The radiative effect of ion-induced inorganic nucleation in the free troposphere

To determine the effect of cosmic rays on the Earth's climate via ion-induced nucleation, a parametrisation of inorganic nucleation was formulated based on experiments at the CERN CLOUD experiment. The parametrisation was implemented in the GLOMAP aerosol microphysics model and used to estimate the radiative effect of the change in ionisation experienced over an 11-year solar cycle

Aerosol climate feedback due to decadal increases in Southern Hemisphere wind speeds

Observations indicate that the westerly jet in the Southern Hemisphere troposphere is accelerating. Using a global aerosol model we estimate that the increase in wind speed of 0.45 + /- 0.2 m s(-1) decade(-1) at 50-65 degrees S since the early 1980s caused a higher sea spray flux, resulting in an increase of cloud condensation nucleus concentrations of more than 85% in some regions, and of 22% on average between 50 and 65 degrees S. These fractional increases are similar in magnitude to the decreases over many northern hemisphere land areas due to changes in air pollution over the same period. The change in cloud drop concentrations causes an increase in cloud reflectivity and a summertime radiative forcing between at 50 and 65 degrees S comparable in magnitude but acting against that from greenhouse gas forcing over the same time period, and thus represents a substantial negative climate feedback. However, recovery of Antarctic ozone depletion in the next two decades will likely cause a fall in wind speeds, a decrease in cloud drop concentration and a correspondingly weaker cloud feedback

Explaining global surface aerosol number concentrations in terms of primary emissions and particle formation

We use observations of total particle number concentration at 36 worldwide sites and a global aerosol model to quantify the primary and secondary sources of particle number. We show that emissions of primary particles can reasonably reproduce the spatial pattern of observed condensation nuclei (CN) (R2=0.51) but fail to explain the observed seasonal cycle at many sites (R2=0.1). The modeled CN concentration in the free troposphere is biased low (normalised mean bias, NMB=−88%) unless a secondary source of particles is included, for example from binary homogeneous nucleation of sulfuric acid and water (NMB=−25%). Simulated CN concentrations in the continental boundary layer (BL) are also biased low (NMB=−74%) unless the number emission of anthropogenic primary particles is increased or an empirical BL particle formation mechanism based on sulfuric acid is used. We find that the seasonal CN cycle observed at continental BL sites is better simulated by including a BL particle formation mechanism (R2=0.3) than by increasing the number emission from primary anthropogenic sources (R2=0.18). Using sensitivity tests we derive optimum rate coefficients for this nucleation mechanism, which agree with values derived from detailed case studies at individual sites

New Approaches to Quantifying Aerosol Influence on the Cloud Radiative Effect

The topic of cloud radiative forcing associated with the atmospheric aerosol has been the focus of intense scrutiny for decades. The enormity of the problem is reflected in the need to understand aspects such as aerosol composition, optical properties, cloud condensation, and ice nucleation potential, along with the global distribution of these properties, controlled by emissions, transport, transformation, and sinks. Equally daunting is that clouds themselves are complex, turbulent, microphysical entities and, by their very nature, ephemeral and hard to predict. Atmospheric general circulation models represent aerosol−cloud interactions at ever-increasing levels of detail, but these models lack the resolution to represent clouds and aerosol−cloud interactions adequately. There is a dearth of observational constraints on aerosol−cloud interactions. We develop a conceptual approach to systematically constrain the aerosol−cloud radiative effect in shallow clouds through a combination of routine process modeling and satellite and surface-based shortwave radiation measurements. We heed the call to merge Darwinian and Newtonian strategies by balancing microphysical detail with scaling and emergent properties of the aerosol−cloud radiation system

