arXiv subjects

D. S. Kosov

Publications and source records attributed to D. S. Kosov.

At least 19 recordsLinked to original sources

arXiv2016

Distribution of waiting times between superoperator quantum jumps in Lindblad dynamics

Time-evolution of open, dissipative quantum system is a stochastic process that consists of a series of quantum jumps that take place at random times. Between quantum jumps quantum system idles for some time in a particular quantum state. Based on superfermion/superboson formalism and general Kossakowski- Lindblad master equation for an open quantum system we develop a method to compute distribution of waiting times between quantum jumps. We illustrate the use of the theory by computing waiting time distribution for model Fermi-system in thermodynamic equilibrium.

cond-mat.stat-mech↗

arXiv2014

Chiral selectivity of amino acid adsorption on chiral surfaces - the case of alanine on Pt

We study the binding pattern of the amino acid alanine on the naturally chiral Pt surfaces Pt(531), Pt(321) and Pt(643). These surfaces are all vicinal to the {111} direction but have different local environments of their kink sites and are thus a model for realistic roughened Pt surfaces. Alanine has only a single methyl group attached to its chiral center, which makes the number of possible binding conformations computationally tractable. Additionally, only the amine and carboxyl group are expected to interact strongly with the Pt substrate. On Pt(531) we study the molecule in its pristine as well as its deprotonated form and find that the deprotonated one is more stable by 0.39 eV. Therefore, we study the molecule in its deprotonated form on Pt(321) and Pt(643). As expected, the oxygen and nitrogen atoms of the deprotonated molecule provide a local binding "tripod" and the most stable adsorption configurations optimize the interaction of this "tripod" with undercoordinated surface atoms. However, the interaction of the methyl group plays an important role: it induces significant chiral selectivity of about 60 meV on all surfaces. Hereby, the L-enantiomer adsorbs preferentially to the Pt(321)$^S$ and Pt(643)$^S$ surfaces while the D-enantiomer is more stable on Pt(531)$^S$. The binding energies increase with increasing surface density of kink sites, i.e. they are largest for Pt(531)$^S$ and smallest for Pt(643)$^S$.

cond-mat.mtrl-sci↗

arXiv2014

Superoperator coupled cluster method for nonequilibrium density matrix

We develop a superoperator coupled cluster method for nonequilibrium open many-body quantum systems described by the Lindblad master equation. The method is universal and applicable to systems of interacting fermions, bosons or their mixtures. We present a general theory and consider its application to the problem of quantum transport through the system with electron-phonon correlations. The results are assessed against the perturbation theory and nonequilibrium configuration interaction theory calculations.

cond-mat.stat-mech↗

arXiv2014

Nonequilibrium configuration interaction method for transport in correlated quantum systems

We present a new approach to treat correlations in nonequilibrium quantum many-particle system. The method is based on ideas of configuration interaction theory of exact nonperturbative ground state electronic structure calculations. We use superoperator techniques in Liouville-Fock space and represent the nonequilibrium density matrix as a linear combination of all possible nonequilibrium quasiparticle excitations built on the appropriate reference state. As an example we consider the electron transport through the system with electron-phonon interaction. The concept of embedding (buffer zones between the reservoirs and the correlated quantum system) is used to derive an exact master equation for the reduced density matrix. Using approximate (truncated) expansion of the trial density matrix we obtain the linear system of equations for two-quasiparticle amplitudes. Then we compute the steady-state current and compare the result with other approaches. The current conserving property of the method is proved.

cond-mat.mes-hall↗

arXiv2013

Enantioselectivity of (321) chiral noble metal surfaces: A Density Functional Theory study of lactate adsorption

The adsorption of the chiral molecule lactate on the intrinsically chiral noble metal surfaces Pt(321), Au(321) and Ag(321) is studied by Density Functional Theory calculations. We use the oPBE-vdW functional which includes van der Waals forces on an ab initio level. It is shown that the molecule binds via its carboxyl and the hydroxyl oxygen atoms to the surface. The binding energy is larger on Pt(321) and Ag(321) than on Au(321). An analysis of the contributions to the binding energy of the different molecular functional groups reveals that the deprotonated carboxyl group contributes most to the binding energy, with a much smaller contribution of the hydroxyl group. The Pt(321) surface shows considerable enantioselectivity of 0.06 eV. On Au(321) and Ag(321) it is much smaller if not vanishing. The chiral selectivity of the Pt(321) surface can be explained by two factors. First, it derives from the difference in van der Waals attraction of L- and D-lactate to the surface that we trace to differences in the binding energy of the methyl group. Second, the multi-point binding pattern for lactate on the Pt(321) surface is sterically more sensitive to surface chirality and also leads to large binding energy contributions of the hydroxyl group. We also calculate the charge transfer to the molecule and the work function to gauge changes in electronic structure of the adsorbed molecule. The work function is lowered by 0.8 eV on Pt(321) with much smaller changes on Au(321) and Ag(321).

