Evolution of Aerosol Properties in the Arctic Polar Vortex
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The severe depletion of stratospheric ozone over Antarctica in late winter and early spring is caused by enhanced CLO abundances arising from heterogeneous reactions on polar stratospheric clouds (PSCs). CLO abundances comparable to those over Antarctica have also been observed throughout the Arctic Vortex, but the accompanying loss of Arctic ozone has been much less severe.
During the winter of 1999-2000, the AROTEL instrument was deployed on the NASA DC-8 at Kiruna, Sweden for the SAGE III Ozone Loss Validation Experiment (SOLVE). Measurements of ozone, temperature and aerosols were made on 18 local science flights from December to March. Extremely low temperatures were observed throughout most of the Arctic vortex and polar stratospheric clouds were observed throughout the Arctic area during January. Significant ozone loss was measured after the sun began to rise on the vortex area in February. Ozone mixing ratios as low as 800 ppbv were observed during flights in March.
The following is the final technical report for grant NAGW-3442, 'Observational and Model Studies of Large-Scale Mixing Processes in the Stratosphere'. Research efforts in the first year concentrated on transport and mixing processes in the polar vortices. Three papers on mixing in the Antarctic were published. The first was a numerical modeling study of wavebreaking and mixing and their relationship to the period of observed stratospheric waves (Bowman). The second paper presented evidence from TOMS for wavebreaking in the Antarctic (Bowman and Mangus 1993). The third paper used Lagrangian trajectory calculations from analyzed winds to show that there is very little transport into the Antarctic polar vortex prior to the vortex breakdown (Bowman). Mixing is significantly greater at lower levels. This research helped to confirm theoretical arguments for vortex isolation and data from the Antarctic field experiments that were interpreted as indicating isolation. A Ph.D. student, Steve Dahlberg, used the trajectory approach to investigate mixing and transport in the Arctic. While the Arctic vortex is much more disturbed than the Antarctic, there still appears to be relatively little transport across the vortex boundary at 450 K prior to the vortex breakdown. The primary reason for the absence of an ozone hole in the Arctic is the earlier warming and breakdown of the vortex compared to the Antarctic, not replenishment of ozone by greater transport. Two papers describing these results have appeared (Dahlberg and Bowman; Dahlberg and Bowman). Steve Dahlberg completed his Ph.D. thesis (Dahlberg and Bowman) and is now teaching in the Physics Department at Concordia College. We also prepared an analysis of the QBO in SBUV ozone data (Hollandsworth et al.). A numerical study in collaboration with Dr. Ping Chen investigated mixing by barotropic instability, which is the probable origin of the 4-day wave in the upper stratosphere (Bowman and Chen). The important result from this paper is that even in the presence of growing, unstable waves, the mixing barriers around
Stratospheric ozone and aerosol distributions were measured across the wintertime Arctic vortex from January to March 1992 with an airborne lidar system as part of the 1992 Airborne Arctic Stratospheric Expedition (AASE II). Aerosols from the Mount Pinatubo eruption were found outside and inside the vortex with distinctly different distributions that clearly identified the dynamics of the vortex. Changes in aerosols inside the vortex indicated advection of air from outside to inside the vortex below 16 kilometers. No polar stratospheric clouds were observed and no evidence was found for frozen volcanic aerosols inside the vortex. Between January and March, ozone depletion was observed inside the vortex from 14 to 20 kilometers with a maximum average loss of about 23 percent near 18 kilometers.
The Microwave Limb Sounder (MLS) observed ozone decreases in the Arctic Vortex beginning in January 1997 at 585K and in February 1997 at 465K.
Between November 1999 and April 2000, two major field experiments, the SAGE III Ozone Loss and Validation Experiment (SOLVE) and the Third European Stratospheric Experiment on Ozone (THESEO 2000), collaborated to form the largest field campaign yet mounted to study Arctic ozone loss. This international campaign involved more than 500 scientists from over 20 countries spread across the high and mid-latitudes of the northern hemisphere. The main scientific aims of SOLVE-THESEO 2000 were to study (a) the processes leading to ozone loss in the Arctic vortex and (b) the effect on ozone amounts over northern mid-latitudes. The campaign included satellites, heavy lift balloon launches, 6 different aircraft, ground stations, and scores of ozone-sonde. Campaign activities were principally conducted in 3 intensive measurement phases centered on early December 1999, late January 2000, and early March 2000. Observations made during the campaign showed that temperatures were unusually cold in the polar lower stratosphere over the course of the 1999-2000 winter. These cold temperatures resulted in the formation of extensive polar stratospheric clouds (PSCs) across the Arctic. Heterogeneous chemical reactions on the surfaces of the PSC particles produced high levels of reactive chlorine within the polar vortex by early January. This reactive chlorine catalytically destroyed about 60% of the ozone in a layer near 20 km between late January and mid-March 2000.
