ALBERT

Beschreibung: Impacts of uncertain climate forecasts on future regional air quality are investigated using downscaled MM5 meteorological fields from the NASA GISS and MIT IGSM global climate models and the CMAQ model in 2050 in the continental US. Three future climate scenarios: high-extreme, low-extreme and base, are developed for regional air quality simulations. GISS, with the IPCC A1B scenario, is used for the base case. IGSM results, in the form of probabilistic distributions, are used to perturb the base case climate to provide 0.5th and 99.5th percentile climate scenarios. Impacts of the extreme climate scenarios on concentrations of summertime fourth-highest daily maximum 8-h average ozone are predicted to be up to 10 ppbv (about one-eighth of the current NAAQS of ozone) in some urban areas, though average differences in ozone concentrations are about 1–2 ppbv on a regional basis. Differences between the extreme and base scenarios in annualized PM2.5 levels are very location dependent and predicted to range between −1.0 and +1.5 μg m−3. Future annualized PM2.5 is less sensitive to the extreme climate scenarios than summertime peak ozone since precipitation scavenging is only slightly affected by the extreme climate scenarios examined. Relative abundances of biogenic VOC and anthropogenic NOx lead to the areas that are most responsive to climate change. Such areas may find that climate change can significantly offset air quality improvements from emissions reductions, particularly during the most severe episodes.

Beschreibung: Lightning NOx emissions calculated using the U.S. National Lightning Detection Network data were found to account for 30% of the total NOx emissions for July–August 2004, a period chosen both for having higher lightning NOx production and high ozone levels, thus maximizing the likelihood that such emissions could impact peak ozone levels. Including such emissions led to modest, but sometimes significant increases in simulated surface ozone when using the Community Multi-scale Air Quality Model (CMAQ). Three model simulations were performed, two with the addition of lightning NOx emissions, and one without. Domain-wide daily maximum 8-h ozone changes due to lightning NOx were less than 2 ppbv in 71% of the cases with a maximum of 10-ppbv; whereas the difference in 1-h ozone was less than 2 ppbv in 77% of the cases with a maximum of 6 ppbv. Daily maximum 1-h and 8-h ozone for grids containing O3 monitoring stations changed slightly, with more than 43% of the cases differing less than 2 ppbv. The greatest differences were 42-ppbv for both 1-h and 8-h O3, though these tended to be on days of lower ozone. Lightning impacts on the season-wide maximum 1-h and 8-h averaged ozone decreased starting from the 1st to 4th highest values (an average of 4th highest, 8-h values is used for attainment demonstration in the U.S.). Background ozone values from the y-intercept of O3 versus NOz curve were 42.2 and 43.9 ppbv for simulations without and with lightning emissions, respectively. Results from both simulations with lightning NOx suggest that while North American lightning production of NOx can lead to significant local impacts on a few occasions, they will have a relatively small impact on typical maximum levels and determination of Policy Relevant Background levels.

Beschreibung: Measurements of atmospheric gases and fine particle chemistry were made in the Mexico City Metropolitan Area (MCMA) at a site ~30 km down wind of the city center. Ammonium nitrate (NH4NO3) dominated the inorganic aerosol fraction and showed a distinct diurnal signature characterized by rapid morning production and a rapid mid-day concentration decrease. The concentration increase was due to both secondary formation and entrainment from the free troposphere. A majority (approximately two-thirds) of the midday concentration decrease was caused by dilution from boundary layer expansion, however a significant fraction (approximately one-third) of the nitrate loss was due to particle evaporation. The water-soluble organic carbon fraction of fine particles (WSOC) and nitrate were highly correlated (R2=0.80) for the entire three-day analysis period, however the WSOC-nitrate correlation was highest (R2=0.88) between the hours of 08:00–12:45, indicating similar sources and processing during this period. The results show that WSOC also experienced evaporation losses and that a significant fraction of the MCMA secondary organic aerosol (SOA) measured at the surface was semi-volatile.

