ALBERT

Description: We analyze the effect of varying East Asian (EA) sulfur emissions on sulfate concentrations in the Northern Hemisphere, using a global coupled oxidant-aerosol model (MOZART-2). We conduct a base and five sensitivity simulations, in which sulfur emissions from each continent are tagged, to establish the source-receptor (S-R) relationship between EA sulfur emissions and sulfate concentrations over source and downwind regions. We find that from west to east across the North Pacific, EA sulfate contributes approximately 80%–20% of sulfate at the surface, but at least 50% at 500 hPa. In addition, EA SO2 emissions account for approximately 30%–50% and 10%–20% of North American background sulfate over the western and eastern US, respectively. The contribution of EA sulfate to the western US at the surface is highest in MAM and JJA, but is lowest in DJF. Reducing EA SO2 emissions will significantly decrease the spatial extent of the EA sulfate influence over the North Pacific both at the surface and at 500 mb in all seasons, but the extent of influence is insensitive to emission increases, particularly in DJF and JJA. We find that EA sulfate concentrations over most downwind regions respond nearly linearly to changes in EA SO2 emissions, but sulfate concentrations over the EA source region increase more slowly than SO2 emissions, particularly at the surface and in winter, due to limited availability of oxidants (mostly H2O2). We find that similar estimates of the S-R relationship for trans-Pacific transport of EA sulfate would be obtained using either sensitivity or tagging techniques. Our findings suggest that future changes in EA sulfur emissions may cause little change in the sulfate induced health impact over downwind continents but SO2 emission reductions may significantly reduce the sulfate related climate cooling over the North Pacific and the United States.

Description: The FORMOSAT-7/COSMIC-2 (F7/C2) will ultimately place 12 satellites in orbit with two launches with 24° inclination and 520 km altitude in 2016 and with 72° inclination and 800 km altitude in 2019. In this study, we examine the electron density probed at the two satellite altitudes 500 and 800 km by means of FORMOSAT-3/COSMIC (F3/C) observations at the packing orbit 500 km altitude and mission orbit 800 km altitude, as well as observing system simulation experiments (OSSE). The electron density derived from 500 and 800 km satellite altitude of the F3/C observation and the OSSE confirm that the standard Abel inversion can correctly derive the electron density profile.

Description: We analyze the effect of varying East Asian (EA) sulfur emissions on sulfate concentrations in the Northern Hemisphere, using a global coupled oxidant-aerosol model (MOZART-2). We conduct a base and five sensitivity simulations, in which sulfur emissions from each continent are tagged, to establish the source-receptor (S-R) relationship between EA sulfur emissions and sulfate concentrations over source and downwind regions. We find that from west to east across the North Pacific, EA sulfate contributes approximately 80%–20% of sulfate at the surface, but at least 50% at 500 hPa. Surface sulfate concentrations are dominated by local anthropogenic sources. Of the sulfate produced from sources other than local anthropogenic emissions (defined here as "background" sulfate), EA sources account for approximately 30%–50% (over the Western US) and 10%–20% (over the Eastern US). The surface concentrations of sulfate from EA sources over the Western US are highest in MAM (up to 0.15 μg/m3), and lowest in DJF (less than 0.06 μg/m3). Reducing EA SO2 emissions will significantly decrease the spatial extent of the EA sulfate influence (represented by the areas where at least 0.1 μg m−3 of sulfate originates from EA) over the North Pacific both at the surface and at 500 hPa in all seasons, but the extent of influence is insensitive to emission increases, particularly in DJF and JJA. We find that EA sulfate concentrations over most downwind regions respond nearly linearly to changes in EA SO2 emissions, but sulfate concentrations over the EA source region increase more slowly than SO2 emissions, particularly at the surface and in winter, due to limited availability of oxidants (in particular of H2O2, which oxidizes SO2 to sulfate in the aqueous phase). We find that similar estimates of the S-R relationship for trans-Pacific transport of EA sulfate would be obtained using either sensitivity (i.e., varying emissions from a region to examine the effects on downwind concentrations) or tagging techniques. Our findings suggest that future changes in EA sulfur emissions may cause little change in the sulfate-induced health impact over downwind continents. However, SO2 emission reductions may significantly reduce the sulfate concentrations and the resulting negative radiative forcing over the North Pacific and the United States, thus providing a warming tendency.

