We develop a non-Markovian full counting statistics formalism taking into account both the sequential tunneling and cotunneling based on the exact particle number resolved time-convolutionless master equation and the Rayleigh-Schrödinger perturbation theory. Then, we study the influences of the quantum coherence and the cotunneling assisted sequential tunneling processes on the non-Markovian full counting statistics of electron tunneling through an open quantum system, which consists of a side-coupled double-quantum-dot molecule weakly coupled to two electron reservoirs. We demonstrate that in the sequential tunneling regime the competition or interplay between the quantum coherence and the cotunneling processes determines whether the super-Poissonian of the shot noise, the skewness and the kurtosis take place and whether the sign transitions of the values of the skewness and the kurtosis occur in the strong quantum-coherent side-coupled double-quantum-dot molecule. These results suggest that it is necessary to consider the effects of the quantum coherence and the cotunneling processes on the full counting statistics of electron tunneling through open strong quantum-coherent quantum systems in the sequential tunneling regime, which provide a deeper insight into understanding of electron tunneling through open quantum systems.
We describe a method for calculating the counting statistics of electronic transport through nanoscale devices with both sequential and cotunneling contributions. The method is based upon a perturbative expansion of the von Neumann equation in Liouvillian space, with current cumulants calculated from the resulting nonMarkovian master equation without further approximation. As application, we consider transport through a single quantum dot and discuss the effects of cotunneling on noise and skewness, as well as the properties of various approximation schemes.
Based on our recently developed quantum transport theory in term of an exact master equation, the corresponding particle-number resolved ($n$-resolved) master equation and the related shot noise spectrum formalism covering the full frequency range are constructed. We demonstrate that the noise spectra of transport current through single quantum dot and double quantum dots show characteristic steps and/or peak-dips in different tunneling frequency regimes through tuning the applied bias voltage and/or gate voltage at low temperatures. The peak-dips crossing the tunneling resonant frequencies is…
We develop a conceptually simple scheme based on a master-equation approach to evaluate the full-counting statistics (FCS) of elastic and inelastic off-resonant tunneling (cotunneling) in quantum dots (QDs) and molecules. We demonstrate the method by showing that it reproduces known results for the FCS and shot noise in the cotunneling regime. For a QD with an excited state, we obtain an analytic expression for the cumulant generating function (CGF) taking into account elastic and inelastic cotunneling. From the CGF we find that the shot noise above the inelastic threshold in the cotunneling r…
In the resonant tunneling regime sequential processes dominate single electron transport through quantum dots or molecules that are weakly coupled to macroscopic electrodes. In the Coulomb blockade regime, however, cotunneling processes dominate. Cotunneling is an inherently quantum phenomenon and thus gives rise to interesting observations, such as an increase in the current shot noise. Since cotunneling processes are inherently fast compared to the sequential processes, it is of interest to examine the short time behaviour of systems where cotunneling plays a role, and whether these systems …
We consider the theoretical description of real-time counting of electrons tunneling through a Coulomb-blockade quantum dot using a detector with finite bandwidth. By tracing out the quantum dot we find that the dynamics of the detector effectively is non-Markovian. We calculate the cumulant generating function corresponding to the resulting non-Markovian rate equation and find that the measured current cumulants behave significantly differently compared to those of a Markovian transport process. Our findings provide a novel interpretation of noise suppression found in a number of systems.
