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Mid-winter lower stratosphere temperatures in the Antarctic vortex: comparison between observations and ECMWF and NCEP operational models

Radiosonde temperature profiles from Belgrano (78° S) and other Antarctic stations have been compared with European Centre for Medium-Range Weather Forecasting (ECMWF) and National Centers for Environmental Prediction (NCEP) operational analyses during the winter of 2003. Results show good agreement between radiosondes and NCEP and a bias in the ECMWF model which is height and temperature dependent, being up to 3°C too cold at 80 and 25–30 hPa, and hence resulting in an overestimation of the predicted potential PSC areas. Here we show the results of the comparison and discuss the potential implications that this bias might have on the ozone depletion computed by Chemical Transport Models based on ECMWF temperature fields, after rejecting the possibility of a bias in the sondes at extreme low temperatures.
Long-range transport of Asian dust and air pollutants to Taiwan: observed evidence and model simulation

Long-range transport of Asian dust and air pollutants are major environmental concerns of Taiwan during the winter monsoon season when northeasterly winds prevail following passages of cold fronts. Based on hourly measurements of Taiwan Environmental Protection Administration (TEPA) air quality monitoring stations, Lidar and in-situ IC, a significant long-range transport dust and air pollutants event on 18 March 2005 has been identified. During this episode, drastically elevated concentrations of PM10, CO and SO2 along with the strong northeasterly on 18 March were observed over background Wanli station, with peaks of about 170 μgm−3, 1.0 ppm and 14 ppb, respectively. We have found that air masses of air pollutants and Asian dust are transported separately. Although the mixing takes place on the way to Taiwan, it mixes slightly when they arrived in Taiwan. The major component of the first PM10 peak were air pollutants, evidenced by the consistent peaks of SO42− and NO3<sup− measured by in-situ IC, while no significant depolarization was measured by Lidar. In contrast, the evident non-spherical particles and hourly PM10 concentration consistently varied with Ca2+ indicating that mineral dust was the major component of the second peak. Trajectory analysis showed that these two peaks come from quite different sources areas. The air masses of the first peak mainly come from anthropogenic area and transport in the low boundary layer (<1500 m) while the masses of the second peak originate from high altitude (>4000 m) of desert areas. Numerical results showed significant agreement of temporal and vertical variation of aerosol concentration with observations. The phenomena of split air parcels between air pollutants and Asian dust transported to Taiwan are strongly associated with the transport paths and stable and dry atmospheric boundary conditions.
First Odin sub-mm retrievals in the tropical upper troposphere: ice cloud properties

More accurate global measurements of the amount of ice in thicker clouds are needed to validate atmospheric models and sub-mm radiometry can be an important component in this respect. A cloud ice retrieval scheme for the first such instrument in space, Odin-SMR, is presented here. Several advantages of sub-mm observations are shown, such as low influence of particle shape and orientation, and a high dynamic range of the retrievals. In the case of Odin-SMR, only cloud ice above ≈12.5 km can be measured. The present retrieval scheme gives a detection threshold of about 4 g/m2 above 12.5 km and does not saturate even for thickest observed clouds (>500 g/m2). The main retrieval uncertainties are the assumed particle size distribution and cloud inhomogeneity effects. The overall retrieval accuracy is estimated to be ~75%. The retrieval error is judged to have large random components and to be significantly lower than this value for averaged results, but high fixed errors can not be excluded. However, a firm lower value can always be provided. Initial results are found to be consistent with similar Aura MLS retrievals, but show important differences to corresponding data from atmospheric models. This first retrieval algorithm is limited to lowermost Odin-SMR tangent altitudes, and further development should improve the detection threshold and the vertical resolution. It should also be possible to decrease the retrieval uncertainty associated with cloud inhomogeneities by detailed analysis of other data sets.
First Odin sub-mm retrievals in the tropical upper troposphere: humidity and cloud ice signals

