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The 13C isotopic ratio of methane, δ13C of CH4, provides additional constraints on the CH4 budget to complement the constraints from CH4 observations. The interpretation of δ13C observations is complicated, however, by uncertainties in the methane sink. The reaction of CH4 with Cl is highly fractionating, increasing the relative abundance of 13CH4, but there is currently no consensus on the strength of the tropospheric Cl sink. Global model simulations of halogen chemistry differ strongly from one another in terms of both the magnitude of tropospheric Cl and its geographic distribution. This study explores the impact of the intermodel diversity in Cl fields on the simulated δ13C of CH4. We use a set of GEOS global model simulations with different predicted Cl fields to test the sensitivity of the δ13C of CH4 to the diversity of Cl output from chemical transport models. We find that δ13C is highly sensitive to both the amount and geographic distribution of Cl. Simulations with Cl providing 0.28 % or 0.66 % of the total CH4 loss bracket the δ13C observations for a fixed set of emissions. Thus, even when Cl provides only a small fraction of the total CH4 loss and has a small impact on total CH4, it provides a strong lever on δ13C. Consequently, it is possible to achieve a good representation of total CH4 using widely different Cl concentrations, but the partitioning of the CH4 loss between the OH and Cl reactions leads to strong differences in isotopic composition depending on which model's Cl field is used. Comparing multiple simulations, we find that altering the tropospheric Cl field leads to approximately a 0.5 ‰ increase in δ13CH4 for each percent increase in how much CH4 is oxidized by Cl. The geographic distribution and seasonal cycle of Cl also impacts the hemispheric gradient and seasonal cycle of δ13C. The large effect of Cl on δ13C compared to total CH4 broadens the range of CH4 source mixtures that can be reconciled with δ13C observations. Stronger constraints on tropospheric Cl are necessary to improve estimates of CH4 sources from δ13C observations.

The tropical tropopause layer (TTL) is the transition region between the well-mixed convective troposphere and the radiatively controlled stratosphere with air masses showing chemical and dynamical properties of both regions. The representation of the TTL in meteorological reanalysis data sets is important for studying the complex interactions of circulation, convection, trace gases, clouds, and radiation. In this paper, we present the evaluation of climatological and long-term TTL temperature and tropopause characteristics in the reanalysis data sets ERA-Interim, ERA5, JRA-25, JRA-55, MERRA, MERRA-2, NCEP-NCAR (R1), and CFSR. The evaluation has been performed as part of the SPARC (Stratosphere–troposphere Processes and their Role in Climate) Reanalysis Intercomparison Project (S-RIP). The most recent atmospheric reanalysis data sets (ERA-Interim, ERA5, JRA-55, MERRA-2, and CFSR) all provide realistic representations of the major characteristics of the temperature structure within the TTL. There is good agreement between reanalysis estimates of tropical mean temperatures and radio occultation data, with relatively small cold biases for most data sets. Temperatures at the cold point and lapse rate tropopause levels, on the other hand, show warm biases in reanalyses when compared to observations. This tropopause-level warm bias is related to the vertical resolution of the reanalysis data, with the smallest bias found for data sets with the highest vertical resolution around the tropopause. Differences in the cold point temperature maximize over equatorial Africa, related to Kelvin wave activity and associated disturbances in TTL temperatures. Interannual variability in reanalysis temperatures is best constrained in the upper TTL, with larger differences at levels below the cold point. The reanalyses reproduce the temperature responses to major dynamical and radiative signals such as volcanic eruptions and the quasi-biennial oscillation (QBO). Long-term reanalysis trends in temperature in the upper TTL show good agreement with trends derived from adjusted radiosonde data sets indicating significant stratospheric cooling of around −0.5 to −1 K per decade. At 100 hPa and the cold point, most of the reanalyses suggest small but significant cooling trends of −0.3 to −0.6 K per decade that are statistically consistent with trends based on the adjusted radiosonde data sets. Advances of the reanalysis and observational systems over the last decades have led to a clear improvement in the TTL reanalysis products over time. Biases of the temperature profiles and differences in interannual variability clearly decreased in 2006, when densely sampled radio occultation data started being assimilated by the reanalyses. While there is an overall good agreement, different reanalyses offer different advantages in the TTL such as realistic profile and cold point temperature, continuous time series, or a realistic representation of signals of interannual variability. Their use in model simulations and in comparisons with climate model output should be tailored to their specific strengths and weaknesses.

