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Measurements at a background site near Beijing showed that pollution controls implemented during the 19th National Congress of the Communist Party of China (NCCPC) were effective in reducing PM 2.5. Mass concentrations of PM 2.5 and its major chemical components were 20.6 %–43.1 % lower during the NCCPC-control period compared with a non-control period, and differences were greater on days with stable meteorological conditions. A receptor model showed that PM 2.5 from traffic-related emissions, biomass burning, industrial processes, and mineral dust was 38.5 %–77.8 % lower during the NCCPC-control versus non-control period, but differences in PM 2.5 from coal burning were small, and secondary sources were higher during the NCCPC-control period. During one pollution episode in the non-control period, secondary sources dominated, and the WRF-Chem model showed that the Beijing–Tianjin–Hebei (BTH) region contributed 73.6 % of PM 2.5 mass. A second pollution episode was linked to biomass burning, and BTH contributed 46.9 % of PM 2.5 mass. Calculations based on Interagency Monitoring of Protected Visual Environments (IMPROVE) algorithms showed that organic matter was the largest contributor to light extinction during the non-control period whereas NH4NO3 was the main contributor during the NCCPC. The Tropospheric Ultraviolet and Visible radiation model showed that the average direct radiative forcing (DRF) values at the Earth's surface were -14.0 and -19.3 W m -2 during the NCCPC-control and non-control periods, respectively, and the DRF for the individual PM 2.5 components were 22.7 %–46.7 % lower during the NCCPC. The information and dataset from this study will be useful for developing air pollution control strategies in the BTH region and for understanding associated aerosol radiative effects. [ABSTRACT FROM AUTHOR]

It has been widely observed around the world that the frequency and intensity of new particle formation (NPF) events are reduced during periods of high relative humidity (RH). The current study focuses on how RH affects the formation of highly oxidized molecules (HOMs), which are key components of NPF and initial growth caused by oxidized organics. The ozonolysis of α -pinene, limonene, and Δ3 -carene, with and without OH scavengers, were carried out under low NOx conditions under a range of RH (from ∼3 % to ∼92 %) in a temperature-controlled flow tube to generate secondary organic aerosol (SOA). A Scanning Mobility Particle Sizer (SMPS) was used to measure the size distribution of generated particles, and a novel transverse ionization chemical ionization inlet with a high-resolution time-of-fight mass spectrometer detected HOMs. A major finding from this work is that neither the detected HOMs nor their abundance changed significantly with RH, which indicates that the detected HOMs must be formed from water-independent pathways. In fact, the distinguished OH - and O3 -derived peroxy radicals (RO2), HOM monomers, and HOM dimers could mostly be explained by the autoxidation of RO2 followed by bimolecular reactions with other RO2 or hydroperoxy radicals (HO2), rather than from a water-influenced pathway like through the formation of a stabilized Criegee intermediate (sCI). However, as RH increased from ∼3 % to ∼92 %, the total SOA number concentrations decreased by a factor of 2–3 while SOA mass concentrations remained relatively constant. These observations show that, while high RH appears to inhibit NPF as evident by the decreasing number concentration, this reduction is not caused by a decrease in RO2 -derived HOM formation. Possible explanations for these phenomena were discussed. [ABSTRACT FROM AUTHOR]

