Redox-activity and in vitro effects of regional atmospheric aerosol pollution: Seasonal differences and correlation between oxidative potential and in vitro toxicity of PM.

Particulate Matter (PM) is a complex and heterogeneous mixture of atmospheric particles recognized as a threat to human health. Oxidative Potential (OP) measurement is a promising and integrative method for estimating PM-induced health impacts since it is recognized as more closely associated with adverse health effects than ordinarily used PM mass concentrations. OP measurements could be introduced in the air quality monitoring, along with the parameters currently evaluated.

Overview of the Alaskan Layered Pollution and Chemical Analysis (ALPACA) Field Experiment.

The Alaskan Layered Pollution And Chemical Analysis (ALPACA) field experiment was a collaborative study designed to improve understanding of pollution sources and chemical processes during winter (cold climate and low-photochemical activity), to investigate indoor pollution, and to study dispersion of pollution as affected by frequent temperature inversions. A number of the research goals were motivated by questions raised by residents of Fairbanks, Alaska, where the study was held. This paper describes the measurement strategies and the conditions encountered during the January and February 2022 field experiment, and reports early examples of how the measurements addressed research goals, particularly those of interest to the residents.

Exposure to urban nanoparticles at low PM[Formula: see text] concentrations as a source of oxidative stress and inflammation.

Exposures to fine particulate matter (PM[Formula: see text]) have been associated with health impacts, but the understanding of the PM[Formula: see text] concentration-response (PM[Formula: see text]-CR) relationships, especially at low PM[Formula: see text], remains incomplete. Here, we present novel data using a methodology to mimic lung exposure to ambient air (2[Formula: see text] 60 [Formula: see text]g m[Formula: see text]), with minimized sampling artifacts for nanoparticles. A reference model (Air Liquid Interface cultures of human bronchial epithelial cells, BEAS-2B) was used for aerosol exposure.

Machine learning for prediction of daily sea surface dimethylsulfide concentration and emission flux over the North Atlantic Ocean (1998-2021).

As the most ubiquitous natural source of sulfur in the atmosphere, dimethylsulfide (DMS) promotes aerosol formation in marine environments, impacting cloud radiative forcing and precipitation, eventually influencing regional and global climate. In this study, we propose a machine learning predictive algorithm based on Gaussian process regression (GPR) to model the distribution of daily DMS concentrations in the North Atlantic waters over 24 years (1998-2021) at 0.25° × 0.

Phytoplankton Impact on Marine Cloud Microphysical Properties Over the Northeast Atlantic Ocean.

The current understanding of the impact of natural cloud condensation nuclei (CCN) variability on cloud properties in marine air is low, thus contributing to climate prediction uncertainty. By analyzing cloud remote sensing observations (2009-2015) at Mace Head (west coast of Ireland), we show the oceanic biota impact on the microphysical properties of stratiform clouds over the Northeast Atlantic Ocean. During spring to summer (seasons of enhanced oceanic biological activity), clouds typically host a higher number of smaller droplets resulting from increased aerosol number concentration in the CCN relevant-size range.

Chemical composition and radiative forcing of atmospheric aerosols over the high-altitude Western Himalayas of India.

Aerosol behavior over the Himalayas plays an important role in the regional climate of South Asia. Previous studies at high-altitude observatories have provided evidence of the impact of long-range transport of pollutants from the Indo-Gangetic Plain (IGP). However, little information exists for the valley areas in the high Himalayas where significant local anthropogenic emissions can act as additional sources of short-living climate forcers and pollutants.

Historical Changes in Seasonal Aerosol Acidity in the Po Valley (Italy) as Inferred from Fog Water and Aerosol Measurements.

Acidity profoundly affects almost every aspect that shapes the composition of ambient particles and their environmental impact. Thermodynamic analysis of gas-particle composition datasets offers robust estimates of acidity, but they are not available for long periods of time. Fog composition datasets, however, are available for many decades; we develop a thermodynamic analysis to estimate the ammonia in equilibrium with fog water and to infer the pre-fog aerosol pH starting from fog chemical composition and pH.

Aerosol Toxins Emitted by Harmful Algal Blooms Susceptible to Complex Air-Sea Interactions.

Critical research is needed regarding harmful algal blooms threatening ecosystem and human health, especially through respiratory routes. Additional complexity comes from the poorly understood factors involved in the physical production of marine aerosols coupled with complex biogeochemical processes at ocean surfaces. Here-by using a marine aerosol generation tank-five bubble-bursting experiments (with contrasting incubation times and, likely, physiological microalgal states) were run to investigate simultaneously the concentrations of the toxins, synthesized by a natural cf.

Global Importance of Hydroxymethanesulfonate in Ambient Particulate Matter: Implications for Air Quality.

