Glycerol confined in zeolitic imidazolate frameworks: The temperature-dependent cooperativity length scale of glassy freezing

In the present work, we employ broadband dielectric spectroscopy to study the molecular dynamics of the prototypical glass former glycerol confined in two microporous zeolitic imidazolate frameworks (ZIF-8 and ZIF-11) with well-defined pore diameters of 1.16 and 1.46 nm, respectively. The spectra reveal information on the modified alpha relaxation of the confined supercooled liquid, whose temperature dependence exhibits clear deviations from the typical super-Arrhenius temperature dependence of the bulk material, depending on temperature and pore size. This allows assigning well-defined cooperativity length scales of molecular motion to certain temperatures above the glass transition. We relate these and previous results on glycerol confined in other host systems to the temperature-dependent length scale deduced from nonlinear dielectric measurements. The combined experimental data can be consistently described by a critical divergence of this correlation length as expected within theoretical approaches assuming that the glass transition is due to an underlying phase transition.Comment: 14 pages, 5 figures + Supplemental Material (4 pages, 6 figures). Final version as accepted for publicatio

Pink noise of ionic conductance through single artificial nanopores revisited

We report voltage-clamp measurements through single conical nanopore obtained by chemical etching of a single ion-track in polyimide film. Special attention is paid on the pink noise of the ionic current (i.e. $1/f$ noise) measured with different filling liquids. The relative pink noise amplitude is almost independent of concentration and pH for KCl solutions, but varies strongly using ionic liquids. In particular we show that depending on the ionic liquid, the transport of charge carriers is strongly facilitated (low noise and higher conductivity than in the bulk) or jammed. These results show that the origin of the pink noise can be ascribed neither to fluctuations of the pore geometry nor to the pore wall charges but rather to a cooperative effect on ions motion

Extreme accumulation of nucleotides in simulated hydrothermal pore systems

We simulate molecular transport in elongated hydrothermal pore systems influenced by a thermal gradient. We find extreme accumulation of molecules in a wide variety of plugged pores. The mechanism is able to provide highly concentrated single nucleotides, suitable for operations of an RNA world at the origin of life. It is driven solely by the thermal gradient across a pore. On the one hand, the fluid is shuttled by thermal convection along the pore, whereas on the other hand, the molecules drift across the pore, driven by thermodiffusion. As a result, millimeter-sized pores accumulate even single nucleotides more than 108-fold into micrometer-sized regions. The enhanced concentration of molecules is found in the bulk water near the closed bottom end of the pore. Because the accumulation depends exponentially on the pore length and temperature difference, it is considerably robust with respect to changes in the cleft geometry and the molecular dimensions. Whereas thin pores can concentrate only long polynucleotides, thicker pores accumulate short and long polynucleotides equally well and allow various molecular compositions. This setting also provides a temperature oscillation, shown previously to exponentially replicate DNA in the protein-assisted PCR. Our results indicate that, for life to evolve, complicated active membrane transport is not required for the initial steps. We find that interlinked mineral pores in a thermal gradient provide a compelling high-concentration starting point for the molecular evolution of life

Microscopic Motion of Particles Flowing through a Porous Medium

We use Stokesian Dynamics simulations to study the microscopic motion of particles suspended in fluids passing through porous media. We construct model porous media with fixed spherical particles, and allow mobile ones to move through this fixed bed under the action of an ambient velocity field. We first consider the pore scale motion of individual suspended particles at pore junctions. The relative particle flux into different possible directions exiting from a single pore, for two and three dimensional model porous media is found to approximately equal the corresponding fractional channel width or area. Next we consider the waiting time distribution for particles which are delayed in a junction, due to a stagnation point caused by a flow bifurcation. The waiting times are found to be controlled by two-particle interactions, and the distributions take the same form in model porous media as in two-particle systems. A simple theoretical estimate of the waiting time is consistent with the simulations. We also find that perturbing such a slow-moving particle by another nearby one leads to rather complicated behavior. We study the stability of geometrically trapped particles. For simple model traps, we find that particles passing nearby can ``relaunch'' the trapped particle through its hydrodynamic interaction, although the conditions for relaunching depend sensitively on the details of the trap and its surroundings.Comment: 16 pages, 19 figure

Inelastic electron tunneling spectroscopy of nanoporous gold films

We investigated the localized electronic properties of nanoporous gold films by using an ultra-high vacuum scanning tunneling microscope at low temperature (4.2 K). Second derivative scanning tunneling spectroscopy shows the plasmon peaks of the nanoporous gold films, which are excited by inelastic tunneling electrons. We propose that the nanorod model is appropriate for nanoporous gold studies at the nanometer-scale. These results are supported by a 3D electron tomography analysis and theoretical calculations of nanoporous gold with ellipsoid shape.Comment: 6 pages, 3 figures. This is the authors' version. The published, high resolution version of this paper, Copyright (2014) by the American Physical Society, can be found at http://journals.aps.org/prb

Wave propagation and shock formation in different magnetic structures

Velocity oscillations "measured" simultaneously at the photosphere and the chromosphere -from time series of spectropolarimetric data in the 10830 A region- of different solar magnetic features allow us to study the properties of wave propagation as a function of the magnetic flux of the structure (i.e. two different-sized sunspots, a tiny pore and a facular region). While photospheric oscillations have similar characteristics everywhere, oscillations measured at chromospheric heights show different amplitudes, frequencies and stages of shock development depending on the observed magnetic feature. The analysis of the power and the phase spectra, together with simple theoretical modeling, lead to a series of results concerning wave propagation within the range of heights of this study. We find that, while the atmospheric cut-off frequency and the propagation properties of the different oscillating modes depend on the magnetic feature, in all the cases the power that reaches the high chromosphere above the atmospheric cut-off comes directly from the photosphere by means of linear vertical wave propagation rather than from non-linear interaction of modes.Comment: Accepted for publication in The Astrophysical Journal. 29 pages, 9 figures, 12pt, preprin