arXiv subjects

Daniel S. Kosov

Publications and source records attributed to Daniel S. Kosov.

At least 37 records · Page 2Linked to original sources

arXiv2019

Fluctuating-time and full counting statistics for quantum transport in a system with internal telegraphic noise

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 three specific cases. In the first, we model stochastic transitions between an Anderson impurity with and without an applied magnetic field $B$. The last two scenarios couple the electronic level to a single vibrational mode via the Holstein model. We then stochastically switch between two vibrational conformations, with different electron-phonon coupling and vibrational frequency, which corresponds to different molecular conformations. Finally, we model the molecule attaching and detaching from an electrode by switching between two different molecule-electrode coupling strengths. We find, for all three cases, that including the telegraph process in the master equation induces relatively strong positive correlations, with Pearson coefficient $p \approx 0.5$, between successive first-passage times. These correlations only appear, however, when there is telegraphic switching between two significantly different transport scenarios, and we show that it arises from the underlying physics of the model. We also find that, in order for correlations to appear, the switching rate $ν$ must be much smaller than the rate of electron transfer $γ$.

cond-mat.mes-hall↗

arXiv2019

Counting quantum jumps: a summary and comparison of fixed-time and fluctuating-time statistics in electron transport

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, and first-passage time statistics. We discuss their weaknesses and strengths, and explain connections between them in terms of renewal theory. In particular, we discuss how different information can be encoded in different statistics when the transport is non-renewal, and how this behavior manifests in the measured physical quantities of open quantum systems. All theoretical results are illustrated via a demonstrative transport scenario: a Markovian master equation for a molecular electronic junction with electron-phonon interactions. {{} We demonstrate that to obtain non-renewal behavior, and thus to have temporal correlations between successive electron tunneling events, there must be a strong coupling between tunneling electrons and out-of-equilibrium quantized molecular vibrations.

cond-mat.mes-hall↗

arXiv2019

Non-renewal statistics in quantum transport through the eyes of first-passage and waiting time distributions

The waiting time distribution has, in recent years, proven to be a useful statistical tool for characterising transport in nanoscale quantum transport. In particular, as opposed to moments of the distribution of transferred charge, which have historically been calculated in the long-time limit, waiting times are able to detect non-renewal behaviour in mesoscopic systems. They have failed, however, to correctly incorporate backtunneling events. Recently, a method has been developed that can describe unidirectional and bidirectional transport on an equal footing: the distribution of first-passage times. Rather than the time between successive electron tunnelings, the first-passage refers to the first time the number of extra electrons in the drain reaches $+1$. Here, we demonstrate the differences between first-passage time statistics and waiting time statistics in transport scenarios where the waiting time either cannot correctly reproduce the higher order current cumulants or cannot be calculated at all. To this end, we examine electron transport through a molecule coupled to two macroscopic metal electrodes. We model the molecule with strong electron-electron and electron-phonon interactions in three regimes: (i) sequential tunneling and cotunneling for a finite bias voltage through the Anderson model, (ii) sequential tunneling with no temperature gradient and a bias voltage through the Holstein model, and (iii) sequential tunneling at zero bias voltage and a temperature gradient through the Holstein model. We show that, for each transport scenario, backtunneling events play a significant role; consequently, the waiting time statistics do not correctly predict the renewal and non-renewal behaviour, whereas the first-passage time distribution does.

cond-mat.mes-hall↗

arXiv2019

Non-equilibrium Green's function theory for non-adiabatic effects in quantum transport: inclusion of electron-electron interactions

Non-equilibrium Green's function theory for non-adiabatic effects in quantum transport [Kershaw and Kosov, J.Chem. Phys. 2017, 147, 224109 and J. Chem. Phys. 2018, 149, 044121] is extended to the case of interacting electrons. We consider a general problem of quantum transport of interacting electrons through a central region with dynamically changing geometry. The approach is based on the separation of time scales in the non-equilibrium Green's functions and the use of Wigner transformation to solve the Kadanoff-Baym equations. The Green's functions and correlation self-energy are non-adiabatically expanded up to the second order central time derivatives. We produced expressions for Green's functions with non-adiabatic corrections and modified formula for electric current; both depend not only on instantaneous molecular junction geometry but also on nuclear velocities and accelerations. The theory is illustrated by the study of electron transport through a model single-resonant level molecular junction with local electron-electron repulsion and a dynamically changing geometry.