Sulfur compounds are an important constituent of particulate matter, with impacts on climate and public health. While most sulfur observed in particulate matter has been assumed to be sulfate, laboratory experiments reveal that hydroxymethanesulfonate (HMS), an adduct formed by aqueous phase chemical reaction of dissolved HCHO and SO, may be easily misinterpreted in measurements as sulfate. Here we present observational and modeling evidence for a ubiquitous global presence of HMS.

Contribution of Water-Soluble Organic Matter from Multiple Marine Geographic Eco-Regions to Aerosols around Antarctica.

We present shipborne measurements of size-resolved concentrations of aerosol components across ocean waters next to the Antarctic Peninsula, South Orkney Islands, and South Georgia Island, evidencing aerosol features associated with distinct eco-regions. Nonmethanesulfonic acid Water-Soluble Organic Matter (WSOM) represented 6-8% and 11-22% of the aerosol PM mass originated in open ocean (OO) and sea ice (SI) regions, respectively. Other major components included sea salt (86-88% OO, 24-27% SI), non sea salt sulfate (3-4% OO, 35-40% SI), and MSA (1-2% OO, 11-12% SI).

Extensive Soot Compaction by Cloud Processing from Laboratory and Field Observations.

Soot particles form during combustion of carbonaceous materials and impact climate and air quality. When freshly emitted, they are typically fractal-like aggregates. After atmospheric aging, they can act as cloud condensation nuclei, and water condensation or evaporation restructure them to more compact aggregates, affecting their optical, aerodynamic, and surface properties.

Evaluation of global simulations of aerosol particle and cloud condensation nuclei number, with implications for cloud droplet formation.

A total of 16 global chemistry transport models and general circulation models have participated in this study; 14 models have been evaluated with regard to their ability to reproduce the near-surface observed number concentration of aerosol particles and cloud condensation nuclei (CCN), as well as derived cloud droplet number concentration (CDNC). Model results for the period 2011-2015 are compared with aerosol measurements (aerosol particle number, CCN and aerosol particle composition in the submicron fraction) from nine surface stations located in Europe and Japan. The evaluation focuses on the ability of models to simulate the average across time state in diverse environments and on the seasonal and short-term variability in the aerosol properties.

Antarctic sea ice region as a source of biogenic organic nitrogen in aerosols.

Climate warming affects the development and distribution of sea ice, but at present the evidence of polar ecosystem feedbacks on climate through changes in the atmosphere is sparse. By means of synergistic atmospheric and oceanic measurements in the Southern Ocean near Antarctica, we present evidence that the microbiota of sea ice and sea ice-influenced ocean are a previously unknown significant source of atmospheric organic nitrogen, including low molecular weight alkyl-amines. Given the keystone role of nitrogen compounds in aerosol formation, growth and neutralization, our findings call for greater chemical and source diversity in the modelling efforts linking the marine ecosystem to aerosol-mediated climate effects in the Southern Ocean.

Surface tension prevails over solute effect in organic-influenced cloud droplet activation.

The spontaneous growth of cloud condensation nuclei (CCN) into cloud droplets under supersaturated water vapour conditions is described by classic Köhler theory. This spontaneous activation of CCN depends on the interplay between the Raoult effect, whereby activation potential increases with decreasing water activity or increasing solute concentration, and the Kelvin effect, whereby activation potential decreases with decreasing droplet size or increases with decreasing surface tension, which is sensitive to surfactants. Surface tension lowering caused by organic surfactants, which diminishes the Kelvin effect, is expected to be negated by a concomitant reduction in the Raoult effect, driven by the displacement of surfactant molecules from the droplet bulk to the droplet-vapour interface.

Results of an interlaboratory comparison of analytical methods for quantification of anhydrosugars and biosugars in atmospheric aerosol.

An interlaboratory comparison was performed to evaluate the analytical methods for quantification of anhydrosugars - levoglucosan, mannosan, galactosan - and biosugars - arabitol, glucose and mannitol - in atmospheric aerosol. The performance of 10 laboratories in Italy currently involved in such analyses was investigated on twenty-six PM (particulate matter) ambient filters, three synthetic PM filters and three aqueous standard solutions. An acceptable interlaboratory variability was found, determined as the mean relative standard deviation (RSD%) of the results from the participating laboratories, with the mean RSD% values ranging from 25% to 46% and decreasing with increasing sugar concentration.

Direct observation of aqueous secondary organic aerosol from biomass-burning emissions.

The mechanisms leading to the formation of secondary organic aerosol (SOA) are an important subject of ongoing research for both air quality and climate. Recent laboratory experiments suggest that reactions taking place in the atmospheric liquid phase represent a potentially significant source of SOA mass. Here, we report direct ambient observations of SOA mass formation from processing of biomass-burning emissions in the aqueous phase.

