Multiparticle fractal aggregation

Kinetic fractal aggregation in a particle bath where a fractionf of the sites are initially occupied is studied withd=2 computer simulations. Independent particles diffusing to a fixed cluster produce an aggregate with fractal dimensionD 1.7 up to a correlation length(f). At larger lengthsD2.(f) asf 0. When the particles remain fixed but the cluster undergoes a rigid random walkD appears constant at larger scales but varies withf. D 1.95 at largef andD 1.7 asf 0. In both cases, the aggregate sizeN(t) grows with timet ^(f) . Aggregation on a surface by independently diffusing particles produces shapes reminiscent of electrochemical dendritic growth. The dependence of growth rate and geometry is studied as a function of particle concentration and sticking probability.     

Random aggregation and random-walking center of mass

Two random aggregation models are used in demonstrating the properties of the random displacementsr _i of the center of mass of aggregating particles. It is found that r _i is a randomly decreasing sequence that scales with the cluster size (steps)s and _i ^=1/s r _i s ^1/D , whereD is the fractal dimension. The center-of-mass random walk is a consistent representation of the dynamics of aggregation.     

Map dependence of the fractal dimension deduced from iterations of circle maps

Every orientation preserving circle mapg with inflection points, including the maps proposed to describe the transition to chaos in phase-locking systems, gives occasion for a canonical fractal dimensionD, namely that of the associated set of for whichf =+g has irrational rotation number. We discuss how this dimension depends on the orderr of the inflection points. In particular, in the smooth case we find numerically thatD(r)=D(r ^–1)=r ^–1/8.     

Application of fractal concepts to polymer statistics and to anomalous transport in randomly porous media

We consider the application of fractal concepts to polymer statistics and to anomalous transport in randomly porous media. It is found that answers to interesting physics questions can be expressed in terms of several new fractal dimensions (in addition to the fractal dimensiond _f ): (1)d _f ^BB , the fractal dimension of the backbone, arises in connection with electric current flow, (2)d _red, the fractal dimension of the singly connected bonds in the backbone, arises in connection with its equivalence to the thermal scaling power, (3)d _E, the fractal dimension of the of the elastic backbone, (4)d _u, the fractal dimension of the unscreened perimeter, arises in connection with the viscosity singularity at the gelation threshold, (5)d _min the fractal dimension of the minimum path (or chemical distance) between two sites, arises in co-nnection with the Aharony-Stauffer conjecture, (6)dw, the fractal dimension of a random walk, (7)d _G, the fractal dimension of growth sites that arise as a random walk creates a cluster. Relations among these fractal dimensions are discussed, some of which can be proved and others of which are conjectures whose validity has been established only in certain limiting cases.Supported in part at the Center for Polymer Studies by grants from ONR and NSF.     

Self-avoiding walk model for proteins

We study a model for the backbone of proteins on a square lattice which consists of the path traced out by a self-avoiding walk (SAW) on the lattice and bridges not belonging to sites on the SAW but connecting nearest neighbor sites of the SAW. We calculated the fractal dimensiond _w for random walk on this model and found thatd _w2.6, in disagreement with a recent suggestion thatd _w should be 2.     

Self-affine fractal clusters: Conceptual questions and numerical results for directed percolation

In this paper we address the question of the existence of a well defined, non-trivial fractal dimensionD of self-affine clusters. In spite of the obvious relevance of such clusters to a wide range of phenomena, this problem is still open since thedifferent published predictions forD have not been tested yet. An interesting aspect of the problem is that a nontrivial global dimension for clusters is in contrast with the trivial global dimension of self-affine functions. As a much studied example of self-affine structures, we investigate the infinite directed percolation cluster at the threshold. We measuredD ind=2 dimensions by the box counting method. Using a correction to scaling analysis, we obtainedD=1.765(10). This result does not agree with any of the proposed relations, but it favorsD=1+(1- )/ , where and are the correlation length exponents and is a Fisher exponent in the cluster scaling.     

Monte Carlo simulation of aggregate morphology for simultaneous coagulation and sintering

A model for simulation of the three-dimensional morphology of nano-structured aggregates formed by concurrent coagulation and sintering is presented. Diffusion controlled cluster–cluster aggregation is assumed to be the prevailing coagulation mechanism which is implemented using a Monte–Carlo algorithm. Sintering is modeled as a successive overlapping of spherical primary particles, which are allowed to grow as to preserve overall mass. Simulations are characterized by individual ratios of characteristic collision to fusion time. A number of resulting aggregate-structures is displayed and reveals structure formation by coagulation and sintering for different values of . These aggregates are described qualitatively and quantitatively by their mass fractal dimension D_f and radius of gyration. The fractal dimension increases from 1.86 for pure aggregation to 2.75 for equal characteristic time scales. As sintering turns out to be more and more relevant, increasingly compact aggregates start to form and the radius of gyration decreases significantly. The simulation results clearly reveal a strong dependence of the fractal dimension on the kinetics of the concurrent coagulation and sintering processes. Considering appropriate values of D_f in aerosol process simulations may therefore be important in many cases.     

