Speedup of doping fronts in organic semiconductors through plasma instability

The dynamics of doping transformation fronts in organic semiconductor plasma is studied for application in light-emitting electrochemical cells. We show that new fundamental effects of the plasma dynamics can significantly improve the device performance. We obtain an electrodynamic instability, which distorts the doping fronts and increases the transformation rate considerably. We explain the physical mechanism of the instability, develop theory, provide experimental evidence, perform numerical simulations, and demonstrate how the instability strength may be amplified technologically. The electrodynamic plasma instability obtained also shows interesting similarity to the hydrodynamic Darrieus-Landau instability in combustion, laser ablation, and astrophysics.     

Convective and absolute Eckhaus instability leading to modulated waves in a finite box

We report an experimental study of the secondary modulational instability of a one-dimensional nonlinear traveling wave in a long bounded channel. Two qualitatively different instability regimes involving fronts of spatiotemporal defects are linked to the convective and absolute nature of the instability. Both transitions appear to be subcritical. The spatiotemporal defects control the global mode structure.     

On the classification of buoyancy-driven chemo-hydrodynamic instabilities of chemical fronts

Exothermic autocatalytic fronts traveling in the gravity field can be deformed by buoyancy-driven convection due to solutal and thermal contributions to changes in the density of the product versus the reactant solutions. We classify the possible instability mechanisms, such as Rayleigh-Benard, Rayleigh-Taylor, and double-diffusive mechanisms known to operate in such conditions in a parameter space spanned by the corresponding solutal and thermal Rayleigh numbers. We also discuss a counterintuitive instability leading to buoyancy-driven deformation of statically stable fronts across which a solute-light and hot solution lies on top of a solute-heavy and colder one. The mechanism of this chemically driven instability lies in the coupling of a localized reaction zone and of differential diffusion of heat and mass. Dispersion curves of the various cases are analyzed. A discussion of the possible candidates of autocatalytic reactions and experimental conditions necessary to observe the various instability scenarios is presented.     

Global Solutions to a Reactive Boussinesq System with Front Data on an Infinite Domain

We prove the existence of global solutions to a coupled system of Navier–Stokes, and reaction-diffusion equations (for temperature and mass fraction) with prescribed front data on an infinite vertical strip or tube. This system models a one-step exothermic chemical reaction. The heat release induced volume expansion is accounted for via the Boussinesq approximation. The solutions are time dependent moving fronts in the presence of fluid convection. In the general setting, the fronts are subject to intensive Rayleigh-Taylor and thermal-diffusive instabilities. Various physical quantities, such as fluid velocity, temperature, and front speed, can grow in time. We show that the growth is at most for large time t by constructing a nonlinear functional on the temperature and mass fraction components. These results hold for arbitrary order reactions in two space dimensions and for quadratic and cubic reactions in three space dimensions. In the absence of any thermal-diffusive instability (unit Lewis number), and with weak fluid coupling, we construct a class of fronts moving through shear flows. Although the front speeds may oscillate in time, we show that they are uniformly bounded for large t. The front equation shows the generic time-dependent nature of the front speeds and the straining effect of the flow field. Received: 15 January 1996 / Accepted: 2 September 1997     

Order parameter description of walk-off effect on pattern selection in degenerate optical parametric oscillators

Degenerate optical parametric oscillators can exhibit both uniformly translating fronts and nonuniformly translating envelope fronts under the walk-off effect. The nonlinear dynamics near threshold is shown to be described by a real convective Swift-Hohenberg equation, which provides the main characteristics of the walk-off effect on pattern selection. The predictions of the selected wave vector and the absolute instability threshold are in very good quantitative agreement with numerical solutions found from the equations describing the optical parametric oscillator.     

The effect of convection on a propagating front with a liquid product: Comparison of theory and experiments

This work is devoted to the investigation of propagating polymerization fronts converting a liquid monomer into a liquid polymer. We consider a simplified mathematical model which consists of the heat equation and equation for the depth of conversion for one-step chemical reaction and of the Navier-Stokes equations under the Boussinesq approximation. We fulfill the linear stability analysis of the stationary propagating front and find conditions of convective and thermal instabilities. We show that convection can occur not only for ascending fronts but also for descending fronts. Though in the latter case the exothermic chemical reaction heats the cold monomer from above, the instability appears and can be explained by the interaction of chemical reaction with hydrodynamics. Hydrodynamics changes also conditions of the thermal instability. The front propagating upwards becomes less stable than without convection, the front propagating downwards more stable. The theoretical results are compared with experiments. The experimentally measured stability boundary for polymerization of benzyl acrylate in dimethyl formamide is well approximated by the theoretical stability boundary. (c) 1998 American Institute of Physics.     

