Simulation of nonequilibrium spin dynamics in quantum dots subjected to periodic laser pulses
Philipp Schering, Philipp W. Scherer, Götz S. Uhrig
备注:
Preprint of the following chapter: P. Schering, P.W. Scherer, and G.S. Uhrig, "Simulation of Nonequilibrium Spin Dynamics in Quantum Dots Subjected to Periodic Laser Pulses", published in High Performance Computing in Science and Engineering '20, edited by W.E. Nagel, D.H. Kröner, and M.M. Resch, 2021, Springer, Cham. Final authenticated version: https://doi.org/10.1007/978-3-030-80602-6_8
发表信息:
High Performance Computing in Science and Engineering '20, pp. 115-131 (2021)
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 parameters to guide future experimental research. Importantly, our simulations reveal the possibility of resonant spin amplification in Faraday geometry, i.e., when a longitudinal magnetic field is applied to the quantum dots.
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 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 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…
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 …
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 have developed a theory of the one-phonon intraband resonance Raman scattering (IRRS) in anisotropic quantum dots subjected to an arbitrarily directed magnetic field. The differential Raman cross section is obtained. The resonance structure of the Raman cross section is studied. It is shown that the quantum dot subjected in a magnetic field can be used as the detector of phonon modes. The interesting multiplet structure of the resonance peaks is studied.
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…
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 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 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 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 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 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…
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.
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 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.
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…
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…
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 …
We study a $3$-level quantum dot in the singly occupied cotunneling regime coupled via a generic tunneling matrix to several multi-channel leads in equilibrium or nonequilibrium. We derive an effective model where also each reservoir has three channels labelled by the quark flavors $u$, $d$ and $s$ with an effective d.o.s. polarized w.r.t. an eight-dimensional $F$-spin corresponding to the eight generators of $SU(3)$. In equilibrium we perform a standard poor man scaling analysis and show that tunneling via virtual intermediate states induces flavor fluctuations on the dot which become $SU(3)$…
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 spin noise in singly charged self-assembled quantum dots is studied theoretically and experimentally under the influence of a perturbation, provided by additional photoexcited charge carriers. The theoretical description takes into account generation and relaxation of charge carriers in the quantum dot system. The spin noise is measured under application of above barrier excitation for which the data are well reproduced by the developed model. Our analysis demonstrates a strong difference of the recharging dynamics for holes and electrons in quantum dots.
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.
Nonequilibrium molecular dynamics simulations is used to study the motion of a C60 molecule on a graphene sheet subjected to a temperature gradient. The C60 molecule is actuated and moves along the system while it just randomly dances along the perpendicular direction. Increasing the temperature gradient increases the directed velocity of C60. It is found that the free energy decreases as the C60 molecule moves toward the cold end. The driving mechanism based on the temperature gradient suggests the construction of nanoscale graphene-based motors.
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 contribut…
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…
We present graphene quantum dots endowed with addition energies as large as 1.6 eV, fabricated by the controlled rupture of a graphene sheet subjected to a large electron current in air. The size of the quantum dot islands is estimated to be in the 1 nm range. The large addition energies allow for Coulomb blockade at room temperature, with possible application to single-electron devices.
In moderately strong magnetic fields, the difference in Lande g-factors in each of the dots of a coupled double quantum dot device may induce oscillations between singlet and triplet states of the entangled electron pair and lead to a nonequilibrium electron spin polarization. We will show that this polarization may partially survive the rapid inhomogeneous decoherence due to random nuclear magnetic fields.
Time-dependent driving influences the quantum and thermodynamic fluctuations of a system, changing the familiar physical picture of electronic noise which is an important source of information the about microscopic mechanism of quantum transport. Giving access to all cumulants of the current, the full counting statistics (FCS) is the powerful theoretical method to study fluctuations in nonequilibrium quantum systems. In this paper, we propose the application of FCS to consider periodic driven junctions. The combination of Floquet theory for time dynamics and nonequilibrium counting-field Green…
We present a formalism for studying the behaviour of quantum systems coupled to nonequilibrium environments exhibiting nonGaussian fluctuations. We discuss the role of a qubit as a detector of the statistics of environmental fluctuations, as well as nonMarkovian effects in both weak and strong coupling limits. We also discuss the differences between the influences of classical and quantum environments. As examples of the application of this formalism we study the dephasing and relaxation of a charge qubit coupled to nonequillibrium electron transport through single and double quantum dots.
