E. Kyrö

Prolonged stratospheric ozone loss in the 1995–96 Arctic winter

It is well established that extensive depletion of ozone, initiated by heterogenous reactions on polar stratospheric clouds (PSCs) can occur in both the Arctic and Antarctic lower stratosphere. Moreover, it has been shown that ozone loss rates in the Arctic region in recent years reached values comparable to those over the Antarctic,. But until now the accumulated ozone losses over the Arctic have been the smaller, mainly because the period of Arctic ozone loss has not—unlike over the Antarctic—persisted well into springtime. Here we report the occurrence—during the unusually cold 1995–96 Arctic winter—of the highest recorded chemical ozone loss over the Arctic region. Two new kinds of behaviour were observed. First, ozone loss at some altitudes was observed long after the last exposure to PSCs. This continued loss appears to be due to a removal of the nitrogen species that slow down chemical ozone depletion. Second, in another altitude range ozone loss rates decreased while PSCs were still present, apparently because of an early transformation of the ozone-destroying chlorine species into less active chlorinenitrate. The balance between these two counteracting mechanisms is probably a fine one, determined by small differences in wintertime stratospheric temperatures. If the apparent cooling trend in the Arctic stratosphere is real, more dramatic ozone losses may occur in the future.

Radiation Dry Bias of the Vaisala RS92 Humidity Sensor

The comparison of simultaneous humidity measurements by the Vaisala RS92 radiosonde and by the Cryogenic Frostpoint Hygrometer (CFH) launched at Alajuela, Costa Rica, during July 2005 reveals a large solar radiation dry bias of the Vaisala RS92 humidity sensor and a minor temperature-dependent calibration error. For soundings launched at solar zenith angles between 10° and 30°, the average dry bias is on the order of 9% at the surface and increases to 50% at 15 km. A simple pressure- and temperature-dependent correction based on the comparison with the CFH can reduce this error to less than 7% at all altitudes up to 15.2 km, which is 700 m below the tropical tropopause. The correction does not depend on relative humidity, but is able to reproduce the relative humidity distribution observed by the CFH.

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.

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.

Chemical Ozone Loss in the Arctic Winter 1994/95 as Determined by the Match Technique

The chemically induced ozone loss inside the Arctic vortex during the winter 1994/95 has been quantified by coordinated launches of over 1000 ozonesondes from 35 stations within the Match 94/95 campaign. Trajectory calculations, which allow diabatic heating or cooling, were used to trigger the balloon launches so that the ozone concentrations in a large number of air parcels are each measured twice a few days apart. The difference in ozone concentration is calculated for each pair and is interpreted as a change caused by chemistry. The data analysis has been carried out for January to March between 370 K and 600 K potential temperature. Ozone loss along these trajectories occurred exclusively during sunlit periods, and the periods of ozone loss coincided with, but slightly lagged, periods where stratospheric temperatures were low enough for polar stratospheric clouds to exist. Two clearly separated periods of ozone loss show up. Ozone loss rates first peaked in late January with a maximum value of 53 ppbv per day (1.6 % per day) at 475 K and faster losses higher up. Then, in mid-March ozone loss rates at 475 K reached 34 ppbv per day (1.3 % per day), faster losses were observed lower down and no ozone loss was found above 480 K during that period. The ozone loss in hypothetical air parcels with average diabetic descent rates has been integrated to give an accumulated loss through the winter. The most severe depletion of 2.0 ppmv (60 %) took place in air that was at 515 K on 1 January and at 450 K on 20 March. Vertical integration over the levels from 370 K to 600 K gives a column loss rate, which reached a maximum value of 2.7 Dobson Units per day in mid-March. The accumulated column loss between 1 January and 31 March was found to be 127 DU (∼36 %).