We present measurements of unusually low mixing ratios of HNO3 in the exceptionally cold Arctic vortex of late-January and early-February 2005. The measurements were obtained by the airborne submillimeter radiometer ASUR during the polar aura validation experiment (PAVE). The distribution of HNO3 inside the vortex reaches minima below 4 ppbv around 22 km altitude and maxima above 13 ppbv around 16 km altitude, with a considerable spatial variability.
The 1999-2000 Arctic stratospheric vortex was unusually cold, especially in the early winter lower stratosphere, with a larger area near polar stratospheric cloud formation temperatures in Dec and Jan, and much lower temperatures averaged over Nov-Jan, than any previously observed Arctic winter.
A number of recently published papers suggest that mountain-wave activity in the stratosphere, producing ice particles when temperatures drop below the ice frost point, may be the primary source of large NAT particles. In this paper we use measurements from the Advanced Very High Resolution Radiometer (AVHRR) instruments on board the National Oceanic and Atmospheric Administration (NOAA) polar-orbiting satellites to map out regions of ice clouds produced by stratospheric mountain-wave activity inside the Arctic vortex. Lidar observations from three DC-8 flights in early December 1999 show the presence of solid nitric acid (Type Ia or NAT) polar stratospheric clouds (PSCs). By using back trajectories and superimposing the position maps on the AVHRR cloud imagery products, we show that these observed NAT clouds could not have originated at locations of high-amplitude mountain-wave activity. We also show that mountain-wave PSC climatology data and Mountain Wave Forecast Model 2.0 (MWFM-2) raw hemispheric ray and grid box averaged hemispheric wave temperature amplitude hindcast data from the same time period are in agreement with the AVHRR data. Our results show that ice cloud formation in mountain waves cannot explain how at least three large scale NAT clouds were formed in the stratosphere in early December 1999.
Over the past several years, world scientific attention was focused on the rapid and unanticipated decrease in the abundance of ozone over Antarctica during the Austral spring. A major aircraft campaign was conducted from December 1988 to February 1989 in response to the recently published Ozone Trends Panel Report which found that the largest decreases in Arctic ozone occurred during January to February at latitudes near the edge of the Arctic vortex. This atlas provides a complete set of TOMS ozone measurements over Europe and the North Atlantic for the duration of the experiment. These were the orbital TOMS measurements provided to the experimenters in near-real-time. In addition, a set of Northern Hemisphere TOMS ozone measurements for the period December 26, 1988 to March 20, 1989 is presented. A comparison of January and February 1989 mean ozone values to prior years is also presented.
In order to test photochemical theories linking chlorofluorocarbon derivatives to O3 depletion at high latitudes in the springtime, several related atmospheric species, including O3, ClO, and BrO were measured in the lower stratosphere. The flight path extended to the center of the polar jet associated with but outside of the Arctic vortex, in which the abundance of O3 was twice its midlatitude value, whereas BrO levels were five parts per trillion (pptv) by volume between 18 and 21 km, and 2.4 pptv below that altitude. The ClO mixing ratio was as much as 65 pptv at 60 N latitude at an altitude of 20 km, and was enhanced over midlatitude values by a factor of three to five at altitudes above 18 km and by as much as a factor of 40 at altitudes below 17 km. Levels of ClO and O3 were highly correlated on all measured distance scales, and both showed an abrupt change in character at 54 N latitude. The ClO abundance north of 54 N was probably caused by low NO2 levels in the flight path.
Three-dimensional model calculations with the NASA/GSFC chemistry and transport model have been designed to consider the impact of heterogeneous processes occurring on polar stratospheric clouds (PSCs) in the Arctic vortex on the HCl distribution. By examining the HCl concentration for a calculation with PSCs relative to a calculation with gas phase chemistry only, the impact of polar processing on reactive chlorine species at middle latitudes is inferred. Results from the chemistry and transport model reproduce basic features of the ClO measurements (Toohey et al., 1991), which were made on the ferry flights of the ER-2 from Stavanger, Norway to Moffett Field, California via Wallops Island, Virginia on February 20 and 21, 1989. The model indicates that perturbed air which is contained within the polar vortex during winter is not homogeneously mixed, and that the ferry flights were made through air with the largest conversion of HCl to reactive chlorine that is seen at middle latitudes.
