0000000000315941
AUTHOR
Colin D. O'dowd
Measurement report: PM<sub>2.5</sub>-bound nitrated aromatic compounds in Xi'an, Northwest China – seasonal variations and contributions to optical properties of brown carbon
Abstract. Nitrated aromatic compounds (NACs) are a group of key chromophores for brown carbon (light-absorbing organic carbon, i.e., BrC) aerosol, which affects radiative forcing. The chemical composition and sources of NACs and their contributions to BrC absorption, however, are still not well understood. In this study, PM 2.5 -bound NACs in Xi'an, Northwest China, were investigated for 112 daily PM 2.5 filter samples from 2015 to 2016. Both the total concentrations and contributions from individual species of NACs show distinct seasonal variations. The seasonally averaged concentrations of NACs are 2.1 (spring), 1.1 (summer), 12.9 (fall), and 56 ng m −3 (winter). Thereinto, 4-nitrophenol …
The role of VOC oxidation products in continental new particle formation
Abstract. Aerosol physical and chemical properties and trace gas concentrations were measured during the QUEST field campaign in March–April, 2003, in Hyytiälä, Finland. Our aim was to understand the role of oxidation products of VOC's such as mono- and sesquiterpenes in atmospheric nucleation events. Particle chemical compositions were measured using the Aerodyne Aerosol Mass Spectrometer, and chemical compositions of aerosol samples collected with low-pressure impactors and a high volume sampler were analysed using a number of techniques. The results indicate that during and after new particle formation, all particles larger than 50 nm in diameter contained similar organic substances that…
Determination of alkylamines in atmospheric aerosol particles: a comparison of gas chromatography–mass spectrometry and ion chromatography approaches
Abstract. In recent years low molecular weight alkylamines have been recognized to play an important role in particle formation and growth in the lower atmosphere. However, major uncertainties are associated with their atmospheric processes, sources and sinks, mostly due to the lack of ambient measurements and the difficulties in accurate quantification of alkylamines at trace level. In this study, we present the evaluation and optimization of two analytical approaches, i.e., gas chromatography–mass spectrometry (GC-MS) and ion chromatography (IC), for the determination of alkylamines in aerosol particles. Alkylamines were converted to carbamates through derivatization with isobutyl chlorof…
Marine aerosols and iodine emissions (Reply)
O'Dowd et al. reply - McFiggans raises some interesting, but partly speculative, issues about the possibility of additional condensable-iodine-vapour (CIV) precursors being involved in marine aerosol formation from biogenic iodine emissions, and about the relative roles of iodine oxide and sulphuric acid in the marine new-particle formation process.
The seaweeds <i>Fucus vesiculosus</i> and <i>Ascophyllum nodosum</i> are significant contributors to coastal iodine emissions
Abstract. Based on the results of a pilot study in 2007, which found high mixing ratios of molecular iodine (I2) above the intertidal macroalgae (seaweed) beds at Mweenish Bay (Ireland), we extended the study to nine different locations in the vicinity of Mace Head Atmospheric Research Station on the west coast of Ireland during a field campaign in 2009. The mean values of I2 mixing ratio found above the macroalgae beds at nine different locations ranged from 104 to 393 ppt, implying a high source strength of I2. Such mixing ratios are sufficient to result in photochemically driven coastal new-particle formation events. Mixing ratios above the Ascophyllum nodosum and Fucus vesiculosus beds …
General overview: European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI)-integrating aerosol research from nano to global scales
In this paper we describe and summarize the main achievements of the European Aerosol Cloud Climate and Air Quality Interactions project (EUCAARI). EUCAARI started on 1 January 2007 and ended on 31 December 2010 leaving a rich legacy including: (a) a comprehensive database with a year of observations of the physical, chemical and optical properties of aerosol particles over Europe, (b) comprehensive aerosol measurements in four developing countries, (c) a database of airborne measurements of aerosols and clouds over Europe during May 2008, (d) comprehensive modeling tools to study aerosol processes fron nano to global scale and their effects on climate and air quality. In addition a new Pan…
Coastal New Particle Formation: A Review of the Current State-Of-The-Art
Environmental Context.Atmospheric aerosols play an important role in determining the earth’s radiative budget, climate change and air quality levels. Much effort has been spent on quantifying the impact of aerosols on climate change; however, the largest gap in our knowledge relates to quantifying natural aerosol systems and the new particle formation process associated with these systems. The marine aerosol system is of particular interest due to the 70% ocean coverage of the earth’s surface. Coastal new particle formation events are though to be more frequent and of stronger intensity compared with open ocean events and thus have been studied in detail to identify possible processes lead…
Water-Insoluble Organics Dominate Brown Carbon in Wintertime Urban Aerosol of China: Chemical Characteristics and Optical Properties.
