Anisotropic Carrier Transport in n-Doped 6H-SiC

Physics of the Solid State - In this paper, a study is presented on the charge transport in n-type doped semiconductor 6H-SiC (in both transient and steady state) using a nonequilibrium quantum...     

Statistical-Mechanical Foundations for a Generalized Thermodynamics of Dissipative Processes

A statistical-mechanical formalism for nonequilibrium systems, namely the nonequilibrium statistical operator method, provides microscopic foundations for a generalized thermodynamics of dissipative processes. This formalism is based on a unifying variational approach that is considered to be encompassed in Jaynes' Predictive Statistical Mechanics and principle of maximization of the statistical-informational entropy. Within the framework of the statistical thermodynamics that follows from the method, we demonstrate the existence of generalized forms of the theorem of minimum (informational) entropy production, the criterion for evolution, and the thermodynamic (in)stability criterion. The formalism is not restricted to local equilibrium but, in principle, to general conditions (its complete domain of validity is not yet fully determined). A H-theorem associated to the formalism is presented in the form of an increase of the informational entropy along the evolution of the system. Some of the results are illustrated in an application to the study of a model for a photoexcited direct-gap semiconductor.     

Phenomenological model of the diffusion of impurity atoms in ultrathin silicon layers with a nonuniform distribution of temperatures

The influence of fluxes of intrinsic nonequilibrium semiconductor defects on impurity diffusion in a nonuniform temperature field is considered in the framework of the phenomenological theory of irreversible processes. The mass transfer coefficient defined as the ratio of the concentrations of nonequilibrium and equilibrium defects is introduced to take the excessive concentration of nonequilibrium defects into account. The introduction of this coefficient into equations for matter and heat fluxes makes it possible to express the parameters of the process of thermal diffusion (the diffusion coefficient and the heat of transport) as a time-dependent function of the excessive concentration of intrinsic nonequilibrium semiconductor defects.     

Hamiltonian dynamics,nanosystems, and nonequilibrium statistical mechanics

An overview is given of recent advances in nonequilibrium statistical mechanics on the basis of the theory of Hamiltonian dynamical systems and in the perspective provided by the nanosciences. It is shown how the properties of relaxation toward a state of equilibrium can be derived from Liouville's equation for Hamiltonian dynamical systems. The relaxation rates can be conceived in terms of the so-called Pollicott–Ruelle resonances. In spatially extended systems, the transport coefficients can also be obtained from the Pollicott–Ruelle resonances. The Liouvillian eigenstates associated with these resonances are in general singular and present fractal properties. The singular character of the nonequilibrium states is shown to be at the origin of the positive entropy production of nonequilibrium thermodynamics. Furthermore, large-deviation dynamical relationships are obtained, which relate the transport properties to the characteristic quantities of the microscopic dynamics such as the Lyapunov exponents, the Kolmogorov–Sinai entropy per unit time, and the fractal dimensions. We show that these large-deviation dynamical relationships belong to the same family of formulas as the fluctuation theorem, as well as a new formula relating the entropy production to the difference between an entropy per unit time of Kolmogorov–Sinai type and a time-reversed entropy per unit time. The connections to the nonequilibrium work theorem and the transient fluctuation theorem are also discussed. Applications to nanosystems are described.     

Perturbation Theory for Continuous Stochastic Equations

The various general perturbational schemes for continuous stochastic equations are considered. These schemes have many analogous features with the iterational solution of Schwinger equation for S-matrix. The following problems are discussed: continuous stochastic evolution equations for probaibility distribution functionals, evolution equations for equal time correlators, perturbation theory for Gaussian and Poissonian additive noise, perturbation theory for birth and death processes. stochastic properties of systems with multiplicative noise. The general results are illustrated by diffusion - controlled reactions, fluctuations in closed systems with chemical processes, propagation of waves in random media in parabolic equation approximation, and nonequilibrium phase transitions in systems with Poissonian breeding centers. The rate of irreversible reaction X + X → A (Smoluchowski process) is calculated with the use of general theory based on continuous stochastic equations for birth and death processes. The threshold criterion and range of fluctuational region for synergetic phase transition in system with Poissonian breeding centers are also considered.     

The entropy flux and the evolution equations for the fluxes including nonlocal terms from the point of view of extended irreversible thermodynamics

The expression for the entropy flux is analysed from the point of view of irreversible thermodynamics. In connection with this problem the evolution equations for the heat flux and for the electric current density including nonlocal terms are derived and discussed. The relation for the entropy flux is compared with that obtained by the statistical nonequilibrium thermodynamics on the basis founded on a generalized Gibbs' ensemble method for nonequilibrium systems.     

