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  • 1
    Publication Date: 2012-03-10
    Description: On the representation of immersion and condensation freezing in cloud models using different nucleation schemes Atmospheric Chemistry and Physics Discussions, 12, 7167-7209, 2012 Author(s): B. Ervens and G. Feingold Ice nucleation in clouds is often observed at temperatures 〉235 K, pointing to heterogeneous freezing as a predominant mechanism. Many models deterministically predict the number concentration of ice particles as a function of temperature and/or supersaturation. Laboratory experiments at constant temperature and/or supersaturation often report heterogeneous freezing as a stochastic, time-dependent process that follows classical nucleation theory which might appear to contradict singular freezing behavior. We explore the extent to which the choice of nucleation scheme (deterministic/stochastic, single/multiple contact angles θ) affects the prediction of the frozen ice nuclei (IN) fraction and cloud evolution. A box model with constant temperature and supersaturation is used to mimic published laboratory experiments of immersion freezing of kaolinite (~243 K), and the fitness of different nucleation schemes. Sensitivity studies show that agreement of all five schemes is restricted to the narrow parameter range (time, temperature, IN diameter) in the original laboratory studies. The schemes are implemented in an adiabatic parcel model that includes feedbacks of the formation and growth of drops and ice particles on supersaturation during the ascent of an air parcel. Model results show that feedbacks of droplets and ice on supersaturation limit ice nucleation events, often leading to smaller differences in number concentration of ice particles and ice water content (IWC) between stochastic and deterministic approaches than expected from the box model studies. However, the different parameterizations of θ distributions and time-dependencies are highly sensitive to IN size and can lead to great differences in predicted ice number concentrations and IWC between the different schemes. Finally, since the choice of nucleation scheme determines the temperature range over which nucleation occurs, at habit-prone temperatures (~253 K) different onset temperatures of freezing create variability in the initial inherent growth ratio of ice particles, which can lead to amplification or reduction in differences in predicted IWC.
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  • 2
    Publication Date: 2012-03-10
    Description: A multi-model assessment of the efficacy of sea spray geoengineering Atmospheric Chemistry and Physics Discussions, 12, 7125-7166, 2012 Author(s): K. J. Pringle, K. S. Carslaw, T. Fan, G.W. Mann, A. Hill, P. Stier, K. Zhang, and H. Tost Artificially increasing the albedo of marine clouds by the mechanical emission of sea spray aerosol has been proposed as a geoengineering technique to slow the warming caused by anthropogenic greenhouse gases. A previous global model study found that only modest increases and sometimes even decreases in cloud drop number (CDN) concentrations would result from plausible emission scenarios. Here we extend that work to examine the conditions under which decreases in CDN can occur, and use three independent global models to quantify maximum achievable CDN changes. We find that decreases in CDN can occur when at least three of the following conditions are met: the injected particle number is 250–300 nm, the background aerosol loading is large (≥150 cm −3 ) and the in-cloud updraught velocity is low (
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  • 3
    Publication Date: 2012-02-25