Results from the CERN pilot CLOUD experiment

During a 4-week run in October–November 2006, a pilot experiment was performed at the CERN Proton Synchrotron in preparation for the Cosmics Leaving OUtdoor Droplets (CLOUD) experiment, whose aim is to study the possible influence of cosmic rays on clouds. The purpose of the pilot experiment was firstly to carry out exploratory measurements of the effect of ionising particle radiation on aerosol formation from trace H2SO4 vapour and secondly to provide technical input for the CLOUD design. A total of 44 nucleation bursts were produced and recorded, with formation rates of particles above the 3 nm detection threshold of between 0.1 and 100 cm -3 s -1, and growth rates between 2 and 37 nm h -1. The corresponding H2O concentrations were typically around 106 cm -3 or less. The experimentally-measured formation rates and htwosofour concentrations are comparable to those found in the atmosphere, supporting the idea that sulphuric acid is involved in the nucleation of atmospheric aerosols. However, sulphuric acid alone is not able to explain the observed rapid growth rates, which suggests the presence of additional trace vapours in the aerosol chamber, whose identity is unknown. By analysing the charged fraction, a few of the aerosol bursts appear to have a contribution from ion-induced nucleation and ion-ion recombination to form neutral clusters. Some indications were also found for the accelerator beam timing and intensity to influence the aerosol particle formation rate at the highest experimental SO2 concentrations of 6 ppb, although none was found at lower concentrations. Overall, the exploratory measurements provide suggestive evidence for ion-induced nucleation or ion-ion recombination as sources of aerosol particles. However in order to quantify the conditions under which ion processes become significant, improvements are needed in controlling the experimental variables and in the reproducibility of the experiments. Finally, concerning technical aspects, the most important lessons for the CLOUD design include the stringent requirement of internal cleanliness of the aerosol chamber, as well as maintenance of extremely stable temperatures (variations below 0.1 °C

Understanding the nature of atmospheric acid processing of mineral dusts in supplying bioavailable phosphorus to the oceans

Acidification of airborne dust particles can dramatically increase the amount of bioavailable phosphorus (P) deposited on the surface ocean. Experiments were conducted to simulate atmospheric processes and determine the dissolution behaviour of phosphorus compounds in dust and dust precursors oils. Acid dissolution occurs rapidly (seconds to minutes) and is controlled by the amount of H + ions present. For H + 10-4 mol per gram of dust, the amount of phosphorus (and Ca) released follows a power law dependent on the amount of H + consumed until all inorganic phosphorus minerals are exhausted and the final pH remains acidic. Once dissolved, phosphorus will stay in solution due to slow precipitation kinetics. Dissolution of apatite-P, the major mineral phase in dust (79-96%), occurs whether CaCO 3 is present or not, though the increase in dissolved phosphorus is greater if CaCO 3 is absent or if the particles are externally mixed. The system was modelled adequately as a simple mixture of apatite-P and calcite. Phosphorus dissolves readily by acid processes in the atmosphere in contrast to iron, which dissolves slower and is subject to re-precipitation at cloud water pH. We show that acidification can increase bioavailable phosphorus deposition over large areas of the globe, and may explain much of the previously observed patterns of variability in leachable phosphorus in oceanic areas where primary productivity is limited by this nutrient (e.g. Mediterranean)

Precipitation sensitivity to autoconversion rate in a numerical weather-prediction model

Aerosols are known to significantly affect cloud and precipitation patterns and intensity, but these interactions are ignored or very simplistically handled in climate and numerical weather-prediction (NWP) models. A suite of one-way nested Met Office Unified Model (UM) runs, with a single-moment bulk microphysics scheme was used to study two convective cases with contrasting characteristics observed in southern England. The autoconversion process that converts cloud water to rain is directly controlled by the assumed droplet number. The impact of changing cloud droplet number concentration (CDNC) on cloud and precipitation evolution can be inferred through changes to the autoconversion rate. This was done for a range of resolutions ranging from regional NWP (1 km) to high resolution (up to 100 m grid spacing) to evaluate the uncertainties due to changing CDNC as a function of horizontal grid resolution. The first case is characterised by moderately intense convective showers forming below an upper-level potential vorticity anomaly, with a low freezing level. The second case, characterised by one persistent stronger storm, is warmer with a deeper boundary layer. The colder case is almost insensitive to even large changes in CDNC, while in the warmer case a change of a factor of 3 in assumed CDNC affects total surface rain rate by ~17%. In both cases the sensitivity to CDNC is similar at all grid spacings <1 km. The contrasting sensitivities of these cases are induced by their contrasting ice-phase proportion. The ice processes in this model damp the precipitation sensitivity to CDNC. For this model the convection is sensitive to CDNC when the accretion process is more significant than the melting process and vice versa

Neutral molecular cluster formation of sulfuric acid-dimethylamine observed in real time under atmospheric conditions

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