Numerical prediction of aerosol particle properties has become an important activity at many research and operational weather centers. This development is due to growing interest from a diverse set of stakeholders, such as air quality regulatory bodies, aviation and military authorities, solar energy plant managers, climate services providers, and health professionals. Owing to the complexity of atmospheric aerosol processes and their sensitivity to the underlying meteorological conditions, the prediction of aerosol particle concentrations and properties in the numerical weather prediction (NWP) framework faces a number of challenges. The modeling of numerous aerosol-related parameters increases computational expense. Errors in aerosol prediction concern all processes involved in the aerosol life cycle including (a) errors on the source terms (for both anthropogenic and natural emissions), (b) errors directly dependent on the meteorology (e.g., mixing, transport, scavenging by precipitation), and (c) errors related to aerosol chemistry (e.g., nucleation, gas-aerosol partitioning, chemical transformation and growth, hygroscopicity). Finally, there are fundamental uncertainties and significant processing overhead in the diverse observations used for verification and assimilation within these systems. Indeed, a significant component of aerosol forecast development consists in streamlining aerosol-related observations and reducing the most important errors through model development and data assimilation. Aerosol particle observations from satellite- and groundbased platforms have been crucial to guide model development of the recent years and have been made more readily available for model evaluation and assimilation. However, for the sustainability of the aerosol particle prediction activities around the globe, it is crucial that quality aerosol observations continue to be made available from different platforms (space, near surface, and aircraft) and freely shared. This paper reviews current requirements for aerosol observations in the context of the operational activities carried out at various global and regional centers. While some of the requirements are equally applicable to aerosol-climate, the focus here is on global operational prediction of aerosol properties such as mass concentrations and optical parameters. It is also recognized that the term "requirements" is loosely used here given the diversity in global aerosol observing systems and that utilized data are typically not from operational sources. Most operational models are based on bulk schemes that do not predict the size distribution of the aerosol particles. Others are based on a mix of "bin" and bulk schemes with limited capability of simulating the size information. However the next generation of aerosol operational models will output both mass and number density concentration to provide a more complete description of the aerosol population. A brief overview of the state of the art is provided with an introduction on the importance of aerosol prediction activities. The criteria on which the requirements for aerosol observations are based are also outlined. Assimilation and evaluation aspects are discussed from the perspective of the user requirements. [ABSTRACT FROM AUTHOR]

In the present study, the WRF-Chem model is used to assess contributions of residential coal combustion (RCC) emissions to the air quality in Beijing-Tianjin-Hebei (BTH) during a persistent air pollution episode from 9 to 25 January 2014. In general, the predicted temporal variations and spatial distributions of the mass concentrations of air pollutants are in good agreement with observations at monitoring sites in BTH. The WRF-Chem model also reasonably reproduces the temporal variations in aerosol species when compared with the aerosol mass spectrometer measurements in Beijing. The RCC emissions play an important role in the haze formation in BTH, contributing about 23.1% of PM2.5 (fine particulate matter) and 42.6% of SO2 during the simulation period on average. Organic aerosols dominate the PM2.5 from the RCC emissions in BTH, with a contribution of 42.8 %, followed by sulfate (17.1 %). The air quality in Beijing is remarkably improved when the RCC emissions in BTH and the surrounding areas are excluded in model simulations, with a 30% decrease in PM2.5 mass concentrations. However, if only the RCC emissions in Beijing are excluded, the local PM2.5 mass concentration is decreased by 18.0%on average. Our results suggest that the implementation of the residential coal replacement by clean energy sources in Beijing is beneficial to the local air quality. Should residential coal replacement be carried out in BTH and its surrounding areas, the air quality in Beijing would be improved remarkably. Further studies would need to consider uncertainties in the emission inventory and meteorological fields. [ABSTRACT FROM AUTHOR]

The features of upper-air visibility at altitudes of 0.1, 0.3, and 0.5 km and the two-dimensional haze characteristics in the northwest of downtown Beijing were studied by using a multi-platform analysis during haze episodes between 17 December 2016 and 6 January 2017. Through the multi-platform data analysis in hourly and daily variation, the upper-air visibility increased along with the decrease of PM2:5 mass concentration. And the upper-air visibility on non-haze days was about 3-5 times higher than that on haze days with the ground-based Raman-Mie lidar data between 13 December 2016 and 11 January 2017. The vertical transport of pollutants can be inferred from the delayed variation of upper-air visibility between high altitude and low altitude. In addition, the two-dimensional haze characteristics could be studied by analyzing the correlation between vertical haze parameters (atmospheric boundary layer, haze thickness, and aerosol optical thickness) and horizontal haze parameter (upper-air visibility). The characteristics of multi-parameters have been analyzed and concluded for different haze levels. [ABSTRACT FROM AUTHOR]

