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.     

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.     

Interhemispheric Differences in Polar Stratospheric HNO3, H2O, CIO, and O3

Simultaneous global measurements of nitric acid (HNO(3)), water (H(2)O), chlorine monoxide (CIO), and ozone (O(3)) in the stratosphere have been obtained over complete annual cycles in both hemispheres by the Microwave Limb Sounder on the Upper Atmosphere Research Satellite. A sizeable decrease in gas-phase HNO(3) was evident in the lower stratospheric vortex over Antarctica by early June 1992, followed by a significant reduction in gas-phase H(2)O after mid-July. By mid-August, near the time of peak CIO, abundances of gas-phase HNO(3) and H(2)O were extremely low. The concentrations of HNO(3) and H(2)O over Antarctica remained depressed into November, well after temperatures in the lower stratosphere had risen above the evaporation threshold for polar stratospheric clouds, implying that denitrification and dehydration had occurred. No large decreases in either gas-phase HNO(3) or H(2)O were observed in the 1992-1993 Arctic winter vortex. Although CIO was enhanced over the Arctic as it was over the Antarctic, Arctic O(3) depletion was substantially smaller than that over Antarctica. A major factor currently limiting the formation of an Arctic ozone "hole" is the lack of denitrification in the northern polar vortex, but future cooling of the lower stratosphere could lead to more intense denitrification and consequently larger losses of Arctic ozone.     

The potential for ozone depletion in the arctic polar stratosphere

The nature of the Arctic polar stratosphere is observed to be similar in many respects to that of the Antarctic polar stratosphere, where an ozone hole has been identified. Most of the available chlorine (HCl and ClONO(2)) was converted by reactions on polar stratospheric clouds to reactive ClO and Cl(2)O(2) throughout the Arctic polar vortex before midwinter. Reactive nitrogen was converted to HNO(3), and some, with spatial inhomogeneity, fell out of the stratosphere. These chemical changes ensured characteristic ozone losses of 10 to 15% at altitudes inside the polar vortex where polar stratospheric clouds had occurred. These local losses can translate into 5 to 8% losses in the vertical column abundance of ozone. As the amount of stratospheric chlorine inevitably increases by 50% over the next two decades, ozone losses recognizable as an ozone hole may well appear.     

Observations of Stratospheric NO2 and O3 at Thule, Greenland

Scattered sunlight and direct light from the moon was used in two wavelength ranges to measure the total column abundances of stratospheric ozone(O(3)) and nitrogen dioxide (NO(2)) at Thule, Greenland (76.5 degrees N), during the period from 29 January to 16 February 1988. The observed O(3) column varied between about 325 and 400 Dobson units, and the lower values were observed when the center of the Arctic polar vortex was closest to Thule. This gradient probably indicates that O(3) levels decrease due to dynamical processes near the center of the Arctic vortex and should be considered in attempts to derive trends in O(3) levels. The observed NO(2) levels were also lowest in the center of the Arctic vortex and were sometimes as low as 5 x 10(14) molecules per square centimeter, which is even less than comparable values measured during Antarctic spring, suggesting that significant heterogeneous photochemistry takes place during the Arctic winter as it does in the Antarctic.     

Arctic air pollution: origins and impacts

Notable warming trends have been observed in the Arctic. Although increased human-induced emissions of long-lived greenhouse gases are certainly the main driving factor, air pollutants, such as aerosols and ozone, are also important. Air pollutants are transported to the Arctic, primarily from Eurasia, leading to high concentrations in winter and spring (Arctic haze). Local ship emissions and summertime boreal forest fires may also be important pollution sources. Aerosols and ozone could be perturbing the radiative budget of the Arctic through processes specific to the region: Absorption of solar radiation by aerosols is enhanced by highly reflective snow and ice surfaces; deposition of light-absorbing aerosols on snow or ice can decrease surface albedo; and tropospheric ozone forcing may also be contributing to warming in this region. Future increases in pollutant emissions locally or in mid-latitudes could further accelerate global warming in the Arctic.     

Ozone loss inside the northern polar vortex during the 1991-1992 winter

Measurements made in the outer ring of the northern polar vortex from October 1991 through March 1992 reveal an altitude-dependent change in ozone, with a decrease at the bottom of the vortex and a substantial increase at the highest altitudes accessible to measurement. The increase is the result of ozone-rich air entering the vortex, and the decrease reflects ozone loss accumulated after the descent of the air through high concentrations of reactive chlorine. The depleted air that is released out of the bottom of the vortex is sufficient to significantly reduce column ozone at mid-latitudes.     

