Copernicus GmbH

Abstract. Dust plumes emitted from the narrow Arabian Red Sea coastal plain are often observed on satellite images and felt in local population centers. Despite its relatively small area, the coastal plain could be a significant dust source; however, its effect is not well quantified as it is not well approximated in global or even regional models. In addition, because of close proximity to the Red Sea, a significant amount of dust from the coastal areas could be deposited into the Red Sea and serve as a vital component of the nutrient balance of marine ecosystems.In the current study, we apply the offline Community Land Model version 4 (CLM4) to better quantify dust emission from the coastal plain during the period of 2009–2011. We verify the spatial and temporal variability in model results using independent weather station reports. We also compare the results with the MERRA Aerosol Reanalysis (MERRAero). We show that the best results are obtained with 1 km model spatial resolution and dust source function based on Meteosat Second Generation Spinning Enhanced Visible and InfraRed Imager (SEVIRI) measurements. We present the dust emission spatial pattern, as well as estimates of seasonal and diurnal variability in dust event frequency and intensity, and discuss the emission regime in the major dust generation hot spot areas. We demonstrate the contrasting seasonal dust cycles in the northern and southern parts of the coastal plain and discuss the physical mechanisms responsible for dust generation.This study provides the first estimates of the fine-scale spatial and temporal distribution of dust emissions from the Arabian Red Sea coastal plain constrained by MERRAero and short-term WRF-Chem simulations. The estimate of total dust emission from the coastal plain, tuned to fit emissions in MERRAero, is 7.5 ± 0.5 Mt a−1. Small interannual variability indicates that the study area is a stable dust source. The mineralogical composition analysis shows that the coastal plain generates around 76 ± 5 kt of iron oxides and 6 ± 0.4 kt of phosphorus annually. Over 65 % of dust is emitted from the northern part of the coastal plain.

Abstract. We present comprehensive long-term ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements of aerosols, nitrogen dioxide (NO2), and formaldehyde (HCHO) from Mohali (30.667∘ N, 76.739∘ E; ∼310 m above mean sea level), located in the densely populated Indo-Gangetic Plain (IGP) of India. We investigate the temporal variation in tropospheric columns, surface volume mixing ratio (VMR), and vertical profiles of aerosols, NO2, and HCHO and identify factors driving their ambient levels and distributions for the period from January 2013 to June 2017. We observed mean aerosol optical depth (AOD) at 360 nm, tropospheric NO2 vertical column density (VCD), and tropospheric HCHO VCD for the measurement period to be 0.63 ± 0.51, (6.7 ± 4.1) × 1015, and (12.1 ± 7.5) × 1015 molecules cm−2, respectively. Concerning the tropospheric NO2 VCDs, Mohali was found to be less polluted than urban and suburban locations of China and western countries, but comparable HCHO VCDs were observed. For the more than 4 years of measurements during which the region around the measurement location underwent significant urban development, we did not observe obvious annual trends in AOD, NO2, and HCHO. High tropospheric NO2 VCDs were observed in periods with enhanced biomass and biofuel combustion (e.g. agricultural residue burning and domestic burning for heating). Highest tropospheric HCHO VCDs were observed in agricultural residue burning periods with favourable meteorological conditions for photochemical formation, which in previous studies have shown an implication for high ambient ozone also over the IGP. Highest AOD is observed in the monsoon season, indicating possible hygroscopic growth of the aerosol particles. Most of the NO2 is located close to the surface, whereas significant HCHO is present at higher altitudes up to 600 m during summer indicating active photochemistry at high altitudes. The vertical distribution of aerosol, NO2, and HCHO follows the change in boundary layer height (BLH), from the ERA5 dataset of European Centre for Medium-Range Weather Forecasts, between summer and winter. However, deep convection during the monsoon transports the pollutants at high altitudes similar to summer despite a shallow ERA5 BLH. Strong gradients in the vertical profiles of HCHO are observed during the months when primary anthropogenic sources dominate the formaldehyde production. High-resolution MODIS AOD measurements correlate well but were systematically higher than MAX-DOAS AODs. The ground-based MAX-DOAS measurements were used to evaluate three NO2 data products and two HCHO data products of the Ozone Monitoring Instrument (OMI) for the first time over India and the IGP. NO2 VCDs from OMI correlate reasonably with MAX-DOAS VCDs but are lower by ∼30 %–50 % due to the difference in vertical sensitivities and the rather large OMI footprint. OMI HCHO VCDs exceed the MAX-DOAS VCDs by up to 30 %. We show that there is significant scope for improvement in the a priori vertical profiles of trace gases, which are used in OMI retrievals. The difference in vertical representativeness was found to be crucial for the observed biases in NO2 and HCHO surface VMR intercomparisons. Using the ratio of NO2 and HCHO VCDs measured from MAX-DOAS, we have found that the peak daytime ozone production regime is sensitive to both NOx and VOCs in winter but strongly sensitive to NOx in other seasons.

