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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.
Exploring the vertical profile of atmospheric organic aerosol: comparing 17 aircraft field campaigns with a global model

The global organic aerosol (OA) budget is highly uncertain and past studies suggest that models substantially underestimate observed concentrations. Few of these studies have examined the vertical distribution of OA. Furthermore, many model-measurement comparisons have been performed with different models for single field campaigns. We synthesize organic aerosol measurements from 17 aircraft campaigns from 2001–2009 and use these observations to consistently evaluate a GEOS-Chem model simulation. Remote, polluted and fire-influenced conditions are all represented in this extensive dataset. Mean observed OA concentrations range from 0.2–8.2 μg sm−3 and make up 15 to 70% of non-refractory aerosol. The standard GEOS-Chem simulation reproduces the observed vertical profile, although observations are underestimated in 13 of the 17 field campaigns (the median observed to simulated ratio ranges from 0.4 to 4.2), with the largest model bias in anthropogenic regions. However, the model is best able to capture the observed variability in these anthropogenically-influenced regions (R2=0.18−0.57), but has little skill in remote or fire-influenced regions. The model bias increases as a function of relative humidity for 11 of the campaigns, possibly indicative of missing aqueous phase SOA production. However, model simulations of aqueous phase SOA suggest a pronounced signature in the mid-troposphere (2–6 km) which is not supported in the observations examined here. Spracklen et al. (2011) suggest adding ~100 Tg yr−1 source of anthropogenically-controlled SOA to close the measurement-model gap, which we add as anthropogenic SOA. This eliminates the model underestimate near source, but leads to overestimates aloft in a few regions and in remote regions, suggesting either additional sinks of OA or higher volatility aerosol at colder temperatures. Sensitivity simulations indicate that fragmentation of organics upon either heterogeneous or gas-phase oxidation could be an important (missing) sink of OA in models, reducing the global SOA burden by 15% and 47% respectively. The best agreement with observations is obtained when the simulated anthropogenically-controlled SOA is increased to ~100 Tg yr−1 accompanied by either a gas-phase fragmentation process or a reduction in the temperature dependence of the organic aerosol partitioning (by decreasing the enthalpy of vaporization from 42 kJ mol−1 to 25 kJ mol−1). These results illustrate that models may require both additional sources and additional sinks to capture the observed concentrations of organic aerosol.
Evaluation on the role of sulfuric acid in the mechanisms of new particle formation for Beijing case

New particle formation (NPF) is considered as an important mechanism for gas-to-particle transformation, and gaseous sulfuric acid is believed as a crucial precursor. Up to now few field-based studies on nucleation mechanisms and the role of sulfuric acid were conducted in China. In this study, simultaneously measurements of particle number size distributions and gaseous sulfuric acid concentrations were performed from July to September in 2008. Totally, 22 new particle formation events were observed during the entire 85 campaign days. The results show that in the case of both higher source and sink values, the result of the competition between source and sink is more likely the key limiting factor to determine the observation of NPF events in Beijing. The concentrations of gaseous sulfuric acid show good correlations with freshly nucleated particles (N3-6 and formation rates (J3 and J1.5. The power-law relationship between H2SO4 concentration and N3-6 or J is adopted to explore the nucleation mechanism. The exponents are showed a great range (from 1 to 7). More than half of the NPF events exhibit an exponent larger than 2.5. For these cases, the thermodynamic process works better than the activation or kinetic nucleation theories to explain the nucleation events in urban atmosphere of Beijing.
Flight-based chemical characterization of biomass burning aerosols within two prescribed burn smoke plumes