Beschreibung: Open-ocean and surf-zone sea-salt aerosol (SSA) emissions algorithms are incorporated in the CAMx aerosol model and applied over an area with an extended Archipelago (Greece), with a fine grid nested over the highly populated Attica peninsula. The maximum indirect impact of SSA on PM10 mass (35%) is located over a marine area with moderate SSA production and elevated shipping emissions (central Aegean Sea) where SSA interacts with anthropogenic nitric acid forming sodium nitrate. SSA increases PM10 levels in the Athens city center up to 27% during stable onshore winds. Under such conditions both open-ocean and surf-zone mechanisms contribute to aerosol production over Attica. A hybrid scheme for gas-to-particle mass transfer is necessary for accurately simulating semi-volatile aerosol components when coarse SSA is included. Dynamically simulating mass transfer to the coarse particles leads to a quadrupling of predicted PM10 nitrate in the Athens city center and up to two orders of magnitude in its coarse mass in comparison to using a bulk equilibrium approach.

Beschreibung: Potential impacts of global climate and emissions changes on regional air quality over southern (western and eastern) Canada and northern Mexico are examined by comparing future summers' (i.e., 2049–2051) average regional O3 and PM2.5 concentrations with historic concentrations (i.e., 2000–2002 summers). Air quality modeling was conducted using CMAQ and meteorology downscaled from the GISS-GCM using MM5. Emissions for North America are found using US EPA, Mexican and Canadian inventories and projected emissions following CAIR and IPCC A1B emissions scenario. Higher temperatures for all sub-regions and regional changes in mixing height, insolation and precipitation are forecast in the 2049–2051 period. Future emissions are calculated to be lower over both Canadian sub-regions, but higher over northern Mexico. Global climate change, alone, is predicted to affect PM2.5 concentrations more than O3: M8hO3 concentrations are estimated to be slightly different in all examined sub-regions while PM2.5 concentrations are estimated to be higher over both Canadian sub-regions (8% over western and 3% over eastern) but 11% lower over northern Mexico. Climate change combined with the projected emissions lead to greater change in pollutant concentrations: M8hO3 concentrations are simulated to be 6% lower over western Canada and 8% lower over eastern Canada while PM2.5 concentrations are simulated to be 5% lower over western Canada and 11% lower over eastern Canada. Although future emissions over northern Mexico are projected higher, pollutant concentrations are simulated to be lower due to US emissions reductions. Global climate change combined with the projected emissions will decrease M8hO3 4% and PM2.5 17% over northern Mexico.

Beschreibung: This paper presents estimates of the spectral solar absorption due to atmospheric aerosols during the 2006 MILAGRO/INTEX-B (Megacity Initiative-Local And Global Research Observations/Phase B of the Intercontinental Chemical Transport Experiment) field campaign. The aerosol absorption was derived from measurements of the spectral solar radiation and the spectral aerosol optical depth made on the J31 aircraft flying over the Gulf of Mexico and over Mexico City. We present the spectral single scattering albedo (SSA) and aerosol absorption optical depth (AAOD) for two flights over the Gulf of Mexico and three flights over Mexico City for wavelengths from 350 to approximately 1650 nm. The spectral aerosol optical properties of each case are different and illustrate the variability of the aerosol optical properties in the Mexico City area. The results can be described in terms of three different wavelength region: The 350–500 nm region where the aerosol absorption often falls off sharply presumably due to organic carbonaceous particles and windblown dust; the 500–1000 nm region where the decrease with wavelength is slower presumably due to black carbon; and the near infrared spectral region (1000 nm to 1650 nm) where it is difficult to obtain reliable results since the aerosol absorption is relatively small and the gas absorption dominates. However, there is an indication of a small and somewhat wavelength independent absorption in the region beyond 1000 nm. For one of the flights over the Gulf of Mexico near the coastline it appears that a cloud/fog formation and evaporation led to an increase of absorption possibly due to a water shell remaining on the particles after the cloud/fog had dissipated. For two of the Mexico City cases, the single scattering albedo is roughly constant between 350–500 nm consistent with other Mexico City results. In three of the cases a single absorption Angstrom exponent (AAE) fits the aerosol absorption optical depth over the entire wavelength range of 350 to 1650 nm relatively well (r2〉0.86).