Secondary organic aerosol (SOA) formation from biogenic precursors is affected by anthropogenic emissions, which are not well understood in polluted areas. In this study, we accomplished a year-round campaign at nine sites in polluted areas located in the Pearl River Delta (PRD) region during 2015. We measured typical biogenic SOA (BSOA) tracers from isoprene, monoterpenes, and β-caryophyllene, as well as major gaseous and particulate pollutants and investigated the impact of anthropogenic pollutants on BSOA formation. The concentrations of BSOA tracers were in the range of 45.4 to 109 ng m−3 with the majority composed of products from monoterpenes (SOAM, 47.2±9.29 ng m−3), isoprene (SOAI, 23.1±10.8 ng m−3), and β-caryophyllene (SOAC, 3.85±1.75 ng m−3). We found that atmospheric oxidants, Ox (O3 plus NO2), and sulfate correlated well with later-generation SOAM tracers, but this was not the case for first-generation SOAM products. This suggested that high Ox and sulfate levels could promote the formation of later-generation SOAM products, which probably led to the relatively aged SOAM that we observed in the PRD. For the SOAI tracers, both 2-methylglyceric acid (NO/NO2-channel product) and the ratio of 2-methylglyceric acid to 2-methyltetrols (HO2-channel products) exhibit NOx dependence, indicating the significant impact of NOx on SOAI formation pathways. The SOAC tracer was elevated in winter at all sites and was positively correlated with levoglucosan, Ox, and sulfate. Thus, the unexpected increase in SOAC in wintertime might be highly associated with the enhancement of biomass burning, O3 chemistry, and the sulfate component in the PRD. The BSOAs that were estimated using the SOA tracer approach showed the highest concentration in fall and the lowest concentration in spring with an annual average concentration of 1.68±0.40 µg m−3. SOAM dominated the BSOA mass all year round. We also found that BSOA correlated well with sulfate and Ox. This implied a significant effect from anthropogenic pollutants on BSOA formation and highlighted that we could reduce BSOA by controlling the anthropogenic emissions of sulfate and Ox precursors in polluted regions.

The precise contribution of the two major sinks for anthropogenic CO2 emissions, terrestrial vegetation and the ocean, and their location and year-to-year variability are not well understood. Top-down estimates of the spatiotemporal variations in emissions and uptake of CO2 are expected to benefit from the increasing measurement density brought by recent in situ and remote CO2 observations. We uniquely apply a batch Bayesian synthesis inversion at relatively high resolution to in situ surface observations and bias-corrected GOSAT satellite column CO2 retrievals to deduce the global distributions of natural CO2 fluxes during 2009–2010. The GOSAT inversion is generally better constrained than the in situ inversion, with smaller posterior regional flux uncertainties and correlations, because of greater spatial coverage, except over North America and northern and southern high-latitude oceans. Complementarity of the in situ and GOSAT data enhances uncertainty reductions in a joint inversion; however, remaining coverage gaps, including those associated with spatial and temporal sampling biases in the passive satellite measurements, still limit the ability to accurately resolve fluxes down to the sub-continental or sub-ocean basin scale. The GOSAT inversion produces a shift in the global CO2 sink from the tropics to the north and south relative to the prior, and an increased source in the tropics of ∼  2 Pg C yr−1 relative to the in situ inversion, similar to what is seen in studies using other inversion approaches. This result may be driven by sampling and residual retrieval biases in the GOSAT data, as suggested by significant discrepancies between posterior CO2 distributions and surface in situ and HIPPO mission aircraft data. While the shift in the global sink appears to be a robust feature of the inversions, the partitioning of the sink between land and ocean in the inversions using either in situ or GOSAT data is found to be sensitive to prior uncertainties because of negative correlations in the flux errors. The GOSAT inversion indicates significantly less CO2 uptake in the summer of 2010 than in 2009 across northern regions, consistent with the impact of observed severe heat waves and drought. However, observations from an in situ network in Siberia imply that the GOSAT inversion exaggerates the 2010–2009 difference in uptake in that region, while the prior CASA-GFED model of net ecosystem production and fire emissions reasonably estimates that quantity. The prior, in situ posterior, and GOSAT posterior all indicate greater uptake over North America in spring to early summer of 2010 than in 2009, consistent with wetter conditions. The GOSAT inversion does not show the expected impact on fluxes of a 2010 drought in the Amazon; evaluation of posterior mole fractions against local aircraft profiles suggests that time-varying GOSAT coverage can bias the estimation of interannual flux variability in this region.

