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Dimethylsulfide (DMS), a gas produced by marine microbial food webs, promotes aerosol formation in pristine atmospheres, altering cloud radiative forcing and precipitation. Recent studies suggest that DMS controls aerosol formation in the summertime Arctic atmosphere and call for an assessment of pan-Arctic DMS emission (EDMS) in a context of dramatic ecosystem changes. Using a remote sensing algorithm, we show that summertime EDMS from ice-free waters increased at a mean rate of 13.3 ± 6.7 Gg S decade -1 (∼33% decade -1 ) north of 70°N between 1998 and 2016. This trend, mostly explained by the reduction in sea-ice extent, is consistent with independent atmospheric measurements showing an increasing trend of methane sulfonic acid, a DMS oxidation product. Extrapolation to an ice-free Arctic summer could imply a 2.4-fold (±1.2) increase in EDMS compared to present emission. However, unexpected regime shifts in Arctic geo- and ecosystems could result in future EDMS departure from the predicted range. Superimposed on the positive trend, EDMS shows substantial interannual changes and nonmonotonic multiyear trends, reflecting the interplay between physical forcing, ice retreat patterns, and phytoplankton productivity. Our results provide key constraints to determine whether increasing marine sulfur emissions, and resulting aerosol-cloud interactions, will moderate or accelerate Arctic warming in the context of sea-ice retreat and increasing low-level cloud cover., Competing Interests: The authors declare no conflict of interest.

Atmospheric stability significantly influences the accumulation and dispersion of air pollutants in the near-surface atmosphere, yet few stability metrics have been applied as predictors in statistical PM 2.5 concentration mapping practices. In this study, eleven stability metrics were derived from radiosonde soundings collected in eastern China for the time period of 2015-2018 and then applied as independent predictors to explore their potential in favoring the prediction of PM 2.5 . The statistical results show that the in situ PM 2.5 concentration measurements correlated well with these stability metrics, especially at monthly and seasonal timescales. In contrast, correlations at the daily timescale differed markedly between stability metric and also varied with seasons. Nevertheless, the modeling results indicate that incorporating these stability metrics into the PM 2.5 modeling framework rendered small contribution to PM 2.5 prediction accuracy, yielding an increase of R 2 by < 5% and a reduction of RMSE by < 1 μg/m 3 on average. Compared with other stability indices, the inversion depth and intensity appeared to have relative larger benefiting potential. In general, our findings indicate that including these stability metrics would not result in significant contribution to the PM 2.5 prediction accuracy in eastern China since their effects could be partially overwhelmed or offset by other predictors such as AOD and boundary layer height., (Copyright © 2019 Elsevier Ltd. All rights reserved.)

Polycyclic aromatic hydrocarbons (PAHs) are ubiquitous atmospheric pollutants of high concern for public health. In the atmosphere they undergo oxidation, mainly through reactions with ·OH and NOx to produce nitro- and oxygenated (oxy-) derivatives. In this study, we developed a new method for the detection of particle-bound PAHs, nitro-PAHs and oxy-PAHs using direct infusion into an atmospheric pressure photoionisation high-resolution mass spectrometer (APPI-HRMS). Method optimisation was done by testing different source temperatures, gas flow rates, mobile phases and dopants. Samples were extracted with methanol, concentrated by evaporation and directly infused in the APPI source after adding toluene as dopant. Acquisition was performed in both polarity modes. The method was applied to target analysis of seasonal PM 2.5 samples from an urban background site in Padua (Italy), in the Po Valley, in which a series of PAHs, nitro- and oxy-PAHs were detected. APPI-HRMS was then used for non-target analysis of seasonal PM 2.5 samples and results compared with nano-electrospray ionisation (nanoESI) HRMS. The results showed that, when samples were characterised by highly oxidised organic compounds, including S-containing compounds, like in summer samples, APPI did not bring any additional information with respect to nanoESI in negative polarity (nanoESI(-)). Conversely, for winter samples, APPI(-) could detect a series of aromatic and poly-aromatic compounds, mainly oxidised and nitrogenated aromatics, that were not otherwise detected with nanoESI., (Copyright © 2019 Elsevier Ltd. All rights reserved.)

Oxidation flow reactors (OFRs) are increasingly used to study the formation and evolution of secondary organic aerosols (SOA) in the atmosphere. The OH/HO 2 and OH/O 3 ratios in OFRs are similar to tropospheric ratios. In the present work, we investigated the production of SOA generated by OH oxydation and ozonolysis of limonene in OFR as a function of OH exposure and O 3 exposure. The results are compared with those obtained from the simulation chambers. The precursor gas is exposed to OH concentrations ranging from 2.11 × 10 8 to 1.91 × 10 9  molec cm -3 , with an estimated exposure time in the OFR of 137 s. In the environmental chambers, the precursor was oxidized using OH concentrations between 2.10 × 10 6 and 2.12 × 10 7  molec cm -3 over exposure times of several hours. In the overlapping OH exposure region, the highest SOA yields are obtained in the OFR, which is explained by the ozonolysis of limonene in the OFR. However, the yields decrease with the increase of OHexp in both systems.

Pollutants, which are usually transported from urban cities to remote glacier basins, and aerosol impurities affect the earth's temperature and climate by altering the radiative properties of the atmosphere. This work focused on the physicochemical properties of atmospheric pollutants across the urban and remote background sites in northwest China. Information on individual particles was obtained using transmission electron microscopy (TEM) and energy dispersive X-ray spectrometry (EDX). Particle size and age-dependent mixing structures of individual particles in clean and polluted air were investigated. Aerosols were classified into eight components: mineral dust, black carbon (soot)/fly ash, sulfates, nitrates, NaCl salt, ammonium, organic matter, and metals. Marked spatial and seasonal changes in individual particle components were observed in the study area. Aerosol particles were generally found to be in the mixing state. For example, salt-coated particles in summer accounted for 31.2-44.8% of the total particles in urban sites and 37.5-74.5% of the total particles in background sites, while in winter, almost all urban sites comprised >50%, which implies a significant effect on the radiative forcing in the study area. We found that in PM 2.5 section, the internally mixed black carbon/organic matter particles clearly increased with diameter. Moreover, urban cities were characterized by atmospheric particles sourced from anthropogenic activities, whereas background locations exhibited much lower aerosol concentrations and increased particle density, originating from natural crustal sources (e.g., mineral dust and NaCl salt), which, together with air mass trajectory analysis, indicates a potential spatial transport process and routes of atmospheric transport from urban cities to background locations. Thus, this work is of importance in evaluating atmospheric conditions in northwest China and northeast Tibetan Plateau regions, to discover the transport processes and facilitate improvements in climatic patterns concerning atmospheric impurities., (Copyright © 2018 Elsevier Ltd. All rights reserved.)

Analysis of observed PM 2.5 in Beijing since 2009 reveals that winter haze over North China Plain (NCP) peaked in 2012 and 2013 and there was an improvement in air quality until 2016. The variation of wintertime PM 2.5 from 2009 to 2016 is influenced by both emission changes and meteorology conditions, and we quantified the relative contributions from these two aspects. Sensitivity simulation by GEOS-Chem suggested that emission reductions over NCP in 2013-2017 caused 10% decrease of regional mean PM 2.5 concentration in 2016 winter compared to 2012 winter level. We removed emission influence on PM 2.5 to get PM 2.5 that influenced by meteorology (met-influenced PM 2.5 ). For met-influenced PM 2.5 , compared to original-observed PM 2.5 (the US Embassy data), percentage of clean days (daily PM 2.5  ≤ 75 μg m -3 ) decreases while that of polluted (75 μg m -3  < daily PM 2.5 ≤150 μg m -3 ) and heavily polluted (150 μg m -3  < daily PM 2.5  ≤ 250 μg m -3 ) days increases. However, proportion of extremely polluted (daily PM 2.5  > 250 μg m -3 ) days stays unchanged, even if emission reduction is doubled, indicating that the extremely polluted situation over NCP is dominated by meteorological conditions, and emission control from 2013 to 2017 has little effects on the extremely polluted days. We developed an effective haze day index (HDI) to represent the weather conditions conducive to haze days. HDI is constructed based on the normalized near surface meridional wind (V850), temperature difference (δT) between near surface (850 hPa) and upper atmosphere (250 hPa), and the relative humidity at 1000 hPa (RH1000). HDI is skillful to detect 72% of the severe haze days (daily PM 2.5  > 150 μg m -3 ). On average, the anomalously high V850 is the main cause of severe haze, while in 2012 winter, RH1000 favorable for secondary aerosols' formation is the largest contributor to haze., (Copyright © 2018 Elsevier Ltd. All rights reserved.)

