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The North China Plain (NCP) has experienced frequent severe haze pollution events in recent years. While extensive measurements have been made in megacities, aerosol sources, processes, and particle growth at urban downwind sites remain less understood. Here, an aerosol chemical speciation monitor and a scanning mobility particle sizer, along with a suite of collocated instruments, were deployed at the downwind site of Xingtai, a highly polluted city in the NCP, for real-time measurements of submicron aerosol (PM1) species and particle number size distributions during May and June 2016. The average mass concentration of PM1 was 30.5 (±19:4) µgm-3, which is significantly lower than that during wintertime. Organic aerosols (OAs) constituted the major fraction of PM1 (38 %), followed by sulfate (25 %) and nitrate (14 %). Positive matrix factorization with the multilinear engine version 2 showed that oxygenated OA (OOA) was the dominant species in OA throughout the study, on average accounting for 78% of OA, while traffic and cooking emissions both accounted for 11% of OA. Our results highlight that aerosol particles at the urban downwind site were highly aged and mainly from secondary formation. However, the diurnal cycle also illustrated the substantial influence of urban emissions on downwind sites, which are characterized by similar pronounced early morning peaks for most aerosol species. New particle formation and growth events were also frequently observed (58% of the time) on both clean and polluted days. Particle growth rates varied from 1.2 to 4.9 nm h-1 and our results showed that sulfate and OOA played important roles in particle growth during clean periods, while OOA was more important than sulfate during polluted events. Further analyses showed that particle growth rates have no clear dependence on air mass trajectories. [ABSTRACT FROM AUTHOR]

The rapid mass increase of atmospheric nitrate is a critical driving force for the occurrence of fine-particle pollution (referred to as haze hereafter) in Beijing. However, the exact mechanisms for this rapid increase of nitrate mass have not been well constrained from field observations. Here we present the first observations of the oxygen-17 excess of atmospheric nitrate (Δ17O(NO-3)) collected in Beijing haze to reveal the relative importance of different nitrate formation pathways, and we also present the simultaneously observed δ15N(NO-3). During our sampling period, 12 h averaged mass concentrations of PM2.5 varied from 16 to 323 µgm-3 with a mean of (141±88(1SD)) µgm-3. The observed Δ17O(NO-3) ranged from 27.5% to 33.9% with a mean of (30.6±1.8) %, while δ15N(NO-3) ranged from -2.5 % to 19.2% with a mean of (7.4±6.8)%. Δ17O(NO-3)-constrained calculations suggest nocturnal pathways (N2O5 CH2O=Cl- and NO3 CHC) dominated nitrate production during polluted days (PM2.5 ≥ 75 µgm-3), with a mean possible fraction of 56-97 %. Our results illustrate the potentiality of Δ17O in tracing nitrate formation pathways; future modeling work with the constraint of isotope data reported here may further improve our understanding of the nitrogen cycle during haze. [ABSTRACT FROM AUTHOR]

In an attempt to take effective action towards mitigating pollution episodes in Athens, precise knowledge of PM2.5 composition and its sources is a prerequisite. Thus, a 2-year chemical composition dataset from aerosol samples collected in an urban background site in central Athens from December 2013 to March 2016 has been obtained and a positive matrix factorization (PMF) was applied in order to identify and apportion fine aerosols to their sources. A total of 850 aerosol samples were collected on a 12 to 24 h basis and analyzed for major ions, trace elements, and organic and elemental carbon, allowing us to further assess the impact of residential heating as a source of air pollution over Athens. The ionic and carbonaceous components were found to constitute the major fraction of the PM2.5 aerosol mass. The annual contribution of the ion mass (IM), particulate organic mass (POM), dust, elemental carbon (EC), and sea salt (SS) was calculated at 31 %, 38 %, 18 %, 8 %, and 3 %, respectively, and exhibited considerable seasonal variation. In winter, the share of IM was estimated down to 23 %, with POMC EC being the dominant component accounting for 52% of the PM2.5 mass, while in summer, IM (42 %) and carbonaceous aerosols (41 %) contributed almost equally. Results from samples collected on a 12 h basis (day and night) during the three intensive winter campaigns indicated the impact of heating on the levels of a series of compounds. Indeed, PM2.5, EC, POM, NO-3, C2O2-4, non sea salt (nss) K+ and selected trace metals including Cd and Pb were increased by up to a factor of 4 in the night compared to the day, highlighting the importance of heating on air quality in Athens. Furthermore, in order to better characterize wintertime aerosol sources and quantify the impact of biomass burning on PM2:5 levels, source apportionment was performed. The data can be interpreted on the basis of six sources, namely biomass burning (31 %), vehicular emissions (19 %), heavy oil combustion (7 %), regional secondary (21 %), marine aerosols (9 %), and dust particles (8 %). Regarding night-to-day patterns their contributions shifted from 19 %, 19 %, 8 %, 31 %, 12 %, and 10% of the PM2.5 mass during day to 39 %, 19 %, 6 %, 14 %, 7 %, and 7% during the night, underlining the significance of biomass burning as the main contributor to fine particle levels during nighttime in winter. [ABSTRACT FROM AUTHOR]

The air quality of the Texas Gulf Coast region historically has been influenced heavily by regional shipping emissions. However, the effects of the recently established North American Emissions Control Area on aerosol concentrations and properties in this region are presently unknown. In order to better understand the current sources and processing mechanisms influencing coastal aerosol near Houston, a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was deployed for 3 weeks at a coastal location during May-June 2016. Total mass loadings of organic and inorganic non-refractory aerosol components during onshore flow periods were similar to those published before establishment of the regulations. Based on estimated methanesulfonic acid (MSA) mass loadings and published biogenic MSA/ non-sea-salt sulfate (nss-SO4) ratios, an average of over 75% of the observed nss-SO4 was from anthropogenic sources, predominantly shipping emissions. Mass spectral analysis indicated that for periods with similar backwardtrajectory-averaged meteorological conditions, air masses in- fluenced by shipping emissions had an increased mass fraction of ions related to carboxylic acids and larger oxygen-tocarbon ratios than those that avoided shipping lanes, suggesting that shipping emissions increase marine organic aerosol (OA) oxidation state. Amine fragment mass loadings were correlated positively with anthropogenic nss-SO4 during onshore flow, implying anthropogenic--biogenic interaction in marine OA production. Model calculations also suggest that advection of shipping-derived aerosol may enhance inland aqueous-phase secondary OA production. These results imply a continuing role of shipping emissions on aerosol properties over the Gulf of Mexico and suggest that further regulation of shipping fuel sulfur content will reduce coastal submicron aerosol mass loadings near Houston. [ABSTRACT FROM AUTHOR]

While residential coal/biomass burning might be a major and underappreciated emission source for PM2:5, especially during winter, it is not well constrained whether burning solid fuels contributes substantially to ambient volatile organic compounds (VOCs), which are precursors to secondary organic aerosols (SOAs) that typically have a higher contribution to particulate matter during winter haze events. In this study, ambient air samples were collected in 2014 from 25 October to 31 December at a rural site on the campus of the University of Chinese Academy of Sciences (UCAS) in northeastern Beijing for the analysis of VOCs. Since temporary intervention measures were implemented on 3-12 November to improve the air quality for the Asian-Pacific Economic Cooperation (APEC) summit held on 5-11 November in Beijing, and wintertime central heating started on 15 November in Beijing after the APEC summit, this sample collection period provided a good opportunity to study the influence of temporary control measures and wintertime heating on ambient VOCs. As a result of the temporary intervention measures implemented during 3--12 November (period II), the total mixing ratios of non-methane hydrocarbons averaged 11.25 ppb, approximately 50% lower than the values of 23.41 ppb in period I (25 October-2 November) and 21.71 ppb in period III (13 November-31 December). The ozone and SOA formation potentials decreased by ~ 50% and ~ 70 %, respectively, during period II relative to period I, with the larger decrease in SOA formation potentials attributed to more effective control over aromatic hydrocarbons mainly from solvent use. Back trajectory analysis revealed that the average mixing ratios of VOCs in southerly air masses were 2.3, 2.3 and 2.9 times those in northerly air masses during periods I, II and III, respectively; all VOC episodes occurred under the influence of southerly winds, suggesting much stronger emissions in the southern urbanized regions than in the northern rural areas. Based on a positive matrix factorization (PMF) receptor model, the altered contributions from traffic emissions and solvent use could explain 47.9% and 37.6% of the reduction in ambient VOCs, respectively, during period II relative to period I, indicating that the temporary control measures on vehicle emissions and solvent use were effective at lowering the ambient levels of VOCs. Coal/biomass burning, gasoline exhaust and industrial emissions were among the major sources, and they altogether contributed 60.3 %, 78.6% and 78.7% of the VOCs during periods I, II and III, respectively. Coal/biomass burning, mostly residential coal burning, became the dominant source, accounting for 45.1% of the VOCs during the wintertime heating period, with a specifically lower average contribution percentage in southerly air masses (38.2 %) than in northerly air masses (48.8 %). The results suggest that emission control in the industry and traffic sectors is more effective in lowering ambient reactive VOCs in non-heating seasons; however, during the winter heating season reducing emissions from residential burning of solid fuels would be of greater importance and would have health co-benefits from lowering both indoor and outdoor air pollution. [ABSTRACT FROM AUTHOR]