Large and effective reductions in emissions of long-lived ozone-depleting substance (ODS) are being achieved through the Montreal Protocol, the effectiveness of which can be seen in the declining atmospheric abundances of many ODSs. An important remaining uncertainty concerns the role of very short-lived substances (VSLSs) which, owing to their relatively short atmospheric lifetimes (less than 6 months), are not regulated under the Montreal Protocol. Recent studies have found an unexplained increase in the global tropospheric abundance of one VSLS, dichloromethane (CH2Cl2), which has increased by around 60 % over the past decade. Here we report dramatic enhancements of several chlorine-containing VSLSs (Cl-VSLSs), including CH2Cl2 and CH2ClCH2Cl (1,2-dichloroethane), observed in surface and upper-tropospheric air in East and South East Asia. Surface observations were, on occasion, an order of magnitude higher than previously reported in the marine boundary layer, whilst upper-tropospheric data were up to 3 times higher than expected. In addition, we provide further evidence of an atmospheric transport mechanism whereby substantial amounts of industrial pollution from East Asia, including these chlorinated VSLSs, can rapidly, and regularly, be transported to tropical regions of the western Pacific and subsequently uplifted to the tropical upper troposphere. This latter region is a major provider of air entering the stratosphere, and so this mechanism, in conjunction with increasing emissions of Cl-VSLSs from East Asia, could potentially slow the expected recovery of stratospheric ozone.

Chlorofluorocarbons (CFCs) are ozone-depleting substances as well as strong greenhouse gases, and the control of their production and use under the Montreal Protocol has had demonstrable benefits to both mitigation of increasing surface UV radiation and climate forcing. A global ban on consumption came into force in 2010, but there is evidence of continuing emissions of certain CFCs from a range of sources. One compound has received little attention in the literature, namely CFC-114 (C2Cl2F4). Of particular interest here is the differentiation between CFC-114 (CClF2CClF2) and its asymmetric isomeric form CFC-114a (CF3CCl2F) as atmospheric long-term measurements in the peer-reviewed literature to date have been assumed to represent the sum of both isomers with a time-invariant isomeric speciation. Here we report the first long-term measurements of the two isomeric forms separately, and find that they have different origins and trends in the atmosphere. Air samples collected at Cape Grim (41° S), Australia, during atmospheric background conditions since 1978, combined with samples collected from deep polar snow (firn) enable us to obtain a near-complete record of both gases since their initial production and release in the 1940s. Both isomers were present in the unpolluted atmosphere in comparably small amounts before 1960. The mixing ratio of CFC-114 doubled from 7.9 to 14.8 parts per trillion (ppt) between the start of the Cape Grim record in 1978 and the end of our record in 2014, while over the same time CFC-114a trebled from 0.35 to 1.03 ppt. Mixing ratios of both isomers are slowly decreasing by the end of this period. This is consistent with measurements of recent aircraft-based samples showing no significant interhemispheric mixing ratio gradient. We also find that the fraction of CFC-114a mixing ratio relative to that of CFC-114 increased from 4.2 to 6.9 % over the 37-year period. This contradicts the current tacit assumption used in international climate change and ozone depletion assessments that both isomers have been largely co-emitted and that their atmospheric concentration ratio has remained approximately constant in time. Complementary observations of air collected in Taiwan indicate a persisting source of CFC-114a in South East Asia which may have been contributing to the changing balance between the two isomers. In addition we present top-down global annual emission estimates of CFC-114 and CFC-114a derived from these measurements using a two-dimensional atmospheric chemistry-transport model. In general, the emissions for both compounds grew steadily during the 1980s, followed by a substantial reduction from the late 1980s onwards, which is consistent with the reduction of emission in response to the Montreal Protocol, and broadly consistent with bottom-up estimates derived by industry. However, we find that small but significant emissions of both isomers remain in 2014. Moreover the inferred changes to the ratio of emissions of the two isomers since the 1990s also indicate that the sources of the two gases are, in part, independent.