Two optical scattering instruments for particle mass measurement, the Thermo Personal Data RAM (PDR-1500) and the TSI Environmental DustTrak DRX (Model 8543) were evaluated by (1) using poly- and mono-disperse test aerosol in the laboratory, and (2) sampling ambient aerosol. The responses of these optical scattering instruments to different particle characteristics (size, composition, concentration) were compared with responses from reference instruments. A Mie scattering calculation was used to explain the dependence of the optical instruments' response to aerosol size and composition. Concurrently, the detection efficiency of one Alphasense Optical Particle Counter (OPCN2) was evaluated in the laboratory as well. The relationship between aerosol mass concentration and optical scattering was determined to be strongly dependent on aerosol size and to a lesser extent on aerosol composition (as reflected in the refractive indices of the materials tested) based on ambient measurements. This confirms that there is no simple way to use optical scattering instruments over a wide range of conditions without adjustments based on knowledge of aerosol size and composition. In particular, a test period measuring ambient aerosol with optical scattering instruments and a mass based method (an Aerodyne Aerosol Mass Spectrometer) determined that roughly two thirds of the variance (R2 = 0:64) of the optical to mass signal ratio is explained by the aerosol mass median diameter alone. These observations and calculations help evaluate the applicability and limitations of these optical scattering instruments, and provide guidance to designing suitable applications for each instrument by considering aerosol sources and aerosol size. [ABSTRACT FROM AUTHOR]

Air quality and visibility are strongly influenced by aerosol loading, which is driven by meteorological conditions. The quantification of their relationships is critical to understanding the physical and chemical processes and forecasting of the polluted events. We investigated and quantified the relationship between PM2:5 (particulate matter with aerodynamic diameter is 2.5 μm and less) mass concentration, visibility and planetary boundary layer (PBL) height in this study based on the data obtained from four long-lasting haze events and seven fog-haze mixed events from January 2014 to March 2015 in Beijing. The statistical results show that there was a negative exponential function between the visibility and the PM2:5 mass concentration for both haze and fog-haze mixed events (with the same R2 of 0.80). However, the fog-haze events caused a more obvious decrease of visibility than that for haze events due to the formation of fog droplets that could induce higher light extinction. The PM2:5 concentration had an inversely linear correlation with PBL height for haze events and a negative exponential correlation for fog-haze mixed events, indicating that the PM2:5 concentration is more sensitive to PBL height in fog-haze mixed events. The visibility had positively linear correlation with the PBL height with an R2 of 0.35 in haze events and positive exponential correlation with an R2 of 0.56 in fog- haze mixed events. We also investigated the physical mechanism responsible for these relationships between visibility, PM2:5 concentration and PBL height through typical haze and fog-haze mixed event and found that a double inversion layer formed in both typical events and played critical roles in maintaining and enhancing the long-lasting polluted events. The variations of the double inversion layers were closely associated with the processes of long-wave radiation cooling in the nighttime and short-wave solar radiation reduction in the daytime. The upper-level stable inversion layer was formed by the persistent warm and humid southwestern airflow, while the low-level inversion layer was initially produced by the surface long-wave radiation cooling in the nighttime and maintained by the reduction of surface solar radiation in the daytime. The obvious descending process of the upper-level inversion layer induced by the radiation process could be responsible for the enhancement of the lowlevel inversion layer and the lowering PBL height, as well as high aerosol loading for these polluted events. The reduction of surface solar radiation in the daytime could be around 35% for the haze event and 94% for the fog-haze mixed event. Therefore, the formation and subsequent descending processes of the upper-level inversion layer should be an important factor in maintaining and strengthening the longlasting severe polluted events, which has not been revealed in previous publications. The interactions and feedbacks between PM2:5 concentration and PBL height linked by radiation process caused a more significant and long-lasting de- terioration of air quality and visibility in fog-haze mixed events. The interactions and feedbacks of all processes were particularly strong when the PM2:5 mass concentration was larger than 150-200 μgm-3. [ABSTRACT FROM AUTHOR]