cond-mat.mes-hall↗

arXiv2018

Distribution of waiting times between electron cotunnelings

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 display nonrenewal statistics. We consider three questions in this paper. Given that an electron has tunneled from the source to the drain via a cotunneling or sequential process, what is the waiting time until another electron cotunnels from the source to the drain? What are the statistical properties of these waiting time intervals? How does cotunneling affect the statistical properties of a system with strong inelastic electron-electron interactions? In answering these questions, we extend the existing formalism for waiting time distributions in single electron transport to include cotunneling processes via an $n$-resolved Markovian master equation. We demonstrate that for a single resonant level the analytic waiting time distribution including cotunneling processes yields information on individual tunneling amplitudes. For both a SRL and an Anderson impurity deep in the Coulomb blockade there is a nonzero probability for two electrons to cotunnel to the drain with zero waiting time inbetween. Furthermore, we show that at high voltages cotunneling processes slightly modify the nonrenewal behaviour of an Anderson impurity with a strong inelastic electron-electron interaction.

cond-mat.mes-hall↗

arXiv2018

Waiting time between charging and discharging processes in molecular junctions

When electric current flows through a molecular junction, the molecule constantly charges and discharges by tunnelling electrons. These charging and discharging events occur at specific but random times and separated by stochastic time intervals. These time intervals can be associated with dwelling time for a charge (electron or hole) to reside on the molecule. In this paper, the statistical properties of these time intervals are studied and general formula for their distribution is derived. The theory is based on the Markovian master equation which takes into account transitions between vibrational states of charged and neutral molecule in the junction. Two quantum jump operators are identified from the Liouvillian of the master equation - one corresponds to charging of the molecule and the other discharges the molecule back to neutral state. The quantum jump operators define the conditional probability that given that the molecule was charged by a tunneling electron at time $t$, the molecule becomes neutral at later time $t+τ$ discharging the electron to the drain electrode. Statistical properties of these time intervals $τ$ are studied with the use of this distribution.

cond-mat.mes-hall↗

arXiv2018

Nonadiabatic corrections to electric current in molecular junction due to nuclear motion at the molecule-electrode interfaces

We present quantum electron transport theory that incorporates dynamical effects of motion of atoms on electrode-molecule interfaces in the calculations of the electric current. The theory is based on non-equilibrium Green's functions. We separate time scales in the Green's functions on fast relative time and slow central time. The derivative with respect to the central time serves as a small parameter in the theory. We solve the real-time Kadanoff-Baym equations for molecular Green's functions using Wigner representation and keep terms up to the second order with respect to the central time derivatives. Molecular Green's functions and consequently the electric current are expressed as functions of molecular junction coordinates as well as velocities and accelerations of molecule-electrode interface nuclei. We apply the theory to model a molecular system and study the effects of non-adiabatic nuclear motion on molecular junction conductivity.

cond-mat.mes-hall↗

arXiv2018

Telegraph noise in Markovian master equation for electron transport through molecular junctions

We present a theoretical approach to solve Markovian master equation for quantum transport with stochastic telegraph noise. Considering probabilities as functionals of a random telegraph process we use the Novikov's functional method to convert stochastic master equation to a set of deterministic differential equations. The equations are then solved in the Laplace space and the expression for the probability vector averaged over ensemble of realisations of stochastic process is obtained. We apply the theory to study manifestations of telegraph noise in transport properties of molecular junctions. We consider the quantum electron transport in a resonant-level molecule as well as polaronic regime transport in a molecular junction with electron-vibration interaction.

cond-mat.mes-hall↗

arXiv2017

Nonequilibrium Green's function theory for nonadiabatic effects in quantum electron transport

We develop nonequilibribrium Green's function based transport theory, which includes effects of nonadiabatic nuclear motion in the calculation of the electric current in molecular junctions. Our approach is based on the separation of slow and fast timescales in the equations of motion for the Green's functions by means of the Wigner representation. Time derivatives with respect to central time serves as a small parameter in the perturbative expansion enabling the computation of nonadiabatic corrections to molecular Green's functions. Consequently, we produce series of analytic expressions for non-adiabatic electronic Green's functions (up to the second order in the central time derivatives); which depend not solely on instantaneous molecular geometry but likewise on nuclear velocities and accelerations. Extended formula for electric current is derived which accounts for the non-adiabatic corrections. This theory is concisely illustrated by the calculations on a model molecular junction.

