The amount of ice present in clouds can affect cloud lifetime, precipitation and radiative properties 1,2 . The formation of ice in clouds is facilitated by the presence of airborne ice nucleating particles 1,2 . Sea spray is one of the major global sources of atmospheric particles, but it is unclear to what extent these particles are capable of nucleating ice 3-11 . Sea spray aerosol contains large amounts of organic material that is ejected into the atmosphere during bubble bursting at the organically enriched sea-air interface or sea surface microlayer [12][13][14][15][16][17][18][19] . Here we show that organic material in the sea surface microlayer nucleates ice under conditions relevant for mixed-phase cloud and high-altitude ice cloud formation. The ice nucleating material is likely biogenic and less than ~0.2 μm in size. We find that exudates separated from cells of the marine diatom T. Pseudonana nucleate ice and propose that organic material associated with phytoplankton cell exudates is a likely candidate for the observed ice nucleating ability of the microlayer samples. Global model simulations of marine organic aerosol in combination with our measurements suggest that marine organic material may be an important source of ice nucleating particles in remote marine environments such as the Southern Ocean, North Pacific and North Atlantic.Atmospheric ice nucleating particles (INPs) allow ice to nucleate heterogeneously at higher temperatures or lower relative humidity than is typical for homogeneous ice nucleation. Heterogeneous ice nucleation proceeds via different pathways depending on temperature and humidity. In low altitude mixed-phase clouds, INPs are commonly immersed in supercooled liquid droplets and freezing can occur on them at temperatures between -36 and 0°C 2 . At higher altitudes and lower temperatures (<-36°C) where cirrus clouds form, nucleation occurs below water saturation, proceeding by homogeneous, deposition or immersion-in-solution nucleation 1 . Understanding the sources of atmospheric INPs is important because they affect cloud lifetime, cloud albedo and precipitation 1,2 . Recent modelling work has shown that the ocean is potentially an important source of biogenic atmospheric INPs particularly in remote, high latitude regions 9,10 . However, it has never been directly shown that there is a source of atmospheric INPs associated with organic material found in marine waters or sea-spray aerosol.Organic material makes up a substantial fraction of sub-micron sea-spray aerosol and it is estimated that 10±5 Tg yr -1 of primary organic sub-micron aerosol is emitted from marine sources globally 12 . Rising bubbles scavenge surface active organic material from the water column at their interfaces and this process facilitates the formation of the organic enriched sea-air interface known as the sea surface microlayer (SML). This organic material is ejected into the atmosphere during bubble bursting resulting in sea spray aerosol containing similar organic material to that of the microlaye...

Abstract. We describe Global Atmosphere 7.0 and Global Land 7.0 (GA7.0/GL7.0), the latest science configurations of the Met Office Unified Model (UM) and the Joint UK Land Environment Simulator (JULES) land surface model developed for use across weather and climate timescales. GA7.0 and GL7.0 include incremental developments and targeted improvements that, between them, address four critical errors identified in previous configurations: excessive precipitation biases over India, warm and moist biases in the tropical tropopause layer (TTL), a source of energy non-conservation in the advection scheme and excessive surface radiation biases over the Southern Ocean. They also include two new parametrisations, namely the UK Chemistry and Aerosol (UKCA) GLOMAP-mode (Global Model of Aerosol Processes) aerosol scheme and the JULES multi-layer snow scheme, which improve the fidelity of the simulation and were required for inclusion in the Global Atmosphere/Global Land configurations ahead of the 6th Coupled Model Intercomparison Project (CMIP6). In addition, we describe the GA7.1 branch configuration, which reduces an overly negative anthropogenic aerosol effective radiative forcing (ERF) in GA7.0 whilst maintaining the quality of simulations of the present-day climate. GA7.1/GL7.0 will form the physical atmosphere/land component in the HadGEM3–GC3.1 and UKESM1 climate model submissions to the CMIP6.

Abstract. Agricultural dust emissions have been estimated to contribute around 20 % to the global dust burden. In contrast to dusts from arid source regions, the ice-nucleating abilities of which have been relatively well studied, soil dusts from fertile sources often contain a substantial fraction of organic matter. Using an experimental methodology which is sensitive to a wide range of ice nucleation efficiencies, we have characterised the immersion mode ice-nucleating activities of dusts (d < 11 µm) extracted from fertile soils collected at four locations around England. By controlling droplet sizes, which ranged in volume from 10 −12 to 10 −6 L (concentration = 0.02 to 0.1 wt % dust), we have been able to determine the ice nucleation behaviour of soil dust particles at temperatures ranging from 267 K (−6 • C) down to the homogeneous limit of freezing at about 237 K (−36 • C). At temperatures above 258 K (−15 • C) we find that the ice-nucleating activity of soil dusts is diminished by heat treatment or digestion with hydrogen peroxide, suggesting that a major fraction of the ice nuclei stems from biogenic components in the soil. However, below 258 K, we find that the ice active site densities tend towards those expected from the mineral components in the soils, suggesting that the inorganic fraction of soil dusts, in particular the K-feldspar fraction, becomes increasingly important in the initiation of the ice phase at lower temperatures. We conclude that dusts from agricultural activities could contribute significantly to atmospheric IN concentrations, if such dusts exhibit similar activities to those observed in the current laboratory study.

Abstract. The seasonal cycle in Arctic aerosol is typified by high concentrations of large aged anthropogenic particles transported from lower latitudes in the late Arctic winter and early spring followed by a sharp transition to low concentrations of locally sourced smaller particles in the summer. However, multi-model assessments show that many models fail to simulate a realistic cycle. Here, we use a global aerosol microphysics model (GLOMAP) and surface-level aerosol observations to understand how wet scavenging processes control the seasonal variation in Arctic black carbon (BC) and sulphate aerosol. We show that the transition from high wintertime concentrations to low concentrations in the summer is controlled by the transition from ice-phase cloud scavenging to the much more efficient warm cloud scavenging in the late spring troposphere. This seasonal cycle is amplified further by the appearance of warm drizzling cloud in the late spring and summer boundary layer. Implementing these processes in GLOMAP greatly improves the agreement between the model and observations at the three Arctic groundstations Alert, Barrow and Zeppelin Mountain on Svalbard. The SO 4 model-observation correlation coefficient (R) increases from: −0.33 to 0.71 at Alert (82.5 • N), from −0.16 to 0.70 at Point Barrow (71.0 • N) and from −0.42 to 0.40 at Zeppelin Mountain (78 • N). The BC model-observation correlation coefficient increases from −0.68 to 0.72 at Alert and from −0.42 to 0.44 at Barrow. Observations at three marginal Arctic sites (Janiskoski, Oulanka and Karasjok) indicate a far weaker aerosol seasonal cycle, which we show is consistent with the much smaller seasonal change in the frequency of ice clouds compared to higher latitude sites. Our results suggest that the seasonal cycle in Arctic aerosol is driven by temperature-dependent scavenging processes that may be susceptible to modification in a future climate.