Experimental Persistence Probability for Fluctuating Steps

The persistence behavior for fluctuating steps on the $Si(111)$ $(\sqrt3 \times \sqrt3)R30^{0} - Al$ surface was determined by analyzing time-dependent STM images for temperatures between 770 and 970K. The measured persistence probability follows a power law decay with an exponent of $\theta=0.77 \pm 0.03$. This is consistent with the value of $\theta= 3/4$ predicted for attachment/detachment limited step kinetics. If the persistence analysis is carried out in terms of return to a fixed reference position, the measured persistence probability decays exponentially. Numerical studies of the Langevin equation used to model step motion corroborate the experimental observations.Comment: LaTeX, 11 pages, 4 figures, minor changes in References sectio

Survival in equilibrium step fluctuations

We report the results of analytic and numerical investigations of the time scale of survival or non-zero-crossing probability $S(t)$ in equilibrium step fluctuations described by Langevin equations appropriate for attachment/detachment and edge-diffusion limited kinetics. An exact relation between long-time behaviors of the survival probability and the autocorrelation function is established and numerically verified. $S(t)$ is shown to exhibit simple scaling behavior as a function of system size and sampling time. Our theoretical results are in agreement with those obtained from an analysis of experimental dynamical STM data on step fluctuations on Al/Si(111) and Ag(111) surfaces.Comment: RevTeX, 4 pages, 3 figure

Distinguishing step relaxation mechanisms via pair correlation functions

Theoretical predictions of coupled step motion are tested by direct STM measurement of the fluctuations of near-neighbor pairs of steps on Si(111)-root3 x root3 R30 - Al at 970K. The average magnitude of the pair-correlation function is within one standard deviation of zero, consistent with uncorrelated near-neighbor step fluctuations. The time dependence of the pair-correlation function shows no statistically significant agreement with the predicted t^1/2 growth of pair correlations via rate-limiting atomic diffusion between adjacent steps. The physical considerations governing uncorrelated step fluctuations occurring via random attachment/detachment events at the step edge are discussed.Comment: 17 pages, 4 figure

Nanoscale Equilibrium Crystal Shapes

The finite size and interface effects on equilibrium crystal shape (ECS) have been investigated for the case of a surface free energy density including step stiffness and inverse-square step-step interactions. Explicitly including the curvature of a crystallite leads to an extra boundary condition in the solution of the crystal shape, yielding a family of crystal shapes, governed by a shape parameter c. The total crystallite free energy, including interface energy, is minimized for c=0, yielding in all cases the traditional PT shape (z x3/2). Solutions of the crystal shape for c≠0 are presented and discussed in the context of meta-stable states due to the energy barrier for nucleation. Explicit scaled relationships for the ECS and meta-stable states in terms of the measurable step parameters and the interfacial energy are presented.Comment: 35 page

EMSL and Institute for Integrated Catalysis (IIC) Catalysis Workshop

Within the context of significantly accelerating scientific progress in research areas that address important societal problems, a workshop was held in November 2010 at EMSL to identify specific and topically important areas of research and capability needs in catalysis-related science