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Register a new userSurvival in equilibrium step fluctuations
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Magdalena Constantin
Publication date
2003
fields
Physics
and research's language is
English
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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.
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Results of analytic and numerical investigations of first-passage properties of equilibrium fluctuations of monatomic steps on a vicinal surface are reviewed. Both temporal and spatial persistence and survival probabilities, as well as the probability of persistent large deviations are considered. Results of experiments in which dynamical scanning tunneling microscopy is used to evaluate these first-passage properties for steps with different microscopic mechanisms of mass transport are also presented and interpreted in terms of theoretical predictions for appropriate models. Effects of discrete sampling, finite system size and finite observation time, which are important in understanding the results of experiments and simulations, are discussed.
The effects of sampling rate and total measurement time have been determined for single-point measurements of step fluctuations within the context of first-passage properties. Time dependent STM has been used to evaluate step fluctuations on Ag(111) films grown on mica as a function of temperature (300-410 K), on screw dislocations on the facets of Pb crystallites at 320K, and on Al-terminated Si(111) over the temperature range 770K - 970K. Although the fundamental time constant for step fluctuations on Ag and Al/Si varies by orders of magnitude over the temperature ranges of measurement, no dependence of the persistence amplitude on temperature is observed. Instead, the persistence probability is found to scale directly with t/Dt where Dt is the time interval used for sampling. Survival probabilities show a more complex scaling dependence which includes both the sampling interval and the total measurement time tm. Scaling with t/Dt occurs only when Dt/tm is a constant. We show that this observation is equivalent to theoretical predictions that the survival probability will scale as Dt/L^z, where L is the effective length of a step. This implies that the survival probability for large systems, when measured with fixed values of tm or Dt should also show little or no temperature dependence.
Time dependent STM has been used to evaluate step fluctuations as a function of temperature (300-450 K) on Ag(111) films grown on mica. The temporal correlation function scales as a power law in time, t^1/n with measured values of 1/n varying over a range of 0.19 pm 0.04 to 0.29 pm 0.04 with no dependence on temperature. The average value of 1/n = 0.24 pm 0.01 is consistent with step-edge diffusion limited fluctuations (n = z = 4, conserved noise). The magnitude of the time correlation function and the width of the fluctuations both scale with temperature with the same apparent activation energy of Eeff = 0.21 pm 0.02 eV, indicating that the correlation time is at most weakly temperature dependent. Direct analysis of the autocorrelation function confirms that the correlation time is at most weakly temperature dependent, and thus the apparent correlation length is strongly temperature dependent. This behavior can be reproduced by assuming that the apparent correlation length is governed by the longest wavelength of step fluctuations that can be sampled in the measurement time interval. Evaluation of the correlation time for previous measurements for Al/Si(111) (z =2) yields the same conclusion about measurement time interval. In both cases the ratio of the measurement time to the effective correlation time is on the order of 10.
Condensation of fluctuations is an interesting phenomenon conceptually distinct from condensation on average. One stricking feature is that, contrary to what happens on average, condensation of fluctuations may occurr even in the absence of interaction. The explanation emerges from the duality between large deviation events in the given system and typical events in a new and appropriately biased system. This surprising phenomenon is investigated in the context of the Gaussian model, chosen as paradigmatical non interacting system, before and after an istantaneous temperature quench. It is shown that the bias induces a mean-field-like effective interaction responsible of the condensation on average. Phase diagrams, covering both the equilibrium and the off-equilibrium regimes, are derived for observables representative of generic behaviors.
We consider the thermodynamic behavior of local fluctuations occurring in a stable or metastable bulk phase. For a system with three or more phases, a simple analysis based on classical nucleation theory predicts that small fluctuations always resemble the phase having the lowest surface tension with the surrounding bulk phase, regardless of the relative chemical potentials of the phases. We also identify the conditions at which a fluctuation may convert to a different phase as its size increases, referred to here as a fluctuation phase transition (FPT). We demonstrate these phenonena in simulations of a two dimensional lattice model by evaluating the free energy surface that describes the thermodynamic properties of a fluctuation as a function of its size and phase composition. We show that a FPT can occur in the fluctuations of either a stable or metastable bulk phase and that the transition is first-order. We also find that the FPT is bracketed by well-defined spinodals, which place limits on the size of fluctuations of distinct phases. Furthermore, when the FPT occurs in a metastable bulk phase, we show that the superposition of the FPT on the nucleation process results in two-step nucleation (TSN). We identify distinct regimes of TSN based on the nucleation pathway in the free energy surface, and correlate these regimes to the phase diagram of the bulk system. Our results clarify the origin of TSN, and elucidate a wide variety of phenomena associated with TSN, including the Ostwald step rule.
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