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Influence of surfactants on the structure of titanium oxide gels : experiments and simulations

We report here on experimental and numerical studies of the influence of surfactants on mineral gel synthesis. The modification of the gel structure when the ratios water-precursor and water-surfactant vary is brought to the fore by fractal dimension measures. A property of {\em polydispersity of the initial hydrolysis} is proposed to explain these results, and is successfuly tested through numerical experiments of three dimensional chemically limited aggregation.

chem-ph↗

Theoretical Approach to the Correlations of a Hard-Sphere Crystal

We present the first theoretical approach to the angular-average of the two-body correlation function $\tilde g(r)$ for simple solids. It is based on three sum rules for $\tilde g(r)$: the compressibility and virial equations and the normalization. We apply the theory to determine this correlation function for the case of the FCC solid phase of hard spheres. The agreement with simulation data is excellent over all the density range. The application to other simple systems is discussed. The approach opens a new route to perturbation theories for simple solids.

cond-mat↗

Kinetics of fragmentation-annihilation processes

We investigate the kinetics of systems in which particles of one species undergo binary fragmentation and pair annihilation. In the latter, nonlinear process, fragments react at collision to produce an inert species, causing loss of mass. We analyse these systems in the reaction-limited regime by solving a continuous model within the mean-field approximation. The rate of fragmentation, for a particle of mass $x$ to break into fragments of masses $y$ and $x-y$, has the form $x^{λ-1}$ ($λ>0$), and the annihilation rate is constant and independent of the masses of the reactants. We find that the asymptotic regime is characterized by the annihilation of small-mass clusters. The results are compared with those for a model with linear mass-loss (i.e.\ with a sink). We also study more complex models, in which the processes of fragmentation and annihilation are controlled by mutually-reacting catalysts. Both pair- and linear-annihilation are considered. Depending on the specific model and initial densities of the catalysts, the time-decay of the cluster-density can now be very unconventional and even non-universal. The interplay between the intervening processes and the existence of a scaling regime are determined by the asymptotic behaviour of the average-mass and of the mass-density, which may either decay indefinitely or tend to a constant value. We discuss further developments of this class of models and their potential applications.

cond-mat↗

Elastic Scattering by Deterministic and Random Fractals: Self-Affinity of the Diffraction Spectrum

The diffraction spectrum of coherent waves scattered from fractal supports is calculated exactly. The fractals considered are of the class generated iteratively by successive dilations and translations, and include generalizations of the Cantor set and Sierpinski carpet as special cases. Also randomized versions of these fractals are treated. The general result is that the diffraction intensities obey a strict recursion relation, and become self-affine in the limit of large iteration number, with a self-affinity exponent related directly to the fractal dimension of the scattering object. Applications include neutron scattering, x-rays, optical diffraction, magnetic resonance imaging, electron diffraction, and He scattering, which all display the same universal scaling.

cond-mat↗

Cooperative Chiral Order in Copolymers of Chiral and Achiral Units

Polyisocyanates can be synthesized with chiral and achiral pendant groups distributed randomly along the chains. The overall chiral order, measured by optical activity, is strongly cooperative and depends sensitively on the concentration of chiral pendant groups. To explain this cooperative chiral order theoretically, we map the random copolymer onto the one-dimensional random-field Ising model. We show that the optical activity as a function of composition is well-described by the predictions of this theory.

cond-mat↗

Generalized Bloch equations for a strongly driven tunneling system

Using the Robertson projection operator formalism, we derive generalized Bloch equations which describe the dynamics of a biased two-level tunneling system strongly driven by an external field and weakly coupled to a super-Ohmic heat bath. The generalized Bloch equations constitute a set of coupled nonlinear integro-differential equations. With their help we investigate the influence of phonons on the phenomenon of dynamical localization.

cond-mat↗

Identification of Amino Acid Sequences with Good Folding Properties in an Off-Lattice Model

Folding properties of a two-dimensional toy protein model containing only two amino-acid types, hydrophobic and hydrophilic, respectively, are analyzed. An efficient Monte Carlo procedure is employed to ensure that the ground states are found. The thermodynamic properties are found to be strongly sequence dependent in contrast to the kinetic ones. Hence, criteria for good folders are defined entirely in terms of thermodynamic fluctuations. With these criteria sequence patterns that fold well are isolated. For 300 chains with 20 randomly chosen binary residues approximately 10% meet these criteria. Also, an analysis is performed by means of statistical and artificial neural network methods from which it is concluded that the folding properties can be predicted to a certain degree given the binary numbers characterizing the sequences.

