Versatile and Targeted Validation of Space-Borne XCO2, XCH4 and XCO Observations by Mobile Ground-Based Direct-Sun Spectrometers

Satellite measurements of the atmospheric concentrations of carbon dioxide (CO2), methane (CH4) and carbon monoxide (CO) require careful validation. In particular for the greenhouse gases CO2 and CH4, concentration gradients are minute challenging the ultimate goal to quantify and monitor anthropogenic emissions and natural surface-atmosphere fluxes. The upcoming European Copernicus Carbon Monitoring mission (CO2M) will focus on anthropogenic CO2 emissions, but it will also be able to measure CH4. There are other missions such as the Sentinel-5 Precursor and the Sentinel-5 series that target CO which helps attribute the CO2 and CH4 variations to specific processes. Here, we review the capabilities and use cases of a mobile ground-based sun-viewing spectrometer of the type EM27/SUN. We showcase the performance of the mobile system for measuring the column-average dry-air mole fractions of CO2 (XCO2), CH4 (XCH4) and CO (XCO) during a recent deployment (Feb./Mar. 2021) in the vicinity of Japan on research vessel Mirai which adds to our previous campaigns on ships and road vehicles. The mobile EM27/SUN has the potential to contribute to the validation of 1) continental-scale background gradients along major ship routes on the open ocean, 2) regional-scale gradients due to continental outflow across the coast line, 3) urban or other localized emissions as mobile part of a regional network and 4) emissions from point sources. Thus, operationalizing the mobile EM27/SUN along these use cases can be a valuable asset to the validation activities for CO2M, in particular, and for various upcoming satellite missions in general.

Mixing state of refractory black carbon aerosol in the South Asian outflow over the northern Indian Ocean during winter

Regional climatic implications of aerosol black carbon (BC), which has a wide variety of anthropogenic sources in large abundance, are well recognized over South Asia. Significant uncertainties remain in its quantification due to a lack of sufficient information on the microphysical properties (its concentration, size, and mixing state with other aerosol components) that determine the absorption potential of BC. In particular, the information on the mixing state of BC is extremely sparse over this region. In this study, the first observations of the size distribution and mixing state of individual refractory black carbon (rBC) particles in the South Asian outflow to the south-eastern Arabian Sea and the northern and equatorial Indian Ocean regions are presented based on measurements using a single particle soot photometer (SP2) aboard the Integrated Campaign for Aerosols, gases, and Radiation Budget (ICARB-2018) ship during winter 2018 (16 January to 13 February). The results revealed significant spatial heterogeneity of BC characteristics. The highest rBC mass concentrations (∼938±293 ng m−3) with the highest relative coating thickness (RCT; the ratio of BC core to its coating diameters) of ∼2.16±0.19 are found over the south-east Arabian Sea (SEAS) region, which is in the proximity of the continental outflow. As we move to farther oceanic regions, though the mass concentrations decreased by nearly half (∼546±80 ng m−3), BC still remained thickly coated (RCT∼2.05±0.07). The air over the remote equatorial Indian Ocean, which received considerable marine air masses compared to the other regions, showed the lowest rBC mass concentrations (∼206±114 ng m−3) with a moderately thick coating (RCT∼1.73±0.16). Even over oceanic regions far from the landmass, regions that received the outflow from the more industrialized east coast/the Bay of Bengal had a thicker coating (∼104 nm) compared to regions that received outflow from the west coast and/or peninsular India (∼86 nm). Although different regions of the ocean depicted contrasting concentrations and mixing state parameters due to the varied extent and nature of the continental outflow as well as the atmospheric lifetime of air masses, the modal parameters of rBC mass–size distributions (mean mass median diameters ∼ 0.19–0.20 µm) were similar over all regions. The mean fraction of BC-containing particles (FBC) varied in the range of 0.08–0.12 (suggesting significant amounts of non-BC particles), whereas the bulk mixing ratio of coating mass to rBC mass was highest (8.31±2.40) over the outflow regions compared to the remote ocean (4.24±1.45), highlighting the role of outflow in providing condensable material for coatings on rBC. These parameters, along with the information on the size-resolved mixing state of BC cores, throw light on the role of sources and secondary processing of their complex mixtures for coatings on BC under highly polluted conditions. Examination of the non-refractory sub-micrometre aerosol chemical composition obtained using the aerosol chemical speciation monitor (ACSM) suggested that the overall aerosol system was sulfate-dominated over the far-oceanic regions. In contrast, organics were equally prominent adjacent to the coastal landmass. An association between the BC mixing state and aerosol chemical composition suggested that sulfate was the probable dominant coating material on rBC cores.

