Coordinated ozonesonde launches from the Intercontinental Transport Experiment (INTEX) Ozonesonde Network Study (IONS) (http://croc.gsfc.nasa.gov/intex/ions.html) in July‐August 2004 provided nearly 300 O3 profiles from eleven North American sites and the R/V Ronald H. Brown in the Gulf of Maine. With the IONS period dominated by low‐pressure conditions over northeastern North America (NENA), the free troposphere in that region was frequently enriched by stratospheric O3. Stratospheric O3 contributions to the NENA tropospheric O3 budget are computed through analyses of O3 laminae (Pierce and Grant, 1998; Teitelbaum et al., 1996), tracers (potential vorticity, water vapor), and trajectories. The lasting influence of stratospheric incursions into the troposphere is demonstrated, and the computed stratospheric contribution to tropospheric column O3 over the R/V Ronald H. Brown and six sites in Michigan, Virginia, Maryland, Rhode Island, and Nova Scotia, 23% ± 3%, is similar to summertime budgets derived from European O3 profiles (Collette and Ancellet, 2005). Analysis of potential vorticity, Wallops ozonesondes (37.9°N, 75.5°W), and Measurements of Ozone by Airbus In‐service Aircraft (MOZAIC) O3 profiles for NENA airports in June‐July‐August 1996–2004 shows that the stratospheric fraction in 2004 may be typical. Boundary layer O3 at Wallops and northeast U.S. sites during IONS also resembled O3 climatology (June‐July‐August 1996–2003). However, statistical classification of Wallops O3 profiles shows the frequency of profiles with background, nonpolluted boundary layer O3 was greater than normal during IONS.
[1] From 1997 to 2003, airborne measurements of O 3 , CO, SO 2 , and aerosol properties were made during summertime air pollution episodes over the mid-Atlantic United States (34.7-44.6°N, 68.4-81.6°W) as part of the Regional Atmospheric Measurement, Modeling, and Prediction Program (RAMMPP). Little diurnal variation was identified in the CO, SO 2 , and Å ngström exponent profiles, although the Å ngström exponent profiles decreased with altitude. Boundary layer O 3 was greater in the afternoon, while lower free tropospheric O 3 was invariant at $55 ppbv. The single scattering albedo increased from morning to afternoon (0.93 ± 0.01À0.94 ± 0.01); however, both profiles decreased with altitude. A cluster analysis of back trajectories in conjunction with the vertical profile data was used to identify source regions and characteristic transport patterns during summertime pollution episodes. When the greatest trajectory density lay over the northern Ohio River Valley, the result was large O 3 values, large SO 2 /CO ratios, highly scattering particles, and large aerosol optical depths. Maximum trajectory density over the southern Ohio River Valley resulted in little pollution. The greatest afternoon O 3 values occurred during periods of stagnation. North-northwesterly and northerly flow brought the least pollution overall. The contribution of regional transport to afternoon boundary layer O 3 was quantified. When the greatest cluster trajectory density lay over the Ohio River Valley ($59% of the profiles), transport accounted for 69-82% of the afternoon boundary layer O 3 . Under stagnant conditions ($27% of the profiles), transport only accounted for 58% of the afternoon boundary layer O 3 . The results from this study provide a description of regional chemical and transport processes that will be valuable to investigators from the Baltimore, New York, and Pittsburgh EPA Supersites.
During the TC4 (Tropical Composition, Clouds, and Climate Coupling) campaign in July–August 2007, daily ozonesondes were launched over coastal Las Tablas, Panamá (7.8°N, 80°W) and several times per week at Alajuela, Costa Rica (10°N, 84°W). Wave activity, detected most prominently in 100–300 m thick ozone laminae in the tropical tropopause layer, occurred in 50% (Las Tablas) and 40% (Alajuela) of the soundings. These layers, associated with vertical displacements and classified as gravity waves (GW, possibly Kelvin waves) by laminar identification, occur with similar structure and frequency over the Paramaribo (5.8°N, 55°W) and San Cristóbal (0.92°S, 90°W) Southern Hemisphere Additional Ozonesondes (SHADOZ) sites. GW‐labeled laminae in individual soundings correspond to cloud outflow as indicated by DC‐8 tracers and other aircraft data, confirming convective initiation of equatorial waves. Layers representing quasi‐horizontal displacements, referred to as Rossby waves by the laminar technique, are robust features in soundings from 23 July to 5 August. The features associated with Rossby waves correspond to extratropical influence, possibly stratospheric, and sometimes to pollution transport. Comparison of Las Tablas and Alajuela ozone budgets with 1999–2007 Paramaribo and San Cristóbal soundings shows that TC4 is typical of climatology for the equatorial Americas. Overall during TC4, convection and associated waves appear to dominate ozone transport in the tropical tropopause layer; intrusions from the extratropics occur throughout the free troposphere.
[1] Airborne observations made on 8 July 2002 over five locations in Virginia and Maryland revealed the presence of two discrete layers of air pollution, one of a smoke plume between $2 and 3 km above mean sea level advected from Quebec forest fires and another, underlying plume from fossil fuel combustion. Within the smoke layer, large increases were observed in submicrometer particle numbers, scattering, and absorption as well as ozone (O 3 ) and CO (but not SO 2 ) mixing ratios. The single-scattering albedos (w 0 ) in the layer between $2 and 3 km (mean value at 550 nm = 0.93 ± 0.02) were consistently smaller than those below (mean value at 550 nm = 0.95 ± 0.01). Aerosol optical depth in the lower 3 km of the atmosphere was determined at each of the five locations, and the value at 550 nm varied between 0.42 ± 0.06 and 1.53 ± 0.21. Calculations of clear-sky aerosol direct radiative forcing by the smoke plume using an atmospheric radiative transfer code indicated that the forcing at the top of the atmosphere was small relative to the forcing at the surface. Thus atmospheric absorption of solar radiation was nearly equal to the attenuation at the surface. The net effect was to cool the surface and heat the air aloft. A morning subsidence inversion positioned the smoke in a dense enough layer above the planetary boundary layer that solar heating of the layer maintained the temperature inversion through the afternoon. This created a positive feedback loop that prevented vertical mixing and dilution of the smoke plume, thereby increasing the regional radiative impact.
[1] Chemical transport models such as the Community Multiscale Air Quality (CMAQ) model provide useful guidance on air pollution control strategies. We evaluate the performance of a 12 km resolution CMAQ simulation with surface and aircraft observations of CO, O 3 , and NO x during the summer of 2002. When all data are considered, on average, modeled and observed CO total column contents (surface to 3,000 m) agreed to within 14% in the morning and 22% in the afternoon. Reducing the deposition velocity for CO improves model-measurement agreement but did not eliminate the model bias. The majority of observed vertical profiles have a maximum near the surface. Although many observed spirals had a secondary maximum at the top of the boundary layer, indicating subgrid-scale shallow convection. The model was not able to replicate these vertical structures. Water vapor profiles likewise showed greater vertical variability in the observations than in the model. General conclusions from these model-measurement comparisons: total CO emissions estimates are either adequate or underestimated,
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