Biomass burning represents a major global source of aerosols impacting direct radiative forcing and cloud properties. Thus, the goal of a number of current studies involves developing a better understanding of how the chemical composition and mixing state of biomass burning aerosols evolve during atmospheric aging processes. During the Ice in Clouds Experiment-Layer Clouds (ICE-L) in the fall of 2007, smoke plumes from two small Wyoming Bureau of Land Management prescribed burns were measured by on-line aerosol instrumentation aboard a C-130 aircraft, providing a detailed chemical characterization of the particles. After ~2–4 min of aging, submicron smoke particles, produced primarily from sagebrush combustion, consisted predominantly of organics by mass, but were comprised primarily of internal mixtures of organic carbon, elemental carbon, potassium chloride, and potassium sulfate. Significantly, the fresh biomass burning particles contained minor mass fractions of nitrate and sulfate, suggesting that hygroscopic material is incorporated very near or at the point of emission. The mass fractions of ammonium, sulfate, and nitrate increased with aging up to ~81–88 min and resulted in acidic particles. Decreasing black carbon mass concentrations occurred due to dilution of the plume. Increases in the fraction of oxygenated organic carbon and the presence of dicarboxylic acids, in particular, were observed with aging. Cloud condensation nuclei measurements suggested all particles >100 nm were active at 0.5% water supersaturation in the smoke plumes, confirming the relatively high hygroscopicity of the freshly emitted particles. For immersion/condensation freezing, ice nuclei measurements at −32 °C suggested activation of ~0.03–0.07% of the particles with diameters greater than 500 nm.
On aerosol hygroscopicity, cloud condensation nuclei (CCN) spectra and critical supersaturation measured at two remote islands of Korea between 2006 and 2009

Aerosol size distribution, total concentration (i.e. condensation nuclei (CN) concentration, NCN), cloud condensation nuclei (CCN) concentration (NCCN), hygroscopicity at ~90% relative humidity (RH) were measured at a background monitoring site at Gosan, Jeju Island, south of the Korean Peninsula in August 2006, April to May 2007 and August to October 2008. Similar measurements took place in August 2009 at another background site (Baengnyeongdo Comprehensive Monitoring Observatory, BCMO) on the island of Baengnyeongdo, off the west coast of the Korean Peninsula. Both islands were found to be influenced by continental sources regardless of season and year. Average values for all of the measured NCCN at 0.2, 0.6 and 1.0% supersaturations (S), NCN, and geometric mean diameter (Dg) from both islands were in the range of 1043–3051 cm−3, 2076–4360 cm−3, 2713–4694 cm−3, 3890–5117 cm−3 and 81–98 nm, respectively. Although the differences in Dg and NCN were small between Gosan and BCMO, NCCN at various S was much higher at the latter, which is closer to China. Most of the aerosols were internally mixed and no notable differences in hygroscopicity were found between the days of strong pollution influence and the non-pollution days for both islands. During the 2008 and 2009 campaigns, critical supersaturation for CCN nucleation (Sc) for selected particle sizes was measured. Particles of 100 nm diameters had mean Sc of 0.19 ± 0.02% during 2008 and those of 81 and 110 nm diameters had mean Sc of 0.26 ± 0.07% and 0.17 ± 0.04%, respectively, during 2009. The values of the hygroscopicity parameter (κ), estimated from measured Sc, were mostly higher than the κ values obtained from the measured hygroscopic growth at ~90% RH. For the 2008 campaign, NCCN at 0.2, 0.6 and 1.0% S were predicted based on measured dry particle size distributions and various ways of representing particle hygroscopicity. The best closure was obtained when temporally varying and size-resolved hygroscopicity information from the HTDMA was used, for which the average relative deviations from the measured values were 28 ± 20% for 0.2% S (mostly under-prediction), 25 ± 52% for 0.6% (balanced between over- and under-prediction) and 19 ± 15% for 1.0% S (balanced). Prescribing a constant hygroscopicity parameter suggested in the literature (κ = 0.3) for all sizes and times resulted in average relative deviations of 28–41% where over-prediction was dominant. When constant hygroscopicity was assumed, the relative deviation tended to increase with decreasing NCCN, which was accompanied by an increase of the sub-100 nm fraction. These results suggest that hygroscopicity information for particles of diameters smaller than 100 nm is crucial for more accurate predictions of NCCN. For confirmation when κ = 0.17, the average κ for sub-100 nm particles in this study, was applied for sub-100 nm and κ = 0.3 for all other sizes, the CCN closure became significantly better than that with κ = 0.3 for all sizes.
Hygroscopic behavior of atmospherically relevant water-soluble carboxylic salts and their influence on the water uptake of ammonium sulfate