Description: A novel approach for the joint retrieval of aerosol optical depth (AOD) and aerosol type, using Meteosat Second Generation – Spinning Enhanced Visible and Infrared Imagers (MSG/SEVIRI) observations in two solar channels, is presented. The retrieval is based on a Time Series (TS) technique, which makes use of the two visible bands at 0.6 μm and 0.8 μm in three orderly scan times (15 min interval between two scans) to retrieve the AOD over land. Using the radiative transfer equation for plane-parallel atmosphere, two coupled differential equations for the upward and downward fluxes are derived. The boundary conditions for the upward and downward fluxes at the top and at the bottom of the atmosphere are used in these equations to provide an analytic solution for the AOD. To derive these fluxes, the aerosol single scattering albedo (SSA) and asymmetry factor are required to provide a solution. These are provided from a set of six pre-defined aerosol types with the SSA and asymmetry factor. We assume one aerosol type for a grid of 1°×1° and the surface reflectance changes little between two subsequent observations. A k-ratio approach is used in the inversion to find the best solution of atmospheric properties and surface reflectance. The k-ratio approach assumes that the surface reflectance is little influenced by aerosol scattering at 1.6 μm and therefore the ratio of surface reflectances in the solar band for two subsequent observations can be well-approximated by the ratio of the reflectances at 1.6 μm. A further assumption is that the surface reflectance varies only slightly over a period of 30 min. The algorithm makes use of numerical minimisation routines to obtain the optimal solution of atmospheric properties and surface reflectance by selection of the most suitable aerosol type from pre-defined sets. A detailed analysis of the retrieval results shows that it is suitable for AOD retrieval over land from SEVIRI data. Six AErosol RObotic NETwork (AERONET) sites with different surface types are used for detailed analysis and 42 other AERONET sites are used for validation. From 445 collocations representing stable and homogeneous aerosol type, we find that 〉75% of the MSG-retrieved AOD at 0.6 and 0.8 μm values compare favourably with AERONET observed AOD values, within an error envelope of ± 0.05 ± 0.15 τ and a high correlation coefficient (R〉0.86). The AOD datasets derived using the TS method with SEVIRI data is also compared with collocated AOD products derived from NASA TERRA and AQUA MODIS (The Moderate-resolution Imaging Spectroradiometer) data using the Dark Dense Vegetation (DDV) method and the Deep Blue algorithms. Using the TS method, the AOD could be retrieved for more pixels than with the NASA Deep Blue algorithm. This method is potentially also useful for surface reflectance retrieval using SEVIRI observations. The current paper focuses on AOD retrieval and analysis, and the analysis and validation of reflectance will be given in a following paper.

Description: Evaluating surface fluxes of CH4 using total column data requires models to accurately account for the transport and chemistry of methane in the free-troposphere and stratosphere, thus reducing sensitivity to the underlying fluxes. Vertical profiles of methane have increased sensitivity to surface fluxes because lower tropospheric methane is more sensitive to surface fluxes than a total column. Resolving the free troposphere from the lower-troposphere also helps to evaluate the impact of transport and chemistry uncertainties on estimated surface fluxes. Here we demonstrate the potential for estimating lower tropospheric CH4 concentrations through the combination of free-tropospheric methane measurements from the Aura Tropospheric Emission Spectrometer (TES) and XCH4 (dry-mole air fraction of methane) from the Greenhouse Gases Observing Satellite Thermal And Near Infrared for Carbon Observations (GOSAT TANSO, herein GOSAT for brevity). The mean precision of these estimates are calculated to be ~ 23 ppb for a monthly average on a 4 × 5 latitude/longitude degree grid making these data suitable for evaluating lower-tropospheric methane concentrations. Smoothing error is approximately 10 ppb or less. The accuracy is primarily determined by knowledge error of XCO2, used to estimate XCH4 from the GOSAT CH4/CO2 "proxy" retrieval. For example, we use different XCO2 fields to quantify XCH4 from the GOSAT CH4/CO2 retrieval, one from Carbontracker and another from the NASA Carbon Monitoring System, and find that differences of up to approximately 60 ppb are possible with a mean value of approximately 35 ppb or less for any given latitude for these lower-tropospheric methane estimates using these two different XCO2 distributions. We show that these lower-tropospheric concentrations are more directly sensitive to the underlying fluxes than a total column using the GEOS-Chem model. In particular, we compare these lower-tropospheric methane estimates with those from the GEOS-Chem model for July 2009 to determine if these data can capture methane enhancements associated with the high-latitude methane fluxes because both TES and GOSAT separately do not show much sensitivity to methane from these sources. We find that the spatial patterns and magnitude of lower tropospheric methane concentrations from GEOS-Chem over Northern European and Siberian wetland fluxes are consistent with these data but modeled concentrations are much larger than measured over Canadian wetland fluxes. Transport of methane significantly affects lower-tropospheric methane concentrations over S.E. Asia as both data and model show methane enhancements that are shifted away from their sources. A possible new finding is that there is no representation of a strong source between the Black and Caspian seas.