In this study, three different sensors of satellites including the Moderate Resolution Imaging Spectroradiometer (MODIS), Multi-angle Imaging SpectroRadiometer (MISR), and Total Ozone Mapping Spectrometer (TOMS) were used to study spatial and temporal variations of aerosols over ten populated cities in Iran. Also, the Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model was used for analyzing the origins of air masses and their trajectory in the area. An increasing trend in aerosol concentration was observed in the most studied cities in Iran during 1979-2016. The cities in the western part of Iran had the highest annual mean of aerosol concentration. The highest aerosol optical depth (AOD) value (0.76 ± 0.51) was recorded in May 2012 over Ahvaz, and the lowest value (0.035 ± 0.27) was recorded in December 2013 over Tabriz. After Ahvaz, the highest AOD value was found over Tehran (annual mean 0.11 ± 0.20). The results show that AOD increases with increasing industrial activities, but the increased frequency of aerosols due to land degradation and desertification is more powerful in Iran. The trajectory analysis by the HYSPLIT model showed that the air masses come from Egypt, Syria, and Lebanon and passed over the Iraq and then reached to Iran during summer. Aerosol radiative forcing (ARF) has been analyzed for Zanjan (Aerosol Robotic Network site) during 2010-2013. The ARF at surface and top of the atmosphere was found to be ranging from - 79 to - 10W m -2 (average - 33.45 W m -2 ) and from - 25 to 6 W m -2 (average - 12.80 W m -2 ), respectively.

Millions of premature deaths worldwide every year mostly in China and India are contributed by the poor air quality. The atmospheric visibility is a proven indicator of the ambient air quality. In this study, nine megacities were selected, including Beijing, Shanghai and Guangzhou from China, Chicago, Los Angeles (LA) and New York City (NYC) from the United States, and Mumbai, Chennai and Jaipur from India. The data of visibility, aerosol optical depth (AOD), and meteorological factors from 1973 to 2015 were collected. The temporal variations of annual and monthly percentages of bad days (visibility < 5km) and good days (visibility > 15km) were evaluated. Visibility of Chicago, LA and NYC gradually improved during the past 43 years and has reached a very good level (good day percentages: 75-88%; bad day percentages: 0 - 4%). Conversely, visibility in Mumbai, Chennai and Jaipur continued deteriorating and suffered an extremely poor visibility situation in recent years (good day percentages: 0; bad day percentages: 6-100%). Likewise, visibility in Beijing, Shanghai and Guangzhou has experienced the worsening period during the industrial development from 1970s and turned better after the 1990s. A strong seasonal pattern of bad day percentages of each year were observed in most cities, especially in the winter, which is caused by the fossil fuel combustion for heating, relatively high relative humidity, and other unfavorable meteorological conditions. The low visibility events occurred more frequently in days with low wind speeds and specific wind directions, further explaining the seasonal patterns of visibility. With population growth from the period of 2000-2010 to the period of 2011-2015, AOD and bad day percentages both increased in Mumbai, Chennai, Jaipur and Beijing while others were relatively stable. This study demonstrated that the macro-control of pollution emissions could effectively reduce air deterioration. The relationships among visibility variation, meteorological, pollutant and population factors provide valuable scientific support for public health researches, air quality managements (monitoring and forecasting), and clean energy initiatives., (Copyright © 2017 Elsevier Inc. All rights reserved.)

Although too small to be seen with the human eye, atmospheric particulate matter has major impacts on the world around us, from our health to global climate. Understanding the sources, properties, and transformations of these particles in the atmosphere is among the major challenges in air quality and climate research today. Significant progress has been made over the past two decades in understanding atmospheric aerosol chemistry and its connections to climate. Advances in technology for characterizing aerosol chemical composition and physical properties have enabled rapid discovery in this area. This article reviews fundamental concepts and recent developments surrounding ambient aerosols, their chemical composition and sources, light-absorbing aerosols, aerosols and cloud formation, and aerosol-based solar radiation management (also known as solar geoengineering).

To investigate the size distributions of chemical compositions and sources of particulate matter (PM) at ground level and from the urban canopy, a study was conducted on a 255 m meteorological tower in Tianjin from December 2013 to January 2014. Thirteen sets of 8 size-segregated particles were collected with cascade impactor at 10 m and 220 m. Twelve components of particles, including water-soluble inorganic ions and carbonaceous species, were analyzed and used to apportion the sources of PM with positive matrix factorization. Our results indicated that the concentrations, size distributions of chemical compositions and sources of PM at the urban canopy were affected by regional transport due to a stable layer approximately 200 m and higher wind speed at 220 m. The concentrations of PM, Cl - and elemental carbon (EC) in fine particles at 10 m were higher than that at 220 m, while the reverse was true for NO 3 - and SO 4 2- . The concentrations of Na + , Ca 2+ , Mg 2+ , Cl - and EC in coarse particles at 10 m were higher than that at 220 m. The size distributions of major primary species, such as Cl - , Na + , Ca 2+ , Mg 2+ and EC, were similar at two different heights, indicating that there were common and dominant sources. The peaks of SO 4 and organic carbon (OC), which were partly secondary generated species, shifted slightly to the smaller particles at 220 m, indicating that there was a different formation mechanism. Industrial pollution and coal combustion, re-suspended dust and marine salt, traffic emissions and transport, and secondary inorganic aerosols were the major sources of PM at both heights. With the increase in vertical height, the influence of traffic emissions, re-suspended dust and biomass burning on PM weakened, but the characteristics of regional transport from Hebei Province and Beijing gradually become obvious.2- , NH 4 + , NO 3 - and organic carbon (OC), which were partly secondary generated species, shifted slightly to the smaller particles at 220 m, indicating that there was a different formation mechanism. Industrial pollution and coal combustion, re-suspended dust and marine salt, traffic emissions and transport, and secondary inorganic aerosols were the major sources of PM at both heights. With the increase in vertical height, the influence of traffic emissions, re-suspended dust and biomass burning on PM weakened, but the characteristics of regional transport from Hebei Province and Beijing gradually become obvious., (Copyright © 2016 Elsevier Ltd. All rights reserved.)

Biomass burning and primary biological aerosol particles (PBAPs) represent important primary sources of organic compounds in the atmosphere. These particles and compounds are able to affect climate and human health. In the present work, using HPLC-orbitrapMS, we determined the atmospheric concentrations of molecular markers such as anhydrosugars and phenolic compounds that are specific for biomass burning, as well as the concentrations of sugars, alcohol sugars and d- and l-amino acids (D-AAs and L-AAs) for studying PBAPs in Belgrade (Serbia) aerosols collected in September-December 2008. In these samples, high levels of all these biomarkers were observed in October. Relative percentages of vanillic (V), syringic compounds (S) and p-coumaric acid (PA), as well as levoglucosan/mannosan (L/M) ratios, helped us discriminate between open fire events and wood combustion for domestic heating during the winter. L-AAs and D-AAs (1% of the total) were observed in Belgrade aerosols mainly in September-October. During open fire events, mean D-AA/L-AA (D/L) ratio values of aspartic acid, threonine, phenylalanine, alanine were significantly higher than mean D/L values of samples unaffected by open fire. High levels of AAs were observed for open biomass burning events. Thanks to four different statistical approaches, we demonstrated that Belgrade aerosols are affected by five sources: a natural source, a source related to fungi spores and degraded material and three other sources linked to biomass burning: biomass combustion in open fields, the combustion of grass and agricultural waste and the combustion of biomass in stoves and industrial plants. The approach employed in this work, involving the determination of specific organic tracers and statistical analysis, proved useful to discriminate among different types of biomass burning events., (Copyright © 2016 Elsevier B.V. All rights reserved.)

