The correct representation of Antarctic clouds in atmospheric models is crucial for accurate projections of the future Antarctic climate. This is particularly true for summer clouds which play a critical role in the surface melting of the ice shelves in the vicinity of the Weddell Sea. The pristine atmosphere over the Antarctic coast is characterized by low concentrations of ice nucleating particles (INPs) which often result in the formation of supercooled liquid clouds. However, when ice formation occurs, the ice crystal number concentrations (ICNCs) are substantially higher than those predicted by existing primary ice nucleation parameterizations. The rime-splintering mechanism, thought to be the dominant secondary ice production (SIP) mechanism at temperatures between −8 and −3 ^∘C, is also weak in the Weather and Research Forecasting model. Including a parameterization for SIP due to breakup (BR) from collisions between ice particles improves the ICNC representation in the modeled mixed-phase clouds, suggesting that BR could account for the enhanced ICNCs often found in Antarctic clouds. The model results indicate that a minimum concentration of about ∼ 0.1 L⁻¹ of primary ice crystals is necessary and sufficient to initiate significant breakup to explain the observations, while our findings show little sensitivity to increasing INPs. The BR mechanism is currently not represented in most weather prediction and climate models; including this process can have a significant impact on the Antarctic radiation budget.

Secondary ice production (SIP) commonly occurs in coastal Antarctic stratocumulus, affecting their ice number concentrations (N_ice) and radiative properties. However, SIP is poorly understood and crudely parametrized in models. By evaluating how well SIP is captured in a cloud‐resolving model, with a high‐resolution nest within a parent domain, we test how an improved comparison with aircraft observations affects the modeled cloud radiative properties. Under the assumption that primary ice is suitably represented by the model, we must enhance SIP by up to an order of magnitude to simulate observed N_ice. Over the nest, a surface warming trend accompanied the SIP increase; however, this trend was not captured by the parent domain over the same region. Our results suggest that the radiative properties of microphysical features resolved in high‐resolution nested domains may not be captured by coarser domains, with implications for large‐scale radiative balance studies over the Antarctic continent.

Airborne measurements of biomass burning organic aerosol (BBOA) from boreal forest fires reveal highly contrasting properties for plumes of different ages. These measurements, performed using an Aerodyne Research Inc. compact time-of-flight aerosol mass spectrometer (C-ToF-AMS) during the BORTAS (quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites) experiment in the summer of 2011, have been used to derive normalised excess organic aerosol (OA) mass concentrations (ΔOA / ΔCO), with higher average ratios observed closer to source (0.190±0.010) than in the far-field (0.097±0.002). The difference in ΔOA / ΔCO between fresh and aged plumes is influenced by a change in dominant combustion conditions throughout the campaign. Measurements at source comprised 3 plume interceptions during a single research flight and sampled largely smouldering fires. Twenty-three interceptions were made across four flights in the far-field, with plumes originating from fires occurring earlier in the campaign when fire activity had been more intense, creating an underlying contrast in emissions prior to any transformations associated with aging. Changing combustion conditions also affect the vertical distribution of biomass burning emissions, as aged plumes from more flaming-dominated fires are injected to higher altitudes of up to 6000 m. Proportional contributions of the mass-to-charge ratio (m/z) 60 and 44 peaks in the AMS mass spectra to the total OA mass (denoted f₆₀ and f₄₄) are used as tracers for primary and oxidised BBOA, respectively. f₄₄ is lower on average in near-field plumes than those sampled in the far-field, in accordance with longer aging times as plumes are transported a greater distance from source. However, high levels of ΔO₃ / ΔCO and −log(NO_x / NO_y) close to source indicate that emissions can be subject to very rapid oxidation over short timescales. Conversely, the lofting of plumes into the upper troposphere can lead to the retention of source profiles after transportation over extensive temporal and spatial scales, with f₆₀ also higher on average in aged plumes. Evolution of OA composition with aging is comparable to observations of BB tracers in previous studies, revealing a consistent progression from f₆₀ to f₄₄. The elevated levels of oxygenation in aged plumes, and their association with lower average ΔOA / ΔCO, are consistent with OA loss through evaporation during aging due to a combination of dilution and chemical processing, while differences in combustion conditions throughout the campaign also have a significant influence on BBOA production and composition.