Spatial fluctuations in reaction-limited aggregation

A general method is used for describing reaction-diffusion systems, namely van Kampen's method of compounding moments, to study the spatial fluctuations in reaction-limited aggregation processes. The general formalism used here and in subsequent publications is developed. Then a particular model is considered that is of special interest, since it describes the occurrence of a phase transition (gelation). The corresponding rate constants for the reaction between two clusters of sizei and sizej areK _ij=ij (i, j=1, 2,). For thediffusion constants D _j of clusters of sizej the following class of models is considered:D _j=D if 1Js andD _j=0 ifj>s. The casess= ands< are studied separately. For the models= the equal-time and the two-time correlation functions are calculated; this modelbreaks down at the gel point. The breakdown is characterized by a divergence of the density fluctuations, and is caused by the large mobility of large clusters. For all models withs< the density fluctuations remain finite att _c, and the equal-time correlation functions in the pre- and in the post-gel stage are calculated. Many explicit and asymptotic results are given. From the exact solution the upper critical dimension in this gelling model isd _c=2.     

Simple cell model with collapse instability

A cell model is introduced in which pairs of particles interact only within the same cell, and then only with a constant coupling ₀. For positive ₀ the statistical thermodynamics is normal, but as ₀ changes sign, the system manifests a collapse phenomenon with all particles tending to aggregate in the same cell. This collapse instability causes high-temperature series to diverge, but known asymptotic properties of Stirling numbers of the second kind allow one to establish Borel summability. The present model is equivalent to continuum models with bounded pair potentials when in the latter the space dimensionD is permitted to go to 0+.     

Different types of self-avoiding walks on deterministic fractals

Normal and indefinitely-growing (IG) self-avoiding walks (SAWs) are exactly enumerated on several deterministic fractals (the Manderbrot-Given curve with and without dangling bonds, and the 3-simplex). On then th fractal generation, of linear sizeL, the average number of steps behaves asymptotically as N=AL ^D _saw+B. In contrast to SAWs on regular lattices, on these factals IGSAWs and normal SAWs have the same fractal dimensionD _saw. However, they have different amplitudes (A) and correction terms (B).     

Dynamical Critical Exponent for the Majority-Vote Model

We investigate the dynamical behavior of the isotropic majority-vote model on a square lattice using a combination of damage spreading and finite-size scaling methods. For initial damage D(0)1/2, the dynamical phase diagram exhibits a chaotic-frozen phase transition at a critical noise parameter q _c =0.0818±0.0002, while for D(0)1/2 the damage does not propagate for any value of the model's parameter 0q<1/2. From simulations at q _c , we find that the dynamical critical exponent is z=0.65±0.05.     

Self-avoiding walks on random fractal environments

Self-avoiding random walks (SAWs) are studied on several hierarchical lattices in a randomly disordered environment. An analytical method to determine whether their fractal dimensionD _saw is affected by disorder is introduced. Using this method, it is found that for some lattices,D _saw is unaffected by weak disorder; while for othersD _saw changes even for infinitestimal disorder. A weak disorder exponent is defined and calculated analytically [ measures the dependence of the variance in the partition function (or in the effective fugacity per step)vL on the end-to-end distance of the SAW,L]. For lattices which are stable against weak disorder (<0) a phase transition exists at a critical valuev=v ^* which separates weak- and strong-disorder phases. The geometrical properties which contribute to the value of are discussed.     

A contact process with a single inhomogeneous site

The one-dimensional basic contact process is a Markov process for which particles give birth on vacant nearest neighbor sites at rate >0 and particles die at rate one. We introduce a one-dimensional contact process with a single inhomogeneous site: the evolution is as above except that a particle located at the origin does not die. Let _c be the critical value of the basic contact process. We show that for _c the upper invariant measures of the inhomogeneous contact process and the basic contact process coincide except at a finite number of sites. The behavior at = _c is much more intersting: the upper invariant measure of the inhomogeneous contact process concentrates on configurations with infinitely many particles, while it is known that the critical basic contact process dies out. So a single inhomogeneity may provoke a perturbation unbounded in space. As a byproduct of our analysis we prove that the connectivity probabilities of the critical basic contact process are not summable. We also give a biological interpretation of this model.     

Fractal behavior in trapping and reaction: A random walk study

We investigate the trapping of a random walker in fractal structures (Sierpinski gaskets) with randomly distributed traps. The survival probability is determined from the number of distinct sites visited in the trap-free fractals. We show that the short-time behavior and the long-time tails of the survival probability are governed by the spectral dimensiond. We interpolate between these two limits by introducing a scaling law. An extension of the theory, which includes a continuous-time random walk on fractals, is discussed as well as the case of direct trapping. The latter case is shown to be governed by the fractal dimensiond.     

Effect of nonequilibrium charge screening in A + B → 0 bimolecular reactions in condensed matter

The formalism of many-particle densities developed earlier by the present authors is applied to the study of the cooperative effects in the kinetics of bimolecular A + B 0 reactions between oppositely charged particles (reactants). It is shown that unlike the Debye-Hückel theory in statistical physics, here charge screening has essentially a nonequilibrium character. For the asymmetric mobility of reactants (D _A = 0,D _B 0 the joint spatial distribution of similar immobile reactants A reveals at short distances a singular character associated with their aggregation. The relevant reaction rate does not approach a steady state (as it does in the symmetric case,D _A =D _B, but increases infinitely in time, thus leading to a concentration decay which is quicker than the algebraic law generally accepted in chemical kinetics,n t _–1.     

