Attribution of aerosol light absorption to black carbon, brown carbon, and dust in China ? interpretations of atmospheric measurements during EAST-AIRE

International audienceBlack carbon, brown carbon, and mineral dust are three of the most important light absorbing aerosols. Their optical properties differ greatly and are distinctive functions of the wavelength of light. Most optical instruments that quantify light absorption, however, are unable to distinguish one type of absorbing aerosol from another. It is thus instructive to separate total absorption from these different light absorbers to gain a better understanding of the optical characteristics of each aerosol type. During the EAST-AIRE (East Asian Study of Tropospheric Aerosols: an International Regional Experiment) campaign near Beijing, we measured light scattering using a nephelometer, and light absorption using an aethalometer and a particulate soot absorption photometer. We also measured the total mass concentrations of carbonaceous (elemental and organic carbon) and inorganic particulates, as well as aerosol number and mass distributions. We were able to identify periods during the campaign that were dominated by dust, biomass burning, fresh (industrial) chimney plumes, other coal burning pollution, and relatively clean (background) air for Northern China. Each of these air masses possessed distinct intensive optical properties, including the single scatter albedo and Ångstrom exponents. Based on the wavelength-dependence and particle size distribution, we apportioned total light absorption to black carbon, brown carbon, and dust; their mass absorption efficiencies at 550 nm were estimated to be 9.5, 0.5, and 0.03 m2/g, respectively. While agreeing with the common consensus that BC is the most important light absorber in the mid-visible, we demonstrated that brown carbon and dust could also cause significant absorption, especially at shorter wavelengths

Water-soluble material on aerosols collected within volcanic eruption clouds

In February and March of 1978, filter samplers mounted on an aircraft were used to collect the aerosol fraction of the eruption clouds from three active Guatemalan volcanoes (Fuego, Pacaya, and Santiaguito). The samples were collected on Teflon (Fluoropore) filters with a nominal pore diameter of 0.5μm. The mass of air sampled by the filters ranged from 0.15 to 6.6 kg. The particulate material collected consisted of fragments of angular silicate ash and droplets of what is interpreted as dilute H2SO4 and HCl. After collection of the samples, each filter was rinsed with 60 ml of distilled-deionized water. Splits of each extract were centrifuged to remove particles greater than or equal to 0.1 μm in diameter, acidified, and analyzed for B, Ba, Be, Ca, Cd, Co, Cu, Fe, Li, Mg, Mn, Mo, Na, Pb, Si, Sr, V, and Zn by inductively coupled plasma—optical emission spectroscopy. Separate splits were analyzed for F and Cl by specific-ion-electrode methods and for U by a fission track technique. The elements dissolved in the aqueous extracts represent components of water-soluble material either formed directly in the eruption cloud or derived from interaction of ash particles and aerosol components of the plume. Calculations of enrichment factors, based upon concentration ratios, showed the elements most enriched in the extracts relative to bulk ash composition were Cd, Cu, V, F, Cl, Zn, and Pb. These elements represent a subset (with the addition of Cl and F) of elements previously reported enriched in atmospheric aerosols in remote regions as well as in volcanic areas. This suggests that some of the enriched elements were widely dispersed as volatile halides emitted from a volcanic source

Large-scale distributions of tropospheric nitric, formic, and acetic acids over the western Pacific basin during wintertime

We report here measurements of the acidic gases nitric (HNO3), formic (HCOOH), and acetic (CH3COOH) over the western Pacific basin during the February-March 1994 Pacific Exploratory Mission-West (PEM-West B). These data were obtained aboard the NASA DC-8 research aircraft as it flew missions in the altitude range of 0.3–12.5 km over equatorial regions near Guam and then further westward encompassing the entire Pacific Rim arc. Aged marine air over the equatorial Pacific generally exhibited mixing ratios of acidic gases \u3c100 parts per trillion by volume (pptv). Near the Asian continent, discrete plumes encountered below 6 km altitude contained up to 8 parts per billion by volume (ppbv) HNO3 and 10 ppbv HCOOH and CH3COOH. Overall there was a general correlation between mixing ratios of acidic gases with those of CO, C2H2, and C2Cl4, indicative of emissions from combustion and industrial sources. The latitudinal distributions of HNO3 and CO showed that the largest mixing ratios were centered around 15°N, while HCOOH, CH3COOH, and C2Cl4 peaked at 25°N. The mixing ratios of HCOOH and CH3COOH were highly correlated (r2 = 0.87) below 6 km altitude, with a slope (0.89) characteristic of the nongrowing season at midlatitudes in the northern hemisphere. Above 6 km altitude, HCOOH and CH3COOH were marginally correlated (r2 = 0.50), and plumes well defined by CO, C2H2, and C2Cl4 were depleted in acidic gases, most likely due to scavenging during vertical transport of air masses through convective cloud systems over the Asian continent. In stratospheric air masses, HNO3 mixing ratios were several parts per billion by volume (ppbv), yielding relationships with O3 and N2O consistent with those previously reported for NOy