The chromophores responsible for light absorption in atmospheric brown carbon (BrC) are not well characterized, which hinders our understanding of BrC chemistry, the links with optical properties, and accurate model representations of BrC to global climate and atmospheric oxidative capacity. In this study, the light absorption properties and chromophore composition of three BrC fractions of different polarities were characterized for urban aerosol collected in Xi'an and Beijing in winter 2013-2014. These three BrC fractions show large differences in light absorption and chromophore composition, but the chromophores responsible for light absorption are similar in Xi'an and Beijing. Water-ins…
Measurement report of the change of PM2.5 composition during the COVID-19 lockdown in urban Xi'an: Enhanced secondary formation and oxidation
Enhanced secondary aerosol formation was observed during the COVID-19 lockdown in Xi'an, especially for polluted episodes. More oxidized‑oxygenated organic aerosol (MO-OOA) and sulfate showed the dominant enhancements, especially in large particle-mode. Meanwhile, relative humidity (RH) showed a positive promotion on the formation of sulfate and MO-OOA during the lockdown, but had no obvious correlation with less oxidized‑oxygenated organic aerosol (LO-OOA) or nitrate. Organosulfurs (OS) displayed a higher contribution (~58%) than inorganic sulfate to total sulfate enhancement in the polluted episode during the lockdown. Although the total nitrate (TN) decreased during the lockdown ascribin…
Severe Pollution in China Amplified by Atmospheric Moisture
AbstractIn recent years, severe haze events often occurred in China, causing serious environmental problems. The mechanisms responsible for the haze formation, however, are still not well understood, hindering the forecast and mitigation of haze pollution. Our study of the 2012–13 winter haze events in Beijing shows that atmospheric water vapour plays a critical role in enhancing the heavy haze events. Under weak solar radiation and stagnant moist meteorological conditions in winter, air pollutants and water vapour accumulate in a shallow planetary boundary layer (PBL). A positive feedback cycle is triggered resulting in the formation of heavy haze: (1) the dispersal of water vapour is cons…
Intercomparison and evaluation of global aerosol microphysical properties among AeroCom models of a range of complexity
Many of the next generation of global climate models will include aerosol schemes which explicitly simulate the microphysical processes that determine the particle size distribution. These models enable aerosol optical properties and cloud condensation nuclei (CCN) concentrations to be determined by fundamental aerosol processes, which should lead to a more physically based simulation of aerosol direct and indirect radiative forcings. This study examines the global variation in particle size distribution simulated by 12 global aerosol microphysics models to quantify model diversity and to identify any common biases against observations. Evaluation against size distribution measurements from…
Brown Carbon Aerosol in Urban Xi'an, Northwest China: The Composition and Light Absorption Properties.