Beschreibung: In this study, the Community Multiscale Air Quality (CMAQ) modeling system is used to simulate the ozone (O3) episodes during the Program of Regional Integrated Experiments of Air Quality over the Pearl River Delta, China, in October 2004 (PRIDE-PRD2004). The simulation suggests that O3 pollution is a regional phenomenon in the PRD. Elevated O3 levels often occurred in the southwestern inland PRD, Pearl River estuary (PRE), and southern coastal areas during the 1-month field campaign. Three evolution patterns of simulated surface O3 are summarized based on different near-ground flow conditions. More than 75% of days featured interaction between weak synoptic forcing and local sea-land circulations. Integrated process rate (IPR) analysis shows that photochemical production is the dominant contributor to O3 enhancement from 09:00 to 15:00 LST (local standard time) in the atmospheric boundary layer over most areas with elevated O3 occurrence in the mid-afternoon. The simulated ozone production efficiency is 2–8 O3 molecules per NOx molecule oxidized in areas with high O3 chemical production. Precursors of O3 originating from different source regions in the central PRD are mixed during transport to downwind rural areas during nighttime and early morning, where they then contribute to the daytime O3 photochemical production. Such close interactions among precursor emissions, transports, and O3 photochemical production result in the regional O3 pollution over the PRD. Sensitivity studies suggest that O3 formation is volatile organic compound-limited in the central inland PRD, PRE, and surrounding coastal areas with less chemical aging (NOx/NOy〉0.6), but is NOx-limited in the rural southwestern PRD with photochemically aged air (NOx/NOy

Beschreibung: The first three Canadian Arctic Atmospheric Chemistry Experiment (ACE) Validation Campaigns at Eureka (80° N, 86° W) were during two extremes of Arctic winter variability: Stratospheric sudden warmings (SSWs) in 2004 and 2006 were among the strongest, most prolonged on record; 2005 was a record cold winter. New satellite measurements from ACE-Fourier Transform Spectrometer (ACE-FTS), Sounding of the Atmosphere using Broadband Emission Radiometry, and Aura Microwave Limb Sounder (MLS), with meteorological analyses and Eureka lidar and radiosonde temperatures, are used to detail the meteorology in these winters, to demonstrate its influence on transport and chemistry, and to provide a context for interpretation of campaign observations. During the 2004 and 2006 SSWs, the vortex broke down throughout the stratosphere, reformed quickly in the upper stratosphere, and remained weak in the middle and lower stratosphere. The stratopause reformed at very high altitude, above where it could be accurately represented in the meteorological analyses. The 2004 and 2006 Eureka campaigns were during the recovery from the SSWs, with the redeveloping vortex over Eureka. 2005 was the coldest winter on record in the lower stratosphere, but with an early final warming in mid-March. The vortex was over Eureka at the start of the 2005 campaign, but moved away as it broke up. Disparate temperature profile structure and vortex evolution resulted in much lower (higher) temperatures in the upper (lower) stratosphere in 2004 and 2006 than in 2005. Satellite temperatures agree well with Eureka radiosondes, and with lidar data up to 50–60 km. Consistent with a strong, cold upper stratospheric vortex and enhanced radiative cooling after the SSWs, MLS and ACE-FTS trace gas measurements show strongly enhanced descent in the upper stratospheric vortex during the 2004 and 2006 Eureka campaigns compared to that in 2005.

Beschreibung: We have determined the solar spectral absorption optical depth of atmospheric aerosols for specific case studies during several field programs (three cases have been reported previously; two are new results). We combined airborne measurements of the solar net radiant flux density and the aerosol optical depth with a detailed radiative transfer model for all but one of the cases. The field programs (SAFARI 2000, ACE Asia, PRIDE, TARFOX, INTEX-A) contained aerosols representing the major absorbing aerosol types: pollution, biomass burning, desert dust and mixtures. In all cases the spectral absorption optical depth decreases with wavelength and can be approximated with a power-law wavelength dependence (Absorption Angstrom Exponent or AAE). We compare our results with other recent spectral absorption measurements and discuss the limitations in using the AAE for calculating the solar absorption. We also discuss the resulting spectral single scattering albedo for these cases.