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Abstract. Formaldehyde (HCHO), the most abundant carbonyl compound in the atmosphere, is generated as an intermediate product in the oxidation of nonmethane hydrocarbons. Proton transfer reaction mass spectrometry (PTR-MS) has the capability to detect HCHO from ion signals at m/z 31 with high time-resolution. However, the detection sensitivity is low compared to other detectable species, and is considerably affected by humidity, due to back reactions between protonated HCHO and water vapor prior to analysis. We performed a laboratory calibration of PTR-MS for HCHO and examined the detection sensitivity and humidity dependence at various field strengths. Subsequently, we deployed the PTR-MS instrument in a field campaign at Mount Tai

Abstract. Mixing of Asian mineral dust with anthropogenic pollutants allows pollutants (e.g. sulfate and nitrate) to be transported over longer distances (e.g. to the northern Pacific, even to North America) along with dust particles. This mixing therefore affects the atmospheric and oceanic environment at local, regional and even continental scales. In this study, we used a three-dimensional regional chemical transport model (Nested Air Quality Predicting Modeling System, NAQPMS) to examine the degree of mixing between Asian mineral dust and anthropogenic pollutants in a superduststorm event during 19-22 March 2010. Influences of the mixing processes on regional atmospheric environmental and oceanic biogeochemical cycles were also investigated. A comparison with measurements showed that the model reproduced well the trajectory of long-range dust transport, the vertical dust profile, and the chemical evolution of dust particles. We found that along-path mixing processes during the long-range transport of Asian dust led to increasingly polluted particles. As a result, ∼ 60 % of the sulfate and 70-95 % of the nitrate in the downwind regions was derived from active mixing processes of minerals with pollutants sourced from the North China Plain and enhanced by transport over South China. This mixing had a significant impact on the regional-scale atmospheric composition and oceanic biogeochemical cycle. Surface HNO 3 , SO 2 and O 3 were decreased by up to 90 %, 40 % and 30 %, respectively, due to the heterogeneous reactions on dust particles. Fe solubility rose from ∼ 0.5 % in the Gobi region to ∼ 3-5 % in the northwestern Pacific, resulting from oxidization of SO 2 on dust particles. Total Fe(II) deposition in the ocean region of East Asia reached 327 tons during the 4-day dust event, and created a calculated primary productivity of ∼ 520 mgC m −2 d −1 in the Kuril Islands, which can support almost 100 % of the observed mean marine primary productivity in spring in this region (526 mgC m −2 d −1 ).

Abstract. Aerosol particles were characterized by an Aerodyne aerosol chemical speciation monitor along with various collocated instruments in Beijing, China, to investigate the role of fireworks (FW) and secondary aerosol in particulate pollution during the Chinese Spring Festival of 2013. Three FW events, exerting significant and short-term impacts on fine particles (PM2.5), were observed on the days of Lunar New Year, Lunar Fifth Day, and Lantern Festival. The FW were shown to have a large impact on non-refractory potassium, chloride, sulfate, and organics in submicron aerosol (PM1), of which FW organics appeared to be emitted mainly in secondary, with its mass spectrum resembling that of secondary organic aerosol (SOA). Pollution events (PEs) and clean periods (CPs) alternated routinely throughout the study. Secondary particulate matter (SPM = SOA + sulfate + nitrate + ammonium) dominated the total PM1 mass on average, accounting for 63–82% during nine PEs in this study. The elevated contributions of secondary species during PEs resulted in a higher mass extinction efficiency of PM1 (6.4 m2 g-1) than during CPs (4.4 m2 g-1). The Chinese Spring Festival also provides a unique opportunity to study the impact of reduced anthropogenic emissions on aerosol chemistry in the city. Primary species showed ubiquitous reductions during the holiday period with the largest reduction being in cooking organic aerosol (OA; 69%), in nitrogen monoxide (54%), and in coal combustion OA (28%). Secondary sulfate, however, remained only slightly changed, and the SOA and the total PM2.5 even slightly increased. Our results have significant implications for controlling local primary source emissions during PEs, e.g., cooking and traffic activities. Controlling these factors might have a limited effect on improving air quality in the megacity of Beijing, due to the dominance of SPM from regional transport in aerosol particle composition.

Abstract.A challenge for the quantitative analysis of tropospheric nitrogen dioxide (NO 2 ) column data from satellite observations is posed partly by the lack of satelliteindependent observations for validation. We performed such observations of the tropospheric NO 2 column using the ground-based Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) technique in the North China Plain (NCP) from 29 May to 29 June, 2006. Comparisons between tropospheric NO 2 columns measured by MAX-DOAS and the Ozone Monitoring Instrument (OMI) onboard the Aura satellite indicate that OMI data (the standard product, version 3) over NCP may have a positive bias of 1.6×10 15 molecules cm −2 (20%), yet within the uncertainty of the OMI data. Combining these results with literature validation results for the US, Europe, and Pacific Ocean suggests that a bias of +20%/−30% is a reasonable estimate, accounting for different regions.

Abstract. HO 2 uptake coefficients for ambient aerosol particles, collected on quartz fiber filter using a high-volume air sampler in China, were measured using an aerosol flow tube coupled with a chemical conversion/laser-induced fluorescence technique at 760 Torr and 298 K, with a relative humidity of 75 %. Aerosol particles were regenerated with an atomizer using the water extracts from the aerosol particles. Over 10 samples, the measured HO 2 uptake coefficients for the aerosol particles at the Mt. Tai site were ranged from 0.13 to 0.34, while those at the Mt. Mang site were in the range of 0.09-0.40. These values are generally larger than those previously reported for single-component particles, suggesting that reactions with the minor components such as metal ions and organics in the particle could contribute to the HO 2 uptake. A box model calculation suggested that the heterogeneous loss of HO 2 by ambient particles could significantly affect atmospheric HO x concentrations and chemistry.

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Abstract. Aerosol nucleation events have been observed at a variety of locations worldwide, and may have significant climatic and health implications. While ions have long been suggested as favorable nucleation embryos, their significance as a global source of particles has remained uncertain. Here, an ion-mediated nucleation (IMN) mechanism, which incorporates new thermodynamic data and physical algorithms, has been integrated into a global chemical transport model (GEOS-Chem) to study ion-mediated particle formation in the global troposphere. The simulated annual mean results have been compared to a comprehensive set of data relevant to particle nucleation around the globe. We show that predicted annual spatial patterns of particle formation agree reasonably well with land-, ship-, and aircraft-based observations. Our simulations show that, globally, IMN in the boundary layer is largely confined to two broad latitude belts: one in the northern hemisphere (∼20 • N-70 • N), and one in the southern hemisphere (∼30 • S-90 • S). In the middle latitude boundary layer over continents, the annual mean IMN rates are generally above 10 4 cm −3 day −1 , with some hot spots reaching 10 5 cm −3 day −1 . The zonally-averaged vertical distribution of IMN rates indicates that IMN is significant in the tropical upper troposphere, the entire middle latitude troposphere, and over Antarctica. Comparing the relative strengths of particle sources due to IMN and due to primary particle emissions demonstrates that IMN is significant on a global scale. Further research is needed to reduce modeling uncertainties and to understand the ultimate contribution of freshly nucleated particles to the abundance of cloud condensation nuclei.