The hygroscopic behavior of atmospherically relevant water-soluble carboxylic salts and their effects on ammonium sulfate were investigated using a hygroscopicity tandem differential mobility analyzer (H-TDMA). No hygroscopic growth is observed for disodium oxalate, while ammonium oxalate shows slight growth (growth factor = 1.05 at 90%). The growth factors at 90% RH for sodium acetate, disodium malonate, disodium succinate, disodium tartrate, diammonium tartrate, sodium pyruvate, disodium maleate, and humic acid sodium salt are 1.79, 1.78, 1.69, 1.54, 1.29, 1.70, 1.78, and 1.19, respectively. The hygroscopic growth of mixtures of organic salts with ammonium sulfate, which are prepared as surrogates of atmospheric aerosols, was determined. A clear shift in deliquescence relative humidity to lower RH with increasing organic mass fraction was observed for these mixtures. Above 80% RH, the contribution to water uptake by the organic salts was close to that of ammonium sulfate for the majority of investigated compounds. The observed hygroscopic growth of the mixed particles at RH above the deliquescence relative humidity of ammonium sulfate agreed well with that predicted using the Zdanovskii-Stokes-Robinson (ZSR) mixing rule. Mixtures of ammonium sulfate with organic salts are more hygroscopic than mixtures with organic acids, indicating that neutralization by gas-phase ammonia and/or association with cations of dicarbonxylic acids may enhance the hygroscopicity of the atmospheric particles.
Column-integrated aerosol microphysical properties from AERONET Sun photometer over southwestern Spain

The aim of the present work is to carry out a detailed analysis of columnar microphysical properties obtained from Cimel sun-photometer measurements in the Southwest of Spain within the frame of the Aerosol Robotic Network (AERONET) – Iberian Network for aerosol measurements (RIMA). AERONET level 2 inversion products are analysed, in particular the particle size distribution together with their associated microphysical parameters for both fine and coarse modes: volume concentration, effective radius and the fine mode volume fraction. This work complements previous works based on aerosol optical depth (AOD) and the Ångström exponent (AE) for a global characterization of atmospheric aerosol in this area of southwestern Spain. The analysed dataset spans between February 2000 and October 2008. Time series and statistical analysis has been carried out for these parameters in order to assess their typical values and seasonality together with their relationships with the AOD and AE. Mean values of volume particle concentration are 0.06±0.07 μm3 μm−2 for total, 0.019±0.015 μm3 μm−2 for fine and 0.04±0.06 μm3 μm−2 for coarse mode; mean effective radii are 0.40±0.19 μm for total, 0.14±0.02 μm for fine and 1.96±0.41 μm for coarse mode. The most relevant features are the clear bimodality of the volume particle size distribution, with a slight dominance of the coarse mode in the overall climatology given the prevailing atmospheric conditions at the site (coastal marine). There is a clear prevalence of the coarse mode in summer months plus September and March, in coincidence with the occurrence of desert dust intrusions and highest AOD values. During desert dust outbreaks, the particle size distribution is practically monomodal with strong prevalence of the coarse mode which also shows a shift of the modal radius toward lower values. The size particle predominance defines the characteristic of the site and it has been analysed under two different parameters: the Ångström exponent and the fine mode volume fraction Vf/Vt. We investigated the relationship between them and also their relationship with the effective radius of the size distribution.
Climatology and trends in the forcing of the stratospheric zonal-mean flow

The momentum budget of the Transformed Eulerian-Mean (TEM) equation is calculated using the European Centre for Medium-Range Weather Forecasts (ECMWF) reanalysis (ERA-40) and the National Centers for Environmental Prediction (NCEP) Reanalysis 2 (R-2). This study outlines the considerable contribution of unresolved waves, deduced to be gravity waves, to the forcing of the zonal-mean flow. A trend analysis, from 1980 to 2001, shows that the onset and break down of the Northern Hemisphere (NH) stratospheric polar night jet has a tendency to occur later in the season in the more recent years. This temporal shift follows long-term changes in planetary wave activity that are mainly due to synoptic waves, with a lag of one month. In the Southern Hemisphere (SH), the polar vortex shows a tendency to persist further into the SH summertime. This also follows a statistically significant decrease in the intensity of the stationary EP flux divergence over the 1980–2001 period. Ozone depletion is well known for strengthening the polar vortex through the thermal wind balance. However, the results of this work show that the SH polar vortex does not experience any significant long-term changes until the month of December, even though the intensification of the ozone hole occurs mainly between September and November. This study suggests that the decrease in planetary wave activity in November provides an important feedback to the zonal wind as it delays the breakdown of the polar vortex. In addition, the absence of strong eddy feedback before November explains the lack of significant trends in the polar vortex in the SH early spring. A long-term weakening in the Brewer-Dobson (B-D) circulation in the polar region is identified in the NH winter and early spring and during the SH late spring and is likely driven by the decrease in planetary wave activity previously mentioned. During the rest of the year, there are large discrepancies in the representation of the B-D circulation and the unresolved waves between the two reanalyses, making trend analyses unreliable.
Modelled and measured effects of clouds on UV Aerosol Indices on a local, regional, and global scale