Light-absorbing organic carbon (i.e., brown carbon or BrC) in the atmospheric aerosol has significant contribution to light absorption and radiative forcing. However, the link between BrC optical properties and chemical composition remains poorly constrained. In this study, we combine spectrophotometric measurements and chemical analyses of BrC samples collected from July 2008 to June 2009 in urban Xi'an, Northwest China. Elevated BrC was observed in winter (5 times higher than in summer), largely due to increased emissions from wintertime domestic biomass burning. The light absorption coefficient of methanol-soluble BrC at 365 nm (on average approximately twice that of water-soluble BrC) w…
The seaweeds Fucus vesiculosus and Ascophyllum nodosum are significant contributors to coastal iodine emissions
Based on the results of a pilot study in 2007, which found high mixing ratios of molecular iodine (I2) above the intertidal macroalgae (seaweed) beds at Mweenish Bay (Ireland), we extended the study to nine different locations in the vicinity of Mace Head Atmospheric Research Station on the west coast of Ireland during a field campaign in 2009. The mean values of I2 mixing ratio found above the macroalgae beds at nine different locations ranged from 104 to 393 ppt, implying a high source strength of I2. Such mixing ratios are sufficient to result in photochemically driven coastal new-particle formation events. Mixing ratios above the Ascophyllum nodosum and Fucus vesiculosus beds increased …
Effects of NH3 and alkaline metals on the formation of particulate sulfate and nitrate in wintertime Beijing
Sulfate and nitrate from secondary reactions remain as the most abundant inorganic species in atmospheric particle matter (PM). Their formation is initiated by oxidation (either in gas phase or particle phase), followed by neutralization reaction primarily by NH3, or by other alkaline species such as alkaline metal ions if available. The different roles of NH3 and metal ions in neutralizing H2SO4 or HNO3, however, are seldom investigated. Here we conducted semi-continuous measurements of SO4 2−, NO3 −, NH4 +, and their gaseous precursors, as well as alkaline metal ions (Na+, K+, Ca2+, and Mg2+) in wintertime Beijing. Analysis of aerosol acidity (estimated from a thermodynamic model) indicat…
Quantification of Coastal New Ultra-Fine Particles Formation from In situ and Chamber Measurements during the BIOFLUX Campaign
Environmental Context. Secondary processes leading to the production of ultra-fine particles by nucle- ation are still poorly understood. A fraction of new particles formed can grow into radiatively active sizes, where they can directly scatter incoming solar radiation and, if partly water soluble, contribute to the cloud condensation nuclei population. New particle formation events have been frequently observed at the Mace Head Atmospheric Research Station (western Ireland), under low tide and sunny conditions, leading to the hypothesis that new particles are formed from iodo-species emitted from macroalgae. Abstract. New particle formation processes were studied during the BIOFLUX campaig…
Contrasting sources and processes of particulate species in haze days with low and high relative humidity in winter time Beijing
Abstract. Although there are many studies of particulate matter (PM) pollution in Beijing, the sources and processes of secondary PM species during haze periods remain unclear. Limited studies have investigated the PM formation in highly-polluted environments under low and high relative humidity (RH) conditions. Herein, we present a systematic comparison of species in submicron particles (PM1) in wintertime Beijing (29 December 2014 to 28 February 2015) for clean periods and pollution periods under low and high RH conditions. PM1 species were measured with an aerosol chemical species monitor (ACSM) and an aethalometer. Sources and processes for organic aerosol (OA) were resolved by positive…
Shipborne measurements of Antarctic submicron organic aerosols: an NMR perspective linking multiple sources and bioregions
Special issue Marine organic matter: from biological production in the ocean toorganic aerosol particles and marine clouds (ACP/OS inter-journalSI).-- 15 pages, 8 figures, 1 table, supplement https://doi.org/10.5194/acp-20-4193-2020
Observations of high concentrations of I2and IO in coastal air supporting iodine-oxide driven coastal new particle formation
[1] Theoretical studies have predicted that concentrations of gaseous I2 and IO of the order of 80–100 ppt and 40–50 ppt, respectively, are required in coastal air to account for photochemically-driven coastal new-particle formation events to occur. However, measurements reported to date (i.e., ∼20 ppt I2, ≤ 10 ppt IO) have not supported the required model predictions. Here, we present measurements of high concentrations of I2 and IO in N.E. Atlantic marine air on the west coast of Ireland. The maximum mixing ratios of daytime I2 and IO over the seaweed beds during low tide were 302 ppt and 35 ppt, respectively. The I2 distribution was rather inhomogeneous, even at the inter-tidal zone, but…
Organosulfates in atmospheric aerosol: synthesis and quantitative analysis of pm<sub>2.5</sub> from xi'an, northwestern china
Abstract. The sources, formation mechanism and amount of organosulfates (OS) in atmospheric aerosol are not yet well understood, partly due to the lack of authentic standards for quantification. In this study, we report an improved robust procedure for the synthesis of organosulfates with different functional groups. Nine authentic organosulfate standards were synthesized and four standards (benzyl sulfate, phenyl sulfate, glycolic acid sulfate, and hydroxyacetone sulfate) were used to quantify their ambient concentrations. The authentic standards and ambient aerosol samples were analyzed using an optimized ultra performance liquid chromatography–electrospray ionization-tandem mass spectrom…