Nucleation, Transformation, and Impacts of Atmospheric Aerosols

Atmospheric aerosols are a key contributor to pollution, adversely affect human health, and can alter global climate. Several questions concerning atmospheric aerosols persist, including: ‘Which atmospheric species are integral for aerosol formation in the atmosphere?’, ‘What happens to aerosols after emission into or formation in the atmosphere?’, ‘Does maternal exposure to aerosols during pregnancy fundamentally alter her offspring?’, and ‘Can we utilize gas phase chemistry models to further our understanding of atmospheric aerosols?’. A series of chamber, observational, and computational studies have been conducted to investigate these scientific questions. Globally, new particle formation (NPF) events account for more than 50% of the aerosols in the troposphere, but the chemical species and mechanisms responsible for NPF have yet to be fully understood. To explicate the role of organic compounds in NPF, laboratory experiments have been conducted to investigate aerosol nucleation and growth from the photochemical oxidation of biogenic and anthropogenic volatile organic compounds (VOCs). Here we show that the NPF is dependent on the VOC species and that the global pattern of NPF is likely governed by the available VOCs. A suite of instruments was deployed in Beijing to measure a comprehensive set of aerosol properties in order to elucidate the aerosol formation mechanisms and the evolution of aerosol properties. NPF consistently occurred on clean, windy days, and the high aerosol mass observed during haze events is attributable to the continuous growth from the nucleation-mode particles over multiple days to produce a high concentration of larger particles. Our results reveal that the severe haze in Beijing is likely due to the concentrated aerosol precursor gases and the large-scale meteorological conditions. Model simulations indicate that the persistent high concentrations of NO2 in Beijing and the frequent periods of high aerosol loading leads to elevated HONO levels and sustained oxidizing capacity. To determine the mechanism through which aerosols influence human health, a series of animal exposure studies have been conducted to investigate the transgenerational effects. In each experiment, Sprague-Dawley rats were continuously exposed between days 0 and 18 of gestation to controlled conditions to represent either clean (~5 µg m^-3) or polluted (~150 µg m^-3) environments. The gestation length, litter size, birth weight, and sex ratio were assessed throughout the animal exposure studies. The preliminary results indicate the development of several organs and the birth weight may be influenced by prenatal exposure to pollutants and the degree of response may also be sex dependent

Markedly enhanced absorption and direct radiative forcing of black carbon under polluted urban environments

Black carbon (BC) exerts profound impacts on air quality and climate because of its high absorption cross-section over a broad range of electromagnetic spectra, but the current results on absorption enhancement of BC particles during atmospheric aging remain conflicting. Here, we quantified the aging and variation in the optical properties of BC particles under ambient conditions in Beijing, China, and Houston, United States, using a novel environmental chamber approach. BC aging exhibits two distinct stages, i.e., initial transformation from a fractal to spherical morphology with little absorption variation and subsequent growth of fully compact particles with a large absorption enhancement. The timescales to achieve complete morphology modification and an absorption amplification factor of 2.4 for BC particles are estimated to be 2.3 h and 4.6 h, respectively, in Beijing, compared with 9 h and 18 h, respectively, in Houston. Our findings indicate that BC under polluted urban environments could play an essential role in pollution development and contribute importantly to large positive radiative forcing. The variation in direct radiative forcing is dependent on the rate and timescale of BC aging, with a clear distinction between urban cities in developed and developing countries, i.e., a higher climatic impact in more polluted environments. We suggest that mediation in BC emissions achieves a cobenefit in simultaneously controlling air pollution and protecting climate, especially for developing countries

Assessing the effects of anthropogenic aerosols on Pacific storm track using a multiscale global climate model