In Situ Northern Mid-Latitude Observations of ClO, O3, and BrO in the Wintertime Lower Stratosphere

In order to test photochemical theories linking chlorofluorocarbon derivatives to ozone(O(3)) depletion at high latitudes in the springtime, several related atmospheric species, including O(3), chlorine monoxide(ClO), and bromine monoxide (BrO) were measured in the lower stratosphere with instruments mounted on the NASA ER-2 aircraft on 13 February 1988. The flight path from Moffett Field, California (37 degrees N, 121 degrees W), to Great Slave Lake, Canada (61 degrees N, 115 degrees W), extended to the center of the polar jet associated with but outside of the Arctic vortex, in which the abundance of O(3) was twice its mid-latitude value, whereas BrO levels were 5 parts per trillion by volume (pptv) between 18 and 21 kilometers, and 2.4 pptv below that altitude. The ClO mixing ratio was as much as 65 pptv at 60 degrees N latitude at an altitude of 20 kilometers, and was enhanced over mid-latitude values by a factor of 3 to 5 at altitudes above 18 kilometers and by as much as a factor of 40 at altitudes below 17 kilometers. Levels of ClO and O(3) were highly correlated on all measured distance scales, and both showed an abrupt change in character at 54 degrees N latitude. The enhancement of ClO abundance north of 54 degrees N was most likely caused by low nitrogen dioxide levels in the flight path.     

Chlorine oxide in the stratospheric ozone layer: ground-based detection and measurement

Stratospheric chlorine oxide, a significant intermediate product in the catalytic destruction of ozone by atomic chlorine, has been detected and measured by a ground-based 204-gigahertz, millimeter-wave receiver. Data taken at latitude 42 degrees N on 17 days between 10 January and 18 February 1980 yield an average chlorine oxide column density of approximately 1.05 x 10(14) per square centimeter or approximately 2/3 that of the average of eight in situ balloon flight measurements (excluding the anomalously high data of 14 July 1977) made over the past 4 years at 32 degrees N. We find less chlorine oxide below 35 kilometers and a larger vertical gradient than predicted by theoretical models of the stratospheric ozone layer.     

The detection of large HNO3-containing particles in the winter Arctic stratosphere

Large particles containing nitric acid (HNO3) were observed in the 1999/2000 Arctic winter stratosphere. These in situ observations were made over a large altitude range (16 to 21 kilometers) and horizontal extent (1800 kilometers) on several airborne sampling flights during a period of several weeks. With diameters of 10 to 20 micrometers, these sedimenting particles have significant potential to denitrify the lower stratosphere. A microphysical model of nitric acid trihydrate particles is able to simulate the growth and sedimentation of these large sizes in the lower stratosphere, but the nucleation process is not yet known. Accurate modeling of the formation of these large particles is essential for understanding Arctic denitrification and predicting future Arctic ozone abundances.     

Elemental tracers of distant regional pollution aerosols

A seven-element tracer system shows that regional pollution aerosols of both North America and Europe have characteristic signatures that can be followed into remote areas up to several thousand kilometers downwind. In aerosols of mixed origin, regional contributions to the tracer elements can be resolved by least-squares procedures. After transport of several hundred kilometers, secondary sulfate can also be apportioned satisfactorily. Regional elemental tracers thus offer a way to determine the sources of pollution aerosol in important areas such as the northeastern United States, Scandinavia, and the Arctic.     

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.     

Measured trends in stratospheric ozone

Recent findings, based on both ground-based and satellite measurements, have established that there has been an apparent downward trend in the total column amount of ozone over mid-latitude areas of the Northern Hemisphere in all seasons. Measurements of the altitude profile of the change in the ozone concentration have established that decreases are taking place in the lower stratosphere in the region of highest ozone concentration. Analysis of updated ozone records, through March of 1991, including 29 stations in the former Soviet Union, and analysis of independently calibrated satellite data records from the Total Ozone Mapping Spectrometer and Stratospheric Aerosol and Gas Experiment instruments confirm many of the findings originally derived from the Dobson record concerning northern midlatitude changes in ozone. The data from many instruments now provide a fairly consistent picture of the change that has occurred in stratospheric ozone levels.     

