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Aircraft observations in a cold-air outbreak to the north of the United Kingdom are used to examine the boundary layer and cloud properties in an overcast mixed-phase stratocumulus cloud layer and across the transition to more broken open-cellular convection. The stratocumulus cloud is primarily composed of liquid drops with small concentrations of ice particles and there is a switch to more glaciated conditions in the shallow cumulus clouds downwind. The rapid change in cloud morphology is accompanied by enhanced precipitation with secondary ice processes becoming active and greater thermodynamic gradients in the subcloud layer. The measurements also show a removal of boundary layer accumulation mode aerosols via precipitation processes across the transition that are similar to those observed in the subtropics in pockets of open cells. Simulations using a convection-permitting (1.5-km grid spacing) regional version of the Met Office Unified Model were able to reproduce many of the salient features of the cloud field although the liquid water path in the stratiform region was too low. Sensitivity studies showed that ice was too active at removing supercooled liquid water from the cloud layer and that improvements could be made by limiting the overlap between the liquid water and ice phases. Precipitation appears to be the key mechanism responsible for initiating the transition from closed- to open-cellular convection by decoupling the boundary layer and depleting liquid water from the stratiform cloud.

Mineral dust is an important component of the climate system, affecting the radiation balance, cloud properties, biogeochemical cycles, regional circulation and precipitation, as well as having negative effects on aviation, solar energy generation and human health. Dust size and composition has an impact on all these processes. However, changes in dust size distribution and composition during transport, particularly for coarse particles, are poorly understood and poorly represented in climate models. Here we present new in situ airborne observations of dust in the Saharan Air Layer (SAL) and the marine boundary layer (MBL) at the beginning of its transatlantic transport pathway, from the AERosol Properties – Dust (AER-D) fieldwork in August 2015, within the peak season of North African dust export. This study focuses on coarse-mode dust properties, including size distribution, mass loading, shape, composition, refractive indices and optical properties. Size distributions from 0.1 to 100 µm diameter (d) are presented, fully incorporating the coarse and giant modes of dust. Within the MBL, mean effective diameter (deff) and volume median diameter (VMD) were 4.6 and 6.0 µm respectively, giant particles with a mode at 20–30 µm were observed, and composition was dominated by quartz and alumino-silicates at d > 1 µm. Within the SAL, particles larger than 20 µm diameter were always present up to 5 km altitude, in concentrations over 10−5 cm−3, constituting up to 40 % of total dust mass. Mean deff and VMD were 4.0 and 5.5 µm respectively. Larger particles were detected in the SAL than can be explained by sedimentation theory alone. Coarse-mode composition was dominated by quartz and alumino-silicates; the accumulation mode showed a strong contribution from sulfate-rich and sea salt particles. In the SAL, measured single scattering albedos (SSAs) at 550 nm representing d < 2.5 µm were 0.93 to 0.98 (mean 0.97). Optical properties calculated for the full size distribution (0.1 < d < 100 µm) resulted in lower SSAs of 0.91–0.98 (mean 0.95) and mass extinction coefficients of 0.27–0.35 m2 g−1 (mean 0.32 m2 g−1). Variability in SSA was mainly controlled by variability in dust composition (principally iron) rather than by variations in the size distribution, in contrast with previous observations over the Sahara where size is the dominant influence. It is important that models are able to capture the variability and evolution of both dust composition and size distribution with transport in order to accurately represent the impacts of dust on climate. These results provide a new SAL dust dataset, fully representing coarse and giant particles, to aid model validation and development.

A key challenge for numerical weather prediction models is representing boundary layer clouds in cold air outbreaks (CAOs). One important aspect is the evolution of microphysical properties as stratocumulus transitions to open cellular convection. Abel et al. (2017) have shown, for the first time from in situ field observations, that the break-up in CAOs over the eastern Atlantic may be controlled by the development of precipitation in the cloud system while the boundary layer becomes decoupled. This paper describes that case and examines in situ measurements from three more CAOs. Flights were conducted using the UK Facility for Airborne Atmospheric Measurements (FAAM) British Aerospace-146 (BAe-146) aircraft in the North Atlantic region around the UK, making detailed microphysical measurements in the stratiform boundary layer. As the cloudy boundary layer evolves prior to break-up, increasing liquid water paths (LWPs) and drop sizes and the formation of liquid precipitation are observed. Small numbers of ice particles, typically a few per litre, are also observed. Eventually LWPs reduce significantly due to loss of water from the stratocumulus cloud (SC) layer. In three of the cases, aerosols are removed from the boundary layer across the transition. This process appears to be similar to those observed in warm clouds and pockets of open cells (POCs) in the subtropics. After break-up, deeper convective clouds form with bases warm enough for secondary ice production (SIP), leading to rapid glaciation. It is concluded that the precipitation is strongly associated with the break-up, with both weakening of the capping inversion and boundary layer decoupling also observed.