Atmospheric aerosols affect weather and global general circulation by modifying cloud and precipitation processes, but the magnitude of cloud adjustment by aerosols remains poorly quantified and represents the largest uncertainty in estimated forcing of climate change. Here we assess the effects of anthropogenic aerosols on the Pacific storm track, using a multiscale global aerosol-climate model (GCM). Simulations of two aerosol scenarios corresponding to the present day and preindustrial conditions reveal long-range transport of anthropogenic aerosols across the north Pacific and large resulting changes in the aerosol optical depth, cloud droplet number concentration, and cloud and ice water paths. Shortwave and long-wave cloud radiative forcing at the top of atmosphere are changed by -2.5 and +1.3 W m(-2), respectively, by emission changes from preindustrial to present day, and an increased cloud top height indicates invigorated midlatitude cyclones. The overall increased precipitation and poleward heat transport reflect intensification of the Pacific storm track by anthropogenic aerosols. Hence, this work provides, for the first time to the authors' knowledge, a global perspective of the effects of Asian pollution outflows from GCMs. Furthermore, our results suggest that the multiscale modeling framework is essential in producing the aerosol invigoration effect of deep convective clouds on a global scale.http://gateway.webofknowledge.com/gateway/Gateway.cgi?GWVersion=2&SrcApp=PARTNER_APP&SrcAuth=LinksAMR&KeyUT=WOS:000335798000044&DestLinkType=FullRecord&DestApp=ALL_WOS&UsrCustomerID=8e1609b174ce4e31116a60747a720701Multidisciplinary SciencesSCI(E)[email protected]; [email protected]

Persistent sulfate formation from London Fog to Chinese haze

Sulfate aerosols exert profound impacts on human and ecosystem health, weather, and climate, but their formation mechanism remains uncertain. Atmospheric models consistently underpredict sulfate levels under diverse environmental conditions. From atmospheric measurements in two Chinese megacities and complementary laboratory experiments, we show that the aqueous oxidation of SO2 by NO2 is key to efficient sulfate formation but is only feasible under two atmospheric conditions: on fine aerosols with high relative humidity and NH3 neutralization or under cloud conditions. Under polluted environments, this SO2 oxidation process leads to large sulfate production rates and promotes formation of nitrate and organic matter on aqueous particles, exacerbating severe haze development. Effective haze mitigation is achievable by intervening in the sulfate formation process with enforced NH3 and NO2 control measures. In addition to explaining the polluted episodes currently occurring in China and during the 1952 London Fog, this sulfate production mechanism is widespread, and our results suggest a way to tackle this growing problem in China and much of the developing world

Atmospheric Measurements of Submicron Aerosols at the California-Mexico Border and in Houston, Texas

Using an innovative arrangement of instruments to obtain a comprehensive set of properties, we present a description of the submicron aerosol properties for two distinct regions. During the 2009 SHARP/SOOT campaign in Houston, TX, the average effective density was 1.54 ± 0.07 g cm^-3, consistent with a population comprised largely of sulfates and organics Even in low concentrations (0.31 ± 0.22 µg m^-3), black carbon concentration has a significant impact on the overall density and optical properties. Under prevailing northerly winds, the average black carbon concentration increases from 0.26 ± 0.18 µg m^-3 to 0.60 ± 0.21 µg m^-3. Throughout the campaign, aerosols are often internally mixed, with one peak in the effective density distribution located at 1.55 ± 0.07 g cm^-3. In addition, we conclude that in this region the meteorology has a discernible impact on the concentration and properties of aerosols. After a frontal passage, there is a significant shift in the size distribution as the concentration of <100 nm particles increase and the average effective density decreases to 1.43 ± 0.08 g cm^-3. In Tijuana, Mexico, the submicron aerosols are heavily influenced by vehicle emissions. We observe an average single scattering albedo of 0.75. This average SSA is lower than observed in many US urban environments, and indicates a high concentration of black carbon. The average black carbon concentration is 2.71 ± 2.65 g cm^-3. The aerosol size distributions reveal a high concentration of small particles (< 100 nm) during the day, which are frequently associated with vehicle emissions. Overall, 46 and 81 nm particles are hydrophobic, have an average effective near 1.30 g cm^-3, a higher volatile growth factors than the larger particles, and exhibit a distinct diurnal cycle, which, on average, ranges between 0.80 during the afternoon and 1.70 g cm^-3 overnight. 46 and 81 nm distributions indicate a uniform aerosol composition. 151 and 240 nm aerosols are less cyclical, and the hygroscopicity, volatility, and effect density distributions all exhibit a bimodal distribution, which indicates an external mixture of aerosols. Black carbon and vehicle and industrial organic emissions appear to be the main components of the external mixture

Benzene Exposure and Cancer Risk from Commercial Gasoline Station Fueling Events Using a Novel Self-Sampling Protocol

