Symmetry in Full Counting Statistics, Fluctuation Theorem, and Relations among Nonlinear Transport Coefficients in the Presence of a Magnetic Field

We study full counting statistics of coherent electron transport through multi-terminal interacting quantum-dots under a finite magnetic field. Microscopic reversibility leads to the symmetry of the cumulant generating function, which generalizes the fluctuation theorem in the context of quantum transport. Using this symmetry, we derive the Onsager-Casimir relation in the linear transport regime and universal relations among nonlinear transport coefficients.Comment: 4.1pages, 1 figur

Kinetics and thermodynamics of first-order Markov chain copolymerization

We report a theoretical study of stochastic processes modeling the growth of first-order Markov copolymers, as well as the reversed reaction of depolymerization. These processes are ruled by kinetic equations describing both the attachment and detachment of monomers. Exact solutions are obtained for these kinetic equations in the steady regimes of multicomponent copolymerization and depolymerization. Thermodynamic equilibrium is identified as the state at which the growth velocity is vanishing on average and where detailed balance is satisfied. Away from equilibrium, the analytical expression of the thermodynamic entropy production is deduced in terms of the Shannon disorder per monomer in the copolymer sequence. The Mayo-Lewis equation is recovered in the fully irreversible growth regime. The theory also applies to Bernoullian chains in the case where the attachment and detachment rates only depend on the reacting monomer

The micro-optical ring electrode Part 2 : theory for the transport limited, steady-state photocurrent.

The micro-optical ring electrode (MORE) is a photoelectrochemical device based on a ring microelectrode that uses the insulating material interior to the ring electrode as a light guide. In this paper, we derive asymptotic analytical expressions for the steady-state, transport limited photocurrent generated at MOREs with thin microrings ((ring inner radius)/(ring outer radius) values > 0.99) for two general types of photoelectrochemical system (a) the PE (photophysical-electrochemical) system, wherein the photoexcited species itself is directly detected on the ring; and (b) the PCE (photophysical-chemical-electrochemical) system, wherein the photoexcited species undergoes a homogeneous electron transfer reaction prior to electrochemical detection. The expressions are generated by exploiting the properties of discontinuous integrals of Bessel functions to solve the diffusion equation for the photogenerated electroactive species both inside and outside the beam. The resultant solutions are then matched at the beam surface. The expressions themselves are used to design experimental protocols that allow for the complete characterization of the photoelectrochemical kinetics of a system and are tested by using them to interpret the results of a MORE study of the photoelectrochemical behaviour of the Ru(bipy)(3)(2+)/Fe3+ photosensitiser/ quenching agent system. The value of the Stern-Volmer constant for the quenching of photoexcited Ru(bipy)(3)(2+) by Fe obtained (0.36 m(3) mol(-1)) compares favourably with the value obtained from fluorescence measurements (0.9 m(3) mol(-1)). (c) 2006 Elsevier B.V. All rights reserved

Microscopic reversibility of quantum open systems

The transition probability for time-dependent unitary evolution is invariant under the reversal of protocols just as in the classical Liouvillian dynamics. In this article, we generalize the expression of microscopic reversibility to externally perturbed large quantum open systems. The time-dependent external perturbation acts on the subsystem during a transient duration, and subsequently the perturbation is switched off so that the total system would thermalize. We concern with the transition probability for the subsystem between the initial and final eigenstates of the subsystem. In the course of time evolution, the energy is irreversibly exchanged between the subsystem and reservoir. The time reversed probability is given by the reversal of the protocol and the initial ensemble. Microscopic reversibility equates the time forward and reversed probabilities, and therefore appears as a thermodynamic symmetry for open quantum systems.Comment: numerical demonstration is correcte

Thermodynamic time asymmetry in nonequilibrium fluctuations

We here present the complete analysis of experiments on driven Brownian motion and electric noise in a $RC$ circuit, showing that thermodynamic entropy production can be related to the breaking of time-reversal symmetry in the statistical description of these nonequilibrium systems. The symmetry breaking can be expressed in terms of dynamical entropies per unit time, one for the forward process and the other for the time-reversed process. These entropies per unit time characterize dynamical randomness, i.e., temporal disorder, in time series of the nonequilibrium fluctuations. Their difference gives the well-known thermodynamic entropy production, which thus finds its origin in the time asymmetry of dynamical randomness, alias temporal disorder, in systems driven out of equilibrium.Comment: to be published in : Journal of Statistical Mechanics: theory and experimen

Fluctuation theorem for entropy production during effusion of a relativistic ideal gas

The probability distribution of the entropy production for the effusion of a relativistic ideal gas is calculated explicitly. This result is then extended to include particle and anti-particle pair production and annihilation. In both cases, the fluctuation theorem is verified.Comment: 6 pages, no figure

Stochastic thermodynamics of chemical reaction networks

For chemical reaction networks described by a master equation, we define energy and entropy on a stochastic trajectory and develop a consistent nonequilibrium thermodynamic description along a single stochastic trajectory of reaction events. A first-law like energy balance relates internal energy, applied (chemical) work and dissipated heat for every single reaction. Entropy production along a single trajectory involves a sum over changes in the entropy of the network itself and the entropy of the medium. The latter is given by the exchanged heat identified through the first law. Total entropy production is constrained by an integral fluctuation theorem for networks arbitrarily driven by time-dependent rates and a detailed fluctuation theorem for networks in the steady state. Further exact relations like a generalized Jarzynski relation and a generalized Clausius inequality are discussed. We illustrate these results for a three-species cyclic reaction network which exhibits nonequilibrium steady states as well as transitions between different steady states.Comment: 14 pages, 2 figures, accepted for publication in J. Chem. Phy

Fluctuation theorem for currents in open quantum systems

A quantum-mechanical framework is set up to describe the full counting statistics of particles flowing between reservoirs in an open system under time-dependent driving. A symmetry relation is obtained which is the consequence of microreversibility for the probability of the nonequilibrium work and the transfer of particles and energy between the reservoirs. In some appropriate long-time limit, the symmetry relation leads to a steady-state quantum fluctuation theorem for the currents between the reservoirs. On this basis, relationships are deduced which extend the Onsager-Casimir reciprocity relations to the nonlinear response coefficients.Comment: 19 page

Single electron transistor strongly coupled to vibrations: Counting Statistics and Fluctuation Theorem

Using a simple quantum master equation approach, we calculate the Full Counting Statistics of a single electron transistor strongly coupled to vibrations. The Full Counting Statistics contains both the statistics of integrated particle and energy currents associated to the transferred electrons and phonons. A universal as well as an effective fluctuation theorem are derived for the general case where the various reservoir temperatures and chemical potentials are different. The first relates to the entropy production generated in the junction while the second reveals internal information of the system. The model recovers Franck-Condon blockade and potential applications to non-invasive molecular spectroscopy are discussed.Comment: extended discussion, to appear in NJ

Universal Properties of Nonlinear Response Functions of Nonequilibrium Steady States

We derive universal properties of nonlinear response functions of nonequilibrium steady states. In particular, sum rules and asymptotic behaviors are derived. Their consequences are illustrated for nonlinear optical materials and nonlinear electrical conductors.Comment: 10 pages, 1 figure; added a few sentences and references to explain detail