. Within the nonequilibrium Green's function technique, we examine the replacement of leads by self-energies in continuum calculations. Our starting point is a formulation of the problem for continuum systems by T.E. Feuchtwang. In this approach there is considerable flexibility in the choice of unperturbed Green's functions. We examine the consequences of this freedom on the treatment of leads. For any choice the leads can be replaced by coupling self-energies which are simple functions of energy. We find that the retar…
Recent developments on studies of transport through quantum dots obtained by applying the time-dependent density matrix renormalization group method are summarized. Some new aspects of Kondo physics which appear in nonequilibrium steady states are discussed both for the single dot case and for the serially coupled double-quantum-dot case.
Large-scale simulations of the spin dynamics in quantum dots subjected to trains of periodic laser pulses enable us to describe and understand related experiments. By comparing the data for different models to experimental results, we gain an improved understanding of the relevant physical mechanisms. Using sophisticated numerical approaches and an efficient implementation combined with extrapolation arguments, nonequilibrium stationary states are reached for parameter ranges close to the ones in real experiments. With the help of high performance computing, we can tune the experimental parame…
Here we address two nonequilibrium Green's functions approaches for a resonant tunneling structure under a sudden switch of a bias. Our aim is to stress that the time-dependent Keldysh formulation of Jauho, Wingreen and Meir, and the partition-free scheme of Stefanucci and Almbladh are formally equivalent in the ubiquitous case of wide-band limit and noninteracting electrons, if leads and dot are in equilibrium before the time-dependent perturbation. We develop explicit closed formulas of the lesser Green's function and time-dependent current, reminding that the different integration limits pr…
Nonequilibrium Green's functions provide a powerful tool for computing the dynamical response and particle exchange statistics of coupled quantum systems. We formulate the theory in terms of the density matrix in Liouville space and introduce superoperator algebra that greatly simplifies the derivation and the physical interpretation of all quantities. Expressions for various observables are derived directly in real time in terms of superoperator nonequilibrium Green's functions (SNGF), rather than the artificial time-loop required in Schwinger's Hilbert-space formulation. Applications for com…
We give nonequilibrium Green's function (NEGF) perspective on thermodynamics formulations for open quantum systems strongly coupled to baths. Scattering approach implying thermodynamic consideration of a super-system (system plus baths) weakly coupled to external super-baths is compared with consideration of thermodynamics of a system strongly coupled to its baths. We analyze both approaches from the NEGF perspective and argue that the latter yields a possibility of thermodynamic formulation consistent with dynamical (quantum transport) description.
Double quantum dots are one of the promising two-state quantum systems for realizing qubits. In the quest of successfully manipulating and reading information in qubit systems, it is of prime interest to control the charge response of the system to a gate voltage, as filled in by the dynamical charge susceptibility. We theoretically study this quantity for a nonequilibrium double quantum dot by using the functional integral approach and derive its general analytical expression. One highlights the existence of two lines of maxima as a function of the dot level energies, each of them being split…
We present a theory of molecular motors based on the Ehrenfest dynamics for the nuclear coordinates and the adiabatic limit of the Kadanoff-Baym equations for the current-induced forces. Electron-electron interactions can be systematically included through many-body perturbation theory, making the nonequilibrium Green's functions formulation suitable for first-principles treatments of realistic junctions. The method is benchmarked against simulations via real-time Kadanoff-Baym equations, finding an excellent agreement. Results on a paradigmatic model of molecular motor show that correlations …
We develop a non-equilibrium theory to describe weak Coulomb blockade effects in open quantum dots. Working within the bosonized description of electrons in the point contacts, we expose deficiencies in earlier applications of this method, and address them using a 1/N expansion in the inverse number of channels. At leading order this yields the self-consistent potential for the charging interaction. Coulomb blockade effects arise as quantum corrections to transport at the next order. Our approach unifies the phase functional and bosonization approaches to the problem, as well as providing a si…
We study the nonlinear elastic quantum electronic transport properties of nanoscopic devices using the Nonequilibrium Green's function (NEGF) method. The Green's function method allows us to expand the $I-V$ characteristics of a given device to arbitrary powers of the applied voltages. By doing so, we are able to relate the NEGF method to the scattering approach, showing their similarities and differences and calculate the conductance coefficients to arbitrary order. We demonstrate that the electronic current given by NEGF is gauge invariant to all orders in powers of $V$, and discuss the requ…
We present a microscopic theory for both equilibrium and nonequilibrium transport properties of coupled double quantum dots (DQD). A general formula for current tunneling through the DQD is derived by the nonequilibrium Green's function method. Using a Hartree-Fock approach, effects of multi-level coupling and nonequilibrium electron distributions in resonant tunneling are considered. We find that the peak in the resonant tunneling current through two symmetric dots will split only when the inter-dot coupling is stronger than dot-lead coupling. We predict that population inversion can be achie…
Orbital Kondo effect in a system of two single-level quantum dots attached to external electron reservoirs is considered theoretically. The dots are coupled via direct hoping term and Coulomb interaction. The Kondo temperature is evaluated from the scaling approach and slave boson technique. The later method is also used to calculate linear conductance of the system. Nonlinear conductance, in turn, is calculated in terms of the nonequilibrium Green function formalism.