Abstract. Fires associated with land use and land cover changes release large amounts of aerosols and trace gases into the atmosphere. Although several inventories of biomass burning emissions cover Brazil, there are still considerable uncertainties and differences among them. While most fire emission inventories utilize the parameters of burned area, vegetation fuel load, emission factors, and other parameters to estimate the biomass burned and its associated emissions, several more recent inventories apply an alternative method based on fire radiative power (FRP) observations to estimate the amount of biomass burned and the corresponding emissions of trace gases and aerosols. The Brazilian Biomass Burning Emission Model (3BEM) and the Fire Inventory from NCAR (FINN) are examples of the first, while the Brazilian Biomass Burning Emission Model with FRP assimilation (3BEM_FRP) and the Global Fire Assimilation System (GFAS) are examples of the latter. These four biomass burning emission inventories were used during the South American Biomass Burning Analysis (SAMBBA) field campaign. This paper analyzes and inter-compared them, focusing on eight regions in Brazil and the time period of 1 September–31 October 2012. Aerosol optical thickness (AOT550 nm) derived from measurements made by the Moderate Resolution Imaging Spectroradiometer (MODIS) operating on board the Terra and Aqua satellites is also applied to assess the inventories' consistency. The daily area-averaged pyrogenic carbon monoxide (CO) emission estimates exhibit significant linear correlations (r, p  >  0.05 level, Student t test) between 3BEM and FINN and between 3BEM_ FRP and GFAS, with values of 0.86 and 0.85, respectively. These results indicate that emission estimates in this region derived via similar methods tend to agree with one other. However, they differ more from the estimates derived via the alternative approach. The evaluation of MODIS AOT550 nm indicates that model simulation driven by 3BEM and FINN typically underestimate the smoke particle loading in the eastern region of Amazon forest, while 3BEM_FRP estimations to the area tend to overestimate fire emissions. The daily regional CO emission fluxes from 3BEM and FINN have linear correlation coefficients of 0.75–0.92, with typically 20–30 % higher emission fluxes in FINN. The daily regional CO emission fluxes from 3BEM_FRP and GFAS show linear correlation coefficients between 0.82 and 0.90, with a particularly strong correlation near the arc of deforestation in the Amazon rainforest. In this region, GFAS has a tendency to present higher CO emissions than 3BEM_FRP, while 3BEM_FRP yields more emissions in the area of soybean expansion east of the Amazon forest. Atmospheric aerosol optical thickness is simulated by using the emission inventories with two operational atmospheric chemistry transport models: the IFS from Monitoring Atmospheric Composition and Climate (MACC) and the Coupled Aerosol and Tracer Transport model to the Brazilian developments on the Regional Atmospheric Modelling System (CCATT-BRAMS). Evaluation against MODIS observations shows a good representation of the general patterns of the AOT550 nm time series. However, the aerosol emissions from fires with particularly high biomass consumption still lead to an underestimation of the atmospheric aerosol load in both models.