Complex patterns in reaction-diffusion systems: A tale of two front instabilities

Two front instabilities in a reaction-diffusion system are shown to lead to the formation of complex patterns. The first is an instability to transverse modulations that drives the formation of labyrinthine patterns. The second is a nonequilibrium Ising-Bloch (NIB) bifurcation that renders a stationary planar front unstable and gives rise to a pair of counterpropagating fronts. Near the NIB bifurcation the relation of the front velocity to curvature is highly nonlinear and transitions between counterpropagating fronts become feasible. Nonuniformly curved fronts may undergo local front transitions that nucleate spiral-vortex pairs. These nucleation events provide the ingredient needed to initiate spot splitting and spiral turbulence. Similar spatiotemporal processes have been observed recently in the ferrocyanide-iodate-sulfite reaction.     

Hydrodynamic instability of multiple four-wave mixing

In the regime of normal dispersion and low-frequency detunings (or high powers), four-wave mixing is shown to undergo a hydrodynamic type of instability. Such instability involves the formation of shocks (steep fronts) from smooth initial data that are regularized through the appearance of trains of fast oscillations, which exhibit solitonlike behavior, colliding elastically.     

Two-dimensional front dynamics and spatial solitons in a nonlinear optical system

Two-dimensional fronts and coarsening dynamics with a t{1/2} power law are analyzed experimentally and theoretically in a nonlinear optical system of a sodium vapor cell with single-mirror feedback. Modifications of the t{1/2} power law are observed in the vicinity of a modulational instability leading to the formation of spatial solitons of different sizes. The experimental and numerical observations give direct evidence for the locking of fronts as the mechanism of soliton formation. A phenomenological equation for the dynamics of the domain radius explains the observed behavior.     

Dynamics of fronts in optical media with linear gain and nonlinear losses

The dynamics of fronts, or kinks, in dispersive media with gain and losses is considered. It is shown that the front parameters, such as the velocity and width, depend on initial conditions. This result is not typical for dissipative systems. For exponentially decreasing initial conditions, the relations for the front parameters are found. A presence of the global bifurcation, when a soliton solution is replaced by the front solution, is demonstrated. It is also shown that in order to observe fronts, the front velocity should be larger than the characteristic velocity of the modulational instability.     

Effects of ionization gradients on inertial-confinement-fusion capsule hydrodynamic stability

A linear perturbation analysis based on velocity potentials is adapted to include the regional, average-ion charge states (Z) in an imploding, inertial-confinement-fusion capsule and shown to lead to superclassical Rayleigh-Taylor growth following deceleration onset. The added instability is ascribed to an inverted ion-entropy gradient driven by the stepwise ionization mismatch DeltaZ across the fuel-pusher interface and is predicted to principally occur in low Atwood-number (<0.5) implosions associated with low-Z pushers. Similar instability enhancement may pertain to supernovae phenomena and ionization fronts in H II protostellar regions.     

Chemical wave propagation with a chemically induced hydrodynamical instability

Propagation of trigger waves in a Belousov-Zhabotinsky (BZ) solution was performed in a capillary slit of parallel glass panes. With an open liquid-air interface, an instability of the upward moving wave fronts was observed up from the middle of the slit. This instability was found to be due to a fluid convection in the upper part of the slit which is generated by diffusion of oxygen through the interface. The explanation for the onset of the convection is based on the fact that oxygen is known to increase the production of bromide in BZ systems.     

Noise generation by instabilities in low Reynolds number supersonic jets

An experimental investigation of noise generation by instabilities in low Reynolds number supersonic air jets has been performed. Sound pressure levels, spectra and acoustic phase fronts were measured with a traversing condenser microphone in the acoustic field of axisymmetric, perfectly expanded, cold jets of Mach numbers 1·4, 2·1 and 2·5. Low Reynolds numbers in the range from Re = 3700 to Re = 8700 were obtained by exhausting the jets into an anechoic vacuum chamber test facility. This contrasts with Reynolds numbers of over 10⁶ for similar jets exhausting into atmospheric pressure. The flow fluctuations of the instability in all three jets have been measured with a hot-wire and the results are documented in a previous paper by Morrison and McLaughlin. Acoustic measurements show that the major portion of the sound radiated by all three jets is produced by the instability's rapid growth and decay that occurs near the end of the potential core. This takes place over a relatively short distance (less than two wavelengths of the instability) in the jet. In the lower two Mach number jets the instability has a phase velocity less than the ambient acoustic velocity. In the Mach number 2·5 jet the instability phase speed is 1·11 times the ambient acoustic velocity. In this case the acoustic phase fronts indicate the possibility of a Mach wave component. It was also determined that low level excitation at the dominant frequency of the instability actually decreased the radiated noise by suppressing the broad band component.     

Transverse instability of line defects of period-2 spiral waves

Spiral waves that arise in period-2 oscillatory media extended in space generically bear "line defects" along which the local kinetics exhibits a period-1 oscillation. Locally, these defect structures can be viewed as a front separating two period-2 oscillatory domains oscillating 2pi out of phase. Here we show that their shape can become sinusoidal with a transverse instability as in bistable fronts. This instability eventually leads to a line-defect filled spatiotemporal chaotic state having erratic proliferations, annihilations, and regenerations of line defects. The same sequence of phenomena is observed in a model reaction-diffusion system as well as in an experimental system.     

