Multivariate analysis of homogeneous nucleation rate measurements. Nucleation in the p-toluic acid/sulfuric acid/water system.
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abstract
Recent kinetic extensions of the nucleation theorem suggest that the logarithm of the steady-state nucleation rate has strong multilinear dependence on the log concentrations of condensable species present in the vapor phase. A further remarkable result is that the coefficients of this linear dependency provide a direct determination of the molecular content of the critical nucleus itself. Building on these results, the powerful utility of multivariate statistical methods is demonstrated here for physically based parametrization and interpretation of nucleation rate measurements. The new approach is applied to recent measurements by Zhang et al. [Science 304, 1487 (2004)] on the p-toluic acid/sulfuric acid/water ternary vapor system. A linear minimum variance parametrization for nucleation rate dependence on vapor composition, accurate over the range of the measurements, is obtained. Estimates of critical nucleus molecular composition are also presented. These suggest that a single molecule of p-toluic acid present in the critical nucleus is sufficient to trigger a ternary nucleation event. Efforts under way to apply the new methods to analysis of new particle formation in the atmosphere are discussed.
