Black-carbon (BC) aerosol can strongly influence planetary boundary layer (PBL) development and thus severe haze formation, but its distinct role compared with scattering aerosols is not yet fully understood. Here, combining numerical simulation and field observation, we found a "tipping point,"where the daily maximum PBL height decreases abruptly when exceeding a critical threshold of aerosol optical depth (AOD), due to a BC-induced decoupling of mixing zones. Because the threshold AOD decreases with increasing BC mass fraction, our results suggest that the abrupt transition of PBL development to adverse conditions can be avoided by reducing the AOD below the threshold but can be avoided more efficiently by reducing the BC mass fraction to increase the threshold (e.g., up to four to six times more effective in extreme haze events in Beijing). To achieve co-benefits for air quality and climate change, our findings clearly demonstrate that high priority should be given to controlling BC emissions.

Nucleation and condensation associated with biogenic volatile organic compounds (BVOCs) are important aerosol formation pathways, yet their contribution to the upper-tropospheric aerosols remains inconclusive, hindering the understanding of aerosol climate effects. Here, we develop new schemes describing these organic aerosol formation processes in the WRF-Chem model and investigate their impact on the abundance of cloud condensation nuclei (CCN) in the upper troposphere (UT) over the Amazon Basin. We find that the new schemes significantly increase the simulated CCN number concentrations in the UT (e.g., up to ∼ 400 cm−3 at 0.52 % supersaturation) and greatly improve the agreement with the aircraft observations. Organic condensation enhances the simulated CCN concentration by 90 % through promoting particle growth, while organic nucleation, by replenishing new particles, contributes an additional 14 %. Deep convection determines the rate of these organic aerosol formation processes in the UT through controlling the upward transport of biogenic precursors (i.e., BVOCs). This finding emphasizes the importance of the biosphere–atmosphere coupling in regulating upper-tropospheric aerosol concentrations over the tropical forest and calls for attention to its potential role in anthropogenic climate change.

Biomass burning (BB) aerosols can influence regional and global climate through interactions with radiation, clouds, and precipitation. Here, we investigate the impact of BB aerosols on the energy balance and hydrological cycle over the Amazon Basin during the dry season. We performed WRF-Chem simulations for a range of different BB emission scenarios to explore and characterize nonlinear effects and individual contributions from aerosol–radiation interactions (ARIs) and aerosol–cloud interactions (ACIs). For scenarios representing the lower and upper limits of BB emission estimates for recent years (2002–2016), we obtained total regional BB aerosol radiative forcings of -0.2 and 1.5Wm-2, respectively, showing that the influence of BB aerosols on the regional energy balance can range from modest cooling to strong warming. We find that ACIs dominate at low BB emission rates and low aerosol optical depth (AOD), leading to an increased cloud liquid water path (LWP) and negative radiative forcing, whereas ARIs dominate at high BB emission rates and high AOD, leading to a reduction of LWP and positive radiative forcing. In all scenarios, BB aerosols led to a decrease in the frequency of occurrence and rate of precipitation, caused primarily by ACI effects at low aerosol loading and by ARI effects at high aerosol loading. Overall, our results show that ACIs tend to saturate at high aerosol loading, whereas the strength of ARIs continues to increase and plays a more important role in highly polluted episodes and regions. This should hold not only for BB aerosols over the Amazon, but also for other light-absorbing aerosols such as fossil fuel combustion aerosols in industrialized and densely populated areas. The importance of ARIs at high aerosol loading highlights the need for accurately characterizing aerosol optical properties in the investigation of aerosol effects on clouds, precipitation, and climate.

