Large global variations in measured airborne metal concentrations driven by anthropogenic sources.

Globally consistent measurements of airborne metal concentrations in fine particulate matter (PM2.5) are important for understanding potential health impacts, prioritizing air pollution mitigation strategies, and enabling global chemical transport model development. PM2.5 filter samples (N ~ 800 from 19 locations) collected from a globally distributed surface particulate matter sampling network (SPARTAN) between January 2013 and April 2019 were analyzed for particulate mass and trace metals content. Metal concentrations exhibited pronounced spatial variation, primarily driven by anthropogenic activities. PM2.5 levels of lead, arsenic, chromium, and zinc were significantly enriched at some locations by factors of 100-3000 compared to crustal concentrations. Levels of metals in PM2.5 and PM10 exceeded health guidelines at multiple sites. For example, Dhaka and Kanpur sites exceeded the US National Ambient Air 3-month Quality Standard for lead (150 ng m-3). Kanpur, Hanoi, Beijing and Dhaka sites had annual mean arsenic concentrations that approached or exceeded the World Health Organization's risk level for arsenic (6.6 ng m-3). The high concentrations of several potentially harmful metals in densely populated cites worldwide motivates expanded measurements and analyses.

Global Sources of Fine Particulate Matter: Interpretation of PM2.5 Chemical Composition Observed by SPARTAN using a Global Chemical Transport Model.

Exposure to ambient fine particulate matter (PM2.5) is a leading risk factor for the global burden of disease. However, uncertainty remains about PM2.5 sources. We use a global chemical transport model (GEOS-Chem) simulation for 2014, constrained by satellite-based estimates of PM2.5 to interpret globally dispersed PM2.5 mass and composition measurements from the ground-based surface particulate matter network (SPARTAN). Measured site mean PM2.5 composition varies substantially for secondary inorganic aerosols (2.4-19.7 µg/m3), mineral dust (1.9-14.7 µg/m3), residual/organic matter (2.1-40.2 µg/m3), and black carbon (1.0-7.3 µg/m3). Interpretation of these measurements with the GEOS-Chem model yields insight into sources affecting each site. Globally, combustion sectors such as residential energy use (7.9 µg/m3), industry (6.5 µg/m3), and power generation (5.6 µg/m3) are leading sources of outdoor global population-weighted PM2.5 concentrations. Global population-weighted organic mass is driven by the residential energy sector (64%) whereas population-weighted secondary inorganic concentrations arise primarily from industry (33%) and power generation (32%). Simulation-measurement biases for ammonium nitrate and dust identify uncertainty in agricultural and crustal sources. Interpretation of initial PM2.5 mass and composition measurements from SPARTAN with the GEOS-Chem model constrained by satellite-based PM2.5 provides insight into sources and processes that influence the global spatial variation in PM2.5 composition.

Retrievals of aerosol optical and microphysical properties from Imaging Polar Nephelometer scattering measurements.

A method for the retrieval of aerosol optical and microphysical properties from in situ light-scattering measurements is presented and the results are compared with existing measurement techniques. The Generalized Retrieval of Aerosol and Surface Properties (GRASP) is applied to airborne and laboratory measurements made by a novel polar nephelometer. This instrument, the Polarized Imaging Nephelometer (PI-Neph), is capable of making high-accuracy field measurements of phase function and degree of linear polarization, at three visible wavelengths, over a wide angular range of 3 to 177°. The resulting retrieval produces particle size distributions (PSDs) that agree, within experimental error, with measurements made by commercial optical particle counters (OPCs). Additionally, the retrieved real part of the refractive index is generally found to be within the predicted error of 0.02 from the expected values for three species of humidified salt particles, with a refractive index that is well established. The airborne measurements used in this work were made aboard the NASA DC-8 aircraft during the Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) field campaign, and the inversion of this data represents the first aerosol retrievals of airborne polar nephelometer data. The results provide confidence in the real refractive index product, as well as in the retrieval's ability to accurately determine PSD, without assumptions about refractive index that are required by the majority of OPCs.

SAM-CAAM: A Concept for Acquiring Systematic Aircraft Measurements to Characterize Aerosol Air Masses.