The Steady State Fluctuation Relation for the Dissipation Function

We give a proof of transient fluctuation relations for the entropy production (dissipation function) in nonequilibrium systems, which is valid for most time reversible dynamics. We then consider the conditions under which a transient fluctuation relation yields a steady state fluctuation relation for driven nonequilibrium systems whose transients relax, producing a unique nonequilibrium steady state. Although the necessary and sufficient conditions for the production of a unique nonequilibrium steady state are unknown, if such a steady state exists, the generation of the steady state fluctuation relation from the transient relation is shown to be very general. It is essentially a consequence of time reversibility and of a form of decay of correlations in the dissipation, which is needed also for, e.g., the existence of transport coefficients. Because of this generality the resulting steady state fluctuation relation has the same degree of robustness as do equilibrium thermodynamic equalities. The steady state fluctuation relation for the dissipation stands in contrast with the one for the phase space compression factor, whose convergence is problematic, for systems close to equilibrium. We examine some model dynamics that have been considered previously, and show how they are described in the context of this work.     

A Variational Principle for Thermodynamical Waves

When the dissipative processes are dominant in the system, the assumption of local equilibrium holds good and the space time evolution of irreversible system can be described by the variational principle of GYARMATI. However when imposed changes in the state variables are fast, the system can not be in a state of local equilibrium and to define the nonequilibrium state of the system it is necessary to extend the formalism of classical irreversible thermodynamics. The wave approach of Onsagerian thermodynamics is one such pursuit and is a direct generalization of the original Onsager-Machlup proposition. An important consequence of this theory is that it leads to transport equations with finite propagation velocities, which are referred to as thermodynamical waves. In this note we endeavour to write the appropriate form of GYARMATI'S variational principle for thermodynamical waves.     

Coexistence in the two-dimensional May-Leonard model with random rates

We employ Monte Carlo simulations to numerically study the temporal evolution and transient oscillations of the population densities, the associated frequency power spectra, and the spatial correlation functions in the (quasi-) steady state in two-dimensional stochastic May-Leonard models of mobile individuals, allowing for particle exchanges with nearest-neighbors and hopping onto empty sites. We therefore consider a class of four-state three-species cyclic predator-prey models whose total particle number is not conserved. We demonstrate that quenched disorder in either the reaction or in the mobility rates hardly impacts the dynamical evolution, the emergence and structure of spiral patterns, or the mean extinction time in this system. We also show that direct particle pair exchange processes promote the formation of regular spiral structures. Moreover, upon increasing the rates of mobility, we observe a remarkable change in the extinction properties in the May-Leonard system (for small system sizes): (1) as the mobility rate exceeds a threshold that separates a species coexistence (quasi-) steady state from an absorbing state, the mean extinction time as function of system size N crosses over from a functional form ∼ e ^cN /N (where c is a constant) to a linear dependence; (2) the measured histogram of extinction times displays a corresponding crossover from an (approximately) exponential to a Gaussian distribution. The latter results are found to hold true also when the mobility rates are randomly distributed.     

Response function theory for far-from-equilibrium statistical systems

A formalism to determine the response function of a sample in conditions far from thermal equilibrium is presented. It consists in a generalization of scattering theory coupled to the statistical theory of irreversible processes, the nonequilibrium statistical operator method, developed by Zubarev. The scattering cross section is expressed in terms of double-time correlation functions, which are related to appropriate nonequilibrium thermodynamic Green's functions. The latter are also used to treat generalized transport equations, and, as an illustration, the method is applied to the study of the time-resolved Raman spectroscopy of a photoexcited semiconductor plasma.     

Observation of size-dependent thermalization in CdSe nanocrystals using time-resolved photoluminescence spectroscopy

We report heat dissipation times in semiconductor nanocrystals of CdSe. Specifically, a previously unresolved, subnanosecond decay component in the low-temperature photoluminescence decay dynamics exhibits longer decay lifetimes (tens to hundreds of picoseconds) for larger nanocrystals as well as a size-independent, ~25-meV spectral shift. We attribute the fast relaxation to transient phonon-mediated relaxation arising from nonequilibrium acoustic phonons. Following acoustic phonon dissipation, the dark exciton state recombines more slowly via LO-phonon assistance resulting in the observed spectral shift. The measured relaxation time scales agree with classical calculations of thermal diffusion, indicating that interfacial thermal conductivity does not limit thermal transport in these semiconductor nanocrystal dispersions.     