Understanding the formation mechanism of severe haze is crucial for the development of efficient pollution control strategy. Recently, multiphase reactions in aerosol water has been suggested as an important source of sulfate aerosol during severe haze (Zheng et al., 2015;Cheng et al., 2016). Though several oxidation mechanisms have been recognized, the dominant oxidation pathway is still under debate reflecting a missing consensus. Based on a model survey with Weather Research and Forecasting model coupled with Chemistry (WRF-Chem), we have investigated the variability of aerosol pH and regimes of sulfate formation through multiphase oxidation during the haze episodes in January of 2013. Our results show a large spatial and temporal variability in the aerosol pH and sulfate formation regimes. Surface aerosol pH shows a clear diurnal variation with low pH during daytime and high pH during night-time for most cases. Aerosol pH tends to decrease with increasing altitude in the lower atmosphere. For the scenario best reproduces the observations in Beijing, NO2, TMI+O2, O3 and H2O2 pathways can all dominate the production of sulfate in specific areas of the Beijing-Tianjin-Hebei (BTH) region. With the increasing height, O3 pathway and gas phase oxidation by OH radicals become more important. Moreover, sensitivity tests also suggest that, emissions of crustal particles, NH3 and soluble iron/manganese have great impacts on aqueous phase chemistry, and should be better constrained in future studies. References: Zheng, G. J., Duan, F. K., Su, H., Ma, Y. L., Cheng, Y., Zheng, B., Zhang, Q., Huang, T., Kimoto, T., Chang, D., Poschl, U., Cheng, Y. F., and He, K. B.: Exploring the severe winter haze in Beijing: the impact of synoptic weather, regional transport and heterogeneous reactions, Atmos. Chem. Phys., 15, 2969-2983, 10.5194/acp-15-2969-2015, 2015. Cheng, Y. F., Zheng, G. J., Wei, C., Mu, Q., Zheng, B., Wang, Z. B., Gao, M., Zhang, Q., He, K. B., Carmichael, G., Poschl, U., and Su, H.: Reactive nitrogen chemistry in aerosol water as a source of sulfate during haze events in China, Sci Adv, 2, e1601530, UNSP e1601530,10.1126/sciadv.1601530, 2016.

Understanding the mechanism of haze formation is crucial for the development of deliberate pollution control strategies. Multiphase chemical reactions in aerosol water have been suggested as an important source of particulate sulfate during severe haze (Cheng et al., 2016;Wang et al., 2016). While the key role of aerosol water has been commonly accepted, the relative importance of different oxidation pathways in the aqueous phase is still under debate, mainly due to questions about aerosol pH. To investigate the spatio-temporal variability of aerosol pH and sulfate formation during winter in the North China Plain (NCP), we have developed a new aerosol water chemistry module (AWAC) for the WRF-Chem model (Weather Research and Forecasting model coupled with Chemistry). Using the WRF-Chem-AWAC model, we performed a comprehensive survey of the atmospheric conditions characteristic for wintertime in the NCP, focusing on January 2013. We find that aerosol pH exhibited a strong vertical gradient and distinct diurnal cycle, which was closely associated with the spatio-temporal variation in the relative abundance of acidic and alkaline fine particle components and their gaseous counterparts. Over Beijing, the average aerosol pH at the surface layer was ~5.4 and remained nearly constant around ~5 up to ~2 km above ground level; further aloft, the acidity rapidly increased to pH ~0 at ~3 km. The pattern of aerosol acidity increase with altitude persisted over the NCP, while the specific levels and gradients of pH varied between different regions. In the region north of ~41°N, the mean pH values at surface level were typically >6 and the main pathway of sulfate formation in aerosol water was S(IV) oxidation by ozone. South of ~41°N, the mean pH values at surface level were typically in the range of 4.4 to 5.7, and different chemical regimes and reaction pathways of sulfate formation prevailed in four different regions, depending on reactant concentrations and atmospheric conditions. The NO2 reaction pathway prevailed in the megacity region of Beijing and the large area of Hebei Province to the south and west of Beijing, as well as part of Shandong Province. The transition metal ion (TMI) pathway dominated in the inland region to the west and the coastal regions to the east of Beijing, and the H2O2 pathway dominated in the region extending further south (Shandong and Henan Provinces). In all of these regions, the O3 and TMI pathways in aerosol water as well as the gas-particle partitioning of H2SO4 vapor became more important with increasing altitude. Although pH is sensitive to the abundance of NH3 and crustal particles, we show that the rapid production of sulfate in the NCP can be maintained over a wide range of aerosol acidity (e.g., pH = 4.2-5.7) with transitions from TMI pathway dominated to NO2/O3 pathway dominated regimes.