Black carbon (BC) particles can have deleterious human health consequences and impact regional and global climate. Uncertainties remain in part due to incomplete knowledge on the evolution of physical properties and mixing state of black carbon from sources to the remote atmosphere. We aim to understand how "road-to-ambient" processing and longer timescale aging in an urban plume affect black carbon physical properties. Refractory black carbon (rBC) was measured during summer 2016 using a singleparticle soot photometer (SP2) in two distinct environments: near a major freeway and downwind of downtown Los Angeles. The near-road measurements were made at distances ranging from 30 to 114m downwind of Interstate 405 in Los Angeles. These results were compared with measurements performed 100 km east of Los Angeles in Redlands, California. Coatings on rBC particles were quantified using two methods. As distance from the highway increased at the nearroad site, we observed decreases in rBC mass and number concentrations and increases in the number fraction of rBC particles with thick coatings (f). The latter likely occurred due to rapid processing of the highway plume and entrainment of urban background particles. Most rBC-containing particles measured near the highway were either uncoated or thinly coated. In Redlands, we found that rBC mass concentrations on weekdays were similar to those observed at the furthest measured distance from the highway (114 m). However, rBC number concentrations for the smallest measured sizes were an order of magnitude lower in Redlands than all measured distances from the highway. Observations of findicate that values in Redlands during periods when estimated photochemical age (PCA) was highest (6-8 h) were similar to corresponding values at the furthest measured distance from the highway. This suggests that the residence time of air in the Los Angeles Basin under typical summertime conditions measured during this campaign may not be sufficient for rBC to acquire thick coatings. However, under certain meteorological conditions, f was observed to be ~ 0:20 in Redlands, with coating thickness histograms showing a larger contribution of rBC particles with coating thickness>80 nm. This occurred during a weekend day when local emissions from diesel vehicles were lower (compared to weekdays) and winds brought air from the desert regions to Redlands, both of which would increase the relative contribution of remote sources of rBC. Afternoon values of f (and O3) were found to be systematically higher on weekends than weekdays, suggesting that the "weekend effect" can create more thickly coated rBC particles presumably due to enhanced secondary organic aerosol (SOA) and reduced available rBC as condensation sites. [ABSTRACT FROM AUTHOR]

Non-refractory submicrometer particulate matter (NR-PM1) was measured in the Seoul Metropolitan Area (SMA), Korea, using an Aerodyne high-resolution timeof- flight aerosol mass spectrometer (HR-ToF-AMS) from 14 April to 15 June 2016, as a part of the Korea-US Air Quality Study (KORUS-AQ) campaign. This was the first highly time-resolved, real-time measurement study of springtime aerosol in SMA and the results reveal valuable insights into the sources and atmospheric processes that contribute to PM pollution in this region. The average concentration of submicrometer aerosol (PM1 =NR-PM1 Cblack carbon (BC)) was 22.1 µgm-3 which was composed of 44% organics, 20% sulfate, 17% nitrate, 12% ammonium, and 7% BC. Organics had an average atomic oxygen-to-carbon (O = C) ratio of 0.49 and an average organic mass-to-carbon (OM/OC) ratio of 1.82. Four distinct sources of OA were identified via positive matrix factorization (PMF) analysis of the HR-ToF-AMS data: vehicle emissions represented by a hydrocarbon-like OA factor (HOA; O=CD0.15; 17% of OA mass), food cooking activities represented by a cooking-influenced OA factor (COA; O= CD0.19; 22% of OA mass), and secondary organic aerosol (SOA) represented by a semi-volatile oxygenated OA factor (SV-OOA; O=CD0.44; 27% of OA mass) and a low-volatility oxygenated OA factor (LV-OOA; O=CD0.91; 34% of OA mass). Our results indicate that air quality in SMA during KORUS-AQ was influenced strongly by secondary aerosol formation, with sulfate, nitrate, ammonium, SV-OOA, and LV-OOA together accounting for 76% of the PM1 mass. In particular, the formation of LV-OOA and sulfate was mainly promoted by elevated ozone concentrations and photochemical reactions during daytime, whereas SV-OOA and nitrate formation was contributed by both nocturnal processing of VOC and nitrogen oxides, respectively, and daytime photochemical reactions. In addition, lower nighttime temperature promoted gas-to-particle partitioning of semivolatile species and formation of SV-OOA and nitrate. During a period of 4 days (from 20 to 23 May ), LV-OOA increased dramatically and accounted for up to 41% of the PM1 mass. This intense LV-OOA formation event was associated with large enhancements of both anthropogenic and biogenic VOCs (e.g., isoprene and toluene), high concentration of Ox (=O3 + NO2), strong solar radiation, and stagnant conditions, suggesting that it was mainly driven by local photochemical formation. We have also investigated the formation and evolution mechanisms of severe haze episodes. Unlike the winter haze events which were mainly caused by intense local emissions coupled with stagnant meteorological conditions, the spring haze events appeared to be influenced by both regional and local factors. For example, there were episodes of long-range transport of plumes followed by calm meteorology conditions, which promoted the formation and accumulation of local secondary species, leading to high concentrations of PM. Overall, our results indicate that PM pollutants in urban Korea originate from complex emission sources and atmospheric processes and that the concentrations and composition of PM are controlled by various factors, including meteorological conditions, local anthropogenic emissions, and upwind sources. [ABSTRACT FROM AUTHOR]

Many stakeholders are seeking methods to reduce carbon dioxide (CO2) emissions in urban areas, but reliable, high-resolution inventories are required to guide these efforts. We present the development of a high-resolution CO2 inventory available for the Greater Toronto Area and surrounding region in Southern Ontario, Canada (area of ~2.8 x 105 km², 26% of the province of Ontario). The new SOCE (Southern Ontario CO2 Emissions) inventory is available at the 2.5 x 2.5 km spatial and hourly temporal resolution and characterizes emissions from seven sectors: area, residential natural-gas combustion, commercial natural-gas combustion, point, marine, on-road, and off-road. To assess the accuracy of the SOCE inventory, we developed an observation--model framework using the GEM-MACH chemistry--transport model run on a high-resolution grid with 2.5 km grid spacing coupled to the Fossil Fuel Data Assimilation System (FFDAS) v2 inventories for anthropogenic CO2 emissions and the European Centre for Medium-Range Weather Forecasts (ECMWF) land carbon model C-TESSEL for biogenic fluxes. A run using FFDAS for the Southern Ontario region was compared to a run in which its emissions were replaced by the SOCE inventory. Simulated CO2 mixing ratios were compared against in situ measurements made at four sites in Southern Ontario -- Downsview, Hanlan's Point, Egbert and Turkey Point -- in 3 winter months, January-March 2016. Model simulations had better agreement with measurements when using the SOCE inventory emissions versus other inventories, quantified using a variety of statistics such as correlation coefficient, root-meansquare error, and mean bias. Furthermore, when run with the SOCE inventory, the model had improved ability to capture the typical diurnal pattern of CO2 mixing ratios, particularly at the Downsview, Hanlan's Point, and Egbert sites. In addition to improved model--measurement agreement, the SOCE inventory offers a sectoral breakdown of emissions, allowing estimation of average time-of-day and day-of-week contributions of different sectors. Our results show that at night, emissions from residential and commercial natural-gas combustion and other area sources can contribute > 80% of the CO2 enhancement, while during the day emissions from the on-road sector dominate, accounting for > 70% of the enhancement. [ABSTRACT FROM AUTHOR]

Most of the global fossil fuel CO2 emissions arise from urbanized and industrialized areas. Bottom-up inventories quantify them but with large uncertainties. In 2010-2011, the first atmospheric in situ CO2 measurement network for Paris, the capital of France, began operating with the aim of monitoring the regional atmospheric impact of the emissions coming from this megacity. Five stations sampled air along a northeast--southwest axis that corresponds to the direction of the dominant winds. Two stations are classified as rural (Traînou -- TRN; Montgé-en-Goële -- MON), two are peri-urban (Gonesse -- GON; Gif-sur-Yvette -- GIF) and one is urban (EIF, located on top of the Eiffel Tower). In this study, we analyze the diurnal, synoptic and seasonal variability of the in situ CO2 measurements over nearly 1 year (8 August 2010-13 July 2011).We compare these datasets with remote CO2 measurements made at Mace Head (MHD) on the Atlantic coast of Ireland and support our analysis with atmospheric boundary layer height (ABLH) observations made in the center of Paris and with both modeled and observed meteorological fields. The average hourly CO2 diurnal cycles observed at the regional stations are mostly driven by the CO2 biospheric cycle, the ABLH cycle and the proximity to urban CO2 emissions. Differences of several µmol mol-1(ppm) can be observed from one regional site to the other. The more the site is surrounded by urban sources (mostly residential and commercial heating, and traffic), the more the CO2 concentration is elevated, as is the associated variability which reflects the variability of the urban sources. Furthermore, two sites with inlets high above ground level (EIF and TRN) show a phase shift of the CO2 diurnal cycle of a few hours compared to lower sites due to a strong coupling with the boundary layer diurnal cycle. As a consequence, the existence of a CO2 vertical gradient above Paris can be inferred, whose amplitude depends on the time of the day and on the season, ranging from a few tenths of ppm during daytime to several ppm during nighttime. The CO2 seasonal cycle inferred from monthly means at our regional sites is driven by the biospheric and anthropogenic CO2 flux seasonal cycles, the ABLH seasonal cycle and also synoptic variations. Enhancements of several ppm are observed at peri-urban stations compared to rural ones, mostly from the influence of urban emissions that are in the footprint of the peri-urban station. The seasonal cycle observed at the urban station (EIF) is specific and very sensitive to the ABLH cycle. At both the diurnal and the seasonal scales, noticeable differences of several ppm are observed between the measurements made at regional rural stations and the remote measurements made at MHD, that are shown not to define background concentrations appropriately for quantifying the regional (~100 km) atmospheric impact of urban CO2 emissions. For wind speeds less than 3 m s-1, the accumulation of local CO2 emissions in the urban atmosphere forms a dome of several tens of ppm at the peri-urban stations, mostly under the influence of relatively local emissions including those from the Charles de Gaulle (CDG) Airport facility and from aircraft in flight. When wind speed increases, ventilation transforms the CO2 dome into a plume. Higher CO2 background concentrations of several ppm are advected from the remote Benelux--Ruhr and London regions, impacting concentrations at the five stations of the network even at wind speeds higher than 9 m s-1. For wind speeds ranging between 3 and 8 m s-1, the impact of Paris emissions can be detected in the peri-urban stations when they are downwind of the city, while the rural stations often seem disconnected from the city emission plume. As a conclusion, our study highlights a high sensitivity of the stations to wind speed and direction, to their distance from the city, but also to the ABLH cycle depending on their elevation. We learn some lessons regarding the design of an urban CO2 network: (1) careful attention should be paid to properly setting regional (~100 km) background sites that will be representative of the different wind sectors; (2) the downwind stations should be positioned as symmetrically as possible in relation to the city center, at the peri-urban/rural border; (3) the stations should be installed at ventilated sites (away from strong local sources) and the air inlet set up above the building or biospheric canopy layer, whichever is the highest; and (4) high-resolution wind information should be available with the CO2 measurements. [ABSTRACT FROM AUTHOR]