The magnitude of aerosol radiative forcing caused by anthropogenic emissions depends on the baseline state of the atmosphere under pristine preindustrial conditions. Measurements show that particle formation in atmospheric conditions can occur solely from biogenic vapors. Here, we evaluate the potential effect of this source of particles on preindustrial cloud condensation nuclei (CCN) concentrations and aerosol-cloud radiative forcing over the industrial period. Model simulations show that the pure biogenic particle formation mechanism has a much larger relative effect on CCN concentrations in the preindustrial atmosphere than in the present atmosphere because of the lower aerosol concentrations. Consequently, preindustrial cloud albedo is increased more than under present day conditions, and therefore the cooling forcing of anthropogenic aerosols is reduced. The mechanism increases CCN concentrations by 20-100% over a large fraction of the preindustrial lower atmosphere, and the magnitude of annual global mean radiative forcing caused by changes of cloud albedo since 1750 is reduced by [Formula: see text] (27%) to [Formula: see text] Model uncertainties, relatively slow formation rates, and limited available ambient measurements make it difficult to establish the significance of a mechanism that has its dominant effect under preindustrial conditions. Our simulations predict more particle formation in the Amazon than is observed. However, the first observation of pure organic nucleation has now been reported for the free troposphere. Given the potentially significant effect on anthropogenic forcing, effort should be made to better understand such naturally driven aerosol processes., Competing Interests: The authors declare no conflict of interest.

Metaproteomic analysis of air particulate matter provides information about the abundance and properties of bioaerosols in the atmosphere and their influence on climate and public health. We developed and applied efficient methods for the extraction and analysis of proteins from glass fiber filter samples of total, coarse, and fine particulate matter. Size exclusion chromatography was applied to remove matrix components, and sodium dodecyl sulfate polyacrylamide gel electrophoresis (SDS-PAGE) was applied for protein fractionation according to molecular size, followed by in-gel digestion and LC-MS/MS analysis of peptides using a hybrid Quadrupole-Orbitrap MS. Maxquant software and the Swiss-Prot database were used for protein identification. In samples collected at a suburban location in central Europe, we found proteins that originated mainly from plants, fungi, and bacteria, which constitute a major fraction of primary biological aerosol particles (PBAP) in the atmosphere. Allergenic proteins were found in coarse and fine particle samples, and indications for atmospheric degradation of proteins were observed. Graphical abstract Workflow for the metaproteomic analysis of atmospheric aerosol samples., Competing Interests: The authors declare that they have no competing interests. Ethical approval This article does not contain any research with human participants or animals. All authors of this manuscript were informed and agreed for submission.

Atmospheric iron aerosol is a bioavailable essential nutrient playing a role in oceanic productivity. Using aerosol time-of-flight mass spectrometry (ATOFMS), the particle size (0.3-1.5 μm), chemical composition and mixing state of Fe-containing particles collected at two European urban sites (London and Barcelona) were characterized. Out of the six particle types accounting for the entire Fe-aerosol population, that arising from long-range transport (LRT) of fine Fe-containing particles (Fe-LRT, 54-82% across the two sites) was predominant. This particle type was found to be internally mixed with nitrate and not with sulfate, and likely mostly associated with urban traffic activities. This is in profound contrast with previous studies carried out in Asia, where the majority of iron-containing particles are mixed with sulfate and are of coal combustion origin. Other minor fine iron aerosol sources included mineral dust (8-11%), traffic brake wear material (1-17%), shipping/oil (1-6%), biomass combustion (4-13%) and vegetative debris (1-3%). Overall, relative to anthropogenic Asian Fe-sulfate dust, anthropogenic European dust internally mixed with additional key nutrients such as nitrate is likely to play a different role in ocean global biogeochemical cycles.

During 11-18 September 2014, the size-resolved aerosol Cloud Condensation Nuclei (CCN) activity and mixing state were measured using Cloud Condensation Nuclei Counter (CCNC), Aerosol Particle Mass (APM) and Scanning Mobility Particle Sizer (SMPS). The results showed that aerosols mainly existed as an internal mixture. For 76, 111, 138 and 181 nm particles, black carbon (BC) accounted for 5.4%, 10%, l0.7% and 6.7% of the particle mass, but as high as 51%, 57%, 70% and 59% of the particle number concentrations, respectively, suggesting that BC was a type of important condensation nuclei in the atmosphere and made significant contributions to particle numbers. The occasionally observed external mixtures were mainly present in 111 and 138 nm particles. The critical supersaturation was 0.25%, 0.13%, 0.06% and 0.015% for 76, 111, 138 and 181 nm particles, respectively. Precipitation and haze had significant effects on the particle CCN activity. The hygroscopicity parameter K was 0.37, 0.29 and 0.39 in rainy, clear and hazy days, respectively. Particle density and CCN activity were impacted by chemical compositions. Compared with clear days, higher contents of inorganic salts and lower contents of organics were found on hazy days, accompanied by lower particle density and higher CCN activity.

Atmospheric aerosol particles of primary or secondary, biogenic or anthropogenic origin are highly complex samples of changing composition in time and space. To assess their effects on climate or human health, the size-dependent chemical composition of these ubiquitous atmospheric constituents must be known. The development of novel analytical methods has enabled more detailed characterization of the organic composition of aerosols. This review gives an overview of the methods used in the chemical characterization of atmospheric aerosol particles, with a focus on mass-spectrometry techniques for organic compounds, either alone or in combination with chromatographic separation. Off-line, on-site, and on-line methods are covered, and the advantages and limitations of the different methods are discussed. The main emphasis is on methods used for detailed characterization of the composition of the organic compounds in aerosol particles. We address and summarize the current state of analytical methods used in aerosol research and discuss the importance of developing novel sampling strategies and analytical instrumentation. Graphical Abstract Challenges in the atmospheric aerosol analytics.

To investigate the pollution characteristics of water soluble ions in fine atmospheric particles in Yangtze River Delta during the haze period from 18th to 24th Jan 2013, a joint sampling campaign using Andersen sampler was conducted at five cities (including Nanjing, Suzhou, Hangzhou, Lin'an and Ningbo). The analysis of size distribution of these ionic species coupled with the local meteorological conditions may shed some insightful light on the haze formation mechanism in this region. The result has shown: firstly, during the observation period, when Yangtze River Delta located at high pressure or in the front of high pressure, and has a large pressure gradient, the lower atmosphere has a significant airflow divergence in favor of pollutant dispersion; while located in weak low pressure and weak high pressure, the equalizing pressure field is not favorable for pollutant dispersion, especially accompanied with lower atmosphere convergence airflow. Secondly, during the hazy period, the concentration of fine particles and total water-soluble inorganic ions (TWSS) has increased dramatically; the increasing proportions of TWSS in fine particles are: Hangzhou 0. 9%, Lin'an 4. 2%, Nanjing 8. 1%. The particle size of secondary ions of SO(4)2-, NO3-, NH4+ complies fine mode(particle size <2. 1 µm), whose peaks migrates from 0. 43-0. 65 µm to 0. 65-1. 1 µm during the observation period, the peak of particle size of Ca2+ , Mg2+ appears at 4.7-5. 8 µm, while the ions of Na+, Cl-, K+ show a bimodal distribution. Moreover, secondary inorganic ions play a significant role in the formation of haze pollution, where the concentrations of secondary inorganic ions of NH4+, SO2- and NO3 have higher increasing rates; their relative proportions of increasing from each monitoring points are: Hangzhou 3%, Lin'an 55% and Nanjing 64.9%. Finally, SO(4)2- has the highest mass contribution to SNA, up to 45% ; also, the NO-/SO- ratios in each monitoring points are always higher than a fair 0. 5, which could indicate the significant contribution of mobile source towards this particle pollution.