Biomass burning (BB) aerosols can influence regional and global climate through interactions with radiation, clouds, and precipitation. Here, we investigate the impact of BB aerosols on the energy balance and hydrological cycle over the Amazon Basin during the dry season. We performed simulations with a fully coupled meteorology–chemistry model, the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem), for a range of different BB emission scenarios to explore and characterize nonlinear effects and individual contributions from aerosol–radiation interactions (ARIs) and aerosol–cloud interactions (ACIs). The ARIs of BB aerosols tend to suppress low-level liquid clouds by local warming and increased evaporation and to facilitate the formation of high-level ice clouds by enhancing updrafts and condensation at high altitudes. In contrast, the ACIs of BB aerosol particles tend to enhance the formation and lifetime of low-level liquid clouds by providing more cloud condensation nuclei (CCN) and to suppress the formation of high-level ice clouds by reducing updrafts and condensable water vapor at high altitudes (>8 km). For scenarios representing the lower and upper limits of BB emission estimates for recent years (2002–2016), we obtained total regional BB aerosol radiative forcings of −0.2 and 1.5 W m−2, respectively, showing that the influence of BB aerosols on the regional energy balance can range from modest cooling to strong warming. We find that ACIs dominate at low BB emission rates and low aerosol optical depth (AOD), leading to an increased cloud liquid water path (LWP) and negative radiative forcing, whereas ARIs dominate at high BB emission rates and high AOD, leading to a reduction of LWP and positive radiative forcing. In all scenarios, BB aerosols led to a decrease in the frequency of occurrence and rate of precipitation, caused primarily by ACI effects at low aerosol loading and by ARI effects at high aerosol loading. The dependence of precipitation reduction on BB aerosol loading is greater in a strong convective regime than under weakly convective conditions. Overall, our results show that ACIs tend to saturate at high aerosol loading, whereas the strength of ARIs continues to increase and plays a more important role in highly polluted episodes and regions. This should hold not only for BB aerosols over the Amazon, but also for other light-absorbing aerosols such as fossil fuel combustion aerosols in industrialized and densely populated areas. The importance of ARIs at high aerosol loading highlights the need for accurately characterizing aerosol optical properties in the investigation of aerosol effects on clouds, precipitation, and climate.

Natural sea-salt aerosols, when interacting with anthropogenic emissions, can enhance the formation of particulate nitrate. This enhancement has been suggested to increase the direct radiative forcing of nitrate, called the “mass-enhancement effect”. Through a size-resolved dynamic mass transfer modeling approach, we show that interactions with sea salt shift the nitrate from sub- to super-micron-sized particles (“redistribution effect”), and hence this lowers its efficiency for light extinction and reduces its lifetime. The redistribution effect overwhelms the mass-enhancement effect and significantly moderates nitrate cooling; e.g., the nitrate-associated aerosol optical depth can be reduced by 10 %–20 % over European polluted regions during a typical sea-salt event, in contrast to an increase by ∼10 % when only accounting for the mass-enhancement effect. Global model simulations indicate significant redistribution over coastal and offshore regions worldwide. Our study suggests a strong buffering by natural sea-salt aerosols that reduces the climate forcing of anthropogenic nitrate, which had been expected to dominate the aerosol cooling by the end of the century. Comprehensive considerations of this redistribution effect foster better understandings of climate change and nitrogen deposition.

