Search

Remote sensing has been a key resource for developing extensive and detailed datasets for studying and constraining aerosol-cloud-climate interactions. However, aerosol-cloud collocation challenges, algorithm limitations, as well as difficulties in unraveling dynamic from aerosol-related effects on cloud microphysics, have long challenged precise retrievals of cloud droplet number concentrations. By combining a series of remote sensing techniques and in situ measurements at ground level, we developed a semiautomated approach that can address several retrieval issues for a robust estimation of cloud droplet number for non-precipitating Planetary Boundary Layer (PBL) clouds. The approach is based on satellite retrievals of the PBL cloud droplet number (Ndsat) using the geostationary meteorological satellite data of the Optimal Cloud Analysis (OCA) product, which is obtained by the Spinning Enhanced Visible and InfraRed Imager (SEVIRI) of the European Organization for the Exploitation of Meteorological Satellites (EUMETSAT). The parameters of the retrieval are optimized through closure with droplet number obtained from a combination of ground-based remote sensing data and in situ observations at ground level. More specifically, the remote sensing data are used to retrieve cloud-scale vertical velocity, and the in situ aerosol measurements at ground level were used constrain as input to a state-of-the-art droplet activation parameterization to predict the respective Cloud Condensation Nuclei (CCN) spectra, cloud maximum supersaturation and droplet number concentration (Nd), accounting for the effects of vertical velocity distribution and lateral entrainment. Closure studies between collocated Nd and Nd sat are then used to evaluate exising droplet spectral width parameters used for the retrieval of droplet number, and determine the optimal values for retrieval. This methodology, used to study aerosol-cloud interactions for non-precipitating clouds formed over the Athens Metropolitan Area (AMA), Greece, during the springtime period from March to May 2020, shows that droplet closure can be achieved to within ±33.4%, comparable to the level of closure obtained in many in situ studies. Given this, the ease of applying this approach with satellite data obtained from SEVIRI with high temporal (15 min) and spatial resolution (3.6 km Ã--4.6 km), opens the possibility of continuous and reliable Ndsat, giving rise to high value datasets for aerosol-cloud-climate interaction studies. [ABSTRACT FROM AUTHOR]

The purpose of this study is to understand the drivers of cloud droplet formation in orographic clouds. We used a combination of modeling, in-situ and remote sensing measurements at the high-altitude Helmos Hellenic Atmospheric Aerosol and Climate Change station ((HAC)2), which is located at the top of Mt. Helmos (1314 metres above sea level), Greece during the Cloud-AerosoL InteractionS in the Helmos background TropOsphere (CALISTHO) campaign in Fall 2021 (https://calishto.panacea-ri.gr/) to examine the origins of the aerosols (i.e., local aerosol from the Planetary Boundary Layer (PBL), or long-range transported aerosol from the Free Tropospheric Layer (FTL) contributing to the Cloud Condensation Nuclei (CCN), their characteristics (hygroscopicity, size distribution and mixing state), as well as the vertical velocities distributions and resulting supersaturations. We found that the characteristics of the PBL aerosol were considerably different from FTL aerosol and use the aerosol particle number and equivalent mass concentration of the black carbon (eBC) in order to determine when the (HAC)2 was within the FTL or PBL based on timeseries of the height of the PBL. During the (HAC)2 cloud events we sample a mixture of interstitial aerosol and droplet residues, which we characterize using a new approach that utilizes the in-situ droplet measurements to determine time periods where the aerosol sample is purely interstitial. From the dataset we determine the properties (size distribution and hygroscopicity) of the pre-cloud, activated and interstitial aerosol. The hygroscopicity of activated aerosol is found to be higher than that of the interstitial or pre-cloud aerosol. A series of closure studies with the droplet parameterization shows that cloud droplet concentration (N d) and supersaturation can be predicted to within 25 % of observations when the aerosol size distributions correspond to pre-cloud conditions. Analysis of the characteristic supersaturation of each aerosol population indicates that droplet formation in clouds is aerosol-limited when formed in FTL airmasses – hence droplet formation is driven by aerosol variations, while clouds formed in the PBL tend to be velocity limited and droplet variations are driven by fluctuations in vertical velocity. Given that the cloud dynamics do not vary significantly between airmasses, the variation in aerosol concentration and type is mostly responsible for these shifts in cloud microphysical state and sensitivity to aerosol. With these insights, remote sensing of cloud droplets in such clouds can be used to infer either CCN spectra (when in the FTL) or vertical velocity (when in the PBL). In conclusion, we show that a coordinated measurement of aerosol and cloud properties, together with the novel analysis approaches presented here allow for the determination of the drivers of droplet formation in orographic clouds and their sensitivity to aerosol and vertical velocity variations. [ABSTRACT FROM AUTHOR]