In the framework of the Dynamics-Aerosol-Chemistry-Cloud Interactions in West Africa (DACCIWA) project, the tropospheric chemical composition in large cities along the Gulf of Guinea is studied using the Weather and Research Forecast and CHIMERE regional models. Simulations are performed for the May-July 2014 period, without and with biomass burning emissions. Model results are compared to satellite data and surface measurements. Using numerical tracer release experiments, it is shown that the biomass burning emissions in Central Africa are impacting the surface aerosol and gaseous species concentrations in Gulf of Guinea cities such as Lagos (Nigeria) and Abidjan (Ivory Coast). Depending on the altitude of the injection of these emissions, the pollutants follow different pathways: directly along the coast or over land towards the Sahel before being vertically mixed in the convective boundary layer and transported to the south-west and over the cities. In July 2014, the maximum increase in surface concentrations due to fires in Central Africa is ≈ 150 µg m-3 for CO, ≈ 10 to 20 µg m-3 for O3 and ≈ 5 µg m-3 for PM10. The analysis of the PM-3 chemical composition shows that this increase is mainly related to an increase in particulate primary and organic matter. [ABSTRACT FROM AUTHOR]

This study investigates the seasonal variation, molecular distribution and stable carbon isotopic composition of diacids, oxocarboxylic acids and α-dicarbonyls to better understand the sources and formation processes of fine aerosols (PM2.5) in Beijing. The concentrations of total dicarboxylic acids varied from 110 to 2580 ng m-3, whereas oxoacids (9.50-353 ng m-3) and dicarbonyls (1.50-85.9 ng m-3) were less abundant. Oxalic acid was found to be the most abundant individual species, followed by succinic acid or occasionally by terephthalic acid (tPh), a plastic waste burning tracer. Ambient concentrations of phthalic acid (37.9 ± 27.3 ng m-3) and tPh (48.7 ± 51.1 ng m-3) were larger in winter than in other seasons, illustrating that fossil fuel combustion and plastic waste incineration contribute more to wintertime aerosols. The year-round mass concentration ratios of malonic acid to succinic acid (C3/C4) were relatively low by comparison with those in other urban aerosols and remote marine aerosols. The values were less than or equal to unity in Beijing, implying that the degree of photochemical formation of diacids in Beijing is insignificant. Moreover, strong correlation coefficients of major oxocarboxylic acids and α-dicarbonyls with nss-K+ suggest that biomass burning contributes significantly to these organic acids and related precursors. The mean δ13C value of succinic acid is the highest among all species, with values of -17.1 ± 3.9‰ (winter) and -17.1 ± 2.0‰ (spring), while malonic acid is more enriched in 13C than others in autumn (-17.6 ± 4.6‰) and summer (-18.7 ± 4.0‰). The δ13C values of major species in Beijing aerosols are generally lower than those in the western North Pacific atmosphere, the downwind region, which indicates that stable carbon isotopic compositions of diacids depend on their precursor sources in Beijing. Therefore, our study demonstrates that in addition to photochemical oxidation, high abundances of diacids, oxocarboxylic acids and α-dicarbonyls in Beijing are largely associated with anthropogenic primary emissions, such as biomass burning, fossil fuel combustion and plastic waste burning. [ABSTRACT FROM AUTHOR]

Measurements of OH, HO2, RO2i (alkene and aromatic-related RO2) and total RO2 radicals taken during the ClearfLo campaign in central London in the summer of 2012 are presented. A photostationary steady-state calculation of OH which considered measured OH reactivity as the OH sink term and the measured OH sources (of which HO2+ NO reaction and HONO photolysis dominated) compared well with the observed levels of OH. Comparison with calculations from a detailed box model utilising the Master Chemical Mechanism v3.2, however, highlighted a substantial discrepancy between radical observations under lower NOx conditions ([NO] < 1 ppbv), typically experienced during the afternoon hours, and indicated that the model was missing a significant peroxy radical sink; the model overpredicted HO2 by up to a factor of 10 at these times. Known radical termination steps, such as HO2 uptake on aerosols, were not sufficient to reconcile the model-measurement discrepancies alone, suggesting other missing termination processes. This missing sink was most evident when the air reaching the site had previously passed over central London to the east and when elevated temperatures were experienced and, hence, contained higher concentrations of VOCs. Uncertainties in the degradation mechanism at low NOx of complex biogenic and diesel related VOC species, which were particularly elevated and dominated OH reactivity under these easterly flows, may account for some of the model-measurement disagreement. Under higher [NO] (> 3 ppbv) the box model increasingly underpredicted total [RO2]. The modelled and observed HO2 were in agreement, however, under elevated NO concentrations ranging from 7 to 15 ppbv. The model uncertainty under low NO conditions leads to more ozone production predicted using modelled peroxy radical concentrations (~3 ppbv h-1) versus ozone production from peroxy radicals measured (~1 ppbv h-1). Conversely, ozone production derived from the predicted peroxy radicals is up to an order of magnitude lower than from the observed peroxy radicals as [NO] increases beyond 7 ppbv due to the model underprediction of RO2 under these conditions. [ABSTRACT FROM AUTHOR]

For PM2.5 filter samples collected daily at the Chinese Research Academy of Environmental Sciences (Beijing, China) from December of 2013 to February of 2014 (the winter period), chemical characteristics and sources were investigated with an emphasis on haze events in different alert levels. During the 3 months, the average PM2.5 concentration was 89 µg m-3, exceeding the Chinese national standard of 75 µg m-3 in 24 h. The maximum PM2.5 concentration was 307 µg m-3, which characterizes developed-type pollution (PM2.5 / PM10>0.5) in the World Health Organization criteria. PM2.5 was dominated by SO42-, NO3-, and pseudo-carbonaceous compounds with obvious differences in concentrations and proportions between non-haze and haze episodes. The non-negative matrix factorization (NMF) analysis provided reasonable PM2.5 source profiles, by which five sources were identified: soil dust, traffic emission, biomass combustion, industrial emission, and coal combustion accounting for 13, 22, 12, 28, and 25% of the total, respectively. The dust impact increased with northwesterlies during non-haze periods and decreased under stagnant conditions during haze periods. A blue alert of heavy air pollution was characterized by the greatest contribution from industrial emissions (61%). During the Chinese Lantern Festival, an orange alert was issued and biomass combustion was found to be the major source owing to firework explosions. Red-alert haze was almost equally contributed by local traffic and transported coal combustion emissions from the vicinity of Beijing (approximately 40% each) that was distinguished by the highest levels of NO3- and SO42-, respectively. This study also reveals that the severity and source of haze are largely dependent on meteorological conditions. [ABSTRACT FROM AUTHOR]

We conducted the first real-time continuous vertical measurements of particle extinction (bext), gaseous NO2, and black carbon (BC) from ground level to 260 m during two severe winter haze episodes at an urban site in Beijing, China. Our results illustrated four distinct types of vertical profiles: (1) uniform vertical distributions (37% of the time) with vertical differences less than 5%, (2) higher values at lower altitudes (29%), (3) higher values at higher altitudes (16%), and (4) significant decreases at the heights of ~100-150 m (14%). Further analysis demonstrated that vertical convection as indicated by mixing layer height, temperature inversion, and local emissions are three major factors affecting the changes in vertical profiles. Particularly, the formation of type 4 was strongly associated with the stratified layer that was formed due to the interactions of different air masses and temperature inversions. Aerosol composition was substantially different below and above the transition heights with ~20-30% higher contributions of local sources (e.g., biomass burning and cooking) at lower altitudes. A more detailed evolution of vertical profiles and their relationship with the changes in source emissions, mixing layer height, and aerosol chemistry was illustrated by a case study. BC showed overall similar vertical profiles as those of bext (R² = 0.92 and 0.69 in November and January, respectively). While NO2 was correlated with bext for most of the time, the vertical profiles of bext/NO2 varied differently for different profiles, indicating the impact of chemical transformation on vertical profiles. Our results also showed that more comprehensive vertical measurements (e.g., more aerosol and gaseous species) at higher altitudes in the megacities are needed for a better understanding of the formation mechanisms and evolution of severe haze episodes in China. [ABSTRACT FROM AUTHOR]

The growth of mega-cities leads to air quality problems directly affecting the citizens. Satellite measurements are becoming of higher quality and quantity, which leads to more accurate satellite retrievals of enhanced air pollutant concentrations over large cities. In this paper, we compare and discuss both an existing and a new method for estimating urban-scale trends in CO emissions using multi-year retrievals from the MOPITT satellite instrument. The first method is mainly based on satellite data, and has the advantage of fewer assumptions, but also comes with uncertainties and limitations as shown in this paper. To improve the reliability of urban-to-regional scale emission trend estimation, we simulate MOPITT retrievals using the Weather Research and Forecast model with chemistry core (WRF-Chem). The difference between model and retrieval is used to optimize CO emissions in WRF-Chem, focusing on the city of Madrid, Spain. This method has the advantage over the existing method in that it allows both a trend analysis of CO concentrations and a quantification of CO emissions. Our analysis confirms that MOPITT is capable of detecting CO enhancements over Madrid, although significant differences remain between the yearly averaged model output and satellite measurements (R² = 0.75) over the city. After optimization, we find Madrid CO emissions to be lower by 48% for 2002 and by 17% for 2006 compared with the EdgarV4.2 emission inventory. The MOPITT-derived emission adjustments lead to better agreement with the European emission inventory TNO-MAC-III for both years. This suggests that the downward trend in CO emissions over Madrid is overestimated in EdgarV4.2 and more realistically represented in TNO-MACC-III. However, our satellite and model based emission estimates have large uncertainties, around 20% for 2002 and 50% for 2006. [ABSTRACT FROM AUTHOR]