Description: Biomass burning, the largest global source of elemental carbon (EC) and primary organic carbon (OC), is strongly associated with many subjects of great scientific concern, such as secondary organic aerosol and brown carbon which exert important effects on the environment and on climate in particular. This study investigated the relationships between levoglucosan and other biomass burning tracers (i.e., water soluble potassium and mannosan) based on both ambient samples collected in Beijing and source samples. Compared with North America and Europe, Beijing was characterized by high ambient levoglucosan concentrations and low winter to summer ratios of levoglucosan, indicating significant impact of biomass burning activities throughout the year in Beijing. Comparison of levoglucosan and water soluble potassium (K+) levels suggested that it was acceptable to use K+ as a biomass burning tracer during summer in Beijing, while the contribution of fireworks to K+ could be significant during winter. Moreover, the levoglucosan to K+ ratio was found to be lower during the typical summer period (0.21 ± 0.16) compared with the typical winter period (0.51 ± 0.15). Levoglucosan correlated strongly with mannosan (R2 = 0.97) throughout the winter and the levoglucosan to mannosan ratio averaged 9.49 ± 1.63, whereas levoglucosan and mannosan exhibited relatively weak correlation (R2 = 0.73) during the typical summer period when the levoglucosan to mannosan ratio averaged 12.65 ± 3.38. Results from positive matrix factorization (PMF) model analysis showed that about 50% of the OC and EC in Beijing were associated with biomass burning processes. In addition, a new source identification method was developed based on the comparison of the levoglucosan to K+ ratio and the levoglucosan to mannosan ratio among different types of biomass. Using this method, the major source of biomass burning aerosol in Beijing was suggested to be the combustion of crop residuals, while the contribution from softwood burning was also non-negligible, especially in winter.

Description: The mass absorption efficiency (MAE) of elemental carbon (EC) in Beijing was quantified using a thermal-optical carbon analyzer. The MAE measured at 632 nm was 8.45±1.71 and 9.41±1.92 m2 g−1 during winter and summer respectively. The daily variation of MAE was found to coincide with the abundance of organic carbon (OC), especially the OC to EC ratio, perhaps due to the enhancement by coating with organic aerosol (especially secondary organic aerosol, SOA) or the artifacts resulting from the redistribution of liquid-like organic particles during the filter-based absorption measurements. Using a converting approach that accounts for the discrepancy caused by measurements methods of both light absorption and EC concentration, previously published MAE values were converted to the equivalent-MAE, which is the estimated value if using the same measurement methods as used in this study. The equivalent-MAE was found to be much lower in the regions heavily impacted by biomass burning (e.g., below 2.7 m2 g−1 for two Indian cities). Results from source samples (including diesel exhaust samples and biomass smoke samples) also demonstrated that emissions from biomass burning would decrease the MAE of EC. Moreover, optical properties of water-soluble organic carbon (WSOC) in Beijing were presented. Light absorption by WSOC exhibited strong wavelength (λ) dependence such that absorption varied approximately as λ−7, which was characteristic of the brown carbon spectra. The MAE of WSOC (measured at 365 nm) was 1.79±0.24 and 0.71±0.20 m2 g−1 during winter and summer respectively. The large discrepancy between the MAE of WSOC during winter and summer was attributed to the difference in the precursors of SOA such that anthropogenic volatile organic compounds (AVOCs) should be more important as the precursors of SOA in winter. The MAE of WSOC in Beijing was much higher than results from the southeastern United States which were obtained using the same method as used in this study, perhaps due to the stronger emissions of biomass burning in China.