The global variation in ice-nucleating particle (INP) concentrations is an important modulator of the cloud-phase feedback, where the albedo of mixed-phase clouds increases in a warming climate. Shallow clouds, such as those observed in cold-air outbreaks (CAOs), are particularly important for cloud-phase feedbacks and highly sensitive to INPs. To investigate the sources and concentrations of INPs in CAOs, we made airborne measurements over the Norwegian and Barents seas as part of the March 2022 Arctic Cold-Air Outbreak (ACAO) field campaign. Aerosol samples were collected on filters at locations above, below and upstream of CAO cloud decks. Throughout the campaign, INP concentrations were comparable to the highest concentrations previously observed in the Arctic. Scanning electron microscopy analysis of samples taken upstream of cloud decks showed that supermicron aerosol was dominated by mineral dusts. Analysis of aerosol particle size measurements to obtain an INP active site density suggested sea spray was unlikely to be the dominant INP type. These site densities were also too great for mineral components alone to be the dominant INP type above −20 °C. Accordingly, it is likely that the dominant INP type was mineral dust mixed with other ice-nucleating materials, possibly of biogenic origin. Back-trajectory analysis and meteorological conditions suggested a lack of local INP sources. We therefore hypothesise that the high INP concentration is most likely to be associated with aged aerosol in Arctic haze that has undergone long-range transport from lower-latitude regions.

This work presents synergistic satellite, airborne and surface-based observations of a pocket of open cells (POC) in the remote south-east Atlantic. The observations were obtained over and upwind of Ascension Island during the CLouds and Aerosol Radiative Impacts and Forcing (CLARIFY) and the Layered Smoke Interacting with Clouds (LASIC) field experiments. A novel aspect of this case study is that an extensive free-tropospheric biomass burning aerosol plume that had been transported from the African continent was observed to be in contact with the boundary layer inversion over the POC and the surrounding closed cellular cloud regime. The in situ measurements show marked contrasts in the boundary layer thermodynamic structure, cloud properties, precipitation and aerosol conditions between the open cells and surrounding overcast cloud field. The data demonstrate that the overlying biomass burning aerosol was mixing down into the boundary layer in the stratocumulus cloud downwind of the POC, with elevated carbon monoxide, black carbon mass loadings and accumulation-mode aerosol concentrations measured beneath the trade-wind inversion. The stratocumulus cloud in this region was moderately polluted and exhibited very little precipitation falling below cloud base. A rapid transition to actively precipitating cumulus clouds and detrained stratiform remnants in the form of thin quiescent veil clouds was observed across the boundary into and deep within the POC. The subcloud layer in the POC was much cleaner than that in the stratocumulus region. The clouds in the POC formed within an ultra-clean layer (accumulation-mode aerosol concentrations of approximately a few cm−3) in the upper region of the boundary layer, which was likely to have been formed via efficient collision–coalescence and sedimentation processes. Enhanced Aitken-mode aerosol concentrations were also observed intermittently in this ultra-clean layer, suggesting that new particle formation was taking place. Across the boundary layer inversion and immediately above the ultra-clean layer, accumulation-mode aerosol concentrations were ∼ 1000 cm−3. Importantly, the air mass in the POC showed no evidence of elevated carbon monoxide over and above typical background conditions at this location and time of year. As carbon monoxide is a good tracer for biomass burning aerosol that is not readily removed by cloud processing and precipitation, it demonstrates that the open cellular convection in the POC is not able to entrain large quantities of the free-tropospheric aerosol that was sitting directly on top of the boundary layer inversion. This suggests that the structure of the mesoscale cellular convection may play an important role in regulating the transport of aerosol from the free troposphere down into the marine boundary layer. We then develop a climatology of open cellular cloud conditions in the south-east Atlantic from 19 years of September Moderate Resolution Imaging Spectroradiometer (MODIS) Terra imagery. This shows that the maxima in open cell frequency (> 0.25) occurs far offshore and in a region where subsiding biomass burning aerosol plumes may often come into contact with the underlying boundary layer cloud. If the results from the observational case study applied more broadly, then the apparent low susceptibility of open cells to free-tropospheric intrusions of additional cloud condensation nuclei could have some important consequences for aerosol–cloud interactions in the region.

