Understanding and Controlling Regime Switching in Molecular Diffusion

Diffusion can be strongly affected by ballistic flights (long jumps) as well as long-lived sticking trajectories (long sticks). Using statistical inference techniques in the spirit of Granger causality, we investigate the appearance of long jumps and sticks in molecular-dynamics simulations of diffusion in a prototype system, a benzene molecule on a graphite substrate. We find that specific fluctuations in certain, but not all, internal degrees of freedom of the molecule can be linked to either long jumps or sticks. Furthermore, by changing the prevalence of these predictors with an outside influence, the diffusion of the molecule can be controlled. The approach presented in this proof of concept study is very generic, and can be applied to larger and more complex molecules. Additionally, the predictor variables can be chosen in a general way so as to be accessible in experiments, making the method feasible for control of diffusion in applications. Our results also demonstrate that data-mining techniques can be used to investigate the phase-space structure of high-dimensional nonlinear dynamical systems.Comment: accepted for publication by PR

(In)commensurability, scaling and multiplicity of friction in nanocrystals and application to gold nanocrystals on graphite

The scaling of friction with the contact size $A$ and (in)commensurabilty of nanoscopic and mesoscopic crystals on a regular substrate are investigated analytically for triangular nanocrystals on hexagonal substrates. The crystals are assumed to be stiff, but not completely rigid. Commensurate and incommensurate configurations are identified systematically. It is shown that three distinct friction branches coexist, an incommensurate one that does not scale with the contact size ($A^0$) and two commensurate ones which scale differently (with $A^{1/2}$ and $A$) and are associated with various combinations of commensurate and incommensurate lattice parameters and orientations. This coexistence is a direct consequence of the two-dimensional nature of the contact layer, and such multiplicity exists in all geometries consisting of regular lattices. To demonstrate this, the procedure is repeated for rectangular geometry. The scaling of irregularly shaped crystals is also considered, and again three branches are found ($A^{1/4}, A^{3/4}, A$). Based on the scaling properties, a quantity is defined which can be used to classify commensurability in infinite as well as finite contacts. Finally, the consequences for friction experiments on gold nanocrystals on graphite are discussed

Criticality in Dynamic Arrest: Correspondence between Glasses and Traffic

Dynamic arrest is a general phenomenon across a wide range of dynamic systems, but the universality of dynamic arrest phenomena remains unclear. We relate the emergence of traffic jams in a simple traffic flow model to the dynamic slow down in kinetically constrained models for glasses. In kinetically constrained models, the formation of glass becomes a true (singular) phase transition in the limit $T\to 0$. Similarly, using the Nagel-Schreckenberg model to simulate traffic flow, we show that the emergence of jammed traffic acquires the signature of a sharp transition in the deterministic limit \pp\to 1, corresponding to overcautious driving. We identify a true dynamical critical point marking the onset of coexistence between free flowing and jammed traffic, and demonstrate its analogy to the kinetically constrained glass models. We find diverging correlations analogous to those at a critical point of thermodynamic phase transitions.Comment: 4 pages, 4 figure

Chaotic properties of spin lattices near second-order phase transitions

We perform a numerical investigation of the Lyapunov spectra of chaotic dynamics in lattices of classical spins in the vicinity of second-order ferromagnetic and antiferromagnetic phase transitions. On the basis of this investigation, we identify a characteristic of the shape of the Lyapunov spectra, the "G-index", which exhibits a sharp peak as a function of temperature at the phase transition, provided the order parameter is capable of sufficiently strong dynamic fluctuations. As a part of this work, we also propose a general numerical algorithm for determining the temperature in many-particle systems, where kinetic energy is not defined.Comment: 9 pages, 11 figure

Lyapunov spectra of billiards with cylindrical scatterers: comparison with many-particle systems

The dynamics of a system consisting of many spherical hard particles can be described as a single point particle moving in a high-dimensional space with fixed hypercylindrical scatterers with specific orientations and positions. In this paper, the similarities in the Lyapunov exponents are investigated between systems of many particles and high-dimensional billiards with cylindrical scatterers which have isotropically distributed orientations and homogeneously distributed positions. The dynamics of the isotropic billiard are calculated using a Monte-Carlo simulation, and a reorthogonalization process is used to find the Lyapunov exponents. The results are compared to numerical results for systems of many hard particles as well as the analytical results for the high-dimensional Lorentz gas. The smallest three-quarters of the positive exponents behave more like the exponents of hard-disk systems than the exponents of the Lorentz gas. This similarity shows that the hard-disk systems may be approximated by a spatially homogeneous and isotropic system of scatterers for a calculation of the smaller Lyapunov exponents, apart from the exponent associated with localization. The method of the partial stretching factor is used to calculate these exponents analytically, with results that compare well with simulation results of hard disks and hard spheres.Comment: Submitted to PR

Goldstone modes in Lyapunov spectra of hard sphere systems

In this paper, we demonstrate how the Lyapunov exponents close to zero of a system of many hard spheres can be described as Goldstone modes, by using a Boltzmann type of approach. At low densities, the correct form is found for the wave number dependence of the exponents as well as for the corresponding eigenvectors in tangent-space. The predicted values for the Lyapunov exponents belonging to the transverse mode are within a few percent of the values found in recent simulations, the propagation velocity for the longitudinal mode is within 1%, but the value for the Lyapunov exponent belonging to the longitudinal mode deviates from the simulations by 30%. For higher densities, the predicted values deviate more from the values calculated in the simulations. These deviations may be due to contributions from ring collisions and similar terms, which, even at low densities, can contribute to the leading order.Comment: 12 pages revtex, 5 figures, accepted by Physical Review

The Lyapunov spectrum of the many-dimensional dilute random Lorentz gas

For a better understanding of the chaotic behavior of systems of many moving particles it is useful to look at other systems with many degrees of freedom. An interesting example is the high-dimensional Lorentz gas, which, just like a system of moving hard spheres, may be interpreted as a dynamical system consisting of a point particle in a high-dimensional phase space, moving among fixed scatterers. In this paper, we calculate the full spectrum of Lyapunov exponents for the dilute random Lorentz gas in an arbitrary number of dimensions. We find that the spectrum becomes flatter with increasing dimensionality. Furthermore, for fixed collision frequency the separation between the largest Lyapunov exponent and the second largest one increases logarithmically with dimensionality, whereas the separations between Lyapunov exponents of given indices not involving the largest one, go to fixed limits.Comment: 8 pages, revtex, 6 figures, submitted to Physical Review