Abstract. Organic carbon (OC) comprises a large fraction of fine particulate matter (PM2.5) in Mexico City. Daily and select 12-h PM2.5 samples were collected in urban and peripheral sites in Mexico City from 17–30 March 2006. Samples were analyzed for OC and elemental carbon (EC) using thermal-optical filter-based methods. Real-time water-soluble organic carbon (WSOC) was collected at the peripheral site. Organic compounds, particularly molecular markers, were quantified by soxhlet extraction with methanol and dichloromethane, derivitization, and gas chromatography with mass spectrometric detection (GCMS). A chemical mass balance model (CMB) based on molecular marker species was used to determine the relative contribution of major sources to ambient OC. Motor vehicles, including diesel and gasoline, consistently accounted for 49% of OC in the urban area and 32% on the periphery. The daily contribution of biomass burning to OC was highly variable, and ranged from 5–26% at the urban site and 7–39% at the peripheral site. The remaining OC unapportioned to primary sources showed a strong correlation with WSOC and was considered to be secondary in nature. Comparison of temporally resolved OC showed that contributions from primary aerosol sources during daylight hours were not significantly different from nighttime. This study provides quantitative understanding of the important sources of OC during the MILAGRO 2006 field campaign.

Abstract. Frequent low visibility, haze and fog events were found in the North China Plain (NCP). Data throughout the NCP during the past 30 years were examined to determine the horizontal distribution and decadal trends of low visibility, haze and fog events. The impact of meteorological factors such as wind and relative humidity (RH) on those events was investigated. Results reveal distinct distributions of haze and fog days, due to their different formation mechanisms. Low visibility, haze and fog days all display increasing trends of before 1995, a steady stage during the period 1995–2003 and a drastically drop thereafter. All three events occurred most frequently during the heating season. Benefiting from emission control measures, haze and fog both show decreasing trends in winter during the past 3 decades, while summertime haze displays continuous increasing trends. The distribution of wind speed and wind direction as well as the topography within the NCP has determinative impacts on the distribution of haze and fog. Weakened south-easterly winds in the southern part of the NCP have resulted in high pollutant concentrations and frequent haze events along the foot of the Taihang Mountains. The orographically generated boundary layer wind convergence line in the central area of the southern NCP is responsible for the frequent fog events in this region. Wind speed has been decreasing throughout the entire southern NCP, resulting in more stable atmospheric conditions and weaker dispersion abilities, calling for harder efforts to control emissions to prevent haze events. Haze events are strongly influenced by the ambient RH. RH values associated with haze days are evidently increasing, suggesting that an increasing fraction of haze events are caused by the hygroscopic growth of aerosols, rather than simply by high aerosol loadings.

Abstract. Recently, Chinese cities have suffered severe events of haze air pollution, particularly in the North China Plain (NCP). Investigating the temporal and spatial distribution of pollutants, emissions, and pollution transport is necessary to better understand the effect of various sources on air quality. We report on mobile differential optical absorption spectroscopy (mobile DOAS) observations of precursors SO2 and NO2 vertical columns in the NCP in the summer of 2013 (from 11 June to 7 July) in this study. The different temporal and spatial distributions of SO2 and NO2 vertical column density (VCD) over this area are characterized under various wind fields. The results show that transport from the southern NCP strongly affects air quality in Beijing, and the transport route, particularly SO2 transport on the route of Shijiazhuang–Baoding–Beijing, is identified. In addition, the major contributors to SO2 along the route of Shijiazhuang–Baoding–Beijing are elevated sources compared to low area sources for the route of Dezhou–Cangzhou–Tianjin–Beijing; this is found using the interrelated analysis between in situ and mobile DOAS observations during the measurement periods. Furthermore, the discussions on hot spots near the city of JiNan show that average observed width of polluted air mass is 11.83 and 17.23 km associated with air mass diffusion, which is approximately 60 km away from emission sources based on geometrical estimation. Finally, a reasonable agreement exists between the Ozone Monitoring Instrument (OMI) and mobile DOAS observations, with a correlation coefficient (R2) of 0.65 for NO2 VCDs. Both datasets also have a similar spatial pattern. The fitted slope of 0.55 is significantly less than unity, which can reflect the contamination of local sources, and OMI observations are needed to improve the sensitivities to the near-surface emission sources through improvements of the retrieval algorithm or the resolution of satellites.