Atmospheric aerosols have important impacts on human health, the environment and the climate system. Micro Pulse Lidar (MPL) is a new effective tool for detecting atmosphere aerosol horizontal distribution. And the extinction coefficient inversion and error analysis are important aspects of data processing. In order to detect the horizontal distribution of atmospheric aerosol near the ground, slope and Fernald algorithms were both used to invert horizontal MPL data and then the results were compared. The error analysis showed that the error of the slope algorithm and Fernald algorithm were mainly from theoretical model and some assumptions respectively. Though there still some problems exist in those two horizontal extinction coefficient inversions, they can present the spatial and temporal distribution of aerosol particles accurately, and the correlations with the forward-scattering visibility sensor are both high with the value of 95%. Furthermore relatively speaking, Fernald algorithm is more suitable for the inversion of horizontal extinction coefficient.

Multiphase reactions of OH radicals are among the most important pathways of chemical aging of organic aerosols in the atmosphere. Reactive uptake of OH by organic compounds has been observed in a number of studies, but the kinetics of mass transport and chemical reaction are still not fully understood. Here we apply the kinetic multilayer model of gas-particle interactions (KM-GAP) to experimental data from OH exposure studies of levoglucosan and abietic acid, which serve as surrogates and molecular markers of biomass burning aerosol (BBA). The model accounts for gas-phase diffusion within a cylindrical coated-wall flow tube, reversible adsorption of OH, surface-bulk exchange, bulk diffusion, and chemical reactions at the surface and in the bulk of the condensed phase. The nonlinear dependence of OH uptake coefficients on reactant concentrations and time can be reproduced by KM-GAP. We find that the bulk diffusion coefficient of the organic molecules is approximately 10(-16) cm(2) s(-1), reflecting an amorphous semisolid state of the organic substrates. The OH uptake is governed by reaction at or near the surface and can be kinetically limited by surface-bulk exchange or bulk diffusion of the organic reactants. Estimates of the chemical half-life of levoglucosan in 200 nm particles in a biomass burning plume increase from 1 day at high relative humidity to 1 week under dry conditions. In BBA particles transported to the free troposphere, the chemical half-life of levoglucosan can exceed 1 month due to slow bulk diffusion in a glassy matrix at low temperature.

A combination of Raman microscopy and diffuse reflectance Fourier transform infrared spectroscopy (FTIR) has been used for the characterization of fine mode (<1 μm) tropospheric aerosols. Peak fitting was used to identify five overlapping bands in the Raman spectra. These bands have been identified as due to combustion generated carbon soot as well as large molecular organic carbon species. The fwhm of the D band at 1400 cm(-1) as well as the ratio of intensities of the D3 band at 1550 cm(-1) to the G band at 1580 cm(-1) can serve as a measure of the aerosol organic carbon content. Raman microscopy combined with spectral mapping capabilities was used to investigate the composition of the fine mode aerosols at the particle level, allowing for the direct determination of aerosol mixing state. Results showed that the fine aerosols were predominately internally mixed particles composed of carbon soot coated with molecular organic carbon species. Characterization of the aerosols by diffuse reflectance FTIR showed that the major organic carbon species were polycarboxylates and polysaccharide-like species typical of humic-like substances (HULIS).

Kosa (Asian dust) is a well-known weather phenomenon in which aerosols are carried by the westerly winds from inland China to East Asia. Recently, the frequency of this phenomenon and the extent of damage caused have been increasing. The airborne bacteria within Kosa are called Kosa bioaerosols. Kosa bioaerosols have affected ecosystems, human health and agricultural productivity in downwind areas. In order to develop a new and useful bacterial source and to identify the source region of Kosa bioaerosols, sampling, isolation, identification, measurement of ultraviolet (UV) radiation tolerance and experimental simulation of UV radiation conditions were performed during Kosa bioaerosol transportation. We sampled these bioaerosols using a Cessna 404 airplane and a bioaerosol sampler at an altitude of approximately 2900 m over the Noto Peninsula on March 27, 2010. The bioaerosol particles were isolated and identified as Bacillus sp. BASZHR 1001. The results of the UV irradiation experiment showed that the UV radiation tolerance of Kosa bioaerosol bacteria was very high compared with that of a soil bacterium. Moreover, the UV radiation tolerance of Kosa bioaerosol spores was higher than that of soil bacterial spores. This suggested that Kosa bioaerosols are transported across the atmosphere as living spores. Similarly, by the experimental simulation of UV radiation conditions, the limited source region of this Kosa bioaerosol was found to be southern Russia and there was a possibility of transport from the Kosa source area., (Copyright © 2014 The Society for Biotechnology, Japan. Published by Elsevier B.V. All rights reserved.)

Secondary organic aerosol (SOA) formation from in-use vehicle emissions was investigated using a potential aerosol mass (PAM) flow reactor deployed in a highway tunnel in Pittsburgh, Pennsylvania. Experiments consisted of passing exhaust-dominated tunnel air through a PAM reactor over integrated hydroxyl radical (OH) exposures ranging from ∼ 0.3 to 9.3 days of equivalent atmospheric oxidation. Experiments were performed during heavy traffic periods when the fleet was at least 80% light-duty gasoline vehicles on a fuel-consumption basis. The peak SOA production occurred after 2-3 days of equivalent atmospheric oxidation. Additional OH exposure decreased the SOA production presumably due to a shift from functionalization to fragmentation dominated reaction mechanisms. Photo-oxidation also produced substantial ammonium nitrate, often exceeding the mass of SOA. Analysis with an SOA model highlight that unspeciated organics (i.e., unresolved complex mixture) are a very important class of precursors and that multigenerational processing of both gases and particles is important at longer time scales. The chemical evolution of the organic aerosol inside the PAM reactor appears to be similar to that observed in the atmosphere. The mass spectrum of the unoxidized primary organic aerosol closely resembles ambient hydrocarbon-like organic aerosol (HOA). After aging the exhaust equivalent to a few hours of atmospheric oxidation, the organic aerosol most closely resembles semivolatile oxygenated organic aerosol (SV-OOA) and then low-volatility organic aerosol (LV-OOA) at higher OH exposures. Scaling the data suggests that mobile sources contribute ∼ 2.9 ± 1.6 Tg SOA yr(-1) in the United States, which is a factor of 6 greater than all mobile source particulate matter emissions reported by the National Emissions Inventory. This highlights the important contribution of SOA formation from vehicle exhaust to ambient particulate matter concentrations in urban areas.