This work evaluates the aerosol oxidative potential (OP) and its changes from modified air pollution emissions during the COVID-19 lockdown period in 2020, with the intent of elucidating the contribution of aerosol sources and related components to aerosol OP. For this, daily particulate matter (PM) samples at an urban background site were collected and analyzed with a chemical (acellular) assay based on Dithiothreitol (DTT) during the COVID-19 restriction period in Athens (Greece). The obtained time-series of OP, PM2.5, organic matter (OM) and SO42− of the pre-, post- and lockdown periods were also compared to the data of the same time periods during the years 2017–2019. Even though all traffic-related emissions have been significantly reduced during the lockdown period (by 30%), there is no reduction in water-soluble OP, organics and sulfate concentrations of aerosol during 2020. The results reveal that the decrease in traffic was not sufficient to drive any measurable change on OP, suggesting that other sources—such as biomass burning and secondary aerosol from long-range transport, which remained unchanged during the COVID lockdown—are the main contributors to OP in Athens, Greece. [ABSTRACT FROM AUTHOR]

Biomass burning is a major source of atmospheric brown carbon (BrC), and through its absorption of UV/VIS radiation, it can play an important role in the planetary radiative balance and atmospheric photochemistry. The considerable uncertainty of BrC impacts is associated with its poorly constrained sources, transformations, and atmospheric lifetime. Here we report laboratory experiments that examined changes in the optical properties of the water-soluble (WS) BrC fraction of laboratory-generated biomass burning particles from hardwood pyrolysis. Effects of direct UVB photolysis and OH oxidation in the aqueous phase on molecular-weight-separated BrC were studied. Results indicated that the majority of low-molecular-weight (MW) BrC (<400 Da) was rapidly photobleached by both direct photolysis and OH oxidation on an atmospheric timescale of approximately 1 h. High MW BrC (≥400 Da) underwent initial photoenhancement up to ∼15 h, followed by slow photobleaching over ∼10 h. The laboratory experiments were supported by observations from ambient BrC samples that were collected during the fire seasons in Greece. These samples, containing freshly emitted to aged biomass burning aerosol, were analyzed for both water- and methanol-soluble BrC. Consistent with the laboratory experiments, high-MW BrC dominated the total light absorption at 365 nm for both methanol and water-soluble fractions of ambient samples with atmospheric transport times of 1 to 68 h. These ambient observations indicate that overall, biomass burning BrC across all molecular weights has an atmospheric lifetime of 15 to 28 h, consistent with estimates from previous field studies – although the BrC associated with the high-MW fraction remains relatively stable and is responsible for light absorption properties of BrC throughout most of its atmospheric lifetime. For ambient samples of aged (>10 h) biomass burning emissions, poor linear correlations were found between light absorptivity and levoglucosan, consistent with other studies suggesting a short atmospheric lifetime for levoglucosan. However, a much stronger correlation between light absorptivity and total hydrous sugars was observed, suggesting that they may serve as more robust tracers for aged biomass burning emissions. Overall, the results from this study suggest that robust model estimates of BrC radiative impacts require consideration of the atmospheric aging of BrC and the stability of high-MW BrC. [ABSTRACT FROM AUTHOR]