Full counting statistics of electron transport is a powerful diagnostic tool for probing the nature of quantum transport beyond what is obtainable from the average current or conductance measurement alone. In particular, the non-Markovian dynamics of quantum dot molecule plays an important role in the nonequilibrium electron tunneling processes. It is thus necessary to understand the non-Markovian full counting statistics in a quantum dot molecule. Here we study the non-Markovian full counting statistics in two typical quantum dot molecules, namely, serially coupled and side-coupled double qua…
Recent experimental progress has made it possible to detect in real-time single electrons tunneling through Coulomb blockade nanostructures, thereby allowing for precise measurements of the statistical distribution of the number of transferred charges, the so-called full counting statistics. These experimental advances call for a solid theoretical platform for equally accurate calculations of distribution functions and their cumulants. Here we develop a general framework for calculating zero-frequency current cumulants of arbitrary orders for transport through nanostructures with strong Coulom…
We present a hierarchical quantum master equation (HQME) approach, which allows the numerically exact evaluation of higher-order current cumulants in the framework of full counting statistics for nonequilibrium charge transport in nanosystems. The novel methodology is exemplarily applied to a model of vibrationally coupled electron transport in a molecular nanojunction. We investigate the influence of cotunneling on avalanche-like transport, in particular in the nonresonant transport regime, where we find that inelastic cotunneling acts as trigger process for resonant avalanches. In this regim…
We present a theory of full counting statistics for electron transport through interacting electron systems with non-Markovian dynamics. We illustrate our approach for transport through a single-level quantum dot and a metallic single-electron transistor to second order in the tunnel-coupling strength, and discuss under which circumstances non-Markovian effects appear in the transport properties.
We investigate theoretically the noise and the full counting statistics of electrons that are emitted from a superconductor into two spatially separated quantum dots by the splitting of Cooper pairs and further on collected in two normal-state electrodes. With negatively-biased drain electrodes and a large superconducting gap, the dynamics of the Cooper pair splitter can be described by a Markovian quantum master equation. Using techniques from full counting statistics, we evaluate the electrical currents, their noise power spectra, and the power-power correlations in the output leads. The cur…
Non-equilibrium transport properties of quantum systems have recently become experimentally accessible in a number of platforms in so-called full-counting experiments that measure transient and steady state non-equilibrium transport dynamics. We show that the effect of the measurement back-action can be exploited to gain access to relevant transport coefficients. This relationship is general, but becomes most conspicuous in the transient dynamics of open quantum systems understrong coupling to non-Markovian environments. In order to explore this regime, a new simulation method for the generati…
We present a theory of frequency-dependent counting statistics of electron transport through nanostructures within the framework of Markovian quantum master equations. Our method allows the calculation of finite-frequency current cumulants of arbitrary order, as we explicitly show for the second- and third-order cumulants. Our formulae generalize previous zero-frequency expressions in the literature and can be viewed as an extension of MacDonald's formula beyond shot noise. When combined with an appropriate treatment of tunneling, using, e.g. Liouvillian perturbation theory in Laplace space, o…
We discuss the description of full counting statistics in quantum transport with a nonMarkovian master equation. We focus on differences arising from whether charge is considered as a classical or a quantum degree of freedom. These differences manifest themselves in the inhomogeneous term of the master equation which describes initial correlations. We describe the influence on current and in particular, the finite-frequency shotnoise. We illustrate these ideas by studying transport through a quantum dot and give results that include both sequential and cotunneling processes. Importantly, the n…
We derive a general expression for the cumulant generating function (CGF) of non-Markovian quantum stochastic transport processes. The long-time limit of the CGF is determined by a single dominating pole of the resolvent of the memory kernel from which we extract the zero-frequency cumulants of the current using a recursive scheme. The finite-frequency noise is expressed not only in terms of the resolvent, but also initial system-environment correlations. As an illustrative example we consider electron transport through a dissipative double quantum dot for which we study the effects of dissipa…
