Regional impacts of ultrafine particle emissions from the surface of the Great Lakes

Quantifying the impacts of aerosols on climate requires a detailed knowledge of both the anthropogenic and the natural contributions to the aerosol population. Recent work has suggested a previously unrecognized natural source of ultrafine particles resulting from breaking waves at the surface of large freshwater lakes. This work is the first modeling study to investigate the potential for this newly discovered source to affect the aerosol number concentrations on regional scales. Using the WRF-Chem modeling framework, the impacts of wind-driven aerosol production from the surface of the Great Lakes were studied for a July 2004 test case. Simulations were performed for a base case with no lake surface emissions, a case with lake surface emissions included, and a default case wherein large freshwater lakes emit marine particles as if they were oceans. Results indicate that the lake surface emissions can enhance the surface-level aerosol number concentration by ~20% over the remote northern Great Lakes and by ~5% over other parts of the Great Lakes. These results were highly sensitive to the new particle formation (i.e., nucleation) parameterization within WRF-Chem; when the new particle formation process was deactivated, surface-layer enhancements from the lake emissions increased to as much as 200%. The results reported here have significant uncertainties associated with the lake emission parameterization and the way ultrafine particles are modeled within WRF-Chem. Nevertheless, the magnitudes of the impacts found in this study suggest that further study to quantify the emissions of ultrafine particles from the surface of the Great Lakes is merited

Thermodynamic characterization of Mexico City aerosol during MILAGRO 2006

International audienceFast measurements of aerosol and gas-phase constituents coupled with the ISORROPIA-II thermodynamic equilibrium model are used to study the partitioning of semivolatile inorganic species and phase state of Mexico City aerosol sampled at the T1 site during the MILAGRO 2006 campaign. Overall, predicted semivolatile partitioning agrees well with measurements. PM2.5 is insensitive to changes in ammonia but is to acidic semivolatile species. Semi-volatile partitioning equilibrates on a timescale between 6 and 20 min. When the aerosol sulfate-to-nitrate molar ratio is less than 1, predictions improve substantially if the aerosol is assumed to follow the deliquescent phase diagram. Treating crustal species as "equivalent sodium" (rather than explicitly) in the thermodynamic equilibrium calculations introduces important biases in predicted aerosol water uptake, nitrate and ammonium; neglecting crustals further increases errors dramatically. This suggests that explicitly considering crustals in the thermodynamic calculations are required to accurately predict the partitioning and phase state of aerosols

Quantification of biogenic volatile organic compounds with a flame ionization detector using the effective carbon number concept

Biogenic volatile organic compounds (BVOCs) are emitted into the atmosphere by plants and include isoprene, monoterpenes, sesquiterpenes, and their oxygenated derivatives. These BVOCs are among the principal factors influencing the oxidative capacity of the atmosphere in forested regions. BVOC emission rates are often measured by collecting samples onto adsorptive cartridges in the field and then transporting these samples to the laboratory for chromatographic analysis. One of the most commonly used detectors in chromatographic analysis is the flame ionization detector (FID). For quantitative analysis with an FID, relative response factors may be estimated using the effective carbon number (ECN) concept. The purpose of this study was to determine the ECN for a variety of terpenoid compounds to enable improved quantification of BVOC measurements. A dynamic dilution system was developed to make quantitative gas standards of VOCs with mixing ratios from 20–55 ppb. For each experiment using this system, one terpene standard was co-injected with an internal reference, n-octane, and analyzed via an automated cryofocusing system interfaced to a gas chromatograph flame ionization detector and mass spectrometer (GC/MS/FID). The ECNs of 16 compounds (14 BVOCs) were evaluated with this approach, with each test compound analyzed at least three times. The difference between the actual carbon number and measured ECN ranged from −24% to −2%. The difference between theoretical ECN and measured ECN ranged from −22% to 9%. Measured ECN values were within 10% of theoretical ECN values for most terpenoid compounds

Characterization of ambient aerosol from measurements of cloud condensation nuclei during the 2003 Atmospheric Radiation Measurement Aerosol Intensive Observational Period at the Southern Great Plains site in Oklahoma

