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.

Abstract. From 2006 to 2007, the daily concentrations of major inorganic water-soluble constituents, mineral aerosol, organic carbon (OC) and elemental carbon (EC) in ambient PM 10 samples were investigated from 16 urban, rural and remote sites in various regions of China, and were compared with global aerosol measurements. A large difference between urban and rural chemical species was found, normally with 1.5 to 2.5 factors higher in urban than in rural sites. Optically-scattering aerosols, such as sulfate (∼16 %), OC (∼15 %), nitrate (∼7 %), ammonium (∼5 %) and mineral aerosol (∼35 %) in most circumstance, are majorities of the total aerosols, indicating a dominant scattering feature of aerosols in China. Of the total OC, ∼55 %-60 % can be attributed to the formation of the secondary organic carbon (SOC). The absorbing aerosol EC only accounts for ∼3.5 % of the total PM 10 . Seasonally, maximum concentrations of most aerosol species were found in winter while mineral aerosol peaks in spring. In addition to the regular seasonal maximum, secondary peaks were found for sulfate and ammonium in summer and for OC and EC

Continuous measurements of atmospheric ammonia (NH₃) were conducted using Ogawa passive samplers from February 2008 to July 2010 at an urban site and from January 2007 to July 2010 at a rural site in Beijing, China. NH₄⁺ in fine particles was also collected at the rural site during 2008–2009. The field comparison between the Ogawa passive samplers and an active analyzer for NH₃ conducted at the urban site assures the quality and accuracy of the measurements. The concentrations of NH₃ at the urban site ranged from 0.7 to 85.1 ppb, with the annual average of 18.5 ± 13.8 and 23.5 ± 18.0 ppb in 2008 and 2009, respectively. The NH₃ concentrations at the rural site were lower than those at urban site, and varied from 0.8 to 42.9 ppb, with the annual average of 4.5 ± 4.6, 6.6 ± 7.0 and 7.1 ± 3.5 ppb in 2007, 2008 and 2009, respectively. The data showed marked seasonal variations at both sites. The results emphasized traffic to be a significant source of NH₃ concentrations in winter in urban areas of Beijing. This was illustrated by the strong correlations of NH₃ with the traffic related pollutants (NO_x and CO) and also by the bimodal diurnal cycle of NH₃ concentrations that was synchronized with traffic. Similar patterns were not observed during the summer, suggesting other non-traffic sources became more important. At the rural site, the daily NH₄⁺ concentrations ranged from 0.10 to 36.53 μg m⁻³, with an average of 7.03 μg m⁻³ from June 2008 to December 2009. Monthly NH₃ were significantly correlated with NH₄⁺ concentrations. Average monthly NH₃/NH₄⁺ ratios varied from 0.13 to 2.28, with an average of 0.73. NH₄⁺ in PM_2.5 was primarily associated with SO₄^−2 at the rural site

Abstract. Atmospheric particle number size distributions (size range 0.003-10µm) were measured between March 2008 and August 2009 at Shangdianzi (SDZ), a rural research station in the North China Plain. These measurements were made in an attempt to better characterize the tropospheric background aerosol in Northern China. The mean particle number concentrations of the total particle, as well as the nucleation, Aitken, accumulation and coarse mode were determined to be 1.2 ± 0.9 × 10 4 , 3.6 ± 7.9 × 10 3 , 4.4 ± 3.4 × 10 3 , 3.5 ± 2.8 × 10 3 and 2 ± 3 cm −3 , respectively. A general finding was that the particle number concentration was higher during spring compared to the other seasons. The air mass origin had an important effect on the particle number concentration and new particle formation events. Air masses from northwest (i.e. inner Asia) favored the new particle formation events, while air masses from southeast showed the highest particle mass concentration. Significant diurnal variations in particle number were observed, which could be linked to new particle formation events, i.e. gas-to-particle conversion. During particle formation events, the number concentration of the nucleation mode rose up to maximum value of 10 4 cm −3 . New particle formation events were observed on 36% of the effective measurement days. The formation rate ranged from 0.7 to 72.7 cm −3 s −1 , with a mean value of 8.0 cm −3 s −1 . The value of the nucleation mode growth rate was in the range of 0.3-14.5 nm h −1 , with a mean value of 4.3 nm h −1 . It was anCorrespondence to: J. Y. Sun (jysun@cams.cma.gov.cn) essential observation that on many occasions the nucleation mode was able to grow into the size of cloud condensation nuclei (CCN) within a matter of several hours. Furthermore, the new particle formation was regularly followed by a measurable increase in particle mass concentration and extinction coefficient, indicative of a high abundance of condensable vapors in the atmosphere under study.

