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Bulletin, Vol. 60 (1). WMO, 2011Evaluation of the accuracy of analysis tools for atmospheric new particle formation
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 7. Korhonen H.; Sihto S.-L.; Kerminen V.-M.; et al. - Copernicus GmbH, 2011Several mathematical tools have been developed in recent years to analyze new particle formation rates and to estimate nucleation rates and mechanisms at sub-3 nm sizes from atmospheric aerosol data. Here we evaluate these analysis tools using 1239 numerical nucleation events for which the nucleation mechanism and formation rates were known exactly. The accuracy of the estimates of particle formation rate at 3 nm (J3) showed significant sensitivity to the details of the analysis, i.e. form of equations used and assumptions made about the initial size of nucleating clusters, with the fraction o ...A two-dimensional volatility basis set: 1. organic-aerosol mixing thermodynamics
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 7. Donahue N.M.; Epstein S.A.; Pandis S.N.; et al. - Copernicus GmbH, 2011We develop the thermodynamic underpinnings of a two-dimensional volatility basis set (2D-VBS) employing saturation mass concentration (Co) and the oxygen content (O:C) to describe volatility, mixing thermodynamics, and chemical evolution of organic aerosol. The work addresses a simple question: "Can we reasonably constrain organic-aerosol composition in the atmosphere based on only two measurable organic properties, volatility and the extent of oxygenation?" This is an extension of our earlier one-dimensional approach employing volatility only (C* = γ Co, where γ is an activity coefficient). U ...On the potential contribution of open lead particle emissions to the central Arctic aerosol concentration
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 7. Held A.; Brooks I.M.; Leck C.; et al. - Copernicus GmbH, 2011We present direct eddy covariance measurements of aerosol number fluxes, dominated by sub-50 nm particles, at the edge of an ice floe drifting in the central Arctic Ocean. The measurements were made during the ice-breaker borne ASCOS (Arctic Summer Cloud Ocean Study) expedition in August 2008 between 2°–10° W longitude and 87°–87.5° N latitude. The median aerosol transfer velocities over different surface types (open water leads, ice ridges, snow and ice surfaces) ranged from 0.27 to 0.68 mm s−1 during deposition-dominated episodes. Emission periods were observed more frequently over the open ...Global distribution of sea salt aerosols: new constraints from in situ and remote sensing observations
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 7. Jaeglé L.; Quinn P.K.; Bates T.S.; et al. - Copernicus GmbH, 2011We combine in situ measurements of sea salt aerosols (SS) from open ocean cruises and ground-based stations together with aerosol optical depth (AOD) observations from MODIS and AERONET, and the GEOS-Chem global chemical transport model to provide new constraints on SS emissions over the world's oceans. We find that the GEOS-Chem model using the Gong (2003) source function overestimates cruise observations of coarse mode SS mass concentrations by factors of 2–3 at high wind speeds over the cold waters of the Southern, North Pacific and North Atlantic Oceans. Furthermore, the model systematical ...Multi-scale modeling study of the source contributions to near-surface ozone and sulfur oxides levels over California during the ARCTAS-CARB period
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 7. Huang M.; Carmichael Gregory R.; Spak S.N.; et al. - Copernicus GmbH, 2011Chronic high surface ozone (O3) levels and the increasing sulfur oxides (SOx = SO2+SO4) ambient concentrations over South Coast (SC) and other areas of California (CA) are affected by both local emissions and long-range transport. In this paper, multi-scale tracer, full-chemistry and adjoint simulations using the STEM atmospheric chemistry model are conducted to assess the contribution of local emission sourcesto SC O3 and to evaluate the impacts of transported sulfur and local emissions on the SC sulfur budgetduring the ARCTAS-CARB experiment period in 2008. Sensitivity simulations quantify c ...The effect of meteorological and chemical factors on the agreement between observations and predictions of fine aerosol composition in southwestern Ontario during BAQS-Met
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 7. Markovic M.Z.; Hayden K.L.; Murphy J.G.; et al. - Copernicus GmbH, 2011The Border Air Quality and Meteorology Study (BAQS-Met) was an intensive, collaborative field campaign during the summer of 2007 that investigated the effects of transboundary pollution, local pollution, and local meteorology on air quality in southwestern Ontario. This analysis focuses on the measurements of the inorganic constituents of particulate matter with diameter of less than 1 μm (PM1), with a specific emphasis on nitrate. We evaluate the ability of AURAMS, Environment Canada's chemical transport model, to represent regional air pollution in SW Ontario by comparing modelled aerosol in ...The Smithsonian solar constant data revisited: no evidence for a strong effect of solar activity in ground-based insolation data
Apparent evidence for a strong signature of solar activity in ground-based insolation data was recently reported. In particular, a strong increase of the irradiance of the direct solar beam with sunspot number as well as a decline of the brightness of the solar aureole and the measured precipitable water content of the atmosphere with solar activity were presented. The latter effect was interpreted as evidence for cosmic-ray-induced aerosol formation. Here I show that these spurious results are due to a failure to correct for seasonal variations and the effects of volcanic eruptions and local ...Atmospheric degradation of 3-methylfuran: kinetic and products study