To know the influence of different weather conditions on the concentration of metal elements in aerosols in the coastal region, total suspended particles (TSP) samples were collected from April to May 2012, and August 2012 to March 2013 in the Qingdao coastal region, and common trace metals were analyzed by using Inductively Coupled Plasma-Mass Spectrometry (ICP-MS) and Inductively Coupled Plasma-Atomic Emission Spectrometry (ICP-AES). The results showed that Al, Ca, Fe, Na, K and Mg were the dominant metal elements in TSP, and the sum of the six elements accounted for 94.2% of the sum of all metals. TSP and metal elements had significant monthly variations, Fe, Al, K, Ca, Mg, Zn, Ba, Mn, Ti, Sr and Li had the highest concentration in November and January, while Be, Sc, Co, Ni and Cr showed the highest value in January. Na had the highest concentration in August, November and February, and the lowest in December. Pb had the highest concentration in January and February, and the lowest in August and December. Enrichment factors indicated that Be, Co, Al, Ca, Fe, K, Mg, Mn, Sr and Ti were mainly affected by natural sources; Li, Cr, Ni, Zn, Ba and Na were affected by natural sources and part of anthropogenic sources; Pb was mainly from anthropogenic sources. Different weather conditions had great impact on TSP and metal elements concentrations, all the measured metals had the highest concentrations in smog except Ti. Compared with the sunny day, the concentration of atmospheric particulate Ti decreased, while the other elements increased by 1 to 4 times in smog. Li, Be, Cr, Ni, Al, Fe, Mg and Mn had little variation in concentration in foggy day, and the concentration of Pb and Na increased considerably. The concentration of Co, Ca and Ti reduced obviously in fog. Except for Cr, Co and Ti, the other elements increased by 1 to 3 times in haze. Most of the elements had the minimal enrichment factors in sunny day, while the other had the maximal enrichment factor in foggy day. Enrichment factors of Ni, Zn, Ba, K, Na, Pb and Sr varied in the order of sunny day < haze day < smog day

The significant effect of anthropogenic pollutants transportation on the physical and optical properties of regional background atmospheric aerosol was studied by using ground-based and satellite remote sensing data obtained at the atmospheric background station (Shangdianzi, Beijing) of North China during October 1 to 15 in 2011. The aerosol mass concentration and reactive gases concentration increased obviously during periods of October 4-5, October 7-9, and October 11-12. Comparing with the background period of October 1-3, volume concentration increased by a factor of 3-6 for reactive gases such as NO(x), and CO, and a factor of 10-20 for SO2. Mass concentration of PM2.5 was about 200 microg x m(-3) on October 9. During haze period, the AOD at 500 nm varied between 0.60 to 1.00. The single scattering albedo (SSA) was lower than 0.88. And the black carbon concentration increased 4-8 times, which suggested the aerosol absorption was very strong during this pollution episode. The absorption of aerosol particles could cause 100-400 W x m(-2) increase of atmospheric radiation. The surface radiation decreased by about 100-300 W x m(-2) due to the aerosol scattering and absorption. This could cause higher stability of atmosphere, which will significantly affect the cloud and precipitation, and thus the regional weather and climate.

Aerosols affect the climate directly through absorption and reflection of sunlight back to space and indirectly by acting as cloud condensation nuclei. This paper is based on more than three decades of satellite data (1979-1994 and 1996-2012) from total ozone mapping spectrometer (TOMS) and ozone monitoring instrument (OMI), which have provided measurements of backscattered radiances in the wavelength range from 331 to 380 nm. These data have been used to determine the aerosol climatology and to investigate the influence of the aerosol index (AI) on the ultraviolet index (UVI) in coastal land areas in Serrekunda (13.28°N, 16.34°W), The Gambia, and Dar-es-Salaam (6.8°S, 39.26°E), Tanzania, as well as in inland areas in Kampala (0.19°N, 32.34°E), Uganda. Heavy aerosol loadings were found to occur in the dry seasons at all three locations. To reduce the influence of clouds, we disregarded TOMS and OMI data for days during which the UV reflectivity was larger than 9% and investigated the correlation of the AI with the UVI for the remaining days at the three locations. We found a high correlation coefficient of 0.82 for Serrekunda, but poor correlation for Kampala and Dar-es-Salaam. The average AI for Serrekunda was found to be about three times higher than that for Kampala or Dar-es-Salaam, and a positive trend was found for the AI in Kampala and Dar-es-Salaam, whereas a negative trend was found for the AI in Serrekunda.

By using a charge-coupled device (CCD) as the detector, side-scatter lidar has great potential applications in the near range atmospheric detection. A new inversion method is proposed for CCD side-scatter lidar (Clidar) to retrieve aerosol phase function and vertical backscattering coefficient. Case studies show the retrieved results from Clidar are in good agreements with those obtained from other instruments. It indicates that the new proposed inversion method is reliable and feasible and that the Clidar is practicable.

Retrieval of aerosol loading in vertical atmospheric columns is a common product of satellite and ground instruments that measure spectral extinction of solar radiation throughout the entire atmosphere. Here we study ground hyperspectral imaging of artificial light sources as a complementary method for retrieving fine aerosol concentrations along quazi-horizontal ambient open paths. Previously, we reported hyperspectral measurements of the aerosol optical thickness in the 500-900 nm range over urban-scale distances (180 m to 4 km), measuring the extinction of radiation emitted from a halogen source. Here we confirm in a laboratory-setup the basic premise that different accumulation-size aerosols generate distinct hyperspectral signatures in this spectral range. Measured hyperspectral attenuation signatures of fine aerosols were comparable to calculated Mie scattering signatures, suggesting that modal aerosol concentrations can be retrieved. A genetic algorithm was adapted to estimate the aerosol modal concentrations from its hyperspectral extinction signature. Retrievals of aerosol concentrations from measured and synthetic hyperspectral signatures indicated a robust algorithm, with an expected retrieval error of 0.2-22% for typical ambient concentrations along an urban-scale open path. The retrieval accuracy was found to depend on the relative aerosol modal concentrations, especially when there is a substantial overlap between the modal spectral signatures.

Aerosols affect climate, health and aviation. Currently, their retrieval assumes a plane-parallel atmosphere and solely vertical radiative transfer. We propose a principle to estimate the aerosol distribution as it really is: a three dimensional (3D) volume. The principle is a type of tomography. The process involves wide angle integral imaging of the sky on a very large scale. The imaging can use an array of cameras in visible light. We formulate an image formation model based on 3D radiative transfer. Model inversion is done using optimization methods, exploiting a closed-form gradient which we derive for the model-fit cost function. The tomography model is distinct, as the radiation source is unidirectional and uncontrolled, while off-axis scattering dominates the images.

Measurements of activity concentrations of (131)I; (129 m)Te, (132)Te, (134)Cs and; (136)Cs, (137)Cs in aerosol were carried out in daily samples after the Fukushima accident during the period of March-April, 2011 in Vilnius. The maximum activity concentrations of (131)I and (137)Cs were found to be 3,700 μBq m(-3) and 1,040 μBq m(-3), respectively. Variations in activity ratios of (132)Te/(129 m)Te and (137)Cs/(136)Cs observed after the accident were explained by the decay of the short-lived isotopes, while those in (134)Cs/(137)Cs by the dilution effect of the Chernobyl-derived (137)Cs. It was found that different behaviours of highly volatile (131)I and (137)Cs resulted in enrichment of ground level aerosol particles by (131)I with respect to (137)Cs. Simulated activity concentrations of (137)Cs attached to aerosol particles for the Vilnius site reasonably agreed with measured activities in aerosol samples during the Fukushima accident., (Copyright © 2013 Elsevier Ltd. All rights reserved.)

Aerosol optical properties over a southern sub-tropical site Skukuza, South Africa were studied to determine the variability of the aerosol characteristics using CIMEL Sunphotometer data as part of the AErosol RObotic NETwork (AERONET) from December 2005 to November 2006. Aerosol optical depth (AOD), Ångström exponent (α), and columnar water vapor (CWV) data were collected, analyzed, and compiled. Participating in this network provided a unique opportunity for understanding the sources of aerosols affecting the atmosphere of South Africa (SA) and the regional radiation budget. The meteorological patterns significantly (p<0.05) influenced the amount and size distribution of the aerosols. Results showed that seasonal variation of AOD at 500 nm (AOD500) over the observation site were characterized by low values (0.10-0.13) in autumn, moderate values (0.14-0.16) in summer and winter seasons, and high to very high values (0.18-0.40) during the spring, with an overall mean value of 0.18±0.12. Ångström exponent α(440-870), varied from 0.5 to 2.89, with significant (p<0.0001) seasonal variability. CWV showed a strong annual cycle with maximum values in the summer and autumn seasons. The relationship between AOD, Ångström exponent (α), and CWV showed a strong dependence (p<0.0001) of α on AOD and CWV, while there was no significant correlation between AOD and CWV. Investigation of the adequacy of the simple use of the spectral AOD and Ångström exponent data was used in deriving the curvature (a2) showed to obtain information for determining the aerosol-particle size. The negative a2 values are characterized by aerosol-size dominated by fine-mode (0.1-1 μm), while the positive curvatures indicate abundance of coarse particles (>1 μm). Trajectory cluster analyses revealed that the air masses during the autumn and winter seasons have longer advection pathways, passing over the ocean and continent. This is reflected in the aerosol properties that are derived from the ocean, desert, and anthropogenic activities that include biomass burning and industrial pollution., (Copyright © 2013 Elsevier B.V. All rights reserved.)

