Particle formation by ion nucleation in the upper troposphere and lower stratosphere.

Unexpectedly high concentrations of ultrafine particles were observed over a wide range of latitudes in the upper troposphere and lower stratosphere. Particle number concentrations and size distributions simulated by a numerical model of ion-induced nucleation, constrained by measured thermodynamic data and observed atmospheric key species, were consistent with the observations. These findings indicate that, at typical upper troposphere and lower stratosphere conditions, particles are formed by this nucleation process and grow to measurable sizes with sufficient sun exposure and low preexisting aerosol surface area. Ion-induced nucleation is thus a globally important source of aerosol particles, potentially affecting cloud formation and radiative transfer.

The seasonal evolution of reactive chlorine in the northern hemisphere stratosphere.

In situ measurements of chlorine monoxide (ClO) at mid- and high northern latitudes are reported for the period October 1991 to February 1992. As early as mid-December and throughout the winter, significant enhancements of this ozone-destroying radical were observed within the polar vortex shortly after temperatures dropped below 195 k. Decreases in ClO observed in February were consistent with the rapid formation of chlorine nitrate (ClONO(2)) by recombination of ClO with nitrogen dioxide (NO(2)) released photochemically from nitric acid (HNO(3)). Outside the vortex, ClO abundances were higher than in previous years as a result of NOx suppression by heterogeneous reactions on sulfate aerosols enhanced by the eruption of Mount Pinatubo.

Stratospheric meteorological conditions in the arctic polar vortex, 1991 to 1992.

Stratospheric meteorological conditions during the Airborne Arctic Stratospheric Expedition II (AASE II) presented excellent observational opportunities from Bangor, Maine, because the polar vortex was located over southeastern Canada for significant periods during the 1991-1992 winter. Temperature analyses showed that nitric acid trihydrates (NAT temperatures below 195 k) should have formed over small regions in early December. The temperatures in the polar vortex warmed beyond NAT temperatures by late January (earlier than normal). Perturbed chemistry was found to be associated with these cold temperatures.

Chemical loss of ozone in the arctic polar vortex in the winter of 1991-1992.

In situ measurements of chlorine monoxide, bromine monoxide, and ozone are extrapolated globally, with the use of meteorological tracers, to infer the loss rates for ozone in the Arctic lower stratosphere during the Airborne Arctic Stratospheric Expedition II (AASE II) in the winter of 1991-1992. The analysis indicates removal of 15 to 20 percent of ambient ozone because of elevated concentrations of chlorine monoxide and bromine monoxide. Observations during AASE II define rates of removal of chlorine monoxide attributable to reaction with nitrogen dioxide (produced by photolysis of nitric acid) and to production of hydrochloric acid. Ozone loss ceased in March as concentrations of chlorine monoxide declined. Ozone losses could approach 50 percent if regeneration of nitrogen dioxide were inhibited by irreversible removal of nitrogen oxides (denitrification), as presently observed in the Antarctic, or without denitrification if inorganic chlorine concentrations were to double.