The Quasi-Biennial Oscillation in atmospheric ozone

Examination of the relationship between tropical stratosphere zonal wind and ozone indicate a variable response in latitude with Northern Hemisphere tropics and polar regions and Southern Hemisphere mid-latitudes showing the strongest response with relatively weaker response at Northern Hemisphere mid-latitudes and the Southern Hemisphere tropics. In tropical regions, the west winds and ozone maxima are in phase while at higher latitudes, a more nearly out-of-phase relationship prevails. At subtropical and middle latitudes, the QBO in ozone does not appear to change phases with altitude. These features are suggestive of an interaction between the tropical zonal winds and poleward transport of horizontal eddies in conjunction with the annual poleward transport of ozone

Airborne measurements of tropospheric ozone destruction and particulate bromide formation in the Arctic

Aircraft profiles of O3 concentrations over the Arctic ice pack in spring exhibit a depletion of O3 beneath the surface temperature inversion. One such profile from the NOAA WP-3D Arctic Gas and Aerosol Sampling Program (AGASP) flights in April, 1986 north of Alert, NWT (YLT, 82.5 N) is shown. The gradient of O3 across the temperature inversion, which is essentially a step function from tropospheric values (35 to 40 ppbv) to 0, is somewhat masked by a 1-min running mean applied to the data. Evidence is presented that O3 destruction beneath the Arctic temperature inversion is the result of a photochemical reaction between gaseous Br compounds and O3 to produce particulate Br aerosol. It is noted that in springtime, O3 at the Alert Baseline Station regularly decreases from 30 to 40 ppbv to near 0 over the period of a few hours to a day. At the same time, there is a production of particulate Br with a near 1.0 anti-correlation to O3 concentration. Surface concentrations of bromoform in the Arctic exhibit a rapid decrease following polar sunrise. AGASP aircraft measurements of filterable bromine particulates in the Arctic (March-April, 1983 and 1986) are shown. The greatest concentrations of Br aerosol (shown as enrichment factors relative to to Na in seawater, EFBR (Na)) were observed in samples collected beneath the surface temperature inversion over ice. Samples collected at the same altitude over open ocean (off Spitzbergen) labeled Marine did not exhibit similar Br enrichments. A second region of particulate Br enrichment was observed in the lower stratosphere, which regularly descends to below 500 mb (5.5 km) in the high Arctic. The NOAA WP-3D flew in the stratosphere on all AGASP flights and occasionally measured O3 concentrations in excess of 300 ppbv

Chemical transport model ozone simulations for spring 2001 over the western Pacific:comparisons with TRACE-P lidar, ozonesondes, and Total Ozone Mapping Spectrometer columns

Two closely related chemical transport models (CTMs) employing the same high-resolution meteorological data (similar to180 km x similar to180 km x similar to600 m) from the European Centre for Medium-Range Weather Forecasts are used to simulate the ozone total column and tropospheric distribution over the western Pacific region that was explored by the NASA Transport and Chemical Evolution over the Pacific (TRACE-P) measurement campaign in February-April 2001. We make extensive comparisons with ozone measurements from the lidar instrument on the NASA DC-8, with ozonesondes taken during the period around the Pacific Rim, and with TOMS total column ozone. These demonstrate that within the uncertainties of the meteorological data and the constraints of model resolution, the two CTMs (FRSGC/UCI and Oslo CTM2) can simulate the observed tropospheric ozone and do particularly well when realistic stratospheric ozone photochemistry is included. The greatest differences between the models and observations occur in the polluted boundary layer, where problems related to the simplified chemical mechanism and inadequate horizontal resolution are likely to have caused the net overestimation of about 10 ppb mole fraction. In the upper troposphere, the large variability driven by stratospheric intrusions makes agreement very sensitive to the timing of meteorological features

Trends and variability of midlatitude stratospheric water vapour deduced from the re-evaluated Boulder balloon series and HALOE

