Edward V. Browell

Validation of the Saharan Dust Plume Conceptual Model Using Lidar, Meteosat, and ECMWF Data

Abstract Lidar observations collected during the Lidar In-space Technology Experiment experiment in conjunction with the Meteosat and European Centre for Medium-Range Weather Forecasts data have been used not only to validate the Saharan dust plume conceptual model constructed from the GARP (Global Atmospheric Research Programme) Atlantic Tropical Experiment data, but also to examine the vicissitudes of the Saharan aerosol including their optical depths across the west Africa and east Atlantic regions. Optical depths were evaluated from both the Meteosat and lidar data. Back trajectory calculations were also made along selected lidar orbits to verify the characteristic anticyclonic rotation of the dust plume over the eastern Atlantic as well as to trace the origin of a dust outbreak over West Africa. A detailed synoptic analysis including the satellite-derived optical depths, vertical lidar backscattering cross section profiles, and back trajectories of the 16–19 September 1994 Saharan dust outbreak over ...

Where did tropospheric ozone over southern Africa and the tropical Atlantic come from in October 1992? Insights from TOMS, GTE TRACE A, and SAFARI 1992

The seasonal tropospheric ozone maximum in the tropical South Atlantic, first recognized from satellite observations (Fishman et al., 1986, 1991), gave rise to the IGAC/ STARE/SAFARI 1992/TRACE A campaigns (International Global Atmospheric Chemistry/South Tropical Atlantic Regional Experiment/Southern African Fire Atmospheric Research Initiative/Transport and Atmospheric Chemistry Near the Equator- Atlantic) in September and October 1992. Along with a new TOMS-based method for deriving tropospheric column ozone, we used the TRACE A/SAFARI 1992 data set to put together a regional picture of the 0 3 distribution during this period. Sondes and aircraft profiling showed a troposphere with layers of high O3 (->90 ppbv) all the way to the tropopause. These features extend in a band from 0 o to 25oS, over the SE Indian Ocean, Africa, the Atlantic, and eastern South America. A combination of trajectory and photochemical modeling (the Goddard (GSFC) isentropic trajectory and tropospheric point model, respectively) shows a strong connection between regions of high ozone and concentrated biomass burning, the latter identified using satellite-derived fire counts (Justice et al., this issue). Back trajectories from a high-O3 tropical Atlantic region (column ozone at Ascension averaged 50 Dobson units (DU)) and forward trajectories from fire- rich and convectively active areas show that the Atlantic and southern Africa are supplied with O3 and O3-forming trace gases by midlevel easterlies and/or recirculating air from Africa, with lesser contributions from South American burning and urban pollution. Limited sampling in the mixed layer over Namibia shows possible biogenic sources of NO. High-level westerlies from Brazil (following deep convective transport of ozone precursors to the upper troposphere) dominate the upper tropospheric 03 budget over Natal, Ascension, and Okaukuejo (Namibia), although most enhanced O3 (75% or more) equatorward of 10oS was from Africa. Deep convection may be responsible for the timing of the seasonal tropospheric 0 3 maximum: Natal and Ascension show a 1- to 2-month lag relative to the period of maximum burning (cf. Baldy et al., this issue; Olson et al., this issue). Photochemical model calculations constrained with TRACE A and SAFARI airborne observations of O3 and 03 precursors (NOx, CO, hydrocarbons) show robust ozone formation (up to 15 ppbv O3/d or several DU/d) in a widespread, persistent, and well-mixed layer to 4 km. Slower but still positive net 03 formation took place throughout the tropical upper troposphere (cf. Pickering et al., this issue (a); Jacob et al., this issue). Thus whether it is faster rates of 0 3 formation in source regions with higher turnover rates or slower 03 production in long-lived stable layers ubiquitous in the TRACE A region, 10-30 DU tropospheric 03 above a -25-DU background can be accounted for. In summary, the 03 maximum studied in October 1992 was caused by a coincidence of abundant 03 precursors from biomass fires, a long residence time of stable air parcels over the eastern Atlantic and southern Africa, and deep convective transport of biomass burning products, with additional NO from lightning and occasionally biogenic sources.