cond-mat.mtrl-sci↗

arXiv2012

Nonequilibrium perturbation theory in Liouville-Fock space for inelastic electron transport

We use a superoperator representation of the quantum kinetic equation to develop nonequilibrium perturbation theory for an inelastic electron current through a quantum dot. We derive a Lindblad-type kinetic equation for an embedded quantum dot (i.e. a quantum dot connected to Lindblad dissipators through a buffer zone). The kinetic equation is converted to non-Hermitian field theory in Liouville-Fock space. The general nonequilibrium many-body perturbation theory is developed and applied to the quantum dot with electron-vibronic and electron-electron interactions. Our perturbation theory becomes equivalent to a Keldysh nonequilibrium Green's function perturbative treatment provided that the buffer zone is large enough to alleviate the problems associated with approximations of the Lindblad kinetic equation.

cond-mat.mes-hall↗

arXiv2012

Solvent induced current-voltage hysteresis and negative differential resistance in molecular junctions

We consider a single molecule circuit embedded into solvent. The Born dielectric solvation model is combined with Keldysh nonequilibrium Green's functions to describe the electron transport properties of the system. Depending on the dielectric constant, the solvent induces multiple nonequilibrium steady states with corresponding hysteresis in molecular current-voltage characteristics as well as negative differential resistance. We identify the physical range of solvent and molecular parameters where the effects are present. The position of the negative differential resistance peak can be controlled by the dielectric constant of the solvent.

cond-mat.mes-hall↗

arXiv2011

Stability analysis of multiple nonequilibrium fixed points in self-consistent electron transport calculations

We present a method to perform stability analysis of nonequilibrium fixed points appearing in self-consistent electron transport calculations. The nonequilibrium fixed points are given by the self-consistent solution of stationary, nonlinear kinetic equation for single-particle density matrix. We obtain the stability matrix by linearizing the kinetic equation around the fixed points and analyze the real part of its spectrum to assess the asymptotic time behavior of the fixed points. We derive expressions for the stability matrices within Hartree-Fock and linear response adiabatic time-dependent density functional theory. The stability analysis of multiple fixed points is performed within the nonequilibrium Hartree-Fock approximation for the electron transport through a molecule with a spin-degenerate single level with local Coulomb interaction.

cond-mat.mes-hall↗

arXiv2011

Kramers problem for nonequilibrium current-induced chemical reactions

We discuss the use of tunneling electron current to control and catalyze chemical reactions. Assuming the separation of time scales for electronic and nuclear dynamics we employ the Langevin equation for the reaction coordinate. The Langevin equation contains current-induced forces and is used to define nonequilibrium, effective potential energy surface for current-carrying molecular systems. The current-induced forces are computed via Keldysh nonequilibrium Green's functions. Once the nonequilibrium, current-depended potential energy surface is defined, the chemical reaction is modeled as an escape of a Brownian particle from the potential well. We demonstrate that the barrier between the reactant and the product states can be controlled by the bias voltage. When the molecule is asymmetrically coupled to the electrodes, the reaction can be catalyzed or stopped depending on the polarity of the tunneling current.

cond-mat.mes-hall↗

arXiv2011

Second-order post-Hartree-Fock perturbation theory for the electron current

Based on the super-fermion representation of quantum kinetic equations we develop nonequilibrium, post-Hartree-Fock many-body perturbation theory for the current through a region of interacting electrons. We apply the theory to out of equilibrium Anderson model and discuss practical implementation of the approach. Our calculations show that nonequilibrium electronic correlations may produce significant quantitative and qualitative corrections to mean-field electronic transport properties. We find that the nonequilibrium leads to enhancement of electronic correlations.

cond-mat.mes-hall↗

arXiv2011

Super-fermion representation of the Lindblad master equation for the electron transport problem

We discuss the use of super-fermion formalism to represent and solve quantum kinetic equations for the electron transport problem. Starting with the Lindblad master equation for the molecule connected to two metal electrodes, we convert the problem of finding the nonequilibrium steady state to the many-body problem with non-Hermitian Liouvillian in super-Fock space. We transform the Liouvillian to the normal ordered form, introduce nonequilibrium quasiparticles by a set of canonical nonunitary transformations and develop general many-body theory for the electron transport through the interacting region. The approach is applied to the electron transport through a single level. We consider a minimal basis hydrogen atom attached to two metal leads in Coulomb blockade regime (out of equilibrium Anderson model) within the nonequilibrium Hartree-Fock approximation as an example of the system with electron interaction. Our approach agrees with exact results given by the Landauer theory for the considered models.