Traffic emissions contribute significantly to urban air pollution. Measurements were conducted over Highway 401 in Toronto, Canada, with a long-path Fourier transform infrared (FTIR) spectrometer combined with a suite of micrometeorological instruments to identify and quantify a range of air pollutants. Results were compared with simultaneous in situ observations at a roadside monitoring station, and with output from a special version of the operational Canadian air quality forecast model (GEM-MACH). Elevated mixing ratios of ammonia (0-23 ppb) were observed, of which 76% were associated with traffic emissions. Hydrogen cyanide was identified at mixing ratios between 0 and 4 ppb. Using a simple dispersion model, an integrated emission factor of on average 2.6 g km-1 carbon monoxide was calculated for this defined section of Highway 401, which agreed well with estimates based on vehicular emission factors and observed traffic volumes. Based on the same dispersion calculations, vehicular average emission factors of 0.04, 0.36, and 0.15 g km-1 were calculated for ammonia, nitrogen oxide, and methanol, respectively. [ABSTRACT FROM AUTHOR]

To control severe air pollution in China, comprehensive pollution control strategies have been implemented throughout the country in recent years. To evaluate the effectiveness of these strategies, the influence of meteorological conditions on levels of air pollution needs to be determined. Using the intensive air pollution control strategies implemented during the Asia-Pacific Economic Cooperation Forum in 2014 (APEC 2014) and the 2015 China Victory Day Parade (Victory Parade 2015) as examples, we estimated the role of meteorological conditions and pollution control strategies in reducing air pollution levels in Beijing. Atmospheric particulate matter of aerodynamic diameter ≥ 2:5 µm (PM2:5) samples were collected and gaseous pollutants (SO2, NO, NOx, and O3) were measured online at a site in Peking University (PKU). To determine the influence of meteorological conditions on the levels of air pollution, we first compared the air pollutant concentrations during days with stable meteorological conditions. However, there were few days with stable meteorological conditions during the Victory Parade. As such, we were unable to estimate the level of emission reduction efforts during this period. Finally, a generalized linear regression model (GLM) based only on meteorological parameters was built to predict air pollutant concentrations, which could explain more than 70% of the variation in air pollutant concentration levels, after incorporating the nonlinear relationships between certain meteorological parameters and the concentrations of air pollutants. Evaluation of the GLM performance revealed that the GLM, even based only on meteorological parameters, could be satisfactory to estimate the contribution of meteorological conditions in reducing air pollution and, hence, the contribution of control strategies in reducing air pollution. Using the GLM, we found that the meteorological conditions and pollution control strategies contributed 30 and 28% to the reduction of the PM2:5 concentration during APEC and 38 and 25% during the Victory Parade, respectively, based on the assumption that the concentrations of air pollutants are only determined by meteorological conditions and emission intensities. We also estimated the contribution of meteorological conditions and control strategies in reducing the concentrations of gaseous pollutants and PM2:5 components with the GLMs, revealing the effective control of anthropogenic emissions. [ABSTRACT FROM AUTHOR]

Mass-concentration-based particle size distributions measured by a high-resolution aerosol mass spectrometer were systematically analyzed to assess long and shortterm temporal characteristics of ambient particle size distributions sampled at a typical urban environment close to emission sources and a suburban coastal site representing a regional and local pollution receptor location in Hong Kong. Measured distributions were bimodal and deconvoluted into submodes, which were analyzed for day-to-day variations and diurnal variations. Traffic and cooking emissions at the urban site contributed substantially to particle mass in both modes, while notable decreases in mass median diameters were limited to the morning rush hour. Inorganic particle components displayed varying diurnal behavior, including nocturnal nitrate formation and daytime photochemical formation evident in both modes. Suburban particle size distributions exhibited notable seasonal disparities with differing influence of local formation, particularly in spring and summer, and transport which dominated in the fall season leading to notably higher sulfate and organic accumulation-mode particle concentrations. Variations in particle mixing state were evaluated by comparison of interspecies mass median diameter trends at both measurement sites. Internal mixing was prevalent in the accumulation mode in spring at the urban site, while greater frequency of time periods with external mixing of particle populations comprising different fractions of organic constituents was observed in summer. At the suburban site, sulfate and nitrate in the accumulation mode more frequently exhibited differing particle size distributions in all seasons, signifying a greater extent of external mixing. At the urban site, periods of greater submicron inorganic mass concentrations were more likely to be caused by increases in both Aitken- and accumulation-mode particle mass in summer, while at the suburban receptor location, organic and nitrate Aitken-mode particle mass contributed more regularly to higher total submicron species mass concentrations in most seasons (spring, summer, and winter). [ABSTRACT FROM AUTHOR]

The simultaneous observation and analysis of atmospheric fine particles (PM2.5) on a regional scale is an important approach to develop control strategies for haze pollution. In this study, samples of filtered PM2.5 were collected simultaneously at three urban sites (Beijing, Tianjin, and Shijiazhuang) and at a regional background site (Xinglong) in the Beijing-Tianjin-Hebei (BTH) region from June 2014 to April 2015. The PM2.5 at the four sites was mainly comprised of organic matter, secondary inorganic ions, and mineral dust. Positive matrix factorization (PMF) demonstrated that, on an annual basis, secondary inorganic aerosol was the largest PM2.5 source in this region, accounting for 29.2-40.5%of the PM2.5 mass at the urban sites; the second-largest PM2.5 source was motor vehicle exhaust, particularly in Beijing (24.9 %), whereas coal combustion was also a large source in Tianjin (12.4 %) and Shijiazhuang (15.5 %), with particular dominance in winter. Secondary inorganic aerosol plays a vital role in the haze process, with the exception of the spring haze in Shijiazhuang and Tianjin, for which the dust source was crucial. In addition to secondary transformations, local direct emissions (coal combustion and motor vehicle exhaust) significantly contribute to the winter haze at the urban sites. Moreover, with the aggravation of haze pollution, the OC/EC mass ratio of PM2.5 decreased considerably and the nitrate-rich secondary aerosol increased during all four seasons in Beijing, both of which indicate that local motor vehicle emissions significantly contribute to the severe haze episodes in Beijing. To assess the impacts of regional transport on haze pollution, the PMF results were further processed with backward-trajectory cluster analysis, revealing that haze pollution usually occurred when air masses originating from polluted industrial regions in the south prevailed and is characterized by high PM2.5 loadings with considerable contributions from secondary aerosols. This study suggests that control strategies to mitigate haze pollution in the BTH region should focus on the reduction of gaseous precursor emissions from fossil fuel combustion (motor vehicle emissions in Beijing and coal combustion in Tianjin, Hebei, and nearby provinces). [ABSTRACT FROM AUTHOR]

Here, we present an assessment of long-term trends in O3 and odd oxygen (O3 CNO2) at the industrial Monterrey metropolitan area (MMA) in NE Mexico. Diurnal amplitudes in Ox (AVd) are used as a proxy for net O3 production, which is influenced by the NO2 photolysis rate. No significant differences in the AVd are observed between weekends and weekdays, although the largest AVd values are observed at sites downwind of industrial areas. The highest O3 mixing ratios are observed in spring, with minimum values in winter. The largest annual variations in O3 are typically observed downwind of the MMA, with the lowest variations generally recorded in highly populated areas and close to industrial areas. A wind sector analysis of mixing ratios of O3 precursors revealed that the dominant sources of emissions are located in the industrial regions within the MMA and surrounding area. Significant increasing trends in O3 in spring, summer, and autumn are observed depending on site location, with trends in annual averages ranging between 0.19 and 0.33 ppbyr-1. Overall, from 1993 to 2014, within the MMA, O3 has increased at an average rate of 0.22 ppbyr-1 (p < 0:01), which is in marked contrast with the decline of 1.15 ppbyr-1 (p < 0:001) observed in the Mexico City metropolitan area (MCMA) for the same period. No clear trend is observed from 1996 to 2014 within the Guadalajara metropolitan area (GMA). [ABSTRACT FROM AUTHOR]

The emission of pollutants is extremely reduced during the annual Chinese Spring Festival (SF) in Shenzhen, China. During the SF, traffic flow drops by ~50% and the industrial plants are almost entirely shut down in Shenzhen. To characterize the variation in ambient air pollutants due to the "Spring Festival effect", various gaseous and particulate pollutants were measured in real time in urban Shenzhen over three consecutive winters (2014-2016). The results indicate that the concentrations of NOx, volatile organic compounds (VOCs), black carbon (BC), primary organic aerosols, chloride, and nitrate in submicron aerosols decrease by 50-80% during SF periods relative to non-Spring Festival periods, regardless of meteorological conditions. This decrease suggests that these pollutants are mostly emitted or secondarily formed from urban local emissions. The concentration variation in species mostly from regional or natural sources, however, is found to be much less, such as for bulk fine particulate matter (PM2.5). More detailed analysis of the Spring Festival effect reveals an urgent need to reduce emissions of SO2 and VOCs on a regional scale rather than on an urban scale to reduce urban PM2.5 in Shenzhen, which can also be useful as a reference for other megacities in China. [ABSTRACT FROM AUTHOR]

Isocyanic acid (HNCO), an acidic gas found in tobacco smoke, urban environments, and biomass-burningaffected regions, has been linked to adverse health outcomes. Gasoline- and diesel-powered engines and biomass burning are known to emit HNCO and hypothesized to emit precursors such as amides that can photochemically react to produce HNCO in the atmosphere. Increasingly, diesel engines in developed countries like the United States are required to use selective catalytic reduction (SCR) systems to reduce tailpipe emissions of oxides of nitrogen. SCR chemistry is known to produce HNCO as an intermediate product, and SCR systems have been implicated as an atmospheric source of HNCO. In this work, we measure HNCO emissions from an SCR system-equipped diesel engine and, in combination with earlier data, use a three-dimensional chemical transport model (CTM) to simulate the ambient concentrations and source/pathway contributions to HNCO in an urban environment. Engine tests were conducted at three different engine loads, using two different fuels and at multiple operating points. HNCO was measured using an acetate chemical ionization mass spectrometer. The diesel engine was found to emit primary HNCO (3-90 mg kg fuel-1/but we did not find any evidence that the SCR system or other aftertreatment devices (i.e., oxidation catalyst and particle filter) produced or enhanced HNCO emissions. The CTM predictions compared well with the only available observational datasets for HNCO in urban areas but underpredicted the contribution from secondary processes. The comparison implied that diesel-powered engines were the largest source of HNCO in urban areas. The CTM also predicted that dailyaveraged concentrations of HNCO reached a maximum of ~110 pptv but were an order of magnitude lower than the 1 ppbv level that could be associated with physiological effects in humans. Precursor contributions from other combustion sources (gasoline and biomass burning) and wintertime conditions could enhance HNCO concentrations but need to be explored in future work. [ABSTRACT FROM AUTHOR]