Biomass burning organic aerosol (BBOA) can be emitted from natural forest fires and human activities such as agricultural burning and domestic energy generation. BBOA is strongly associated with atmospheric brown carbon (BrC) that absorbs near-ultraviolet and visible light, resulting in significant impacts on regional visibility degradation and radiative forcing. The mixing state of BBOA can play a critical role in the prediction of aerosol optical properties. In this work, single-particle measurements from a Soot-Particle Aerosol Mass Spectrometer coupled with a light scattering module (LS-SP-AMS) were performed to examine the mixing state of BBOA, refractory black carbon (rBC), and potassium (K, a tracer for biomass burning aerosol) in an air mass influenced by wildfire emissions transported from northern Québec to Toronto, representing aged biomass burning plumes. Cluster analysis of single-particle measurements identified five BBOA-related particle types. rBC accounted for 3–14 wt % of these particle types on average. Only one particle type exhibited a strong ion signal for K+, with mass spectra characterized by low molecular weight organic species. The remaining four particle types were classified based on the apparent molecular weight of the BBOA constituents. Two particle types were associated with low potassium content and significant amounts of high molecular weight (HMW) organic compounds. Our observations indicate non-uniform mixing of particles within a biomass burning plume in terms of molecular weight and illustrate that HMW BBOA can be a key contributor to low-volatility BrC observed in BBOA particles. The average mass absorption efficiency of low-volatility BBOA is about 0.8–1.1 m2 g−1 based on a theoretical closure calculation. Our estimates indicate that low-volatility BBOA contributes ∼ 33–44 % of thermo-processed particle absorption at 405 nm; and almost all of the BBOA absorption was associated with low-volatility organics.

The climatic impacts of black carbon (BC) aerosol, an important absorber of solar radiation in the atmosphere, remain poorly constrained and are intimately related to its particle-scale physical and chemical properties. Using particle-resolved modelling informed by quantitative measurements from a soot-particle aerosol mass spectrometer, we confirm that the mixing state (the distribution of co-emitted aerosol amongst fresh BC-containing particles) at the time of emission significantly affects BC-aerosol optical properties even after a day of atmospheric processing. Both single particle and ensemble aerosol mass spectrometry observations indicate that BC near the point of emission co-exists with hydrocarbon-like organic aerosol (HOA) in two distinct particle types: HOA-rich and BC-rich particles. The average mass fraction of black carbon in HOA-rich and BC-rich particle classes was

Using surface meteorological observation and high-resolution emission data, this paper discusses the application of the PLAM/h index (Parameter Linking Air-quality to Meteorological conditions/haze) in the prediction of large-scale low visibility and fog-haze events. Based on the two-dimensional probability density function diagnosis model for emissions, the study extends the diagnosis and prediction of the meteorological pollution index PLAM to the regional visibility fog-haze intensity. The results show that combining the influence of regular meteorological conditions and emission factors together in the PLAM/h parameterization scheme is very effective in improving the diagnostic identification ability of the fog-haze weather in North China. The determination coefficients for four seasons (spring, summer, autumn, and winter) between PLAM/h and visibility observation are 0.76, 0.80, 0.96, and 0.86, respectively, and all of their significance levels exceed 0.001, showing the ability of PLAM/h to predict the seasonal changes and differences of fog-haze weather in the North China region. The high-value correlation zones are located in Jing-Jin-Ji (Beijing, Tianjin, Hebei), Bohai Bay rim, and southern Hebei–northern Henan, indicating that the PLAM/h index is related to the distribution of frequent heavy fog-haze weather in North China and the distribution of emission high-value zone. Through comparative analysis of the heavy fog-haze events and large-scale clear-weather processes in winter and summer, it is found that PLAM/h index 24 h forecast is highly correlated with the visibility observation. Therefore, the PLAM/h index has good capability in identification, analysis, and forecasting.