Odin-SMR is a limb-sounder operating in the 500 GHz region with the capability of performing measurements down to altitudes of about 10 km with relatively low influence of ice clouds. Until now spectra from tropospheric tangent altitudes have been disregarded due to inadequate handling of scattering. A first method to extract upper tropospheric quantities has now been developed, yielding the humidity in two layers around 200 and 130 hPa and information on cloud ice content above 200 hPa. First results are compared with in situ MOZAIC measurements and presented to give a global view of the horizontal distribution. The seasonal structures are in agreement with other satellite measurements. The main concern for these retrievals is the calibration performance. A careful analysis indicates a systematic calibration error of about 1 K, but also a random component that differs between the two bands. The random calibration uncertainty results in retrieval errors of 10–60% depending on humidity and band. Presently this prohibits use of single retrievals, but averages can be presented with good accuracy. The fixed calibration error can largely be removed, leaving the spectroscopic uncertainties to dominate the humidity retrieval accuracy, with a worst case estimate of 30%. However, the comparison of MOZAIC data and the measurements for the 200 hPa layer shows a systematic difference of <10%. This indicates that the actual systematic error is low and gives further confidence in the capability of Odin-SMR to measure humidity in the upper tropical troposphere.
Persistence and photochemical decay of springtime total ozone anomalies in the Canadian Middle Atmosphere Model

The persistence and decay of springtime total ozone anomalies over the entire extratropics (midlatitudes plus polar regions) is analysed using results from the Canadian Middle Atmosphere Model (CMAM), a comprehensive chemistry-climate model. As in the observations, interannual anomalies established through winter and spring persist with very high correlation coefficients (above 0.8) through summer until early autumn, while decaying in amplitude as a result of photochemical relaxation in the quiescent summertime stratosphere. The persistence and decay of the ozone anomalies in CMAM agrees extremely well with observations, even in the southern hemisphere when the model is run without heterogeneous chemistry (in which case there is no ozone hole and the seasonal cycle of ozone is quite different from observations). However in a version of CMAM with strong vertical diffusion, the northern hemisphere anomalies decay far too rapidly compared to observations. This shows that ozone anomaly persistence and decay does not depend on how the springtime anomalies are created or on their magnitude, but reflects the transport and photochemical decay in the model. The seasonality of the long-term trends over the entire extratropics is found to be explained by the persistence of the interannual anomalies, as in the observations, demonstrating that summertime ozone trends reflect winter/spring trends rather than any change in summertime ozone chemistry. However this mechanism fails in the northern hemisphere midlatitudes because of the relatively large impact, compared to observations, of the CMAM polar anomalies. As in the southern hemisphere, the influence of polar ozone loss in CMAM increases the midlatitude summertime loss, leading to a relatively weak seasonal dependence of ozone loss in the Northern Hemisphere compared to the observations.
Classification of aerosol properties derived from AERONET direct sun data

Aerosol spectral measurements by sunphotometers can be characterized by three independent pieces of information: 1) the optical thickness (AOT), a measure of the column aerosol concentration, 2) the optical thickness average spectral dependence, given by the Angstrom exponent (α), and 3) the spectral curvature of α (δα). We propose a simple graphical method to visually convert (α, δα) to the contribution of fine aerosol to the AOT and the size of the fine aerosols. This information can be used to track mixtures of pollution aerosol with dust, to distinguish aerosol growth from cloud contamination and to observe aerosol humidification. The graphical method is applied to the analysis of yearly records at 8 sites in 3 continents, characterized by different levels of pollution, biomass burning and mineral dust concentrations. Results depict the dominance of fine mode aerosols in driving the AOT at polluted sites. In stable meteorological conditions, we see an increase in the size of the fine aerosol as the pollution stagnates and increases in optical thickness. Coexistence of coarse and fine particles is evidenced at the polluted sites downwind of arid regions.
Water-side turbulence enhancement of ozone deposition to the ocean

A parameterization for the deposition velocity of an ocean-reactive atmospheric gas (such as ozone) is developed. The parameterization is based on integration of the turbulent-molecular transport equation (with a chemical source term) in the ocean. It extends previous work that only considered reactions within the oceanic molecular sublayer. The sensitivity of the ocean-side transport to reaction rate and wind forcing is examined. A more complicated case with a much more reactive thin surfactant layer is also considered. The full atmosphere-ocean deposition velocity is obtained by matching boundary conditions at the interface. For an assumed ocean reaction rate of 103 s−1, the enhancement for ozone deposition by oceanic turbulence is found to be up to a factor of three for meteorological data obtained in a recent cruise off the East Coast of the U.S.
Arctic smoke – record high air pollution levels in the European Arctic due to agricultural fires in Eastern Europe in spring 2006