Tens of millions of individuals go to gasoline stations on a daily basis in the United States. One of the constituents of gasoline is benzene, a Group 1 carcinogen that has been strongly linked to both occupational and non-occupational leukemias. While benzene content in gasoline is federally regulated, there is approximately a thirty-year data gap in United States research on benzene exposures from pumping gasoline. Using a novel self-sampling protocol with whole air canisters, we conducted a gasoline pumping exposure assessment for benzene, toluene, ethylbenzene, and xylene (BTEX) on Baltimore, MD consumers. Geometric mean exposures (geometric standard deviations) were 3.2 (2.7) ppb,9.5 (3.5) ppb, 2.0 (2.8) ppb, and 7.3 (3.0) ppb, respectively, on 32 samples. Using the benzene exposures, we conducted consumer and occupational probabilistic risk assessments and contextualized the risk with ambient benzene exposure risk. We found that the consumer scenarios did not approach the 1:1,000,000 excess risk management threshold and that the occupational scenario did not exceed the 1:10,000 excess risk management threshold. Further, in all Monte Carlo trials, the ambient risk from benzene exposure exceeded that of pumping risk for consumers, but that in approximately 30% of occupational trials, the pumping risk exceeded the ambient risk

Laboratory Chamber Evaluation of Flow Air Quality Sensor PM2.5 and PM10 Measurements

The emergence of low-cost air quality sensors as viable tools for the monitoring of air quality at population and individual levels necessitates the evaluation of these instruments. The Flow air quality tracker, a product of Plume Labs, is one such sensor. To evaluate these sensors, we assessed 34 of them in a controlled laboratory setting by exposing them to PM10 and PM2.5 and compared the response with Plantower A003 measurements. The overall coefficient of determination (R2) of measured PM2.5 was 0.76 and of PM10 it was 0.73, but the Flows&rsquo; accuracy improved after each introduction of incense. Overall, these findings suggest that the Flow can be a useful air quality monitoring tool in air pollution areas with higher concentrations, when incorporated into other monitoring frameworks and when used in aggregate. The broader environmental implications of this work are that it is possible for individuals and groups to monitor their individual exposure to particulate matter pollution

Measurements of Submicron Aerosols at the California-Mexico Border during the Cal-Mex 2010 Field Campaign

We present measurements of submicron aerosols in Tijuana, Mexico during the Cal-Mex 2010 field campaign. A suite of aerosol instrumentations were deployed, including a hygroscopic-volatility tandem differential mobility analyzer (HV-TDMA), aerosol particle mass analyzer (APM), condensation particle counter (CPC), cavity ring-down spectrometer (CRDS), and nephelometer to measure the aerosol size distributions, effective density, hygroscopic growth factors (HGF), volatility growth factors (VGF), and optical properties. The average mass concentration of PM0.6 is 10.39 +/- 7.61 1.mu g m(-3), and the derived average black carbon (BC) mass concentration is 2.87 +/- 2.65 mu g m(-3). There is little new particle formation or particle growth during the day, and the mass loading is dominated by organic aerosols and BC, which on average are 37% and 27% of PM1.0, respectively. For four particle sizes of 46, 81,151, and 240 nm, the measured particle effective density, HGFs, and VGFs exhibit distinct diurnal trends and size-dependence. For smaller particles (46 and 81 mm), the effective density distribution is unimodal during the day and night, signifying an internally mixed aerosol composition. In contrast, larger particles (151 and 240 nm) exhibit a bi-modal effective density distribution during the daytime, indicating an external mixture of fresh BC and organic aerosols, but a unimodal distribution during the night, corresponding to an internal mixture of BC and organic aerosols. The smaller particles show a noticeable diurnal trend in the effective density distribution, with the highest effective density (1.70 g cm(-3)) occurring shortly after midnight and the lowest value (0.90 g cm(-3)) occurring during the afternoon, corresponding most likely to primary organic aerosols and BC, respectively. Both HGFs and VGFs measured are strongly size-dependent. HGFs increase with increasing particle size, indicating that the largest particles are more hygroscopic. VGFs decrease with increasing particle size, indicating that larger particles are more volatile. The hygroscopicity distributions of smaller particles (46 and 81 nm) are unimodal, with a HGF value close to unity. Large particles typically exhibit a bi-modal distribution, with a non-hygroscopic mode and a hygroscopic mode. For all particle sizes, the VGF distributions are bimodal, with a primary non-volatile mode and a secondary volatile mode. The average extinction, scattering, and absorption coefficients are 86.04, 63.07, and 22.97 Mm(-1), respectively, and the average SSA is 0.75. Our results reveal that gasoline and diesel vehicles produce a significant amount of black carbon particles in this US Mexico border region, which impacts the regional environment and climate. Published by Elsevier Ltd