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A small fraction of aerosol particles known as Ice-Nucleating Particles (INPs) have the potential to trigger ice formation in cloud droplets at higher temperatures than homogeneous freezing. INPs can strongly reduce the water content and albedo of shallow mixed-phase clouds and also influence the development of convective clouds. Therefore, it is important to understand which aerosol types serve as INPs and how effectively they nucleate ice. Using a combination of INP measurements and Scanning Electron Microscopy with Energy Dispersive Spectroscopy (SEM-EDS), we quantify both the INP concentrations over a range of activation temperatures and the size-resolved composition. We show that the INP population of aerosol samples collected from an aircraft over the UK during July of 2017 is consistent with ice-nucleation on mineral dust below about −20 °C, but some other INP type must account for ice-nucleation at higher temperatures. Biological aerosol particles above ∼2 μm were detected based on visual detection of their morphological features in all the analysed samples at concentrations of at least 10 to 100 L−1in the boundary layer. We suggest that given the presence of biological material, it could substantially contribute to the enhanced ice-nucleation ability of the samples at above −20 °C. Organic material attached to mineral dust could be responsible for at least part of this enhancement. These results are consistent with a growing body of data which suggests mineral dust alone cannot explain the INP population in the mid-latitude terrestrial atmosphere and that biological ice nucleating particles are most likely important for cloud glaciation.

Desert dust is one of the most important atmospheric ice‐nucleating aerosol species around the globe. However, there have been very few measurements of ice‐nucleating particle (INP) concentrations in dusty air close to desert sources. In this study we report the concentration of INPs in dust laden air over the tropical Atlantic within a few days' transport of one of the world's most important atmospheric sources of desert dust, the Sahara. These measurements were performed as part of the Ice in Clouds Experiment‐Dust campaign based in Cape Verde, during August 2015. INP concentrations active in the immersion mode, determined using a droplet‐on‐filter technique, ranged from around 102m−3at −12°C to around 105m−3at −23°C. There is about 2 orders of magnitude variability in INP concentration for a particular temperature, which is determined largely by the variability in atmospheric dust loading. These measurements were made at altitudes from 30 to 3,500 m in air containing a range of dust loadings. The ice active site density (ns) for desert dust dominated aerosol derived from our measurements agrees with several laboratory‐based parameterizations for ice nucleation by desert dust within 1 to 2 orders of magnitude. The small variability in nsvalues determined from our measurements (within about 1 order of magnitude) is striking given that the back trajectory analysis suggests that the sources of dust were geographically diverse. This is consistent with previous work, which indicates that desert dust's ice‐nucleating activity is only weakly dependent on source. For the first time, we measured ice‐nucleating particle concentrations in the dusty eastern tropical Atlantic from an aircraftIce‐nucleating particle concentrations ranged from 102m−3at −12°C to around 105m−3at −23°CDerived ice active site densities were within 1 to 2 orders of magnitude of laboratory‐based parameterizations depending on temperature

Near real-time measurements of light non-methane hydrocarbons NMHCs and peroxyacetyl nitrate PAN have been performed in the free troposphere using two fast gas chromatography GC instruments designed for use on aircraft. A GC-helium ionisation detector HID system measured 15 C2–C5hydrocarbons with 5 min time resolution and a dual channel GC-Electron Capture Detector ECD measured PAN with 90 s resolution. Both instruments had low parts per trillion by volume pptV detection limits and ran continuously at the remote Jungfraujoch JFJ research station in the Swiss Alps 46.55°N, 7.98°E, 3580 m above mean sea level AMSL, during FebruaryMarch 2003. Carbon monoxide, ozone, nitrogen oxide and nitrogen dioxide and all odd nitrogen species NOy were also measured continuously. Hydrocarbons and CO were strongly correlated in all air-masses whilst PAN exhibited both positive and negative correlations with respect to O3, dependent on age and origin of the air-mass sampled. PAN was found to contribute ∼20 to the NOysampled on average. The experiment, as well as providing interesting datasets from this remote location, also demonstrated that when optimised, GC techniques have the potential to measure at a time resolution significantly greater than is traditionally considered, with high sensitivity and low uncertainty.