Intercomparisons of airborne measurements of aerosol ionic chemical composition during TRACE-P and ACE-Asia

As part of the two field studies, Transport and Chemical Evolution over the Pacific (TRACE-P) and the Asian Aerosol Characterization Experiment (ACE-Asia), the inorganic chemical composition of tropospheric aerosols was measured over the western Pacific from three separate aircraft using various methods. Comparisons are made between the rapid online techniques of the particle into liquid sampler (PILS) for measurement of a suite of fine particle a mist chamber/ion chromatograph (MC/IC) measurement of fine sulfate, and the longer time-integrated filter and micro-orifice impactor (MOI) measurements. Comparisons between identical PILS on two separate aircraft flying in formation showed that they were highly correlated (e.g., sulfate r2 of 0.95), but were systematically different by 10 ± 5% (linear regression slope and 95% confidence bounds), and had generally higher concentrations on the aircraft with a low-turbulence inlet and shorter inlet-to-instrument transmission tubing. Comparisons of PILS and mist chamber measurements of fine sulfate on two different aircraft during formation flying had an r 2 of 0.78 and a relative difference of 39% ± 5%. MOI ionic data integrated to the PILS upper measurement size of 1.3 mm sampling from separate inlets on the same aircraft showed that for sulfate, PILS and MOI were within 14% ± 6% and correlated with an r 2 of 0.87. Most ionic compounds were within ±30%, which is in the range of differences reported between PILS and integrated samplers from ground-based comparisons. In many cases, direct intercomparison between the various instruments is difficult due to differences in upper-size detection limits. However, for this study, the results suggest that the fine particle mass composition measured from aircraft agree to within 30–40%

Nitrous oxide dynamics in low oxygen regions of the Pacific: insights from the MEMENTO database

The Eastern Tropical Pacific (ETP) is believed to be one of the largest marine sources of the greenhouse gas nitrous oxide N2O). Future N2Oemissions from the ETP are highly uncertain because oxygen minimum zones are expected to expand, affecting both regional production and consumption of N2O. Here we assess three primary uncertainties in how N2O may respond to changing O2 levels: (1) the relationship between N2O production and O2 (is it linear or exponential at low O2 concentrations?), (2) the cutoff point at which net N2O production switches to net N2O consumption (uncertainties in this parameterization can lead to differences in model ETP N2O concentrations of more than 20%), and (3) the rate of net N2O consumption at low O2. Based on the MEMENTO database, which is the largest N2O dataset currently available, we find that N2O production in the ETP increases linearly rather than exponentially with decreasing O2. Additionally, net N2O consumption switches to net N2O production at ~ 10 μM O2, a value in line with recent studies that suggest consumption occurs on a larger scale than previously thought. N2O consumption is on the order of 0.129 mmol N2O m−3 yr−1 in the Peru–Chile Undercurrent. Based on these findings, it appears that recent studies substantially overestimated N2O production in the ETP. In light of expected deoxygenation, future N2O production is still uncertain, but due to higher-than-expected consumption levels, it is possible that N2Oconcentrations may decrease rather than increase as oxygen minimum zones expand

ScanFish Optical Plankton Counter (OPC) data from R/V Pelican cruises PE03-NGOMEX, PE04-NGOMEX, PE06-NGOMEX, PE07-NGOMEX, PE09-05, and PE11-06 in the Northern Gulf of Mexico between 2003 and 2010

