Airborne quantification of net methane and carbon dioxide fluxes from European Arctic wetlands in Summer 2019.

Arctic wetlands and surrounding ecosystems are both a significant source of methane (CH4) and a sink of carbon dioxide (CO2) during summer months. However, precise quantification of this regional CH4 source and CO2 sink remains poorly characterized. A research flight using the UK Facility for Airborne Atmospheric Measurement was conducted in July 2019 over an area (approx. 78 000 km2) of mixed peatland and forest in northern Sweden and Finland. Area-averaged fluxes of CH4 and carbon dioxide were calculated using an aircraft mass balance approach. Net CH4 fluxes normalized to wetland area ranged between 5.93 ± 1.87 mg m-2 h-1 and 4.44 ± 0.64 mg m-2 h-1 (largest to smallest) over the region with a meridional gradient across three discrete areas enclosed by the flight survey. From largest to smallest, net CO2 sinks ranged between -513 ± 74 mg m-2 h-1 and -284 ± 89 mg m-2 h-1 and result from net uptake of CO2 by vegetation and soils in the biosphere. A clear gradient of decreasing bulk and area-averaged CH4 flux was identified from north to south across the study region, correlated with decreasing peat bog land area from north to south identified from CORINE land cover classifications. While N2O mole fraction was measured, no discernible gradient was measured over the flight track, but a minimum flux threshold using this mass balance method was calculated. Bulk (total area) CH4 fluxes determined via mass balance were compared with area-weighted upscaled chamber fluxes from the same study area and were found to agree well within measurement uncertainty. The mass balance CH4 fluxes were found to be significantly higher than the CH4 fluxes reported by many land-surface process models compiled as part of the Global Carbon Project. There was high variability in both flux distribution and magnitude between the individual models. This further supports previous studies that suggest that land-surface models are currently ill-equipped to accurately capture carbon fluxes inthe region. This article is part of a discussion meeting issue 'Rising methane: is warming feeding warming? (part 2)'.

δ13C methane source signatures from tropical wetland and rice field emissions.

The atmospheric methane (CH4) burden is rising sharply, but the causes are still not well understood. One factor of uncertainty is the importance of tropical CH4 emissions into the global mix. Isotopic signatures of major sources remain poorly constrained, despite their usefulness in constraining the global methane budget. Here, a collection of new δ13CCH4 signatures is presented for a range of tropical wetlands and rice fields determined from air samples collected during campaigns from 2016 to 2020. Long-term monitoring of δ13CCH4 in ambient air has been conducted at the Chacaltaya observatory, Bolivia and Southern Botswana. Both long-term records are dominated by biogenic CH4 sources, with isotopic signatures expected from wetland sources. From the longer-term Bolivian record, a seasonal isotopic shift is observed corresponding to wetland extent suggesting that there is input of relatively isotopically light CH4 to the atmosphere during periods of reduced wetland extent. This new data expands the geographical extent and range of measurements of tropical wetland and rice δ13CCH4 sources and hints at significant seasonal variation in tropical wetland δ13CCH4 signatures which may be important to capture in future global and regional models. This article is part of a discussion meeting issue 'Rising methane: is warming feeding warming? (part 2)'.

Isotopic signatures of methane emissions from tropical fires, agriculture and wetlands: the MOYA and ZWAMPS flights.

We report methane isotopologue data from aircraft and ground measurements in Africa and South America. Aircraft campaigns sampled strong methane fluxes over tropical papyrus wetlands in the Nile, Congo and Zambezi basins, herbaceous wetlands in Bolivian southern Amazonia, and over fires in African woodland, cropland and savannah grassland. Measured methane δ13CCH4 isotopic signatures were in the range -55 to -49‰ for emissions from equatorial Nile wetlands and agricultural areas, but widely -60 ± 1‰ from Upper Congo and Zambezi wetlands. Very similar δ13CCH4 signatures were measured over the Amazonian wetlands of NE Bolivia (around -59‰) and the overall δ13CCH4 signature from outer tropical wetlands in the southern Upper Congo and Upper Amazon drainage plotted together was -59 ± 2‰. These results were more negative than expected. For African cattle, δ13CCH4 values were around -60 to -50‰. Isotopic ratios in methane emitted by tropical fires depended on the C3 : C4 ratio of the biomass fuel. In smoke from tropical C3 dry forest fires in Senegal, δ13CCH4 values were around -28‰. By contrast, African C4 tropical grass fire δ13CCH4 values were -16 to -12‰. Methane from urban landfills in Zambia and Zimbabwe, which have frequent waste fires, had δ13CCH4 around -37 to -36‰. These new isotopic values help improve isotopic constraints on global methane budget models because atmospheric δ13CCH4 values predicted by global atmospheric models are highly sensitive to the δ13CCH4 isotopic signatures applied to tropical wetland emissions. Field and aircraft campaigns also observed widespread regional smoke pollution over Africa, in both the wet and dry seasons, and large urban pollution plumes. The work highlights the need to understand tropical greenhouse gas emissions in order to meet the goals of the UNFCCC Paris Agreement, and to help reduce air pollution over wide regions of Africa. This article is part of a discussion meeting issue 'Rising methane: is warming feeding warming? (part 2)'.