During the summertime, dust from the Sahara can be efficiently transported westwards within the Saharan air layer (SAL). This can lead to high aerosol loadings being observed above a relatively clean marine boundary layer (MBL) in the tropical Atlantic Ocean. These dust layers can impart significant radiative effects through strong visible and IR light absorption and scattering, and can also have indirect impacts by altering cloud properties. The processing of the dust aerosol can result in changes in both direct and indirect radiative effects, leading to significant uncertainty in climate prediction in this region. During August 2015, measurements of aerosol and cloud properties were conducted off the coast of west Africa as part of the Ice in Cloud Experiment – Dust (ICE-D) and AERosol properties – Dust (AER-D) campaigns. Observations were obtained over a 4-week period using the UK Facility for Atmospheric Airborne Measurements (FAAM) BAe 146 aircraft based on Santiago Island, Cabo Verde. Ground-based observations were collected from Praia (14∘57′ N, 23∘29′ W; 100 m a.s.l.), also located on Santiago Island. The dust in the SAL was mostly sampled in situ at altitudes of 2–4 km, and the potential dust age was estimated by backward trajectory analysis. The particle mass concentration (at diameter d = 0.1–20 µm) decreased with transport time. Mean effective diameter (Deff) for supermicron SAL dust (d = 1–20 µm) was found to be 5–6 µm regardless of dust age, whereas submicron Deff (d = 0.1–1 µm) showed a decreasing trend with longer transport. For the first time, an airborne laser-induced incandescence instrument (the single particle soot photometer – SP2) was deployed to measure the hematite content of dust. For the Sahel-influenced dust in the SAL, the observed hematite mass fraction of dust (FHm) was found to be anti-correlated with the single scattering albedo (SSA, λ = 550 nm, for particles d < 2.5 µm); as potential dust age increased from 2 to 7 days, FHm increased from 2.5 to 4.5 %, SSA decreased from 0.97 to 0.93 and the derived imaginary part (k) of the refractive index at 550 nm increased from 0.0015 to 0.0035. However, the optical properties of Sahara-influenced plumes (not influenced by the Sahel) were independent of dust age and hematite content with SSA ∼ 0.95 and k ∼ 0.0028. This indicates that the absorbing component of dust may be source dependent, or that gravitational settling of larger particles may lead to a higher fraction of more absorbing clay–iron aggregates at smaller sizes. Mie calculation using the measured size distribution and size-resolved refractive indices of the absorbing components (black carbon and hematite) reproduces the measured SSA to within ±0.02 for SAL dust by assuming a goethite ∕ hematite mass ratio of 2. Overall, hematite and goethite constituted 40–80 % of the absorption for particles d < 2.5 µm, and black carbon (BC) contributed 10–37 %. This highlights the importance of size-dependent composition in determining the optical properties of dust and also the contribution from BC within dust plumes.

During austral summer 2015, the Microphysics of Antarctic Clouds (MAC) field campaign collected unique and detailed airborne and ground-based in situ measurements of cloud and aerosol properties over coastal Antarctica and the Weddell Sea. This paper presents the first results from the experiment and discusses the key processes important in this region, which is critical to predicting future climate change. The sampling was predominantly of stratus clouds, at temperatures between −20 and 0 °C. These clouds were dominated by supercooled liquid water droplets, which had a median concentration of 113 cm−3 and an interquartile range of 86 cm−3. Both cloud liquid water content and effective radius increased closer to cloud top. The cloud droplet effective radius increased from 4 ± 2 µm near cloud base to 8 ± 3 µm near cloud top. Cloud ice particle concentrations were highly variable with the ice tending to occur in small, isolated patches. Below approximately 1000 m, glaciated cloud regions were more common at higher temperatures; however, the clouds were still predominantly liquid throughout. When ice was present at temperatures higher than −10 °C, secondary ice production most likely through the Hallett–Mossop mechanism led to ice concentrations 1 to 3 orders of magnitude higher than the number predicted by commonly used primary ice nucleation parameterisations. The drivers of the ice crystal variability are investigated. No clear dependence on the droplet size distribution was found. The source of first ice in the clouds remains uncertain but may include contributions from biogenic particles, blowing snow or other surface ice production mechanisms. The concentration of large aerosols (diameters 0.5 to 1.6 µm) decreased with altitude and were depleted in air masses that originated over the Antarctic continent compared to those more heavily influenced by the Southern Ocean and sea ice regions. The dominant aerosol in the region was hygroscopic in nature, with the hygroscopicity parameter κ having a median value for the campaign of 0.66 (interquartile range of 0.38). This is consistent with other remote marine locations that are dominated by sea salt/sulfate.

