New Particle Formation in the Remote Troposphere: A Comparison of Observations at Various Sites

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Abstract
Measurements show that new particles are formed by homogenous nucleation over a wide range of conditions in the remote troposphere. In our studies, large nucleation events are found exclusively in regions of enhanced sulfuric acid vapor (H2SO4g) concentrations, with maximum concentrations never exceeding 5×107 molecules cm−3. Although these data suggest that H2SO4g participated, comparisons between ambient conditions in regions of nucleation to conditions necessary for binary H2SO4 water (H2O) nucleation indicate that the mechanism may vary with elevation. In remote marine regions, at altitudes greater than ∼4 km above sea level, observations of nucleation in clear air along cloud perimeters are in fair agreement with current classical binary nucleation models. In these regions, the low temperatures associated with high altitudes may produce sufficiently saturated H2SO4 for the production of new H2SO4/H2O particles. However, uncertainties with current binary nucleation models limit decisive comparisons. In warmer regions, closer to the earth's surface, measured H2SO4 concentrations are clearly insufficient for binary nucleation. Conditions at these sites are similar to those observed in an earlier study where there was circumstantial evidence for a ternary mechanism involving H2SO4, H2O, and ammonia (NH3) [Weber et al., 1998], suggesting that this may be a significant route for particle production at lower altitudes where surface‐derived species, like NH3, are more apt to participate.