Quantum transport equations for two-band semiconductor systems

Employing nonequilibrium Green's functions and the equation of motion technique, transport equations for two-band semiconductor systems are derived and their physical significance is discussed.     

Fluid mechanics revisited

Öttinger's recent nontraditional incorporation of fluctuations into the formulation of the friction matrix appearing in the phenomenological GENERIC theory of nonequilibrium irreversible processes is shown to furnish transport equations for single-component gases and liquids undergoing heat transfer which support the view that revisions to the Navier–Stokes–Fourier (N–S–F) momentum/energy equation set are necessary, as empirically proposed by the author on the basis of an experimentally supported theory of diffuse volume transport. The hypothesis that the conventional N–S–F equations prevail without modification only in the case of “incompressible” fluids, where the density ρ of the fluid is uniform throughout, serves to determine the new phenomenological parameter α^′ appearing in the GENERIC friction matrix. In the case of ideal gases the consequences of this constitutive hypothesis are shown to yield results identical to those derived theoretically by Öttinger on the basis of a “proper” coarse-graining of Boltzmann's kinetic equation. A major consequence of the present work is that the fluid's specific momentum density v is equal to its volume velocity v_v, rather than to its mass velocity v_m, contrary to current views dating back 250 years to Euler. In the case of rarefied gases the proposed modifications are also observed to agree with those resulting from Klimontovich's molecularly based, albeit ad hoc, self-diffusion addendum to Boltzmann's collision integral. Despite the differences in their respective physical models—molecular vs. phenomenological—the role played by Klimontovich's collisional addition to Boltzmann's equation in modifying the N–S–F equations is noted to constitute a molecular counterpart of Öttinger's phenomenological fluctuation addition to the GENERIC friction matrix. Together, these two theories collectively recognize the need to address multiple- rather than single-encounter collisions between a test molecule and its neighbors when formulating physically satisfactory statistical–mechanical theories of irreversible transport processes in gases. Overall, the results of the present work implicitly support the unorthodox view, implicit in the GENERIC scheme, that the translation of Newton's discrete mass-point molecular mechanics into continuum mechanics, the latter as embodied in the Cauchy linear momentum equation of fluid mechanics, cannot be correctly effected independently of the laws of thermodynamics. While Öttinger's modification of GENERIC necessitates fundamental changes in the foundations of fluid mechanics in regard to momentum transport, no basic changes are required in the foundations of linear irreversible thermodynamics (LIT) beyond recognizing the need to add volume to the usual list of extensive physical properties undergoing transport in single-species fluid continua, namely mass, momentum and energy. An alternative, nonGENERICally based approach to LIT, derived from our findings, is outlined at the conclusion of the paper. Finally, our proposed modifications of both Cauchy's linear momentum equation and Newton's rheological constitutive law for fluid-phase continua are noted to be mirrored by counterparts in the literature for solid-phase continua dating back to the classical interdiffusion experiments of Kirkendall and their subsequent interpretation by Darken in terms of diffuse volume transport.     

Time-local gaussian processes,path integrals and nonequilibrium nonlinear diffusion

In this paper we discuss the concept of time-local gaussian processes. These are processes for which the state variable at time t + τ is gaussian distributed around its most probable value at that time, for a specified realization a small time interval τ earlier. On one hand it will be shown that these processes are related to a very simple path sum. On the other hand the associated stochastic differential equation is derived by means of the Kramers-Moyal method, and will be seen to be the most general nonlinear Fokker-Planck equation. The significance of the present formulation for nonequilibrium processes and the comprehension of critical phenomena will be evaluated.     

Thermodynamics of nonequilibrium radiation. (II) Irreversible evolution and experimental setup

Giving continuation to the study of the thermodynamics of nonequilibrium radiation presented in the preceding article [Physica A 300 (2001) 386], we derive the evolution in time of its macroscopic nonequilibrium state. The case of a semiconductor sample and the coupling of radiation and transverse optical phonons is explicitly considered. Excitation of the latter drives the radiation field out of equilibrium. Under constant excitation, a steady state sets in which is analyzed. It is shown that the quasitemperature per mode of the radiation field, which has been defined in the preceding paper, can be determined in optical experiments such as Raman scattering.