Beta-attenuation monitors are used worldwide to monitor PM mass concentration with high temporal resolution. Hourly PM10 and PM2.5 dry mass concentrations are publicly available with the tacit assumption that water is effectively removed prior to the measurement. However, as both the filter material of the monitor and the aerosol particles are capable of retaining a significant amount of water even at low relative humidities, the basic assumption may not be valid, resulting in significant bias in reported PM10 and PM2.5 concentrations. Here we show that in PM10 measurement, particle-free air can produce apparent hourly average PM concentrations in the range of 13+21 μg m-3 under conditions of fluctuating relative humidity. Positive and negative apparent readings are observed with increasing and decreasing relative humidities, respectively. Similar phenomena have been observed when the instrument filter was previously loaded with atmospheric aerosol. As a result the potential measurement biases in hourly readings arising from the interaction with water may be in the range of 53...+69%. [ABSTRACT FROM AUTHOR]

Monitoring PM2.5 (particulate matter with aerodynamic diameter d ≤2.5 μm) mass concentration has become of more importance recently because of the negative impacts of fine particles on human health. However, monitoring PM2.5 during cloudy and nighttime periods is difficult since nearly all the passive instruments used for aerosol remote sensing are not able to measure aerosol optical depth (AOD) under either cloudy or nighttime conditions. In this study, an empirical model based on the regression between PM2.5 and the near-surface backscatter measured by ceilometers was developed and tested using 6 years of data (2006 to 2011) from the Howard University Beltsville Campus (HUBC) site. The empirical model can explain ~56, ~34 and ~42% of the variability in the hourly average PM2.5 during daytime clear, daytime cloudy and nighttime periods, respectively. Meteorological conditions and seasons were found to influence the relationship between PM2.5 mass concentration and the surface backscatter. Overall the model can explain ~48% of the variability in the hourly average PM2.5 at the HUBC site when considering the seasonal variation. The model also was tested using 4 years of data (2012 to 2015) from the Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) site, which was geographically and climatologically different from the HUBC site. The results show that the empirical model can explain ~66 and ~82% of the variability in the daily average PM2.5 at the ARM SGP site and HUBC site, respectively. The findings of this study illustrate the strong need for ceilometer data in air quality monitoring under cloudy and nighttime conditions. Since ceilometers are used broadly over the world, they may provide an important supplemental source of information of aerosols to determine surface PM2.5 concentrations. [ABSTRACT FROM AUTHOR]

We applied a global three-dimensional chemical transport model (GEOS-Chem) to examine the impacts of the East Asian monsoon on the interannual variations of mass concentrations and direct radiative forcing (DRF) of black carbon (BC) over eastern China (110-125° E, 20-45° N). With emissions fixed at the year 2010 levels, model simulations were driven by the Goddard Earth Observing System (GEOS-4) meteorological fields for 1986-2006 and the Modern Era Retrospective-analysis for Research and Applications (MERRA) meteorological fields for 1980-2010. During the period of 1986-2006, simulated June-July-August (JJA) and December-January-February (DJF) surface BC concentrations were higher in MERRA than in GEOS-4 by 0.30 μg m-3 (44 %) and 0.77 μg m-3 (54 %), respectively, because of the generally weaker precipitation in MERRA. We found that the strength of the East Asian summer monsoon (EASM; East Asian winter monsoon, EAWM) negatively correlated with simulated JJA (DJF) surface BC concentrations (r = -0.7 (-0.7) in GEOS-4 and -0.4 (-0.7) in MERRA), mainly by the changes in atmospheric circulation. Relative to the 5 strongest EASM years, simulated JJA surface BC concentrations in the 5 weakest monsoon years were higher over northern China (110-125° E, 28-45° N) by 0.04-0.09 μg m-3 (3-11 %), but lower over southern China (110-125° E, 20-27° N) by 0.03-0.04 μg m-3 (10-11 %). Compared to the 5 strongest EAWM years, simulated DJF surface BC concentrations in the 5 weakest monsoon years were higher by 0.13-0.15 μg m-3 (5-8 %) in northern China and by 0.04-0.10 μg m-3 (3-12 %) in southern China. The resulting JJA (DJF) mean all-sky DRF of BC at the top of the atmosphere was 0.04 W m-2 (3 %; 0.03 W m-2, 2 %) higher in northern China but 0.06 W m-2 (14 %; 0.03 W m-2, 3 %) lower in southern China. In the weakest monsoon years, the weaker vertical convection at the elevated altitudes led to the lower BC concentrations above 1-2 km in southern China, and therefore the lower BC DRF in the region. The differences in vertical profiles of BC between the weakest and strongest EASM years (1998-1997) and EAWM years (1990-1996) reached up to -0.09 μg m-3 (-46 %) and -0.08 μg m-3 (-11 %) at 1-2 km in eastern China. [ABSTRACT FROM AUTHOR]