Based on the observational data of the volume fractions of ozone, NOx and VOCs in the near surface layer were over the urban area of Xuzhou from 2013 to 2016. This research studied the characteristics of ozone concentration variation and its relationship with the concentration of the precursors. The result shows that the concentration of ozone from May to August is higher than in other months, and the highest concentration occurredin June. In general, ozone concentration is higher, in summer and autumn than that in spring and winter. ozone concentration exceeded mainly in May and June. The diurnal variation of ozone concentration has a single peak in afternoon . With higher solar radiation intensity , ozone concentration increased from 8 to 12 in the morning. Affected by solar radiation and city traffic, the diurnal variation of NOx and VOCs has two peaks. Because of photochemical reactions, NOx and VOCs were negatively correlated with ozone concentration. VOCs / NOx discriminant method was used to get the sensitive control factors of ozone. The results showed that the ozone generation in Xuzhou urban district was sensitive to VOCs, and belonged to VOCs control area in summer. Alkanes, olefins and aromatics are the main substances generating ozone in urban atmosphere of Xuzhou.

以江苏省徐州市为研究对象,从徐州市大气污染源排放、区域地理位置及地形、地貌、本地污染物积聚与区域性污染物输入等方面来分析对空气质量的影响,找出造成徐州市重污染天气的形成途径,从而提出有针对性的大气污染防治措施,以期为徐州市空气质量提升提供帮助.

The objective of this study is to determine the adequacy of using a relatively coarse horizontal resolution (i.e. 36 km) to simulate long-term trends of pollutant concentrations and radiation variables with the coupled WRF-CMAQ model. WRF-CMAQ simulations over the continental United State are performed over the 2001 to 2010 time period at two different horizontal resolutions of 12 and 36 km. Both simulations used the same emission inventory and model configurations. Model results are compared both in space and time to assess the potential weaknesses and strengths of using coarse resolution in long-term air quality applications. The results show that the 36 km and 12 km simulations are comparable in terms of trends analysis for both pollutant concentrations and radiation variables. The advantage of using the coarser 36 km resolution is a significant reduction of computational cost, time and storage requirement which are key considerations when performing multiple years of simulations for trend analysis. However, if such simulations are to be used for local air quality analysis, finer horizontal resolution may be beneficial since it can provide information on local gradients. In particular, divergences between the two simulations are noticeable in urban, complex terrain and coastal regions. (C) 2016 Elsevier Ltd. All rights reserved.

Fine-particle pollution associated with winter haze threatens the health of more than 400 million people in the North China Plain. Sulfate is a major component of fine haze particles. Record sulfate concentrations of up to ~300 μg m-3 were observed during the January 2013 winter haze event in Beijing. State-of-the-art air quality models that rely on sulfate production mechanisms requiring photochemical oxidants cannot predict these high levels because of the weak photochemistry activity during haze events. We find that the missing source of sulfate and particulate matter can be explained by reactive nitrogen chemistry in aerosol water. The aerosol water serves as a reactor, where the alkaline aerosol components trap SO2, which is oxidized by NO2 to form sulfate, whereby high reaction rates are sustained by the high neutralizing capacity of the atmosphere in northern China. This mechanism is self-amplifying because higher aerosol mass concentration corresponds to higher aerosol water content, leading to faster sulfate production and more severe haze pollution.

