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To evaluate the SEVIRI retrieval for aerosols above clouds presented in Part 1 of the companion paper, the algorithm is applied over the south-east Atlantic Ocean during the CLARIFY-2017 field campaign period. The first step of our analysis compares the retrieved aerosol and cloud properties against equivalent products from the MODIS MOD06ACAERO retrieval (Meyer et al., 2015). While the correlation between the two satellite retrievals of the above-cloud aerosol optical thickness (AOT) is good (R = 0.78), the AOT retrieved by SEVIRI is 20.3 % smaller than that obtained from the MODIS retrieval. This difference in AOT is attributed mainly to the more absorbing aerosol model assumed for the SEVIRI retrieval compared to MODIS. The underlying cloud optical thickness (COT) derived from the two satellites is in good agreement (R = 0.90). The cloud droplet effective radius (CER) retrieved by SEVIRI is consistently smaller than MODIS by 2.2 µm, which is mainly caused by the use of different spectral bands of the satellite instruments. In the second part of our analysis, we compare the forecast water vapour profiles used for the SEVIRI atmospheric correction as well as the aforementioned aerosol and cloud products with in situ measurements made from the Facility for Airborne Atmospheric Measurements (FAAM) aircraft platform during the CLARIFY-2017 campaign. Around Ascension Island, the column water vapour used to correct the SEVIRI signal is overestimated by 3.1 mm in the forecast compared to that measured by dropsondes. However, the evidence suggests that the accuracy of the atmospheric correction improves closer to the African coast. Consistency is observed between the SEVIRI above-cloud AOT and in situ measurements (from cavity ring-down spectroscopy instruments) when the measured single-scattering albedo is close to that assumed in the retrieval algorithm. On the other hand, the satellite retrieval overestimates the AOT when the assumed aerosol model is not absorbing enough. Consistency is also found between the cloud properties retrieved by SEVIRI and the CER measured by a cloud droplet probe and the liquid water path derived from a microwave radiometer. Despite the instrumental limitations of the geostationary satellite, the consistency obtained between SEVIRI, MODIS and the aircraft measurements demonstrates the ability of the retrieval in providing additional information on the temporal evolution of the aerosol properties above clouds.

The representations of clouds, aerosols, and cloud–aerosol–radiation impacts remain some of the largest uncertainties in climate change, limiting our ability to accurately reconstruct past climate and predict future climate. The south-east Atlantic is a region where high atmospheric aerosol loadings and semi-permanent stratocumulus clouds are co-located, providing an optimum region for studying the full range of aerosol–radiation and aerosol–cloud interactions and their perturbations of the Earth's radiation budget. While satellite measurements have provided some useful insights into aerosol–radiation and aerosol–cloud interactions over the region, these observations do not have the spatial and temporal resolution, nor the required level of precision to allow for a process-level assessment. Detailed measurements from high spatial and temporal resolution airborne atmospheric measurements in the region are very sparse, limiting their use in assessing the performance of aerosol modelling in numerical weather prediction and climate models. CLARIFY-2017 was a major consortium programme consisting of five principal UK universities with project partners from the UK Met Office and European- and USA-based universities and research centres involved in the complementary ORACLES, LASIC, and AEROCLO-sA projects. The aims of CLARIFY-2017 were fourfold: (1) to improve the representation and reduce uncertainty in model estimates of the direct, semi-direct, and indirect radiative effect of absorbing biomass burning aerosols; (2) to improve our knowledge and representation of the processes determining stratocumulus cloud microphysical and radiative properties and their transition to cumulus regimes; (3) to challenge, validate, and improve satellite retrievals of cloud and aerosol properties and their radiative impacts; (4) to improve the impacts of aerosols in weather and climate numerical models. This paper describes the modelling and measurement strategies central to the CLARIFY-2017 deployment of the FAAM BAe146 instrumented aircraft campaign, summarizes the flight objectives and flight patterns, and highlights some key results from our initial analyses.

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.

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 −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.

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.

The next generation of European polar orbiting weather satellites will carry a novel instrument, the Ice Cloud Imager (ICI), which uses passive observations between 183 and 664 GHz to make daily global observations of cloud ice. Successful use of these observations requires accurate modelling of cloud ice scattering, and this study uses airborne observations from two flights of the Facility for Airborne Atmospheric Measurements (FAAM) BAe 146 research aircraft to validate radiative transfer simulations of cirrus clouds at frequencies between 325 and 664 GHz using the Atmospheric Radiative Transfer Simulator (ARTS) and a state-of-the-art database of cloud ice optical properties. Particular care is taken to ensure that the inputs to the radiative transfer model are representative of the true atmospheric state by combining both remote-sensing and in situ observations of the same clouds to create realistic vertical profiles of cloud properties that are consistent with both observed particle size distributions and bulk ice mass. The simulations are compared to measurements from the International Submillimetre Airborne Radiometer (ISMAR), which is an airborne demonstrator for ICI. It is shown that whilst they are generally able to reproduce the observed cloud signals, for a given ice water path (IWP) there is considerable sensitivity to the cloud microphysics, including the distribution of ice mass within the cloud and the ice particle habit. Accurate retrievals from ICI will therefore require realistic representations of cloud microphysical properties.

Abstract Secondary ice production (SIP) commonly occurs in coastal Antarctic stratocumulus, affecting their ice number concentrations (Nice) 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 Nice. 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.

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.

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 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

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.

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.

In situ airborne observations of cloud microphysics, aerosol properties, and thermodynamic structure over the transition from sea ice to ocean are presented from the Aerosol-Cloud Coupling And Climate Interactions in the Arctic (ACCACIA) campaign. A case study from 23 March 2013 provides a unique view of the cloud microphysical changes over this transition under cold-air outbreak conditions. Cloud base lifted and cloud depth increased over the transition from sea ice to ocean. Mean droplet number concentrations, Ndrop, also increased from 110 ± 36 cm−3 over the sea ice to 145 ± 54 cm−3 over the marginal ice zone (MIZ). Downstream over the ocean, Ndrop decreased to 63 ± 30 cm−3. This reduction was attributed to enhanced collision-coalescence of droplets within the deep ocean cloud layer. The liquid water content increased almost four fold over the transition and this, in conjunction with the deeper cloud layer, allowed rimed snowflakes to develop and precipitate out of cloud base downstream over the ocean. The ice properties of the cloud remained approximately constant over the transition. Observed ice crystal number concentrations averaged approximately 0.5–1.5 L−1, suggesting only primary ice nucleation was active; however, there was evidence of crystal fragmentation at cloud base over the ocean. Little variation in aerosol particle number concentrations was observed between the different surface conditions; however, some variability with altitude was observed, with notably greater concentrations measured at higher altitudes ( > 800 m) over the sea ice. Near-surface boundary layer temperatures increased by 13 °C from sea ice to ocean, with corresponding increases in surface heat fluxes and turbulent kinetic energy. These significant thermodynamic changes were concluded to be the primary driver of the microphysical evolution of the cloud. This study represents the first investigation, using in situ airborne observations, of cloud microphysical changes with changing sea ice cover and addresses the question of how the microphysics of Arctic stratiform clouds may change as the region warms and sea ice extent reduces.