A number of tasks needed to be performed to operate the DC-8 aircraft in the Arctic Ozone Expedition during 1989. These included development of improved navigational computer programs and performing advanced planning for flight tracks. The missions required further work in the field to plan flight tracks and to establish a data archive. The DC-8 aircraft was operated during the deployment phase of the Arctic Ozone Expedition. Data were collected revealing the presence of extensive systems of polar stratospheric clouds. The data also showed the evolution of the chlorine and nitrogen chemistry within the Arctic vortex. A navigational computer code was improved so that the DC-8 navigators could perform their function more efficiently.
The present study compares small-scale (less than 100 km) features in ER-2 measurements of ClO, O3, H2O, N2O, and NO(y) outside the lower stratospheric Arctic vortex of 1988-1989 with features on potential vorticity maps from ECMWF. The potential vorticity maps are obtained from T106 analyses and forecasts. Some of the plots were truncated to lower resolution (T63 or T42) which smooths out the finer-scale structure. Comparison of these lower resolution plots shows how much detail is lost by excessive smoothing. It is also evident that the forecast plots lose fine-scale structure due to dissipation in the model resulting mainly from horizontal diffusion. It is concluded that blobs of air on the maps at latitudes between the vortex edge and 25 deg N having potential vorticities characteristic of the vortex did indeed originate from the vortex, but that the real atmosphere is more sharply differentiated than the meteorological analyses, implying that the potential vorticity maps underestimate the amount of peeled-off material.
HALOE observations of H2O and CH4 are compared with in situ techniques aboard the ER-2 aircraft during the northern winter of 1991/92, in particular for the dates 911208, 920108, 920217, 920222, and 920320 when the spatial coincidences are close, within +/- 1 deg latitude and +/- 12 deg longitude. The results reveal the limitations of comparing high resolution in situ aircraft data with a remote sounding limb scanner. Of the five comparison dates, three had HALOE/ER-2 coincidences which occurred near the edge of the Arctic vortex; the vertical variability in the HALOE results and the horizontal variability in the ER-2 observations on these days show that the vortex edge is not a region where exact agreement can be expected except by chance. On a 4th comparison date, there was substantial overlap away from the vortex edge, although for some species the aircraft data show considerable variability near the coincidence point. On the 5th comparison date, the ER-2 had no overlap in altitude with the lowest HALOE observations; however, a short linear interpolation over about 1 km altitude results in smooth composite profiles. Generally speaking the agreement between HALOE and the ER-2 at overlap altitudes is about 12 percent in the case of water vapor, which shows low horizontal and vertical variability. The agreement for methane, with limited data having altitude overlap, is better than 6 percent.
Global ozone observations from the Microwave Limb Sounder (MLS) aboard the Upper Atmosphere Research Satellite (UARS) are presented, in both vertically resolved and column abundance formats. The authors review the zonal-mean ozone variations measured over the two and a half years since launch in September 1991. Well-known features such as the annual and semiannual variations are ubiquitous. In the equatorial regions, longer-term changes are believed to be related to the quasi-biennial oscillation (QBO), with a strong semiannual signal above 20 hPa. Ozone values near 50 hPa exhibit an equatorial low from October 1991 to June 1992, after which the low ozone pattern splits into two subtropical lows (possibly in connection with residual circulation changes tied to the QBO) and returns to an equatorial low in September 1993. The ozone hole development at high southern latitudes is apparent in MLS column data integrated down to 100 hPa, the MLS data reinforce current knowledge of this lower-stratospheric phenomenon by providing a height-dependent view of the variations. The region from 30 deg S to 30 deg N (an area equal to half the global area) shows very little change in the ozone column from year to year and within each year. The most striking ozone changes have occurred at northern midlatitudes, with the October 1992 to July 1993 column values significantly lower than during the prior year. The zonal-mean changes manifest themselves as a slower rate of increase during the 1992/93 winter, and there is some evidence for a lower fall minimum. A recovery occurs during late summer of 1993; early 1994 values are significantly larger than during the two previous winters. The timing and latitudinal extent of the northern midlatitude decreases appear to rule out observed ClO enhancements in the Arctic vortex, with related chemical processing and ozone dilution effects, as a unique cause. Local depletion from ClO-related chemical mechanisms alone is also not sufficient, based on MLS ClO data. The puzzling asymmetric nature of the changes probably requires a dynamical component as an explanation. A combination of effects (including chemical destruction via heterogeneous processes and QBO phasing) apparently needs to be invoked. This dataset will place constraints on future modeling studies, which are required to better understand the source of the observed changes.
Two critical areas of research were addressed successfully by this research. The first involves NASA ER-2 airborne observations of ClO and BrO radical destruction of ozone within the arctic vortex. The second involves the analysis of diurnal variations in ClO, to test the production and loss rates of ClO that constitutes the test for coupling reactions between the chlorine and nitrogen systems. We discuss results from this research in order.