Particulate matter (PM) mass concentrations, seasonal cycles, source sector, and source region contributions in Central Asia (CA) are analyzed for the period April 2008–July 2009 using the Sulfur Transport and dEposition Model (STEM) chemical transport model and modeled meteorology from the Weather Research and Forecasting (WRF) model. Predicted aerosol optical depth (AOD) values (annual mean value ~0.2) in CA vary seasonally, with lowest values in the winter. Surface PM2.5 concentrations (annual mean value ~10 μg m−3) also exhibit a seasonal cycle, with peak values and largest variability in the spring/summer, and lowest values and variability in the winter (hourly values from 2 to 90 μg m−3). Surface concentrations of black carbon (BC) (mean value ~0.1 μg m−3) show peak values in the winter. The simulated values are compared to surface measurements of AOD as well as PM2.5, PM10, BC, and organic carbon (OC) mass concentrations at two regional sites in Kyrgyzstan (Lidar Station Teplokluchenka (LST) and Bishkek). The predicted values of AOD and PM mass concentrations and their seasonal cycles are fairly well captured. The carbonaceous aerosols are underpredicted in winter, and analysis suggests that the winter heating emissions are underestimated in the current inventory. Dust, from sources within and outside CA, is a significant component of the PM mass and drives the seasonal cycles of PM and AOD. On an annual basis, the power and industrial sectors are found to be the most important contributors to the anthropogenic portion of PM2.5. Residential combustion and transportation are shown to be the most important sectors for BC. Biomass burning within and outside the region also contributes to elevated PM and BC concentrations. The analysis of the transport pathways and the variations in particulate matter mass and composition in CA demonstrates that this region is strategically located to characterize regional and intercontinental transport of pollutants. Aerosols at these sites are shown to reflect dust, biomass burning, and anthropogenic sources from Europe; South, East, and Central Asia; and Russia depending on the time period. Simulations for a reference 2030 emission scenario based on pollution abatement measures already committed to in current legislation show that PM2.5 and BC concentrations in the region increase, with BC growing more than PM2.5 on a relative basis. This suggests that both the health impacts and the climate warming associated with these particles may increase over the next decades unless additional control measures are taken. The importance of observations in CA to help characterize the changes that are rapidly taking place in the region are discussed.

Abstract. The ability of a coupled meteorology–chemistry model, i.e., Weather Research and Forecast and Community Multiscale Air Quality (WRF-CMAQ), to reproduce the historical trend in aerosol optical depth (AOD) and clear-sky shortwave radiation (SWR) over the Northern Hemisphere has been evaluated through a comparison of 21-year simulated results with observation-derived records from 1990 to 2010. Six satellite-retrieved AOD products including AVHRR, TOMS, SeaWiFS, MISR, MODIS-Terra and MODIS-Aqua as well as long-term historical records from 11 AERONET sites were used for the comparison of AOD trends. Clear-sky SWR products derived by CERES at both the top of atmosphere (TOA) and surface as well as surface SWR data derived from seven SURFRAD sites were used for the comparison of trends in SWR. The model successfully captured increasing AOD trends along with the corresponding increased TOA SWR (upwelling) and decreased surface SWR (downwelling) in both eastern China and the northern Pacific. The model also captured declining AOD trends along with the corresponding decreased TOA SWR (upwelling) and increased surface SWR (downwelling) in the eastern US, Europe and the northern Atlantic for the period of 2000–2010. However, the model underestimated the AOD over regions with substantial natural dust aerosol contributions, such as the Sahara Desert, Arabian Desert, central Atlantic and northern Indian Ocean. Estimates of the aerosol direct radiative effect (DRE) at TOA are comparable with those derived by measurements. Compared to global climate models (GCMs), the model exhibits better estimates of surface-aerosol direct radiative efficiency (Eτ). However, surface-DRE tends to be underestimated due to the underestimated AOD in land and dust regions. Further investigation of TOA-Eτ estimations as well as the dust module used for estimates of windblown-dust emissions is needed.