Heavy rainfall from convective clouds can lead to devastating flash flooding, and observations of aerosols and clouds are required to improve cloud parameterisations used in precipitation forecasts. We present measurements of boundary layer aerosol concentration, size, and composition from a series of research flights performed over the southwest peninsula of the UK during the COnvective Precipitation Experiment (COPE) of summer 2013. We place emphasis on periods of southwesterly winds, which locally are most conducive to convective cloud formation, when marine air from the Atlantic reached the peninsula. Accumulation-mode aerosol mass loadings were typically 2–3 µg m−3 (corrected to standard cubic metres at 1013.25 hPa and 273.15 K), the majority of which was sulfuric acid over the sea, or ammonium sulfate inland, as terrestrial ammonia sources neutralised the aerosol. The cloud condensation nuclei (CCN) concentrations in these conditions were ∼ 150–280 cm−3 at 0.1 % and 400–500 cm−3 at 0.9 % supersaturation (SST), which are in good agreement with previous Atlantic measurements, and the cloud drop concentrations at cloud base ranged from 100 to 500 cm−3. The concentration of CCN at 0.1 % SST was well correlated with non-sea-salt sulfate, meaning marine sulfate formation was likely the main source of CCN. Marine organic aerosol (OA) had a similar mass spectrum to previous measurements of sea spray OA and was poorly correlated with CCN. In one case study that was significantly different to the rest, polluted anthropogenic emissions from the southern and central UK advected to the peninsula, with significant enhancements of OA, ammonium nitrate and sulfate, and black carbon. The CCN concentrations here were around 6 times higher than in the clean cases, and the cloud drop number concentrations were 3–4 times higher. Sources of ice-nucleating particles (INPs) were assessed by comparing different parameterisations used to predict INP concentrations, using measured aerosol concentrations as input. The parameterisations based on total aerosol produced INP concentrations that agreed within an order of magnitude with measured first ice concentrations at cloud temperatures as low as −12 °C. Composition-specific parameterisations for mineral dust, fluorescent particles, and sea spray OA were 3–4 orders of magnitude lower than the measured first ice concentrations, meaning a source of INPs was present that was not characterised by our measurements and/or one or more of the composition-specific parameterisations greatly underestimated INPs in this environment.

This paper assesses the reasons for high ice number concentrations observed in orographic clouds by comparing in situ measurements from the Ice NUcleation Process Investigation And Quantification field campaign (INUPIAQ) at Jungfraujoch, Switzerland (3570 m a.s.l.) with the Weather Research and Forecasting model (WRF) simulations over real terrain surrounding Jungfraujoch. During the 2014 winter field campaign, between 20 January and 28 February, the model simulations regularly underpredicted the observed ice number concentration by 103 L−1. Previous literature has proposed several processes for the high ice number concentrations in orographic clouds, including an increased ice nucleating particle (INP) concentration, secondary ice multiplication and the advection of surface ice crystals into orographic clouds. We find that increasing INP concentrations in the model prevents the simulation of the mixed-phase clouds that were witnessed during the INUPIAQ campaign at Jungfraujoch. Additionally, the inclusion of secondary ice production upwind of Jungfraujoch into the WRF simulations cannot consistently produce enough ice splinters to match the observed concentrations. A flux of surface hoar crystals was included in the WRF model, which simulated ice concentrations comparable to the measured ice number concentrations, without depleting the liquid water content (LWC) simulated in the model. Our simulations therefore suggest that high ice concentrations observed in mixed-phase clouds at Jungfraujoch are caused by a flux of surface hoar crystals into the orographic clouds.

Single-particle compositional analysis of filter samples collected on board the Facility for Airborne Atmospheric Measurements (FAAM) BAe-146 aircraft is presented for six flights during the springtime Aerosol–Cloud Coupling and Climate Interactions in the Arctic (ACCACIA) campaign (March–April 2013). Scanning electron microscopy was utilised to derive size-segregated particle compositions and size distributions, and these were compared to corresponding data from wing-mounted optical particle counters. Reasonable agreement between the calculated number size distributions was found. Significant variability in composition was observed, with differing external and internal mixing identified, between air mass trajectory cases based on HYbrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) analyses. Dominant particle classes were silicate-based dusts and sea salts, with particles notably rich in K and Ca detected in one case. Source regions varied from the Arctic Ocean and Greenland through to northern Russia and the European continent. Good agreement between the back trajectories was mirrored by comparable compositional trends between samples. Silicate dusts were identified in all cases, and the elemental composition of the dust was consistent for all samples except one. It is hypothesised that long-range, high-altitude transport was primarily responsible for this dust, with likely sources including the Asian arid regions.

The fluorescent nature of aerosol at a high-altitude Alpine site was studied using a wide-band integrated bioaerosol (WIBS-4) single particle multi-channel ultraviolet – light-induced fluorescence (UV-LIF) spectrometer. This was supported by comprehensive cloud microphysics and meteorological measurements with the aims of cataloguing concentrations of bio-fluorescent aerosols at this high-altitude site and also investigating possible influences of UV–fluorescent particle types on cloud–aerosol processes. Analysis of background free tropospheric air masses, using a total aerosol inlet, showed there to be a minor increase in the fluorescent aerosol fraction during in-cloud cases compared to out-of-cloud cases. The size dependence of the fluorescent aerosol fraction showed the larger aerosol to be more likely to be fluorescent with 80 % of 10 μm particles being fluorescent. Whilst the fluorescent particles were in the minority (NFl∕NAll = 0.27 ± 0.19), a new hierarchical agglomerative cluster analysis approach, Crawford et al. (2015) revealed the majority of the fluorescent aerosols were likely to be representative of fluorescent mineral dust. A minor episodic contribution from a cluster likely to be representative of primary biological aerosol particles (PBAP) was also observed with a wintertime baseline concentration of 0.1 ± 0.4 L−1. Given the low concentration of this cluster and the typically low ice-active fraction of studied PBAP (e.g. pseudomonas syringae), we suggest that the contribution to the observed ice crystal concentration at this location is not significant during the wintertime.

