Worldwide, smoke from forest fires has deleterious health effects. Even so, because of the complexity of fire mechanics, public health authorities face challenges in forecasting and thus mitigating population exposure to smoke. The population in the Amazon basin regularly suffers from fire smoke tied to agriculture and land-use change.
View Article and Find Full Text PDFFollowing old-growth forest loss and subsequent land abandonment, secondary forest grows throughout the Amazon biome. For Amazonas, agricultural colonization was unsuccessful in many regions, leading to the regeneration of secondary forest and carbon storage under favorable climate conditions. Herein, the extent of regeneration in Amazonas and its timescale are investigated, including a granular analysis of its 62 municipalities, based on the MapBiomas dataset from 1985 to 2021.
View Article and Find Full Text PDFUnderstanding 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.
View Article and Find Full Text PDFPhotoionization detectors (PIDs) are lightweight and respond in real time to the concentrations of volatile organic compounds (VOCs), making them suitable for environmental measurements on many platforms. However, the nonselective sensing mechanism of PIDs challenges data interpretation, particularly when exposed to the complex VOC mixtures prevalent in the Earth's atmosphere. Herein, two approaches to this challenge are investigated.
View Article and Find Full Text PDFActivation of cloud droplets of aerosol particles from biogenic precursors plays a critical role in Earth's climate system. However, the molecular-level understanding of the cloud condensation nuclei (CCN) activation process for secondary organic matter (SOM) is still lacking. Here, we reduced the gap by segregating SOM from α-pinene based on water solubility.
View Article and Find Full Text PDFMolecular ionization potentials (IP) and photoionization cross sections (σ) can affect the sensitivity of photoionization detectors (PIDs) and other sensors for gaseous species. This study employs several methods of machine learning (ML) to predict IP and σ values at 10.6 eV (117 nm) for a dataset of 1251 gaseous organic species.
View Article and Find Full Text PDFUrbanization and fires perturb the quantities and composition of fine organic aerosol in the central Amazon, with ramifications for radiative forcing and public health. These disturbances include not only direct emissions of particulates and secondary organic aerosol (SOA) precursors but also changes in the pathways through which biogenic precursors form SOA. The composition of ambient organic aerosol is complex and incompletely characterized, encompassing millions of potential structures relatively few of which have been synthesized and characterized.
View Article and Find Full Text PDFLiquid-liquid phase separation (LLPS) of atmospheric particles impacts a range of atmospheric processes. Driven by thermodynamics, LLPS occurs in mixed organic-inorganic particles when high inorganic salt concentrations exclude organic compounds, which develop into a separate phase. The effect of particle size on the thermodynamic and kinetic drivers of LLPS, however, remains incompletely understood.
View Article and Find Full Text PDFThe interaction of aerosols and the planetary boundary layer (PBL) plays an important role in deteriorating urban air quality. Aerosols from different sources may have different effects on regulating PBL structures owing to their distinctive dominant compositions and vertical distributions. To characterize the complex feedback of aerosols on PBL over the Beijing megacity, multiple approaches, including in situ observations in the autumn and winter of 2016-2019, backward trajectory clusters, and large-eddy simulations, were adopted.
View Article and Find Full Text PDFEnviron Sci Technol
September 2022
Volatile organic compounds (VOCs) emitted from forests are important chemical components that affect ecosystem functioning, atmospheric chemistry, and regional climate. Temperature differences between a forest and an adjacent river can induce winds that influence VOC fate and transport. Quantitative observations and scientific understanding, however, remain lacking.
View Article and Find Full Text PDFThe chemical pathways for the production of secondary organic aerosols (SOA) are influenced by the concentration of nitrogen oxides (NO), including the production of organonitrates (ON). Herein, a series of experiments conducted in an environmental chamber investigated the production and partitioning of total organonitrates from α-pinene photo-oxidation from <1 to 24 ppb NO. Gas-phase and particle-phase organonitrates (gON and pON, respectively) were measured by laser-induced fluorescence (LIF).
View Article and Find Full Text PDFThe phase behavior, the number and type of phases, in atmospheric particles containing mixtures of hydrocarbon-like organic aerosol (HOA) and secondary organic aerosol (SOA) is important for predicting their impacts on air pollution, human health, and climate. Using a solvatochromic dye and fluorescence microscopy, we determined the phase behavior of 11 HOA proxies (O/C = 0-0.29) each mixed with 7 different SOA materials generated in environmental chambers (O/C 0.