Characterizing the Particle Composition and Cloud Condensation Nuclei from Shipping Emission in Western Europe.

Commercial shipping is considered as an important source of air pollution and cloud condensation nuclei (CCN). To assess the climatic and environmental impacts of shipping, detailed characterization of ship plumes near the point of emission and understanding of ship plume evolution further downwind are essential. This airborne measurement study presents the online characterization of particulate phase ship emissions in the region of Western Europe in 2019 prior to new international sulfur emission controls becoming enacted. More than 30 ships from both the sulfur emission control area (SECA) in the English Channel and the open sea (OS) are measured and compared. Ships within the SECA emitted much less sulfate (SO4) compared with those at OS. When shifted to a lower apparent fuel sulfur content (FSC) at similar engine loads, the peak of the fresh ship emitting the particle number size distribution shifted from around 60-80 nm in diameter to below 40 nm in diameter. The emission factors (EFs) of sulfate are predicted to decrease by around 94% after the 2020 regulation on ship sulfur emission in the open ocean. The EFs of refractory black carbon (rBC) and organic compounds (Org) do not appear to be directly affected by the lower sulfur contents. The total number concentration for condensation nuclei (CN) >2.5 nm and >0.1 µm are predicated to be reduced by 69 and 56%, respectively. Measured plume evolution results indicate that the S(IV) to S(VI) conversion rate was around 23.4% per hour at the beginning of plume evolution, and the CCN and CN >2.5 nm ratio increased with plume age primarily due to condensation and coagulation. We estimate that the new sulfur emission regulation will lead to a reduction of more than 80% in CCN from fresh ship emissions. The ship-emitted EFs results presented here will also inform emission inventories, policymaking, climate, and human health studies.

Characterizing the aging of biomass burning organic aerosol by use of mixing ratios: a meta-analysis of four regions.

Characteristic organic aerosol (OA) emission ratios (ERs) and normalized excess mixing ratios (NEMRs) for biomass burning (BB) events have been calculated from ambient measurements recorded during four field campaigns. Normalized OA mass concentrations measured using Aerodyne Research Inc. quadrupole aerosol mass spectrometers (Q-AMS) reveal a systematic variation in average values between different geographical regions. For each region, a consistent, characteristic ratio is seemingly established when measurements are collated from plumes of all ages and origins. However, there is evidence of strong regional and local-scale variability between separate measurement periods throughout the tropical, subtropical, and boreal environments studied. ERs close to source typically exceed NEMRs in the far-field, despite apparent compositional change and increasing oxidation with age. The absence of any significant downwind mass enhancement suggests no regional net source of secondary organic aerosol (SOA) from atmospheric aging of BB sources, in contrast with the substantial levels of net SOA formation associated with urban sources. A consistent trend of moderately reduced ΔOA/ΔCO ratios with aging indicates a small net loss of OA, likely as a result of the evaporation of organic material from initial fire emissions. Variability in ERs close to source is shown to substantially exceed the magnitude of any changes between fresh and aged OA, emphasizing the importance of fuel and combustion conditions in determining OA loadings from biomass burning.

Assessment of the photochemistry of OH and NO3 on Jeju Island during the Asian-dust-storm period in the spring of 2001.

In this study, we examined the influence of the long-range transport of dust particles and air pollutants on the photochemistry of OH and NO3 on Jeju Island, Korea (33.17 degrees N, 126.10 degrees E) during the Asian-dust-storm (ADS) period of April 2001. Three ADS events were observed during the periods of April 10-12, 13-14, and 25-26. Average concentration levels of daytime OH and nighttime NO3 on Jeju Island during the ADS period were estimated to be about 1x10(6) and 2x10(8) moleculescm(-3) ( approximately 9 pptv), respectively. OH levels during the ADS period were lower than those during the non-Asian-dust-storm (NADS) period by a factor of 1.5. This was likely to result from higher CO levels and the significant loading of dust particles, reducing the photolysis frequencies of ozone. Decreases in NO3 levels during the ADS period was likely to be determined mainly by the enhancement of the N2O5 heterogeneous reaction on dust aerosol surfaces. Averaged over 24 h, the reaction between HO2 and NO was the most important source of OH during the study period, followed by ozone photolysis, which contributed more than 95% of the total source. The reactions with CO, NO2, and non-methane hydrocarbons (NMHCs) during the study period were major sinks for OH. The reaction of N2O5 on aerosol surfaces was a more important sink for nighttime NO3 during the ADS due to the significant loading of dust particles. The reaction of NO3 with NMHCs and the gas-phase reaction of N2O5 with water vapor were both significant loss mechanisms during the study period, especially during the NADS. However, dry deposition of these oxidized nitrogen species and a heterogeneous reaction of NO3 were of no importance.

Marine cloud brightening.

