Driven diffusion in a periodically compartmentalized tube: homogeneity versus intermittency of particle motion

We study the effect of a driving force F on drift and diffusion of a point Brownian particle in a tube formed by identical ylindrical compartments, which create periodic entropy barriers for the particle motion along the tube axis. The particle transport exhibits striking features: the effective mobility monotonically decreases with increasing F, and the effective diffusivity diverges as F → ∞, which indicates that the entropic effects in diffusive transport are enhanced by the driving force. Our consideration is based on two different scenarios of the particle motion at small and large F, homogeneous and intermittent, respectively. The scenarios are deduced from the careful analysis of statistics of the particle transition times between neighboring openings. From this qualitative picture, the limiting small-F and large-F behaviors of the effective mobility and diffusivity are derived analytically. Brownian dynamics simulations are used to find these quantities at intermediate values of the driving force for various compartment lengths and opening radii. This work shows that the driving force may lead to qualitatively different anomalous transport features, depending on the geometry design

Kinetics of stochastically-gated diffusion-limited reactions and geometry of random walk trajectories

In this paper we study the kinetics of diffusion-limited, pseudo-first-order A + B -> B reactions in situations in which the particles' intrinsic reactivities vary randomly in time. That is, we suppose that the particles are bearing "gates" which interchange randomly and independently of each other between two states - an active state, when the reaction may take place, and a blocked state, when the reaction is completly inhibited. We consider four different models, such that the A particle can be either mobile or immobile, gated or ungated, as well as ungated or gated B particles can be fixed at random positions or move randomly. All models are formulated on a $d$-dimensional regular lattice and we suppose that the mobile species perform independent, homogeneous, discrete-time lattice random walks. The model involving a single, immobile, ungated target A and a concentration of mobile, gated B particles is solved exactly. For the remaining three models we determine exactly, in form of rigorous lower and upper bounds, the large-N asymptotical behavior of the A particle survival probability. We also realize that for all four models studied here such a probalibity can be interpreted as the moment generating function of some functionals of random walk trajectories, such as, e.g., the number of self-intersections, the number of sites visited exactly a given number of times, "residence time" on a random array of lattice sites and etc. Our results thus apply to the asymptotical behavior of the corresponding generating functions which has not been known as yet.Comment: Latex, 45 pages, 5 ps-figures, submitted to PR

Reciprocating motion on the nanoscale

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Communications: Drift and diffusion in a tube of periodically varying diameter. Driving force induced intermittency

We show that the effect of driving force F on the effective mobility and diffusion coefficient of a particle in a tube formed by identical compartments may be qualitatively different depending on the compartment shape. In tubes formed by cylindrical (spherical) compartments the mobility monotonically decreases (increases) with F and the diffusion coefficient diverges (remains finite) as F tends to infinity. In tubes formed by cylindrical compartments, at large F there is intermittency in the particle transitions between openings connecting neighboring compartments

Particle size effect on diffusion in tubes with dead ends: Nonmonotonic size dependence of effective diffusion constant

Diffusion of a spherical particle of radius r in a tube with identical periodic dead ends is analyzed. It is shown that the effective diffusion constant follows the Stokes–Einstein relation, Deff(r)∝1∕r, only when r is larger or much smaller than the radius of the dead end entrance. In between, Deff(r) not only deviates from the 1∕r behavior but may also even become a nonmonotonic function, which increases with the particle radius for a certain range of r