We present microphysical observations of cumulus clouds measured over the southwest peninsula of the UK during the COnvective Precipitation Experiment (COPE) in August 2013, which are framed into a wider context using ground-based and airborne radar measurements. Two lines of cumulus clouds formed in the early afternoon along convergence lines aligned with the peninsula. The lines became longer and broader during the afternoon due to new cell formation and stratiform regions forming downwind of the convective cells. Ice concentrations up to 350 L−1, well in excess of the expected ice nuclei (IN) concentrations, were measured in the mature stratiform regions, suggesting that secondary ice production was active. Detailed sampling focused on an isolated liquid cloud that glaciated as it matured to merge with a band of cloud downwind. In the initial cell, drizzle concentrations increased from ∼ 0.5 to ∼ 20 L−1 in around 20 min. Ice concentrations developed up to a few per litre, which is around the level expected of primary IN. The ice images were most consistent with freezing drizzle, rather than smaller cloud drops or interstitial IN forming the first ice. As new cells emerged in and around the cloud, ice concentrations up to 2 orders of magnitude higher than the predicted IN concentrations developed, and the cloud glaciated over a period of 12–15 min. Almost all of the first ice particles to be observed were frozen drops, while vapour-grown ice crystals were dominant in the latter stages. Our observations are consistent with the production of large numbers of small secondary ice crystals/fragments, by a mechanism such as Hallett–Mossop or droplets shattering upon freezing. Some of the small ice froze drizzle drops on contact, while others grew more slowly by vapour deposition. Graupel and columns were seen in cloud penetrations up to the −12 °C level, though many ice particles were mixed habit due to riming and growth by vapour deposition at multiple temperatures. Our observations demonstrate that the freezing of drizzle/raindrops is an important process that dominates the formation of large ice in the intermediate stages of cloud development. As these frozen drops were the first precipitation observed, interactions between the warm-rain and secondary ice production processes appear to be key to determining the timing and location of precipitation.

During the winter of 2013 and 2014 measurements of cloud microphysical properties over a 5-week period at the high-alpine site Jungfraujoch, Switzerland, were carried out as part of the Cloud Aerosol Characterisation Experiments (CLACE) and the Ice Nucleation Process Investigation and Quantification project (INUPIAQ). Measurements of aerosol properties at a second, lower site, Schilthorn, Switzerland, were used as input for a primary ice nucleation scheme to predict ice nuclei concentrations at Jungfraujoch. Frequent, rapid transitions in the ice and liquid properties of the clouds at Jungfraujoch were identified that led to large fluctuations in ice mass fractions over temporal scales of seconds to hours. During the measurement period we observed high concentrations of ice particles that exceeded 1000 L−1 at temperatures around −15 °C, verified by multiple instruments. These concentrations could not be explained using the usual primary ice nucleation schemes, which predicted ice nucleus concentrations several orders of magnitude smaller than the peak ice crystal number concentrations. Secondary ice production through the Hallett–Mossop process as a possible explanation was ruled out, as the cloud was rarely within the active temperature range for this process. It is shown that other mechanisms of secondary ice particle production cannot explain the highest ice particle concentrations. We describe four possible mechanisms that could lead to high cloud ice concentrations generated from the snow-covered surfaces surrounding the measurement site. Of these we show that hoar frost crystals generated at the cloud enveloped snow surface could be the most important source of cloud ice concentrations. Blowing snow was also observed to make significant contributions at higher wind speeds when ice crystal concentrations were < 100 L−1.

Black carbon aerosol (BC) deposited to the Arctic sea ice or present in the free troposphere can significantly affect the Earth's radiation budget at high latitudes yet the BC burden in these regions and the regional source contributions are poorly constrained. Aircraft measurements of aerosol composition in the European Arctic were conducted during the Aerosol–Cloud Coupling And Climate Interactions in the Arctic (ACCACIA) campaign in March 2013. Pollutant plumes were encountered throughout the lower to upper Arctic troposphere featuring enhancements in CO and aerosol mass loadings, which were chemically speciated into BC and non-refractory sulphate and organic matter. FLEXPART-WRF simulations have been performed to evaluate the likely contribution to the pollutants from regional ground sources. By combining up-to-date anthropogenic and open fire biomass burning (OBB) inventories, we have been able to compare the contributions made to the observed pollution layers from the sources of eastern/northern Asia (AS), Europe (EU) and North America (NA). Over 90 % of the contribution to the BC was shown to arise from non-OBB anthropogenic sources. AS sources were found to be the major contributor to the BC burden, increasing background BC loadings by a factor of 3–5 to 100.8 ± 48.4 ng sm−3 (in standard air m3 at 273.15 K and 1013.25 mbar) and 55.8 ± 22.4 ng sm−3 in the middle and upper troposphere respectively. AS plumes close to the tropopause (about 7.5–8 km) were also observed, with BC concentrations ranging from 55 to 73 ng sm−3, which will potentially have a significant radiative impact. EU sources influenced the middle troposphere with a BC mean concentration of 70.8 ± 39.1 ng sm−3 but made a minor contribution to the upper troposphere due to the relatively high latitude of the source region. The contribution of NA was shown to be much lower at all altitudes with BC mean concentration of 20 ng sm−3. The BC transported to the Arctic is mixed with a non-BC volume fraction representing between 90–95 % of the mass, and has a relatively uniform core size distribution with mass median diameter 190–210 nm and geometric standard deviation σg = 1.55–1.65 and this varied little across all source regions. It is estimated that 60–95 % of BC is scavenged between emission and receptor based on BC / ΔCO comparisons between source inventories and measurement. We show that during the springtime of 2013, the anthropogenic pollution particularly from sources in Asia, contributed significantly to BC across the European Arctic free troposphere. In contrast to previous studies, the contribution from open wildfires was minimal. Given that Asian pollution is likely to continue to rise over the coming years, it is likely that the radiative forcing in the Arctic will also continue to increase.

Measurements from four case studies in spring and summer-time Arctic stratocumulus clouds during the Aerosol-Cloud Coupling And Climate Interactions in the Arctic (ACCACIA) campaign are presented. We compare microphysics observations between cases and with previous measurements made in the Arctic and Antarctic. During ACCACIA, stratocumulus clouds were observed to consist of liquid at cloud tops, often at distinct temperature inversions. The cloud top regions precipitated low concentrations of ice into the cloud below. During the spring cases median ice number concentrations (~ 0.5 L−1) were found to be lower by about a factor of 5 than observations from the summer campaign (~ 3 L−1). Cloud layers in the summer spanned a warmer temperature regime than in the spring and enhancement of ice concentrations in these cases was found to be due to secondary ice production through the Hallett–Mossop (H–M) process. Aerosol concentrations during spring ranged from ~ 300–400 cm−3 in one case to lower values of ~ 50–100 cm−3 in the other. The concentration of aerosol with sizes Dp > 0.5 μm was used in a primary ice nucleus (IN) prediction scheme (DeMott et al., 2010). Predicted IN values varied depending on aerosol measurement periods but were generally greater than maximum observed median values of ice crystal concentrations in the spring cases, and less than the observed ice concentrations in the summer due to the influence of secondary ice production. Comparison with recent cloud observations in the Antarctic summer (Grosvenor et al., 2012), reveals lower ice concentrations in Antarctic clouds in comparable seasons. An enhancement of ice crystal number concentrations (when compared with predicted IN numbers) was also found in Antarctic stratocumulus clouds spanning the H–M temperature zone; however, concentrations were about an order of magnitude lower than those observed in the Arctic summer cases but were similar to the peak values observed in the colder Arctic spring cases, where the H–M mechanism did not operate.

