During Biogenic Aerosols—Effects on Clouds and Climate (BAECC), the U.S. Department of Energy’s Atmospheric Radiation Measurement (ARM) Program deployed the Second ARM Mobile Facility (AMF2) to Hyytiälä, Finland, for an 8-month intensive measurement campaign from February to September 2014. The primary research goal is to understand the role of biogenic aerosols in cloud formation. Hyytiälä is host to the Station for Measuring Ecosystem–Atmosphere Relations II (SMEAR II), one of the world’s most comprehensive surface in situ observation sites in a boreal forest environment. The station has been measuring atmospheric aerosols, biogenic emissions, and an extensive suite of parameters relevant to atmosphere–biosphere interactions continuously since 1996. Combining vertical profiles from AMF2 with surface-based in situ SMEAR II observations allows the processes at the surface to be directly related to processes occurring throughout the entire tropospheric column. Together with the inclusion of extensive surface precipitation measurements and intensive observation periods involving aircraft flights and novel radiosonde launches, the complementary observations provide a unique opportunity for investigating aerosol–cloud interactions and cloud-to-precipitation processes in a boreal environment. The BAECC dataset provides opportunities for evaluating and improving models of aerosol sources and transport, cloud microphysical processes, and boundary layer structures. In addition, numerical models are being used to bridge the gap between surface-based and tropospheric observations.
During the Carbonaceous Aerosols and Radiative Effects Study (CARES), activation fraction of size-resolved aerosol particles and aerosol chemical composition were characterized at the T1 site (~60 km downwind of Sacramento, California) from 10 June to 28 June 2010. The hygroscopicity of CCN-active particles (κCCN) with diameter from 100 to 171 nm, derived from the size-resolved activated fraction, varied from 0.10 to 0.21, with an average of 0.15, which was substantially lower than that proposed for continental sites in earlier studies. The low κCCN value was due to the high organic volume fraction, averaged over 80% at the T1 site. The derived κCCN exhibited little diurnal variation, consistent with the relatively constant organic volume fraction observed. At any time, over 90% of the size selected particles with diameter between 100 and 171 nm were CCN active, suggesting most particles within this size range were aged background particles. Due to the large organic volume fraction, organic hygroscopicity (κorg) strongly impacted particle hygroscopicity and therefore calculated CCN concentration. For vast majority of the cases, an increase of κorg from 0.03 to 0.18, which are within the typical range, doubled the calculated CCN concentration. Organic hygroscopicity was derived from κCCN and aerosol chemical composition, and its variations with the fraction of total organic mass spectral signal at m/z 44 (f44) and O : C were compared to results from previous studies. Overall, the relationships between κorg and f44 are quite consistent for organic aerosol (OA) observed during field studies and those formed in smog chamber. Compared to the relationship between κorg and f44, the relationship between κorg and O : C exhibits more significant differences among different studies, suggesting κorg may be better parameterized using f44. A least squares fit yielded κorg = 2.04 (± 0.07) × f44 − 0.11 (± 0.01) with the Pearson R2 value of 0.71. One possible explanation for the stronger correlation between κorg and f44 is that the m/z 44 signal (mostly contributed by the CO2+ ion) is more closely related to organic acids, which may dominate the overall κorg due to their relatively high water solubility and hygroscopicity
<p><strong>Abstract.</strong> Fundamental to quantifying the influence of human activities on climate and air quality is an understanding of how anthropogenic emissions affect the concentrations and composition of airborne particulate matter (PM). The central Amazon basin, especially around the city of Manaus, Brazil, has experienced rapid changes in the past decades due to ongoing urbanization. Herein, changes in the concentration and composition of submicron PM due to pollution downwind of the Manaus metropolitan region are reported as part of the GoAmazon2014/5 experiment. A high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and a suite of other gas- and particle-phase instruments were deployed at the <q>T3</q> research site, 70&#8201;km downwind of Manaus, during the wet season. At this site, organic components represented on average 79&#8201;&#177;&#8201;7&#8201;% of the non-refractory PM1 mass concentration, which was in the same range as several upwind sites. The organic PM<sub>1</sub> was, however, considerably more oxidized at T3 compared to upwind measurements. Positive-matrix factorization (PMF) was applied to the time series of organic mass spectra collected at the T3 site, yielding three factors representing secondary processes (73&#8201;&#177;&#8201;15&#8201;% of total organic mass concentration) and three factors representing primary anthropogenic emissions (27&#8201;&#177;&#8201;15&#8201;%). Fuzzy c-means clustering (FCM) was applied to the afternoon time series of concentrations of NO<sub>y</sub>, ozone, total particle number, black carbon, and sulfate. Four clusters were identified and characterized by distinct airmass origins and particle compositions. Two clusters, Bkgd-1 and Bkgd-2, were associated with background conditions. Bkgd-1 appeared to represent near-field atmospheric PM production and oxidation of a day or less. Bkgd-2 appeared to represent material transported and oxidized for two or more days, often with out-of-basin contributions. Two other clusters, Pol-1 and Pol-2, represented the Manaus influence, one apparently associated with the northern region of Manaus and the other with the southern region of the city. A composite of the PMF and FCM analyses provided insights into the anthropogenic effects on PM concentration and composition. The increase in mass concentration of submicron PM ranged from 25&#8201;% to 200&#8201;% under polluted compared to background conditions, including contributions from both primary and secondary PM. Furthermore, a comparison of PMF factor loadings for different clusters suggested a shift in the pathways of PM production under polluted conditions. Nitrogen oxides may have played a critical role in these shifts. Increased concentrations of nitrogen oxides can shift pathways of PM production from HO<sub>2</sub>-dominant to NO-dominant as well as increase the concentrations of oxidants in the atmosphere. Consequently, the oxidation of biogenic and anthropogenic precursor gases as well as the oxidative processing of pre-existing atmospheric PM can be accelerated. The combined set of results demonstrates the susceptibility of atmospheric chemistry, air quality, and associated climate forcing to anthropogenic perturbations over tropical forests.</p>
With their extensive coverage, marine low clouds greatly impact global climate. Presently, marine low clouds are poorly represented in global climate models, and the response of marine low clouds to changes in atmospheric greenhouse gases and aerosols remains the major source of uncertainty in climate simulations. The Eastern North Atlantic (ENA) is a region of persistent but diverse subtropical marine boundary layer clouds, whose albedo and precipitation are highly susceptible to perturbations in aerosol properties. In addition, the ENA is periodically impacted by continental aerosols, making it an excellent location to study the cloud condensation nuclei (CCN) budget in a remote marine region periodically perturbed by anthropogenic emissions, and to investigate the impacts of long-range transport of aerosols on remote marine clouds. The Aerosol and Cloud Experiments in Eastern North Atlantic (ACE-ENA) campaign was motivated by the need of comprehensive in-situ measurements for improving the understanding of marine boundary layer CCN budget, cloud and drizzle microphysics, and the impact of aerosol on marine low cloud and precipitation. The airborne deployments took place from June 21 to July 20, 2017 and January 15 to February 18, 2018 in the Azores. The flights were designed to maximize the synergy between in-situ airborne measurements and ongoing long-term observations at a ground site. Here we present measurements, observation strategy, meteorological conditions during the campaign, and preliminary findings. Finally, we discuss future analyses and modeling studies that improve the understanding and representation of marine boundary layer aerosols, clouds, precipitation, and the interactions among them.
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