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Permeation of COâ and Nâ through glassy poly(dimethyl phenylene) oxide under steady- and presteady-state conditions
Glassy polymers are often used for gas separations because of their high selectivity. Although the dualâmode permeation model correctly fits their sorption and permeation isotherms, its physical interpretation is disputed, and it does not describe permeation far from steady state, a condition expected when separations involve intermittent renewable energy sources. To develop a more comprehensive permeation model, we combine experiment, molecular dynamics, and multiscale reactionâdiffusion modeling to characterize the timeâdependent permeation of Nâ and COâ through a glassy poly(dimethyl phenylene oxide) membrane, a model system. Simulations of experimental timeâdependent permeation data for both gases in the presteadyâstate and steadyâstate regimes show that both singleâ and dualâmode reactionâdiffusion models reproduce the experimental observations, and that sorbed gas concentrations lag the external pressure rise. The results point to environmentâsensitive diffusion coefficients as a vital characteristic of transport in glassy polymers
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 spatio-temporal
processes have been observed recently in the ferrocyanide-iodate-sulfite
reaction.Comment: Text: 14 pages compressed Postscript (90kb) Figures: 9 pages
compressed Postscript (368kb
Propagation Failure in Excitable Media
We study a mechanism of pulse propagation failure in excitable media where
stable traveling pulse solutions appear via a subcritical pitchfork
bifurcation. The bifurcation plays a key role in that mechanism. Small
perturbations, externally applied or from internal instabilities, may cause
pulse propagation failure (wave breakup) provided the system is close enough to
the bifurcation point. We derive relations showing how the pitchfork
bifurcation is unfolded by weak curvature or advective field perturbations and
use them to demonstrate wave breakup. We suggest that the recent observations
of wave breakup in the Belousov-Zhabotinsky reaction induced either by an
electric field or a transverse instability are manifestations of this
mechanism.Comment: 8 pages. Aric Hagberg: http://cnls.lanl.gov/~aric; Ehud
Meron:http://www.bgu.ac.il/BIDR/research/staff/meron.htm
A Phase Front Instability in Periodically Forced Oscillatory Systems
Multiplicity of phase states within frequency locked bands in periodically
forced oscillatory systems may give rise to front structures separating states
with different phases. A new front instability is found within bands where
(). Stationary fronts shifting the
oscillation phase by lose stability below a critical forcing strength and
decompose into traveling fronts each shifting the phase by . The
instability designates a transition from stationary two-phase patterns to
traveling -phase patterns
Multi-Phase Patterns in Periodically Forced Oscillatory Systems
Periodic forcing of an oscillatory system produces frequency locking bands
within which the system frequency is rationally related to the forcing
frequency. We study extended oscillatory systems that respond to uniform
periodic forcing at one quarter of the forcing frequency (the 4:1 resonance).
These systems possess four coexisting stable states, corresponding to uniform
oscillations with successive phase shifts of . Using an amplitude
equation approach near a Hopf bifurcation to uniform oscillations, we study
front solutions connecting different phase states. These solutions divide into
two groups: -fronts separating states with a phase shift of and
-fronts separating states with a phase shift of . We find a new
type of front instability where a stationary -front ``decomposes'' into a
pair of traveling -fronts as the forcing strength is decreased. The
instability is degenerate for an amplitude equation with cubic nonlinearities.
At the instability point a continuous family of pair solutions exists,
consisting of -fronts separated by distances ranging from zero to
infinity. Quintic nonlinearities lift the degeneracy at the instability point
but do not change the basic nature of the instability. We conjecture the
existence of similar instabilities in higher 2n:1 resonances (n=3,4,..) where
stationary -fronts decompose into n traveling -fronts. The
instabilities designate transitions from stationary two-phase patterns to
traveling 2n-phase patterns. As an example, we demonstrate with a numerical
solution the collapse of a four-phase spiral wave into a stationary two-phase
pattern as the forcing strength within the 4:1 resonance is increased
Breathing Spots in a Reaction-Diffusion System
A quasi-2-dimensional stationary spot in a disk-shaped chemical reactor is
observed to bifurcate to an oscillating spot when a control parameter is
increased beyond a critical value. Further increase of the control parameter
leads to the collapse and disappearance of the spot. Analysis of a bistable
activator-inhibitor model indicates that the observed behavior is a consequence
of interaction of the front with the boundary near a parity breaking front
bifurcation.Comment: 4 pages RevTeX, see also http://chaos.ph.utexas.edu/ and
http://t7.lanl.gov/People/Aric
Domain Walls in Non-Equilibrium Systems and the Emergence of Persistent Patterns
Domain walls in equilibrium phase transitions propagate in a preferred
direction so as to minimize the free energy of the system. As a result, initial
spatio-temporal patterns ultimately decay toward uniform states. The absence of
a variational principle far from equilibrium allows the coexistence of domain
walls propagating in any direction. As a consequence, *persistent* patterns may
emerge. We study this mechanism of pattern formation using a non-variational
extension of Landau's model for second order phase transitions. PACS numbers:
05.70.Fh, 42.65.Pc, 47.20.Ky, 82.20MjComment: 12 pages LaTeX, 5 postscript figures To appear in Phys. Rev.
Phase Transitions in a Forest-Fire Model
We investigate a forest-fire model with the density of empty sites as control
parameter. The model exhibits three phases, separated by one first-order phase
transition and one 'mixed' phase transition which shows critical behavior on
only one side and hysteresis. The critical behavior is found to be that of the
self-organized critical forest-fire model [B. Drossel and F. Schwabl, Phys.
Rev. Lett. 69, 1629 (1992)], whereas in the adjacent phase one finds the spiral
waves of the Bak et al. forest-fire model [P. Bak, K. Chen and C. Tang, Phys.
Lett. A 147, 297 (1990)]. In the third phase one observes clustering of trees
with the fire burning at the edges of the clusters. The relation between the
density distribution in the spiral state and the percolation threshold is
explained and the implications for stationary states with spiral waves in
arbitrary excitable systems are discussed. Furthermore, we comment on the
possibility of mapping self-organized critical systems onto 'ordinary' critical
systems.Comment: 30 pages RevTeX, 9 PostScript figures (Figs. 1,2,4 are of reduced
quality), to appear in Phys. Rev.
Streamer Propagation as a Pattern Formation Problem: Planar Fronts
Streamers often constitute the first stage of dielectric breakdown in strong
electric fields: a nonlinear ionization wave transforms a non-ionized medium
into a weakly ionized nonequilibrium plasma. New understanding of this old
phenomenon can be gained through modern concepts of (interfacial) pattern
formation. As a first step towards an effective interface description, we
determine the front width, solve the selection problem for planar fronts and
calculate their properties. Our results are in good agreement with many
features of recent three-dimensional numerical simulations.Comment: 4 pages, revtex, 3 ps file
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