Abstract. Ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements of sulfur dioxide (SO2) have been performed at the Xianghe station (39.8° N, 117.0° E) located at ~ 50 km southeast of Beijing from March 2010 to February 2013. Tropospheric SO2 vertical profiles and corresponding vertical column densities (VCDs), retrieved by applying the optimal estimation method to the MAX-DOAS observations, have been used to study the seasonal and diurnal cycles of SO2, in combination with correlative measurements from in situ instruments, as well as meteorological data. A marked seasonality was observed in both SO2 VCD and surface concentration, with a maximum in winter (February) and a minimum in summer (July). This can be explained by the larger emissions in winter due to the domestic heating and, in case of surface concentration, by more favorable meteorological conditions for the accumulation of SO2 close to the ground during this period. Wind speed and direction are also found to be two key factors in controlling the level of the SO2-related pollution at Xianghe. In the case of east or southwest wind, the SO2 concentration does not change significantly with the wind speed, since the city of Tangshan and heavy polluting industries are located to the east and southwest of the station, respectively. In contrast, when wind comes from other directions, the stronger the wind, the less SO2 is observed due to a more effective dispersion. Regarding the diurnal cycle, the SO2 amount is larger in the early morning and late evening and lower at noon, in line with the diurnal variation of pollutant emissions and atmospheric stability. A strong correlation with correlation coefficients between 0.6 and 0.9 is also found between SO2 and aerosols in winter, suggesting that anthropogenic SO2, through the formation of sulfate aerosols, contributes significantly to the total aerosol content during this season. The observed diurnal cycles of MAX-DOAS SO2 surface concentration are also in very good agreement (correlation coefficient close to 0.9) with those from collocated in situ data, indicating the good reliability and robustness of our retrieval.

Abstract. Ground-based Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) measurements of nitrous acid (HONO) and its precursor NO2 (nitrogen dioxide) as well as aerosols have been performed daily in Beijing city centre (39.98° N, 116.38° E) from July 2008 to April 2009 and at the suburban site of Xianghe (39.75° N, 116.96° E) located ~60 km east of Beijing from March 2010 to December 2012. This extensive dataset allowed for the first time the investigation of the seasonal cycle of HONO as well as its diurnal variation in and in the vicinity of a megacity. Our study was focused on the HONO and NO2 near-surface concentrations (0–200 m layer) and total vertical column densities (VCDs) and also aerosol optical depths (AODs) and extinction coefficients retrieved by applying the Optimal Estimation Method to the MAX-DOAS observations. Monthly averaged HONO near-surface concentrations at local noon display a strong seasonal cycle with a maximum in late fall/winter (~0.8 and 0.7 ppb at Beijing and Xianghe, respectively) and a minimum in summer (~0.1 ppb at Beijing and 0.03 ppb at Xianghe). The seasonal cycles of HONO and NO2 appear to be highly correlated, with correlation coefficients in the 0.7–0.9 and 0.5–0.8 ranges at Beijing and Xianghe, respectively. The stronger correlation of HONO with NO2 and also with aerosols observed in Beijing suggests possibly larger role of NO2 conversion into HONO in the Beijing city center than at Xianghe. The observed diurnal cycle of HONO near-surface concentration shows a maximum in the early morning (about 1 ppb at both sites) likely resulting from night-time accumulation, followed by a decrease to values of about 0.1–0.4 ppb around local noon. The HONO / NO2 ratio shows a similar pattern with a maximum in the early morning (values up to 0.08) and a decrease to ~0.01–0.02 around local noon. The seasonal and diurnal cycles of the HONO near-surface concentration are found to be similar in shape and in relative amplitude to the corresponding cycles of the HONO total VCD and are therefore likely driven mainly by the balance between HONO sources and the photolytic sink, whereas dilution effects appear to play only a minor role. The estimation of OH radical production from HONO and O3 photolysis based on retrieved HONO near-surface concentrations and calculated photolysis rates indicate that in the 0–200 m altitude range, HONO is by far the largest source of OH radicals in winter as well as in the early morning at all seasons, while the contribution of O3 dominates in summer from mid-morning until mid-afternoon.