New particle formation (NPF) has been observed in many highly polluted environments of South East Asia, including Beijing, where the extent of its contribution to intense haze events is still an open question. Estimated characteristics of NPF events, such as their starting times and formation and growth rates of particles, are more accurate when the detection range of particles extends to smaller sizes. In order to understand the very first steps of particle formation, we used a neutral cluster and air ion spectrometer (NAIS) to investigate particle characteristics at sizes exactly at which atmospheric nucleation and cluster activity occurs. Observations over a continuous 3-month period in Beijing showed 26 NPF events. These events generally coincided with periods with relatively clean air when the wind direction was from the less industrialised north. No NPF events were observed when the daily mean PM2.5 concentration exceeded 43 µgm-3, which was the upper threshold for particle formation in Beijing. The fraction of particles that are charged in the size range 2-42 nm was normally about 15 %. However, this fraction increased to 20-30% during haze events and decreased to below 10% during NPF events. With the NAIS, we very precisely determined the starting times of NPF to a greater accuracy than has been possible in Beijing before and provided a temporal distribution of NPF events with a maximum at about 08:30 LT. Particle formation rates varied between 12 and 38 cm-3 s-1. Particle growth rates were estimated to be in the range of 0.5-9.0 nmh-1. These results are more reliable than previous studies in Beijing as the measurements were conducted for the first time at the exact sizes at which clusters form into particles and provide useful insight into the formation of haze events. [ABSTRACT FROM AUTHOR]

The WRF-Chem model coupled with a singlelayer urban canopy model (UCM) is integrated for 5 years at convection-permitting scale to investigate the individual and combined impacts of urbanization-induced changes in land cover and pollutant emissions on regional climate in the Yangtze River Delta (YRD) region in eastern China. Simulations with the urbanization effects reasonably reproduced the observed features of temperature and precipitation in the YRD region. Urbanization over the YRD induces an urban heat island (UHI) effect, which increases the surface temperature by 0.53 °C in summer and increases the annual heat wave days at a rate of 3.7 d yr-1 in the major megacities in the YRD, accompanied by intensified heat stress. In winter, the near-surface air temperature increases by approximately 0.7 °C over commercial areas in the cities but decreases in the surrounding areas. Radiative effects of aerosols tend to cool the surface air by reducing net shortwave radiation at the surface. Compared to the more localized UHI effect, aerosol effects on solar radiation and temperature influence a much larger area, especially downwind of the city cluster in the YRD. Results also show that the UHI increases the frequency of extreme summer precipitation by strengthening the convergence and updrafts over urbanized areas in the afternoon, which favor the development of deep convection. In contrast, the radiative forcing of aerosols results in a surface cooling and upper-atmospheric heating, which enhances atmospheric stability and suppresses convection. The combined effects of the UHI and aerosols on precipitation depend on synoptic conditions. Two rainfall events under two typical but different synoptic weather patterns are further analyzed. It is shown that the impact of urban land cover and aerosols on precipitation is not only determined by their influence on local convergence but also modulated by large-scale weather systems. For the case with a strong synoptic forcing associated with stronger winds and larger spatial convergence, the UHI and aerosol effects are relatively weak. When the synoptic forcing is weak, however, the UHI and aerosol effects on local convergence dominate. This suggests that synoptic forcing plays a significant role in modulating the urbanization-induced land-cover and aerosol effects on individual rainfall event. Hence precipitation changes due to urbanization effects may offset each other under different synoptic conditions, resulting in little changes in mean precipitation at longer timescales. [ABSTRACT FROM AUTHOR]

Even though emission inventories indicate that wood combustion is a major source of polycyclic aromatic hydrocarbons (PAHs), estimating its impacts on PAH concentration in ambient air remains challenging. In this study the effect of local small-scale wood combustion on the benzo[a]pyrene (BaP) concentrations in ambient air in the Helsinki metropolitan area in Finland is evaluated, using ambient air measurements, emission estimates, and dispersion modeling. The measurements were conducted at 12 different locations during the period from 2007 to 2015. The spatial distributions of annual average BaP concentrations originating from wood combustion were predicted for four of those years: 2008, 2011, 2013, and 2014. According to both the measurements and the dispersion modeling, the European Union target value for the annual average BaP concentrations (1 ng m-3) was clearly exceeded in certain suburban detached-house areas. However, in most of the other urban areas, including the center of Helsinki, the concentrations were below the target value. The measured BaP concentrations highly correlated with the measured levoglucosan concentrations in the suburban detached-house areas. In street canyons, the measured concentrations of BaP were at the same level as those in the urban background, clearly lower than those in suburban detached-house areas. The predicted annual average concentrations matched with the measured concentrations fairly well. Both the measurements and the modeling clearly indicated that wood combustion was the main local source of ambient air BaP in the Helsinki metropolitan area. [ABSTRACT FROM AUTHOR]

Polycyclic aromatic hydrocarbons (PAHs), particularly benzo[a]pyrene (BaP), are toxic compounds emitted from various anthropogenic sources. Understanding the BaP concentrations, dynamics and decomposition in soil is required to assess the critical loads of BaP in urban environments. This study is the first attempt to evaluate all major input and output components of benzo[a]pyrene (BaP) balance and to calculate the permissible load on the urban environment in different land-use zones in the Eastern district of Moscow. BaP contamination of the snow cover in the Eastern district of Moscow was related to daily BaP fallout from the atmosphere. In 2010, the mean content of the pollutant in the snow dust was 1942 ng g-1, whereas the average intensity of its fallout was 7.13 ngm-2 per day. Across the territory, BaP winter fallout intensities varied from 0.3 to 1100 ngm-2 per day. The average BaP content in the surface (0-10 cm) soil horizons was 409 ng g-1, which is 83 times higher than the local background value and 20 times higher than the maximum permissible concentration (MPC) accepted in Russia. The variations in soil and snow BaP concentrations among different land-use zones were examined. A significant contribution of BaP from the atmosphere to urban soils was identified. Based on the measurements of BaP atmospheric fallout and BaP reserves in the soils, the critical loads of BaP for the land-use zones in the Eastern district were calculated for different values of degradation intensity and different exposure times. It was established that at an annual degradation intensity of 1-10 %, ecologically safe BaP levels in the soils of all land-use zones, excluding the agricultural zone, will only be reached after many decades or centuries. [ABSTRACT FROM AUTHOR]

In the present study, the WRF-CHEM model is used to evaluate the contributions of trans-boundary transport to the air quality in Beijing during a persistent air pollution episode from 5 to 14 July 2015 in Beijing-Tianjin-Hebei (BTH), China. Generally, the predicted temporal variations and spatial distributions of PM2.5 (fine particulate matter), O3 (ozone), and NO2 are in good agreement with observations in BTH. The WRF-CHEM model also reproduces reasonably well the temporal variations of aerosol species compared to measurements in Beijing. The factor separation approach is employed to evaluate the contributions of trans-boundary transport of non-Beijing emissions to the PM2.5 and O3 levels in Beijing. On average, in the afternoon during the simulation episode, the local emissions contribute 22.4 % to the O3level in Beijing, less than 36.6 % from non-Beijing emissions. The O3 concentrations in Beijing are decreased by 5.1 % in the afternoon due to interactions between local and non-Beijing emissions. The non-Beijing emissions play a dominant role in the PM2.5 level in Beijing, with a contribution of 61.5 %, much higher than 13.7 %, from Beijing local emissions. The emission interactions between local and non-Beijing emissions enhance the PM2.5 concentrations in Beijing, with a contribution of 5.9 %. Therefore, the air quality in Beijing is generally determined by the trans-boundary transport of non-Beijing emissions during summertime, showing that the cooperation with neighboring provinces to mitigate pollutant emissions is key for Beijing to improve air quality. [ABSTRACT FROM AUTHOR]

Highly time-resolved chemical characterization of nonrefractory submicrometer particulate matter (NR-PM1) was conducted in Seoul, the capital and largest metropolis of Korea, using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). The measurements were performed during winter, when elevated particulate matter (PM) pollution events are often observed. This is the first time that detailed real-time aerosol measurement results have been reported from Seoul, Korea, and they reveal valuable insights into the sources and atmospheric processes that contribute to PM pollution in this region. The average concentration of submicron aerosol (PM1 = NR-PM1+ black carbon (BC)) was 27.5 μg m-3, and the total mass was dominated by organics (44 %), followed by nitrate (24 %) and sulfate (10 %). The average atomic ratios of oxygen to carbon (O / C), hydrogen to carbon (H / C), and nitrogen to carbon (N / C) of organic aerosols (OA) were 0.37, 1.79, and 0.018, respectively, which result in an average organic mass-to-carbon (OM / OC) ratio of 1.67. The concentrations (2.6-90.7 μg m-3) and composition of PM1 varied dynamically during the measurement period due to the influences of different meteorological conditions, emission sources, and air mass origins. Five distinct sources of OA were identified via positive matrix factorization (PMF) analysis of the HR-ToF-AMS data: vehicle emissions represented by a hydrocarbon-like OA factor (HOA, O / C = 0.06), cooking activities represented by a cooking OA factor (COA, O / C = 0.14), wood combustion represented by a biomass burning OA factor (BBOA, O / C = 0.34), and secondary organic aerosol (SOA) represented by a semivolatile oxygenated OA factor (SV-OOA, O / C = 0.56) and a low-volatility oxygenated OA factor (LV-OOA, O / C = 0.68). On average, primary OA (POA = HOA + COA + BBOA) accounted for 59 % the OA mass, whereas SV-OOA and LV-OOA contributed 15 and 26 %, respectively. Our results indicate that air quality in Seoul during winter is influenced strongly by secondary aerosol formation, with sulfate, nitrate, ammonium, SV-OOA, and LV-OOA together accounting for 64 % of the PM1 mass during this study. However, aerosol sources and composition were found to be significantly different between clean and polluted periods. During stagnant periods with low wind speed (WS) and high relative humidity (RH), PM concentration was generally high (average ±1σ = 43.6 ± 12.4 μg m-3) with enhanced fractions of nitrate (27 %) and SV-OOA (8 %), which suggested a strong influence from local production of secondary aerosol. Low-PM loading periods (12.6 ± 7.1 μg m-3) tended to occur under higher-WS and lower-RH conditions and appeared to be more strongly influenced by regional air masses, as indicated by higher mass fractions of sulfate (12 %) and LV-OOA (20 %) in PM1. Overall, our results indicate that PM pollutants in urban Korea originate from complex emission sources and atmospheric processes and that their concentrations and composition are controlled by various factors, including meteorological conditions, local anthropogenic emissions, and upwind sources. [ABSTRACT FROM AUTHOR]

