Dynamic Monte Carlo Simulations of Anisotropic Colloids

We put forward a simple procedure for extracting dynamical information from Monte Carlo simulations, by appropriate matching of the short-time diffusion tensor with its infinite-dilution limit counterpart, which is supposed to be known. This approach --discarding hydrodynamics interactions-- first allows us to improve the efficiency of previous Dynamic Monte Carlo algorithms for spherical Brownian particles. In a second step, we address the case of anisotropic colloids with orientational degrees of freedom. As an illustration, we present a detailed study of the dynamics of thin platelets, with emphasis on long-time diffusion and orientational correlations.Comment: 12 pages, 9 figure

Speckle visibility spectroscopy and variable granular fluidization

We introduce a dynamic light scattering technique capable of resolving motion that changes systematically, and rapidly, with time. It is based on the visibility of a speckle pattern for a given exposure duration. Applying this to a vibrated layer of glass beads, we measure the granular temperature and its variation with phase in the oscillation cycle. We observe several transitions involving jammed states, where the grains are at rest during some portion of the cycle. We also observe a two-step decay of the temperature on approach to jamming.Comment: 4 pages, 4 figures, experimen

Unexpected Effect of Internal Degrees of Freedom on Transverse Phonons in Supercooled Liquids

We show experimentally that in a supercooled liquid composed of molecules with internal degrees of freedom the internal modes contribute to the frequency dependent shear viscosity and damping of transverse phonons, which results in an additional broadening of the transverse Brillouin lines. Earlier, only the effect of internal modes on the frequency dependent bulk viscosity and damping of longitudinal phonons was observed and explained theoretically in the limit of weak coupling of internal degrees of freedom to translational motion. A new theory is needed to describe this new effect. We also demonstrate, that the contributions of structural relaxation and internal processes to the width of the Brillouin lines can be separated by measurements under high pressure

Dynamic correlations in stochastic rotation dynamics

The dynamic structure factor, vorticity and entropy density dynamic correlation functions are measured for Stochastic Rotation Dynamics (SRD), a particle based algorithm for fluctuating fluids. This allows us to obtain unbiased values for the longitudinal transport coefficients such as thermal diffusivity and bulk viscosity. The results are in good agreement with earlier numerical and theoretical results, and it is shown for the first time that the bulk viscosity is indeed zero for this algorithm. In addition, corrections to the self-diffusion coefficient and shear viscosity arising from the breakdown of the molecular chaos approximation at small mean free paths are analyzed. In addition to deriving the form of the leading correlation corrections to these transport coefficients, the probabilities that two and three particles remain collision partners for consecutive time steps are derived analytically in the limit of small mean free path. The results of this paper verify that we have an excellent understanding of the SRD algorithm at the kinetic level and that analytic expressions for the transport coefficients derived elsewhere do indeed provide a very accurate description of the SRD fluid.Comment: 33 pages including 16 figure

Resolving long-range spatial correlations in jammed colloidal systems using photon correlation imaging

We introduce a new dynamic light scattering method, termed photon correlation imaging, which enables us to resolve the dynamics of soft matter in space and time. We demonstrate photon correlation imaging by investigating the slow dynamics of a quasi two-dimensional coarsening foam made of highly packed, deformable bubbles and a rigid gel network formed by dilute, attractive colloidal particles. We find the dynamics of both systems to be determined by intermittent rearrangement events. For the foam, the rearrangements extend over a few bubbles, but a small dynamical correlation is observed up to macroscopic length scales. For the gel, dynamical correlations extend up to the system size. These results indicate that dynamical correlations can be extremely long-ranged in jammed systems and point to the key role of mechanical properties in determining their nature.Comment: Published version (Phys. Rev. Lett. 102, 085702 (2009)) The Dynamical Activity Mapsprovided as Supplementary Online Material are also available on http://w3.lcvn.univ-montp2.fr/~lucacip/dam/movies.ht

Quantized time correlation function approach to non-adiabatic decay rates in condensed phase: Application to solvated electrons in water and methanol