Time-dependent nonequilibrium Green's functions (TDNEGF) are shown to provide a flexible, effective tool for the description of quantum mechanical single particle scattering on a spatially localized, time-dependent potential. Focusing on numerical methods, arbitrary space and time dependence of the potential can be treated, provided it is zero before an initial time instant. In this case, appropriate version of the Dyson and Keldysh equations lead to a transparent description with clear physical interpretation. The interaction of a short laser pulse and an electron propagating initially in fre…
We develop a perturbative renormalization-group method in real time to describe nonequilibrium properties of discrete quantum systems coupled linearly to an environment. We include energy broadening and dissipation and develop a cutoff-independent formalism. We present quantitatively reliable results for the nonlinear conductance in the mixed-valence and empty-orbital regime of the nonequilibrium Anderson impurity model with finite on-site Coulomb repulsion.
The role of multimode vibrational dynamics in electron transport through single molecule junctions is investigated. The study is based on a generic model, which describes charge transport through a single molecule that is attached to metal leads. To address vibrationally-coupled electron transport, we employ a nonequilibrium Green's function approach that extends a method recently proposed by Galperin et al. [Phys. Rev. B 73, 045314 (2006)] to multiple vibrational modes. The methodology is applied to two systems: a generic model with two vibrational degrees of freedom and benzenedibutanethiola…
Excitonic contributions to absorption and photocurrent generation in semiconductor nanostructures are described theoretically and simulated numerically using steady-state non-equilibrium Green's function theory. In a first approach, the coherent interband polarization including Coulomb corrections is determined from a Bethe-Salpeter-type equation for the equal time interband single-particle charge carrier Green's function. The effects of excitonic absorption on photocurrent generation are considered on the same level of approximation via the derivation of the corresponding corrections to the e…
This paper is devoted to the study and interpretation of the spectral function $\mathbf{A}(ω, T)$ of the Keldysh nonequilibrium Green's function. The spatial diagonal of the spectral function is often interpreted as a time-dependent local density of states. We show that this object can take negative values implying that a simple probability interpretation as a time-dependent density of states is not possible. The same issue also occurs for the Wigner function $P(x,p)$ where it is solved by taking the uncertainty principle into account. We follow the same path and incorporate the time-energy un…
We review a recent theoretical development based on non-equilibrium Green's function formalism to study heat transport in nanomechanical devices modeled by phononic systems of coupled quantum oscillators driven by ac forces and connected to phononic reservoirs. We present the relevant equations to calculate the heat currents flowing along different regions of the setup, as well as the power developed by the time-dependent forces. We also present different strategies to evaluate the Green's functions exactly or approximately within the weak driving regime. We finally discuss the different mecha…
We consider optical spectroscopy of molecular junctions from the quantum transport perspective when radiation field is quantized and optical response of the system is simulated as photon flux. Using exact expressions for photon and electronic fluxes derived within the nonequilibrium Green function (NEGF) methodology and utilizing fourth order diagrammatic perturbation theory in molecular coupling to radiation field we perform simulations employing realistic parameters. Results of the simulations are compared to the bare perturbation theory (PT) usually employed in studies on nonlinear optical …
Due to random dopant fluctuations, the device-to-device variability is a serious challenge to emerging nanoelectronics. In this work we present theoretical formalisms and numerical simulations of quantum transport variability, based on the nonequilibrium Green's functions and the multiple scattering theory. We have developed a general formalism using the diagrammatic technique within the coherent potential approximation (CPA) that can be applied to a wide range of disorder concentrations. In addition, we have developed a method by using a perturbative expansion within the low concentration app…
Quantum tunneling dominates coherent transport at low temperatures in many systems of great interest. In this work we report a many--body tunneling (MBT), by nonperturbatively solving the Anderson multi-impurity model, and identify it a fundamental tunneling process on top of the well--acknowledged sequential tunneling and cotunneling. We show that the MBT involves the dynamics of doublons in strongly correlated systems. Proportional to the numbers of dynamical doublons, the MBT can dominate the off--resonant transport in the strongly correlated regime. A $T^{3/2}$--dependence of the MBT curre…
We analyze the quantum interference effects appearing in the charge current through the double quantum dots coupled in T-shape configuration to an isotropic superconductor and metallic lead. Owing to proximity effect the quantum dots inherit a pairing which has the profound influence on nonequilibrium charge transport, especially in the subgap regime |eV| < Delta. We discuss under what conditions the Fano-type lineshapes might appear in such Andreev conductance and consider a possible interplay with the strong correlation effects.
The interplay between interference effects and electron-electron interactions in electron transport through an interacting double quantum dot system is investigated using a hierarchical quantum master equation approach which becomes exact if carried to infinite order and converges well if the temperature is not too low. Decoherence due to electron-electron interactions is found to give rise to pronounced negative differential resistance, enhanced broadening of structures in current-voltage characteristics and an inversion of the electronic population. Dependence on gate voltage is shown to be …