Microphysical measurements collected during eleven profiles, by the UK BAe-146 aircraft, through marine stratocumulus as part of the Variability of the American Monsoon Systems (VAMOS) Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx) are compared to collocated overpasses of the Moderate Resolution Imaging Spectroradiometer (MODIS) aboard the Aqua and Terra satellite platforms. The full depth of the cloud is sampled in each case using a Cloud Droplet Probe (CDP) and a Two-Dimensional Stereo Probe (2DS) together sizing cloud and precipitation droplets in the diameter range 2–1260 μm. This allows the total optical depth (τc) of the cloud and effective radius (re) of the droplet size distribution to be compared to MODIS cloud retrievals of the same quantities along with the secondarily derived total liquid water path. When compared to the effective radius at cloud top, the MODIS retrieved re using the 2.1 μm wavelength channel overestimates the in situ measurements on average by 13% with the largest overestimations coinciding with the detection by the 2DS of drizzle sized droplets. We show through consideration of the full vertical profile and penetration depths of the wavelengths used in the retrieval that the expected retrieved values are less than those at cloud top thus increasing the apparent bias in re retrievals particularly when using the 1.6 and 2.1 μm channels, with the 3.7 μm channel retrievals displaying the best agreement with in situ values. Retrievals of τc also tend to overestimate in situ values which, coupled with a high bias in re retrievals, lead to an overestimation of liquid water path. There is little apparent correlation between the variation of the three near-infrared re retrievals and the vertical structure of the cloud observed in situ. Retrievals are performed using measured profiles of water vapour and temperature along with an accurate knowledge of the width of the droplet size distribution which improve agreement between in situ and retrieved values but cannot completely explain the observed biases. Additionally we show that cloud heterogeneity and three-dimensional radiative effects may high skew the mean when averaging over comparison domains but cannot explain all of the apparent high bias. An intercomparison between in situ measurements from the BAe-146 and C-130 platforms is also presented, highlighting the uncertainties associated with in situ observations.

In-situ aircraft observations of ice crystal concentrations in Antarctic clouds are presented for the first time. Orographic, layer and wave clouds around the Antarctic Peninsula and Larsen Ice shelf regions were penetrated by the British Antarctic Survey's Twin Otter aircraft, which was equipped with modern cloud physics probes. The clouds studied were mostly in the free troposphere and hence ice crystals blown from the surface are unlikely to have been a major source for the ice phase. The temperature range covered by the experiments was 0 to −21 °C. The clouds were found to contain supercooled liquid water in most regions and at heterogeneous ice formation temperatures ice crystal concentrations (60 s averages) were often less than 0.07 l−1, although values up to 0.22 l−1 were observed. Estimates of observed aerosol concentrations were used as input into the DeMott et al. (2010) ice nuclei (IN) parameterisation. The observed ice crystal number concentrations were generally in broad agreement with the IN predictions, although on the whole the predicted values were higher. Possible reasons for this are discussed and include the lack of IN observations in this region with which to characterise the parameterisation, and/or problems in relating ice concentration measurements to IN concentrations. Other IN parameterisations significantly overestimated the number of ice particles. Generally ice particle concentrations were much lower than found in clouds in middle latitudes for a given temperature. Higher ice crystal concentrations were sometimes observed at temperatures warmer than −9 °C, with values of several per litre reached. These were attributable to secondary ice particle production by the Hallett Mossop process. Even in this temperature range it was observed that there were regions with little or no ice that were dominated by supercooled liquid water. It is likely that in some cases this was due to a lack of seeding ice crystals to act as rimers to initiate secondary ice particle production. This highlights the chaotic and spatially inhomogeneous nature of this process and indicates that the accurate representation of it in global models is likely to represent a challenge. However, the contrast between Hallett Mossop zone ice concentrations and the fairly low concentrations of heterogeneously nucleated ice suggests that the Hallet Mossop process has the potential to be very important in remote, pristine regions such as around the Antarctic coast.

In this paper, aircraft measurements are presented of liquid phase (ice-free) wave clouds made at temperatures greater than −5°C that formed over Scotland, UK. The horizontal variations of the vertical velocity across wave clouds display a distinct pattern. The maximum updraughts occur at the upshear flanks of the clouds and the strong downdraughts at the downshear flanks. The cloud droplet concentrations were a couple of hundreds per cubic centimetres, and the drops generally had a mean diameter between 15–45 μm. A small proportion of the drops were drizzle. The measurements presented here and in previous recent studies suggest a different interaction of dynamics and microphysics in wave clouds from the accepted model. The results in this paper provide a case for future numerical simulation of wave cloud and the interaction between wave and cloud.

Contrails and especially their evolution into cirrus-like clouds are thought to have very important effects on local and global radiation budgets, though are generally not well represented in global climate models. Lack of contrail parameterisations is due to the limited availability of in situ contrail measurements which are difficult to obtain. Here we present a methodology for successful sampling and interpretation of contrail microphysical and radiative data using both in situ and remote sensing instrumentation on board the FAAM BAe146 UK research aircraft as part of the COntrails Spreading Into Cirrus (COSIC) study. Forecast models were utilised to determine flight regions suitable for contrail formation and sampling; regions that were both free of cloud but showed a high probability of occurrence of air mass being supersaturated with respect to ice. The FAAM research aircraft, fitted with cloud microphysics probes and remote sensing instruments, formed a distinctive spiral-shaped contrail in the predicted area by flying in an orbit over the same ground position as the wind advected the contrails to the east. Parts of these contrails were sampled during the completion of four orbits, with sampled contrail regions being between 7 and 30 min old. Lidar measurements were useful for in-flight determination of the location and spatial extent of the contrails, and also to report extinction values that agreed well with those calculated from the microphysical data. A shortwave spectrometer was also able to detect the contrails, though the signal was weak due to the dispersion and evaporation of the contrails. Post-flight the UK Met Office NAME III dispersion model was successfully used as a tool for modelling the dispersion of the persistent contrail; determining its location and age, and determining when there was interference from other measured aircraft contrails or when cirrus encroached on the area later in the flight. The persistent contrails were found to consist of small (~10 μm) plate-like crystals where growth of ice crystals to larger sizes (~100 μm) was typically detected when higher water vapour levels were present. Using the cloud microphysics data, extinction co-efficient values were calculated and found to be 0.01–1 km−1. The contrails formed during the flight (referred to as B587) were found to have a visible lifetime of ~40 min, and limited water vapour supply was thought to have suppressed ice crystal growth.

