H. Claude

Halogen Occultation Experiment ozone channel validation

The HALogen Occultation Experiment (HALOE) instrument on UARS observes vertical profiles of ozone and other gases of interest for atmospheric chemistry using the solar occultation technique. A broadband radiometer in the 9.6-μm band is used for ozone measurements. Version 17 ozone retrieved by HALOE is intercompared successfully with about 400 profiles of other sounders, including ozonesondes, lidars, balloons, rocketsondes, and other satellites. Usually, the HALOE data are within the error range of the correlative measurements between about 100 and 0.03 mbar atmospheric pressure. Between about 30 and 1 mbar, HALOE agrees typically within 5%, with a tendency to be low. In the first year of data, larger errors sometimes occur in the lower stratosphere due to the necessary correction for Pinatubo aerosol effects, but these differences do not exceed 20%. The data show internal consistency for sunrise and sunset events at the same locations. Some examples of observed ozone distributions, including polar regions, are given.

Correlations between tropopause height and total ozone: Implications for long‐term changes

For the central European station of Hohenpeissenberg, averaging of ozone profiles grouped by tropopause height shows that the ozone mixing ratio profile in the lower stratosphere shifts up and down with the tropopause. The shift is largest near the tropopause and becomes negligible above 20 to 25 km. As a consequence a high tropopause is correlated with low total ozone and a low tropopause with high total ozone. Independent of season, total ozone decreases by 16 Dobson units (DU) per kilometer increase in tropopause height. At Hohenpeissenberg the tropopause has moved up by 150±70 m (2 σ) per decade over the last 30 years. If the −16 DU per kilometer correlation between total ozone and tropopause height is valid on the timescale of years, it is speculated that the observed increase in tropopause height could explain about 25% of the observed −10 DU per decade decrease of total ozone. This is of the same magnitude as the 30% fraction of midlatitude ozone depletion which current stratospheric models have difficulty accounting for. For Hohenpeissenberg the increase in tropopause height appears to be correlated with observed tropospheric warming: At 5 km altitude, for example, temperature has increased by 0.7±0.3 K per decade (2 σ) since 1967.

Trends of ozone in the troposphere

Using a set of selected surface ozone (nine stations) and ozone vertical profile measurements (from six stations), we have documented changes in tropospheric ozone at a number of locations. From two stations at high northern hemisphere (NH) latitudes there has been a significant decline in ozone amounts throughout the troposphere since the early 1980s. At midlatitudes of the NH where data are the most abundant, on the other hand, important regional differences prevail. The two stations in the eastern United States show that changes in ozone concentrations since the early 1970s have been relatively small. At the two sites in Europe, however, ozone amounts increased rapidly into the mid-1980s, but have increased less rapidly (or in some places not at all) since then. Increases at the Japanese ozonesonde station have been largest in the lower troposphere, but have slowed in the recent decade. The tropics are sparsely sampled but do not show significant changes. Small increases are suggested at southern hemisphere (SH) midlatitudes by the two surface data records. In Antarctica large declines in the ozone concentration are noted in the South Pole data, and like those at high latitudes of the NH, seem to parallel the large decreases in the stratosphere.

In-situ measurements of stratospheric ozone depletion rates in the Arctic winter 1991/1992: A Lagrangian approach

A Lagrangian approach has been used to assess the degree of chemically induced ozone loss in the Arctic lower stratosphere in winter 1991/1992. Trajectory calculations are used to identify air parcels probed by two ozonesondes at different points along the trajectories. A statistical analysis of the measured differences in ozone mixing ratio and the time the air parcel spent in sunlight between the measurements provides the chemical ozone loss. Initial results were first described by von der Gathen et al. [1995]. Here we present a more detailed description of the technique and a more comprehensive discussion of the results. Ozone loss rates of up to 10 ppbv per sunlit hour (or 54 ppbv per day) were found inside the polar vortex on the 475 K potential temperature surface (about 19.5 km in altitude) at the end of January. The period of rapid ozone loss coincides and slightly lags a period when temperatures were cold enough for type I polar stratospheric clouds to form. It is shown that the ozone loss occurs exclusively during the sunlit portions of the trajectories. The time evolution and vertical distribution of the ozone loss rates are discussed.