During the APEC (Asia-Pacific Economic Cooperation) Economic Leaders' 2014 Summit in Beijing, strict regional air emission controls were implemented, providing a unique opportunity to investigate the transport and formation mechanism of fine particulate matter (PM2.5). This study explores the use of vertical observation methods to investigate the influence of regional transport on PM2.5 pollution in Beijing before and during the APEC Summit. Vertical profiles of extinction coefficient, wind, temperature and relative humidity were monitored at a rural site on the border of Beijing and Hebei Province. Three PM2.5 pollution episodes were analyzed. In episode 1 (27 October to 1 November), regional transport accompanied by the accumulation of pollutants under unfavorable meteorological conditions led to the pollution. In episode 2 (2-5 November), pollutants left from episode 1 were retained in the boundary layer of the region for 2 days and then settled down to the surface, leading to an explosive increase of PM2.5. The regional transport of aged aerosols played a crucial role in the heavy PM2.5 pollution. In episode 3 (6-11 November), emissions from large point sources had been controlled for several days while primary emissions from diesel vehicles might have led to the pollution. It is found that ground-level observation of meteorological conditions and air quality could not fully explain the pollution process, while vertical parameters (aerosol optical properties, winds, relative humidity and temperature) improved the understanding of regional transport influence on heavy pollution processes. Future studies may consider including vertical observations to aid investigation of pollutant transport, especially during episodic events of rapidly increasing concentrations. [ABSTRACT FROM AUTHOR]

An observation-constrained box model based on the Carbon Bond mechanism, version 5 (CB05), was used to study photochemical processes along the NASA P-3B flight track and spirals over eight surface sites during the September 2013 Houston, Texas deployment of the NASA Deriving Information on Surface Conditions from COlumn and VERtically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) campaign. Data from this campaign provided an opportunity to examine and improve our understanding of atmospheric photochemical oxidation processes related to the formation of secondary air pollutants such as ozone (O3/. O3 production and its sensitivity to NOx and volatile organic compounds (VOCs) were calculated at different locations and times of day. Ozone production efficiency (OPE), defined as the ratio of the ozone production rate to the NOx oxidation rate, was calculated using the observations and the simulation results of the box and Community Multiscale Air Quality (CMAQ) models. Correlations of these results with other parameters, such as radical sources and NOx mixing ratio, were also evaluated. It was generally found that O3 production tends to be more VOC-sensitive in the morning along with high ozone production rates, suggesting that control of VOCs may be an effective way to control O3 in Houston. In the afternoon, O3 production was found to be mainly NOx -sensitive with some exceptions. O3 production near major emissions sources such as Deer Park was mostly VOC-sensitive for the entire day, other urban areas near Moody Tower and Channelview were VOC-sensitive or in the transition regime, and areas farther from downtown Houston such as Smith Point and Conroe were mostly NOx - sensitive for the entire day. It was also found that the control of NOx emissions has reduced O3 concentrations over Houston but has led to larger OPE values. The results from this work strengthen our understanding of O3 production; they indicate that controlling NOx emissions will provide air quality benefits over the greater Houston metropolitan area in the long run, but in selected areas controlling VOC emissions will also be beneficial. [ABSTRACT FROM AUTHOR]

This paper presents an analysis of methane emissions from the Los Angeles Basin at monthly timescales across a 4-year time period - from September 2011 to August 2015. Using observations acquired by a ground-based near-infrared remote sensing instrument on Mount Wilson, California, combined with atmospheric CH4-CO2 tracer-tracer correlations, we observed -18 to +22% monthly variability in CH4: CO2 from the annual mean in the Los Angeles Basin. Top-down estimates of methane emissions for the basin also exhibit significant monthly variability (-19 to +31% from annual mean and a maximum month-to-month change of 47%). During this period, methane emissions consistently peaked in the late summer/early fall and winter. The estimated annual methane emissions did not show a statistically significant trend over the 2011 to 2015 time period. [ABSTRACT FROM AUTHOR]

An accurate understanding of urban air quality requires considering a coupled behavior between the dispersion of reactive pollutants and atmospheric dynamics. Currently, urban air pollution is mostly dominated by traffic emission, where nitrogen oxides (NOx) and volatile organic compounds (VOCs) are the primary emitted pollutants. However, modeling reactive pollutants with a large set of chemical reactions, using a computational fluid dynamic (CFD) model, requires a large amount of computational (CPU) time. In this sense, the selection of the chemical reactions needed in different atmospheric conditions becomes essential in finding the best compromise between CPU time and accuracy. The purpose of this work is to assess the differences in NO and NO2 concentrations by considering three chemical approaches: (a) passive tracers (non-reactive), (b) the NOx-O3 photostationary state and (c) a reduced complex chemical mechanism based on 23 species and 25 reactions. The appraisal of the effects of chemical reactions focuses on studying the NO and NO2 dispersion in comparison with the tracer behavior within the street. In turn, the effect of including VOC reactions is also analyzed taking into account several VOC/NOx ratios of traffic emission. Given that the NO and NO2 dispersion can also be affected by atmospheric conditions, such as wind flow or the background concentration from season-dependent pollutants, in this work the influence of wind speeds and background O3 concentrations are studied. The results show that the presence of ozone in the street plays an important role in NO and NO2 concentrations. Therefore, greater differences linked to the chemical approach used are found with higher O3 concentrations and faster wind speeds. This bears relation to the vertical flux as a function of ambient wind speed since it increases the pollutant exchange between the street and the overlying air. This detailed study allows one to ascertain under which atmospheric conditions the inclusion of chemical reactions are necessary for the study of NO and NO2 dispersion. The conclusions can be applied to future studies in order to establish the chemical reactions needed in terms of an accurate modeling of NO and NO2 dispersion and the CPU time required in a real urban area. [ABSTRACT FROM AUTHOR]

The usefulness of mercury (Hg) isotopes for tracing the sources and pathways of Hg (and its vectors) in atmospheric fine particles (PM2.5/ is uncertain. Here, we measured Hg isotopic compositions in 30 potential source materials and 23 PM2.5 samples collected in four seasons from the megacity Beijing (China) and combined the seasonal variation in both mass-dependent fractionation (represented by the ratio 202Hg/198Hg, δ202Hg) and mass-independent fractionation of isotopes with odd and even mass numbers (represented by Δ199Hg and Δ200Hg, respectively) with geochemical parameters and meteorological data to identify the sources of PM2.5-Hg and possible atmospheric particulate Hg transformation. All PM2.5 samples were highly enriched in Hg and other heavy metals and displayed wide ranges of both δ202Hg (-2.18 to 0.51 ‰) and Δ199Hg (-0.53 to 0.57 ‰), as well as small positive Δ200Hg (0.02 to 0.17 ‰). The results indicated that the seasonal variation in Hg isotopic composition (and elemental concentrations) was likely derived from variable contributions from anthropogenic sources, with continuous input due to industrial activities (e.g., smelting, cement production and coal combustion) in all seasons, whereas coal combustion dominated in winter and biomass burning mainly found in autumn. The more positive Δ199Hg of PM2.5-Hg in spring and early summer was likely derived from long-range-transported Hg that had undergone extensive photochemical reduction. The study demonstrated that Hg isotopes may be potentially used for tracing the sources of particulate Hg and its vectors in the atmosphere. [ABSTRACT FROM AUTHOR]

This study explores the interdecadal variability and trends of surface horizontal visibility at the urban area of Athens from 1931 to 2013, using the historical archives of the National Observatory of Athens (NOA). A prominent deterioration of visibility in the city was detected, with the long-term linear trend amounting to -2.8 km decade-1 (p < 0.001), over the entire study period. This was not accompanied by any significant trend in relative humidity or precipitation over the same period. A slight recovery of visibility levels seems to be established in the recent decade (2004- 2013). It was found that very good visibility (>20 km) occurred at a frequency of 34% before the 1950s, while this percentage drops to just 2% during the decade 2004-2013. The rapid impairment of the visual air quality in Athens around the 1950s points to the increased levels of air pollution on a local and/or regional scale, related to high urbanization rates and/or increased anthropogenic emissions on a global scale at that period. Visibility was found to be negatively/positively correlated with relative humidity/wind speed, the correlation being statistically valid at certain periods. Wind regime and mainly wind direction and corresponding air mass origin were found to highly control visibility levels in Athens. The comparison of visibility variation in Athens and at a non-urban reference site on Crete island revealed similar negative trends over the common period of observations. This suggests that apart local sources, visibility in Athens is highly determined by aerosol load of regional origin. AVHRR and MODIS satellite-derived aerosol optical depth (AOD) retrievals over Athens and surface measurements of PM10 confirmed the relation of visibility to aerosol load. [ABSTRACT FROM AUTHOR]