We extend the second-order von Neumann approach within the generalized master equation formalism for quantum electronic transport to include the counting field. The resulting non-Markovian evolution equation for the reduced density matrix of the system resolved with respect to the number of transported charges enables the evaluation of the noise and higher-order cumulants of the full counting statistics. We apply this formalism to an analytically solvable model of a single-level quantum dot coupled to highly biased leads with Lorentzian energy-dependent tunnel coupling and demonstrate that, al…
Using a microscopic model for stochastic transport through a single quantum dot that is modified by the Coulomb interaction of environmental (weakly coupled) quantum dots, we derive generic properties of the full counting statistics for multi-stable Markovian transport systems. We study the temporal crossover from multi-modal to broad uni-modal distributions depending on the initial mixture, the long-term asymptotics and the divergence of the cumulants in the limit of a large number of transport branches. Our findings demonstrate that the counting statistics of a single resonant level may be u…
We develop a theory for the full counting statistics (FCS) for a class of nanoelectromechanical systems (NEMS), describable by a Markovian generalized master equation. The theory is applied to two specific examples of current interest: vibrating C60 molecules and quantum shuttles. We report a numerical evaluation of the first three cumulants for the C60-setup; for the quantum shuttle we use the third cumulant to substantiate that the giant enhancement in noise observed at the shuttling transition is due to a slow switching between two competing conduction channels. Especially the last example …
We present a theory of finite-frequency noise in non-equilibrium conductors. It is shown that Non-Markovian correlations are essential to describe the physics of quantum noise. In particular, we show the importance of a correct treatment of the initial system-bath correlations, and how these can be calculated using the formalism of quantum master equations. Our method is particularly important in interacting systems, and when the measured frequencies are larger that the temperature and applied voltage. In this regime, quantum-noise steps are expected in the power spectrum due to vacuum fluctua…
We investigate the current noise of a charge qubit coupled to a phonon bath in different parameter regimes. We find, using the theory of Full Counting Statistics of non-Markovian systems, that the current fluctuations are strongly influenced by memory effects generated from the interplay between quantum coherence and the dynamics of the phonon bath.
We develop a scheme for the computation of the full-counting statistics of transport described by Markovian master equations with an arbitrary time dependence. It is based on a hierarchy of generalized density operators, where the trace of each operator yields one cumulant. This direct relation offers a better numerical efficiency than the equivalent number-resolved master equation. The proposed method is particularly useful for conductors with an elaborate time-dependence stemming, e.g., from pulses or combinations of slow and fast parameter switching. As a test bench for the evaluation of th…
We formalize the derivation of a generalized coarse-graining $n$-resolved master equation by introducing a virtual detector counting the number of transferred charges in single-electron transport. Our approach enables the convenient inclusion of coherences and Lamb shift in counting statistics. As a Markovian example with Lindblad-type density matrices, we consider the Born-Markov-Secular (BMS) approximation which is a special case of the non-Markovian dynamical coarse graining (DCG) approach. For illustration we consider transport through two interacting levels that are either serially or par…
We formulate a full-counting statistics description to study energy exchange in multi-terminal junctions. Our approach applies to quantum systems that are coupled either additively or non-additively (cooperatively) to multiple reservoirs. We derive a Markovian Redfield-type equation for the counting-field dependent reduced density operator. Under the secular approximation, we confirm that the cumulant generating function satisfies the heat exchange fluctuation theorem. Our treatment thus respects the second law of thermodynamics. We exemplify our formalism on a multi-terminal two-level quantum…
In quantum transport through nanoscale devices, fluctuations arise from various sources: the discreteness of charge carriers, the statistical non-equilibrium that is required for device operation, and unavoidable quantum uncertainty. As experimental techniques have improved over the last decade, measurements of these fluctuations have become available.} They have been accompanied by a plethora of theoretical literature using many different fluctuation statistics to describe the quantum transport. In this paper, we overview three prominent fluctuation statistics: full counting, waiting time, an…
We investigate theoretically and experimentally the full counting statistics of bidirectional single-electron tunneling through a double quantum dot in a GaAs/GaAlAs heterostructure and compare with predictions of the fluctuation theorem (FT) for Markovian stochastic processes. We observe that the quantum point contact electrometer used to study the transport induces nonequilibrium shot noise and dot-level fluctuations and strongly modifies the tunneling statistics. As a result, the FT appears to be violated. We show that it is satisfied if the back-action of the electrometer is taken into acc…