cond-mat.mes-hall↗

arXiv2009

Nonequilibrium Fock space for the electron transport problem

Based on the formalism of thermo field dynamics we propose a concept of nonequilibrium Fock space and nonequilibrium quasiparticles for quantum many-body system in nonequilibrium steady state. We develop a general theory as well as demonstrate the utility of the approach on the example of electron transport through the interacting region. The proposed approach is compatible with advanced methods of electronic structure calculations such as coupled cluster theory and configuration interaction.

cond-mat.stat-mech↗

arXiv2009

Asymptotic non-equilibrium steady state operators

We present a method for the calculation of asymptotic operators for nonequilibrium steady-state quantum systems. The asymptotic steady-state operator is obtained by averaging the corresponding operator in Heisenberg representation over infinitely long time. Several examples are considered to demonstrate the utility of our method. The results obtained within our approach are compared to those obtained within the Schwinger-Keldysh nonequilibrium Green's functions.

cond-mat.stat-mech↗

arXiv2009

Calculation of semiclassical free energy differences along non-equilibrium classical trajectories

We have derived several relations, which allow the evaluation of the system free energy changes in the leading order in $\hbar^{2}$ along classically generated trajectories. The results are formulated in terms of purely classical Hamiltonians and trajectories, so that semiclassical partition functions can be computed, e.g., via classical molecular dynamics simulations. The Hamiltonians, however, contain additional potential-energy terms, which are proportional to $\hbar^{2}$ and are temperature-dependent. We discussed the influence of quantum interference on the nonequilibrium work and problems with unambiguous definition of the semiclassical work operator.

cond-mat.stat-mech↗

arXiv2009

Microscopic origin of the jump diffusion model

The present paper is aimed at studying the microscopic origin of the jump diffusion. Starting from the $N$-body Liouville equation and making only the assumption that molecular reorientation is overdamped, we derive and solve the new (hereafter generalized diffusion) equation. This is the most general equation which governs orientational relaxation of an equilibrium molecular ensemble in the hindered rotation limit and in the long time limit. The generalized diffusion equation is an extension of the small-angle diffusion equation beyond the impact approximation. We establish the conditions under which the generalized diffusion equation can be identified with the jump diffusion equation, and also discuss the similarities and differences between the two approaches.

cond-mat.stat-mech↗

arXiv2008

A unified approach to the derivation of work theorems for equilibrium and steady-state, classical and quantum Hamiltonian systems

We present a unified and simple method for deriving work theorems for classical and quantum Hamiltonian systems, both under equilibrium conditions and in a steady state. Throughout the paper, we adopt the partitioning of the total Hamiltonian into the system part, the bath part, and their coupling. We rederive many equalities which are available in the literature and obtain a number of new equalities for nonequilibrium classical and quantum systems. Our results can be useful for determining partition functions and (generalized) free energies through simulations and/or measurements performed on nonequilibrium systems.

cond-mat.stat-mech↗

arXiv2008

Calculations of canonical averages from the grand canonical ensemble

Grand canonical and canonical ensembles become equivalent in the thermodynamic limit, but when the system size is finite the results obtained in the two ensembles deviate from each other. In many important cases, the canonical ensemble provides an appropriate physical description but it is often much easier to perform the calculations in the corresponding grand canonical ensemble. We present a method to compute averages in canonical ensemble based on calculations of the expectation values in grand canonical ensemble. The number of particles, which is fixed in the canonical ensemble, is not necessarily the same as the average number of particles in the grand canonical ensemble.

cond-mat.stat-mech↗

arXiv2007

Directed motion and useful work from an isotropic nonequilibrium distribution

We demonstrate that a gas of classical particles trapped in an external asymmetric potential undergoes a quasiperiodic motion, if the temperature of its initial velocity distribution $T_{ne}$ differs from the equilibrium temperature, $T_{eq}$. The magnitude of the effect is determined by the value of $T_{ne}-T_{eq}$, and the direction of the motion is determined by the sign of this expression. The "loading'' and "unloading'' of the gas particles change directions of their motion, thereby creating a possibility of shuttle-like motion. The system works as a Carnot engine where the heat flow between kinetic and potential parts of the nonequilibrium distribution produces the useful work.

cond-mat.stat-mech↗