A. C. Aiken

Evolution of Organic Aerosols in the Atmosphere

Framework for Change Organic aerosols make up 20 to 90% of the particulate mass of the troposphere and are important factors in both climate and human heath. However, their sources and removal pathways are very uncertain, and their atmospheric evolution is poorly characterized. Jimenez et al. (p. 1525; see the Perspective by Andreae) present an integrated framework of organic aerosol compositional evolution in the atmosphere, based on model results and field and laboratory data that simulate the dynamic aging behavior of organic aerosols. Particles become more oxidized, more hygroscopic, and less volatile with age, as they become oxygenated organic aerosols. These results should lead to better predictions of climate and air quality. Organic aerosols are not compositionally static, but they evolve dramatically within hours to days of their formation. Organic aerosol (OA) particles affect climate forcing and human health, but their sources and evolution remain poorly characterized. We present a unifying model framework describing the atmospheric evolution of OA that is constrained by high–time-resolution measurements of its composition, volatility, and oxidation state. OA and OA precursor gases evolve by becoming increasingly oxidized, less volatile, and more hygroscopic, leading to the formation of oxygenated organic aerosol (OOA), with concentrations comparable to those of sulfate aerosol throughout the Northern Hemisphere. Our model framework captures the dynamic aging behavior observed in both the atmosphere and laboratory: It can serve as a basis for improving parameterizations in regional and global models.

Design, modeling, optimization, and experimental tests of a particle beam width probe for the aerodyne aerosol mass spectrometer

Aerodynamic lens inlets have revolutionized aerosol mass spectrometry by allowing the introduction of a very narrow particle beam into a vacuum chamber for subsequent analysis. The real-time measurement of particle beam width after an aerodynamic lens is of interest for two reasons: (1) it allows a correction to be made to the measured particle concentration if the beam is so broad, due to poor focusing by non-spherical particles, that some particles miss the detection system; and (2) under constant lens pressure it can provide a surrogate particle non-sphericity measurement. For these reasons, a beam width probe (BWP) has been designed and implemented for the Aerodyne Aerosol Mass Spectrometer (AMS), although this approach is also applicable to other instruments that use aerodynamic lens inlets. The probe implemented here consists of a thin vertical wire that can be precisely positioned to partially block the particle beam at fixed horizontal locations in order to map out the width of the particle beam. A computer model was developed to optimize the BWP and interpret its experimental data. Model assumptions were found to be reasonably accurate for all laboratory-generated particle types to which the model was compared. Comparisons of particle beam width data from a number of publications are also shown here. Particle losses due to beam broadening are found to be minor for the AMS for both laboratory and ambient particles. The model was then used to optimize the choice of the BWP dimensions, and to guide its use during continuous operation. A wire diameter approximately 1.55 times larger than the beam width to be measured provides near optimal sensitivity toward both collection efficiency and surrogate non-sphericity information. Wire diameters of 0.62 mm and 0.44 mm (for the AMS “long” and “short” chambers, respectively) provide reasonable sensitivity over the expected range of particle beam widths, for both spherical and non-spherical particles. Three other alternative BWP geometries were also modeled and discussed.

Morphology and mixing state of individual freshly emitted wildfire carbonaceous particles

Biomass burning is one of the largest sources of carbonaceous aerosols in the atmosphere, significantly affecting earth’s radiation budget and climate. Tar balls, abundant in biomass burning smoke, absorb sunlight and have highly variable optical properties, typically not accounted for in climate models. Here we analyse single biomass burning particles from the Las Conchas fire (New Mexico, 2011) using electron microscopy. We show that the relative abundance of tar balls (80%) is 10 times greater than soot particles (8%). We also report two distinct types of tar balls; one less oxidized than the other. Furthermore, the mixing of soot particles with other material affects their optical, chemical and physical properties. We quantify the morphology of soot particles and classify them into four categories: ~50% are embedded (heavily coated), ~34% are partly coated, ~12% have inclusions and~4% are bare. Inclusion of these observations should improve climate model performances.

The importance of aerosol mixing state and size-resolved composition on CCN concentration and the variation of the importance with atmospheric aging of aerosols

The study presents results form a detailed CCn study where different assumptions of CCN compositions and mixing states for a data set acquired during the MILAGRO experiment in Mexico City are evaluated and compared. The authors make five assumptions of different complexity and try to reproduce measured CCN number concentrations. They show that the assumption of an external mixture often leads to good results although it may not represent the true composition/mixing state of the aerosol but rather opposing effects cancel. The findings are useful and promise that relatively simple assumptions can be made to predict CCN number concentrations, even in pol-

Enhanced light absorption by mixed source black and brown carbon particles in UK winter

Black carbon (BC) and light-absorbing organic carbon (brown carbon, BrC) play key roles in warming the atmosphere, but the magnitude of their effects remains highly uncertain. Theoretical modelling and laboratory experiments demonstrate that coatings on BC can enhance BCs light absorption, therefore many climate models simply assume enhanced BC absorption by a factor of ∼1.5. However, recent field observations show negligible absorption enhancement, implying models may overestimate BCs warming. Here we report direct evidence of substantial field-measured BC absorption enhancement, with the magnitude strongly depending on BC coating amount. Increases in BC coating result from a combination of changing sources and photochemical aging processes. When the influence of BrC is accounted for, observationally constrained model calculations of the BC absorption enhancement can be reconciled with the observations. We conclude that the influence of coatings on BC absorption should be treated as a source and regionally specific parameter in climate models.