The idea behind the marine cloud-brightening (MCB) geoengineering technique is that seeding marine stratocumulus clouds with copious quantities of roughly monodisperse sub-micrometre sea water particles might significantly enhance the cloud droplet number concentration, and thereby the cloud albedo and possibly longevity. This would produce a cooling, which general circulation model (GCM) computations suggest could-subject to satisfactory resolution of technical and scientific problems identified herein-have the capacity to balance global warming up to the carbon dioxide-doubling point. We describe herein an account of our recent research on a number of critical issues associated with MCB. This involves (i) GCM studies, which are our primary tools for evaluating globally the effectiveness of MCB, and assessing its climate impacts on rainfall amounts and distribution, and also polar sea-ice cover and thickness; (ii) high-resolution modelling of the effects of seeding on marine stratocumulus, which are required to understand the complex array of interacting processes involved in cloud brightening; (iii) microphysical modelling sensitivity studies, examining the influence of seeding amount, seed-particle salt-mass, air-mass characteristics, updraught speed and other parameters on cloud-albedo change; (iv) sea water spray-production techniques; (v) computational fluid dynamics studies of possible large-scale periodicities in Flettner rotors; and (vi) the planning of a three-stage limited-area field research experiment, with the primary objectives of technology testing and determining to what extent, if any, cloud albedo might be enhanced by seeding marine stratocumulus clouds on a spatial scale of around 100×100 km. We stress that there would be no justification for deployment of MCB unless it was clearly established that no significant adverse consequences would result. There would also need to be an international agreement firmly in favour of such action.

Screening of monoclonal antibody formulations based on high-throughput thermostability and viscosity measurements: design of experiment and statistical analysis.

The purpose of this study was to demonstrate the utility of combining a design of experiment (DOE) approach with high-throughput formulation screening to identify the main factors affecting protein thermostability and solution viscosity. The optimization of buffer compositions was guided by statistical analysis of the data to obtain the targeted combination of low viscosity and high thermostability. Different monoclonal antibody (mAb) formulation variables were evaluated in the study to achieve optimization of two parameters: (i) thermostability characterized by temperature of hydrophobic exposure and (ii) viscosity. High-throughput measurements were employed to characterize both parameters. The significance of each factor and the two-way interactions between them was studied by multivariable regression analysis. An experimental design was used to estimate the significance of all factors, including interaction effects. The range of optimal buffer compositions that maximized thermostability and minimized viscosity of a mAb formulation was determined. The described high-throughput methods are well suited for characterization of multiple protein formulation compositions with minimized resources such as time and material. The DOE approach can be successfully applied to the screening of mAb formulations early in the development lifecycle.

Global temperature stabilization via controlled albedo enhancement of low-level maritime clouds.

An assessment is made herein of the proposal that controlled global cooling sufficient to balance global warming resulting from increasing atmospheric CO2 concentrations might be achieved by seeding low-level, extensive maritime clouds with seawater particles that act as cloud condensation nuclei, thereby activating new droplets and increasing cloud albedo (and possibly longevity). This paper focuses on scientific and meteorological aspects of the scheme. Associated technological issues are addressed in a companion paper. Analytical calculations, cloud modelling and (particularly) GCM computations suggest that, if outstanding questions are satisfactorily resolved, the controllable, globally averaged negative forcing resulting from deployment of this scheme might be sufficient to balance the positive forcing associated with a doubling of CO2 concentration. This statement is supported quantitatively by recent observational evidence from three disparate sources. We conclude that this technique could thus be adequate to hold the Earth's temperature constant for many decades. More work--especially assessments of possible meteorological and climatological ramifications--is required on several components of the scheme, which possesses the advantages that (i) it is ecologically benign--the only raw materials being wind and seawater, (ii) the degree of cooling could be controlled, and (iii) if unforeseen adverse effects occur, the system could be immediately switched off, with the forcing returning to normal within a few days (although the response would take a much longer time).

Simplification of the representation of the organic component of atmospheric particulates.

We present an analysis of recent field data to investigate the variation in the organic component of atmospheric aerosol and its behaviour in the moist environment. In all locations the degree of oxygenation of the organic material increases with photochemical age, as does the particulate hygroscopicity. These changes will generally occur in spatial scales comparable to a single cell in global models at representative boundary layer wind speeds. Using ADDEM, a new model of the equilibrium state of multicomponent aerosol, we show that inorganic component changes must be responsible for the increase in particulate hygroscopicity with photochemical age. It is suggested that a common representation of nearfield and background organic aerosol composition is sufficient to describe the behaviour of organic components in a variety of field experiments; nearfield small mode organics being dominated by a combustion-derived unoxidised signature, whilst the background accumulation mode is more oxygenated and dominates in air masses with a photochemical age of more than a couple of days. This representation may be used within the sub-saturated regime to predict the behaviour of ambient particulates in the moist atmosphere. Whether a similar common representation can be used for cloud activation prediction in supersaturated environments, or for investigation of gas-to-particle partitioning, should be investigated.