Measurements were made by a new cloud condensation nuclei (CCN) instrument (CCNC3) during the Atmospheric Radiation Measurement (ARM) Program's Aerosol Intensive Observational Period (IOP) in May 2003 in Lamont, Oklahoma. An inverse aerosol/CCN closure study is undertaken, in which the predicted number concentration of particles available for activation (N_P) at the CCNC3 operating supersaturations is compared to that observed (N_O). N_P is based on Köhler Theory, with assumed and inferred aerosol composition and mixing state, and the airborne aerosol size distribution measured by the Caltech Dual Automatic Classified Aerosol Detector (DACAD). An initial comparison of N_O and N_P, assuming the ambient aerosol is pure ammonium sulfate ((NH_4)_2SO_4), results in closure ratios (N_P/N_O) ranging from 1.18 to 3.68 over the duration of the IOP, indicating that the aerosol is less hygroscopic than (NH_4)_2SO_4. N_P and N_O are found to agree when the modeled aerosol population has characteristics of an external mixture of particles, in which insoluble material is preferentially distributed among particles with small diameters (<50 nm) and purely insoluble particles are present over a range of diameters. The classification of sampled air masses by closure ratio and aerosol size distribution is discussed in depth. Inverse aerosol/CCN closure analysis can be a valuable means of inferring aerosol composition and mixing state when direct measurements are not available, especially when surface measurements of aerosol composition and mixing state are not sufficient to predict CCN concentrations at altitude, as was the case under the stratified aerosol layer conditions encountered during the IOP

Development of a regional-scale pollen emission and transport modeling framework for investigating the impact of climate change on allergic airway disease

Exposure to bioaerosol allergens such as pollen can cause exacerbations of allergenic airway disease (AAD) in sensitive populations, and thus cause serious public health problems. Assessing these health impacts by linking the airborne pollen levels, concentrations of respirable allergenic material, and human allergenic response under current and future climate conditions is a key step toward developing preventive and adaptive actions. To that end, a regional-scale pollen emission and transport modeling framework was developed that treats allergenic pollens as non-reactive tracers within the coupled Weather Research and Forecasting Community Multiscale Air Quality (WRF/CMAQ) modeling system. The <b>S</b>imulator of the <b>T</b>iming <b>a</b>nd <b>M</b>agnitude of <b>P</b>ollen <b>S</b>eason (STaMPS) model was used to generate a daily pollen pool that can then be emitted into the atmosphere by wind. The STaMPS is driven by species-specific meteorological (temperature and/or precipitation) threshold conditions and is designed to be flexible with respect to its representation of vegetation species and plant functional types (PFTs). The hourly pollen emission flux was parameterized by considering the pollen pool, friction velocity, and wind threshold values. The dry deposition velocity of each species of pollen was estimated based on pollen grain size and density. An evaluation of the pollen modeling framework was conducted for southern California (USA) for the period from March to June 2010. This period coincided with observations by the University of Southern California's Children's Health Study (CHS), which included O₃, PM_2.5, and pollen count, as well as measurements of exhaled nitric oxide in study participants. Two nesting domains with horizontal resolutions of 12 and 4 km were constructed, and six representative allergenic pollen genera were included: birch tree, walnut tree, mulberry tree, olive tree, oak tree, and brome grasses. Under the current parameterization scheme, the modeling framework tends to underestimate walnut and peak oak pollen concentrations, and tends to overestimate grass pollen concentrations. The model shows reasonable agreement with observed birch, olive, and mulberry tree pollen concentrations. Sensitivity studies suggest that the estimation of the pollen pool is a major source of uncertainty for simulated pollen concentrations. Achieving agreement between emission modeling and observed pattern of pollen releases is the key for successful pollen concentration simulations

Vertically resolved aerosol optical properties over the ARM SGP site

We will present an overview of early airborne results obtained aboard the Center for Interdisciplinary Remotely-Piloted Aircraft Studies (CIRP AS) Twin Otter aircraft during the Atmospheric Radiation Measurement (ARM) program aerosol intensive observation period in May 2003