Changes in ozone over Europe: Analysis of ozone measurements from sondes, regular aircraft (MOZAIC) and alpine surface sites

We use ozone observations from sondes, regular aircraft, and alpine surface sites in a self-consistent analysis to determine robust changes in the time evolution of ozone over Europe. The data are most coherent since 1998, with similar interannual variability and trends. Ozone has decreased slowly since 1998, with an annual mean trend of −0.15 ppb yr−1 at ∼3 km and the largest decrease in summer. There are some substantial differences between the sondes and other data, particularly in the early 1990s. The alpine and aircraft data show that ozone increased from late 1994 until 1998, but the sonde data do not. Time series of differences in ozone between pairs of locations reveal inconsistencies in various data sets. Differences as small as few ppb for 2-3 years lead to different trends for 1995-2008, when all data sets overlap. Sonde data from Hohenpeissenberg and in situ data from nearby Zugspitze show ozone increased by ∼1 ppb yr−1 during 1978-1989. We construct a mean alpine time series using data for Jungfraujoch, Zugspitze, and Sonnblick. Using Zugspitze data for 1978-1989, and the mean time series since 1990, we find that the ozone increased by 6.5-10 ppb in 1978-1989 and 2.5-4.5 ppb in the 1990s and decreased by 4 ppb in the 2000s in summer with no significant changes in other seasons. It is hard to reconcile all these changes with trends in emissions of ozone precursors, and in ozone in the lowermost stratosphere. We recommend data sets that are suitable for evaluation of model hindcasts.

Chemical depletion of Arctic ozone in winter 1999/2000

During Arctic winters with a cold, stable stratospheric circulation, reactions on the surface of polar stratospheric clouds (PSCs) lead to elevated abundances of chlorine monoxide (ClO) that, in the presence of sunlight, destroy ozone. Here we show that PSCs were more widespread during the 1999/2000 Arctic winter than for any other Arctic winter in the past two decades. We have used three fundamentally different approaches to derive the degree of chemical ozone loss from ozonesonde, balloon, aircraft, and satellite instruments. We show that the ozone losses derived from these different instruments and approaches agree very well, resulting in a high level of confidence in the results. Chemical processes led to a 70% reduction of ozone for a region ∼1 km thick of the lower stratosphere, the largest degree of local loss ever reported for the Arctic. The Match analysis of ozonesonde data shows that the accumulated chemical loss of ozone inside the Arctic vortex totaled 117 ± 14 Dobson units (DU) by the end of winter. This loss, combined with dynamical redistribution of air parcels, resulted in a 88 ± 13 DU reduction in total column ozone compared to the amount that would have been present in the absence of any chemical loss. The chemical loss of ozone throughout the winter was nearly balanced by dynamical resupply of ozone to the vortex, resulting in a relatively constant value of total ozone of 340 ± 50 DU between early January and late March. This observation of nearly constant total ozone in the Arctic vortex is in contrast to the increase of total column ozone between January and March that is observed during most years.

Validation of Aura Microwave Limb Sounder Ozone by ozonesonde and lidar measurements

We present validation studies of MLS version 2.2 upper tropospheric and stratospheric ozone profiles using ozonesonde and lidar data as well as climatological data. Ozone measurements from over 60 ozonesonde stations worldwide and three lidar stations are compared with coincident MLS data. The MLS ozone stratospheric data between 150 and 3 hPa agree well with ozonesonde measurements, within 8% for the global average. MLS values at 215 hPa are biased high compared to ozonesondes by A`20% at middle to high latitude, although there is a lot of variability in this altitude region. Comparisons between MLS and ground-based lidar measurements from Mauna Loa, Hawaii, from the Table Mountain Facility, California, and from the Observatoire de Haute-Provence, France, give very good agreement, within A`5%, for the stratospheric values. The comparisons between MLS and the Table Mountain Facility tropospheric ozone lidar show that MLS data are biased high by A`30% at 215 hPa, consistent with that indicated by the ozonesonde data. We obtain better global average agreement between MLS and ozonesonde partial column values down to 215 hPa, although the average MLS values at low to middle latitudes are higher than the ozonesonde values by up to a few percent. MLS v2.2 ozone data agree better than the MLS v1.5 data with ozonesonde and lidar measurements. MLS tropical data show the wave one longitudinal pattern in the upper troposphere, with similarities to the average distribution from ozonesondes. High upper tropospheric ozone values are also observed by MLS in the tropical Pacific from June to November.

