Surface crystallization of supercooled water in clouds.

The process by which liquid cloud droplets homogeneously crystallize into ice is still not well understood. The ice nucleation process based on the standard and classical theory of homogeneous freezing initiates within the interior volume of a cloud droplet. Current experimental data on homogeneous freezing rates of ice in droplets of supercooled water, both in air and emulsion oil samples, show considerable scatter. For example, at -33 degrees C, the reported volume-based freezing rates of ice in supercooled water vary by as many as 5 orders of magnitude, which is well outside the range of measurement uncertainties. Here, we show that the process of ice nucleus formation at the air (or oil)-liquid water interface may help to explain why experimental results on ice nucleation rates yield different results in different ambient phases. Our results also suggest that surface crystallization of ice in cloud droplets can explain why low amounts of supercooled water have been observed in the atmosphere near -40 degrees C.

Arctic "ozone hole" in a cold volcanic stratosphere.

Optical depth records indicate that volcanic aerosols from major eruptions often produce clouds that have greater surface area than typical Arctic polar stratospheric clouds (PSCs). A trajectory cloud-chemistry model is used to study how volcanic aerosols could affect springtime Arctic ozone loss processes, such as chlorine activation and denitrification, in a cold winter within the current range of natural variability. Several studies indicate that severe denitrification can increase Arctic ozone loss by up to 30%. We show large PSC particles that cause denitrification in a nonvolcanic stratosphere cannot efficiently form in a volcanic environment. However, volcanic aerosols, when present at low altitudes, where Arctic PSCs cannot form, can extend the vertical range of chemical ozone loss in the lower stratosphere. Chemical processing on volcanic aerosols over a 10-km altitude range could increase the current levels of springtime column ozone loss by up to 70% independent of denitrification. Climate models predict that the lower stratosphere is cooling as a result of greenhouse gas built-up in the troposphere. The magnitude of column ozone loss calculated here for the 1999--2000 Arctic winter, in an assumed volcanic state, is similar to that projected for a colder future nonvolcanic stratosphere in the 2010 decade.

Role of the stratospheric polar freezing belt in denitrification.

Homogeneous freezing of nitric acid hydrate particles can produce a polar freezing belt in either hemisphere that can cause denitrification. Computed denitrification profiles for one Antarctic and two Arctic cold winters are presented. The vertical range over which denitrification occurs is normally quite deep in the Antarctic but limited in the Arctic. A 4 kelvin decrease in the temperature of the Arctic stratosphere due to anthropogenic and/or natural effects can trigger the occurrence of widespread severe denitrification. Ozone loss is amplified in a denitrified stratosphere, so the effects of falling temperatures in promoting denitrification must be considered in assessment studies of ozone recovery trends.

Quantifying denitrification and its effect on ozone recovery

Upper Atmosphere Research Satellite observations indicate that extensive denitrification without significant dehydration currently occurs only in the Antarctic during mid to late June. The fact that denitrification occurs in a relatively warm month in the Antarctic raises concern about the likelihood of its occurrence and associated effects on ozone recovery in a colder and possibly more humid future Arctic lower stratosphere. Polar stratospheric cloud lifetimes required for Arctic denitrification to occur in the future are presented and contrasted against the current Antarctic cloud lifetimes. Model calculations show that widespread severe denitrification could enhance future Arctic ozone loss by up to 30%.

Stratospheric Chlorine Injection by Volcanic Eruptions: HCI Scavenging and Implications for Ozone.

Because the output of volatile chlorine during a major volcanic event can greatly exceed the annual anthropogenic emissions of chlorine to the atmosphere, the fate of volcanic chlorine must be known. Although numerous observations have shown that volcanoes do not significantly contribute to the stratospheric chlorine burden, no quantitative explanation has been published. Hydrogen chloride (HCI) scavenging processes during the early phases of a volcanic eruption are discussed. A plume dynamics and thermodynamics model is used to show that HCI removal in condensed supercooled water can reduce HCI vapor concentrations by up to four orders of magnitude, preventing substantial stratospheric chlorine injection.