This paper presents an updated trend analysis of water vapour in the lower midlatitude stratosphere from the Boulder balloon-borne NOAA frostpoint hygrometer measurements and from the Halogen Occulation Experiment (HALOE). Two corrections for instrumental bias are applied to homogenise the frostpoint data series, and a quality assessment of all soundings after 1991 is presented. Linear trend estimates based on the corrected data for the period 1980–2000 are up to 40% lower than previously reported. Vertically resolved trends and variability are calculated with a multi regression analysis including the quasi-biennal oscillation and equivalent latitude as explanatory variables. In the range of 380 to 640 K potential temperature (≈14 to 25 km), the frostpoint data from 1981 to 2006 show positive linear trends between 0.3±0.3 and 0.7±0.1%/yr. The same dataset shows trends between −0.2±0.3 and 1.0±0.3%/yr for the period 1992 to 2005. HALOE data over the same time period suggest negative trends ranging from −1.1±0.2 to −0.1±0.1%/yr. In the lower stratosphere, a rapid drop of water vapour is observed in 2000/2001 with little change since. At higher altitudes, the transition is more gradual, with slowly decreasing concentrations between 2001 and 2007. This pattern is consistent with a change induced by a drop of water concentrations at entry into the stratosphere. Previously noted differences in trends and variability between frostpoint and HALOE remain for the homogenised data. Due to uncertainties in reanalysis temperatures and stratospheric transport combined with uncertainties in observations, no quantitative inference about changes of water entering the stratosphere in the tropics could be made with the mid latitude measurements analysed here

The role of ozone atmosphere-snow gas exchange on polar, boundary-layer tropospheric ozone ? a review and sensitivity analysis

International audienceRecent research on snowpack processes and atmosphere-snow gas exchange has demonstrated that chemical and physical interactions between the snowpack and the overlaying atmosphere have a substantial impact on the composition of the lower troposphere. These observations also imply that ozone deposition to the snowpack possibly depends on parameters including the quantity and composition of deposited trace gases, solar irradiance, snow temperature and the substrate below the snowpack. Current literature spans a remarkably wide range of ozone deposition velocities (vdO3); several studies even reported positive ozone fluxes out of the snow. Overall, published values range from ~?

On the origin of elevated surface ozone concentrations at Izana Observatory, Tenerife during late March 1996

The origin of relatively high surface ozone concentrations measured at Izana Observatory (Canary Islands) during the end of March 1996 is studied using a coupled chemistry-GCM (ECHAM4) at T63 resolution (1.875° × 1.875°). Meteorological fields (geopotential height, potential vorticity, specific humidity), and a model-simulated stratospheric ozone tracer as well as 3-D back trajectories, show the stratospheric origin of these relatively high surface ozone values caused by cross-tropopause exchange at the western flank of an upper level trough/cut-off low (COL) over the extratropical North-Atlantic Ocean. The good agreement between observations and model results (within 10–15%) indicates that the high resolution chemistry-GCM is a useful tool towards the understanding of natural sources controlling background surface ozone variability. The results underscore the importance of stratosphere-troposphere exchange (STE) during late winter/early spring for lower free tropospheric ozone at subtropical latitudes

Validation of northern latitude Tropospheric Emission Spectrometer stare ozone profiles with ARC-IONS sondes during ARCTAS: sensitivity, bias and error analysis