Lattice random walks for sets of random walkers. First passage times

We have studied the mean first passage time for the first of aset of random walkers to reach a given lattice point on infinite lattices ofD dimensions. In contrast to the well-known result ofinfinite mean first passage times for one random walker in all dimensionsD, we findfinite mean first passage times for certain well-specified sets of random walkers in all dimensions, exceptD = 2. The number of walkers required to achieve a finite mean time for the first walker to reach the given lattice point is a function of the lattice dimensionD. ForD > 4, we find that only one random walker is required to yield a finite first passage time, provided that this random walker reaches the given lattice point with unit probability. We have thus found a simple random walk property which sticks atD > 4.Supported in part by a grant from Charles and Renée Taubman and by the National Science Foundation, Grant CHE78-21460.     

On the survival probability of a random walk in a finite lattice with a single trap

We consider the survival of a random walker in a finite lattice with periodic boundary conditions. The initial position of the random walker is uniformly distributed on the lattice with respect to the trap. We show that the survival of a random walker, U _n>, can be exactly related to the expected number of distinct sites visted on a trap-free lattice by U _n=1–S _n/N ^D (*) whereN ^D is the number of lattice points inD dimensions. We then analyze the behavior of S_n in any number of dimensions by using Tauberian methods. We find that at sufficiently long times S _n decays exponentially withn in all numbers of dimensions. InD = 1 and 2 dimensions there is an intermediate behavior which can be calculated and is valid forN ²N 1 whenD = 1 andN lnN n 1 whenD = 2. No such crossover exists when Z3. The form of (*) suggests that the single trap approximation is indeed a valid low-concentration limit for survival on an infinite lattice with a finite concentration of traps.     

Measurement of Aggregate Fractal Dimensions Using Static Light Scattering

Aggregates formed from colloidal particles will vary in shape according to the aggregation regime prevalent. Compact structures are formed when the aggregation is slow, whilst loose tenuous structures are formed when rapid (or diffusion limited) aggregation prevails. These structures can be fractal in nature, that is, there is a relationship between porosity and the number of primary particles making up the aggregate, and is described by the fractal dimension, d_F. Fractal dimensions of hematite aggregates have been measured experimentally using the static light scattering technique. Fractal dimensions varied with aggregation regimes; for the rapid aggregation regime, d_F was found to be 2.8, whilst for conditions in which aggregation was slow (retardation forces prevail), d_F's of 2.3 were measured. For conditions which lead to aggregation in which both diffusion and retardation forces play a part, structures with fractal dimensions such that 2.3 < d_F < 2.8 were found. The effects of adsorbed fulvic acid, a naturally occuring organic acid, on the kinetics of hematite aggregation and on the resulting structure of hematite aggregates were also investigated. The study of aggregate structure shows that the fractal dimensions of hematite aggregates which are partially coated with fulvic acid molecules are higher than those obtained with no adsorbed fulvic acid. The scattering exponents obtained from static light scattering experiments of these aggregates range from 2.83 ± 0.08 to 3.42 ± 0.1. The scattering exponents of greater than 3 indicate that the scattering is the result of objects that contains pores which are bounded by surfaces with a fractal structure, and can be related only to surface fractal dimension. The high fractal dimensions are due to restructuring within the aggregates, which only occured at low coverage by the organic acid.     

Nanoparticle aggregation due to dewetting of sandwiched buffer layers

The deposition of Au onto thin condensed volatile buffer layers produces small clusters. Sublimation of the buffer converts these clusters into compact or ramified structures, depending on the thickness of the buffer, in a process called buffer-layer-assisted growth. We have used bilayer structures of Xe on CO₂ or Xe on H₂O on amorphous carbon substrates to investigate effects of second layer dewetting and the impact of the initial particle size on aggregation. Compact particles formed by Xe desorption aggregate during removal of the CO₂ or H₂O layer but little aggregation occurs for ramified particles produced on Xe layers thicker than 100 ML. Instead, the large structures tend to break up on the CO₂ film, producing smaller, more compact particles. CO₂ and H₂O impurities in the Xe film significantly reduce particle coalescence and accelerate Xe dewetting.     

Percolation,fractals, and anomalous diffusion

Both the infinite cluster and its backbone are self-similar at the percolation threshold,p _c . This self-similarity also holds at concentrationsp nearp _c , for length scalesL which are smaller than the percolation connectedness length,. ForL<, the number of bonds on the infinite cluster scales asL ^D , where the fractal dimensionalityD is equal to(d-/v). Geometrical fractal models, which imitate the backbone and on which physical models are exactly solvable, are presented. Above six dimensions, one has D=4 and an additional scaling length must be included. The effects of the geometrical structure of the backbone on magnetic spin correlations and on diffusion at percolation are also discussed.