Organic aerosols are ubiquitous in the atmosphere and play a central role in climate, air quality, and public health. The aerosol size distribution is key in determining its optical properties and cloud condensation nucleus activity. The dominant portion of organic aerosol is formed through gas-phase oxidation of volatile organic compounds, so-called secondary organic aerosols (SOAs). Typical experimental measurements of SOA formation include total SOA mass and atomic oxygen-to-carbon ratio. These measurements, alone, are generally insufficient to reveal the extent to which condensed-phase reactions occur in conjunction with the multigeneration gas-phase photooxidation. Combining laboratory chamber experiments and kinetic gas-particle modeling for the dodecane SOA system, here we show that the presence of particle-phase chemistry is reflected in the evolution of the SOA size distribution as well as its mass concentration. Particle-phase reactions are predicted to occur mainly at the particle surface, and the reaction products contribute more than half of the SOA mass. Chamber photooxidation with a midexperiment aldehyde injection confirms that heterogeneous reaction of aldehydes with organic hydroperoxides forming peroxyhemiacetals can lead to a large increase in SOA mass. Although experiments need to be conducted with other SOA precursor hydrocarbons, current results demonstrate coupling between particle-phase chemistry and size distribution dynamics in the formation of SOAs, thereby opening up an avenue for analysis of the SOA formation process.

Aerosol was collected with Anderson cascade sampler at three altitudes of the Mount Huang in the summer 2011. Samples were analyzed by the ion chromatography (IC, Metrohm). The results showed that the mean mass concentrations of all the ions were 13.21 microg x m(-1), 10.94 microg x m(-3), 9.97 microg x m(-3), at the foot, mid height and the summit of the mountain, respectively. The mass concentration of water-soluble components of aerosol decreased with altitude. The major anion and cation of aerosols were SO4(2-) and NH4+, respectively. The descending order of mass concentration of major ionic species was: SO4(2-) > NH4+ > Ca2+ > NO3- and NH4+ account for about 75% of total ionic concentrations of PM2.1 in three sampling sites. The concentration of SO4(2-) and NH4+ decreased conspicuously with altitude. The major cation and anion of coarse mode particles were Ca2+ and NO3-, respectively. The slope of the linear regression line between anion and cation of PM10 and PM2.1 approximates 1, indicating acid-base balance in aerosol particles. Aerosols over the region Mount Huang were influenced by anthropogenic source of surrounding areas to a certain extent. The result also suggested that the correlation between NH4+ and SO4(2-) was 0. 98 and these ions predominantly existed in the form of (NH4)2SO4 and NH4HSO4. Backward trajectory analysis revealed that the air mass was originated from southern coastal regions, the East China Sea, the Yellow Sea and the northern China. Due to the northern air masses go through heavily polluted areas, concentrations of water-soluble ions in these air masses were higher than that of other air masses. The concentration of K+ in northern air mass was several times higher than that in southwestern air mass.

In order to model the properties and chemical composition of secondary organic aerosol (SOA), estimated physical property data for many thousands of organic compounds are required. Seven methods for estimating liquid density are assessed against experimental data for a test set of 56 multifunctional organic compounds. The group contribution method of Schroeder coupled with the Rackett equation using critical properties by Nannoolal was found to give the best liquid density values for this test set. During this work some problems with the representation of certain groups (aromatic amines and phenols) within the critical property estimation methods were identified, highlighting the importance (and difficulties) of deriving the parameters of group contribution methods from good quality experimental data. A selection of the estimation methods are applied to the 2742 compounds of an atmospheric chemistry mechanism, which showed that they provided consistent liquid density values for compounds with such atmospherically important (but poorly studied) functional groups as hydroperoxide, peroxide, peroxyacid, and PAN. Estimated liquid density values are also presented for a selection of compounds predicted to be important in atmospheric SOA. Hygroscopic growth factor (a property expected to depend on liquid density) has been calculated for a wide range of particle compositions. A low sensitivity of the growth factor to liquid density was found, and a single density value of 1350 kg·m(-3) could be used for all multicomponent SOA in the calculation of growth factors for comparison with experimentally measured values in the laboratory or the field without incurring significant error.

Isoprene is a substantial contributor to the global secondary organic aerosol (SOA) burden, with implications for public health and the climate system. The mechanism by which isoprene-derived SOA is formed and the influence of environmental conditions, however, remain unclear. We present evidence from controlled smog chamber experiments and field measurements that in the presence of high levels of nitrogen oxides (NO(x) = NO + NO2) typical of urban atmospheres, 2-methyloxirane-2-carboxylic acid (methacrylic acid epoxide, MAE) is a precursor to known isoprene-derived SOA tracers, and ultimately to SOA. We propose that MAE arises from decomposition of the OH adduct of methacryloylperoxynitrate (MPAN). This hypothesis is supported by the similarity of SOA constituents derived from MAE to those from photooxidation of isoprene, methacrolein, and MPAN under high-NOx conditions. Strong support is further derived from computational chemistry calculations and Community Multiscale Air Quality model simulations, yielding predictions consistent with field observations. Field measurements taken in Chapel Hill, North Carolina, considered along with the modeling results indicate the atmospheric significance and relevance of MAE chemistry across the United States, especially in urban areas heavily impacted by isoprene emissions. Identification of MAE implies a major role of atmospheric epoxides in forming SOA from isoprene photooxidation. Updating current atmospheric modeling frameworks with MAE chemistry could improve the way that SOA has been attributed to isoprene based on ambient tracer measurements, and lead to SOA parameterizations that better capture the dependency of yield on NO(x).

The pollution of particulate matter was serious in Beijing City from the synchronous observation of particulate matter mass concentration and aerosol optical characteristics in 2009. The annual mean concentrations of PM2.5 and PM10 were (65 +/- 14) microg x m(-3) and (117 +/- 31) microg x m(-3), respectively, which exceeded the national ambient air quality annual standards to be implemented in 2016. There were 35% and 26% days of 2009 that the daily standards were exceeded. There was a significant correlation between fine particulate (PM2.5) and inhalable particle (PM10), with a correlation coefficient (R) of approximately 0.90 (P < 0.001). PM10 contained a large percentage of PM2.5, with an annual percentage of about 61%. The percentage became much higher from spring to winter, while the correlation between PM2.5 and PM10 became much stronger. The annual mean of AOD (500 nm) and Angstrom exponent were (0.55 +/- 0.1) and (1.12 +/- 0.08), respectively. There were significant correlations between PM2.5, PM10 and AOD in the four seasons and the whole year, and the correlation coefficients were greater than or equal to 0.50. Furthermore, the correlation functions and coefficients had seasonal variations. The correlations were more significant in summer and autumn than in spring and winter. The annual correlation could cover up the seasonal systematic differences. The correlations between AOD revised by Mixed Layer Height and PM2.5 PM10 revised by Relative Humidity became stronger, and the exponential correlations were superior to the linear correlations.