Description: Light absorbing organic carbon, often called brown carbon, has the potential to significantly contribute to the visible light-absorption budget, particularly at shorter wavelengths. Currently, the relative contributions of particulate brown carbon to light absorption, as well as the sources of brown carbon, are poorly understood. With this in mind size-resolved direct measurements of brown carbon were made at both urban (Atlanta), and rural (Yorkville) sites in Georgia. Measurements in Atlanta were made at both a representative urban site and a road-side site adjacent to a main highway. Fine particle absorption was measured with a multi-angle absorption photometer (MAAP) and seven-wavelength Aethalometer, and brown carbon absorption was estimated based on Mie calculations using direct size-resolved measurements of chromophores in solvents. Size-resolved samples were collected using a cascade impactor and analyzed for water-soluble organic carbon (WSOC), organic and elemental carbon (OC and EC), and solution light-absorption spectra of water and methanol extracts. Methanol extracts were more light-absorbing than water extracts for all size ranges and wavelengths. Absorption refractive indices of the organic extracts were calculated from solution measurements for a range of wavelengths and used with Mie theory to predict the light absorption by fine particles comprised of these components, under the assumption that brown carbon and other aerosol components were externally mixed. For all three sites, chromophores were predominately in the accumulation mode with an aerodynamic mean diameter of 0.5 μm, an optically effective size range resulting in predicted particle light absorption being a factor of 2 higher than bulk solution absorption. Mie-predicted brown carbon absorption at 350 nm contributed a significant fraction (20 to 40%) relative to total light absorption, with the highest contributions at the rural site where organic to elemental carbon ratios were highest. Brown carbon absorption, however, was highest by the roadside site due to vehicle emissions. The direct size-resolved measurement of brown carbon in solution definitively shows that it is present and optically important in the near-UV range in both a rural and urban environment during the summer when biomass burning emissions are low. These results allow estimates of brown carbon aerosol absorption from direct measurements of chromophores in aerosol extracts.

Description: A global three-dimensional (i.e. latitude, longitude, altitude) climatology of tropospheric ozone is derived from the ozone sounding record by trajectory mapping. Approximately 52 000 ozonesonde profiles from more than 100 stations worldwide since 1965 are used. The small number of stations results in a sparse geographical distribution. Here, forward and backward trajectory calculations are performed for each sounding to map ozone measurements to a number of other locations, and so to fill in the spatial domain. This is possible because the lifetime of ozone in the troposphere is of the order of weeks. This physically based interpolation method offers obvious advantages over typical statistical interpolation methods. The trajectory-mapped ozone values show reasonable agreement, where they overlap, to the actual soundings, and the patterns produced separately by forward and backward trajectory calculations are similar. Major regional features of the tropospheric ozone distribution are clearly evident in the global maps. An interpolation algorithm based on spherical functions is further used for smoothing and to fill in remaining data gaps. The resulting three-dimensional global tropospheric ozone climatology facilitates visualization and comparison of different years, decades, and seasons, and offers some intriguing insights into the global variation of tropospheric ozone. It will be useful for climate and air quality model initialization and validation, and as an a priori climatology for satellite data retrievals. Further division of the climatology into decadal and annual averages can provide a global view of tropospheric ozone changes, although uncertainties with regard to the performance of older sonde types, as well as more recent variations in operating procedures, need to be taken into account.

Description: North China Plain (NCP) is one of the most populated and polluted regions in China. During the recent years, haze and fog occur frequently and cause severely low visibility in this region. In order to better understand the impact of aerosol particles on the formation of haze and fog, a long-term record of haze and fog occurrences in the past 56 yr (from 1954–2009) over NCP is analyzed. The results show that there are rapid changes in the occurrences of haze and fog over NCP. The occurrences of haze and fog were low during 1970–1980, and reached a maximum during 1981–1998. After 1999, the occurrences of haze and fog slightly decreased. There was a nonlinear relationship between the occurrences of haze and fog. When the occurrence of haze was lower than 40 days yr−1, the occurrence of fog was strongly proportional to the occurrence of haze. However, when the occurrence of haze was high (larger than 75 days yr−1), the occurrence of fog was not sensitive to the occurrence of haze. In order to better understand the relationship between the occurrences of haze and fog as well as the effect of aerosol particles on the formation of haze and fog, an in-situ field experiment was conducted during a period with a mixed occurrence of haze and fog. The analysis of the experiment suggests that there were considerably high aerosol concentrations during the measurement period with an averaged aerosol number concentration of 24 000 cm−3. The measurement also shows that a large amount of aerosol particles can act as condensation nuclei to enhance the formation of fog droplets. As a result, a large amount of fog droplets (〉1000 cm−3) with small size (5–6 μm) were observed during the fog period, resulting in extremely low visibility (less than 100 m).