We study electron pumping in the strong coupling and non-Markovian regime. Our model is a single quantum dot with periodically modulated energy and tunnelling amplitudes. We identify four parameters to control the direction of the current: the driving phase, the coupling strength, the driving frequency and the location of the maxima of the spectral density. In the high-frequency regime, we use a Markovian embedding strategy to map our model to three serial quantum dots weakly coupled to the reservoirs allowing us to use a Floquet master equation. We observe a rectification effect of the pumped…
We consider the counting statistics of electron transport through a double quantum dot with special emphasis on the dephasing induced by a nearby charge detector. The double dot is embedded in a dissipative enviroment, and the presence of electrons on the double dot is detected with a nearby quantum point contact. Charge transport through the double dot is governed by a non-Markovian generalized master equation. We describe how the cumulants of the current can be obtained for such problems, and investigate the difference between the dephasing mechanisms induced by the quantum point contact and…
We study Markovian stochastic motion on a graph with finite number of nodes and adiabatically periodically driven transition rates. We show that, under general conditions, the quantized currents that appear at low temperatures are a manifestation of topological invariants in the counting statistics of currents. This observation provides an approach for classification of topological properties of the counting statistics, as well as for extensions of the phenomenon of the robust quantization of currents at low temperatures to the properties of the counting statistics which persist to finite temp…
We develop and test a computational framework to study heat exchange in interacting, nonequilibrium open quantum systems. Our iterative full counting statistics path integral (iFCSPI) approach extends a previously well-established influence functional path integral method, by going beyond reduced system dynamics to provide the cumulant generating function of heat exchange. The method is straightforward; we implement it for the nonequilibrium spin boson model to calculate transient and long-time observables, focusing on the steady-state heat current flowing through the system under a temperatur…
Many molecular junctions display stochastic telegraphic switching between two distinct current values, which is therefore an important source of fluctuations in nanoscale quantum transport. We investigate electronic fluctuations arising via Markovian master equations; identifying regions of non-renewal behavior due to telegraphic switching. Non-renewal behavior is characterized by the emergence of correlations between successive first-passage times of detection in one of the leads. Our method of including telegraphic switching is general for any source-molecule-drain setup, but we consider thr…
Molecular electronics is a rapidly developing field focused on using molecules as the structural basis for electronic components. It is common in such devices for the system of interest to couple simultaneously to multiple environments. Here we consider a model comprised of a double quantum dot (or molecule) coupled strongly to vibrations and weakly to two electronic leads held at arbitrary bias voltage. The strong vibrational coupling invalidates treating the bosonic and electronic environments simply as acting additively, as would be the case in the weak coupling regime or for flat leads at …
We consider stochastic and open quantum systems with a finite number of states, where a stochastic transition between two specific states is monitored by a detector. The long-time counting statistics of the observed realizations of the transition, parametrized by cumulants, is the only available information about the system. We present an analytical method for reconstructing generators of the time evolution of the system compatible with the observations. The practicality of the reconstruction method is demonstrated by the examples of a laser-driven atom and the kinetics of enzyme-catalyzed rea…
We investigate the spin dynamics of a quantum dot with a spin-1/2 ground state in the Coulomb blockade regime and in the presence of a magnetic rf field leading to electron spin resonances (ESR). We show that by coupling the dot to leads, spin properties on the dot can be accessed via the charge current in the stationary and non-stationary limit. We present a microscopic derivation of the current and the master equation of the dot using superoperators, including contributions to decoherence and energy shifts due to the tunnel coupling. We give a detailed analysis of sequential and co-tunneling…
To investigate frequency-dependent current noise (FDCN) in open quantum systems at steady states, we present a theory which combines Markovian quantum master equations with a finite time full counting statistics. Our formulation of the FDCN generalizes previous zero-frequency expressions and can be viewed as an application of MacDonald's formula for electron transport to heat transfer. As a demonstration, we consider the paradigmatic example of quantum heat transfer in the context of a non-equilibrium spin-boson model. We adopt a recently developed polaron-transformed Redfield equation which a…