In spring 2006, the European Arctic was abnormally warm, setting new historical temperature records. During this warm period, smoke from agricultural fires in Eastern Europe intruded into the European Arctic and caused the most severe air pollution episodes ever recorded there. This paper confirms that biomass burning (BB) was indeed the source of the observed air pollution, studies the transport of the smoke into the Arctic, and presents an overview of the observations taken during the episode. Fire detections from the MODIS instruments aboard the Aqua and Terra satellites were used to estimate the BB emissions. The FLEXPART particle dispersion model was used to show that the smoke was transported to Spitsbergen and Iceland, which was confirmed by MODIS retrievals of the aerosol optical depth (AOD) and AIRS retrievals of carbon monoxide (CO) total columns. Concentrations of halocarbons, carbon dioxide and CO, as well as levoglucosan and potassium, measured at Zeppelin mountain near Ny Ålesund, were used to further corroborate the BB source of the smoke at Spitsbergen. The ozone (O3) and CO concentrations were the highest ever observed at the Zeppelin station, and gaseous elemental mercury was also elevated. A new O3 record was also set at a station on Iceland. The smoke was strongly absorbing – black carbon concentrations were the highest ever recorded at Zeppelin – and strongly perturbed the radiation transmission in the atmosphere: aerosol optical depths were the highest ever measured at Ny Ålesund. We furthermore discuss the aerosol chemical composition, obtained from filter samples, as well as the aerosol size distribution during the smoke event. Photographs show that the snow at a glacier on Spitsbergen became discolored during the episode and, thus, the snow albedo was reduced. Samples of this polluted snow contained strongly elevated levels of potassium, sulphate, nitrate and ammonium ions, thus relating the discoloration to the deposition of the smoke aerosols. This paper shows that, to date, BB has been underestimated as a source of aerosol and air pollution for the Arctic, relative to emissions from fossil fuel combustion. Given its significant impact on air quality over large spatial scales and on radiative processes, the practice of agricultural waste burning should be banned in the future.
Investigations of the photochemical isotope equilibrium between O2, CO2 and O3

Contrary to tropospheric CO2 whose oxygen isotopic composition follows a standard mass dependent relationship, i.e. δ17O~0.5δ18O, stratospheric CO2 is preferentially enriched in 17O, leading to a strikingly different relation: δ17O~1.7δ18O. It has been shown repeatedly that the isotope anomaly is inherited from O3 via photolytically produced O(1D) that undergoes isotope exchange with CO2 and the anomaly may well serve as a tracer of stratospheric chemistry if details of the exchange mechanism are understood. We have studied the photochemical isotope equilibrium in UV-irradiated O2-CO2 and O3-CO2 mixtures to quantify the transfer of the anomaly from O3 to CO2 at room temperature. By following the time evolution of the oxygen isotopic compositions of CO2 and O2 under varying initial isotopic compositions of both, O2/O3 and CO2, the isotope equilibria between the two reservoirs were determined. A very strong dependence of the isotope equilibrium on the O2/CO2-ratio was established. Equilibrium enrichments of 17O and 18O in CO2 relative to O2 diminish with increasing CO2 content, and this reduction in the equilibrium enrichments does not follow a standard mass dependent relation. When molecular oxygen exceeds the amount of CO2 by a factor of about 20, 17O and 18O in equilibrated CO2 are enriched by (142±4)&permil; and (146±4)&permil;, respectively, at room temperature and at a pressure of 225 hPa, independent of the initial isotopic compositions of CO2 and O2 or O3. From these findings we derive a simple and general relation between the starting isotopic compositions and amounts of O2 and CO2 and the observed slope in a three oxygen isotope diagram. Predictions from this relation are compared with published laboratory and atmospheric data.
Observing cirrus halos to constrain in-situ measurements of ice crystal size

In this study, characteristic optical sizes of ice crystals in synoptic cirrus are determined using airborne measurements of ice crystal size distributions, optical extinction and water content. The measurements are compared with coincident visual observations of ice cloud optical phenomena, in particular the 22° and 46° halos. In general, the scattering profiles derived from the in-situ cloud probe measurements are consistent with the observed halo characteristics. It is argued that this implies that the measured ice crystals were small, probably with characteristic optical radii between 10 and 20 μm. There is a current contention that in-situ measurements of high concentrations of small ice crystals reflect artifacts from the shattering of large ice crystals on instrument inlets. Significant shattering cannot be entirely excluded using this approximate technique, but it is not indicated. On the basis of the in-situ measurements, a parameterization is provided that relates the optical effective radius of ice crystals to the temperature in mid-latitude synoptic cirrus.