Aerosol–cloud drop concentration closure in warm cumulus

Our understanding of the activation of aerosol particles into cloud drops during the formation of warm cumulus clouds presently has a limited observational foundation. Detailed observations of aerosol size and composition, cloud microphysics and dynamics, and atmospheric thermodynamic state were collected in a systematic study of 21 cumulus clouds by the Center for Interdisciplinary Remotely-Piloted Aircraft Studies (CIRPAS) Twin Otter aircraft during NASA's Cirrus Regional Study of Tropical Anvils and Cirrus Layers–Florida Area Cirrus Experiment (CRYSTAL-FACE). An “aerosol-cloud” closure study was carried out in which a detailed cloud activation parcel model, which predicts cloud drop concentration using observed aerosol concentration, size distribution, cloud updraft velocity, and thermodynamic state, is evaluated against observations. On average, measured droplet concentration in adiabatic cloud regions is within 15% of the predictions. This agreement is corroborated by independent measurements of aerosol activation carried out by two cloud condensation nucleus (CCN) counters on the aircraft. Variations in aerosol concentration, which ranged from 300 to 3300 cm^(−3), drives large microphysical differences (250–2300 cm^(−3)) observed among continental and maritime clouds in the South Florida region. This is the first known study in which a cloud parcel model is evaluated in a closure study using a constraining set of data collected from a single platform. Likewise, this is the first known study in which relationships among aerosol size distribution, CCN spectrum, and cloud droplet concentration are all found to be consistent with theory within experimental uncertainties much less than 50%. Vertical profiles of cloud microphysical properties (effective radius, droplet concentration, dispersion) clearly demonstrate the boundary layer aerosol's effect on cloud microphysics throughout the lowest 1 km of cloud depth. Onboard measurements of aerosol hygroscopic growth and the organic to sulfate mass ratio are related to CCN properties. These chemical data are used to quantify the range of uncertainty associated with the simplified treatment of aerosol composition assumed in the closure study

Cloud formation in the plumes of solar chimney power generation facilities: A modeling study

The solar chimney power facility has the potential to become a valuable technology for renewable energy production. Its financial viability depends on a thorough understanding of the processes affecting its performance, particularly because of the large startup costs associated with facility design and construction. This paper describes the potential impacts on plant capacity resulting from cloud formation within or downwind of the solar chimney. Several proposed modifications to the basic concept of the solar chimney power facility have the potential to cause significant additions of water vapor to the air passing through the collector. As the air continues up through and out of the chimney, this excess water can condense to form cloud. This possibility is explored using a cloud parcel model initialized to simulate the range of expected operating conditions for a proposed solar chimney facility in southwestern Australia. A range of temperatures and updraft velocities is simulated for each of four seasonal representations and three levels of water vapor enhancement. Both adiabatic environments and the effects of entrainment are considered. The results indicate that for very high levels of water vapor, enhancement cloud formation within the chimney is likely; at more moderate levels of water vapor enhancement, the likelihood of plume formation is difficult to fully assess as the results depend strongly on the choice of entrainment rate. Finally, the impacts of these outcomes on facility capacity are estimated. Copyright © 2009 by ASME

Chemical characterization of biogenic secondary organic aerosol generated from plant emissions under baseline and stressed conditions: inter- and intra-species variability for six coniferous species

The largest global source of secondary organic aerosol (SOA) in the atmosphere is derived from the oxidation of biogenic emissions. Plant stressors associated with a changing environment can alter both the quantity and composition of the compounds that are emitted. Alterations to the biogenic volatile organic compound (BVOC) profile could impact the characteristics of the SOA formed from those emissions. This study investigated the impacts of one global change stressor, increased herbivory, on the composition of SOA derived from real plant emissions. Herbivory was simulated via application of methyl jasmonate (MeJA), a proxy compound. Experiments were repeated under pre- and post-treatment conditions for six different coniferous plant types. Volatile organic compounds (VOCs) emitted from the plants were oxidized to form SOA via dark ozone-initiated chemistry. The SOA chemical composition was measured using a Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-AMS). The aerosol mass spectra of pre-treatment biogenic SOA from all plant types tended to be similar with correlations usually greater than or equal to 0.90. The presence of a stressor produced characteristic differences in the SOA mass spectra. Specifically, the following <i>m/z</i> were identified as a possible biogenic stress AMS marker with the corresponding HR ion(s) shown in parentheses: <i>m/z</i> 31 (CH₃O⁺), <i>m/z</i> 58 (C₂H₂O₂⁺, C₃H₆O⁺), <i>m/z</i> 29 (C₂H₅⁺), <i>m/z</i> 57 (C₃H₅O⁺), <i>m/z</i> 59 (C₂H₃O₂⁺, C₃H₇O⁺), <i>m/z</i> 71 (C₃H₃O₂⁺, C₄H₇O⁺), and <i>m/z</i> 83 (C₅H₇O⁺). The first aerosol mass spectrum of SOA generated from the oxidation of the plant stress hormone, MeJA, is also presented. Elemental analysis results demonstrated an O : C range of baseline biogenic SOA between 0.3 and 0.47. The O : C of standard MeJA SOA was 0.52. Results presented here could be used to help identify a biogenic plant stress marker in ambient data sets collected in forest environments