Aircraft measurements of the microphysics of a tropical convective anvil (at temperatures ~−60 °C) forming above the Hector storm, over the Tiwi Islands, Northern Australia, have been conducted with a view to determining ice crystal aggregation efficiencies from in situ measurements. The observed microphysics have been compared to an explicit bin-microphysical model of the anvil region, which includes crystal growth by vapour diffusion and aggregation and the process of differential sedimentation. It has been found in flights made using straight and level runs perpendicular to the storm that the number of ice crystals initially decreased with distance from the storm as aggregation took place resulting in larger crystals, followed by their loss from the cloud layer due to sedimentation. The net result was that the mass (i.e. Ice Water Content) in the anvil Ci cloud decreased, but also that the average particle size (weighted by number) remained relatively constant along the length of the anvil outflow. Comparisons with the explicit microphysics model showed that the changes in the shapes of the ice crystal spectra as a function of distance from the storm could be explained by the model if the aggregation efficiency was set to values of Eagg~0.5 and higher. This result is supported by recent literature on aggregation efficiencies for complex ice particles and suggests that either the mechanism of particle interlocking is important to the aggregation process, or that other effects are occuring, such as enhancement of ice-aggregation by high electric fields that arise as a consequence of charge separation within the storm. It is noteworthy that this value of the ice crystal aggregation efficiency is much larger than values used in cloud resolving models at these temperatures, which typically use E~0.0016. These results are important to understanding how cold clouds evolve in time and for the treatment of the evolution of tropical Ci in numerical models.

We present a case study of Aitken and accumulation mode aerosol observed downwind of the anvil of a deep tropical thunderstorm. The measurements were made by condensation nuclei counters flown on the Egrett high-altitude aircraft from Darwin during the ACTIVE campaign, in monsoon conditions producing widespread convection over land and ocean. Maximum measured concentrations of aerosol with diameter greater than 10 nm were 25 000 cm−3 (STP). By calculating back-trajectories from the observations, and projecting onto infrared satellite images, the time since the air exited cloud was estimated. In this way a time scale of about 3 hours was derived for the Aitken aerosol concentration to reach its peak. We examine the hypothesis that the growth in aerosol concentrations can be explained by production of sulphuric acid from SO2 followed by particle nucleation and coagulation. Estimates of the sulphuric acid production rate show that the observations are only consistent with this hypothesis if the particles coagulate to sizes >10 nm much more quickly than is suggested by current theory. Alternatively, other condensible gases (possibly organic) drive the growth of aerosol particles in the TTL.

In situ high resolution aircraft measurements of cloud microphysical properties were made in coordination with ground based remote sensing observations of a line of small cumulus clouds, using Radar and Lidar, as part of the Aerosol Properties, PRocesses And InfluenceS on the Earth's climate (APPRAISE) project. A narrow but extensive line (~100 km long) of shallow convective clouds over the southern UK was studied. Cloud top temperatures were observed to be higher than −8 °C, but the clouds were seen to consist of supercooled droplets and varying concentrations of ice particles. No ice particles were observed to be falling into the cloud tops from above. Current parameterisations of ice nuclei (IN) numbers predict too few particles will be active as ice nuclei to account for ice particle concentrations at the observed, near cloud top, temperatures (−7.5 °C). The role of mineral dust particles, consistent with concentrations observed near the surface, acting as high temperature IN is considered important in this case. It was found that very high concentrations of ice particles (up to 100 L−1) could be produced by secondary ice particle production providing the observed small amount of primary ice (about 0.01 L−1) was present to initiate it. This emphasises the need to understand primary ice formation in slightly supercooled clouds. It is shown using simple calculations that the Hallett-Mossop process (HM) is the likely source of the secondary ice. Model simulations of the case study were performed with the Aerosol Cloud and Precipitation Interactions Model (ACPIM). These parcel model investigations confirmed the HM process to be a very important mechanism for producing the observed high ice concentrations. A key step in generating the high concentrations was the process of collision and coalescence of rain drops, which once formed fell rapidly through the cloud, collecting ice particles which caused them to freeze and form instant large riming particles. The broadening of the droplet size-distribution by collision-coalescence was, therefore, a vital step in this process as this was required to generate the large number of ice crystals observed in the time available. Simulations were also performed with the WRF (Weather, Research and Forecasting) model. The results showed that while HM does act to increase the mass and number concentration of ice particles in these model simulations it was not found to be critical for the formation of precipitation. However, the WRF simulations produced a cloud top that was too cold and this, combined with the assumption of continual replenishing of ice nuclei removed by ice crystal formation, resulted in too many ice crystals forming by primary nucleation compared to the observations and parcel modelling.

The global organic aerosol (OA) budget is highly uncertain and past studies suggest that models substantially underestimate observed concentrations. Few of these studies have examined the vertical distribution of OA. Furthermore, many model-measurement comparisons have been performed with different models for single field campaigns. We synthesize organic aerosol measurements from 17 aircraft campaigns from 2001–2009 and use these observations to consistently evaluate a GEOS-Chem model simulation. Remote, polluted and fire-influenced conditions are all represented in this extensive dataset. Mean observed OA concentrations range from 0.2–8.2 μg sm−3 and make up 15 to 70% of non-refractory aerosol. The standard GEOS-Chem simulation reproduces the observed vertical profile, although observations are underestimated in 13 of the 17 field campaigns (the median observed to simulated ratio ranges from 0.4 to 4.2), with the largest model bias in anthropogenic regions. However, the model is best able to capture the observed variability in these anthropogenically-influenced regions (R2=0.18−0.57), but has little skill in remote or fire-influenced regions. The model bias increases as a function of relative humidity for 11 of the campaigns, possibly indicative of missing aqueous phase SOA production. However, model simulations of aqueous phase SOA suggest a pronounced signature in the mid-troposphere (2–6 km) which is not supported in the observations examined here. Spracklen et al. (2011) suggest adding ~100 Tg yr−1 source of anthropogenically-controlled SOA to close the measurement-model gap, which we add as anthropogenic SOA. This eliminates the model underestimate near source, but leads to overestimates aloft in a few regions and in remote regions, suggesting either additional sinks of OA or higher volatility aerosol at colder temperatures. Sensitivity simulations indicate that fragmentation of organics upon either heterogeneous or gas-phase oxidation could be an important (missing) sink of OA in models, reducing the global SOA burden by 15% and 47% respectively. The best agreement with observations is obtained when the simulated anthropogenically-controlled SOA is increased to ~100 Tg yr−1 accompanied by either a gas-phase fragmentation process or a reduction in the temperature dependence of the organic aerosol partitioning (by decreasing the enthalpy of vaporization from 42 kJ mol−1 to 25 kJ mol−1). These results illustrate that models may require both additional sources and additional sinks to capture the observed concentrations of organic aerosol.