Decadal hemispheric Weather Research and Forecast-Community Multiscale Air Quality simulations from 1990 to 2010 were conducted to examine the meteorology and air quality responses to the aerosol direct radiative effects. The model's performance for the simulation of hourly surface temperature, relative humidity, wind speed, and direction was evaluated through comparison with observations from NOAA's National Climatic Data Center Integrated Surface Data. The inclusion of aerosol direct radiative effects improves the model's ability to reproduce the trend in daytime temperature range which over the past two decadeswas increasing in eastern China but decreasing in eastern U.S. and Europe. Trends and spatial and diurnal variations of the surface-level gaseous and particle concentrations to the aerosol direct effect were analyzed. The inclusion of aerosol direct radiative effects was found to increase the surface-level concentrations of SO2, NO2, O-3, SO42-, NO3-, and particulate matter 2.5 in eastern China, eastern U.S., and Europe by 1.5-2.1%, 1-1.5%, 0.1-0.3%, 1.6-2.3%, 3.5-10.0%, and 2.2-3.2%, respectively, on average over the entire 21 year period. However, greater impacts are noted during polluted days with increases of 7.6-10.6%, 6.2-6.7%, 2.0-3.0%, 7.8-9.5%, 11.1-18.6%, and 7.2-10.1%, respectively. Due to the aerosol direct radiative effects, stabilizing of the atmosphere associated with reduced planetary boundary layer height and ventilation leads to an enhancement of pollution. Consequently, the continual increase of aerosol optical depth (AOD) in eastern China leads to an increasing trend in the air quality feedback which exacerbates air pollution, while emission reductions in eastern U.S. and Europe result in a declining trend in both AODs and feedback which make the air pollution control strategies more effective.

Trends in air quality across the Northern Hemisphere over a 21-year period (1990–2010) were simulated using the Community Multiscale Air Quality (CMAQ) multiscale chemical transport model driven by meteorology from Weather Research and Forecasting (WRF) simulations and internally consistent historical emission inventories obtained from EDGAR. Thorough comparison with several ground observation networks mostly over Europe and North America was conducted to evaluate the model performance as well as the ability of CMAQ to reproduce the observed trends in air quality over the past 2 decades in three regions: eastern China, the continental United States and Europe. The model successfully reproduced the observed decreasing trends in SO2, NO2, 8 h O3 maxima, SO42− and elemental carbon (EC) in the US and Europe. However, the model fails to reproduce the decreasing trends in NO3− in the US, potentially pointing to uncertainties of NH3 emissions. The model failed to capture the 6-year trends of SO2 and NO2 in CN-API (China – Air Pollution Index) from 2005 to 2010, but reproduced the observed pattern of O3 trends shown in three World Data Centre for Greenhouse Gases (WDCGG) sites over eastern Asia. Due to the coarse spatial resolution employed in these calculations, predicted SO2 and NO2 concentrations are underestimated relative to all urban networks, i.e., US-AQS (US – Air Quality System; normalized mean bias (NMB) = −38% and −48%), EU-AIRBASE (European Air quality data Base; NMB = −18 and −54%) and CN-API (NMB = −36 and −68%). Conversely, at the rural network EU-EMEP (European Monitoring and Evaluation Programme), SO2 is overestimated (NMB from 4 to 150%) while NO2 is simulated well (NMB within ±15%) in all seasons. Correlations between simulated and observed O3 wintertime daily 8 h maxima (DM8) are poor compared to other seasons for all networks. Better correlation between simulated and observed SO42− was found compared to that for SO2. Underestimation of summer SO42− in the US may be associated with the uncertainty in precipitation and associated wet scavenging representation in the model. The model exhibits worse performance for NO3− predictions, particularly in summer, due to high uncertainties in the gas/particle partitioning of NO3− as well as seasonal variations of NH3 emissions. There are high correlations (R > 0.5) between observed and simulated EC, although the model underestimates the EC concentration by 65% due to the coarse grid resolution as well as uncertainties in the PM speciation profile associated with EC emissions. The almost linear response seen in the trajectory of modeled O3 changes in eastern China over the past 2 decades suggests that control strategies that focus on combined control of NOx and volatile organic compound (VOC) emissions with a ratio of 0.46 may provide the most effective means for O3 reductions for the region devoid of nonlinear response potentially associated with NOx or VOC limitation resulting from alternate strategies. The response of O3 is more sensitive to changes in NOx emissions in the eastern US because the relative abundance of biogenic VOC emissions tends to reduce the effectiveness of VOC controls. Increasing NH3 levels offset the relative effectiveness of NOx controls in reducing the relative fraction of aerosol NO3− formed from declining NOx emissions in the eastern US, while the control effectiveness was assured by the simultaneous control of NH3 emission in Europe.