Since there have been individual reports of persistent haze–fog events in January 2013 in central-eastern China, questions on factors causing the drastic differences in changes in 2013 from changes in adjacent years have been raised. Changes in major chemical components of aerosol particles over the years also remain unclear. The extent of meteorological factors contributing to such changes is yet to be determined. The study intends to present the changes in daily based major water-soluble constituents, carbonaceous species, and mineral aerosol in PM10 at 13 stations within different haze regions in China from 2006 to 2013, which are associated with specific meteorological conditions that are highly related to aerosol pollution (parameterized as an index called Parameter Linking Aerosol Pollution and Meteorological Elements – PLAM). No obvious changes were found in annual mean concentrations of these various chemical components and PM10 in 2013, relative to 2012. By contrast, wintertime mass of these components was quite different. In Hua Bei Plain (HBP), sulfate, organic carbon (OC), nitrate, ammonium, element carbon (EC), and mineral dust concentrations in winter were approximately 43, 55, 28, 23, 21, and 130 μg m−3, respectively; these masses were approximately 2 to 4 times higher than those in background mass, which also exhibited a decline during 2006 to 2010 and then a rise till 2013. The mass of these concentrations and PM10, except minerals, respectively, increased by approximately 28 to 117 % and 25 % in January 2013 compared with that in January 2012. Thus, persistent haze–fog events occurred in January 2013, and approximately 60 % of this increase in component concentrations from 2012 to 2013 can be attributed to severe meteorological conditions in the winter of 2013. In the Yangtze River Delta (YRD) area, winter masses of these components, unlike HBP, have not significantly increase since 2010; PLAM were also maintained at a similar level without significant changes. In the Pearl River Delta (PRD) area, the regional background concentrations of the major chemical components were similar to those in the YRD, accounting for approximately 60–80 % of those in HBP. Since 2010, a decline has been found for winter concentrations, which can be partially attributable to persistently improving meteorological conditions and emission cutting with an emphasis on coal combustion in this area. In addition to the scattered and centralized coal combustion for heating, burning biomass fuels contributed to the large increase in concentrations of carbonaceous aerosol in major haze regions in winter, except in the PRD. No obvious changes were found for the proportions of each chemical components of PM10 from 2006 to 2013. Among all of the emissions recorded in chemical compositions in 2013, coal combustion was still the largest anthropogenic source of aerosol pollution in various areas in China, with a higher sulfate proportion of PM10 in most areas of China, and OC was normally ranked third. PM10 concentrations increased by approximately 25 % in January of 2013 relative to 2012, which caused persistent haze–fog events in HBP; emissions also reduced by approximately 35 % in Beijing and its vicinity (BIV) in late autumn of 2014, thereby producing the Asia Pacific Economic Cooperation (APEC) blue (extremely good air quality); thus, one can expect that the persistent haze–fog events would be reduced significantly in the BIV, if approx. one-third of the 2013 winter emissions were reduced, which can also be viewed as the upper limit of atmospheric aerosol pollution capacity in this area.

Top–down estimates of the spatiotemporal variations in emissions and uptake of CO2 will benefit from the increasing measurement density brought by recent and future additions to the suite of in situ and remote CO2 measurement platforms. In particular, the planned NASA Active Sensing of CO2 Emissions over Nights, Days, and Seasons (ASCENDS) satellite mission will provide greater coverage in cloudy regions, at high latitudes, and at night than passive satellite systems, as well as high precision and accuracy. In a novel approach to quantifying the ability of satellite column measurements to constrain CO2 fluxes, we use a portable library of footprints (surface influence functions) generated by the Stochastic Time-Inverted Lagrangian Transport (STILT) model in combination with the Weather Research and Forecasting (WRF) model in a regional Bayesian synthesis inversion. The regional Lagrangian particle dispersion model framework is well suited to make use of ASCENDS observations to constrain weekly fluxes in North America at a high resolution, in this case at 1° latitude × 1° longitude. We consider random measurement errors only, modeled as a function of the mission and instrument design specifications along with realistic atmospheric and surface conditions. We find that the ASCENDS observations could potentially reduce flux uncertainties substantially at biome and finer scales. At the grid scale and weekly resolution, the largest uncertainty reductions, on the order of 50%, occur where and when there is good coverage by observations with low measurement errors and the a priori uncertainties are large. Uncertainty reductions are smaller for a 1.57 μm candidate wavelength than for a 2.05 μm wavelength, and are smaller for the higher of the two measurement error levels that we consider (1.0 ppm vs. 0.5 ppm clear-sky error at Railroad Valley, Nevada). Uncertainty reductions at the annual biome scale range from ~40% to ~75% across our four instrument design cases and from ~65% to ~85% for the continent as a whole. Tests suggest that the quantitative results are moderately sensitive to assumptions regarding a priori uncertainties and boundary conditions. The a posteriori flux uncertainties we obtain, ranging from 0.01 to 0.06 Pg C yr−1 across the biomes, would meet requirements for improved understanding of long-term carbon sinks suggested by a previous study.