The ice nucleation efficiency of propane flame soot particles with and without a sulphuric acid coating was investigated using the aerosol and cloud chamber facility AIDA (Aerosol Interaction and Dynamics in the Atmosphere). The test soot for cloud formation simulations was produced using a propane flame Combustion Aerosol Standard generator (CAST, Jing-CAST Technologies). The organic carbon content (OC) of the test soot was altered in a reproducible fashion by changing the fuel/air mixture of the generator. The soot content of ice nuclei was subsequently investigated using a combination of a pumped counterflow virtual impactor (PCVI) to separate and evaporate the ice crystals, and a DMT single particle soot photometer (SP2) to examine the mixing state of the BC containing ice residuals. Ice nucleation was found to be most efficient for uncoated soot of low organic carbon content (~5 % organic carbon content) where deposition freezing occurred at an ice saturation ratio Sice ~ 1.22 at a temperature T = 226.6 K with 25 % of the test soot becoming active as ice nuclei. Propane flame soot of higher organic carbon content (~30 % and ~70 % organic carbon content) showed significantly lower ice nucleation efficiency (an activated fraction of the order of a few percent in the experiments) than the low organic carbon content soot, with water saturation being required for freezing to occur. Ice nucleation occurred over the range Sice = 1.22–1.70, and T = 223.2–226.6 K. Analysis of the SP2 data showed that the 5 % organic carbon content soot had an undetectable OC coating whereas the 30 % organic carbon content soot had a thicker or less volatile OC coating. The application of a sulphuric acid coating to the flame soot shifted the threshold of the onset of freezing towards that of the homogeneous freezing of sulphuric acid; for the minimum OC flame soot this inhibited nucleation since the onset of freezing occurred at colder temperatures and required a greater ice saturation ratio; for the medium and maximum OC flame soot, the addition of a sulphuric acid significantly reduced the freezing threshold.

Atmospheric composition affects the radiative balance of the Earth through the creation of greenhouse gases and the formation of aerosols. The latter interact with incoming solar radiation, both directly and indirectly through their effects on cloud formation and lifetime. The tropics have a major influence on incoming sunlight however the tropical atmosphere is poorly characterised, especially outside Amazonia. The origins of air masses influencing a measurement site in a protected rainforest in Borneo, South East Asia, were assessed and the likely sources of a range of trace gases and particles were determined. This was conducted by interpreting in situ measurements made at the site in the context of ECMWF backwards air mass trajectories. Two different but complementary methods were employed to interpret the data: comparison of periods classified by cluster analysis of trajectories, and inspection of the dependence of mean measured values on geographical history of trajectories. Sources of aerosol particles, carbon monoxide and halocarbons were assessed. The likely source influences include: terrestrial organic biogenic emissions; long range transport of anthropogenic emissions; biomass burning; sulphurous emissions from marine phytoplankton, with a possible contribution from volcanoes; marine production of inorganic mineral aerosol; and marine production of halocarbons. Aerosol sub- and super-saturated water affinity was found to be dependent on source (and therefore composition), with more hygroscopic aerosol and higher numbers of cloud condensation nuclei measured in air masses of marine origin. The prevailing sector during the majority of measurements was south-easterly, which is from the direction of the coast closest to the site, with a significant influence inland from the south-west. This analysis shows that marine and terrestrial air masses have different dominant chemical sources. Comparison with the AMAZE-08 project in the Amazon basin shows Bornean composition to arise from a different, more complex mixture of sources. In particular sulphate loadings are much greater than in Amazonia which is likely to mainly be the result of the marine influence on the site. This suggests that the significant region of the tropics made up of island networks is not well represented by extrapolation from measurements made in the Amazon. In addition, it is likely that there were no periods where the site was influenced only by the rainforest, with even the most pristine inland periods showing some evidence of non-rainforest aerosol. This is in contrast to Amazonia which experienced periods dominated by rainforest emissions.

The VAMOS Ocean-Cloud-Atmosphere-Land Regional Experiment (VOCALS-REx) was conducted from 15 October to 15 November 2008 in the South East Pacific (SEP) region to investigate interactions between land, sea and atmosphere in this unique tropical eastern ocean environment and to improve the skill of global and regional models in representing the region. This study synthesises selected aircraft, ship and surface site observations from VOCALS-REx to statistically summarise and characterise the atmospheric composition and variability of the Marine Boundary Layer (MBL) and Free Troposphere (FT) along the 20° S parallel between 70° W and 85° W. Significant zonal gradients in mean MBL sub-micron aerosol particle size and composition, carbon monoxide, sulphur dioxide and ozone were seen over the campaign, with a generally more variable and polluted coastal environment and a less variable, more pristine remote maritime regime. Gradients in aerosol and trace gas concentrations were observed to be associated with strong gradients in cloud droplet number. The FT was often more polluted in terms of trace gases than the MBL in the mean; however increased variability in the FT composition suggests an episodic nature to elevated concentrations. This is consistent with a complex vertical interleaving of airmasses with diverse sources and hence pollutant concentrations as seen by generalised back trajectory analysis, which suggests contributions from both local and long-range sources. Furthermore, back trajectory analysis demonstrates that the observed zonal gradients both in the boundary layer and the free troposphere are characteristic of marked changes in airmass history with distance offshore – coastal boundary layer airmasses having been in recent contact with the local land surface and remote maritime airmasses having resided over ocean for in excess of ten days. Boundary layer composition to the east of 75° W was observed to be dominated by coastal emissions from sources to the west of the Andes, with evidence for diurnal pumping of the Andean boundary layer above the height of the marine capping inversion. Analysis of intra-campaign variability in atmospheric composition was not found to be significantly correlated with observed low-frequency variability in the large scale flow pattern; campaign-average interquartile ranges of CO, SO2 and O3 concentrations at all longitudes were observed to dominate over much smaller differences in median concentrations calculated between periods of different flow regimes. The campaign climatology presented here aims to provide a valuable dataset to inform model simulation and future process studies, particularly in the context of aerosol-cloud interaction and further evaluation of dynamical processes in the SEP region for conditions analogous to those during VOCALS-REx. To this end, our results are discussed in terms of coastal, transitional and remote spatial regimes in the MBL and FT and a gridded dataset are provided as a resource.

Simultaneous observations of cloud microphysical properties were obtained by in-situ aircraft measurements and ground based Radar/Lidar. Widespread mid-level stratus cloud was present below a temperature inversion (~5 °C magnitude) at 3.6 km altitude. Localised convection (peak updraft 1.5 m s−1) was observed 20 km west of the Radar station. This was associated with convergence at 2.5 km altitude. The convection was unable to penetrate the inversion capping the mid-level stratus. The mid-level stratus cloud was vertically thin (~400 m), horizontally extensive (covering 100 s of km) and persisted for more than 24 h. The cloud consisted of supercooled water droplets and small concentrations of large (~1 mm) stellar/plate like ice which slowly precipitated out. This ice was nucleated at temperatures greater than −12.2 °C and less than −10.0 °C, (cloud top and cloud base temperatures, respectively). No ice seeding from above the cloud layer was observed. This ice was formed by primary nucleation, either through the entrainment of efficient ice nuclei from above/below cloud, or by the slow stochastic activation of immersion freezing ice nuclei contained within the supercooled drops. Above cloud top significant concentrations of sub-micron aerosol were observed and consisted of a mixture of sulphate and carbonaceous material, a potential source of ice nuclei. Particle number concentrations (in the size range 0.1