Winter has the worst air pollution of the year in the megacity of Beijing. Despite extensive winter studies in recent years, our knowledge of the sources, formation mechanisms and evolution of aerosol particles is not complete. Here we have a comprehensive characterization of the sources, variations and processes of submicron aerosols that were measured by an Aerodyne high-resolution aerosol mass spectrometer from 17 December 2013 to 17 January 2014 along with offline filter analysis by gas chromatography/ mass spectrometry. Our results suggest that submicron aerosols composition was generally similar across the winter of different years and was mainly composed of organics (60%), sulfate (15%) and nitrate (11%). Positive matrix factorization of high- and unit-mass resolution spectra identified four primary organic aerosol (POA) factors from traffic, cooking, biomass burning (BBOA) and coal combustion (CCOA) emissions as well as two secondary OA (SOA) factors. POA dominated OA, on average accounting for 56%, with CCOA being the largest contributor (20%). Both CCOA and BBOA showed distinct polycyclic aromatic hydrocarbons (PAHs) spectral signatures, indicating that PAHs in winter were mainly from coal combustion (66%) and biomass burning emissions (18%). BBOA was highly correlated with levoglucosan, a tracer compound for biomass burning (r² = 0:93), and made a considerable contribution to OA in winter (9%). An aqueous-phase-processed SOA (aq- OOA) that was strongly correlated with particle liquid water content, sulfate and S-containing ions (e.g. CH2SO+ 2) was identified. On average aq-OOA contributed 12% to the total OA and played a dominant role in increasing oxidation degrees of OA at high RH levels (> 50%). Our results illustrate that aqueous-phase processing can enhance SOA production and oxidation states of OA as well in winter. Further episode analyses highlighted the significant impacts of meteorological parameters on aerosol composition, size distributions, oxidation states of OA and evolutionary processes of secondary aerosols. [ABSTRACT FROM AUTHOR]

C1-C4 alkyl nitrates (RONO2) were measured concurrently at a mountain site, Tai Mo Shan (TMS), and an urban site, Tsuen Wan (TW), at the base of the same mountain in Hong Kong from September to November 2010. Although the levels of parent hydrocarbons were much lower at TMS (p <0.05), similar alkyl nitrate levels were found at both sites regardless of the elevation difference, suggesting various source contributions of alkyl nitrates at the two sites. Prior to using a positive matrix factorization (PMF) model, the data at TW were divided into "meso" and "non-meso" scenarios for the investigation of source apportionments with the influence of mesoscale circulation and regional transport, respectively. Secondary formation was the prominent contributor of alkyl nitrates in the meso scenario (60±2%, 60.2±1.2 pptv), followed by biomass burning and oceanic emissions, while biomass burning and secondary formation made comparable contributions to alkyl nitrates in the nonmeso scenario, highlighting the strong emissions of biomass burning in the inland Pearl River delta (PRD) region. In contrast to TW, the alkyl nitrate levels measured at TMS mainly resulted from the photooxidation of the parent hydrocarbons at TW during mesoscale circulation, i.e., valley breezes, corresponding to 52-86% of the alkyl nitrate levels at TMS. Furthermore, regional transport from the inland PRD region made significant contributions to the levels of alkyl nitrates (~58-82%) at TMS in the non-meso scenario, resulting in similar levels of alkyl nitrates observed at the two sites. The simulation of secondary formation pathways using a photochemical box model found that the reaction of alkyl peroxy radicals (RO2) with nitric oxide (NO) dominated the formation of RONO2 at both sites, and the formation of alkyl nitrates contributed negatively to O3 production, with average reduction rates of 4.1 and 4.7 pptv pptv-1 at TMS and TW, respectively. [ABSTRACT FROM AUTHOR]

The rugged surface of an urban area due to varying buildings can interact with solar beams and affect both the magnitude and spatiotemporal distribution of surface solar fluxes. Here we systematically examine the impact of buildings on downward surface solar fluxes over urban Beijing by using a 3-D radiation parameterization that accounts for 3-D building structures vs. the conventional plane-parallel scheme. We find that the resulting downward surface solar flux deviations between the 3-D and the plane-parallel schemes are generally ±1-10Wm-2 at 800m grid resolution and within ±1Wm-2 at 4 km resolution. Pairs of positive-negative flux deviations on different sides of buildings are resolved at 800m resolution, while they offset each other at 4 km resolution. Flux deviations from the unobstructed horizontal surface at 4 km resolution are positive around noon but negative in the early morning and late afternoon. The corresponding deviations at 800m resolution, in contrast, show diurnal variations that are strongly dependent on the location of the grids relative to the buildings. Both the magnitude and spatiotemporal variations of flux deviations are largely dominated by the direct flux. Furthermore, we find that flux deviations can potentially be an order of magnitude larger by using a finer grid resolution. Atmospheric aerosols can reduce the magnitude of downward surface solar flux deviations by 10-65%, while the surface albedo generally has a rather moderate impact on flux deviations. The results imply that the effect of buildings on downward surface solar fluxes may not be critically significant in mesoscale atmospheric models with a grid resolution of 4 km or coarser. However, the effect can play a crucial role in meso-urban atmospheric models as well as microscale urban dispersion models with resolutions of 1m to 1 km. [ABSTRACT FROM AUTHOR]

Traffic-related pollution is a major concern in urban areas due to its deleterious effects on human health. The characteristics of the traffic emissions on four highway environments in the Helsinki metropolitan area were measured with a mobile laboratory, equipped with state-of-the-art instrumentation. Concentration gradients were observed for all traffic-related pollutants, particle number (CN), particulate mass (PM1), black carbon (BC), organics, and nitrogen oxides (NO and NO2). Flow dynamics in different environments appeared to be an important factor for the dilution of the pollutants. For example, the half-decay distances for the traffic-related CN concentrations varied from 8 to 83m at different sites. The PM1 emissions from traffic mostly consisted of organics and BC. At the most open site, the ratio of organics to BC increased with distance to the highway, indicating condensation of volatile and semi-volatile organics on BC particles. These condensed organics were shown to be hydrocarbons as the fraction of hydrocarbon fragments in organics increased. Regarding the CN size distributions, particle growth during the dilution was not observed; however the mass size distributions measured with a soot particle aerosol mass spectrometer (SP-AMS), showed a visible shift of the mode, detected at ~ 100 nm at the roadside, to a larger size when the distance to the roadside increased. The fleet average emission factors appeared to be lower for the CN and higher for the NO2 than ten years ago. The reason is likely to be the increased fraction of light-duty (LD) diesel vehicles in the past ten years. The fraction of heavy-duty (HD) traffic, although constituting less than 10% of the total traffic flow, was found to have a large impact on the emissions. [ABSTRACT FROM AUTHOR]

Large urban emissions of greenhouse gases result in large atmospheric enhancements relative to background that are easily measured. Using CO2 mole fractions and Δ14C and δ13C values of CO2 in the Los Angeles megacity observed in inland Pasadena (2006-2013) and coastal Palos Verdes peninsula (autumn 2009-2013), we have determined time series for CO2 contributions from fossil fuel combustion (Cff) for both sites and broken those down into contributions from petroleum and/or gasoline and natural gas burning for Pasadena. We find a 10% reduction in Pasadena Cff during the Great Recession of 2008-2010, which is consistent with the bottom-up inventory determined by the California Air Resources Board. The isotopic variations and total atmospheric CO2 from our observations are used to infer seasonality of natural gas and petroleum combustion. The trend of CO2 contributions to the atmosphere from natural gas combustion is out of phase with the seasonal cycle of total natural gas combustion seasonal patterns in bottom-up inventories but is consistent with the seasonality of natural gas usage by the area's electricity generating power plants. For petroleum, the inferred seasonality of CO2 contributions from burning petroleum is delayed by several months relative to usage indicated by statewide gasoline taxes. Using the high-resolution Hestia-LA data product to compare Cff from parts of the basin sampled by winds at different times of year, we find that variations in observed fossil fuel CO2 reflect seasonal variations in wind direction. The seasonality of the local CO2 excess from fossil fuel combustion along the coast, on Palos Verdes peninsula, is higher in autumn and winter than spring and summer, almost completely out of phase with that from Pasadena, also because of the annual variations of winds in the region. Variations in fossil fuel CO2 signals are consistent with sampling the bottom-up Hestia-LA fossil CO2 emissions product for sub-city source regions in the LA megacity domain when wind directions are considered. [ABSTRACT FROM AUTHOR]

Knowledge on the microphysical properties of atmospheric aerosols is essential to better evaluate their radiative forcing. This paper presents an estimate of the real part of the refractive indices (n) and effective densities (ρeff) of chemically segregated atmospheric aerosols in Guangzhou, China. Vacuum aerodynamic diameter, chemical compositions, and light-scattering intensities of individual particles were simultaneously measured by a single-particle aerosol mass spectrometer (SPAMS) during the fall of 2012. On the basis of Mie theory, n at a wavelength of 532 nm and ρeff were estimated for 17 particle types in four categories: organics (OC), elemental carbon (EC), internally mixed EC and OC (ECOC), and Metal-rich. The results indicate the presence of spherical or nearly spherical shapes for the majority of particle types, whose partial scattering cross-section versus sizes were well fitted to Mie theoretical modeling results. While sharing n in a narrow range (1.47-1.53), majority of particle types exhibited a wide range of ρeff (0.87-1.51 g cm-3). The OC group is associated with the lowest ρeff (0.87-1.07 g cm-3), and the Metal-rich group with the highest ones (1.29-1.51 g cm-3). It is noteworthy that a specific EC type exhibits a complex scattering curve versus size due to the presence of both compact and irregularly shaped particles. Overall, the results on the detailed relationship between physical and chemical properties benefits future research on the impact of aerosols on visibility and climate. [ABSTRACT FROM AUTHOR]

The mixing layer is an important meteorological factor that affects air pollution. In this study, the atmospheric mixing layer height (MLH) was observed in Beijing from July 2009 to December 2012 using a ceilometer. By comparison with radiosonde data, we found that the ceilometer underestimates the MLH under conditions of neutral stratification caused by strong winds, whereas it overestimates the MLH when sand-dust is crossing. Using meteorological, PM2.5, and PM10 observational data, we screened the observed MLH automatically; the ceilometer observations were fairly consistent with the radiosondes, with a correlation coefficient greater than 0.9. Further analysis indicated that the MLH is low in autumn and winter and high in spring and summer in Beijing. There is a significant correlation between the sensible heat flux and MLH, and the diurnal cycle of the MLH in summer is also affected by the circulation of mountainous plain winds. Using visibility as an index to classify the degree of air pollution, we found that the variation in the sensible heat and buoyancy term in turbulent kinetic energy (TKE) is insignificant when visibility decreases from 10 to 5 km, but the reduction of shear term in TKE is near 70%. When visibility decreases from 5 to 1 km, the variation of the shear term in TKE is insignificant, but the decrease in the sensible heat and buoyancy term in TKE is approximately 60%. Although the correlation between the daily variation of the MLH and visibility is very poor, the correlation between them is significantly enhanced when the relative humidity increases beyond 80%. This indicates that humidity-related physicochemical processes is the primary source of atmospheric particles under heavy pollution and that the dissipation of atmospheric particles mainly depends on the MLH. The presented results of the atmospheric mixing layer provide useful empirical information for improving meteorological and atmospheric chemistry models and the forecasting and warning of air pollution. [ABSTRACT FROM AUTHOR]