Dataset: ScanFish OPCAn optical plankton counter (OPC) and CTD mounted to a ScanFish platform were towed and undulated behind the R/V Pelican during cruises PE03-NGOMEX, PE04-NGOMEX, PE06-NGOMEX, PE07-NGOMEX, PE09-05, and PE11-06 in the Northern Gulf of Mexico between 2003 and 2010. CTD and MIDAS data were synchronized and merged with simultaneously collected OPC data and aggregated into 1 second time bins. Bottom depth was obtained from the NOAA NCEI coastal relief model. For a complete list of measurements, refer to the supplemental document 'Field_names.pdf', and a full dataset description is included in the supplemental file 'Dataset_description.pdf'. The most current version of this dataset is available at: http://www.bco-dmo.org/dataset/746081NSF Division of Ocean Sciences (NSF OCE) OCE-1043261, NSF Division of Ocean Sciences (NSF OCE) OCE-1043248, NSF Division of Ocean Sciences (NSF OCE) OCE-1043249, National Oceanic and Atmospheric Administration (NOAA) NA06NOS4780148, National Oceanic and Atmospheric Administration (NOAA) NA09NOS4780198, Gulf Research Program of the National Academies of Sciences, Engineering, and Medicine (GRP) NAS-GRP-200000641

Mesozooplankton sample data from R/V Pelican cruises PE03-NGOMEX, PE04-NGOMEX, PE06-NGOMEX, PE07-NGOMEX, PE09-05 in the Northern Gulf of Mexico from 2003-2008

Dataset: Pump mesozooplankton samplesCTD casts using a high-capacity, diaphragm pump were conducted during the R/V Pelican cruises PE03-NGOMEX, PE04-NGOMEX, PE06-NGOMEX, PE07-NGOMEX, and PE09-05 in the Northern Gulf of Mexico between 2003 and 2008. Plankton samples were collected from discrete depths during the CTD casts. Subsamples of sample contents were manually counted, identified, and measured in the laboratory. For a complete list of measurements, refer to the supplemental document 'Field_names.pdf', and a full dataset description is included in the supplemental file 'Dataset_description.pdf'. The most current version of this dataset is available at: http://www.bco-dmo.org/dataset/746107NSF Division of Ocean Sciences (NSF OCE) OCE-1043261, NSF Division of Ocean Sciences (NSF OCE) OCE-1043248, NSF Division of Ocean Sciences (NSF OCE) OCE-1043249, National Oceanic and Atmospheric Administration (NOAA) NA06NOS4780148, National Oceanic and Atmospheric Administration (NOAA) NA09NOS4780198, Gulf Research Program of the National Academies of Sciences, Engineering, and Medicine (GRP) NAS-GRP-200000641

Atmospheric implications of studies of Central American volcanic eruption clouds

During February 1978 a group of scientists from the National Center for Atmospheric Research, several colleges and universities, the U.S. Geological Survey, and NASA used a specially equipped Beech Queen Air aircraft to make 11 sampling flights in Guatemala through the eruption clouds from the volcanoes Pacaya, Fuego, and Santiguito. Measurements were made of SO42−, SO2, HCl, HF, and 11 cations that were in water-soluble form, on samples collected by a specially designed filter pack. Particle size distributions were obtained with a piezoelectric cascade impactor, and the particles were identified by energy dispersive X ray analysis. Evacuated canisters were flown to obtain samples for gas Chromatographic analysis. Some of the conclusions reached are that since most of the sulfur was found to be in the form of SO2, the H2SO4 droplets resulting from major explosive eruptions must largely result from the reaction of SO2 with OH, at the same time depleting the atmosphere of OH; the volume concentration ratio [SO2]/[HCl] always somewhat exceeded unity; and the amount of fine ash remaining in the stratosphere for long periods of time may depend on the crystallinity of the magma. Correlation spectrometry showed that each volcano was emitting 300–1500 metric tons of SO2 per day

ACE-ASIA - Regional climatic and atmospheric chemical effects of Asian dust and pollution

Although continental-scale plumes of Asian dust and pollution reduce the amount of solar radiation reaching the earth's surface and perturb the chemistry of the atmosphere, our ability to quantify these effects has been limited by a lack of critical observations, particularly of layers above the surface. Comprehensive surface, airborne, shipboard, and satellite measurements of Asian aerosol chemical composition, size, optical properties, and radiative impacts were performed during the Asian Pacific Regional Aerosol Characterization Experiment (ACE-Asia) study. Measurements within a massive Chinese dust storm at numerous widely spaced sampling locations revealed the highly complex structure of the atmosphere, in which layers of dust, urban pollution, and biomass-burning smoke may be transported long distances as distinct entities or mixed together. The data allow a first-time assessment of the regional climatic and atmospheric chemical effects of a continental-scale mixture of dust and pollution. Our results show that radiative flux reductions during such episodes are sufficient to cause regional climate change