cond-mat.mes-hall↗

arXiv2017

Restoring the Pauli principle in the random phase approximation ground state

Random phase approximation ground state contains electronic configurations where two (and more) identical electrons can occupy the same molecular spin-orbital violating the Pauli exclusion principle. This overcounting of electronic configurations happens due to quasiboson approximation in the treatment of electron-hole pair operators. We describe the method to restore the Pauli principle in the RPA wavefunction. The proposed theory is illustrated by the calculations of molecular dipole moments and electronic kinetic energies. The Hartree-Fock based RPA, which is corrected for the Pauli principle, gives the results of comparable accuracy with Møller-Plesset second order perturbation theory and coupled-cluster singles and doubles method.

physics.chem-ph↗

arXiv2017

Non-renewal statistics for electron transport in a molecular junction with electron-vibration interaction

Quantum transport of electrons through a molecule is a series of individual electron tunnelling events separated by stochastic waiting time intervals. We study the emergence of temporal correlations between successive waiting times for the electron transport in a vibrating molecular junction. Using master equation approach, we compute joint probability distribution for waiting times of two successive tunnelling events. We show that the probability distribution is completely reset after each tunnelling event if molecular vibrations are thermally equilibrated. If we treat vibrational dynamics exactly without imposing the equilibration constraint, the statistics of electron tunnelling events become non-renewal. Non-renewal statistics between two waiting times $τ_1$ and $τ_2$ means that the density matrix of the molecule is not fully renewed after time $τ_1$ and the probability of observing waiting time $τ_2$ for the second electron transfer depends on the previous electron waiting time $τ_1$. The strong electron-vibration coupling is required for the emergence of the non-renewal statistics. We show that in Franck-Condon blockade regime the extremely rare tunnelling events become positively correlated.

cond-mat.mes-hall↗

arXiv2017

Expectation values of single-particle operators in the random phase approximation ground state

We developed a method for computing matrix elements of single-particle operators in the correlated random phase approximation ground state. Working with the explicit random phase approximation ground state wavefunction, we derived practically useful and simple expression for a molecular property in terms of random phase approximation amplitudes. The theory is illustrated by the calculation of molecular dipole moments for a set of representative molecules.

physics.chem-ph↗

arXiv2016

Waiting time distribution for electron transport in a molecular junction with electron-vibration interaction

On the elementary level, electronic current consists of individual electron tunnelling events that are separated by random time intervals. The waiting time distribution is a probability to observe the electron transfer in the detector electrode at time $t+τ$ given that an electron was detected in the same electrode at earlier time $t$. We study waiting time distribution for quantum transport in a vibrating molecular junction. By treating the electron-vibration interaction exactly and molecule-electrode coupling perturbatively, we obtain master equation and compute the distribution of waiting times for electron transport. The details of waiting time distributions are used to elucidate microscopic mechanism of electron transport and the role of electron-vibration interactions. We find that as nonequilibrium develops in molecular junction, the skewness and dispersion of the waiting time distribution experience stepwise drops with the increase of the electric current. These steps are associated with the excitations of vibrational states by tunnelling electrons. In the strong electron-vibration coupling regime, the dispersion decrease dominates over all other changes in the waiting time distribution as the molecular junction departs far away from the equilibrium.

cond-mat.mes-hall↗

arXiv2016

Distribution of residence times as a marker to distinguish different pathways for quantum transport

Electron transport through a nanoscale system is an inherently stochastic quantum mechanical process. Electric current is a time series of electron tunnelling events separated by random intervals. Thermal and quantum noise are two sources of this randomness. In this paper, we used the quantum master equation to consider the following questions: (i) Given that an electron has tunnelled into the electronically unoccupied system from the source electrode at some particular time, how long is it until an electron tunnels out to the drain electrode to leave the system electronically unoccupied, where there were no intermediate tunnelling events ("the" tunnelling path)? (ii) Given that an electron has tunnelled into the unoccupied system from the source electrode at some particular time, how long is it until an electron tunnels out to the drain electrode to leave the system electronically unoccupied, where there were no intermediate tunnelling events ("an" tunnelling path)? (iii) What are the distributions of these times? We show that electron correlations suppress the difference between "the" and "an" electron tunnelling paths.

