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.

Organic aerosol (OA) data acquired by the Aerosol Mass Spectrometer (AMS) in 37 field campaigns were deconvolved into hydrocarbon‐like OA (HOA) and several types of oxygenated OA (OOA) components. HOA has been linked to primary combustion emissions (mainly from fossil fuel) and other primary sources such as meat cooking. OOA is ubiquitous in various atmospheric environments, on average accounting for 64%, 83% and 95% of the total OA in urban, urban downwind, and rural/remote sites, respectively. A case study analysis of a rural site shows that the OOA concentration is much greater than the advected HOA, indicating that HOA oxidation is not an important source of OOA, and that OOA increases are mainly due to SOA. Most global models lack an explicit representation of SOA which may lead to significant biases in the magnitude, spatial and temporal distributions of OA, and in aerosol hygroscopic properties.

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[1] The aerosol mass spectrometer (AMS), manufactured by Aerodyne Research, Inc., has been shown to be capable of delivering quantitative information on the chemical composition and size of volatile and semivolatile fine airborne particulate matter with high time resolution. Analytical and software tools for interpreting the data from this instrument and generating meaningful, quantitative results have been developed and are presented here with a brief description of the instrument. These include the conversion of detected ion rates from the quadrupole mass spectrometer during the mass spectrum (MS) mode of operation to atmospheric mass concentrations of chemical species (in mg m À3 ) by applying calibration data. It is also necessary to correct for variations in the electron multiplier performance, and a method involving the measurement of the instrument's response to gas phase signals is also presented. The techniques for applying particle velocity calibration data and transforming signals from time of flight (TOF) mode to chemical mass distributions in terms of aerodynamic diameter (dM/dlog(D a ) distributions) are also presented. It is also possible to quantify the uncertainties in both MS and TOF data by evaluating the ion counting statistics and variability of the background signal, respectively. This paper is accompanied by part 2 of this series, in which these methods are used to process and analyze AMS results on ambient aerosol from two U.K. cities at different times of the year.

Two Aerodyne Aerosol Mass Spectrometers (AMS) were deployed at three sites representing urban, semi-rural and rural areas during the Pacific 2001 experiment in the Lower Fraser Valley (LFV), British Columbia, Canada in August 2001. The AMS provides on-line quantitative measurements of the size and chemical composition of the non-refractory fraction of submicron aerosol particles. A significant accumulation mode with a peak around 400-500 nm was observed at all sites that was principally composed of sulphate, organics, ammonium and some nitrate. Another significant mode with a peak below 200 nm was also observed at the urban site and when urban plumes affected the other sites. This paper focuses on the variability of the organic particulate composition and size distribution as a function of location and photochemical activity with a particular emphasis on the urban and rural areas. The small organic mode at the urban site was well correlated with gas phase CO, 1,3-butadiene, benzene and toluene with Pearson's r values of 0.76, 0.71, 0.79 and 0.69, respectively, suggesting that combustion-related emissions are likely to be the main source of the small organic mode at this site. The mass spectra of the urban organic particulate are similar to those of internal combustion engine lubricating oil, and of diesel exhaust aerosol particles, implying that they were composed of a mixture of n-alkanes, branched alkanes, cycloalkanes, and aromatics. In contrast, organic particulate at the rural site was dominated by shorter chain oxidized organic compounds. Correlations between the two organic modes and gas phase compounds at the rural site indicated that a significant part of the small mode originated from combustion sources, while the large accumulation organic mode appeared to be the result of photochemical processing. Processing of organic particulate during a relatively high O 3 episode at the rural site appeared to increase the modal diameter of the accumulation mode from about 400 to 600 nm and almost doubled its mass loading. r

Abstract. Measurements of aerosol properties were made in aged polluted and clean background air masses encountered at the North Norfolk (UK) coastline as part of the TORCH2 field campaign in May 2004. Hygroscopic growth factors (GF) at 90% relative humidity (RH) for D 0 =27-217 nm particles and size-resolved chemical composition were simultaneously measured using a Hygroscopicity Tandem Differential Mobility Analyser (HTDMA) and an Aerodyne aerosol mass spectrometer (Q-AMS), respectively. Both hygroscopic properties and chemical composition showed pronounced variability in time and with particles size. With this data set we could demonstrate that the Zdanovskii-Stokes-Robinson (ZSR) mixing rule combined with chemical composition data from the AMS makes accurate quantitative predictions of the mean GF of mixed atmospheric aerosol particles possible. In doing so it is crucial that chemical composition data are acquired with high resolution in both particle size and time, at least matching the actual variability of particle properties. The closure results indicate an ensemble GF of the organic fraction of ∼1.20±0.10 at 90% water activity. Thus the organics contribute somewhat to hygroscopic growth, particularly at small sizes, however the inorganic salts still dominate.Furthermore it has been found that most likely substantial evaporation losses of NH 4 NO 3 occurred within the HTDMA instrument, exacerbated by a long residence time of ∼1 min. Such an artefact is in agreement with our laboratory experiments and literature data for pure NH 4 NO 3 , both showing similar evaporation losses within HTDMAs with residence times of ∼1 min. Short residence times and low temperatures are hence recommended for HTDMAs in order to minimise such evaporation artefacts.

Abstract. The VAMOS 1 Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx) was an international field program designed to make observations of poorly understood but critical components of the coupled climate system of the southeast Pacific. This region is characterized by strong coastal upwelling, the coolest SSTs in the tropi- cal belt, and is home to the largest subtropical stratocumulus deck on Earth. The field intensive phase of VOCALSREx took place during October and November 2008 and constitutes a critical part of a broader CLIVAR program (VOCALS) designed to develop and promote scientific activities leading to improved understanding, model simulations, and predictions of the southeastern Pacific (SEP) coupled ocean-atmosphere-land system, on diurnal to interannual timescales. The other major components of VOCALS are a modeling program with a model hierarchy ranging from the local to global scales, and a suite of extended observations from regular research cruises, instrumented moorings, Published by Copernicus Publications on behalf of the European Geosciences Union. R. Wood et al.: VOCALS operationsand satellites. The two central themes of VOCALS-REx focus upon (a) links between aerosols, clouds and precipitation and their impacts on marine stratocumulus radiative properties, and (b) physical and chemical couplings between the upper ocean and the lower atmosphere, including the role that mesoscale ocean eddies play. A set of hypotheses designed to be tested with the combined field, monitoring and modeling work in VOCALS is presented here. A further goal of VOCALS-REx is to provide datasets for the evaluation and improvement of large-scale numerical models. VOCALSREx involved five research aircraft, two ships and two surface sites in northern Chile. We describe the instrument payloads and key mission strategies for these platforms and give a summary of the missions conducted.

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