Surface ozone depletion episodes in the Arctic and Antarctic from historical ozonesonde records

International audienceEpisodes of ozone depletion in the lowermost Arctic atmosphere (0--2 km) at polar sunrise have been intensively studied at Alert, Canada, and are thought to result from catalytic reactions involving bromine. Recent observations of high concentrations of tropospheric BrO over large areas of the Arctic and Antarctic suggest that such depletion events should also be seen by ozonesondes at other polar stations. An examination of historical ozonesonde records shows that such events occur frequently at Alert, Eureka and Resolute, but much less frequently at Churchill and at other stations. The differences appear to be attributable to differences in surface meteorology. The long record at Resolute shows depletions since 1966, but with an apparent increase in their frequency since about 1985. This is surprising, since the Br involved in the depletion mechanism is believed to be entirely of natural origin

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%)

Mass tracking for chemical analysis: the causes of ozone formation in southern Ontario during BAQS-Met 2007

A three-level nested regional air pollution model has been used to study the processes leading to high ozone concentrations in the southern Great Lakes region of North America. The highest resolution simulations show that complex interactions between the lake-breeze circulation and the synoptic flow lead to significant enhancements in the photochemical production and transport of ozone at the local scale. Mass tracking of individual model processes show that Lakes Erie and St. Clair frequently act as photochemical ozone production regions, with average mid-day production rates of up to 3 ppbv per hour. Enhanced ozone levels are evident over these two lakes in 23-day-average surface ozone fields. Analysis of other model fields and aircraft measurements suggests that vertical circulation enhances ozone levels at altitudes up to 1500 m over Lake St. Clair, whereas subsidence enhances ozone over Lake Erie in a shallow layer only 250 m deep. Mass tracking of model transport shows that lake-breeze surface convergence zones combined with the synoptic flow can then carry ozone and its precursors hundreds of kilometers from these source areas, in narrow, elongated features. Comparison with surface mesonet ozone observations confirm the presence, magnitude, and timing of these features, which can create local ozone enhancements on the order of 30 ppbv above the regional ozone levels. Sensitivity analyses of model-predicted ozone and HO<sub>x</sub> concentrations show that most of the region is VOC-limited, and that the secondary oxidation pathways of aromatic hydrocarbons have a key role in setting the region's ozone and HO<sub>x</sub> levels

Impact of the assimilation of ozone from the Tropospheric Emission Spectrometer on surface ozone across North America

We examine the impact of assimilating ozone observations from the Tropospheric Emission Spectrometer (TES) on North American surface ozone abundances in the GEOS-Chem model in August 2006. The assimilation reduces the negative bias in the modeled free tropospheric ozone, which enhances the ozone flux into the boundary layer. Surface ozone abundances increased by as much as 9 ppb in western North America and by less than 2 ppb in the southeast, resulting in a total background source of ozone of 20-40 ppb. The enhanced ozone in the model reduced the model bias with respect to surface ozone observations in the western USA, but exacerbated it in the east. This increase in the bias in the boundary layer in the east, despite the agreement between the assimilation and ozonesonde measurements in the free troposphere, suggests errors in the ozone sources or sinks or in boundary layer mixing in the model. © 2009

Quantifying the Impact of BOReal Forest Fires on Tropospheric Oxidants Over the Atlantic Using Aircraft and Satellites (BORTAS) Experiment: Design, Execution and Science Overview

We describe the design and execution of the BORTAS (Quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites) experiment, which has the overarching objective of understanding the chemical aging of air masses that contain the emission products from seasonal boreal wildfires and how these air masses subsequently impact downwind atmospheric composition. The central focus of the experiment was a two-week deployment of the UK BAe-146-301 Atmospheric Research Aircraft (ARA) over eastern Canada, based out of Halifax, Nova Scotia. Atmospheric ground-based and sonde measurements over Canada and the Azores associated with the planned July 2010 deployment of the ARA, which was postponed by 12 months due to UK-based flights related to the dispersal of material emitted by the Eyjafjallajokull volcano, went ahead and constituted phase A of the experiment. Phase B of BORTAS in July 2011 involved the same atmospheric measurements, but included the ARA, special satellite observations and a more comprehensive ground-based measurement suite. The high-frequency aircraft data provided a comprehensive chemical snapshot of pyrogenic plumes from wildfires, corresponding to photochemical ( and physical) ages ranging from \u3c 1 day to greater than or similar to 10 days, largely by virtue of widespread fires over Northwestern Ontario. Airborne measurements reported a large number of emitted gases including semi-volatile species, some of which have not been been previously reported in pyrogenic plumes, with the corresponding emission ratios agreeing with previous work for common gases. Analysis of the NOy data shows evidence of net ozone production in pyrogenic plumes, controlled by aerosol abundance, which increases as a function of photochemical age. The coordinated ground-based and sonde data provided detailed but spatially limited information that put the aircraft data into context of the longer burning season in the boundary layer. Ground-based measurements of particulate matter smaller than 2.5 mu m ( PM2.5) over Halifax show that forest fires can on an episodic basis represent a substantial contribution to total surface PM2.5

Quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites (BORTAS) experiment: Design, execution and science overview

We describe the design and execution of the BORTAS (Quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites) experiment, which has the overarching objective of understanding the chemical aging of air masses that contain the emission products from seasonal boreal wildfires and how these air masses subsequently impact downwind atmospheric composition. The central focus of the experiment was a two-week deployment of the UK BAe-146-301 Atmospheric Research Aircraft (ARA) over eastern Canada, based out of Halifax, Nova Scotia. Atmospheric ground-based and sonde measurements over Canada and the Azores associated with the planned July 2010 deployment of the ARA, which was postponed by 12 months due to UK-based flights related to the dispersal of material emitted by the Eyjafjallajökull volcano, went ahead and constituted phase A of the experiment. Phase B of BORTAS in July 2011 involved the same atmospheric measurements, but included the ARA, special satellite observations and a more comprehensive ground-based measurement suite. The high-frequency aircraft data provided a comprehensive chemical snapshot of pyrogenic plumes from wildfires, corresponding to photochemical (and physical) ages ranging from \u3c 1 day to ∼ \u3c span styleCombining double low line position: relative; top:-.5em; left:-.80em styleCombining double low line margin-left:-.7em 45 sr 10 days, largely by virtue of widespread fires over Northwestern Ontario. Airborne measurements reported a large number of emitted gases including semi-volatile species, some of which have not been been previously reported in pyrogenic plumes, with the corresponding emission ratios agreeing with previous work for common gases. Analysis of the NOy data shows evidence of net ozone production in pyrogenic plumes, controlled by aerosol abundance, which increases as a function of photochemical age. The coordinated ground-based and sonde data provided detailed but spatially limited information that put the aircraft data into context of the longer burning season in the boundary layer. Ground-based measurements of particulate matter smaller than 2.5 μm (PM2.5) over Halifax show that forest fires can on an episodic basis represent a substantial contribution to total surface PM2.5.

A Global Ozone Climatology from Ozone Soundings via Trajectory Mapping: A Stratospheric Perspective

This study explores a domain-filling trajectory approach to generate a global ozone climatology from sparse ozonesonde data. Global ozone soundings of 51,898 profiles at 116 stations over 44 years (1965-2008) are used, from which forward and backward trajectories are performed for 4 days, driven by a set of meteorological reanalysis data. Ozone mixing ratios of each sounding from the surface to 26 km altitude are assigned to the entire path along the trajectory. The resulting global ozone climatology is archived monthly for five decades from the 1960s to the 2000s with grids of 5 degree 5 degree 1 km (latitude, longitude, and altitude). It is also archived yearly from 1965 to 2008. This climatology is validated at 20 ozonesonde stations by comparing the actual ozone sounding profile with that found through the trajectories, using the ozone soundings at all the stations except one being tested. The two sets of profiles are in good agreement, both individually with correlation coefficients between 0.975 and 0.998 and root mean square (RMS) differences of 87 to 482 ppbv, and overall with a correlation coefficient of 0.991 and an RMS of 224 ppbv. The ozone climatology is also compared with two sets of satellite data, from the Satellite Aerosol and Gas Experiment (SAGE) and the Optical Spectrography and InfraRed Imager System (OSIRIS). Overall, the ozone climatology compares well with SAGE and OSIRIS data by both seasonal and zonal means. The mean difference is generally under 20 above 15 km. The comparison is better in the northern hemisphere, where there are more ozonesonde stations, than in the southern hemisphere; it is also better in the middle and high latitudes than in the tropics, where assimilated winds are imperfect in some regions. This ozone climatology can capture known features in the stratosphere, as well as seasonal and decadal variations of these features. Furthermore, it provides a wealth of detail about longitudinal variations in the stratosphere such as the spring ozone maximum over the Canadian Arctic. It also covers higher latitudes than current satellite data. The climatology shows clearly the depletion of ozone from the 1970s to the mid 1990s and ozone recovery in the 2000s. When this climatology is used as the upper boundary condition in an Environment Canada operational chemical forecast model, the forecast is improved in the vicinity of the upper tropospherelower stratosphere region. As this ozone climatology is neither dependent on a priori data or photochemical modeling, it provides independent information and insight that can supplement satellite data and model simulations and enhance our understanding of stratospheric ozone