We compare Tropospheric Emission Spectrometer (TES) versions 3 and 4, V003 and V004, respectively, nadir-stare ozone profiles with ozonesonde profiles from the Arctic Intensive Ozonesonde Network Study (ARCIONS, http://croc.gsfc.nasa.gov/arcions/ during the Arctic Research on the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) field mission. The ozonesonde data are from launches timed to match Aura's overpass, where 11 coincidences spanned 44° N to 71° N from April to July 2008. Using the TES "stare" observation mode, 32 observations are taken over each coincidental ozonesonde launch. By effectively sampling the same air mass 32 times, comparisons are made between the empirically-calculated random errors to the expected random errors from measurement noise, temperature and interfering species, such as water. This study represents the first validation of high latitude (>70°) TES ozone. We find that the calculated errors are consistent with the actual errors with a similar vertical distribution that varies between 5% and 20% for V003 and V004 TES data. In general, TES ozone profiles are positively biased (by less than 15%) from the surface to the upper-troposphere (~1000 to 100 hPa) and negatively biased (by less than 20%) from the upper-troposphere to the lower-stratosphere (100 to 30 hPa) when compared to the ozonesonde data. Lastly, for V003 and V004 TES data between 44° N and 71° N there is variability in the mean biases (from −14 to +15%), mean theoretical errors (from 6 to 13%), and mean random errors (from 9 to 19%)

Tropospheric water-vapour and ozone cross-sections in a zonal plane over the Central Equatorial Pacific Ocean

Tropospheric water-vapour and ozone measurements, using calibrated balloon-borne sensors, are reported from the Central Equatorial Pacific Experiment (CEPEX). The sensors were launched from the Research Vessel Vickers along 2 degrees S latitude between 156 degrees E (west of the international date line) and 155 degrees W (east of the date line). These measurements are combined with those from water-vapour sondes launched over the western Pacific warm pool, during the Coupled Ocean-Atmosphere Response Experiment (TOGA-COARE). Taking the two experiments CEPEX and TOGA-COARE together, the sensors included frost-point hygrometers, Humicap-A Vaisala sondes, Humicap-H Vaisala sondes and electrochemical ozone-sondes. Taken together, the CEPEX and TOGA-COARE data provide over 150 vertical profiles of water vapour within the troposphere in varied conditions of convective activity ranging from disturbed to suppressed. The primary motivation behind the present analyses is to understand the role of tropical deep convection in the vertical distribution of water-vapour. With this in mind, the profiles have been analysed in relation to occasions of recent deep convection and occasions when convection was suppressed. We employ three different criteria to identify the profiles influenced by deep convection brightness temperature in the infrared-window channel of the Japanese Geostationary Meteorological Satellite (GMS); ozone as a quasi-conservative tracer for deep convection; and using water vapour itself, that is the wettest versus the driest soundings. Irrespective of the criteria used, we report here that the atmosphere, while under the influence of active deep convection, was found to have relative humidities in excess of 75% over most of the troposphere between the surface and about 14 km. The sondes were launched routinely over a period of 45 days (between CEPEX and TOGA-COARE), without biasing the sample towards convectively disturbed conditions. A feature of the convectively disturbed profile is a distinct minimum in relative humidity at about 700 hPa, where it was as low as 65%. The low relative humidity was accompanied by relatively high ozone mixing ratios, which raises the possibility of long-range transport of dry sub-tropical air into the warm, convectively disturbed, regions of the equatorial Pacific Ocean. Inspection of the analysed fields, and the wind fields from the sondes, supports this assertion. It then follows that the omnipresent minimum of moist static energy and minimum relative humidity at 700 hPa in the inner tropics may be the result of long-range, inclined, transport of dry air from non-convective regions. This detection suggests a linkage between the large-scale circulation, deep convection and the thermodynamic structure within the equatorial troposphere. The results presented here demonstrate the applicability of ozone as a quasi-conservative tracer of transport in the context of deep convection. The ozone-based criterion is used to diagnose recent deep convection, independent of the GMS satellite observations, and allows one to follow the evolution of relative humidity and of water-vapour mixing ratio after the dissipation of the cloud anvil to optically thin conditions. We show that the troposphere dries to low humidity soon after anvil dissipation. This observation leads to the hypothesis that moistening of the atmosphere, away from the core of Cb convection, occurs by evaporation of precipitation falling out of the anvils. After anvil dissipation, the ensuing subsidence in clear air causes the relative humidity and the water mixing ratio to decrease