Tropospheric ozone (O3) is a major component of photochemical smog and is a known human health hazard, as well as a damaging factor for vegetation. Its precursor compounds, nitrogen oxides (NOx) and volatile organic compounds (VOCs), have a variety of anthropogenic and biogenic sources and exhibit non-linear effects on ozone production. As an update to previous studies on ground-level ozone in the Greater Toronto Area (GTA), we present an analysis of NO2, VOC and O3 data from federal and provincial governmental monitoring sites in the GTA from 2000 to 2012. We show that, over the study period, summertime 24 h VOC reactivity and NO2 midday (11:00–15:00) concentrations at all sites decreased significantly; since 2000, all sites experienced a decrease in NO2 of 28–62% and in measured VOC reactivity of at least 53–71%. Comparing 2002–2003 to 2011–2012, the summed reactivity of OH towards NO2 and a suite of measured VOCs decreased from 8.6 to 4.6 s−1. Ratios of reactive VOC pairs indicate that the effective OH concentration experienced by primary pollutants in the GTA has increased significantly over the study period. Despite the continuous decrease in precursor levels, ozone concentrations are not following the same pattern at all stations; it was found that the Canada-wide Standard for ozone continues to be exceeded at all monitoring stations. Additionally, while the years 2008–2011 had consistently lower ozone levels than previous years, 2012 experienced one of the highest recorded summertime ozone concentrations and a large number of smog episodes. We demonstrate that these high ozone observations in 2012 may be a result of the number of days with high solar radiation, the number of stagnant periods and the transport of high ozone levels from upwind regions.

The Himalaya mountains along the southern edge of the Tibetan Plateau act as a natural barrier for the transport of atmospheric aerosols from the polluted regions of South Asia to the main body of the Tibetan Plateau. In this study, we investigate the seasonal and diurnal variations of aerosol optical properties measured at two Aerosol Robotic Network (AERONET) sites on the southern side of the Himalaya (Pokhara, 812 m above sea level (a.s.l.) and EVK2-CNR, 5079 m a.s.l. in Nepal) and one on the northern side (Qomolangma (Mt. Everest) station for Atmospheric and Environmental Observation and Research, Chinese Academy of Sciences (QOMS_CAS) in Tibet, 4076 m a.s.l. in China). While observations at QOMS_CAS and EVK2-CNR can generally be representative of a remote background atmosphere, Pokhara is a lower-elevation suburban site with much higher aerosol load due to both the influence of local anthropogenic activities and to its proximity to the Indo-Gangetic Plains. The annual mean aerosol optical depth (AOD) during the investigated period was 0.05 at QOMS_CAS, 0.04 at EVK2-CNR and 0.51 at Pokhara, respectively. Seasonal variations of aerosols are profoundly affected by large-scale atmospheric circulation. Vegetation fires, peaking during April in the Himalayan region and northern India, contribute to a growing fine mode AOD at the three stations. Dust transported to these sites, wind erosion and hydrated/cloud-processed aerosols lead to an increase in coarse mode AOD during the monsoon season at QOMS_CAS and EVK2-CNR. Meanwhile, coarse mode AOD at EVK2-CNR is higher than at QOMS_CAS in August and September, indicating that the transport of coarse mode aerosols from the southern to the northern side may be effectively reduced. The effect of precipitation scavenging is clearly seen at Pokhara, which sees significantly reduced aerosol loads during the monsoon season. Unlike the seasonal variations, diurnal variations are mainly influenced by meso-scale systems and local topography. The diurnal pattern in precipitation appears to contribute to diurnal changes in AOD through the effect of precipitation scavenging. AOD exhibits diurnal patterns related to emissions in Pokhara, while it does not at the other two high-altitude sites. At EVK2-CNR, the daytime airflow carries aerosols up from lower-altitude polluted regions, leading to increasing AOD, while the other two stations are less influenced by valley winds. Surface heating influences the local convection, which further controls the vertical aerosol exchange and the diffusion rate of pollution to the surrounding areas. Fine and coarse mode particles are mixed together on the southern side of the Himalaya in spring, which may lead to the greater inter-annual difference in diurnal cycles of Ångström exponent (AE) at EVK2-CNR than that at QOMS_CAS.

