Femtosecond electron diffraction (FED) has the potential to directly observe transition state processes. The relevant motions for this barrier-crossing event occur on the hundred femtosecond time-scale. Recent advances in the development of high-flux electron pulse sources with the required time resolution and sensitivity to capture barrier-crossing processes are described in the context of attaining atomic level details of such structural dynamics-seeing chemical events as they occur. Initial work focused on the ordered-to-disordered phase transition of Al under strong driving conditions for which melting takes on nm or molecular scale dimensions. This work has been extended to Au, which clearly shows a separation in time-scales for lattice heating and melting. It also demonstrates that superheated face-centred cubic (FCC) metals melt through thermal mechanisms involving homogeneous nucleation to propagate the disordering process. A new concept exploiting electron-electron correlation is introduced for pulse characterization and determination of t=0 to within 100fs as well as for spatial manipulation of the electron beam. Laser-based methods are shown to provide further improvements in time resolution with respect to pulse characterization, absolute t=0 determination, and the potential for electron acceleration to energies optimal for time-resolved diffraction.

We investigate the linear stability of a thin, suspended, annular film of conducting fluid with a voltage difference applied between its inner and outer edges. For a sufficiently large voltage, such a film is unstable to radially-driven electroconvection due to charges which develop on its free surfaces. The film can also be subjected to a Couette shear by rotating its inner edge. This combination is experimentally realized using films of smectic A liquid crystals. In the absence of shear, the convective flow consists of a stationary, azimuthally one-dimensional pattern of symmetric, counter-rotating vortex pairs. When Couette flow is applied, an azimuthally traveling pattern results. When viewed in a co-rotating frame, the traveling pattern consists of pairs of asymmetric vortices. We calculate the neutral stability boundary for arbitrary radius ratio α and Reynolds number Re of the shear flow, and obtain the critical control parameter Rc (α, Re) and the critical azimuthal mode number mc (α, Re). The Couette flow suppresses the onset of electroconvection, so that Rc (α, Re) > Rc (α, 0). The calculated suppression is compared with experiments performed at α = 0.56 and 0 ≤ Re ≤ 0.22. Fluids, 11, 3613 (1999). See also http://mobydick.physics.utoronto.ca. Physics of

We report experiments on convection driven by a radial electrical force in suspended annular smectic A liquid crystal films. In the absence of an externally imposed azimuthal shear, a stationary one-dimensional (1D) pattern consisting of symmetric vortex pairs is formed via a supercritical transition at the onset of convection. Shearing reduces the symmetries of the base state and produces a traveling 1D pattern whose basic periodic unit is a pair of asymmetric vortices. For a sufficiently large shear, the primary bifurcation changes from supercritical to subcritical. We describe measurements of the resulting hysteresis as a function of the shear at radius ratio η ∼ 0.8. This simple pattern forming system has an unusual combination of symmetries and control parameters and should be amenable to quantitative theoretical analysis.Typeset using REVT E X 1

It has been experimentally observed that weakly conducting suspended films of smectic liquid crystals undergo electroconvection when subjected to a large enough potential difference. The resulting counter-rotating vortices form a very simple convection pattern and exhibit a variety of interesting nonlinear effects. The linear stability problem for this system has recently been solved. The convection mechanism, which involves charge separation at the free surfaces of the film, is applicable to any sufficiently two-dimensional fluid.In this paper, we derive an amplitude equation which describes the weakly nonlinear regime, by starting from the basic electrohydrodynamic equations. This regime has been the subject of several recent experimental studies. The lowest order amplitude equation we derive is of the Ginzburg-Landau form, and describes a forward bifurcation as is observed experimentally. The coefficients of the amplitude equation are calculated and compared with the values independently deduced from the linear stability calculation.

We use direct numerical simulation to study electrically driven convection in an annular thin film. The simulation models a laboratory experiment that consists of a weakly conducting, submicron thick liquid crystal film suspended between two concentric electrodes. The film is driven to convect by imposing a sufficiently large voltage across it. The flow is driven by a surface charge density inversion which is unstable to the imposed electrical force. This mechanism is closely analogous to the mass density inversion which is unstable to the buoyancy force in conventional, thermally driven Rayleigh-Bénard convection. The simulation uses a pseudospectral method with Chebyshev polynomials in the radial direction and Fourier modes in the azimuthal direction. The numerical results, which are in good agreement with previous experimental data and theoretical predictions, reveal several insights. The mode competition near a codimension-two point exhibits hysteresis. The primary bifurcation is supercritical for a broad range of fluid and geometrical parameters.