Methane retrievals from greenhouse gases observing satellite (GOSAT) shortwave infrared measurements: performance comparison of proxy and physics retrieval algorithms

We compare two conceptually different methods for determining methane column-averaged mixing ratios image from Greenhouse Gases Observing Satellite (GOSAT) shortwave infrared (SWIR) measurements. These methods account differently for light scattering by aerosol and cirrus. The proxy method retrieves a CO_2 column which, in conjunction with prior knowledge on CO_2 acts as a proxy for scattering effects. The physics-based method accounts for scattering by retrieving three effective parameters of a scattering layer. Both retrievals are validated on a 19-month data set using ground-based X_CH_4 at 12 stations of the Total Carbon Column Observing Network (TCCON), showing comparable performance: for the proxy retrieval we find station-dependent retrieval biases from −0.312% to 0.421% of X_CH_4 a standard deviation of 0.22% and a typical precision of 17 ppb. The physics method shows biases between −0.836% and −0.081% with a standard deviation of 0.24% and a precision similar to the proxy method. Complementing this validation we compared both retrievals with simulated methane fields from a global chemistry-transport model. This identified shortcomings of both retrievals causing biases of up to 1ings and provide a satisfying validation of any methane retrieval from space-borne SWIR measurements, in our opinion it is essential to further expand the network of TCCON stations.

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 depletion in and below the Arctic vortex for 1997

The winter 1996/97 was quite unusual with late vortex formation and polar stratospheric cloud (PSC) development and subsequent record low temperatures in March. Ozone depletion in the Arctic vortex is determined using ozonesondes. The diabatic cooling is calculated with PV-theta mapped ozone mixing ratios and the large ozone depletions, especially at the center of the vortex where most PSC existence was predicted, enhances the diabatic cooling by up to 80%. The average vortex chemical ozone depletion from January 6 to April 6 is 33, 46, 46, 43, 35, 33, 32 and 21 % in air masses ending at 375, 400, 425, 450, 475, 500, 525, and 550 K (about 14–22 km). This depletion is corrected for transport of ozone across the vortex edge calculated with reverse domain-filling trajectories. 375 K is in fact below the vortex, but the calculation method is applicable at this level with small changes. The column integrated chemical ozone depletion amounts to about 92 DU (21%), which is comparable to the depletions observed during the previous four winters.

Polar vortex evolution during the 2002 Antarctic major warming as observed by the Odin satellite

In September 2002 the Antarctic polar vortex split in two under the influence of a sudden warming. During this event, the Odin satellite was able to measure both ozone (O3) and chlorine monoxide (ClO), a key constituent responsible for the so-called “ozone hole”, together with nitrous oxide (N2O), a dynamical tracer, and nitric acid (HNO3) and nitrogen dioxide (NO2), tracers of denitrification. The submillimeter radiometer (SMR) microwave instrument and the Optical Spectrograph and Infrared Imager System (OSIRIS) UV-visible light spectrometer (VIS) and IR instrument on board Odin have sounded the polar vortex during three different periods: before (19–20 September), during (24–25 September), and after (1–2 and 4–5 October) the vortex split. Odin observations coupled with the Reactive Processes Ruling the Ozone Budget in the Stratosphere (REPROBUS) chemical transport model at and above 500 K isentropic surfaces (heights above 18 km) reveal that on 19–20 September the Antarctic vortex was dynamically stable and chemically nominal: denitrified, with a nearly complete chlorine activation, and a 70% O3 loss at 500 K. On 25–26 September the unusual morphology of the vortex is monitored by the N2O observations. The measured ClO decay is consistent with other observations performed in 2002 and in the past. The vortex split episode is followed by a nearly complete deactivation of the ClO radicals on 1–2 October, leading to the end of the chemical O3 loss, while HNO3 and NO2 fields start increasing. This acceleration of the chlorine deactivation results from the warming of the Antarctic vortex in 2002, putting an early end to the polar stratospheric cloud season. The model simulation suggests that the vortex elongation toward regions of strong solar irradiance also favored the rapid reformation of ClONO2. The observed dynamical and chemical evolution of the 2002 polar vortex is qualitatively well reproduced by REPROBUS. Quantitative differences are mainly attributable to the too weak amounts of HNO3 in the model, which do not produce enough NO2 in presence of sunlight to deactivate chlorine as fast as observed by Odin.