J. Browse

A marine biogenic source of atmospheric ice-nucleating particles

The amount of ice present in clouds can affect cloud lifetime, precipitation and radiative properties. The formation of ice in clouds is facilitated by the presence of airborne ice-nucleating particles. 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. 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. 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 probably biogenic and less than approximately 0.2 micrometres in size. We find that exudates separated from cells of the marine diatom Thalassiosira 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 Ocean and North Atlantic Ocean.

Uncertainty in the magnitude of aerosol-cloud radiative forcing over recent decades

Aerosols and their effect on the radiative properties of clouds are one of the largest sources of uncertainty in calculations of the Earths energy budget. Here the sensitivity of aerosol-cloud albedo effect forcing to 31 aerosol parameters is quantified. Sensitivities are compared over three periods; 1850-2008, 1978-2008, and 1998-2008. Despite declining global anthropogenic SO2 emissions during 1978-2008, a cancelation of regional positive and negative forcings leads to a near-zero global mean cloud albedo effect forcing. In contrast to existing negative estimates, our results suggest that the aerosol-cloud albedo effect was likely positive (0.006 to 0.028 W m −2 ) in the recent decade, making it harder to explain the temperature hiatus as a forced response. Proportional contributions to forcing variance from aerosol processes and natural and anthropogenic emissions are found to be period dependent. To better constrain forcing estimates, the processes that dominate uncertainty on the timescale of interest must be better understood.

The global aerosol synthesis and science project (GASSP): Measurements and modeling to reduce uncertainty

The largest uncertainty in the historical radiative forcing of climate is caused by changes in aerosol particles due to anthropogenic activity. Sophisticated aerosol microphysics processes have been included in many climate models in an effort to reduce the uncertainty. However, the models are very challenging to evaluate and constrain because they require extensive in-situ measurements of the particle size distribution, number concentration and chemical composition that are not available from global satellite observations. The Global Aerosol Synthesis and Science Project (GASSP) aims to improve the robustness of global aerosol models by combining new methodologies for quantifying model uncertainty, an extensive global dataset of aerosol in-situ microphysical and chemical measurements, and new ways to assess the uncertainty associated with comparing sparse point measurements with low resolution models. GASSP has assembled over 45,000 hours of measurements from ships and aircraft as well as data from over 350 ground stations. The measurements have been harmonized into a standardized format that is easily used by modellers and non-specialist users. Available measurements are extensive, but they biased to polluted regions of the northern hemisphere, leaving large pristine regions and many continental areas poorly sampled. The aerosol radiative forcing uncertainty can be reduced using a rigorous model-data synthesis approach. Nevertheless, our research highlights significant remaining challenges because of the difficulty of constraining many interwoven model uncertainties simultaneously. Although the physical realism of global aerosol models still needs to be improved, the uncertainty in aerosol radiative forcing will be reduced most effectively by systematically and rigorously constraining the models using extensive syntheses of measurements.

The Climatic Importance of Uncertainties in Regional Aerosol–Cloud Radiative Forcings over Recent Decades

AbstractRegional patterns of aerosol radiative forcing are important for understanding climate change on decadal time scales. Uncertainty in aerosol forcing is likely to vary regionally and seasonally because of the short aerosol lifetime and heterogeneous emissions. Here the sensitivity of regional aerosol cloud albedo effect (CAE) forcing to 31 aerosol process parameters and emission fluxes is quantified between 1978 and 2008. The effects of parametric uncertainties on calculations of the balance of incoming and outgoing radiation are found to be spatially and temporally dependent. Regional uncertainty contributions of opposite sign cancel in global-mean forcing calculations, masking the regional importance of some parameters. Parameters that contribute little to uncertainty in Earth’s global energy balance during recent decades make significant contributions to regional forcing variance. Aerosol forcing sensitivities are quantified within 11 climatically important regions, where surface temperatures ar...

Is Black Carbon an Unimportant Ice‐Nucleating Particle in Mixed‐Phase Clouds?

Abstract It has been hypothesized that black carbon (BC) influences mixed‐phase clouds by acting as an ice‐nucleating particle (INP). However, the literature data for ice nucleation by BC immersed in supercooled water are extremely varied, with some studies reporting that BC is very effective at nucleating ice, whereas others report no ice‐nucleating ability. Here we present new experimental results for immersion mode ice nucleation by BC from two contrasting fuels (n‐decane and eugenol). We observe no significant heterogeneous nucleation by either sample. Using a global aerosol model, we quantify the maximum relative importance of BC for ice nucleation when compared with K‐feldspar and marine organic aerosol acting as INP. Based on the upper limit from our laboratory data, we show that BC contributes at least several orders of magnitude less INP than feldspar and marine organic aerosol. Representations of its atmospheric ice‐nucleating ability based on older laboratory data produce unrealistic results when compared against ambient observations of INP. Since BC is a complex material, it cannot be unambiguously ruled out as an important INP species in all locations at all times. Therefore, we use our model to estimate a range of values for the density of active sites that BC particles must have to be relevant for ice nucleation in the atmosphere. The estimated values will guide future work on BC, defining the required sensitivity of future experimental studies.

The Effect of Atmospheric Acid Processing on the Global Deposition of Bioavailable Phosphorus From Dust

The role of dust as a source of bioavailable phosphorus (Bio-P) is quantified using a new parameterization for apatite dissolution in combination with global soil data maps and a global aerosol transport model. Mineral dust provides 31.2 Gg P yr-1 of Bio-P to the oceans, with 14.3 Gg P yr-1 from labile P present in the dust, and an additional 16.9 Gg P yr 1 from acid dissolution of apatite in the atmosphere, representing an increase of 120%. The North Atlantic, northwest Pacific, and Mediterranean Sea are identified as important sites of Bio-P deposition from mineral dust. The acid dissolution process increases the fraction of total P that is bioavailable from ~10% globally from the labile pool to 23% in the Atlantic Ocean, 45% in the Pacific Ocean, and 21% in the Indian Ocean, with an ocean global mean value of 22%. Strong seasonal variations, especially in the North Pacific, northwest Atlantic, and Indian Ocean, are driven by large-scale meteorology and pollution sources from industrial and biomass burning regions. Globally constant values of total P content and bioavailable fraction used previously do not capture the simulated variability. We find particular sensitivity to the representation of particle-to-particle variability of apatite, which supplies Bio-P through acid-dissolution, and calcium carbonate, which helps to buffer the dissolution process. A modest 10% external mixing results in an increase of Bio-P deposition by 18%. The total Bio-P calculated here (31.2 Gg P yr-1) represents a minimum compared to previous estimates due to the relatively low total P in the global soil map used.