Dust invasion is an important type of particle pollution in China. During 1 to 6 May in 2011, a dust event was observed in the Yangtze River Delta region (YRD). The highest PM10 (particles up to 10 μ in diameter) concentration reached over 1000 μg m−3 and the visibility was below 3 km. In this study, the Community Multi-scale Air Quality modeling system (CMAQ5.0) coupled with an in-line windblown dust model was used to simulate the formation, spatial and temporal characteristics of this dust event, and analyze its impacts. The threshold friction velocity for loose, fine-grained soil with low surface roughness in the dust model was revised based on Chinese data to improve the model performance. This dust storm broke out in Xinjiang and Mongolia during 28 to 30 April and arrived in the YRD region on 1 May. The transported dust particles contributed to the mean surface layer concentrations of PM10 in the YRD region 78.9% during 1 to 6 May with their impact weakening from north to south due to the removal of dust particles along the path. The dry deposition, wet deposition and total deposition of PM10 in the YRD reached 184.7 kt, 172.6 kt and 357.32 kt, respectively. The dust particles also had significant impacts on optical/radiative characteristics by absorption and scattering. In Shanghai, the largest perturbations of aerosol optical depth (AOD) and irradiance were about 0.8 DU and −130 W m−2, which could obviously influence the radiation balance in this region. The decrease of actinic fluxes impacts future photochemistry. In Shanghai, the negative effects on the NO2 and O3 photolysis could be −35% when dust particles arrived. The concentrations of O3 and OH were reduced by 1.5% and 3.1% in the whole of China, and by 9.4% and 12.1% in the YRD region, respectively. Such changes in O3 and OH levels can affect the future formation of secondary aerosols in the atmosphere by directly determining the oxidation rate of their precursors. The work of this manuscript is meaningful for understanding the dust emissions in China as well as for the application of CMAQ in Asia. It is also helpful for understanding the formation mechanism and impacts of dust pollution in the YRD.

China is regarded as the largest contributor of mercury (Hg) to the global atmospheric Hg budget. However, concentration levels and depositions of atmospheric Hg in China are poorly known. Continuous measurements of atmospheric gaseous elemental mercury (GEM) were carried out from May 2008 to May 2009 at the summit of Mt. Leigong in south China. Simultaneously, deposition fluxes of THg and MeHg in precipitation, throughfall and litterfall were also studied. Atmospheric GEM concentrations averaged 2.80±1.51 ng m−3, which was highly elevated compared to global background values but much lower than semi-rural and industrial/urban areas in China. Sources identification indicates that both regional industrial emissions and long range transport of Hg from central, south and southwest China were corresponded to the elevated GEM level. Seasonal and diurnal variations of GEM were observed, which reflected variations in source intensity, deposition processes and meteorological factors. Precipitation and throughfall deposition fluxes of THg and MeHg in Mt. Leigong were comparable or lower compared to those reported in Europe and North America, whereas litterfall deposition fluxes of THg and MeHg were higher compared to Europe and North America. This highlights the importance of vegetation to Hg atmospheric cycling. In th remote forest ecosystem of China, deposition of GEM via uptake of foliage followed by litterfall was very important for the depletion of atmospheric Hg. Elevated GEM level in ambient air may accelerate the foliar uptake of Hg through air which may partly explain the elevated litterfall deposition fluxes of Hg observed in Mt. Leigong.

Soil moisture content is one of the most important parameters as input conditions in forecasting model systems of dust storm, but it can not be directly obtained from daily routine weather report. In this paper, a scheme is developed to calculate the surface soil moisture content in China by using both precipitation and evaporation. Precipitation is directly from routine weather report, while evaporation is indirectly calculated by using meteorological elements which are also from routine weather report. According to the formula by Penman, evaporation can be considered as a linear composition of dynamic evaporation and thermodynamic evaporation caused by radiation. First, an equation for calculating daily global radiation within China is given by using regression analysis and the data of global radiation and cloud cover from 116 meteorological stations in China. Then, an equation for calculating evaporation within China is given by using regression analysis and the data of cloud cover, air temperature, precipitation, relative humidity, and wind velocity from 701 meteorological stations. Finally, a scheme for calculating soil moisture content within China is established by using regression analysis and the soil moisture content, precipitation, and evaporation at 79 agro-meteorological stations. Validation results show that the forecasting accuracy of the Chinese dust numerical model can be improved by using this scheme.