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A global model perturbed parameter ensemble of 60 simulations was used to explore how combinations of six parameters related to secondary organic aerosol (SOA) formation affect particle number concentrations and organic aerosol mass. The parameters represent the formation of organic compounds with different volatilities from biogenic and anthropogenic sources. The most plausible parameter combinations were determined by comparing the simulations against observations of the number concentration of particles larger than 3 nm diameter (N3), the number concentration of particles larger than 50 nm diameter (N50), and the organic aerosol (OA) mass concentration. The simulations expose a high degree of model equifinality in which the skill of widely different parameter combinations cannot be distinguished against observations. We therefore conclude that, based on the observations we have used, a six-parameter SOA scheme is under-determined. Nevertheless, the model skill in simulating N3 and N50 is clearly determined by the low-volatility and extremely low-volatility compounds that affect new particle formation and growth, and the skill in simulating OA mass is determined by the low-volatility and semi-volatile compounds. The biogenic low-volatility class of compounds that grow nucleated clusters and condense on all particles is found to have the strongest effect on the model skill in simulating N3, N50, and OA. The simulations also expose potential structural deficiencies in the model: we find that parameter combinations that are best for N3 and N50 are worst for OA mass, and the ensemble exaggerates the observed seasonal cycle of particle concentrations – a deficiency that we conclude requires an additional anthropogenic source of either primary or secondary particles.

Meteoric smoke particles (MSPs) provide a steady source of condensation nuclei to the Arctic lower stratosphere, with heterogeneous nucleation to sulphuric acid aerosol particles. Internally mixed meteoric-sulphuric particles likely also play a significant role in the formation of polar stratospheric clouds and thereby influence stratospheric ozone depletion chemistry, particularly in the quiescent stratosphere.In several Arctic winter field campaigns (EUPLEX 2002/3, RECONCILE 2009/10, ESSenCe 2010/11), in-situ stratospheric aerosol particle concentrations measurements were made from the high-altitude Geophysica aircraft, the COPAS instrument measuring total and refractory (non-volatile) particle concentrations at 20 km altitude (see Curtius et al., 2003; Weigel et al., 2014). These measurements are consistent with there being a substantial seasonal source of meteoric-sulphuric particles to the lower Arctic stratosphere, from each year’s influx of MSPs within the winter-time Arctic polar vortex. In this study we investigate the effect of MSPs on the quiescent Junge layer particle concentration as the polar vortex builds up and after it dissipates. We use the nudged configuration of the UM-UKCA stratosphere-troposphere composition-climate model to reproduce the vertical profile of stratospheric particles measured in-situ during the COPAS 2003 campaign. Our model simulates two types of stratospheric aerosol particles - pure sulphuric acid particles and sulphuric acid particles with a MSP-core. We show that the model is able to reproduce the vertical profile of aerosol particles observed during the COPAS measurements in winter 2003.Our findings illustrate the influx of MSP and SO2 from higher altitudes through the polar vortex, the winter-time build-up of SO2 triggering homogeneous nucleation of pure sulphuric particles, also with the seasonal source of MSP-core sulphuric particles nucleated heterogeneously. We assess the effects of MSPs on the quiescent period particle concentration in the Arctic during winter through to spring.

The widespread presence of meteoric smoke particles (MSPs) within a distinct class of stratospheric aerosol particles has become clear from in-situ measurements in the Arctic, Antarctic and at mid-latitudes. We apply an adapted version of the interactive stratosphere aerosol configuration of the composition-climate model UM-UKCA, to predict the global distribution of meteoric-sulphuric particles nucleated heterogeneously on MSP cores. We compare the UM-UKCA results to new MSP-sulphuric simulations with the European stratosphere-troposphere chemistry-aerosol modelling system IFS-CB05-BASCOE-GLOMAP.The simulations show a strong seasonal cycle in meteoric-sulphuric particle abundance results from the winter-time source of MSPs transported down into the stratosphere in the polar vortex. Coagulation during downward transport sees high latitude MSP concentrations reduce from ~500 per cm3 at 40km to ~20 per cm3 at 25km, the uppermost extent of the stratospheric aerosol particle layer (the Junge layer). Once within the Junge layer's supersaturated environment, meteoric-sulphuric particles form readily on the MSP cores, growing to 50-70nm dry-diameter (Dp) at 20-25km. Further inter-particle coagulation between these non-volatile particles reduces their number to 1-5 per cc at 15-20km, particle sizes there larger, at Dp ~100nm.The model predicts meteoric-sulphurics in high-latitude winter comprise >90% of Dp>10nm particles above 25km, reducing to ~40% at 20km, and ~10% at 15km. These non-volatile particle fractions are slightly less than measured from high-altitude aircraft in the lowermost Arctic stratosphere (Curtius et al., 2005; Weigel et al., 2014), and consistent with mid-latitude aircraft measurements of lower stratospheric aerosol composition (Murphy et al., 1998), total particle concentrations also matching in-situ balloon measurements from Wyoming (Campbell and Deshler, 2014). The MSP-sulphuric interactions also improve agreement with SAGE-II observed stratospheric aerosol extinction in the quiescent 1998-2002 period. Simulations with a factor-8-elevated MSP input form more Dp>10nm meteoric-sulphurics, but the increased number sees fewer growing to Dp ~100nm, the increased MSPs reducing the stratospheric aerosol layer’s light extinction.