Reaction zones in highly unstable detonations

Experimental images of detonation fronts are made for several fuel-oxidizer mixtures, including hydrocarbon–air systems. Schlieren and planar laser induced fluorescence techniques are used to image both the shock configurations and the OH reaction front structure in a single experiment. The experiments are carried out in a narrow rectangular channel. The degree of instability of detonation fronts in different mixtures is evaluated by comparing calculated mixture parameters with the longitudinal neutral stability curve. The images reveal that the structure of the front increases dramatically in complexity as the mixture parameters move away from the neutral stability curve into the unstable region. Of the mixtures studied, nitrogen-diluted hydrocarbon mixtures are predicted to be the most unstable, and these show the greatest degree of wrinkling in the shock and OH fronts, with distortion occurring over a wide range of spatial scales. In the most unstable cases, separation of the shock and OH front occurs, and localized explosions in these regions are observed in a high-speed schlieren movie. This is in dramatic contrast to the weakly unstable waves that have smooth reaction fronts and quasi-steady reaction zones with no evidence of localized explosions. A key feature of highly unstable waves is very fine scale wrinkling of the OH and shock fronts, which is absent in the low-activation energy cases. This may be due to the superposition of cellular structures with a wide range of cell sizes. In contrast to soot foils, images of the OH front have a more stochastic appearance, and organized cellular structure is not as apparent.     

The effects of fluid motion on oscillatory and chaotic fronts

We study oscillatory and chaotic reaction fronts described by the Kuramoto-Sivashinsky equation coupled to different types of fluid motion. We first apply a Poiseuille flow on the fronts inside a two-dimensional slab. We show regions of period doubling transition to chaos for different values of the average speed of Poiseuille flow. We also analyze the effects of a convective flow due to a Rayleigh-Taylor instability. Here the front is a thin interface separating two fluids of different densities inside a two-dimensional vertical slab. Convection is caused by buoyancy forces across the front as the lighter fluid is under a heavier fluid. We first obtain oscillatory and chaotic solutions arising from instabilities intrinsic to the front. Then, we determine the changes on the solutions due to fluid motion.     

Diffusion-driven pattern formation in ionic chemical solutions

The driving force in diffusion-driven pattern formation is the difference in the diffusional flux of the key species, which in the case of ionic systems builds up a local electric field at the concentration gradients. The arising additional migrational flux not only decreases but also enhances the instability of the base state, depending on the charge distribution among the components. The opposite charges on the slower diffusing autocatalyst and its reacting counterpart favor pattern formation and shift the onset of instability to a smaller difference in the diffusion coefficients. The same charges, in addition to having the opposite effect, may even lead to the complete stabilization of planar reaction fronts unstable in the neutral system.     

Onset of turbulence from the receptivity stage of fluid flows

The traditional viewpoint of fluid flow considers the transition to turbulence to occur by the secondary and nonlinear instability of wave packets, which have been created experimentally by localized harmonic excitation. The boundary layer has been shown theoretically to support spatiotemporal growing wave fronts by Sengupta, Rao, and Venkatasubbaiah [Phys. Rev. Lett. 96, 224504 (2006)] by a linear mechanism, which is shown here to grow continuously, causing the transition to turbulence. Here, we track spatiotemporal wave fronts to a nonlinear turbulent state by solving the full 2D Navier-Stokes equation, without any limiting assumptions. Thus, this is the only demonstration of deterministic disturbances evolving from a receptivity stage to the full turbulent flow. This is despite the prevalent competing conjectures of the event being three-dimensional and/or stochastic in nature.     

Spatiotemporal chaos in the dynamics of buoyantly and diffusively unstable chemical fronts

Nonlinear dynamics resulting from the interplay between diffusive and buoyancy-driven Rayleigh-Taylor (RT) instabilities of autocatalytic traveling fronts are analyzed numerically for various values of the relevant parameters. These are the Rayleigh numbers of the reactant A and autocatalytic product B solutions as well as the ratio D=D(B)/D(A) between the diffusion coefficients of the two key chemical species. The interplay between the coarsening dynamics characteristic of the RT instability and the constant short wavelength modulation of the diffusive instability can lead in some regimes to complex dynamics dominated by irregular succession of birth and death of fingers. By using spectral entropy measurements, we characterize the transition between order and spatial disorder in this system. The analysis of the power spectrum and autocorrelation function, moreover, identifies similarities between the various spatial patterns. The contribution of the diffusive instability to the complex dynamics is discussed.     

Modeling dewetting of ultra-thin solid films

We review some models for the dynamics of dewetting of ultra-thin solid films. We discuss the similarities and the differences between faceted and non-faceted systems. The faceting of the dewetting rim leads to corrections in the velocity of dewetting fronts both in flat and axisymmetric geometries. The faceting of the edge of the dewetting rim leads to a strong anisotropy of the dewetting instability. Faceting also induces novel dewetting regimes such as layer-by-layer dewetting, and monolayer dewetting.