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Highly-resolved vertical profiles of ozone and reactive nitrogen in the lower troposphere were obtained using Millersville University's tethered balloon system and NASA's P-3B aircraft during the July 2011 Baltimore, MD/Washington DC and the September 2013 Houston, TX deployments of the NASA DISCOVER-AQ air quality field mission. The tethered balloon and surface measurement sites were located at Edgewood, MD and Smith Point, TX. The balloon profiles are used to connect aircraft data from the lowest portion of NASA's P-3B spirals (300 m AGL) to the surface thus creating complete profiles from the surface to 3–5 km AGL. The highest concentrations of surface ozone at these coastal sites resulted from mean flow transport of polluted air over an adjacent body of water followed by advection back over land several hours later, due to a bay or gulf breeze. Several meteorological processes including horizontal advection, vertical mixing, thermally direct circulation (i.e., bay, gulf, and, sea breezes) combined with chemical processes like photochemical production and deposition played a role in the local ozone maxima. Several small-scale, but highly polluted layers from the Chesapeake Bay advected landward over Edgewood, MD. The Houston Metro area was subject to large-scale recirculation of emissions from petrochemical sources by the Gulf of Mexico and Galveston Bay breezes. [ABSTRACT FROM AUTHOR]

To investigate the variability of in situ profile shapes under a variety of meteorological and pollution conditions, results are presented of an agglomerative hierarchical cluster analysis of the in situ O 3 and NO 2 profiles for each of the four campaigns of the NASA DISCOVER-AQ mission. Understanding the observed profile variability for these trace gases is useful for understanding the accuracy of the assumed profile shapes used in satellite retrieval algorithms as well as for understanding the correlation between satellite column observations and surface concentrations. The four campaigns of the DISCOVER-AQ mission took place in Maryland during July 2011, the San Joaquin Valley of California during January–February 2013, the Houston, Texas, metropolitan region during September 2013, and the Denver-Front Range region of Colorado during July–August 2014. Several distinct profile clusters emerged for the California, Texas, and Colorado campaigns for O 3 , indicating significant variability of O 3 profile shapes, while the Maryland campaign presented only one distinct O 3 cluster. In contrast, very few distinct profile clusters emerged for NO 2 during any campaign for this particular clustering technique, indicating the NO 2 profile behavior was relatively uniform throughout each campaign. However, changes in NO 2 profile shape were evident as the boundary layer evolved through the day, but they were apparently not significant enough to yield more clusters. The degree of vertical mixing (as indicated by temperature lapse rate) associated with each cluster exerted an important influence on the shapes of the median cluster profiles for O 3 , as well as impacted the correlations between the associated column and surface data for each cluster for O 3 . The correlation analyses suggest satellites may have the best chance to relate to surface O 3 under the conditions encountered during the Maryland campaign Clusters 1 and 2, which include deep, convective boundary layers and few interruptions to this connection from complex meteorology, chemical environments, or orography. The regional CMAQ model captured the shape factors for O 3 , and moderately well captured the NO 2 shape factors, for the conditions associated with the Maryland campaign, suggesting that a regional air quality model may adequately specify a priori profile shapes for remote sensing retrievals. CMAQ shape factor profiles were not as well represented for the other regions. [ABSTRACT FROM AUTHOR]

Predictions of O 3 , CO, total NO y and individual NO y species (NO, NO 2 , HNO 3 , PAN, alkyl nitrates and aerosol nitrate) from a fine resolution regional air quality modeling system for the South Coast Air Basin (SoCAB) and San Joaquin Valley Air Basin (SJVAB) of California are presented and evaluated for the 2008 ARCTAS-CARB campaign. The measurements of the chemical compounds from the fire plumes during the field campaign allow for the evaluation of the model's ability to simulate fire-influenced air masses as well. In general, the model successfully simulated the broad spatial distribution of chemical compounds in both air basins as well as the variation within the basins. Using inventories that reflect 2008 emissions levels, the model performed well in simulating NO x (NO + NO 2 ) in SoCAB. Therefore, the under prediction of O 3 over these areas is more likely caused by uncertainties with the VOC emissions, chemistry, or discrepancies in the meteorology. The model did not capture the relatively high levels of O 3 , and some reactive nitrogen species that were measured off shore of the SoCAB, indicating potential missing sources or the transport from on shore to off shore was not successfully captured. In SJVAB, the model had good performance in simulating different chemical compounds in the Fresno and Arvin areas. However, enhanced concentrations of O 3 , NO x , HNO 3 and PAN near dairy farms were significantly underestimated in the model. Negative biases also exist for O 3 and HNO 3 near oil fields, suggesting larger uncertainties associated with these emission sources. While the model simulated the total NO y mixing ratios reasonably well, the prediction for partitioning between individual compounds showed larger uncertainties in the model simulation. Although the fire emissions inventory was updated to include the latest emissions estimates and speciation profiles, our model shows limited improvement in simulating the enhancement of O 3 , CO, and PAN under fire impact as compared to a previous version of the modeling system. Further improvements in simulating fire emissions, especially the timing and the plume injection heights, are desired in order to better simulate the impact of fires. [ABSTRACT FROM AUTHOR]