View Article and Find Full Text PDFAerosol-cloud interactions remain uncertain in assessing climate change. While anthropogenic activities produce copious aerosol nanoparticles smaller than 10 nanometers, they are too small to act as efficient cloud condensation nuclei (CCN). The mechanisms responsible for particle growth to CCN-relevant sizes are poorly understood.
View Article and Find Full Text PDFWe revealed that the absorption aerosol lying below or above the morning residual layer (MRL) promotes (stove effect, heating the MRL layer) or strongly inhibits (dome effect, heating the temperature inversion layer) the development of planetary boundary layer (PBL) after sunrise, while scattering aerosol exhibits similar suppression (surface or aloft umbrella effect) on the PBL regardless of its vertical location. However, the role of different type of aerosols (i.e.
View Article and Find Full Text PDFThe influence of relative humidity (RH) on the condensational growth of organic aerosol particles remains incompletely understood. Herein, the RH dependence was investigated via a series of experiments for α-pinene ozonolysis in a continuously mixed flow chamber in which recurring cycles of particle growth occurred every 7 to 8 h at a given RH. In 5 h, the mean increase in the particle mode diameter was 15 nm at 0% RH and 110 nm at 75% RH.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
February 2021
Secondary organic aerosol (SOA) produced by atmospheric oxidation of primary emitted precursors is a major contributor to fine particulate matter (PM) air pollution worldwide. Observations during winter haze pollution episodes in urban China show that most of this SOA originates from fossil-fuel combustion but the chemical mechanisms involved are unclear. Here we report field observations in a Beijing winter haze event that reveal fast aqueous-phase conversion of fossil-fuel primary organic aerosol (POA) to SOA at high relative humidity.
View Article and Find Full Text PDFThe uptake of gaseous organic species by atmospheric particles can be affected by the reactive interactions among multiple co-condensing species, yet the underlying mechanisms remain poorly understand. Here, the uptake of unary and binary mixtures of glyoxal and pinanediol by neutral and acidic sulfate particles is investigated. These species are important products from the oxidation of volatile organic compounds (VOCs) under atmospheric conditions.
View Article and Find Full Text PDFTropical forests are acknowledged to be the largest global source of isoprene (CH) and monoterpenes (CH) emissions, with current synthesis studies suggesting few tropical species emit isoprenoids (20-38%) and do so with highly variable emission capacities, including within the same genera. This apparent lack of a clear phylogenetic thread has created difficulties both in linking isoprenoid function with evolution and for the development of accurate biosphere-atmosphere models. Here, we present a systematic emission study of "hyperdominant" tree species in the Amazon Basin.
View Article and Find Full Text PDFDiffusion coefficients in mixtures of organic molecules and water are needed for many applications, ranging from the environmental modeling of pollutant transport, air quality, and climate, to improving the stability of foods, biomolecules, and pharmaceutical agents for longer use and storage. The Stokes-Einstein relation has been successful for predicting diffusion coefficients of large molecules in organic-water mixtures from viscosity, yet it routinely underpredicts, by orders of magnitude, the diffusion coefficients of small molecules in organic-water mixtures. Herein, a unified description of diffusion coefficients of large and small molecules in organic-water mixtures, based on the fractional Stokes-Einstein relation, is presented.
View Article and Find Full Text PDFExtreme droughts associated with changes in the climate have occurred every 5 years in the Amazon during the 21st century, with the most severe being in 2015. The increase in biomass burning (BB) events that occurred during the 2015 drought had several negative socioeconomic and environmental impacts, one of which was a decrease in the air quality. This study is an investigation into the air quality in the Manaus Metropolitan Region (MMR) (central Amazon, Brazil) during the dry (September to October) and wet (April to May) seasons of 2015 and 2016.
View Article and Find Full Text PDFAn unmanned aerial vehicle (UAV) equipped with miniature monitors was used to study the vertical profiles of PM (particulate matter with a ≤2.5-μm diameter) and black carbon (BC) in Macau, China, from the surface to 500 m above ground level (AGL). Twelve- and 11-day measurements were conducted during February and March 2018, respectively.
View Article and Find Full Text PDFAtmospheric aerosol-cloud interactions remain among the least understood processes within the climate system, leaving large uncertainties in the prediction of future climates. In particular, the nature of the surfaces of aerosol particles formed from biogenic terpenes, such as α-pinene, is poorly understood despite the importance of surface phenomena in their formation, growth, radiative properties, and ultimate fate. Herein we report the coupling of a site-specific deuterium labeling strategy with vibrational sum frequency generation (SFG) spectroscopy to probe the surface C-H oscillators in α-pinene-derived secondary organic aerosol material (SOM) generated in an atmospheric flow tube reactor.
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