Validation of Aura Microwave Limb Sounder stratospheric ozone measurements

[1] The Earth Observing System (EOS) Microwave Limb Sounder (MLS) aboard the Aura satellite has provided essentially daily global measurements of ozone (O3) profiles from the upper troposphere to the upper mesosphere since August of 2004. This paper focuses on validation of the MLS stratospheric standard ozone product and its uncertainties, as obtained from the 240 GHz radiometer measurements, with a few results concerning mesospheric ozone. We compare average differences and scatter from matched MLS version 2.2 profiles and coincident ozone profiles from other satellite instruments, as well as from aircraft lidar measurements taken during Aura Validation Experiment (AVE) campaigns. Ozone comparisons are also made between MLS and balloon-borne remote and in situ sensors. We provide a detailed characterization of random and systematic uncertainties for MLS ozone. We typically find better agreement in the comparisons using MLS version 2.2 ozone than the version 1.5 data. The agreement and the MLS uncertainty estimates in the stratosphere are often of the order of 5%, with values closer to 10% (and occasionally 20%) at the lowest stratospheric altitudes, where small positive MLS biases can be found. There is very good agreement in the latitudinal distributions obtained from MLS and from coincident profiles from other satellite instruments, as well as from aircraft lidar data along the MLS track.

Intrusions into the lower stratospheric Arctic vortex during the winter of 1991–1992

Investigations of the kinematics of the lower stratospheric Arctic vortex during the winter of 1991–1992 using the contour advection with surgery technique reveal three distinct events in which there was substantial intrusion of midlatitude air into the vortex, in apparent contradiction of the view that the polar vortex constitutes an isolated air mass. Two of these events, in late January and mid-February, were well documented. They were predicted in high-resolution forecasts by the European Centre for Medium-Range Weather Forecasts, most clearly in experimental forecasts with reduced diffusion. Direct confirmation of the presence of the intrusions and of their calculated locations was provided by aerosol observations from the airborne differential absorption laser lidar aboard the NASA DC-8, taken as part of the second Airborne Arctic Stratospheric Expedition campaign; aerosol-rich air of midlatitude origin was seen in the expected position of the intrusions. The reality of the February event was also confirmed by in situ measurements from the NASA ER-2. Such events may be significant for the chemical processes taking place within the winter vortex. The intrusions were evidently related to the meteorology of the northern stratosphereduring this winter and in particular to persistent tropospheric blocking over the northeastern Atlantic Ocean and western Europe and concomitant ridging into the lower stratospheric vortex in this region. Nevertheless, preliminary investigations have indicated that such events are not uncommon in other northern hemisphere winters, although no such events were found in the southern hemisphere during the Antarctic winter of 1987.

Assessment of ozone photochemistry in the western North Pacific as inferred from PEM-West A observations during the fall 1991

This study examines the influence of photochemical processes on ozone distributions in the western North Pacific. The analysis is based on data generated during NASAs western Pacific Exploratory Mission (PEM-West A) during the fall of 1991. Ozone trends were best described in terms of two geographical domains: the western North Pacific rim (WNPR) and the western tropical North Pacific (WTNP). For both geographical regions, ozone photochemical destruction, D(O3), decreased more rapidly with altitude than did photochemical formation, F(O3). Thus the ozone tendency, P(O3), was typically found to be negative for z 6–8 km. For nearly all altitudes and latitudes, observed nonmethane hydrocarbon (NMHC) levels were shown to be of minor importance as ozone precursor species. Air parcel types producing the largest positive values of P(O3) included fresh continental boundary layer (BL) air and high-altitude (z > 7 km) parcels influenced by deep convection/lightning. Significant negative P(O3) values were found when encountering clean marine BL air or relatively clean lower free-tropospheric air. Photochemical destruction and formation fluxes for the Pacific rim region were found to exceed average values cited for marine dry deposition and stratospheric injection in the northern hemisphere by nearly a factor of 6. This region was also found to be in near balance with respect to column-integrated O3 photochemical production and destruction. By contrast, for the tropical regime column-integrated O3 showed photochemical destruction exceeding production by nearly 80%. Both transport of O3 rich midlatitude air into the tropics as well as very high-altitude (10–17 km) photochemical O3 production were proposed as possible additional sources that might explain this estimated deficit. Results from this study further suggest that during the fall time period, deep convection over Asia and Malaysia/Indonesia provided a significant source of high-altitude NOx to the western Pacific. Given that the high-altitude NOx lifetime is estimated at between 3 and 9 days, one would predict that this source added significantly to high altitude photochemical O3 formation over large areas of the western Pacific. When viewed in terms of strong seasonal westerly flow, its influence would potentially span a large part of the Pacific.