The aim of this study is to investigate the seasonal variations in the physicochemical properties of atmospheric ultra-fine particles (UFPs, d ≤ 100 nm) and submicron particles (PM1, d ≤ 1 μm) in an east Asian urban area, which are hypothesized to be affected by the interchange of summer and winter monsoons. An observation experiment was conducted at TARO (Taipei Aerosol and Radiation Observatory), an urban aerosol station in Taipei, Taiwan, from October 2012 to August 2013. The measurements included the mass concentration and chemical composition of UFPs and PM1, as well as the particle number concentration (PNC) and the particle number size distribution (PSD) with size range of 4-736 nm. The results indicated that the mass concentration of PM1 was elevated during cold seasons with a peak level of 18.5 μgm-3 in spring, whereas the highest concentration of UFPs was measured in summertime with a mean of 1.64 μgm-3. Moreover, chemical analysis revealed that the UFPs and PM1 were characterized by distinct composition; UFPs were composed mostly of organics, whereas ammonium and sulfate were the major constituents of PM1. The seasonal median of total PNCs ranged from 13.9×10³ cm-3 in autumn to 19.4×103 cm-3 in spring. Median concentrations for respective size distribution modes peaked in different seasons. The nucleationmode PNC (N4-25) peaked at 11.6×10³ cm-3 in winter, whereas the Aitken-mode (N25-100) and accumulation-mode (N100-736) PNC exhibited summer maxima at 6.0×10³ and 3.1×10³ cm-3, respectively. The change in PSD during summertime was attributed to the enhancement in the photochemical production of condensable organic matter that, in turn, contributed to the growth of aerosol particles in the atmosphere. In addition, clear photochemical production of particles was observed, mostly in the summer season, which was characterized by average particle growth and formation rates of 4.0×1.1 nm h-1 and 1.4×0.8 cm-3 s-1, respectively. The prevalence of new particle formation (NPF) in summer was suggested as a result of seasonally enhanced photochemical oxidation of SO2 that contributed to the production of H2SO4, and a low level of PM10 (d ≤ 10 μm) that served as the condensation sink. Regarding the sources of aerosol particles, correlation analysis of the PNCs against NOx revealed that the local vehicular exhaust was the dominant contributor of the UFPs throughout the year. Conversely, the Asian pollution outbreaks had significant influence in the PNC of accumulation-mode particles during the seasons of winter monsoons. The results of this study implied the significance of secondary organic aerosols in the seasonal variations of UFPs and the influences of continental pollution outbreaks in the downwind areas of Asian outflows. [ABSTRACT FROM AUTHOR]