We study electronic and optical properties of single layer phosphorene quantum dots with various shapes, sizes, and edge types (including disordered edges) subjected to an external electric field normal to the structure plane. Compared to graphene quantum dots, in phosphorene clusters of similar shape and size there is a set of edge states with energies dispersed at around the Fermi level. These states make the majority of phosphorene quantum dots metallic and enrich the phosphorene absorption gap with low-energy absorption peaks tunable by the electric field. The presence of the edge states d…
We report the inclusion of phonon scattering to our recently established numerical package QmeQ for transport in quantum dot systems. This enables straightforward calculations for a large variety of devices. As examples we show (i) transport in a double-dot structure, where energy relaxation is crucial to match the energy difference between the levels, and (ii) the generation of electrical power by contacting cold electric contacts with quantum dot states, which are subjected to heated phonons.
We present a simple technique to fabricate graphene quantum dots in a cryostat. It relies upon the controlled rupture of a suspended graphene sheet subjected to the application of a large electron current. This results in the in-situ formation of a clean and ultra-narrow constriction, which hosts one quantum dot, and occasionally a few quantum dots in series. Conductance spectroscopy indicates that individual quantum dots can possess an addition energy as large as 180 meV and a level spacing as large as 25 meV. Our technique has several assets: (i) the dot is suspended, thus the electrostatic …
The dynamics of low energy charge carriers in a graphene quantum dot subjected to a time-dependent local field is investigated numerically. In particular, we study a configuration where a Coulomb electric field is provided by an ion traversing the graphene sample. A Galerkin-like numerical scheme is introduced to solve the massless Dirac equation describing charge carriers subjected to space- and time-dependent electromagnetic potentials and is used to evaluate the field induced interband transitions. It is demonstrated that as the ion goes through graphene, electron-hole pairs are generated d…
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…
A theoretical investigation has been made of the magnetoplasmon excitations in a quasi-one-dimensional electron system comprised of vertically stacked, self-assembled InAs/GaAs quantum dots. The smaller length scales involved in the experiments impel us to consider a perfectly periodic system of two-dimensionally confined InAs quantum dot layers separated by GaAs spacers. Subsequent system is subjected to a two-dimensional confining (harmonic) potential in the x-y plane and an applied magnetic field (B) in the symmetric gauge. This scheme defines virtually a system of quantum wire comprised of…
We investigate the influence of the Coulomb interaction on the adiabatic pumping current through quantum dots. Using nonequilibrium Green's functions techniques, we derive a general expression for the current based on the instantaneous Green's function of the dot. We apply this formula to study the dependence of the charge pumped per cycle on the time-dependent pumping potentials. The possibility of charge quantization in the presence of a finite Coulomb repulsion energy is investigated in the light of recent experiments.
We study the quantum transport and the nonequilibrium vibrational states of a quantum dot embedded between a normal and a superconducting lead with the charge on the quantum dot linearly coupled to a harmonic oscillator of frequency $ω$. To the leading order in the charge-vibration interaction, we calculate the current and the nonequilibrium phonon occupation by the Keldsyh Green's function technique. We analyze the inelastic, vibration-assisted tunneling processes in the regime $ω<Δ$, with the superconducting energy gap $Δ$, and for sharp resonant transmission through the dot. When the energy…
We investigate quantum photovoltaic effect in double quantum dots by applying nonequilibrium quantum master equation. The drastic suppression of the photovoltaic current is observed near the open circuit voltage, which leads to the large filling factor. We find that there always exists an optimal inter-dot tunneling that significantly enhances the photovoltaic current. The maximal output power will also be obtained around the optimal inter-dot tunneling. Moreover, the open circuit voltage approximately behaves as the product of the eigen-level gap and the Carnot efficiency. These results sugge…
In the present work, we theoretically study the nonlinear regime of charge transport through a quantum dot coupled to the source and drain reservoirs. The investigation is carried out using a nonequilibrium Green's functions formalism beyond the Hartree-Fock approximation. Employed approximations for the relevant Green's functions allow to trace a transition from Coulomb blockade regime to Kondo regime in the thermoelectric transport. Effects arising when electrons move in response to thermal gradient applied across the system are discussed, including experimentally observed thermovoltage zero…
We show that nonequilibrium spin fluctuations significantly influence the electronic transport in a single-electron transistor, when the spin relaxation on the island is slow compared to other relaxation processes, and when size effects play a role. To describe spin fluctuations we generalize the `orthodox' tunneling theory to take into account the electron spin, and show that the transition between consecutive charge states can occur via a high-spin state. This significantly modifies the shape of Coulomb steps and gives rise to additional resonances at low temperatures. Recently some of our p…
We derive the quantum rate equations for an Aharonov-Bohm interferometer with two vertically coupled quantum dots embedded in each of two arms by means of the nonequilibrium Green's function in the sequential tunneling regime. Basing on these equations, we investigate time-dependent resonant tunneling under a small amplitude irradiation and find that the resonant photon-assisted tunneling peaks in photocurrent demonstrate a combination behavior of Fano and Lorentzian resonances due to the interference effect between the two pathways in this parallel configuration, which is controllable by thre…
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.