A new, alternative form of the golden rule formula defining the non-adiabatic transition rate between two quantum states in condensed phase is presented. The formula involves the quantum time correlation function of the energy gap, of the non-adiabatic coupling, and their cross terms. Those quantities can be inferred from their classical counterparts, determined via MD simulations. The formalism is applied to the problem of the non-adiabatic relaxation of an equilibrated p-electron in water and methanol. We find that, in both solvent, the relaxation is induced by the coupling to the vibrational modes and the quantum effects modify the rate by a factor of 2-10 depending on the quantization procedure applied. The resulting p-state lifetime for a hypothetical equilibrium excited state appears extremely short, in the sub-100 fs regime. Although this result is in contrast with all previous theoretical predictions, we also illustrate that the lifetimes computed here are very sensitive to the simulated electronic quantum gap and to the strongly correlated non-adiabatic coupling

Reconstruction of thermally-symmetrized quantum autocorrelation functions from imaginary-time data

In this paper, I propose a technique for recovering quantum dynamical information from imaginary-time data via the resolution of a one-dimensional Hamburger moment problem. It is shown that the quantum autocorrelation functions are uniquely determined by and can be reconstructed from their sequence of derivatives at origin. A general class of reconstruction algorithms is then identified, according to Theorem 3. The technique is advocated as especially effective for a certain class of quantum problems in continuum space, for which only a few moments are necessary. For such problems, it is argued that the derivatives at origin can be evaluated by Monte Carlo simulations via estimators of finite variances in the limit of an infinite number of path variables. Finally, a maximum entropy inversion algorithm for the Hamburger moment problem is utilized to compute the quantum rate of reaction for a one-dimensional symmetric Eckart barrier.Comment: 15 pages, no figures, to appear in Phys. Rev.

On the origin of the λ\lambda-transition in liquid Sulphur

Developing a novel experimental technique, we applied photon correlation spectroscopy using infrared radiation in liquid Sulphur around $T_\lambda$, i.e. in the temperature range where an abrupt increase in viscosity by four orders of magnitude is observed upon heating within few degrees. This allowed us - overcoming photo-induced and absorption effects at visible wavelengths - to reveal a chain relaxation process with characteristic time in the ms range. These results do rehabilitate the validity of the Maxwell relation in Sulphur from an apparent failure, allowing rationalizing the mechanical and thermodynamic behavior of this system within a viscoelastic scenario.Comment: 5 pages, 4 eps figures, accepted in Phys. Rev. Let

Quantum Monte Carlo Dynamics: the Stationary Phase Monte Carlo Path Integral Calculation of Finite Temperature Time Correlation Functions

We present a numerically exact procedure for the calculation of an important class of finite temperature quantum mechanical time correlation functions. The present approach is based around the stationary phase Monte Carlo (SPMC) method, a general mathematical tool for the calculation of high dimensional averages of oscillatory integrands. In the present context the method makes possible the direct numerical path integral calculation of real-time quantum dynamical quantities for times appreciably greater than the thermal time (βħ). Illustrative applications involving finite temperature anharmonic motion are presented. Issues of importance with respect to future applications are identified and discussed

First science results from SOFIA/FORCAST: The mid-infrared view of the compact HII region W3A

The massive star forming region W3 was observed with the faint object infrared camera for the SOFIA telescope (FORCAST) as part of the Short Science program. The 6.4, 6.6, 7.7, 19.7, 24.2, 31.5 and 37.1 \um bandpasses were used to observe the emission of Polycyclic Aromatic Hydrocarbon (PAH) molecules, Very Small Grains and Big Grains. Optical depth and color temperature maps of W3A show that IRS2 has blown a bubble devoid of gas and dust of $\sim$0.05 pc radius. It is embedded in a dusty shell of ionized gas that contributes 40% of the total 24 \um emission of W3A. This dust component is mostly heated by far ultraviolet, rather than trapped Ly$\alpha$ photons. This shell is itself surrounded by a thin ($\sim$0.01 pc) photodissociation region where PAHs show intense emission. The infrared spectral energy distribution (SED) of three different zones located at 8, 20 and 25\arcsec from IRS2, show that the peak of the SED shifts towards longer wavelengths, when moving away from the star. Adopting the stellar radiation field for these three positions, DUSTEM model fits to these SEDs yield a dust-to-gas mass ratio in the ionized gas similar to that in the diffuse ISM. However, the ratio of the IR-to-UV opacity of the dust in the ionized shell is increased by a factor $\simeq$3 compared to the diffuse ISM.Comment: Accepted for publication in ApJ letters; 13 pages, 3 figures 1 tabl