Four years of continuous aerosol number size distribution measurements from the Arctic Climate Observatory in Tiksi, Russia, are analyzed. Tiksi is located in a region where in situ information on aerosol particle properties has not been previously available. Particle size distributions were measured with a differential mobility particle sizer (in the diameter range of 7-500 nm) and with an aerodynamic particle sizer (in the diameter range of 0.5-10 μm). Source region effects on particle modal features and number, and mass concentrations are presented for different seasons. The monthly median total aerosol number concentration in Tiksi ranges from 184 cm-3 in November to 724 cm-3 in July, with a local maximum in March of 481 cm-3. The total mass concentration has a distinct maximum in February-March of 1.72- 2.38 μg m-3 and two minimums in June (0.42 μgm-3) and in September-October (0.36-0.57 μgm-3). These seasonal cycles in number and mass concentrations are related to isolated processes and phenomena such as Arctic haze in early spring, which increases accumulation and coarse-mode numbers, and secondary particle formation in spring and summer, which affects the nucleation and Aitken mode particle concentrations. Secondary particle formation was frequently observed in Tiksi and was shown to be slightly more common in marine, in comparison to continental, air flows. Particle formation rates were the highest in spring, while the particle growth rates peaked in summer. These results suggest two different origins for secondary particles, anthropogenic pollution being the important source in spring and biogenic emissions being significant in summer. The impact of temperature-dependent natural emissions on aerosol and cloud condensation nuclei numbers was significant: the increase in both the particle mass and the CCN (cloud condensation nuclei) number with temperature was found to be higher than in any previous study done over the boreal forest region. In addition to the precursor emissions of biogenic volatile organic compounds, the frequent Siberian forest fires, although far away, are suggested to play a role in Arctic aerosol composition during the warmest months. Five fire events were isolated based on clustering analysis, and the particle mass and cloud condensation nuclei number were shown to be somewhat affected by these events. In addition, during calm and cold months, aerosol concentrations were occasionally increased by local aerosol sources in trapping inversions. These results provide valuable information on interannual cycles and sources of Arctic aerosols. [ABSTRACT FROM AUTHOR]

Real-time mass spectra of the non-refractory species in submicron aerosol particles were recorded in a tropical rainforest in the central Amazon Basin during the wet season from February to March 2008, as a part of the Amazonian Aerosol Characterization Experiment (AMAZE- 08). Organic material accounted on average for more than 80% of the non-refractory submicron particle mass concentrations during the period of measurements. There was insufficient ammonium to neutralize sulfate. In this acidic, isoprene-rich, HO2-dominant environment, positive-matrix factorization of the time series of particle mass spectra identified four statistical factors to account for the 99% of the variance in the signal intensities of the organic constituents. The first factor was identified as associated with regional and local pollution and labeled "HOA" for its hydrocarbon-like characteristics. A second factor was associated with longrange transport and labeled "OOA-1" for its oxygenated characteristics. A third factor, labeled "OOA-2," was implicated as associated with the reactive uptake of isoprene oxidation products, especially of epoxydiols to acidic haze, fog, or cloud droplets. A fourth factor, labeled "OOA-3," was consistent with an association with the fresh production of secondary organic material (SOM) by the mechanism of gasphase oxidation of biogenic volatile organic precursors followed by gas-to-particle conversion of the oxidation products. The suffixes 1, 2, and 3 on the OOA labels signify ordinal ranking with respect to the extent of oxidation represented by the factor. The process of aqueous-phase oxidation of water-soluble products of gas-phase photochemistry might also have been associated to some extent with the OOA-2 factor. The campaign-average factor loadings had a ratio of 1:4 V 1 for OOA-2 VOOA-3, suggesting the comparable importance of particle-phase compared to gas-phase pathways for the production of SOM during the study period. [ABSTRACT FROM AUTHOR]

Multi-wavelength depolarization Raman lidar measurements from Magurele, Romania are used in this study along with simulated mass-extinction efficiencies to calculate the mass concentration profiles of different atmospheric components, due to their different depolarization contribution to the 532 nm backscatter coefficient. Linear particle depolarization ratio (δpart) was computed using the relative amplification factor and the system-dependent molecular depolarization. The low depolarizing component was considered as urban/smoke, with a mean δpart of 3 %, while for the high depolarizing component (mineral dust) a mean δpart of 35% was assumed. For this study 11 months of lidar measurements were analysed. Two study cases are presented in details: one for a typical Saharan dust aerosol intrusion, 10 June 2012 and one for 12 July 2012 when a lofted layer consisting of biomass burning smoke extended from 3 to 4.5 km height. Optical Properties of Aerosols and Clouds software package (OPAC) classification and conversion factors were used to calculate mass concentrations. We found that calibrated depolarization measurements are critical in distinguishing between smoke-reach aerosol during the winter and dustreach aerosol during the summer, as well as between elevated aerosol layers having different origins. Good agreement was found between lidar retrievals and DREAM- Dust REgional Atmospheric Model forecasts in cases of Saharan dust. Our method was also compared against LIRIC (The Lidar/Radiometer Inversion Code) and very small differences were observed. [ABSTRACT FROM AUTHOR]