Reactive nitrogen and ozone over the western Pacific: Distribution, partitioning, and sources

Measurements of important reactive nitrogen species (NO, NO2, HNO3, PAN, PPN, NO3−, NOy), C1 to C6 hydrocarbons, O3, chemical tracers (C2Cl4, CO), and meteorological parameters were made in the troposphere (0 to 12 km) over the western Pacific (0°–50°N) during the Pacific Exploratory Mission-West A campaign (September–October 1991). Under clean conditions, mixing ratios of NO, NO2, NOy, and O3 increased with altitude and showed a distinct latitudinal gradient. PAN showed a midtropospheric maximum, while nitric acid mixing ratios were generally highest near the surface. Measured NOy concentrations were significantly greater than the sum of individually measured nitrogen species (mainly NOx, PAN, and HNO3), suggesting that a large fraction of reactive nitrogen present in the atmosphere is made up of hitherto unknown species. This shortfall was larger in the tropics (≈65%) compared to midlatitudes (≈40%) and was minimal in air masses with high HNO3 mixing ratios (>100 ppt). A global three-dimensional photochemical model has been used to compare observations with predictions and to assess the significance of major sources. It is possible that the tropical lightning source is much greater than commonly assumed, and both lightning source and its distribution remain a major area of uncertainty in the budgets of NOy and NOx. A large disagreement between measurement and theory exists in the atmospheric distribution of HNO3. It appears that surface-based anthropogenic emissions provide nearly 65% of the global atmospheric NOy reservoir. Relatively constant NOx/NOy ratios imply that NOy and NOx are in chemical equilibrium and the NOy reservoir may be an important in situ source of atmospheric NOx. Data are interpreted to suggest that only about 20% of the upper tropospheric (7–12 km) NOx is directly attributable to its surface NOx source, and free tropospheric sources are dominant. In situ release of NOx from the NOy reservoir, lightning, direct transport of surface NOx, aircraft emissions, and small stratospheric input collectively maintain the NOx balance in the atmosphere. It is shown that atmospheric ratios of reactive nitrogen and sulfur species, along with trajectory analysis, can be used to pinpoint the source of Asian continental outflow. Compared to rural atmospheres over North America, air masses over the Pacific are highly efficient in net O3 production. Sources of tropospheric NOx cannot yet be accurately defined due to shortcomings in measurements and theory.

Processes influencing ozone levels in Alaskan forest fire plumes during long-range transport over the North Atlantic

[1] A case of long-range transport of a biomass burning plume from Alaska to Europe is analyzed using a Lagrangian approach. This plume was sampled several times in the free troposphere over North America, the North Atlantic and Europe by three different aircraft during the IGAC Lagrangian 2K4 experiment which was part of the ICARTT/ ITOP measurement intensive in summer 2004. Measurements in the plume showed enhanced values of CO, VOCs and NOy, mainly in form of PAN. Observed O-3 levels increased by 17 ppbv over 5 days. A photochemical trajectory model, CiTTyCAT, was used to examine processes responsible for the chemical evolution of the plume. The model was initialized with upwind data and compared with downwind measurements. The influence of high aerosol loading on photolysis rates in the plume was investigated using in situ aerosol measurements in the plume and lidar retrievals of optical depth as input into a photolysis code (Fast-J), run in the model. Significant impacts on photochemistry are found with a decrease of 18% in O-3 production and 24% in O-3 destruction over 5 days when including aerosols. The plume is found to be chemically active with large O-3 increases attributed primarily to PAN decomposition during descent of the plume toward Europe. The predicted O-3 changes are very dependent on temperature changes during transport and also on water vapor levels in the lower troposphere which can lead to O-3 destruction. Simulation of mixing/dilution was necessary to reproduce observed pollutant levels in the plume. Mixing was simulated using background concentrations from measurements in air masses in close proximity to the plume, and mixing timescales ( averaging 6.25 days) were derived from CO changes. Observed and simulated O-3/CO correlations in the plume were also compared in order to evaluate the photochemistry in the model. Observed slopes change from negative to positive over 5 days. This change, which can be attributed largely to photochemistry, is well reproduced by multiple model runs even if slope values are slightly underestimated suggesting a small underestimation in modeled photochemical O-3 production. The possible impact of this biomass burning plume on O-3 levels in the European boundary layer was also examined by running the model for a further 5 days and comparing with data collected at surface sites, such as Jungfraujoch, which showed small O-3 increases and elevated CO levels. The model predicts significant changes in O-3 over the entire 10 day period due to photochemistry but the signal is largely lost because of the effects of dilution. However, measurements in several other BB plumes over Europe show that O-3 impact of Alaskan fires can be potentially significant over Europe.