Abstract. Anthropogenic emissions of air pollutants in China influence not only local and regional environments but also the global atmospheric environment; therefore, it is important to understand how China's air pollutant emissions will change and how they will affect regional air quality in the future. Emission scenarios in 2020 were projected using forecasts of energy consumption and emission control strategies based on emissions in 2005, and on recent development plans for key industries in China. We developed four emission scenarios: REF[0] (current control legislations and implementation status), PC[0] (improvement of energy efficiencies and current environmental legislation), PC[1] (improvement of energy efficiencies and better implementation of environmental legislation), and PC[2] (improvement of energy efficiencies and strict environmental legislation). Under the REF[0] scenario, the emission of SO2, NOx, VOC and NH3 will increase by 17%, 50%, 49% and 18% in 2020, while PM10 emissions will be reduced by 10% over East China, compared to that in 2005. In PC[2], sustainable energy polices will reduce SO2, NOx and PM10 emissions by 4.1 Tg, 2.6 Tg and 1.8 Tg, respectively; better implementation of current control policies will reduce SO2, NOx and PM10 emission by 2.9 Tg, 1.8 Tg, and 1.4 Tg, respectively; strict emission standards will reduce SO2, NOx and PM10 emissions by 3.2 Tg, 3.9 Tg, and 1.7 Tg, respectively. Under the PC[2] scenario, SO2 and PM10 emissions will decrease by 18% and 38%, while NOx and VOC emissions will increase by 3% and 8%, compared to that in 2005. Future air quality in China was simulated using the Community Multi-scale Air Quality Model (CMAQ). Under REF[0] emissions, compared to 2005, the surface concentrations of SO2, NO2, hourly maximum ozone in summer, PM2.5, total sulfur and nitrogen depositions will increase by 28%, 41%, 8%, 8%, 19% and 25%, respectively, over east China. Under the PC[2] emission scenario, the surface concentrations of SO2, PM2.5, total sulfur depositions will decrease by 18%, 16% and 15%, respectively, and the surface concentrations of NO2, nitrate, hourly maximum ozone in summer, total nitrogen depositions will be kept as 2005 level, over east China. The individual impacts of SO2, NOx, NH3, NMVOC and primary PM emission changes on ozone and PM2.5 concentrations have been analyzed using sensitivity analysis. The results suggest that NOx emission control need to be enhanced during the summertime to obtain both ozone and PM2.5 reduction benefits. NH3 emission controls should also be considered in order to reduce both nitrate concentration and total nitrogen deposition in the future.

Abstract. In this paper, we present ship-based Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) measurements of tropospheric trace gases' distribution along the Yangtze River during winter 2015. The measurements were performed along the Yangtze River between Shanghai and Wuhan, covering major industrial areas in eastern China. Tropospheric vertical column densities (VCDs) of nitrogen dioxide (NO2), sulfur dioxide (SO2), and formaldehyde (HCHO) were retrieved using the air mass factor calculated by the radiative transfer model. Enhanced tropospheric NO2 and SO2 VCDs were detected over downwind areas of industrial zones over the Yangtze River. In addition, spatial distributions of atmospheric pollutants are strongly affected by meteorological conditions; i.e., positive correlations were found between concentration of pollutants and wind speed over these areas, indicating strong influence of transportation of pollutants from high-emission upwind areas along the Yangtze River. Comparison of tropospheric NO2 VCDs between ship-based MAX-DOAS and Ozone Monitoring Instrument (OMI) satellite observations shows good agreement with each other, with a Pearson correlation coefficient (R) of 0.82. In this study, the NO2 ∕ SO2 ratio was used to estimate the relative contributions of industrial sources and vehicle emissions to ambient NO2 levels. Analysis results of the NO2 ∕ SO2 ratio show a higher contribution of industrial NO2 emissions in Jiangsu Province, while NO2 levels in Jiangxi and Hubei provinces are mainly related to vehicle emissions. These results indicate that different pollution control strategies should be applied in different provinces. In addition, multiple linear regression analysis of ambient carbon monoxide (CO) and odd oxygen (Ox) indicated that the primary emission and secondary formation of HCHO contribute 54.4 ± 3.7 % and 39.3 ± 4.3 % to the ambient HCHO, respectively. The largest contribution from primary emissions in winter suggested that photochemically induced secondary formation of HCHO is reduced due to lower solar irradiance in winter. Our findings provide an improved understanding of major pollution sources along the eastern part of the Yangtze River which are useful for designing specific air pollution control policies.