The VAMOS1 Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx) was an international field program designed to make observations of poorly understood but critical components of the coupled climate system of the southeast Pacific. This region is characterized by strong coastal upwelling, the coolest SSTs in the tropical belt, and is home to the largest subtropical stratocumulus deck on Earth. The field intensive phase of VOCALS-REx took place during October and November 2008 and constitutes a critical part of a broader CLIVAR program (VOCALS) designed to develop and promote scientific activities leading to improved understanding, model simulations, and predictions of the southeastern Pacific (SEP) coupled ocean-atmosphere-land system, on diurnal to interannual timescales. The other major components of VOCALS are a modeling program with a model hierarchy ranging from the local to global scales, and a suite of extended observations from regular research cruises, instrumented moorings, and satellites. The two central themes of VOCALS-REx focus upon (a) links between aerosols, clouds and precipitation and their impacts on marine stratocumulus radiative properties, and (b) physical and chemical couplings between the upper ocean and the lower atmosphere, including the role that mesoscale ocean eddies play. A set of hypotheses designed to be tested with the combined field, monitoring and modeling work in VOCALS is presented here. A further goal of VOCALS-REx is to provide datasets for the evaluation and improvement of large-scale numerical models. VOCALS-REx involved five research aircraft, two ships and two surface sites in northern Chile. We describe the instrument payloads and key mission strategies for these platforms and give a summary of the missions conducted. 1 Variability of the American Monsoon Systems, an international CLIVAR program.

A case study of atmospheric aerosol measurements exploring the impact of the vertical distribution of aerosol chemical composition upon the radiative budget in North-Western Europe is presented. Sub-micron aerosol chemical composition was measured by an Aerodyne Aerosol Mass Spectrometer (AMS) on both an airborne platform and a ground-based site at Cabauw in the Netherlands. The examined period in May 2008 was characterised by enhanced pollution loadings in North-Western Europe and was dominated by ammonium nitrate and Organic Matter (OM). Both ammonium nitrate and OM were observed to increase with altitude in the atmospheric boundary layer. This is primarily attributed to partitioning of semi-volatile gas phase species to the particle phase at reduced temperature and enhanced relative humidity. Increased ammonium nitrate concentrations in particular were found to strongly increase the ambient scattering potential of the aerosol burden, which was a consequence of the large amount of associated water as well as the enhanced mass. During particularly polluted conditions, increases in aerosol optical depth of 50–100% were estimated to occur due to the observed increase in secondary aerosol mass and associated water uptake. Furthermore, the single scattering albedo was also shown to increase with height in the boundary layer. These enhancements combined to increase the negative direct aerosol radiative forcing by close to a factor of two at the median percentile level. Such increases have major ramifications for regional climate predictions as semi-volatile components are often not included in aerosol models. The results presented here provide an ideal opportunity to test regional and global representations of both the aerosol vertical distribution and subsequent impacts in North-Western Europe. North-Western Europe can be viewed as an analogue for the possible future air quality over other polluted regions of the Northern Hemisphere, where substantial reductions in sulphur dioxide emissions have yet to occur. Anticipated reductions in sulphur dioxide in polluted regions will result in an increase in the availability of ammonia to form ammonium nitrate as opposed to ammonium sulphate. This will be most important where intensive agricultural practises occur. Our observations over North-Western Europe, a region where sulphur dioxide emissions have already been reduced, indicate that failure to include the semi-volatile behaviour of ammonium nitrate will result in significant errors in predicted aerosol direct radiative forcing. Such errors will be particularly significant on regional scales.

The spatial distribution of aerosol chemical composition and the evolution of the Organic Aerosol (OA) fraction is investigated based upon airborne measurements of aerosol chemical composition in the planetary boundary layer across Europe. Sub-micron aerosol chemical composition was measured using a compact Time-of-Flight Aerosol Mass Spectrometer (cToF-AMS). A range of sampling conditions were evaluated, including relatively clean background conditions, polluted conditions in North-Western Europe and the near-field to far-field outflow from such conditions. Ammonium nitrate and OA were found to be the dominant chemical components of the sub-micron aerosol burden, with mass fractions ranging from 20–50% each. Ammonium nitrate was found to dominate in North-Western Europe during episodes of high pollution, reflecting the enhanced NOx and ammonia sources in this region. OA was ubiquitous across Europe and concentrations generally exceeded sulphate by 30–160%. A factor analysis of the OA burden was performed in order to probe the evolution across this large range of spatial and temporal scales. Two separate Oxygenated Organic Aerosol (OOA) components were identified; one representing an aged-OOA, termed Low Volatility-OOA and another representing fresher-OOA, termed Semi Volatile-OOA on the basis of their mass spectral similarity to previous studies. The factors derived from different flights were not chemically the same but rather reflect the range of OA composition sampled during a particular flight. Significant chemical processing of the OA was observed downwind of major sources in North-Western Europe, with the LV-OOA component becoming increasingly dominant as the distance from source and photochemical processing increased. The measurements suggest that the aging of OA can be viewed as a continuum, with a progression from a less oxidised, semi-volatile component to a highly oxidised, less-volatile component. Substantial amounts of pollution were observed far downwind of continental Europe, with OA and ammonium nitrate being the major constituents of the sub-micron aerosol burden. Such anthropogenically perturbed air masses can significantly perturb regional climate far downwind of major source regions.

A synthesis of UK based airborne in-situ measurements of aerosol properties representing air masses from North-West Europe and the North-East Atlantic is presented. The major focus of the study is the vertical distribution of sub-micron aerosol chemical composition. Vertical profiles are derived from a Quadrupole Aerosol Mass Spectrometer (Q-AMS). Background sub-micron aerosol vertical profiles are identified and are primarily composed of organic matter and sulphate aerosol. Such background conditions occurred predominantly during periods associated with long-range air mass transport across the Atlantic. These instances may serve as useful model input of aerosol to Western Europe. Increased mass concentration episodes are coincident with European outflow and periods of stagnant/recirculating air masses. Such periods are characterised by significantly enhanced concentrations of nitrate aerosol relative to those of organic matter and sulphate. Periods of enhanced ground level PM2.5 loadings are coincident with instances of high nitrate mass fractions measured on-board the aircraft, indicating that nitrate is a significant contributor to regional pollution episodes. The vertical structure of the sulphate and organic aerosol profiles were shown to be primarily driven by large-scale dynamical processes. The vertical distribution of nitrate is likely determined by both dynamic and thermodynamic processes, with chemical partitioning of gas phase precursors to the particle phase occurring at lower temperatures at the top of the boundary layer. Such effects have profound implications for the aerosol's lifetime and subsequent impacts, highlighting the requirement for accurate representation of the aerosol vertical distribution.