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 7. Tapia A.; Villanueva F.; Salgado M.S.; et al. - Copernicus GmbH, 2011A study of the kinetics and products obtained from the reactions of 3-methylfuran with the main atmospheric oxidants has been performed. The rate coefficients for the gas-phase reaction of 3-methylfuran with OH and NO3 radicals have been determined at room temperature and atmospheric pressure (air and N2 as bath gases), using a relative method with different experimental techniques. The rate coefficients obtained for these reactions were (in units cm3 molecule−1 s−1) kOH = (1.13 ± 0.22) × 10−10 and kNO3 = (1.26 ± 0.18) × 10−11. Products from the reaction of 3-methylfuran with OH, NO3 and Cl at ...Analysis on the impact of aerosol optical depth on surface solar radiation in the Shanghai megacity, China
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 7. Xu J.; Li C.; Shi H.; et al. - Copernicus GmbH, 2011This study investigated the decadal variation of the direct surface solar radiation (DiSR) and the diffuse surface solar radiation (DfSR) during 1961–2008 in the Shanghai megacity as well as their relationships to Aerosol Optical Depth (AOD) under clear-sky conditions. Three successive periods with unique features of long term variation of DiSR were identified for both clear-sky and all-sky conditions: a "dimming" period from the late 1960s to the mid 1980s, a "stabilization"/"slight brightening" period from the mid 1980s to the mid 1990s, and a "renewed dimming" period thereafter. During the ...Impact of model grid spacing on regional- and urban- scale air quality predictions of organic aerosol
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 7. Stroud C.A.; Makar P.A.; Moran M.D.; et al. - Copernicus GmbH, 2011Regional-scale chemical transport model predictions of urban organic aerosol to date tend to be biased low relative to observations, a limitation with important implications for applying such models to human exposure health studies. We used a nested version of Environment Canada's AURAMS model (42- to- 15- to- 2.5-km nested grid spacing) to predict organic aerosol concentrations for a temporal and spatial domain corresponding to the Border Air Quality and Meteorology Study (BAQS-Met), an air-quality field study that took place in the southern Great Lakes region in the summer of 2007. The use o ...Pseudo steady states of HONO measured in the nocturnal marine boundary layer: a conceptual model for HONO formation on aqueous surfaces
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 7. Wojtal P.; Halla J.D.; McLaren R. - Copernicus GmbH, 2011A complete understanding of the formation mechanism of nitrous acid (HONO) in the ambient atmosphere is complicated by a lack of understanding of processes occurring when aqueous water is present. We report nocturnal measurements of HONO, SO2 and NO2 by differential optical absorption spectroscopy over the ocean surface in a polluted marine environment. In this aqueous environment, we observed reproducible pseudo steady states (PSS) of HONO every night, that are fully formed shortly after sunset, much faster than seen in urban environments. During the PSS period, HONO is constant with time, in ...New particle formation events in semi-clean South African savannah
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 7. Vakkari V.; Laakso H.; Kulmala M.; et al. - Copernicus GmbH, 2011This study is based on 18 months (20 July 2006–5 February 2008) of continuous measurements of aerosol particle size distributions, air ion size distributions, trace gas concentrations and basic meteorology in a semi-clean savannah environment in Republic of South Africa. New particle formation and growth was observed on 69% of the days and bursts of non-growing ions/sub-10 nm particles on additional 14% of the days. This new particle formation frequency is the highest reported from boundary layer so far. Also the new particle formation and growth rates were among the highest reported in the li ...Characteristics, sources, and transport of aerosols measured in spring 2008 during the aerosol, radiation, and cloud processes affecting Arctic Climate (ARCPAC) Project
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Brock C.A.; Cozic J.; Bahreini R.; et al. - Copernicus GmbH, 2011We present an overview of the background, scientific goals, and execution of the Aerosol, Radiation, and Cloud Processes affecting Arctic Climate (ARCPAC) project of April 2008. We then summarize airborne measurements, made in the troposphere of the Alaskan Arctic, of aerosol particle size distributions, composition, and optical properties and discuss the sources and transport of the aerosols. The aerosol data were grouped into four categories based on gas-phase composition. First, the background troposphere contained a relatively diffuse, sulfate-rich aerosol extending from the top of the sea ...Impact of deep convection and dehydration on bromine loading in the upper troposphere and lower stratosphere
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Aschmann J.; Sinnhuber B.-M.; Chipperfield M.P.; et al. - Copernicus GmbH, 2011Stratospheric bromine loading due to very short-lived substances is investigated with a three-dimensional chemical transport model over a period of 21 years using meteorological input data from the European Centre for Medium-Range Weather Forecasts ERA-Interim reanalysis from 1989 to the end of 2009. Within this framework we analyze the impact of dehydration and deep convection on the amount of stratospheric bromine using an idealized and a detailed full chemistry approach. We model the two most important brominated short-lived substances, bromoform (CHBr3) and dibromomethane (CH2Br2), assumin ...
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