Size-segregated aerosol samples were collected using Andersen cascade sampler from Sep. 2009 to Aug. 2010 in Xinglong, a regional atmospheric background station. The water-soluble inorganic ions were analyzed by IC. The result showed that the annual concentrations of the total water-soluble inorganic ions were (89.66 +/- 47.66), (54.44 +/- 34.08) and (44.39 +/- 29.95) microg x m(-3) in TSP, PM2.1 and PM1.1 respectively. SO4(2-), NO3(-), Ca(2) and NH4(+) were the dominant contributors of water-soluble inorganic ions. The total water-soluble inorganic ions in PM2.1 accounted for 61% of TSP. The total water-soluble inorganic ions in PM1.1 accounted for 50% and 82% in TSP and PM2.1, respectively. The seasonal variations of the total water-soluble inorganic ion concentration in TSP, PM2.1 and PM1.1 were the same, following the order of summer > autumn > springs > winter. The mean molar ratio of NH4(+) to SO4(2-) was larger than 2, indicating that NH4(+) was not completely neutralized by SO4(2-). NH4(+) -SO4(2-) and NH4(+) -NO3(-) concentrations were strongly correlated (R2 0.96 and 0.87), indicating that NH4(+) was mainly present as (NH4) 2SO4 and NH4NO3.

Isoprene and monoterpenes are important precursors of secondary organic aerosols (SOA) in continents. However, their contributions to aerosols over oceans are still inconclusive. Here we analyzed SOA tracers from isoprene and monoterpenes in aerosol samples collected over oceans during the Chinese Arctic and Antarctic Research Expeditions. Combined with literature reports elsewhere, we found that the dominant tracers are the oxidation products of isoprene. The concentrations of tracers varied considerably. The mean average values were approximately one order of magnitude higher in the Northern Hemisphere than in the Southern Hemisphere. High values were generally observed in coastal regions. This phenomenon was ascribed to the outflow influence from continental sources. High levels of isoprene could emit from oceans and consequently have a significant impact on marine SOA as inferred from isoprene SOA during phytoplankton blooms, which may abruptly increase up to 95 ng/m³ in the boundary layer over remote oceans.

We investigate mass transfer during the isothermal absorption of atmospheric trace soluble gases by a single droplet whose size is comparable to the molecular mean free path in air at normal conditions. It is assumed that the trace reactant diffuses to the droplet surface and then reacts with the substances inside the droplet according to the first-order rate law. Our analysis applies a flux-matching theory of transport processes in gases and assumes constant thermophysical properties of the gases and liquids. We derive an integral equation of Volterra type for the transient molecular flux density to a liquid droplet and solve it numerically. Numerical calculations are performed for absorption of sulfur dioxide (SO(2)), dinitrogen trioxide (N(2)O(3)), and chlorine (Cl(2)) by liquid nanoaerosols accompanied by chemical dissociation reaction. It is shown that during gas absorption by nanoaerosols, the kinetic effects play a significant role, and neglecting kinetic effects leads to a significant overestimation of the soluble gas flux into a droplet during the entire period of gas absorption.

Purpose: Exploratory data analysis (EDA) is applied in this research to study the behavior of radioactive aerosols present in the surface atmosphere of Granada, using (7)Be as radiotracer. The reason for this study is to reduce the large number of parameters involved in understanding their behavior, given the complexity of the atmosphere., Methods: Aerosol particles were collected weekly in Granada (Spain) over a 5-year period. Low-background gamma spectrometry was used to determine concentrations of (7)Be-aerosol activity. The variables studied were: (7)Be concentration, cosmic ray intensity, temperature, temperature interval, rainfall, relative humidity, and Saharan intrusions. Least significant difference test (LSD), hierarchical cluster analysis (HCA), and principal component analysis (PCA) with varimax rotation have been applied to study the datasets., Results and Discussion: The results of our study reveal that aerosol behavior is represented by two principal components which explain 86.23 % of total variance. Components PC1 and PC2 respectively explain 74.61 and 11.62 % of total variance. PC1 explains the cyclical and seasonal pattern of the samples, while PC2 is related to the production of (7)Be. In addition, PCA and HCA show good distribution of the samples by families with two groups, summer and winter, at the extremes and spring-autumn in the middle. This result corroborates that there are no differences between spring and autumn in the climate of Granada., Conclusions: EDA has been found to be quite useful in studying the behavior of radioactive aerosols in the surface atmosphere of a city with the climate and geographical characteristics of Granada.

The formation of new atmospheric aerosol particles and their subsequent growth have been observed frequently at various locations all over the world. The atmospheric nucleation rate (or formation rate) and growth rate (GR) are key parameters to characterize the phenomenon. Recent progress in measurement techniques enables us to measure atmospheric nucleation at the size (mobility diameter) of 1.5 (±0.4) nm. The detection limit has decreased from 3 to 1 nm within the past 10 years. In this protocol, we describe the procedures for identifying new-particle-formation (NPF) events, and for determining the nucleation, formation and growth rates during such events under atmospheric conditions. We describe the present instrumentation, best practices and other tools used to investigate atmospheric nucleation and NPF at a certain mobility diameter (1.5, 2.0 or 3.0 nm). The key instruments comprise devices capable of measuring the number concentration of the formed nanoparticles and their size, such as a suite of modern condensation particle counters (CPCs) and air ion spectrometers, and devices for characterizing the pre-existing particle number concentration distribution, such as a differential mobility particle sizer (DMPS). We also discuss the reliability of the methods used and requirements for proper measurements and data analysis. The time scale for realizing this procedure is 1 year.

Limitations in current capabilities to constrain aerosols adversely impact atmospheric simulations. Typically, aerosol burdens within models are constrained employing satellite aerosol optical properties, which are not available under cloudy conditions. Here we set the first steps to overcome the long-standing limitation that aerosols cannot be constrained using satellite remote sensing under cloudy conditions. We introduce a unique data assimilation method that uses cloud droplet number (N(d)) retrievals to improve predicted below-cloud aerosol mass and number concentrations. The assimilation, which uses an adjoint aerosol activation parameterization, improves agreement with independent N(d) observations and with in situ aerosol measurements below shallow cumulus clouds. The impacts of a single assimilation on aerosol and cloud forecasts extend beyond 24 h. Unlike previous methods, this technique can directly improve predictions of near-surface fine mode aerosols responsible for human health impacts and low-cloud radiative forcing. Better constrained aerosol distributions will help improve health effects studies, atmospheric emissions estimates, and air-quality, weather, and climate predictions.

To collect comprehensive information on the characteristics and sources of water-soluble ions in the atmospheric aerosol in Qingdao, samples of total suspended particles (TSP) were collected from January to December 2008, and the concentrations of the major water-soluble inorganic ions were analyzed using ion chromatography. The results showed that SO4(2-), NO3-, NH4+ and Cl- were the dominant water-soluble ions in TSP, the sum of the four accounting for 86.9% of water-soluble ions in mass concentration. TSP and water-soluble inorganic ions showed obvious seasonal variations and there were a variety of sources. The mass concentrations of Na+, NH4+, Ca2+, F- and Mg2+ were highest in winter and lowest in summer. The concentrations of K+ and PO4(3-) were highest in autumn and lowest in summer. NO3-, Cl- and SO4(2-) concentrations had the highest values in spring, winter, and spring, respectively. Different weather conditions had great influence on the concentrations of TSP and water-soluble ions. The mass concentrations of TSP were highest in dust weather followed by haze, smog, fog and sunny days. The average mass concentrations of Na+ , Mg2+, Ca2+, F- , Cl- and PO4(3-) were highest in smog days while the other ions in haze days.