The chemical composition of submicron (fine mode) and supermicron (coarse mode) aerosol particles has been investigated at the Jungfraujoch high alpine research station (3580 m a.s.l., Switzerland) as part of the GAW aerosol monitoring program since 1999. A clear seasonality was observed for all major components throughout the period with low concentrations in winter (predominantly free tropospheric aerosol) and higher concentrations in summer (enhanced vertical transport of boundary layer pollutants). In addition, mass closure was attempted during intensive campaigns in March 2004, February–March 2005 and August 2005. Ionic, carbonaceous and non-refractory components of the aerosol were quantified as well as the PM1 and coarse mode total aerosol mass concentrations. A relatively low conversion factor of 1.8 for organic carbon (OC) to particulate organic matter (OM) was found in winter (February–March 2005). Organics, sulfate, ammonium, and nitrate were the major components of the fine aerosol fraction that were identified, while calcium and nitrate were the only two measured components contributing to the coarse mode. The aerosol mass concentrations for fine and coarse mode aerosol measured during the intensive campaigns were not typical of the long-term seasonality due largely to dynamical differences. Average fine and coarse mode concentrations during the intensive field campaigns were 1.7 μg m−3 and 2.4 μg m−3 in winter and 2.5 μg m−3 and 2.0 μg m−3 in summer, respectively. The mass balance of aerosols showed higher contributions of calcium and nitrate in the coarse mode during Saharan dust events (SDE) than without SDE.

Measurements of aerosol properties were made in aged polluted and clean background air masses encountered at the North Norfolk (UK) coastline as part of the TORCH2 field campaign in May 2004. Hygroscopic growth factors (GF) at 90% relative humidity (RH) for D0=27–217 nm particles and size-resolved chemical composition were simultaneously measured using a Hygroscopicity Tandem Differential Mobility Analyser (HTDMA) and an Aerodyne aerosol mass spectrometer (Q-AMS), respectively. Both hygroscopic properties and chemical composition showed pronounced variability in time and with particles size. With this data set we could demonstrate that the Zdanovskii-Stokes-Robinson (ZSR) mixing rule combined with chemical composition data from the AMS makes accurate quantitative predictions of the mean GF of mixed atmospheric aerosol particles possible. In doing so it is crucial that chemical composition data are acquired with high resolution in both particle size and time, at least matching the actual variability of particle properties. The closure results indicate an ensemble GF of the organic fraction of ~1.20±0.10 at 90% water activity. Thus the organics contribute somewhat to hygroscopic growth, particularly at small sizes, however the inorganic salts still dominate. Furthermore it has been found that most likely substantial evaporation losses of NH4NO3 occurred within the HTDMA instrument, exacerbated by a long residence time of ~1 min. Such an artefact is in agreement with our laboratory experiments and literature data for pure NH4NO3, both showing similar evaporation losses within HTDMAs with residence times of ~1 min. Short residence times and low temperatures are hence recommended for HTDMAs in order to minimise such evaporation artefacts.

The study of the growth of nucleation-mode particles is important, as this prevents their loss through diffusion and allows them to reach sizes where they may become effective cloud condensation nuclei. Hyytiälä, a forested site in southern Finland, frequently experiences particle nucleation events during the spring and autumn, where particles first appear during the morning and continue to grow for several hours afterwards. As part of the QUEST 2 intensive field campaign during March and April 2003, an Aerodyne Aerosol Mass Spectrometer (AMS) was deployed alongside other aerosol instrumentation to study the particulate composition and dynamics of growth events and characterise the background aerosol. Despite the small mass concentrations, the AMS was able to distinguish the grown particles in the

Measurements are presented from a sampling location 50 km downwind of Greater London, UK, to investigate the timescales required for the atmospheric transformations of aerosol in urban emissions plumes in the context of photochemical age based on the benzene to toluene ratio. It is shown that particles at or around 100 nm in diameter exhibit the greatest systematic variability in chemical properties, and thus hygroscopic properties, on a timescale of 1–2 days. The smaller Aitken mode and larger accumulation mode particles exhibit less variability on these timescales, which we propose is as a result of their different residence times in the atmosphere. The larger accumulation particles have been in the atmosphere longer than the 100 nm particles and their chemistry and hygroscopic properties have been integrated over several days and potentially over several source regions. In contrast, the smaller Aitken mode particles show little systematic variability with photochemical age because their atmospheric lifetimes are short, thus chemical changes and hence changes in water affinity have not had time to occur. Increases in the particle diameter of up to 40% are observed at 90% relative humidity in the accumulation mode from the uptake of water as the particles become increasingly soluble in nature.

A suite of aerosol physical and chemical measurements were made at the Mace Head Atmospheric Research Station, Co. Galway, Ireland, a coastal site on the eastern seaboard of the north Atlantic Ocean during NAMBLEX. The data have been used in this paper to show that over a wide range of aerosol sizes there is no impact of the inter-tidal zone or the surf zone on measurements made at 7 m above ground level or higher. During the measurement period a range of air mass types were observed. During anticyclonic periods and conditions of continental outflow Aitken and accumulation mode were enhanced by a factor of 5 compared to the marine sector, whilst coarse mode particles were enhanced during westerly conditions. Baseline marine conditions were rarely met at Mace Head during NAMBLEX and high wind speeds were observed for brief periods only. The NAMBLEX experiment focussed on a detailed assessment of photochemistry in the marine environment, investigating the linkage between the HOx and the halogen radical cycles. Heterogeneous losses are important in both these cycles. In this paper loss rates of gaseous species to aerosol surfaces were calculated for a range of uptake coefficients. Even when the accommodation coefficient is unity, lifetimes due to heterogeneous loss of less than 10 s were never observed and rarely were they less than 500 s. Diffusional limitation to mass transfer is important in most conditions as the coarse mode is always significant. We calculate a minimum overestimate of 50% in the loss rate if this is neglected and so it should always be considered when calculating loss rates of gaseous species to particle surfaces. HO2 and HOI have accommodation coefficients of around 0.03 and hence we calculate lifetimes due to loss to particle surfaces of 2000 s or greater under the conditions experienced during NAMBLEX. Aerosol composition data collected during this experiment provide representative information on the input aerosol characteristics to western Europe. During NAMBLEX the submicron aerosol was predominately acidified sulphate and organic material, which was most likely internally mixed. The remaining accumulation mode aerosol was sea salt. The organic and sulphate fractions were approximately equally important, though the mass ratio varies considerably between air masses. Mass spectral fingerprints of the organic fraction in polluted conditions are similar to those observed at other locations that are characterised by aged continental aerosol. In marine conditions, the background input of both sulphate and organic aerosol into Europe was observed to be between 0.5 and 1 µg m−3. Key differences in the mass spectra were observed during the few clean periods but were insufficient to ascertain whether these changes reflect differences in the source fingerprint of the organic aerosol. The coarse mode was composed of sea salt and showed significant displacement of chloride by nitrate and to a lesser extent sulphate in polluted conditions.