NOx is important for particle growth as it can participate in HOM formation and alter the HOM volatility distribution., Atmospheric new-particle formation (NPF) affects climate by contributing to a large fraction of the cloud condensation nuclei (CCN). Highly oxygenated organic molecules (HOMs) drive the early particle growth and therefore substantially influence the survival of newly formed particles to CCN. Nitrogen oxide (NOx) is known to suppress the NPF driven by HOMs, but the underlying mechanism remains largely unclear. Here, we examine the response of particle growth to the changes of HOM formation caused by NOx. We show that NOx suppresses particle growth in general, but the suppression is rather nonuniform and size dependent, which can be quantitatively explained by the shifted HOM volatility after adding NOx. By illustrating how NOx affects the early growth of new particles, a critical step of CCN formation, our results help provide a refined assessment of the potential climatic effects caused by the diverse changes of NOx level in forest regions around the globe.

Atmospheric aerosol formation from biogenic vapors is strongly affected by air pollutants, like NOx, SO2, and NH3., A major fraction of atmospheric aerosol particles, which affect both air quality and climate, form from gaseous precursors in the atmosphere. Highly oxygenated organic molecules (HOMs), formed by oxidation of biogenic volatile organic compounds, are known to participate in particle formation and growth. However, it is not well understood how they interact with atmospheric pollutants, such as nitrogen oxides (NOx) and sulfur oxides (SOx) from fossil fuel combustion, as well as ammonia (NH3) from livestock and fertilizers. Here, we show how NOx suppresses particle formation, while HOMs, sulfuric acid, and NH3 have a synergistic enhancing effect on particle formation. We postulate a novel mechanism, involving HOMs, sulfuric acid, and ammonia, which is able to closely reproduce observations of particle formation and growth in daytime boreal forest and similar environments. The findings elucidate the complex interactions between biogenic and anthropogenic vapors in the atmospheric aerosol system.

Understanding the cloud vertical structure and its variation in space and time is important to reduce the uncertainty in climate forcing. Here, we present the cloud climatology over the oceanic regions (Arabian Sea, Bay of Bengal, and South Indian Ocean) adjacent to the Indian subcontinent using data from the Multiangle Imaging Spectroradiometer (MISR), Moderate Resolution Imaging Spectroradiometer (MODIS), GCM-Oriented CALIPSO Cloud Product (GOCCP), and International Satellite Cloud Climatology Project (ISCCP). Fractional cloud cover (fc) shows stronger seasonal variations over the Arabian Sea (mean annual fc lies in the range 0.5–0.61) and Bay of Bengal (mean annual fc lies in the range 0.69–0.75) relative to the South Indian Ocean (mean annual fc lies in the range 0.64–0.71). Inter-comparison of statistics from passive (MISR, MODIS and ISCCP) and active (GOCCP) sensors reveals the challenges in interpreting satellite data for climate implications. While MISR detects more low clouds because of its stere...

