468 research outputs found

    One-laser interferometric broadband coherent anti-Stokes Raman scattering

    Get PDF
    We introduce an interferometric technique for eliminating the non-resonant background of broadband coherent anti-Stokes Raman scattering (CARS) microscopy. CARS microscopy has been used for imaging a number of biological samples and processes, but the studies are mostly limited to detecting lipids in biological systems by probing the C-H stretch. Non-resonant background and incoherent noise sources can easily overwhelm less intense signals from other molecular vibrations. In this study, we demonstrate a one-laser broadband interferometric technique that separates the spontaneous Raman scattering-related component of the CARS signal from the non-resonant background using liquid benzonitrile as a model system.Tak W. Kee, Hongxia Zhao, and Marcus T. Ciceron

    Heterogeneous Diffusion in Highly Supercooled Liquids

    Full text link
    The diffusivity of tagged particles is demonstrated to be very heterogeneous on time scales comparable to or shorter than the α\alpha relaxation time τα\tau_{\alpha} (\cong the stress relaxation time) in a highly supercooled liquid via 3D molecular dynamics simulation. The particle motions in the relatively active regions dominantly contribute to the mean square displacement, giving rise to a diffusion constant systematically larger than the Einstein-Stokes value. The van Hove self-correlation function Gs(r,t)G_s(r,t) is shown to have a long distance tail which can be scaled in terms of r/t1/2r/t^{1/2} for t \ls 3\tau_{\alpha}. Its presence indicates heterogeneous diffusion in the active regions. However, the diffusion process eventually becomes homogeneous on time scales longer than the life time of the heterogeneity structure (3τα\sim 3 \tau_{\alpha}).Comment: 4 pages, 5 figure

    Dynamical heterogeneities in a supercooled Lennard-Jones liquid

    Full text link
    We present the results of a large scale molecular dynamics computer simulation study in which we investigate whether a supercooled Lennard-Jones liquid exhibits dynamical heterogeneities. We evaluate the non-Gaussian parameter for the self part of the van Hove correlation function and use it to identify ``mobile'' particles. We find that these particles form clusters whose size grows with decreasing temperature. We also find that the relaxation time of the mobile particles is significantly shorter than that of the bulk, and that this difference increases with decreasing temperature.Comment: 8 pages of RevTex, 4 ps figure

    Anisotropic Local Stress and Particle Hopping in a Deeply Supercooled Liquid

    Get PDF
    The origin of the microscopic motions that lead to stress relaxation in deeply supercooled liquid remains unclear. We show that in such a liquid the stress relaxation is locally anisotropic which can serve as the driving force for the hopping of the system on its free energy surface. However, not all hopping are equally effective in relaxing the local stress, suggesting that diffusion can decouple from viscosity even at local level. On the other hand, orientational relaxation is found to be always coupled to stress relaxation.Comment: 4 pages, 3 figure

    Structural Relaxation, Self Diffusion and Kinetic Heterogeneity in the Two Dimensional Lattice Coulomb Gas

    Full text link
    We present Monte Carlo simulation results on the equilibrium relaxation dynamics in the two dimensional lattice Coulomb gas, where finite fraction ff of the lattice sites are occupied by positive charges. In the case of high order rational values of ff close to the irrational number 1g1-g (g(51)/2g\equiv(\sqrt{5} -1)/2 is the golden mean), we find that the system exhibits, for wide range of temperatures above the first-order transition, a glassy behavior resembling the primary relaxation of supercooled liquids. Single particle diffusion and structural relaxation show that there exists a breakdown of proportionality between the time scale of diffusion and that of structural relaxation analogous to the violation of the Stokes-Einstein relation in supercooled liquids. Suitably defined dynamic cooperativity is calculated to exhibit the characteristic nature of dynamic heterogeneity present in the system.Comment: 12 pages, 20 figure

    String-like Clusters and Cooperative Motion in a Model Glass-Forming Liquid

    Full text link
    A large-scale molecular dynamics simulation is performed on a glass-forming Lennard-Jones mixture to determine the nature of dynamical heterogeneities which arise in this model fragile liquid. We observe that the most mobile particles exhibit a cooperative motion in the form of string-like paths (``strings'') whose mean length and radius of gyration increase as the liquid is cooled. The length distribution of the strings is found to be similar to that expected for the equilibrium polymerization of linear polymer chains.Comment: 6 pages of RevTex, 6 postscript figures, uses epsf.st

    Hole-burning experiments within solvable glassy models

    Full text link
    We reproduce the results of non-resonant spectral hole-burning experiments with fully-connected (equivalently infinite-dimensional) glassy models that are generalizations of the mode-coupling approach to nonequilibrium situations. We show that an ac-field modifies the integrated linear response and the correlation function in a way that depends on the amplitude and frequency of the pumping field. We study the effect of the waiting and recovery-times and the number of oscillations applied. This calculation will help descriminating which results can and which cannot be attributed to dynamic heterogeneities in real systems.Comment: 4 pages, 8 figures, RevTe

    Spectroscopic Detection of Stratospheric Hydrogen Cyanide

    Full text link
    corecore