chem-ph↗

Chaos in Axially Symmetric Potentials with Octupole Deformation

Classical and quantum mechanical results are reported for the single particle motion in a harmonic oscillator potential which is characterized by a quadrupole deformation and an additional octupole deformation. The chaotic character of the motion is srongly dependent on the quadrupole deformation in that for a prolate deformation virtually no chaos is discernible while for the oblate case the motion shows strong chaos when the octupole term is turned on.

nucl-th↗

Packing Transitions in Nanosized Li Clusters

Packing transitions in the lowest energy structures of Li clusters as a function of size have been identified via simulated annealing. For N>21, the large $p$ character of Li leads to unexpected ionic structures. At N~25, a packing pattern based on interpenetrating 13-atom icosahedra and similar to that of Na and K appears. This pattern persists until at N=55, where another transition to a structure based on a Mackay icosahedron occurs. For clusters of size 55 and 147, the optimized FCC structure representative of the bulk is still slightly higher in energy than the optimal MIC. (RK-94-03)

chem-ph↗

Viscosities of the Gay-Berne nematic liquid crystal

We present molecular dynamics simulation measurements of the viscosities of the Gay-Berne phenomenological model of liquid crystals in the nematic and isotropic phases. The temperature dependence of the rotational and shear viscosities, including the nonmonotonic behavior of one shear viscosity are in good agreement with experimental data. The bulk viscosities are significantly larger than the shear viscosities, again in agreement with experiment.

cond-mat↗

Coherent Control of Isotope Separation in HD+ Photodissociation by Strong Fields

The photodissociation of the HD+ molecular ion in intense short- pulsed linearly polarized laser fields is studied using a time- dependent wave-packet approach where molecular rotation is fully included. We show that applying a coherent superposition of the fundamental radiation with its second harmonic can lead to asymmetries in the fragment angular distributions, with significant differences between the hydrogen and deuterium distributions in the long wavelength domain where the permanent dipole is most efficient. This effect is used to induce an appreciable isotope separation.

chem-ph↗

Molecular geometry optimization with a genetic algorithm

We present a method for reliably determining the lowest energy structure of an atomic cluster in an arbitrary model potential. The method is based on a genetic algorithm, which operates on a population of candidate structures to produce new candidates with lower energies. Our method dramatically outperforms simulated annealing, which we demonstrate by applying the genetic algorithm to a tight-binding model potential for carbon. With this potential, the algorithm efficiently finds fullerene cluster structures up to ${\rm C}_{60}$ starting from random atomic coordinates.

mtrl-th↗

Dynamical simulation of transport in one-dimensional quantum wires

Transport of single-channel spinless interacting fermions (Luttinger liquid) through a barrier has been studied by numerically exact quantum Monte Carlo methods. A novel stochastic integration over the real-time paths allows for direct computation of nonequilibrium conductance and noise properties. We have examined the low-temperature scaling of the conductance in the crossover region between a very weak and an almost insulating barrier.

cond-mat↗

Nuclear spin--rotation interaction in the hydrogen molecular ion

The nuclear spin--rotation interaction in the hyperfine structure of the hydrogen molecular ion is investigated. The interaction constants are determined and are found to differ in sign and magnitude compared to another theory, but they are in agreement with some values derived from experiment.

atom-ph↗

A Blocking Technique for Emulating Very Large Polyelectrolytes

A new Monte Carlo method for computing thermodynamical properties of very large polyelectrolytes is presented. It is based on a renormalization group relating the original polymer to a smaller system, where in addition to the naively rescaled forces, a corrective nearest-neighbor interaction originating from the short distance Coulomb cutoff is introduced. The method is derived for low T but is in the unscreened case valid for all T. Large polymers with N monomers are emulated by Monte Carlo calculations on smaller systems, K=N/Q. The computational gain of the method is Q^3. It is explored with emphasis on room temperature. Results for N=10000 are presented.

chem-ph↗

Fluid mixtures of parallel hard cubes

The direct correlation function of a fluid mixture of parallel hard cubes is obtained by using Rosenfeld's fundamental measure approximation. This approximation is thermodynamically consistent (compressibility and virial equations of state are equal) and predicts a spinodal instability of the binary mixture for large-to-small side ratio larger than roughly 10, in qualitative agreement with simulations on the lattice version of the model. In two dimensions the system never demix, also in agreement with the simulations.

cond-mat↗