A modest operational program of systematic aircraft measurements can resolve key satellite-aerosol-data-record limitations. Satellite observations provide frequent, global aerosol-amount maps, but offer only loose aerosol property constraints needed for climate and air quality applications. We define and illustrate the feasibility of flying an aircraft payload to measure key aerosol optical, microphysical, and chemical properties in situ. The flight program could characterize major aerosol air-mass types statistically, at a level-of-detail unobtainable from space. It would: (1) enhance satellite aerosol retrieval products with better climatology assumptions, and (2) improve translation between satellite-retrieved optical properties and species-specific aerosol mass and size simulated in climate models to assess aerosol forcing, its anthropogenic components, and other environmental impacts. As such, Systematic Aircraft Measurements to Characterize Aerosol Air Masses (SAM-CAAM) could add value to data records representing several decades of aerosol observations from space, improve aerosol constraints on climate modeling, help interrelate remote-sensing, in situ, and modeling aerosol-type definitions, and contribute to future satellite aerosol missions. Fifteen Required Variables are identified, and four Payload Options of increasing ambition are defined, to constrain these quantities. "Option C" could meet all the SAM-CAAM objectives with about 20 instruments, most of which have flown before, but never routinely several times per week, and never as a group. Aircraft integration, and approaches to data handling, payload support, and logistical considerations for a long-term, operational mission are discussed. SAM-CAAM is feasible because, for most aerosol sources and specified seasons, particle properties tend to be repeatable, even if aerosol loading varies.

Polarized Imaging Nephelometer for in situ airborne measurements of aerosol light scattering.

Global satellite remote sensing of aerosols requires in situ measurements to enable the calibration and validation of algorithms. In order to improve our understanding of light scattering by aerosol particles, and to enable routine in situ airborne measurements of aerosol light scattering, we have developed an instrument, called the Polarized Imaging Nephelometer (PI-Neph). We designed and built the PI-Neph at the Laboratory for Aerosols, Clouds and Optics (LACO) of the University of Maryland, Baltimore County (UMBC). This portable instrument directly measures the ambient scattering coefficient and phase matrix elements of aerosols, in the field or onboard an aircraft. The measured phase matrix elements are the P(11), phase function, and P(12). Lasers illuminate the sampled ambient air and aerosol, and a wide field of view camera detects scattered light in a scattering angle range of 3° to 176°. The PI-Neph measures an ensemble of particles, supplying the relevant quantity for satellite remote sensing, as opposed to particle-by-particle measurements that have other applications. Comparisons with remote sensing measurements will have to consider aircraft inlet effects. The PI-Neph first measured at a laser wavelength of 532nm, and was first deployed successfully in 2011 aboard the B200 aircraft of NASA Langley during the Development and Evaluation of satellite ValidatiOn Tools by Experimenters (DEVOTE) project. In 2013, we upgraded the PI-Neph to measure at 473nm, 532nm, and 671nm nearly simultaneously. LACO has deployed the PI-Neph on a number of airborne field campaigns aboard three different NASA aircraft. This paper describes the PI-Neph measurement approach and validation by comparing measurements of artificial spherical aerosols with Mie theory. We provide estimates of calibration uncertainties, which show agreement with the small residuals between measurements of P(11) and -P(12)/P(11) and Mie theory. We demonstrate the capability of the PI-Neph to measure ambient aerosol with two data sets from the Deep Convective Clouds and Chemistry (DC3) field campaign, from flights over Colorado in June 2012.

Smoke invigoration versus inhibition of clouds over the Amazon.

The effect of anthropogenic aerosols on clouds is one of the most important and least understood aspects of human-induced climate change. Small changes in the amount of cloud coverage can produce a climate forcing equivalent in magnitude and opposite in sign to that caused by anthropogenic greenhouse gases, and changes in cloud height can shift the effect of clouds from cooling to warming. Focusing on the Amazon, we show a smooth transition between two opposing effects of aerosols on clouds: the microphysical and the radiative. We show how a feedback between the optical properties of aerosols and the cloud fraction can modify the aerosol forcing, changing the total radiative energy and redistributing it over the atmospheric column.