We quantify both the spatial and temporal variability of column integrated O 3 , NO 2 , CO, SO 2 , and HCHO over the Baltimore/Washington, DC area using output from the Weather Research and Forecasting model with on-line chemistry (WRF/Chem) for the entire month of July 2011, coinciding with the first deployment of the NASA Earth Venture program mission Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ). Using structure function analyses, we find that the model reproduces the spatial variability observed during the campaign reasonably well, especially for O 3 . The Tropospheric Emissions: Monitoring of Pollution (TEMPO) instrument will be the first NASA mission to make atmospheric composition observations from geostationary orbit and partially fulfills the goals of the Geostationary Coastal and Air Pollution Events (GEO-CAPE) mission. We relate the simulated variability to the precision requirements defined by the science traceability matrices of these space-borne missions. Results for O 3 from 0 to 2 km altitude indicate that the TEMPO instrument would be able to observe O 3 air quality events over the Mid-Atlantic area, even on days when the violations of the air quality standard are not widespread. The results further indicated that horizontal gradients in CO from 0 to 2 km would be observable over moderate distances (≥20 km). The spatial and temporal results for tropospheric column NO 2 indicate that TEMPO would be able to observe not only the large urban plumes at times of peak production, but also the weaker gradients between rush hours. This suggests that the proposed spatial and temporal resolutions for these satellites as well as their prospective precision requirements are sufficient to answer the science questions they are tasked to address. [ABSTRACT FROM AUTHOR]

Abstract: During a classic heat wave with record high temperatures and poor air quality from July 18 to 23, 2011, an elevated reservoir of air pollutants was observed over and downwind of Baltimore, MD, with relatively clean conditions near the surface. Aircraft and ozonesonde measurements detected ∼120 ppbv ozone at 800 m altitude, but ∼80 ppbv ozone near the surface. High concentrations of other pollutants were also observed around the ozone peak: ∼300 ppbv CO at 1200 m, ∼2 ppbv NO2 at 800 m, ∼5 ppbv SO2 at 600 m, and strong aerosol optical scattering (2 × 10−4 m−1) at 600 m. These results suggest that the elevated reservoir is a mixture of automobile exhaust (high concentrations of O3, CO, and NO2) and power plant emissions (high SO2 and aerosols). Back trajectory calculations show a local stagnation event before the formation of this elevated reservoir. Forward trajectories suggest an influence on downwind air quality, supported by surface ozone observations on the next day over the downwind PA, NJ and NY area. Meteorological observations from aircraft and ozonesondes show a dramatic veering of wind direction from south to north within the lowest 5000 m, implying that the development of the elevated reservoir was caused in part by the Chesapeake Bay breeze. Based on in situ observations, CMAQ forecast simulations with 12 km resolution overestimated surface ozone concentrations and failed to predict this elevated reservoir; however, CMAQ research simulations with 4 km and 1.33 km resolution more successfully reproduced this event. These results show that high resolution is essential for resolving coastal effects and predicting air quality for cities near major bodies of water such as Baltimore on the Chesapeake Bay and downwind areas in the Northeast. [Copyright &y& Elsevier]

The nonlinear chemical processes involved in ozone production (P(O 3)) have necessitated using proxy indicators to convey information about the primary dependence of P(O 3) on volatile organic compounds (VOCs) or nitrogen oxides (NO x). In particular, the ratio of remotely sensed columns of formaldehyde (HCHO) to nitrogen dioxide (NO 2) has been widely used for studying O 3 sensitivity. Previous studies found that the errors in retrievals and the incoherent relationship between the column and the near-surface concentrations are a barrier in applying the ratio in a robust way. In addition to these obstacles, we provide calculational-observational evidence, using an ensemble of 0-D photochemical box models constrained by DC-8 aircraft measurements on an ozone event during the Korea-United States Air Quality (KORUS-AQ) campaign over Seoul, to demonstrate the chemical feedback of NO 2 on the formation of HCHO is a controlling factor for the transition line between NO x -sensitive and NO x -saturated regimes. A fixed value (~2.7) of the ratio of the chemical loss of NO x (LNO x) to the chemical loss of HO 2 +RO 2 (LRO x) perceptibly differentiates the regimes. Following this value, data points with a ratio of HCHO/NO 2 less than 1 can be safely classified as NO x -saturated regime, whereas points with ratios between 1 and 4 fall into one or the other regime. We attribute this mainly to the HCHO-NO 2 chemical relationship causing the transition line to occur at larger (smaller) HCHO/NO 2 ratios in VOC-rich (VOC-poor) environments. We then redefine the transition line to LNO x /LRO x ~2.7 that accounts for the HCHO-NO 2 chemical relationship leading to HCHO = 3.7 × (NO 2 – 1.14 × 1016 molec.cm-2). Although the revised formula is locally calibrated (i.e., requires for readjustment for other regions), its mathematical format removes the need for having a wide range of thresholds used in HCHO/NO 2 ratios that is a result of the chemical feedback. Therefore, to be able to properly take the chemical feedback into consideration, the use of HCHO = a × (NO 2 – b) formula should be preferred to the ratio in future works. We then use the Geostationary Trace gas and Aerosol Sensor Optimization (GeoTASO) airborne instrument to study O 3 sensitivity in Seoul. The unprecedented spatial (250 × 250 m2) and temporal (~every 2 h) resolutions of HCHO and NO 2 observations form the sensor enhance our understanding of P(O 3) in Seoul; rather than providing a crude label for the entire city, more in-depth variabilities in chemical regimes are observed that should be able to inform mitigation strategies correspondingly. • Ozone sensitivity over Seoul on an exceptionally degraded air quality day. • Various thresholds for HCHO/NO 2 should be defined to label chemical regimes. • The inherent dependence of HCHO production on NO x levels complicates the ratio. • We redesign the formula to reflect the chemical feedback of NO x on HCHO. • GeoTASO provides in-depth variabilities in chemical regimes over Seoul. [ABSTRACT FROM AUTHOR]