A trajectory-based estimate of the tropospheric ozone column using the residual method

We estimate the tropospheric column ozone using a forward trajectory model to increase the horizontal resolution of the Aura Microwave Limb Sounder (MLS) derived stratospheric column ozone. Subtracting the MLS stratospheric column from Ozone Monitoring Instrument total column measurements gives the trajectory enhanced tropospheric ozone residual (TTOR). Because of different tropopause definitions, we validate the basic residual technique by computing the 200-hPa-to-surface column and comparing it to the same product from ozonesondes and Tropospheric Emission Spectrometer measurements. Comparisons show good agreement in the tropics and reasonable agreement at middle latitudes, but there is a persistent low bias in the TTOR that may be due to a slight high bias in MLS stratospheric column. With the improved stratospheric column resolution, we note a strong correlation of extratropical tropospheric ozone column anomalies with probable troposphere-stratosphere exchange events or folds. The folds can be identified by their colocation with strong horizontal tropopause gradients. TTOR anomalies due to folds may be mistaken for pollution events since folds often occur in the Atlantic and Pacific pollution corridors. We also compare the 200-hPa-to-surface column with Global Modeling Initiative chemical model estimates of the same quantity. While the tropical comparisons are good, we note that chemical model variations in 200-hPa-to-surface column at middle latitudes are much smaller than seen in the TTOR.

Ozone and temperature trends in the upper stratosphere at five stations of the Network for the Detection of Atmospheric Composition Change

Upper stratospheric ozone anomalies from the satellite-borne Solar Backscatter Ultra-Violet (SBUV), Stratospheric Aerosol and Gas Experiment II (SAGE II), Halogen Occultation Experiment (HALOE), Global Ozone Monitoring by Occultation of Stars (GOMOS), and Scanning Imaging Absorption Spectrometer for Atmospheric Chartography (SCIAMACHY) instruments agree within 5% or better with ground-based data from lidars and microwave radiometers at five stations of the Network for the Detection of Atmospheric Composition Change (NDACC), from 45°S to 48°N. From 1979 until the late 1990s, all available data show a clear decline of ozone near 40 km, by 10%–15%. This decline has not continued in the last 10 years. At some sites, ozone at 40 km appears to have increased since 2000, consistent with the beginning decline of stratospheric chlorine. The phaseout of chlorofluorocarbons after the International Montreal Protocol in 1987 has been successful, and is now showing positive effects on ozone in the upper stratosphere. Temperature anomalies near 40 km altitude from European Centre for Medium Range Weather Forecast reanalyses (ERA-40), from National Centers for Environmental Prediction (NCEP) operational analyses, and from HALOE and lidar measurements show good consistency at the five stations, within about 3 K. Since about 1985, upper stratospheric temperatures have been fluctuating around a constant level at all five NDACC stations. This non-decline of upper stratospheric temperatures is a significant change from the more or less linear cooling of the upper stratosphere up until the mid-1990s, reported in previous trend assessments. It is also at odds with the almost linear 1 K per decade cooling simulated over the entire 1979–2010 period by chemistry–climate models (CCMs). The same CCM simulations, however, track the historical ozone anomalies quite well, including the change of ozone tendency in the late 1990s.

Arctic Ozone Loss in Threshold Conditions: Match Observations in 1997/1998 and 1998/1999

Chemical ozone loss rates inside the Arctic polar vortex were determined in early 1998 and early 1999 by using the Match technique based on coordinated ozonesonde measurements. These two winters provide the only opportunities in recent years to investigate chemical ozone loss in a warm Arctic vortex under threshold conditions, i.e., where the preconditions for chlorine activation, and hence ozone destruction, only occurred occasionally. In 1998, results were obtained in January and February between 410 and 520 K. The overall ozone loss was observed to be largely insignificant, with the exception of late February, when those air parcels exposed to temperatures below 195 K were affected by chemical ozone loss. In 1999, results are confined to the 475 K isentropic level, where no significant ozone loss was observed. Average temperatures were some 8°–10° higher than those in 1995, 1996, and 1997, when substantial chemical ozone loss occurred. The results underline the strong dependence of the chemical ozone loss on the stratospheric temperatures. This study shows that enhanced chlorine alone does not provide a sufficient condition for ozone loss. The evolution of stratospheric temperatures over the next decade will be the determining factor for the amount of wintertime chemical ozone loss in the Arctic stratosphere.