Clouds containing supercooled water are important for both climate and weather, but our knowledge of which aerosol particle types nucleate ice in these clouds is far from complete. Combustion aerosols have strong anthropogenic sources, and if these aerosol types were to nucleate ice in clouds, they might exert a climate forcing. Here, we quantified the atmospheric ice‐nucleating particle (INP) concentrations during the United Kingdom's annual Bonfire Night celebrations, which are characterized by large amounts of combustion aerosol from bonfires and fireworks. We used three immersion mode techniques covering more than 6 orders of magnitude in INP concentration over the temperature range from −10°C to homogeneous freezing. We found no observable systematic change in the INP concentration on three separate nights, despite more than a factor of 10 increase in aerosol number concentrations, up to a factor of 10 increase in PM10concentration, and more than a factor of 100 increase in black carbon (BC) mass concentration relative to pre‐event levels. This implies that BC and other combustion aerosol such as ash did not compete with the INPs present in the background air. Furthermore, the upper limit of the ice‐active site surface density, ns(T), of BC generated in these events was shown to be consistent with several other recent laboratory studies, showing a very low ice‐nucleating activity of BC. We conclude that combustion aerosol particles similar to those emitted on Bonfire Night are at most of secondary importance for the INP population relevant for mixed‐phase clouds in typical midlatitude terrestrial locations. Liquid water droplets found in clouds can cool to well below 0°C while remaining in the liquid phase (this is known as supercooling). These supercooled droplets can remain liquid down to below around −33°C without freezing, unless there is a certain type of aerosol particle present: an ice‐nucleating particle (INP). Hence, INPs have the potential to drastically change the properties and lifetime of clouds, but the sources of INP in the atmosphere are poorly defined. In this study we measured the INP concentration before, during, and after a major combustion aerosol event in the United Kingdom, Bonfire Night. This celebration is characterized by bonfires (primarily made of waste wood, but also containing garden and household waste) and fireworks. We found that aerosol particles emitted during the celebration are not as effective at nucleating ice as aerosol particle already present in the atmosphere. We conclude that aerosol particles emitted from combustion processes such as those observed on Bonfire Night are not an important source of INPs. Ice‐nucleating particle concentrations were unaffected by high aerosol loading during Bonfire Night celebrationsAerosol concentrations rose by up to a factor of 10 and black carbon by up to a factor of 100 during these bonfire and firework eventsOur limiting active site density for Bonfire Night black carbon is consistent with other recent work with low ice‐nucleating activities

Bayesian inference has been used to determine rigorous estimates of hydroxyl radical concentrations () and air mass dilution rates (K) averaged following air masses between linked observations of nonmethane hydrocarbons (NMHCs) spanning the North Atlantic during the Intercontinental Transport and Chemical Transformation (ITCT)‐Lagrangian‐2K4 experiment. The Bayesian technique obtains a refined (posterior) distribution of a parameter given data related to the parameter through a model and prior beliefs about the parameter distribution. Here, the model describes hydrocarbon loss through OH reaction and mixing with a background concentration at rate K. The Lagrangian experiment provides direct observations of hydrocarbons at two time points, removing assumptions regarding composition or sources upstream of a single observation. The estimates are sharpened by using many hydrocarbons with different reactivities and accounting for their variability and measurement uncertainty. A novel technique is used to construct prior background distributions of many species, described by variation of a single parameter α. This exploits the high correlation of species, related by the first principal component of many NMHC samples. The Bayesian method obtains posterior estimates of , Kand αfollowing each air mass. Median values are typically between 0.5 and 2.0 × 106molecules cm−3, but are elevated to between 2.5 and 3.5 × 106molecules cm−3, in low‐level pollution. A comparison of estimates from absolute NMHC concentrations and NMHC ratios assuming zero background (the “photochemical clock” method) shows similar distributions but reveals systematic high bias in the estimates from ratios. Estimates of Kare ∼0.1 day−1but show more sensitivity to the prior distribution assumed.

The atmospheric composition of the central North Atlantic region has been sampled using the FAAM BAe146 instrumented aircraft during the Intercontinental Transport of Ozone and Precursors (ITOP) campaign, part of the wider International Consortium for Atmospheric Research on Transport and Transformation (ICARTT). This paper presents an overview of the ITOP campaign. Between late July and early August 2004, twelve flights comprising 72 hours of measurement were made in a region from approximately 20 to 40°W and 33 to 47°N centered on Faial Island, Azores, ranging in altitude from 50 to 9000 m. The vertical profiles of O3and CO are consistent with previous observations made in this region during 1997 and our knowledge of the seasonal cycles within the region. A cluster analysis technique is used to partition the data set into air mass types with distinct chemical signatures. Six clusters provide a suitable balance between cluster generality and specificity. The clusters are labeled as biomass burning, low level outflow, upper level outflow, moist lower troposphere, marine and upper troposphere. During this summer, boreal forest fire emissions from Alaska and northern Canada were found to provide a major perturbation of tropospheric composition in CO, PAN, organic compounds and aerosol. Anthropogenic influenced air from the continental boundary layer of the USA was clearly observed running above the marine boundary layer right across the mid‐Atlantic, retaining high pollution levels in VOCs and sulfate aerosol. Upper level outflow events were found to have far lower sulfate aerosol, resulting from washout on ascent, but much higher PAN associated with the colder temperatures. Lagrangian links with flights of other aircraft over the USA and Europe show that such signatures are maintained many days downwind of emission regions. Some other features of the data set are highlighted, including the strong perturbations to many VOCs and OVOCs in this remote region.