    Description: Observations of glyoxal and formaldehyde as metrics for the anthropogenic impact on rural photochemistry Atmospheric Chemistry and Physics Discussions, 12, 6049-6084, 2012 Author(s): J. P. DiGangi, S. B. Henry, A. Kammrath, E. S. Boyle, L. Kaser, R. Schnitzhofer, M. Graus, A. Turnipseed, J.-H. Park, R. J. Weber, R. S. Hornbrook, C. A. Cantrell, R. L. Maudlin III, S. Kim, Y. Nakashima, G. M. Wolfe, Y. Kajii, E. C. Apel, A. H. Goldstein, A. Guenther, T. Karl, A. Hansel, and F. N. Keutsch We present simultaneous fast, in-situ measurements of formaldehyde and glyoxal from two rural campaigns, BEARPEX 2009 and BEACHON-ROCS, both located in Pinus Ponderosa forests with emissions dominated by biogenic volatile organic compounds (VOCs). Despite considerable variability in the formaldehyde and glyoxal concentrations, the ratio of glyoxal to formaldehyde, R GF , displayed a very regular diurnal cycle over nearly 2 weeks of measurements. The only deviations in R GF were toward higher values and were the result of a biomass burning event during BEARPEX 2009 and very fresh anthropogenic influence during BEACHON-ROCS. Other rapid changes in glyoxal and formaldehyde concentrations have hardly any affect on R GF and could reflect transitions between low and high NO regimes. The trend of increased R GF from both anthropogenic reactive VOC mixtures and biomass burning compared to biogenic reactive VOC mixtures is robust due to the short timescales over which the observed changes in R GF occurred. Satellite retrievals, which suggest higher R GF for biogenic areas, are in contrast to our observed trends. It remains important to address this discrepancy, especially in view of the importance of satellite retrievals and in-situ measurements for model comparison. In addition, we propose that R GF , together with the absolute concentrations of glyoxal and formaldehyde, represents a useful metric for biogenic or anthropogenic reactive VOC mixtures. In particular, R GF yields information about not simply the VOCs in an airmass, but the VOC processing that directly couples ozone and secondary organic aerosol production.
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  • 4
    Publication Date: 2012-02-25
    Description: Characterization of aerosol and cloud water at a mountain site during WACS 2010: secondary organic aerosol formation through oxidative cloud processing Atmospheric Chemistry and Physics Discussions, 12, 6019-6047, 2012 Author(s): A. K. Y. Lee, K. L. Hayden, P. Herckes, W. R. Leaitch, J. Liggio, A. M. Macdonald, and J. P. D. Abbatt The water-soluble fractions of aerosol samples and cloud water collected during Whistler Aerosol and Cloud Study (WACS 2010) were analyzed using an Aerodyne aerosol mass spectrometer (AMS). This is the first study to report AMS organic spectra of re-aerosolized cloud water, and to make direct comparison between the AMS spectra of cloud water and aerosol samples collected at the same location. In general, the aerosol and cloud organic spectra were very similar, indicating that the cloud water organics likely originated from secondary organic aerosol (SOA) formed nearby. By using a photochemical reactor to oxidize both aerosol filter extracts and cloud water, we find evidence that fragmentation of aerosol water-soluble organics increases their volatility during oxidation. By contrast, enhancement of AMS-measurable organic mass by up to 30% was observed during aqueous-phase photochemical oxidation of cloud water organics. We propose that additional SOA material was produced by functionalizing dissolved organics via OH oxidation, where these dissolved organics are sufficiently volatile that they are not usually part of the aerosol. This work points out that water-soluble organic compounds of intermediate volatility (IVOC), such as cis -pinonic acid, produced via gas-phase oxidation of monoterpenes, can be important aqueous-phase SOA precursors in a biogenic-rich environment.