Meteorology, air quality, and health in London: The ClearfLo project

AbstractAir quality and heat are strong health drivers, and their accurate assessment and forecast are important in densely populated urban areas. However, the sources and processes leading to high concentrations of main pollutants, such as ozone, nitrogen dioxide, and fine and coarse particulate matter, in complex urban areas are not fully understood, limiting our ability to forecast air quality accurately. This paper introduces the Clean Air for London (ClearfLo; www.clearflo.ac.uk) project’s interdisciplinary approach to investigate the processes leading to poor air quality and elevated temperatures.Within ClearfLo, a large multi-institutional project funded by the U.K. Natural Environment Research Council (NERC), integrated measurements of meteorology and gaseous, and particulate composition/loading within the atmosphere of London, United Kingdom, were undertaken to understand the processes underlying poor air quality. Long-term measurement infrastructure installed at multiple levels (street and eleva...

Aerosol single scattering albedo dependence on biomass combustion efficiency: Laboratory and field studies

Single scattering albedo (ω) of fresh biomass burning (BB) aerosols produced from 92 controlled laboratory combustion experiments of 20 different woods and grasses was analyzed to determine the factors that control the variability in ω. Results show that ω varies strongly with fire-integrated modified combustion efficiency (MCEFI)—higher MCEFI results in lower ω values and greater spectral dependence of ω. A parameterization of ω as a function of MCEFI for fresh BB aerosols is derived from the laboratory data and is evaluated by field observations from two wildfires. The parameterization suggests that MCEFI explains 60% of the variability in ω, while the 40% unexplained variability could be accounted for by other parameters such as fuel type. Our parameterization provides a promising framework that requires further validation and is amenable for refinements to predict ω with greater confidence, which is critical for estimating the radiative forcing of BB aerosols.

The Green Ocean Amazon Experiment (GoAmazon2014/5) Observes Pollution Affecting Gases, Aerosols, Clouds, and Rainfall over the Rain Forest

AbstractThe Observations and Modeling of the Green Ocean Amazon 2014–2015 (GoAmazon2014/5) experiment took place around the urban region of Manaus in central Amazonia across 2 years. The urban pollution plume was used to study the susceptibility of gases, aerosols, clouds, and rainfall to human activities in a tropical environment. Many aspects of air quality, weather, terrestrial ecosystems, and climate work differently in the tropics than in the more thoroughly studied temperate regions of Earth. GoAmazon2014/5, a cooperative project of Brazil, Germany, and the United States, employed an unparalleled suite of measurements at nine ground sites and on board two aircraft to investigate the flow of background air into Manaus, the emissions into the air over the city, and the advection of the pollution downwind of the city. Herein, to visualize this train of processes and its effects, observations aboard a low-flying aircraft are presented. Comparative measurements within and adjacent to the plume followed t...

Reduction in haze formation rate on prebiotic Earth in the presence of hydrogen.

Recent attempts to resolve the faint young Sun paradox have focused on an early Earth atmosphere with elevated levels of the greenhouse gases methane (CH(4)) and carbon dioxide (CO(2)) that could have provided adequate warming to Earths surface. On Titan, the photolysis of CH(4) has been shown to create a thick haze layer that cools its surface. Unlike Titan, however, early Earths atmosphere likely contained high amounts of CO(2) and hydrogen (H(2)). In this work, we examine haze formation in an early Earth atmosphere composed of CO(2), H(2), N(2), and CH(4), with a CO(2)/CH(4) ratio of 10 and a H(2)/CO(2) ratio of up to 15. To initiate aerosol formation, a broad-spectrum ultraviolet (UV) energy source with emission at Lyman-alpha was used to simulate the solar spectrum. Aerosol composition and total aerosol mass produced as a function of reagent gas were measured with an aerosol mass spectrometer (AMS). Results show an order of magnitude decrease in haze production with the addition of H(2), with no significant change in the chemical composition of the haze. We calculate that the presence of H(2) on early Earth could thus have favored warmer surface temperatures and yet allowed photochemical haze formation to deliver complex organic species to early Earths surface.

Ice nucleation activity of diesel soot particles at cirrus relevant temperature conditions: Effects of hydration, secondary organics coating, soot morphology, and coagulation: Ice Nucleation of Soot Particles

Ice formation by diesel soot particles was investigated at temperatures ranging from −40 to −50°C. Size-selected soot particles were physically and chemically aged in an environmental chamber, and their ice nucleating properties were determined using a continuous flow diffusion type ice nucleation chamber. Bare (freshly formed), hydrated, and compacted soot particles, as well as α-pinene secondary organic aerosol (SOA)-coated soot particles at high relative humidity conditions, showed ice formation activity at subsaturation conditions with respect to water but below the homogeneous freezing threshold conditions. However, SOA-coated soot particles at dry conditions were observed to freeze at homogeneous freezing threshold conditions. Overall, our results suggest that heterogeneous ice nucleation activity of freshly emitted diesel soot particles are sensitive to some of the aging processes that soot can undergo in the atmosphere.