While the effects of aging on the mass, chemical composition, and hygroscopicity of organic aerosols are becoming better understood, the corresponding impacts on their direct radiative forcing and adverse health effects remain unclear. Through a combination of laboratory experiments and field observations, the objective of this work is to investigate the effects of atmospheric processing on the light absorptivity and oxidative potential (ability to generate Reactive Oxygen Species, ROS) of biomass burning organic aerosols (BBOA). In the laboratory, changes in the light absorptivity of molecular weight separated BBOA due to photochemical aging were systemically examined. Results suggest that the extent to which photo-bleaching and photo-enhancement occurs is dependent on the molecular weight fraction of BBOA. The effects of atmospheric aging on ambient BBOA, using filter samples collected in Crete, Greece, were also investigated. Focusing on samples that transition from freshly emitted to highly aged BBOA, results suggest that light absorbing large molecular weight compounds can be long-lived components in BBOA, thus more likely to have a larger impact on the aerosol direct radiative forcing. To better understand the health impacts of BBOA, results elucidating the role of atmospheric aging on their oxidative potential will also be presented. [ABSTRACT FROM AUTHOR]

Many studies have drawn attention to the associations of oxygenated polycyclic aromatic hydrocarbons (OPAHs) with harmful health effects, advocating for their systematic monitoring alongside simple PAHs to better understand the aerosol carcinogenic potential in urban areas. To address this need, this study conducted an extensive PM 2.5 sampling campaign in Athens, Greece, at the Thissio Supersite of the National Observatory of Athens, from December 2018 to July 2021, aiming to characterize the levels and variability of polycyclic aromatic compounds (PACs), perform source apportionment, and assess health risk. Cumulative OPAH concentrations (Σ-OPAHs) were in the same range as Σ-PAHs (annual average 4.2 and 5.6 ng m -3 , respectively). They exhibited a common seasonal profile with enhanced levels during the heating seasons, primarily attributed to residential wood burning (RWB). The episodic impact of biomass burning was also observed during a peri-urban wildfire event in May 2021, when PAH and OPAH concentrations increased by a factor of three compared to the monthly average. The study period also included the winter 2020-2021 COVID-19 lockdown, during which PAH and OPAH levels decreased by >50 % compared to past winters. Positive matrix factorization (PMF) source apportionment, based on a carbonaceous aerosol speciation dataset, identified PAC sources related to RWB, local traffic (gasoline vehicles) and urban traffic (including diesel emissions), as well as an impact of regional organic aerosol. Despite its seasonal character, RWB accounted for nearly half of Σ-PAH and over two-thirds of Σ-OPAH concentrations. Using the estimated source profiles and contributions, the source-specific carcinogenic potency of the studied PACs was calculated, revealing that almost 50 % was related to RWB. These findings underscore the urgent need to regulate domestic biomass burning at a European level, which can provide concrete benefits for improving urban air quality, towards the new stricter EU standards, and reducing long-term health effects., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024. Published by Elsevier B.V.)

Oxidative potential (OP), which is the ability of certain components in atmospheric particles to generate reactive oxidative species (ROS) and deplete antioxidants in vivo, is a prevailing toxicological mechanism underlying the adverse health effects associated with exposure to ambient aerosols. While previous studies have identified the high OP of fresh biomass burning organic aerosols (BBOA), it remains unclear how it evolves throughout atmospheric transport. Using the dithiothreitol (DTT) assay as a measure of OP, a combination of field observations and laboratory experiments is used to determine how atmospheric aging transforms the intrinsic OP (OP mass ) of BBOA. For ambient BBOA collected during the fire seasons in Greece, OP DTT ) of BBOA. For ambient BBOA collected during the fire seasons in Greece, OP mass DTT was observed to increase by a factor of 2.1 ± 0.9 for samples of atmospheric ages up to 68 h. Laboratory experiments indicate that aqueous photochemical aging (aging by UVB and UVA photolysis; as well as OH oxidation), as well as aging by ozone and atmospheric dilution can transform the OP mass DTT of the water-soluble fraction of wood smoke within 2 days of atmospheric transport. The results from this work suggest that the air quality impacts of biomass burning emissions can extend beyond regions near fire sites and should be accounted for.