Abstract. Sea salt aerosols (SSA) are dominant particles in the Arctic atmosphere and determine the polar radiative balance. SSA react with acidic pollutants that lead to changes in physical and chemical properties of their surface, which in turn alter their hygroscopic and optical properties. Transmission electron microscopy with energy-dispersive X-ray spectrometry was used to analyze morphology, composition, size, and mixing state of individual SSA at Ny-Ålesund, Svalbard, in summertime. Individual fresh SSA contained cubic NaCl coated by certain amounts of MgCl2 and CaSO4. Individual partially aged SSA contained irregular NaCl coated by a mixture of NaNO3, Na2SO4, Mg(NO3)2, and MgSO4. The comparison suggests the hydrophilic MgCl2 coating in fresh SSA likely intrigued the heterogeneous reactions at the beginning of SSA and acidic gases. Individual fully aged SSA normally had Na2SO4 cores and an amorphous coating of NaNO3. Elemental mappings of individual SSA particles revealed that as the particles ageing Cl gradually decreased, the C, N, O, and S content increased. 12C- mapping from nanoscale secondary ion mass spectrometry indicates that organic matter increased in the aged SSA compared with the fresh SSA. 12C- line scan further shows that organic matter was mainly concentrated on the aged SSA surface. These new findings indicate that this mixture of organic matter and NaNO3 on particle surfaces likely determines their hygroscopic and optical properties. These abundant SSA as reactive surfaces adsorbing inorganic and organic acidic gases can shorten acidic gas lifetime and influence the possible gaseous reactions in the Arctic atmosphere, which need to be incorporated into atmospheric chemical models in the Arctic troposphere.

Abstract. Scattering of solar radiation by aerosol particles is highly dependent on relative humidity (RH) as hygroscopic particles take up water with increasing RH. To achieve a better understanding of the effect of aerosol hygroscopic growth on light scattering properties and radiative forcing, the aerosol scattering coefficients at RH in the range of 40 to ∼ 90 % were measured using a humidified nephelometer system in the Yangtze River Delta of China in March 2013. In addition, the aerosol size distribution and chemical composition were measured. During the observation period, the mean and standard deviation (SD) of enhancement factors at RH = 85 % for the scattering coefficient (f (85 %)), backscattering coefficient (f b (85 %)), and hemispheric backscatter fraction (f β (85 %)) were 1.58 ± 0.12, 1.25 ± 0.07, and 0.79 ± 0.04, respectively, i.e., aerosol scattering coefficient and backscattering coefficient increased by 58 and 25 % as the RH increased from 40 to 85 %. Concurrently, the aerosol hemispheric backscatter fraction decreased by 21 %. The relative amount of organic matter (OM) or inorganics in PM 1 was found to be a main factor determining the magnitude of f (RH). The highest values of f (RH) corresponded to the aerosols with a small fraction of OM, and vice versa. The relative amount of NO − 3 in fine particles was strongly correlated with f (85 %), which suggests that NO − 3 played a vital role in aerosol hygroscopic growth during this study. The mass fraction of nitrate also had a close relationship to the curvature of the humidograms; higher mass fractions of nitrate were associated with humidograms that had the least curvature. Aerosol hygroscopic growth caused a 47 % increase in the calculated aerosol direct radiative forcing at 85 % RH, compared to the forcing at 40 % RH.

Abstract. Long-term measurements of particle number size distributions were carried out both at an urban background site (Peking University, PKU) and a regional Global Atmospheric Watch station (Shangdianzi, SDZ) from March to November in 2008. In total, 52 new particle formation (NPF) events were observed simultaneously at both sites, indicating that this is a regional phenomenon in the North China Plain. On average, the mean condensation sink value before the nucleation events started was 0.025 s −1 in the urban environment, which was 1.6 times higher than that at regional site. However, higher particle formation and growth rates were observed at PKU (10.8 cm −3 s −1 and 5.2 nm h −1 ) compared with those at SDZ (4.9 cm −3 s −1 and 4.0 nm h −1 ). These results implied that precursors were much more abundant in the polluted urban environment. Different from the observations in cleaner environments, the background conditions of the observed particle homogeneous nucleation events in the North China Plain could be characterized as the co-existing of a stronger source of precursor gases and a higher condensational sink of pre-existing aerosol particles. Secondary aerosol formation following nucleation events results in an increase of particle mass concentration, particle light scattering coefficient, and cloud condensation nuclei (CCN) number concentration, with consequences on visibility, radiative effects, and air quality. Typical regional NPF events with significant particle nucleation rates and subsequent particle growth over a sufficiently long time period at both sites were chosen to investigate the influence of NPF on the number concentration of "potential" CCN. As a result, the NPF and the subsequent condensable growth increased the CCN number concentration in the North China Plain by factors in the range from 5.6 to 8.7. Moreover, the potential contribution of anthropogenic emissions to the CCN number concentration was more than 50 %, to which more attention should be drawn in regional and global climate modeling, especially in the polluted urban areas.