Complex Hygroscopic Behavior of Ambient Aerosol Particles Revealed by a Piezoelectric Technique.

Understanding the complex interactions between atmospheric aerosols and water vapor in subsaturated regions of the atmosphere is crucial for modeling and predicting aerosol-cloud-radiation-climate interactions. However, the microphysical mechanisms of these interactions for ambient aerosols remain poorly understood. For this study, size-resolved samples were collected from a high-altitude, relatively clean site situated in the Western Ghats of India during the monsoon season, in order to study background and preindustrial processes as a baseline for climate functioning within the context of the most polluted region of the world. Measurements of humidity-dependent mass-based growth factors, hygroscopicity, deliquescence behavior, and aerosol liquid water content (ALWC) were made by a novel approach using a quartz crystal microbalance based on a piezo-electric sensor. The climate-relevant fine-mode aerosols (≤2.5 µm) exhibited strong size-dependent variations in their interactions with water vapor and contributed a high fraction of ALWC. Deliquescence occurred for relatively large aerosols (diameter >180 nm) but was absent for smaller aerosols. The deliquescence relative humidity for ambient aerosols was significantly lower than that of pure inorganic salts, suggesting a strong influence of organic species. Our study establishes an improved approach for accurately measuring aerosol water uptake characteristics of ambient aerosols in the subsaturated regime, aiding in the assessment of radiative forcing effects and improving climate models.

Black carbon over tropical Indian coast during the COVID-19 lockdown: inconspicuous role of coastal meteorology.

Black carbon (BC) aerosols critically impact the climate and hydrological cycle. The impact of anthropogenic emissions and coastal meteorology on BC dynamics, however, remains unclear over tropical India, a globally identified hotspot. In this regard, we have performed in situ measurements of BC over a megacity (Chennai, 12° 59' 26.5″ N, 80° 13' 51.8″ E) on the eastern coast of India during January-June 2020, comprising the period of COVID-19-induced strict lockdown. Our measurements revealed an unprecedented reduction in BC concentration by an order of magnitude as reported by other studies for various other pollutants. This was despite having stronger precipitation during pre-lockdown and lesser precipitation washout during the lockdown. Our analyses, taking mesoscale dynamics into account, unravels stronger BC depletion in the continental air than marine air. Additionally, the BC source regime also shifted from a fossil-fuel dominance to a biomass burning dominance as a result of lockdown, indicating relative reduction in fossil fuel combustion. Considering the rarity of such a low concentration of BC in a tropical megacity environment, our observations and findings under near-natural or background levels of BC may be invaluable to validate model simulations dealing with BC dynamics and its climatic impacts in the Anthropocene.

Air quality during demolition and recovery activities in post-Katrina New Orleans.

Air samples were collected during demolition and cleanup operations in the Lakeview district of New Orleans, Louisiana, USA, in late 2005 during the period immediately after Hurricane Katrina. Three different high-volume air samples were collected around waste collection areas that were created to temporarily hold the debris from the cleanup of residential properties in the area. Particulate concentrations were elevated and included crystalline fibers associated with asbestos. Metal concentrations on particulate matter resembled those measured in sediments deposited by floodwaters with the exception of Ba, which was elevated at all three locations. The highest organic contaminant concentration measured on particulates was the pesticide Ziram (Zinc, bis[diethylcarbamodithioato-S,S']-, [T-4]-) at 2,200 microg/g of particulate matter during sampling period 2. Ziram is used in latex paint, adhesives, caulking, and wallboard as a preservative. Fungal isolates developed from particulate air samples included species associated with disease including Aspergillus and Penicillium species. These data represent the most comprehensive assessment of demolition activities during the period immediately after Hurricane Katrina.

Vapor-phase transport of explosives from buried sources in soils.

The fate and transport of explosives in the soil pore vapor spaces affects both the potential detection of buried ordnance by chemical sensors and vadose zone transport of explosives residues. The efficacy of chemical sensors and their potential usefulness for detecting buried unexploded ordnance (UXO) is difficult to determine without understanding how its chemical signatures are transported through soil. The objectives of this study were to quantify chemical signature transport through soils under various environmental conditions in unsaturated soils and to develop a model for the same. Flux chambers, large soil containers, and batch tests were used to determine explosives signature movement and process descriptors for model development. Low signatures were observed for explosives (2,4-dinitrotoluene, 2,6-dinitrotoluene, and 1,3-dinitrobenzene) under all environmental conditions. A diffusion model was used to describe the chemical transport mechanism in the soil pore air. The soil-air partition constant was treated as a fit parameter in the model owing to the uncertainty in its a priori estimation. The model predictions of the trends in experimental fluxes and the soil concentration were only marginal at best. It was concluded that better estimates of the partition constant are required for more accurate estimation of the chemical concentration at the soil-air interface. Chemical sensors will need to be very sensitive because of low signatures. However, this may result in many false alarms because of explosives residues not associated with UXO on firing ranges. Low explosives signatures also should result in insignificant air environmental exposures.

Volatilization of contaminants from suspended sediment in a water column during dredging.

Remedial dredging of contaminated bed sediments in rivers and lakes results in the suspension of sediment solids in the water column, which can potentially be a source for evaporation of hydrophobic organic compounds (HOCs) associated with the sediment solids. Laboratory experiments were conducted in an oscillating grid chamber to simulate the suspension of contaminated sediments and flux to air from the surface of the water column. A contaminated field sediment from Indiana Harbor Canal (IHC) and a laboratory-inoculated University Lake (UL) sediment, Baton Rouge, LA, were used in the experiments, where water and solids concentration and particle size distribution were measured in addition to contaminant fluxes to air. A transient model that takes into account contaminant desorption from sediment to water and evaporation from the water column was used to simulate water and sediment concentrations and air fluxes from the solids suspension. In experiments with both sediments, the total suspended solids (TSS) concentration and the average particle diameter of the suspended solids decreased with time. As expected, the evaporative losses were higher for compounds with higher vapor pressure and lower hydrophobicity. For the laboratory-inoculated sediment (UL), the water concentrations and air fluxes were high initially and decreased steadily implying that contaminant release to the water column from the suspended solids was rapid, followed by evaporative decay. For the field sediments (IHC), the fluxes and water concentrations increased initially and subsequently decreased steadily. This implied that the initial desorption to water was slow and that perhaps the presence of oil and grease and aging influenced the contaminant release. Comparison of the model and experimental data suggested that a realistic determination of the TSS concentration that can be input into the model was the most critical parameter for predicting air emission rates.

Vapor phase transport of unexploded ordnance compounds through soils.

Unexploded ordnance (UXO) is a source of concern at several U.S. Department of Defense (DOD) sites. Localization of munitions and fate and transport of the explosive compounds from these munitions are a major issue of concern. A set of laboratory experiments were conducted in specially designed flux chambers to measure the evaporative flux of three explosive compounds (2,4-dinitrotoluene, 2,6-dinitrotoluene, and 1,3-dinitrobenzene) from three different soils. The effect of different soil moisture contents, the relative humidity of air contacting the soil surface, and soil temperature on the chemical fluxes were evaluated. A diffusion model was used to describe the chemical transport mechanism in the soil pore air. The soil-air partition constant was treated as a fit parameter in the model because of the uncertainty in the a priori estimation. The model predicts the qualitative trends of the experimental fluxes satisfactorily. Under extremely dry conditions, the flux decreased more rapidly than that predicted by the model. The fluxes from soils at 24 degrees C were higher than those at 14 degrees C, indicating a larger volatilization driving force at the higher temperature.