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.

We demonstrate, for the first time, continuous real-time observations of airborne bio-fluorescent aerosols recorded at the British Antarctic Survey's Halley VI Research Station, located on the Brunt Ice Shelf close to the Weddell Sea coast (lat 75°34′59′′ S, long 26°10′0′′ W) during Antarctic summer, 2015. As part of the NERC MAC (Microphysics of Antarctic Clouds) aircraft aerosol cloud interaction project, observations with a real-time ultraviolet-light-induced fluorescence (UV-LIF) spectrometer were conducted to quantify airborne biological containing particle concentrations along with dust particles as a function of wind speed and direction over a 3-week period. Significant, intermittent enhancements of both non- and bio-fluorescent particles were observed to varying degrees in very specific wind directions and during strong wind events. Analysis of the particle UV-induced emission spectra, particle sizes and shapes recorded during these events suggest the majority of particles were likely a subset of dust with weak fluorescence emission responses. A minor fraction, however, were likely primary biological particles that were very strongly fluorescent, with a subset identified as likely being pollen based on comparison with laboratory data obtained using the same instrument. A strong correlation of bio-fluorescent particles with wind speed was observed in some, but not all, periods. Interestingly, the fraction of fluorescent particles to total particle concentration also increased significantly with wind speed during these events. The enhancement in concentrations of these particles could be interpreted as due to resuspension from the local ice surface but more likely due to emissions from distal sources within Antarctica as well as intercontinental transport. Likely distal sources identified by back trajectory analyses and dispersion modelling were the coastal ice margin zones in Halley Bay consisting of bird colonies with likely associated high bacterial activity together with contributions from exposed ice margin bacterial colonies but also long-range transport from the southern coasts of Argentina and Chile. Dispersion modelling also demonstrated emissions from shipping lanes, and therefore marine anthropogenic sources cannot be ruled out. Average total concentrations of total fluorescent aerosols were found to be 1.9 ± 2.6 L−1 over a 3-week period crossing over from November into December, but peak concentrations during intermittent enhancement events could be up to several tens per litre. While this short pilot study is not intended to be generally representative of Antarctic aerosol, it demonstrates the usefulness of the UV-LIF measurement technique for quantification of airborne bioaerosol concentrations and to understand their dispersion. The potential importance for microbial colonisation of Antarctica is highlighted.

Measurements of mid- to far-infrared nadir radiances obtained from the UK Facility for Airborne Atmospheric Measurements (FAAM) BAe 146 aircraft during the Cirrus Coupled Cloud-Radiation Experiment (CIRCCREX) are used to assess the performance of various ice cloud bulk optical property models. Through use of a minimization approach, we find that the simulations can reproduce the observed spectra in the mid-infrared to within measurement uncertainty, but they are unable to simultaneously match the observations over the far-infrared frequency range. When both mid- and far-infrared observations are used to minimize residuals, first-order estimates of the spectral flux differences between the best-performing simulations and observations indicate a compensation effect between the mid- and far-infrared such that the absolute broadband difference is < 0.7 W m−2. However, simply matching the spectra using the mid-infrared (far-infrared) observations in isolation leads to substantially larger discrepancies, with absolute differences reaching ∼ 1.8 (3.1) W m−2. These results show that simulations using these microphysical models may give a broadly correct integrated longwave radiative impact but that this masks spectral errors, with implicit consequences for the vertical distribution of atmospheric heating. They also imply that retrievals using these models applied to mid-infrared radiances in isolation will select cirrus optical properties that are inconsistent with far-infrared radiances. As such, the results highlight the potential benefit of more extensive far-infrared observations for the assessment and, where necessary, the improvement of current ice bulk optical models.