Connecting marine productivity to sea-spray via nanoscale biological processes: Phytoplankton Dance or Death Disco?

Bursting bubbles at the ocean-surface produce airborne salt-water spray-droplets, in turn, forming climate-cooling marine haze and cloud layers. The reflectance and ultimate cooling effect of these layers is determined by the spray's water-uptake properties that are modified through entrainment of ocean-surface organic matter (OM) into the airborne droplets. We present new results illustrating a clear dependence of OM mass-fraction enrichment in sea spray (OMss) on both phytoplankton-biomass, determined from Chlorophyll-a (Chl-a) and Net Primary Productivity (NPP).

Aerosol liquid water driven by anthropogenic nitrate: implications for lifetimes of water-soluble organic gases and potential for secondary organic aerosol formation.

Aerosol liquid water (ALW) influences aerosol radiative properties and the partitioning of gas-phase water-soluble organic compounds (WSOCg) to the condensed phase. A recent modeling study drew attention to the anthropogenic nature of ALW in the southeastern United States, where predicted ALW is driven by regional sulfate. Herein, we demonstrate that ALW in the Po Valley, Italy, is also anthropogenic but is driven by locally formed nitrate, illustrating regional differences in the aerosol components responsible for ALW.

On the water-soluble organic nitrogen concentration and mass size distribution during the fog season in the Po Valley, Italy.

The study of organic nitrogen gained importance in recent decades due to its links with acid rain, pollution, and eutrophication. In this study, aerosol and fog water samples collected from two sites in Italy during November 2011 were analyzed to characterize their organic nitrogen content. Organic nitrogen contributed 19-25% of the total soluble nitrogen in the aerosol and around 13% in fog water.

Important source of marine secondary organic aerosol from biogenic amines.

Relevant concentrations of dimethyl- and diethylammonium salts (DMA+ and DEA+) were measured in submicrometer marine aerosol collected over the North Atlantic during periods of high biological activity (HBA) in clean air masses (median concentration (minimum-maximum)=26(6-56) ng m(-3)). Much lower concentrations were measured during periods of low biological activity (LBA): 1 (<0.4-20) ng m(-3) and when polluted air masses were advected to the sampling site: 2 (<0.

High frequency new particle formation in the Himalayas.

Rising air pollution levels in South Asia will have worldwide environmental consequences. Transport of pollutants from the densely populated regions of India, Pakistan, China, and Nepal to the Himalayas may lead to substantial radiative forcing in South Asia with potential effects on the monsoon circulation and, hence, on regional climate and hydrological cycles, as well as to dramatic impacts on glacier retreat. An improved description of particulate sources is needed to constrain the simulation of future regional climate changes.

Combined determination of the chemical composition and of health effects of secondary organic aerosols: the POLYSOA project.

Epidemiological studies show a clear link between increased mortality and enhanced concentrations of ambient aerosols. The chemical and physical properties of aerosol particles causing these health effects remain unclear. A major fraction of the ambient aerosol particle mass is composed of secondary organic aerosol (SOA).

Source attribution of water-soluble organic aerosol by nuclear magnetic resonance spectroscopy.

The functional group compositions of atmospheric aerosol water-soluble organic compoundswere obtained employing proton nuclear magnetic resonance (1H NMR) spectroscopy in a series of recent experiments in several areas of the world characterized by different aerosol sources and pollution levels. Here, we discuss the possibility of using 1H NMR functional group distributions to identifythe sources of aerosol in the different areas. Despite the limited variability of functional group compositions of atmospheric aerosol samples, characteristic 1H NMR fingerprints were derived for three major aerosol sources: biomass burning, secondary formation from anthropogenic and biogenic VOCs, and emission from the ocean.

An anion-exchange high-performance liquid chromatography method coupled to total organic carbon determination for the analysis of water-soluble organic aerosols.

The chemical composition of water-soluble organic carbon (WSOC) in atmospheric aerosol particles is largely unexplored, due to the myriad of individual compounds, which has hampered attempts to attain a full characterization at the molecular level. An alternative approach, focusing on the analysis of a few main chemical classes, allowed the quantitative fractionation of WSOC into neutral compounds (NC), mono- and di-acids (MDA) and polyacids (PA) through an anion-exchange liquid chromatographic method. Previous attempts to quantify NC, MDA and PA relied on a low-pressure chromatographic technique using a volatile buffer, followed by total organic carbon (TOC) analysis of the fractions, or alternatively on a faster HPLC-UV method which provided a quantification of the fractions based on empirical relationships between UV signal and TOC concentration.