Aerosols from biomass burning over the tropical South Atlantic region: Distributions and impacts

The NASA Global Tropospheric Experiment (GTE) Transport and Atmospheric Chemistry Near the Equator-Atlantic (TRACE A) expedition was conducted September 21 through October 26, 1992, to investigate factors responsible for creating the seasonal South Atlantic tropospheric ozone maximum. During these flights, fine aerosol (0.1–3.0 μm) number densities were observed to be enhanced roughly tenfold over remote regions of the tropical South Atlantic and greater over adjacent continental areas, relative to northern hemisphere observations and to measurements recorded in the same area during the wet season. Chemical and meteorological analyses as well as visual observations indicate that the primary source of these enhancements was biomass burning occurring within grassland regions of north central Brazil and southeastern Africa. These fires exhibited fine aerosol (N) emission ratios relative to CO (dN/dCO) of 22.5 ± 9.7 and 23.6 ± 15.1 cm−3 parts per billion by volume (ppbv)−1 over Brazil and Africa, respectively. Convection coupled with counterclockwise flow around the South Atlantic subtropical anticyclone subsequently distributed these aerosols throughout the remote South Atlantic troposphere. We calculate that dilute smoke from biomass burning produced an average tenfold enhancement in optical depth over the continental regions as well as a 50% increase in this parameter over the middle South Atlantic Ocean; these changes correspond to an estimated net cooling of up to 25 W m−2 and 2.4 W m−2 during clear-sky conditions over savannas and ocean respectively. Over the ocean our analyses suggest that modification of CCN concentrations within the persistent eastern Atlantic marine stratocumulus clouds by entrainment of subsiding haze layers could significantly increase cloud albedo resulting in an additional surface radiative cooling potentially greater in magnitude than that caused by direct extinction of solar radiation by the aerosol particles themselves.

Ozone and aerosol distributions and air mass characteristics over the South Pacific during the burning season

In situ and laser remote measurements of gases and aerosols were made with airborne instrumentation to establish a baseline chemical signature of the atmosphere above the South Pacific Ocean during the NASA Global Tropospheric Experiment (GTE)/Pacific Exploratory Mission-Tropics A (PEM-Tropics A) conducted in August-October 1996. This paper discusses general characteristics of the air masses encountered during this experiment using an airborne lidar system for measurements of the large-scale variations in ozone (O3) and aerosol distributions across the troposphere, calculated potential vorticity (PV) from the European Centre for Medium-Range Weather Forecasting (ECMWF), and in situ measurements for comprehensive air mass composition. Between 8°S and 52°S, biomass burning plumes containing elevated levels of O3, over 100 ppbv, were frequently encountered by the aircraft at altitudes ranging from 2 to 9 km. Air with elevated O3 was also observed remotely up to the tropopause, and these air masses were observed to have no enhanced aerosol loading. Frequently, these air masses had some enhanced PV associated with them, but not enough to explain the observed O3 levels. A relationship between PV and O3 was developed from cases of clearly defined O3 from stratospheric origin, and this relationship was used to estimate the stratospheric contribution to the air masses containing elevated O3 in the troposphere. The frequency of observation of the different air mass types and their average chemical composition is discussed in this paper.

Aircraft observations of thin cirrus clouds near the tropical tropopause

This work describes aircraft-based lidar observations of thin cirrus clouds at the tropical tropopause in the central Pacific obtained during the Tropical Ozone Transport Experiment/Vortex Ozone Transport Experiment (TOTE/VOTE) in December 1995 and February 1996. Thin cirrus clouds were found at the tropopause on each of the four flights which penetrated within 15° of the equator at 200–210 east longitude. South of 15°N, thin cirrus were detected above the aircraft about 65% of the time that data were available. The altitudes of these clouds exceeded 18 km at times. The cirrus observations could be divided into two basic types: thin quasi-laminar wisps and thicker, more textured structures. On the basis of trajectory analyses and temperature histories, these two types were usually formed respectively by (1) in situ cooling on both a synoptic scale and mesoscale and (2) recent (a few days) outflow from convection. There is evidence from one case that the thicker clouds can also be formed by in situ cooling. The actual presence or absence of thin cirrus clouds was also consistent with the temperature and convective histories derived from back trajectory calculations. Notably, at any given time, only a relatively small portion (at most 25%) of the west central tropical Pacific has been influenced by convection within the previous 10 days. The structures of some of the thin cirrus clouds formed in situ strongly resembled long-wavelength (500–1000 km) gravity waves observed nearly simultaneously by the ER-2 on one of the flights. Comparison with in situ water vapor profiles made by the NASA ER-2 aircraft provide some observational support for the hypothesis that thin cirrus clouds play an important role in dehydrating tropospheric air as it enters the stratosphere.