Atmospheric burnup of the cosmos-954 reactor

On 24 January 1978 the Russian satellite Cosmos-954 reentered the atmosphere over northern Canada. By use of high-altitude balloons, the atmosphere was sampled during 1978 up to an altitude of 39 kilometers to detect particulate debris from the reactor on board the satellite. Enriched uranium-bearing aerosols at concentrations and particle sizes compatible with partial burnup of the Cosmos-954 reactor were detected only in the high polar stratosphere.     

Large-scale nitrogen oxide plumes in the tropopause region and implications for ozone

Continuous measurements of nitrogen oxide and ozone were performed from a commercial airliner during 1 year at cruising altitudes below and above the tropopause. The upper tropospheric nitrogen oxides distribution was found to be strongly influenced by large-scale plumes extending about 100 to 1300 kilometers along the flight track. The plumes were frequently observed downwind of thunderstorms and frontal systems, which most probably caused upward transport of polluted air from the continental boundary layer or nitrogen oxide production in lightning strokes, or both. Particularly in summer, average ozone concentrations in the plumes were enhanced compared to the tropospheric background levels.     

The sensitivity of polar ozone depletion to proposed geoengineering schemes

The large burden of sulfate aerosols injected into the stratosphere by the eruption of Mount Pinatubo in 1991 cooled Earth and enhanced the destruction of polar ozone in the subsequent few years. The continuous injection of sulfur into the stratosphere has been suggested as a "geoengineering" scheme to counteract global warming. We use an empirical relationship between ozone depletion and chlorine activation to estimate how this approach might influence polar ozone. An injection of sulfur large enough to compensate for surface warming caused by the doubling of atmospheric CO2 would strongly increase the extent of Arctic ozone depletion during the present century for cold winters and would cause a considerable delay, between 30 and 70 years, in the expected recovery of the Antarctic ozone hole.     

White-light filaments for atmospheric analysis

Most long-path remote spectroscopic studies of the atmosphere rely on ambient light or narrow-band lasers. High-power femtosecond laser pulses have been found to propagate in the atmosphere as dynamically self-guided filaments that emit in a continuum from the ultraviolet to the infrared. This white light exhibits a directional behavior with enhanced backward scattering and was detected from an altitude of more than 20 kilometers. This light source opens the way to white-light and nonlinear light detection and ranging applications for atmospheric trace-gas remote sensing or remote identification of aerosols. Air ionization inside the filaments also opens promising perspectives for laser-induced condensation and lightning control. The mobile femtosecond-terawatt laser system, Teramobile, has been constructed to study these applications.     

Increasing river discharge to the Arctic Ocean

Synthesis of river-monitoring data reveals that the average annual discharge of fresh water from the six largest Eurasian rivers to the Arctic Ocean increased by 7% from 1936 to 1999. The average annual rate of increase was 2.0 +/- 0.7 cubic kilometers per year. Consequently, average annual discharge from the six rivers is now about 128 cubic kilometers per year greater than it was when routine measurements of discharge began. Discharge was correlated with changes in both the North Atlantic Oscillation and global mean surface air temperature. The observed large-scale change in freshwater flux has potentially important implications for ocean circulation and climate.     

Human-induced Arctic moistening

The Arctic and northern subpolar regions are critical for climate change. Ice-albedo feedback amplifies warming in the Arctic, and fluctuations of regional fresh water inflow to the Arctic Ocean modulate the deep ocean circulation and thus exert a strong global influence. By comparing observations to simulations from 22 coupled climate models, we find influence from anthropogenic greenhouse gases and sulfate aerosols in the space-time pattern of precipitation change over high-latitude land areas north of 55 degrees N during the second half of the 20th century. The human-induced Arctic moistening is consistent with observed increases in Arctic river discharge and freshening of Arctic water masses. This result provides new evidence that human activity has contributed to Arctic hydrological change.     

Temperatures, winds, and composition in the saturnian system

Stratospheric temperatures on Saturn imply a strong decay of the equatorial winds with altitude. If the decrease in winds reported from recent Hubble Space Telescope images is not a temporal change, then the features tracked must have been at least 130 kilometers higher than in earlier studies. Saturn's south polar stratosphere is warmer than predicted from simple radiative models. The C/H ratio on Saturn is seven times solar, twice Jupiter's. Saturn's ring temperatures have radial variations down to the smallest scale resolved (100 kilometers). Diurnal surface temperature variations on Phoebe suggest a more porous regolith than on the jovian satellites.