The influence of boreal biomass burning emissions on the distribution of tropospheric ozone over North America and the North Atlantic during 2010

We have analysed the sensitivity of the tropospheric ozone distribution over North America and the North Atlantic to boreal biomass burning emissions during the summer of 2010 using the GEOS-Chem 3-D global tropospheric chemical transport model and observations from in situ and satellite instruments. We show that the model ozone distribution is consistent with observations from the Pico Mountain Observatory in the Azores, ozonesondes across Canada, and the Tropospheric Emission Spectrometer (TES) and Infrared Atmospheric Sounding Instrument (IASI) satellite instruments. Mean biases between the model and observed ozone mixing ratio in the free troposphere were less than 10 ppbv. We used the adjoint of GEOS-Chem to show the model ozone distribution in the free troposphere over Maritime Canada is largely sensitive to NOx emissions from biomass burning sources in Central Canada, lightning sources in the central US, and anthropogenic sources in the eastern US and south-eastern Canada. We also used the adjoint of GEOS-Chem to evaluate the Fire Locating And Monitoring of Burning Emissions (FLAMBE) inventory through assimilation of CO observations from the Measurements Of Pollution In The Troposphere (MOPITT) satellite instrument. The CO inversion showed that, on average, the FLAMBE emissions needed to be reduced to 89% of their original values, with scaling factors ranging from 12% to 102%, to fit the MOPITT observations in the boreal regions. Applying the CO scaling factors to all species emitted from boreal biomass burning sources led to a decrease of the model tropospheric distributions of CO, PAN, and NOx by as much as -20 ppbv, -50 pptv, and -20 pptv respectively. The modification of the biomass burning emission estimates reduced the model ozone distribution by approximately -3 ppbv (-8%) and on average improved the agreement of the model ozone distribution compared to the observations throughout the free troposphere, reducing the mean model bias from 5.5 to 4.0 ppbv for the Pico Mountain Observatory, 3.0 to 0.9 ppbv for ozonesondes, 2.0 to 0.9 ppbv for TES, and 2.8 to 1.4 ppbv for IASI

The influence of boreal biomass burning emissions on the distribution of tropospheric ozone over North America and the North Atlantic during 2010

We have analysed the sensitivity of the tropospheric ozone distribution over North America and the North Atlantic to boreal biomass burning emissions during the summer of 2010 using the GEOS-Chem 3-D global tropospheric chemical transport model and observations from in situ and satellite instruments. We show that the model ozone distribution is consistent with observations from the Pico Mountain Observatory in the Azores, ozonesondes across Canada, and the Tropospheric Emission Spectrometer (TES) and Infrared Atmospheric Sounding Instrument (IASI) satellite instruments. Mean biases between the model and observed ozone mixing ratio in the free troposphere were less than 10 ppbv. We used the adjoint of GEOS-Chem to show the model ozone distribution in the free troposphere over Maritime Canada is largely sensitive to NO<sub>x</sub> emissions from biomass burning sources in Central Canada, lightning sources in the central US, and anthropogenic sources in the eastern US and south-eastern Canada. We also used the adjoint of GEOS-Chem to evaluate the Fire Locating And Monitoring of Burning Emissions (FLAMBE) inventory through assimilation of CO observations from the Measurements Of Pollution In The Troposphere (MOPITT) satellite instrument. The CO inversion showed that, on average, the FLAMBE emissions needed to be reduced to 89% of their original values, with scaling factors ranging from 12% to 102%, to fit the MOPITT observations in the boreal regions. Applying the CO scaling factors to all species emitted from boreal biomass burning sources led to a decrease of the model tropospheric distributions of CO, PAN, and NO<sub>x</sub> by as much as −20 ppbv, −50 pptv, and −20 pptv respectively. The modification of the biomass burning emission estimates reduced the model ozone distribution by approximately −3 ppbv (−8%) and on average improved the agreement of the model ozone distribution compared to the observations throughout the free troposphere, reducing the mean model bias from 5.5 to 4.0 ppbv for the Pico Mountain Observatory, 3.0 to 0.9 ppbv for ozonesondes, 2.0 to 0.9 ppbv for TES, and 2.8 to 1.4 ppbv for IASI