cond-mat.mes-hall↗

arXiv2016

Linear Response Theory for Symmetry Improved Two Particle Irreducible Effective Actions

We investigate the linear response of an O(N) scalar quantum field theory subject to external perturbations using the symmetry improved two particle irreducible effective action formalism [A. Pilaftsis and D. Teresi, Nucl. Phys. B874, 594 (2013)]. Despite satisfactory equilibrium behavior, we find a number of unphysical effects at the linear response level. Goldstone boson field fluctuations are over-determined, with the only consistent solution being to set the fluctuations and their driving sources to zero, except for momentum modes where the Higgs and Goldstone self-energies obey a particular relationship. Also Higgs field fluctuations propagate masslessly, despite the Higgs propagator having the correct mass. These pathologies are independent of any truncation of the effective action and still exist even if we relax the over-determining Ward identities, so long as the constraint is formulated O(N)-covariantly. We discuss possible reasons for the apparent incompatibility of the constraints and linear response approximation and possible ways forward.

hep-th↗

arXiv2014

Adsorption and ring-opening of lactide on a chiral metal surface studied by Density Functional Theory

We study the adsorption and ring-opening of lactide on the naturally chiral metal surface Pt(321)$^S$. Lactide is a precursor for polylactic acid ring-opening polymerization and Pt is a well known catalyst surface. We study here the energetics of the ring-opening of lactide on a surface that has a high density of kink atoms. These sites are expected to be present on a realistic Pt surface and show enhanced catalytic activity. The use of a naturally chiral surface also enables us to study potential chiral selectivity effects of the reaction at the same time. Using Density Functional Theory (DFT) with a functional that includes the van der Waals forces in a first-principles manner, we find modest adsorption energies of around 1.4 eV for the pristine molecule and different ring-opened states. The energy barrier to be overcome in the ring-opening reaction is found to be very small at 0.32 eV and 0.30 eV for LL- and its chiral partner DD-lactide, respectively. These energies are much smaller than the activation energy for a dehydrogenation reaction of 0.78 eV. Our results thus indicate that (a) ring-opening reactions of lactide on Pt(321) can be expected already at very low temperatures and Pt might be a very effective catalyst for this reaction; (b) the ring-opening reaction rate shows noticeable enantioselectivity.

cond-mat.mtrl-sci↗

arXiv2013

Out-of-equilibrium one-dimensional disordered dipole chain

We consider a chain of one-dimensional dipole moments connected to two thermal baths with different temperatures. The system is in nonequilibrium steady state and heat flows through it. Assuming that fluctuation of the dipole moment is a small parameter, we develop an analytically solvable model for the problem. The effect of disorder is introduced by randomizing the positions of the dipole moments. We show that the disorder leads to Anderson-like transition from conducting to a thermal insulating state of the chain. It is shown that considered chain supports both ballistic and diffusive heat transports depending on the strength of the disorder. We demonstrate that nonequilibrium leads to the emergence of the long-range order between dipoles along the chain and make the conjecture that the interplay between nonequilibrium and next-to-nearest-neighbor interactions results in the emergence of long-range correlations in low-dimensional classical systems.

cond-mat.stat-mech↗

arXiv2013

Out-of-equilibrium catalysis of chemical reactions by electronic tunnel currents

We present an escape rate theory for current-induced chemical reactions. We use Keldysh nonequilibrium Green's functions to derive a Langevin equation for the reaction coordinate. Due to the out of equilibrium electronic degrees of freedom, the friction, noise, and effective temperature in the Langevin equation depend locally on the reaction coordinate. As an example, we consider the dissociation of diatomic molecules induced by the electronic current from a scanning tunnelling microscope tip. In the resonant tunnelling regime, the molecular dissociation involves two processes which are intricately interconnected: a modification of the potential energy barrier and heating of the molecule. The decrease of the molecular barrier (i.e. the current induced catalytic reduction of the barrier) accompanied by the appearance of the effective, reaction-coordinate-dependent temperature is an alternative mechanism for current-induced chemical reactions, which is distinctly different from the usual paradigm of pumping vibrational degrees of freedom.

cond-mat.mes-hall↗