During the Carbonaceous Aerosols and Radiative Effects Study (CARES) the DOE G-1 aircraft was used to sample aerosol and gas phase compounds in the Sacramento, CA plume and surrounding region. We present data from 66 plume transects obtained during 13 flights in which southwesterly winds transported the plume towards the foothills of the Sierra Nevada Mountains. Plume transport occurred partly over land with high isoprene emission rates. Our objective is to empirically determine whether organic aerosol (OA) can be attributed to anthropogenic or biogenic sources, and to determine whether there is a synergistic effect whereby OA concentrations are enhanced by the simultaneous presence of high concentrations of CO and either isoprene, MVK+MACR (sum of methyl vinyl ketone and methacrolein) or methanol, which are taken as tracers of anthropogenic and biogenic emissions, respectively. Linear and bilinear correlations between OA, CO, and each of three biogenic tracers, "Bio", for individual plume transects indicate that most of the variance in OA over short time and distance scales can be explained by CO. For each transect and species a plume perturbation, (i.e., ΔOA, defined as the difference between 90th and 10th percentiles) was defined and regressions done amongst Δ values in order to probe day to day and location dependent variability. Species that predicted the largest fraction of the variance in ΔOA were ΔO3 and ΔCO. Background OA was highly correlated with background methanol and poorly correlated with other tracers. Because background OA was ~ 60 % of peak OA in the urban plume, peak OA should be primarily biogenic and therefore non-fossil. Transects were split into subsets according to the percentile rankings of ΔCO and ΔBio, similar to an approach used by Setyan et al. (2012) and Shilling et al. (2013) to determine if anthropogenic-biogenic interactions enhance OA production. As found earlier, ΔOA in the data subset having high ΔCO and high ΔBio was several-fold greater than in other subsets. Part of this difference is consistent with a synergistic interaction between anthropogenic and biogenic precursors and part to an independent linear dependence of ΔOA on precursors. Highest values of ΔO3 also occur in the high ΔCO-high ΔBio data set, raising the possibility that the coincidence of high concentrations of anthropogenic and biogenic tracers as well as OA and O3 may be associated with high temperatures, clear skies, and poor ventilation in addition to specific interaction between anthropogenic and biogenic compounds. [ABSTRACT FROM AUTHOR]

Atmospheric aerosols exert highly uncertain impacts on radiative forcing and also have detrimental effects on human health. While aerosol particles are widely characterized in megacities in China, aerosol composition, sources and particle growth in rural areas in the Tibetan Plateau remain less understood. Here we present the results from an autumn study that was conducted from 5 September to 15 October 2013 at a national background monitoring station (3295ma.s.l.) in the Tibetan Plateau. The submicron aerosol composition and particle number size distributions were measured in situ with an Aerodyne Aerosol Chemical Speciation Monitor (ACSM) and a Scanning Mobility Particle Sizer (SMPS). The average mass concentration of submicron aerosol (PM1) is 11.4 μgm-3 (range: 1.0-78.4 μgm-3) for the entire study, which is much lower than observed at urban and rural sites in eastern China. Organics dominated PM1, accounting for 43% on average, followed by sulfate (28%) and ammonium (11%). Positive Matrix Factorization analysis of ACSM organic aerosol (OA) mass spectra identified an oxygenated OA (OOA) and a biomass burning OA (BBOA). The OOA dominated OA composition, accounting for 85% on average, 17% of which was inferred from aged BBOA. The BBOA contributed a considerable fraction of OA (15%) due to the burning of cow dung and straw in September. New particle formation and growth events were frequently observed (80% of time) throughout the study. The average particle growth rate is 2.0 nm h1 (range: 0.8- 3.2 nm h-1). By linking the evolution of particle number size distribution to aerosol composition, we found an elevated contribution of organics during particle growth periods and also a positive relationship between the growth rate and the fraction of OOA in OA, which potentially indicates an important role of organics in particle growth in the Tibetan Plateau. [ABSTRACT FROM AUTHOR]

Organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC) and main ions were measured in a total of 1510 PM2.5 daily aerosol samples collected from May 2008 to April 2013 in Athens, Greece. OC and EC concentrations were 2.1 ± 1.3 μgm-3 and 0.54 ± 0.39 μgm-3 , accounting for 11 ± 3 % and 3 ± 1 % of PM2.5 mass, respectively, with an average OC / EC ratio of 4.7 ± 3.1. Significant correlation was found between OC and EC during the whole period, indicating emissions by common primary sources on a regional scale. WSOC concentration ranged from 0.03 to 10.6pgm-3 , with an average of 1.5 ± 0.9 μgm-3 . By considering the Finokalia (Crete) station as a reference, it was estimated that, during the warm season in Athens, 67 ± 7% of emitted OC and 53 ± 12% of emitted EC is regional, while, during cold months, the regional contribution of OC is only 33 ± 7 % and of EC 29 ± 8 %. Furthermore, secondary organic carbon (SOC) was calculated for the warm period of the year (April to October). The estimated SOC constituted about 75 ± 6 % of PM2.5 organic carbon in Athens, highlighting significant aging processes on a regional scale. In the period 2011-2013 and during wintertime, an increase in OC and EC levels was observed, attributed to an increase in wood burning for domestic heating due to the economic crisis. [ABSTRACT FROM AUTHOR]

Daily PM2.5 (aerosol particles with an aerodynamic diameter of less than 2.5 μm) samples were collected at an urban site in Chengdu, an inland megacity in southwest China, during four 1-month periods in 2011, with each period in a different season. Samples were subject to chemical analysis for various chemical components ranging from major water-soluble ions, organic carbon (OC), element carbon (EC), trace elements to biomass burning tracers, anhydrosugar levoglucosan (LG), and mannosan (MN). Two models, the ISORROPIA II thermodynamic equilibrium model and the positive matrix factorization (PMF) model, were applied to explore the likely chemical forms of ionic constituents and to apportion sources for PM2.5. Distinctive seasonal patterns of PM2.5 and associated main chemical components were identified and could be explained by varying emission sources and meteorological conditions. PM2.5 showed a typical seasonality of waxing in winter and waning in summer, with an annual mean of 119 μgm-3. Mineral soil concentrations increased in spring, whereas biomass burning species elevated in autumn and winter. Six major source factors were identified to have contributed to PM2.5 using the PMF model. These were secondary inorganic aerosols, coal combustion, biomass burning, iron and steel manufacturing, Mo-related industries, and soil dust, and they contributed 37 ± 18, 20 ± 12, 11 ± 10, 11 ± 9, 11 ± 9, and 10 ± 12 %, respectively, to PM2.5 masses on annual average, while exhibiting large seasonal variability. On annual average, the unknown emission sources that were not identified by the PMF model contributed 1 ± 11 % to the measured PM2.5 mass. Various chemical tracers were used for validating PMF performance. Antimony (Sb) was suggested to be a suitable tracer of coal combustion in Chengdu. Results of LG and MN helped constrain the biomass burning sources, with wood burning dominating in winter and agricultural waste burning dominating in autumn. Excessive Fe (Ex-Fe), defined as the excessive portion in measured Fe that cannot be sustained by mineral dust, is corroborated to be a straightforward useful tracer of iron and steel manufacturing pollution. In Chengdu, Mo / Ni mass ratios were persistently higher than unity, and considerably distinct from those usually observed in ambient airs. V / Ni ratios averaged only 0.7. Results revealed that heavy oil fuel combustion should not be a vital anthropogenic source, and additional anthropogenic sources for Mo are yet to be identified. Overall, the emission sources identified in Chengdu could be dominated by local sources located in the vicinity of Sichuan, a result different from those found in Beijing and Shanghai, wherein cross-boundary transport is significant in contributing pronounced PM2.5. These results provided implications for PM2.5 control strategies. [ABSTRACT FROM AUTHOR]

During African Monsoon Multidisciplinary Analyses (AMMA) airborne measurements of ozone, CO and nitrogen oxides (NOx) were collected by French and German Falcon aircraft near three cities in West Africa (Cotonou, Niamey and Ouagadougou). They have been analysed to identify the good conditions to observe ozone plumes related to city emissions during the monsoon season. Results show that an O3 increase of 40-50 ppbv above the summer average concentration took place during two specific events: one near Cotonou on the coast of the Gulf of Guinea, and the other near Niamey in the Sahel region. In both cases a high level of NOx (3-5 ppbv) is related to the ozone production. Air mass transport simulations with FLEXPART and a tracer simulation with the BOLAM mesoscale model shows that Southern Hemisphere biomass burning emissions are always at higher altitude (>3 km) compared to the city emissions. In Niamey and Ouagadougou, the daily variability of ozone and CO correlates with the FLEXPART analysis showing the role of air mass stagnation near the city for 1-2 days and advection of emissions from the vegetated areas. Absence of ozone enhancements for high CO values can be explained by the occurrence of deep convection near the city. In the Sahel region, convection must be accounted for to understand the small number of observed ozone plumes but also to explain the high level of NOx in the 3-5 ppbv range, due to increasing soil emissions after rainfall. To verify that daily ozone production can reach 20 ppbv day-1 for the NOx and CO conditions encountered near West African cities, a simulation of the CiTTyCAT Lagrangian model was conducted using the observed average chemical composition reported by other aircraft during AMMA. Such ozone production is possible for NOx levels up to 5 ppb showing that West African cities are potentially significant sources of tropospheric ozone. [ABSTRACT FROM AUTHOR]