The UV Aerosol Indices (UVAI) form one of very few available tools in satellite remote sensing that provide information on aerosol absorption. The UVAI are also quite insensitive to surface type and are determined in the presence of clouds – situations where most aerosol retrieval algorithms do not work. The UVAI are most sensitive to elevated layers of absorbing aerosols, such as mineral dust and smoke, but they can also be used to study non-absorbing aerosols, such as sulphate and secondary organic aerosols. Although UVAI are determined for cloud-contaminated pixels, clouds do affect the value of UVAI in several ways: (1) they shield the underlying scene (potentially containing aerosols) from view, (2) they enhance the apparent surface albedo of an elevated aerosol layer, and (3) clouds unpolluted by aerosols also yield non-zero UVAI, here referred to as "cloudUVAI". The main purpose of this paper is to demonstrate that clouds can cause significant UVAI and that this cloudUVAI can be well modelled using simple assumptions on cloud properties. To this aim, we modelled cloudUVAI by using measured cloud optical parameters – either with low spatial resolution from SCIAMACHY, or high resolution from MERIS – as input. The modelled cloudUVAI were compared with UVAI determined from SCIAMACHY reflectances on different spatial (local, regional and global) and temporal scales (single measurement, daily means and seasonal means). The general dependencies of UVAI on cloud parameters were quite well reproduced, but several issues remain unclear: compared to the modelled cloudUVAI, measured UVAI show a bias, in particular for large cloud fractions. Also, the spread in measured UVAI is larger than in modelled cloudUVAI. In addition to the original, Lambert Equivalent Reflector (LER)-based UVAI algorithm, we have also investigated the effects of clouds on UVAI determined using the so-called Modified LER (MLER) algorithm (currently applied to TOMS and OMI data). For medium-sized clouds the MLER algorithm performs better (UVAI are closer to 0), but like for LER UVAI, MLER UVAI can become as large as −1.2 for small clouds and deviate significantly from zero for cloud fractions near 1. The effects of clouds should therefore also be taken into account when MLER UVAI data are used. Because the effects of clouds and aerosols on UVAI are not independent, a simple subtraction of modelled cloudUVAI from measured UVAI does not yield a UVAI representative of a cloud-free scene when aerosols are present. We here propose a first, simple approach for the correction of cloud effects on UVAI. The method is shown to work reasonably well for small to medium-sized clouds located above aerosols.
Interpreting elevated space-borne HCHO columns over the Mediterranean Sea using the OMI sensor

Formaldehyde (HCHO) is an oxidation product of a wide range of volatile organic compounds (VOCs) and important atmospheric constituent found in both the polluted urban atmosphere and remote background sites. In this study, remotely sensed data of HCHO vertical column densities are analyzed over the Mediterranean Sea using the Ozone Monitoring Instrument (OMI). Data analysis indicates a marked seasonal cycle with a summer maximum and winter minimum confined to the marine environment during a three year period (2005–2007) examined. A possible retrieval artifact associated with Saharan dust transport over the region is explored by changing intensity of Saharan dust sources in GEOS-Chem following the recommendation of Generoso et al. (2008). Recalculated air mass factors (AMF), based on the new values of aerosol loadings, lead to a reduction of the summertime "hot spot" in OMI retrieval of HCHO vertical columns over the Mediterranean Sea; however, even after the correction, enhanced values are still present in this region. To explain these values, marine biogenic sources of VOCs are examined. Calculations indicate that emission of phytoplankton-produced isoprene is not likely to explain the enhanced HCHO vertical columns over the Mediterranean Sea. Model simulations in conjunction with measurements studies may be required to fully explore the complex mechanism of HCHO formation over the Mediterranean and its implications for the air quality in the region.