Optical probes are frequently used for the detection of microphysical cloud particle properties such as liquid and ice phase, size and morphology. These properties can eventually influence the angular light scattering properties of cirrus clouds as well as the growth and accretion mechanisms of single cloud particles. In this study we compare four commonly used optical probes to examine their response to small cloud particles of different phase and asphericity. Cloud simulation experiments were conducted at the Cosmics-Leaving-OUtdoor-Droplets (CLOUD) chamber at European Organisation for Nuclear Research (CERN). The chamber was operated in a series of multi-step adiabatic expansions to produce growth and sublimation of ice particles at super- and sub-saturated ice conditions and for initial temperatures of −30, −40 and −50 °C. The experiments were performed for ice cloud formation via homogeneous ice nucleation. We report the microphysical properties of small quasi-spherical ice particles in deep convection simulations and small hexagonal ice particles typical for in situ cirrus. Ice crystal asphericity and a degree of submicron complexity deduced from measurements of spatially resolved single particle light scattering patterns by the Particle Phase Discriminator mark 2 (PPD-2K, Karlsruhe edition) were compared with Cloud and Aerosol Spectrometer with Polarisation (CASPOL) measurements and images captured by the 3View Cloud Particle Imager (3V-CPI). Averaged path light scattering properties of the simulated ice clouds were measured using the Scattering-Intensity-Measurements-for-the-Optical-detectioN-of-icE (SIMONE) and single particle scattering properties were measured by the CASPOL. We show the ambiguity of several optical measurements in ice fraction determination of homogeneously frozen ice, in the case where sublimating quasi-spherical ice particles are present. Moreover, most of the instruments have shown a rather low sensitivity to the crystal complexity for small ice cloud particles that were grown under typical atmospheric conditions. Bulk averaged path depolarisation measurements of these clouds showed higher correlation to single particle measurements at high concentration and small diameters of cloud particles. These results have implications for the interpretation of atmospheric measurements and parametrisations for modelling, particularly for low particle number concentration clouds. This ensemble of optical instruments, using both averaged path and single particle detection presented here, in conjugation with the CLOUD chamber, reveals the possible discrepancies in comparisons of airborne and remote sensing measurements.

[1] Structural evolution of monsoon clouds in the core monsoon region of India has been examined using multisensor data. Invigoration of warm clouds above 4.5 km (occurring in only 15.4% days of the last 11 monsoon seasons) is associated with a transition from negative to positive normalized rainfall anomaly. Cloud top pressure reduces with an increase in aerosol optical depth at a higher rate of invigoration in drier condition (characterized by large fraction of absorbing aerosols) than wet condition. Cloud effective radius for warm clouds does not show any significant change with an increase in aerosol concentration in the presence of high liquid water path, probably due to strong buffering role of meteorology. The structural evolution of monsoon clouds is influenced by both dynamic and microphysical processes that prolong the cloud lifetime, resulting in infrequent rainfall. Our results call for improved representation of aerosol and cloud vertical structures in the climate models to resolve this issue.

International audience; The magnitude of aerosol radiative forcing caused by anthropogenic emissions depends on the baseline state of the atmosphere under Q:11 pristine preindustrial conditions. Measurements in the European Organisation for Nuclear Research (CERN) CLOUD chamber show that particle formation in atmospheric conditions can occur solely from Q:12 biogenic vapors. Here, we evaluate the potential effect of this source of particles on preindustrial cloud condensation nucleus (CCN) concentrations and aerosol cloud radiative forcing over the industrial period.Model simulations show that the pure biogenic particle formation mechanism has a much larger relative effect on CCN concentrations in the preindustrial atmosphere than in the present atmosphere because of the lower aerosol concentrations. Consequently, preindustrial cloud albedo is increased more than under present day conditions, and therefore, the cooling forcing of anthropogenic aerosols is reduced. Q:13 The mechanism increases CCN concentrations by 20–100% over a large fraction of the preindustrial lower atmosphere, and the magnitude of annual global mean radiative forcing caused by changes of cloud albedo since 1750 is reduced by 0.22 W m−² (27%) to −0.60 W m−².Model uncertainties, relatively slow formation rates, and limited available ambient measurements make it difficult to establish the significance of a mechanism that has its dominant effect under preindustrial conditions. Our simulations predict more particle formation in the Amazon than is observed. However, the first observation of pure organic nucleation has now been reported for the free troposphere. Given the potentially significant effect on anthropogenic forcing, effort should be made to better understand such naturally driven aerosol processes.