High-resolution CH₄ and CO₂ measurements were made on board the FAAM BAe-146 UK (Facility for Airborne Atmospheric Measurements, British Aerospace-146) atmospheric research aircraft during a number of field campaigns. The system was based on an infrared spectrometer using the cavity-enhanced absorption spectroscopy technique. Correction functions to convert the mole fractions retrieved from the spectroscopy to dry-air mole fractions were derived using laboratory experiments and over a 3 month period showed good stability. Long-term performance of the system was monitored using WMO (World Meteorological Office) traceable calibration gases. During the first year of operation (29 flights) analysis of the system's in-flight calibrations suggest that its measurements are accurate to 1.28 ppb (1σ repeatability at 1 Hz = 2.48 ppb) for CH₄ and 0.17 ppm (1σ repeatability at 1 Hz = 0.66 ppm) for CO₂. The system was found to be robust, no major motion or altitude dependency could be detected in the measurements. An inter-comparison between whole-air samples that were analysed post-flight for CH₄ and CO₂ by cavity ring-down spectroscopy showed a mean difference between the two techniques of −2.4 ppb (1σ = 2.3 ppb) for CH₄ and −0.22 ppm (1σ = 0.45 ppm) for CO₂. In September 2012, the system was used to sample biomass-burning plumes in Brazil as part of the SAMBBA project (South AMerican Biomass Burning Analysis). From these and simultaneous CO measurements, emission factors for savannah fires were calculated. These were found to be 2.2 ± 0.2 g (kg dry matter)⁻¹ for CH₄ and 1710 ± 171 g (kg dry matter)⁻¹ for CO₂, which are in excellent agreement with previous estimates in the literature.

Isotopic data provide powerful constraints on regional and global methane emissions and their source profiles. However, inverse modeling of spatially resolved methane flux is currently constrained by a lack of information on the variability of source isotopic signatures. In this study, isotopic signatures of emissions in the Fennoscandian Arctic have been determined in chambers over wetland, in the air 0.3 to 3 m above the wetland surface and by aircraft sampling from 100 m above wetlands up to the stratosphere. Overall, the methane flux to atmosphere has a coherent δ¹³C isotopic signature of −71 ± 1‰, measured in situ on the ground in wetlands. This is in close agreement with δ¹³C isotopic signatures of local and regional methane increments measured by aircraft campaigns flying through air masses containing elevated methane mole fractions. In contrast, results from wetlands in Canadian boreal forest farther south gave isotopic signatures of −67 ± 1‰. Wetland emissions dominate the local methane source measured over the European Arctic in summer. Chamber measurements demonstrate a highly variable methane flux and isotopic signature, but the results from air sampling within wetland areas show that emissions mix rapidly immediately above the wetland surface and methane emissions reaching the wider atmosphere do indeed have strongly coherent C isotope signatures. The study suggests that for boreal wetlands (>60°N) global and regional modeling can use an isotopic signature of −71‰ to apportion sources more accurately, but there is much need for further measurements over other wetlands regions to verify this.

We describe the motivation, design, and execution of the Greenhouse gAs Uk and Global Emissions (GAUGE) project. The overarching scientific objective of GAUGE was to use atmospheric data to estimate the magnitude, distribution, and uncertainty of the UK greenhouse gas (GHG, defined here as CO₂, CH₄, and N₂O) budget, 2013–2015. To address this objective, we established a multi-year and interlinked measurement and data analysis programme, building on an established tall-tower GHG measurement network. The calibrated measurement network comprises ground-based, airborne, ship-borne, balloon-borne, and space-borne GHG sensors. Our choice of measurement technologies and measurement locations reflects the heterogeneity of UK GHG sources, which range from small point sources such as landfills to large, diffuse sources such as agriculture. Atmospheric mole fraction data collected at the tall towers and on the ships provide information on sub-continental fluxes, representing the backbone to the GAUGE network. Additional spatial and temporal details of GHG fluxes over East Anglia were inferred from data collected by a regional network. Data collected during aircraft flights were used to study the transport of GHGs on local and regional scales. We purposely integrated new sensor and platform technologies into the GAUGE network, allowing us to lay the foundations of a strengthened UK capability to verify national GHG emissions beyond the project lifetime. For example, current satellites provide sparse and seasonally uneven sampling over the UK mainly because of its geographical size and cloud cover. This situation will improve with new and future satellite instruments, e.g. measurements of CH₄ from the TROPOspheric Monitoring Instrument (TROPOMI) aboard Sentinel-5P. We use global, nested, and regional atmospheric transport models and inverse methods to infer geographically resolved CO₂ and CH₄ fluxes. This multi-model approach allows us to study model spread in a posteriori flux estimates. These models are used to determine the relative importance of different measurements to infer the UK GHG budget. Attributing observed GHG variations to specific sources is a major challenge. Within a UK-wide spatial context we used two approaches: (1) Δ¹⁴CO₂ and other relevant isotopologues (e.g. δ¹³CCH₄) from collected air samples to quantify the contribution from fossil fuel combustion and other sources, and (2) geographical separation of individual sources, e.g. agriculture, using a high-density measurement network. Neither of these represents a definitive approach, but they will provide invaluable information about GHG source attribution when they are adopted as part of a more comprehensive, long-term national GHG measurement programme. We also conducted a number of case studies, including an instrumented landfill experiment that provided a test bed for new technologies and flux estimation methods. We anticipate that results from the GAUGE project will help inform other countries on how to use atmospheric data to quantify their nationally determined contributions to the Paris Agreement.