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  • 5
    Publication Date: 2012-02-25
    Description: Evaluation of chemical transport model predictions of primary organic aerosol for air masses classified by particle-component-based factor analysis Atmospheric Chemistry and Physics Discussions, 12, 5939-6018, 2012 Author(s): C. A. Stroud, M. D. Moran, P. A. Makar, S. Gong, W. Gong, J. Zhang, J. G. Slowik, J. P. D. Abbatt, G. Lu, J. R. Brook, C. Mihele, Q. Li, D. Sills, K. B. Strawbridge, M. L. McGuire, and G. J. Evans Observations from the 2007 Border Air Quality and Meteorology Study (BAQS-Met 2007) in southern Ontario (ON), Canada, were used to evaluate Environment Canada's regional chemical transport model predictions of primary organic aerosol (POA). Environment Canada's operational numerical weather prediction model and the 2006 Canadian and 2005 US national emissions inventories were used as input to the chemical transport model (named AURAMS). Particle-component-based factor analysis was applied to aerosol mass spectrometer measurements made at one urban site (Windsor, ON) and two rural sites (Harrow and Bear Creek, ON) to derive hydrocarbon-like organic aerosol (HOA) factors. Co-located carbon monoxide (CO), PM 2.5 black carbon (BC), and PM 1 SO 4 measurements were also used for evaluation and interpretation, permitting a detailed diagnostic model evaluation. At the urban site, good agreement was observed for the comparison of daytime campaign PM 1 POA and HOA mean values: 1.1 μg m −3 vs. 1.2 μg m −3 , respectively. However, a POA overprediction was evident on calm nights due to an overly-stable model surface layer. Biases in model POA predictions trended from positive to negative with increasing HOA values. This trend has several possible explanations, including (1) underweighting of urban locations in particulate matter (PM) spatial surrogate fields, (2) overly-coarse model grid spacing for resolving urban-scale sources, and (3) lack of a model particle POA evaporation process during dilution of vehicular POA tail-pipe emissions to urban scales. Furthermore, a trend in POA bias was observed at the urban site as a function of the BC/HOA ratio, suggesting a possible association of POA underprediction for diesel combustion sources. For several time periods, POA overprediction was also observed for sulphate-rich plumes, suggesting that our model POA fractions for the PM 2.5 chemical speciation profiles may be too high for these point sources. At the rural Harrow site, significant underpredictions in PM 1 POA concentration were found compared to observed HOA concentration and were associated, based on back-trajectory analysis, with (1) transport from the Detroit/Windsor urban complex, (2) longer-range transport from the US Midwest, and (3) biomass burning. Daytime CO concentrations were significantly overpredicted at Windsor but were unbiased at Harrow. Collectively, these biases provide support for a hypothesis that combines a current underweighting of PM spatial surrogate fields for urban locations with insufficient model vertical mixing for sources close to the urban measurement sites. The magnitude of the area POA emissions sources in the US and Canadian inventories (e.g., food cooking, road and soil dust, waste disposal burning) suggests that more effort should be placed at reducing uncertainties in these sectors, especially spatial and temporal surrogates.
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  • 6
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    Springer Nature
    Publication Date: 2012-02-25
    Description: Money matters Nature Climate Change 2, 133 24022012 doi: 10.1038/nclimate1446 Soulless economics as well as corporate and personal greed constrain climate-friendly behaviour. But explaining climate change in cultural and artistic terms may soften hardened hearts.
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  • 7
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    Springer Nature
    Publication Date: 2012-02-25
    Description: Peak timber Nature Climate Change 2, 141 24022012 doi: 10.1038/nclimate1432 Nicola Jones
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  • 8
    Publication Date: 2012-02-25
    Description: Enhanced warming over the global subtropical western boundary currents Nature Climate Change 2, 161 29012012 doi: 10.1038/nclimate1353 Lixin Wu Wenju Cai Liping Zhang Hisashi Nakamura Axel Timmermann Terry Joyce Michael J. McPhaden Michael Alexander Bo Qiu Martin Visbeck Ping Chang Benjamin Giese An analysis indicates that the warm, powerful currents that flow along the western edges of ocean basins warmed more than twice as quickly than the global ocean as a whole over the past century. This enhanced warming could have important effects on climate because these currents affect the air–sea exchange of heat, moisture and carbon dioxide.
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  • 9
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    Springer Nature
    Publication Date: 2012-02-25
    Description: Evolutionary ecology: Survival of the fittest Nature Climate Change 2, 147 24022012 doi: 10.1038/nclimate1443 Anna Petherick
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  • 10
    Publication Date: 2012-02-25
    Description: Economics: The rising costs of hurricanes Nature Climate Change 2, 148 24022012 doi: 10.1038/nclimate1427 Stéphane Hallegatte The impact of climate change on economic losses from tropical cyclones is a major concern. New research shows that — like changes in population and assets — climate change may double global losses from hurricanes.
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