Aerosol radiative effects over two environmentally distinct locations, Kanpur (urban site) and Gandhi College (rural location) in the Indo-Gangetic plain (IGP), a regional aerosol hot spot, utilizing the measured optical and physical characteristics of aerosols, an aerosol optical properties model and a radiative transfer model, are examined. Shortwave aerosol radiative forcing (ARF) at the top of the atmosphere (TOA) is < -12 W m( - 2) over Kanpur and Gandhi College. ARF at the surface is ≥ -30 W m( - 2). Atmospheric warming is maximum during premonsoon (>30 W m( - 2)). Shortwave atmospheric heating due to aerosols is >0.4 K/day over IGP and peaks during premonsoon at >0.6 K/day due to lower single scattering albedo (SSA) and higher surface albedo. TOA forcing is always less negative over Kanpur when compared to Gandhi College due to lower surface albedo except in postmonsoon owing to higher SSA. This happens as TOA forcing depends on SSA and surface albedo in addition to aerosol optical depth. The magnitude of longwave forcing and atmospheric cooling in an absolute sense is significantly small and contributes only about 20% or less to the net (shortwave + longwave) forcing. Aerosol radiative effects over these two locations, despite differences in aerosol characteristics, are similar, thus confirming that aerosols and their radiative influence get transported due to circulation. ARF over Kanpur and Gandhi College is an order of magnitude higher when compared to greenhouse gas forcing. A large reduction in surface reaching solar irradiance accompanied by large atmospheric warming can have implications on precipitation and hydrological cycle, and these aerosol radiative effects should be included while performing regional-scale aerosol climate assessments.

The eastward transport of aerosols exported from mainland Asia strongly influences air quality in the Japanese archipelago. The bulk of the inhalable particulate matter (PM(10)) in these intrusions comprises either natural, desert-derived minerals (mostly supermicron silicates) or anthropogenic pollutants (mostly submicron sulphates), in various states of mixing. We analyse PM(10) collected in Kumamoto, SW Japan, during three contrasting types of aerosol intrusions, the first being dominated by desert PM which became increasingly mixed with anthropogenic components as time progressed, the second being a relatively minor event mixing fine, distal desert PM with anthropogenic materials, and the third being dominated by anthropogenic pollutants. Whereas the chemistry of the natural mineral component is characterised by "crustal" elements (Si, Al, Fe, Mg, K, Li, P, Sc, V, Rb, Sr, Zr, Th, lanthanoids), the anthropogenic component is rich in secondary inorganic compounds and more toxic metallic elements (NH(4)(+), SO(4)(2-), As, Pb, Cd, Cu, Zn, Sn, Bi, Sb, and Ge). Some desert-dust (Kosa) intrusions are more calcareous than others, implicating geologically different source areas, and contain enhanced levels of NO(3)(-), probably as supermicron Ca(NO(3))(2) particles produced by chemical reaction between NOx pollutants (mostly from industry and traffic) and carbonate during atmospheric transport. The overall trace element chemistry of aerosol intrusions into Kumamoto shows low V/Rb, low NO(3)(-)/SO(4)(2-), enhanced As levels, and unfractionated La/Ce values, which are all consistent with anthropogenic sources including coal emissions rather than those derived from the refining and combustion of oil fractionates. Geographically dispersed, residual sulphatic plumes of this nature mix with local traffic (revealed by OC and EC concentrations) and industrial emissions and dissipate only slowly, due to the dominance of submicron accumulation mode PM which is atmospherically persistent, and raise questions over the chronic health effects of breathing finely respirable sulphatic aerosol containing enhanced amounts of toxic metals., (Copyright © 2012 Elsevier B.V. All rights reserved.)

Integrated PM2.5 aerosol samples were collected at Baima Spring Scenic Area, a forest site of Yaan, Sichuan Province, during the summer of 2010. Organic speciation including isoprene oxidation products (2-methyltetrols, C5-alkene trols, 2-methylyceric acid), alpha-/beta-pinene oxidation products (norpinic acid, 3-hydroxyglutaric acid, 3-methy-1,2,3-butanetricarboxylic acid), and small molecular carboxylic acid (malic acid, 2-hydroxyglutaric acid) were analyzed. The generation mechanisms of SOA as well as their influencing factors were particularly discussed. Results show that average concentrations of 2-methyltetrols, C5-alkene triols, 2-methyglyceric acid, norpinic acid, 3-hydroxyglutaric acid and 3-methy-1,2,3-butanetricarboxylic acid are 63.3, 45.0, 4.4, 4.1, 5.0, 5.3 ng x m(-3) respectively, of 24-hour lapse samples. SOA compounds are consistent with higher concentrations in the day than during the night only except for norpinic acid. Relatively high level of biogenic SOA at the study area is concerned with many environmental factors, i. e. local abundant vegetations, warm and humid climate, sunken valley topography, the atmospheric pollution state, etc.

Feature of aerosol particle number concentration, condition and impact factor of new particle formation (NPF) were investigated in Nanjing during summer. In this study, aerosol particle number concentration and gaseous pollutants (O3, SO2 and NO2) measurements were carried out by Wide-Range Particle Spectrometer (WPS) and Differential Optical Absorption Spectroscopy (DOAS) in July 2010. Combining with observations from Automatic Weather Station and Backward Trajectory Simulation, the condition and impact factor of NPF were discussed. Results showed that the averaged 10-500 nm particle number concentration was 1.7 x 10(4) cm(-3), similar to some typical observation values in North American and Europe; the 10-25 nm particle number concentration accounted for 25% of the total number concentration. Six NPF events occurred during observation. We analyzed that stable wind speed and direction, strong solar radiation promoted the NPF. The humidity during NPF event varied from 50% to 70%. Results indicated that clean ocean air mass brought from easterly and southerly wind promoted the NPF by Backward Trajectory Model Simulation. During the NPF event, the 10 - 25 nm particle number concentration positively correlated with the concentration of SO2, and negatively correlated with O3, whereas poorly correlated with NO2.

Atmospheric and climatic data measured at Thala site (Tunisia) for a long-time period (1977-2001) are used to analyse the monthly, seasonal, and annual variations of the aerosol optical depth at 1 μm wavelength. We have shown that aerosol and microphysical properties and the dominating aerosol types depend on seasons. A comparison of the seasonal cycle of aerosol optical characteristics at Thala site showed that the contribution of long-range transported particles is expected to be larger in summer as a consequence of the weather stability typical of this season. Also, the winter decrease in atmospheric turbidity may result from increases in relative humidity and decreases in temperature, leading to increased particle size and mass and increased fall and deposition velocities. The spring and autumn weather patterns usually carry fine dust and sand particles for the desert area to Thala region. The annual behaviour of the aerosol optical depth recorded a period of stead increase started in 1986 until 2001. Trends in atmospheric turbidity after 1988 could be explained other ways by the contribution of the eruption of Mount Pinatubo in 1991 and by local or regional changes in climate or in aerosol emissions.

Many of the significant advances in our understanding of atmospheric particles can be attributed to the application of mass spectrometry. Mass spectrometry provides high sensitivity with fast response time to probe chemically complex particles. This review focuses on recent developments and applications in the field of mass spectrometry of atmospheric aerosols. In Part II of this two-part review, we concentrate on real-time mass spectrometry techniques, which provide high time resolution for insight into brief events and diurnal changes while eliminating the potential artifacts acquired during long-term filter sampling. In particular, real-time mass spectrometry has been shown recently to provide the ability to probe the chemical composition of ambient individual particles <30 nm in diameter to further our understanding of how particles are formed through nucleation in the atmosphere. Further, transportable real-time mass spectrometry techniques are now used frequently on ground-, ship-, and aircraft-based studies around the globe to further our understanding of the spatial distribution of atmospheric aerosols. In addition, coupling aerosol mass spectrometry techniques with other measurements in series has allowed the in situ determination of chemically resolved particle effective density, refractive index, volatility, and cloud activation properties., (Copyright © 2011 Wiley Periodicals, Inc.)

Many of the significant advances in our understanding of atmospheric particles can be attributed to the application of mass spectrometry. Mass spectrometry provides high sensitivity with a fast response time to probe chemically complex particles. This review focuses on recent developments and applications in the field of mass spectrometry of atmospheric aerosols. In Part I of this two-part review, we concentrate on off-line mass spectrometry techniques, which require sample collection on filters but can provide detailed molecular speciation. In particular, off-line mass spectrometry techniques utilizing tandem mass spectrometry experiments and high resolution mass analyzers provide improved insight into secondary organic aerosol formation and heterogeneous reaction pathways through detailed structural elucidation at the molecular level., (Copyright © 2011 Wiley Periodicals, Inc.)