We develop an iterative, numerically exact approach for the treatment of nonequilibrium quantum transport and dissipation problems that avoids the real-time sign problem associated with standard Monte Carlo techniques. The method requires a well-defined decorrelation time of the non-local influence functional for proper convergence to the exact limit. Since finite decorrelation times may arise either from temperature or from a voltage drop at zero temperature, the approach is well suited for the description of the real-time dynamics of single-molecule devices and quantum dots driven to a stead…
We have studied the electronic properties and optical absorption spectra of three different cases of donor centers, D^{0}, D^{-} and D^{2-}, which are subjected to a perpendicular magnetic field, using the exact diagonalization method. The energies of the lowest lying states are obtained as function of the applied magnetic field strength B and the distance zeta between the positive ion and the confinement xy-plane. Our calculations indicate that the positive ion induces transitions in the ground-state, which can be observed clearly in the absorption spectra, but as zeta goes to 0 the strength …
We study the nonequilibrium spin current through a quantum dot consisting of two localized spin-1/2 coupled to two ferromagnetic insulators. The influence of an intra-dot magnetic field and exchange coupling, different dot-reservoir coupling configurations, and the influence of magnon chemical potential differences vs. magnetic field gradients onto the spin current are examined. We discuss various spin switching mechanisms and find that, in contrast to electronic transport, the spin current is very sensitive to the specific coupling configuration and band edges. In particular, we identify 1- a…
We study numerically the optical properties of low-buckled silicene and AB-stacked bilayer graphene quantum dots subjected to an external electric field, which is normal to their surface. Within the tight-binding model, the optical absorption is calculated for quantum dots, of triangular and hexagonal shapes, with zigzag and armchair edge terminations. We show that in triangular silicene clusters with zigzag edges a rich and widely tunable infrared absorption peak structure originates from transitions involving zero energy states. The edge of absorption in silicene quantum dots undergoes red s…
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.
We address the electronic properties of quantum dots in the two-dimensional $α-\mathcal{T}_3$ lattice when subjected to a perpendicular magnetic field. Implementing an infinite mass boundary condition, we first solve the eigenvalue problem for an isolated quantum dot in the low-energy, long-wavelength approximation where the system is described by an effective Dirac-like Hamiltonian that interpolates between the graphene (pseudospin 1/2) and Dice (pseudospin 1) limits. Results are compared to a full numerical (finite-mass) tight-binding lattice calculation. In a second step we analyse charge t…
We analyze the effect of Coulomb interaction on the noise of electric current through an open quantum dot. We demonstrate that the ensemble average value of the noise power acquires an interaction correction even for a dot coupled to the leads by reflectionless point contacts, when the ensemble average conductance is known to have no interaction corrections. To leading order, the correction to the noise originates from the formation of a nonequilibrium state of the Coulomb field describing the interaction between electrons. We find the dependence of the current noise power on the electron temp…
Using the Keldysh nonequilibrium Green function technique, we study the current and shot noise spectroscopy of a single molecular quantum dot coupled to a local phonon mode. It is found that in the presence of electron-phonon coupling, in addition to the resonant peak associated with the single level of the dot, satellite peaks with the separation set by the frequency of phonon mode appear in the differential conductance. In the ``single level'' resonant tunneling region, the differential shot noise power exhibit two split peaks. However, only single peaks show up in the ``phonon assisted'' re…