Atmospheric aerosols and their effect on clouds are thought to be important for anthropogenic radiative forcing of the climate, yet remain poorly understood1. Globally, around half of cloud condensation nuclei originate from nucleation of atmospheric vapours2. It is thought that sulfuric acid is essential to initiate most particle formation in the atmosphere3,4, and that ions have a relatively minor role5. Some laboratory studies, however, have reported organic particle formation without the intentional addition of sulfuric acid, although contamination could not be excluded6,7. Here we present evidence for the formation of aerosol particles from highly oxidized biogenic vapours in the absence of sulfuric acid in a large chamber under atmospheric conditions. The highly oxygenated molecules (HOMs) are produced by ozonolysis of α-pinene. We find that ions from Galactic cosmic rays increase the nucleation rate by one to two orders of magnitude compared with neutral nucleation. Our experimental findings are supported by quantum chemical calculations of the cluster binding energies of representative HOMs. Ion-induced nucleation of pure organic particles constitutes a potentially widespread source of aerosol particles in terrestrial environments with low sulfuric acid pollution.

New particle formation in the atmosphere produces around half of the cloud condensation nuclei that seed cloud droplets. Such particles have a pivotal role in determining the properties of clouds and the global radiation balance. Dunne et al. used the CLOUD (Cosmics Leaving Outdoor Droplets) chamber at CERN to construct a model of aerosol formation based on laboratory measured nucleation rates. They found that nearly all nucleation involves either ammonia or biogenic organic compounds. Furthermore in the present day atmosphere cosmic ray intensity cannot meaningfully affect climate via nucleation.Science this issue p. 1119Fundamental questions remain about the origin of newly formed atmospheric aerosol particles because data from laboratory measurements have been insufficient to build global models. In contrast gas phase chemistry models have been based on laboratory kinetics measurements for decades. We built a global model of aerosol formation by using extensive laboratory measurements of rates of nucleation involving sulfuric acid ammonia ions and organic compounds conducted in the CERN CLOUD (Cosmics Leaving Outdoor Droplets) chamber. The simulations and a comparison with atmospheric observations show that nearly all nucleation throughout the present day atmosphere involves ammonia or biogenic organic compounds in addition to sulfuric acid. A considerable fraction of nucleation involves ions but the relatively weak dependence on ion concentrations indicates that for the processes studied variations in cosmic ray intensity do not appreciably affect climate through nucleation in the present day atmosphere.U http://science.sciencemag.org/content/sci/354/6316/1119.full.pdf

About half of present-day cloud condensation nuclei originate from atmospheric nucleation, frequently appearing as a burst of new particles near midday1. Atmospheric observations show that the growth rate of new particles often accelerates when the diameter of the particles is between one and ten nanometres2,3. In this critical size range, new particles are most likely to be lost by coagulation with pre-existing particles4, thereby failing to form new cloud condensation nuclei that are typically 50 to 100 nanometres across. Sulfuric acid vapour is often involved in nucleation but is too scarce to explain most subsequent growth5,6, leaving organic vapours as the most plausible alternative, at least in the planetary boundary layer7,8,9,10. Although recent studies11,12,13 predict that low-volatility organic vapours contribute during initial growth, direct evidence has been lacking. The accelerating growth may result from increased photolytic production of condensable organic species in the afternoon2, and the presence of a possible Kelvin (curvature) effect, which inhibits organic vapour condensation on the smallest particles (the nano-Köhler theory)2,14, has so far remained ambiguous. Here we present experiments performed in a large chamber under atmospheric conditions that investigate the role of organic vapours in the initial growth of nucleated organic particles in the absence of inorganic acids and bases such as sulfuric acid or ammonia and amines, respectively. Using data from the same set of experiments, it has been shown15 that organic vapours alone can drive nucleation. We focus on the growth of nucleated particles and find that the organic vapours that drive initial growth have extremely low volatilities (saturation concentration less than 10−4.5 micrograms per cubic metre). As the particles increase in size and the Kelvin barrier falls, subsequent growth is primarily due to more abundant organic vapours of slightly higher volatility (saturation concentrations of 10−4.5 to 10−0.5 micrograms per cubic metre). We present a particle growth model that quantitatively reproduces our measurements. Furthermore, we implement a parameterization of the first steps of growth in a global aerosol model and find that concentrations of atmospheric cloud concentration nuclei can change substantially in response, that is, by up to 50 per cent in comparison with previously assumed growth rate parameterizations., Nature, 533 (7604), ISSN:0028-0836, ISSN:1476-4687