Airborne measurements of fire emission factors for African biomass burning sampled during the MOYA campaign

Airborne sampling of methane (CH4), carbon dioxide (CO2), carbon monoxide (CO), and nitrous oxide (N2O) mole fractions was conducted during field campaigns targeting fires over Senegal in February and March 2017 and Uganda in January 2019. The majority of fire plumes sampled were close to or directly over burning vegetation, with the exception of two longer-range flights over the West African Atlantic seaboard (100–300 km from source), where the continental outflow of biomass burning emissions from a wider area of West Africa was sampled. Fire emission factors (EFs) and modified combustion efficiencies (MCEs) were estimated from the enhancements in measured mole fractions. For the Senegalese fires, mean EFs and corresponding uncertainties in units of gram per kilogram of dry fuel were 1.8±0.19 for CH4, 1633±171.4 for CO2, and 67±7.4 for CO, with a mean MCE of 0.94±0.005. For the Ugandan fires, mean EFs were 3.1±0.35 for CH4, 1610±169.7 for CO2, and 78±8.9 for CO, with a mean modified combustion efficiency of 0.93±0.004. A mean N2O EF of 0.08±0.002 g kg−1 is also reported for one flight over Uganda; issues with temperature control of the instrument optical bench prevented N2O EFs from being obtained for other flights over Uganda. This study has provided new datasets of African biomass burning EFs and MCEs for two distinct study regions, in which both have been studied little by aircraft measurement previously. These results highlight the important intracontinental variability of biomass burning trace gas emissions and can be used to better constrain future biomass burning emission budgets. More generally, these results highlight the importance of regional and fuel-type variability when attempting to spatially scale biomass burning emissions. Further work to constrain EFs at more local scales and for more specific (and quantifiable) fuel types will serve to improve global estimates of biomass burning emissions of climate-relevant gases.

Mixing state of refractory black carbon aerosol in the South Asian outflow over the northern Indian Ocean during winter

Regional climatic implications of aerosol black carbon (BC) are well recognized over South Asia, which has a wide variety of anthropogenic sources in a large abundance. Significant uncertainties remain in its quantification due to lack of sufficient information on the microphysical properties (its concentration, size, and mixing state with other aerosol components), which determine the absorption potential of BC. Especially the information on mixing state of BC is extremely sparse over this region. In this study, first-ever observations of the size distribution and mixing state of individual refractory black carbon (rBC) particles in the south Asian outflow to Southeastern Arabian Sea, northern and equatorial Indian Ocean regions are presented based on measurements using a single particle soot photometer (SP2) aboard the ship cruise of the Integrated Campaign for Aerosols, gases, and Radiation Budget (ICARB-2018) during winter-2018 (16 January to 13 February). The results revealed significant spatial heterogeneity of BC characteristics. Highest rBC mass concentrations (~ 938 ± 293 ng m−3) with the highest relative coating thickness (RCT; the ratio of BC core to its coating diameters) of ~ 2.16 ± 0.19 are found over the Southeast Arabian Sea (SEAS) region, which is in the proximity of the continental outflow. As we move to farther oceanic regions, though the mass concentrations decreased by nearly half (~ 546 ± 80 ng m−3), BC still remained thickly coated (RCT ~ 2.05 ± 0.07). The air over the remote equatorial Indian Ocean, which received considerable marine air masses compared to the other regions, showed the lowest rBC mass concentrations (~ 206 ± 114 ng m−3), with a moderately thick coating (RCT ~ 1.73 ± 0.16). Even over oceanic regions far from the landmass, regions which received the outflow from more industrialized east coast/the Bay of Bengal had thicker coating (~ 104 nm) compared to regions that received outflow from the west coast/peninsular India (~ 86 nm). Although different regions of the ocean depicted contrasting concentrations and mixing state parameters due to varying extent and nature of the continental outflow as well as the atmospheric lifetime of air masses, the modal parameters of rBC mass-size distributions were similar over all the regions. The observed mono-modal distribution with mean mass median diameters (MMD) in the range of 0.19–0.20 μm suggested mixed sources of BC. The mean fraction of BC containing particles (FBC) varied in the range 0.20–0.28 (suggesting significant amounts of non-BC particles), whereas the bulk mixing ratio of coating mass to rBC mass was highest (8.77 ± 2.77) over the outflow regions compared to the remote ocean (4.29 ± 1.54) highlighting the role of outflow in providing condensable material for coating on rBC. These parameters, along with the information on size-resolved mixing state of BC cores, throw light on the role of sources and secondary processing of their complex mixtures for coating on BC under highly polluted conditions. Examination of the non-refractory sub-micrometre aerosol chemical composition obtained using the aerosol chemical speciation monitor (ACSM) suggested that the overall aerosol system was sulfate dominated over the far-oceanic regions. In contrast, organics were equally prominent adjacent to the coastal landmass. Association between the BC mixing state and aerosol chemical composition suggested that sulfate was the probable dominant coating material on rBC cores.