Ozone, a major contributor to poor air quality, has an array of adverse effects on human, animal, and plant health. In the Los Angeles basin, a megacity that has pursued cleaner air for decades, unhealthy levels of ozone have decreased but remain stubbornly frequent even as the ozone precursors NO x (nitrogen oxides ≡ NO 2 + NO) and VOC (volatile organic compounds) have decreased. We describe a combined analysis of decadal trends in these precursors, differences in emissions with day-of-week, and of the impact of temperature to assess the role of VOC and NO x and the likely effects of additional emission reductions on the occurrence of high ozone in the region.
Air quality policy in the Los Angeles megacity is a guidepost for other megacities. Over the last 2 decades, the policy has substantially reduced aerosol (OA) concentrations and the frequency of high aerosol events in the region. During this time, the emissions contributing to, and the temperature associated with, high aerosol events have changed. Early in the record, aerosol concentrations responded to a variety of different sources. We show that emission control has been effective with a strong decrease in temperature-independent sources. As a result, the response of aerosol to temperature has become a dominant feature of high aerosol events in the basin. The organic fraction of the aerosol (OA) increases with the temperature approaching 35% at 40 °C. We describe a simple conceptual model of aerosol in Los Angeles, illustrating how benzene, toluene, ethylbenzene, and xylenes (BTEX) and isoprene, along with molecules for which these are plausible surrogates such as monoterpenes, are sufficient to explain the observed temperature dependence of PM 2.5.
Abstract. Various atmospheric sources and sinks regulate the abundance of tropospheric formaldehyde (HCHO), which is an important trace gas impacting the HOx (≡ HO2 + OH) budget and the concentration of ozone (O3). In this study, we present the formation and destruction terms of ambient HCHO and O3 calculated from in situ observations of various atmospheric trace gases measured at three different sites across Europe during summertime. These include a coastal site in Cyprus, in the scope of the Cyprus Photochemistry Experiment (CYPHEX) in 2014, a mountain site in southern Germany, as part of the Hohenpeißenberg Photochemistry Experiment (HOPE) in 2012, and a forested site in Finland, where measurements were performed during the Hyytiälä United Measurements of Photochemistry and Particles (HUMPPA) campaign in 2010. We show that, at all three sites, formaldehyde production from the OH oxidation of methane (CH4), acetaldehyde (CH3CHO), isoprene (C5H8) and methanol (CH3OH) can almost completely balance the observed loss via photolysis, OH oxidation and dry deposition. Ozone chemistry is clearly controlled by nitrogen oxides (NOx ≡ NO + NO2) that include O3 production from NO2 photolysis and O3 loss via the reaction with NO. Finally, we use the HCHO budget calculations to determine whether net ozone production is limited by the availability of VOCs (volatile organic compounds; VOC-limited regime) or NOx (NOx-limited regime). At the mountain site in Germany, O3 production is VOC limited, whereas it is NOx limited at the coastal site in Cyprus. The forested site in Finland is in the transition regime.
Abstract. Mechanisms of tropospheric ozone (O3) formation are generally well understood. However, studies reporting on net ozone production rates (NOPRs) directly derived from in situ observations are challenging and are sparse in number. To analyze the role of nitric oxide (NO) in net ozone production in the upper tropical troposphere above the Atlantic Ocean and western Africa, we present in situ trace gas observations obtained during the CAFE-Africa (Chemistry of the Atmosphere: Field Experiment in Africa) campaign in August and September 2018. The vertical profile of in situ measured NO along the flight tracks reveals lowest NO mixing ratios of less than 20 pptv between 2 and 8 km altitude and highest mixing ratios of 0.15–0.2 ppbv above 12 km altitude. Spatial distribution of tropospheric NO above 12 km altitude shows that the sporadically enhanced local mixing ratios (>0.4 ppbv) occur over western Africa, which we attribute to episodic lightning events. Measured O3 shows little variability in mixing ratios at 60–70 ppbv, with slightly decreasing and increasing tendencies towards the boundary layer and stratosphere, respectively. Concurrent measurements of CO, CH4, OH, HO2 and H2O enable calculations of NOPRs along the flight tracks and reveal net ozone destruction at −0.6 to −0.2 ppbv h−1 below 6 km altitude and balance of production and destruction around 7–8 km altitude. We report vertical average NOPRs of 0.2–0.4 ppbv h−1 above 12 km altitude with NOPRs occasionally larger than 0.5 ppbv h−1 over western Africa coincident with enhanced NO. We compare the observational results to simulated data retrieved from the general circulation model ECHAM/MESSy Atmospheric Chemistry (EMAC). Although the comparison of mean vertical profiles of NO and O3 indicates good agreement, local deviations between measured and modeled NO are substantial. The vertical tendencies in NOPRs calculated from simulated data largely reproduce those from in situ experimental data. However, the simulation results do not agree well with NOPRs over western Africa. Both measurements and simulations indicate that ozone formation in the upper tropical troposphere is NOx limited.
Abstract. Nitrogen oxides (NOx) are principle components of air pollution and serve as important ozone precursors. As the San Joaquin Valley (SJV) experiences some of the worst air quality in the United States, reducing NOx emissions is a pressing need, yet quantifying current emissions is complicated due to a mixture of mobile and agriculture sources. We performed airborne eddy covariance flux measurements during the Re-Evaluating the Chemistry of Air Pollutants in CAlifornia (RECAP-CA) field campaign in June 2021. Combining footprint calculations and land cover statistics, we disaggregate the observed fluxes into component fluxes characterized by three different land cover types. On average we find emissions of 2.95 mg m-2 h-1 over highways, 1.24 mg m-2 h-1 over urban areas and 0.79 mg m-2 h-1 over croplands. The calculated NOx emissions using flux observations are utilized to evaluate anthropogenic emission inventories and soil NOx emission schemes. We show that two anthropogenic inventories for mobile sources, EMFAC (EMssion FACtor) and FIVE (Fuel-based Inventory for Vehicle Emissions), yield similar agreement with emissions derived from measured fluxes over urban regions with 24 % and 22 % low bias, respectively. Three soil NOx schemes, including MEGAN v3 (Model of Emissions of Gases and Aerosols from Nature), BEIS v3.14 (Biogenic Emission Inventory System) and BDISNP (Berkeley Dalhousie Iowa Soil NO Parameterization), show substantial underestimates over the study domain. Compared to the cultivated soil NOx emissions derived from measured fluxes, MEGAN and BEIS are lower by more than one order of magnitude and BDISNP is lower by a factor of 2.7. Despite the low bias, observed soil NOx emissions and BDISNP present a similar spatial pattern as well as temperature dependence. We conclude that soil NOx is a key feature of the NOx emissions in the SJV and that a state-of-the-science model of these emissions is needed to simulate emissions for modeling air quality in the region.
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