Merikanto J

University of Leeds, Leeds, ENG, United Kingdom

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Publications (3)0 Total impact

  • Source
    Article: Effects of boundary layer particle formation on cloud droplet number and changes in cloud albedo from 1850 to 2000
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    ABSTRACT: We use a global aerosol microphysics model to estimate the effect of particle formation through activation nucleation in the boundary layer (BL) on cloud droplet number concentration (CDNC) on global and regional scales. The calculations are carried out for years 1850 and 2000 using historical emissions inventories for primary particles and aerosol precursor gases. Predicted CDNC in 2000 are in good agreement with in-situ observations when activation nucleation is included. We find that BL particle formation increases global annual mean CDNC by approximately the same relative amount in both years (16.0% in 1850 and 13.5% in 2000). As a result, global mean changes in cloud albedo are similar with and without BL particle formation. However, there are substantial regional effects of up to 50% enhancement or suppression of the 1850–2000 albedo change. Over most modern-day polluted northern hemisphere regions, including BL particle formation scheme suppresses the 1850–2000 increase in CDNC and cloud albedo because BL particle formation is already large in 1850. Over the Arctic the albedo change is suppressed by 23% in the annual mean and by 43% in summer when BL particle formation is taken into account. The albedo change of the persistent stratocumulus cloud deck west of Chile is enhanced by 49%.
    Atmospheric Chemistry and Physics. 01/2010;
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    Article: Impact of nucleation on global CCN
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    ABSTRACT: Cloud condensation nuclei (CCN) are derived from particles emitted directly into the atmosphere (primary emissions) or from the growth of nanometer-sized particles nucleated in the atmosphere. It is important to separate these two sources because they respond in different ways to gas and particle emission control strategies and environmental changes. Here, we use a global aerosol microphysics model to quantify the contribution of primary and nucleated particles to global CCN. The model considers primary emissions of sea spray, sulfate and carbonaceous particles, and nucleation processes appropriate for the free troposphere and boundary layer. We estimate that 45% of global low-level cloud CCN at 0.2% supersaturation are secondary aerosol derived from nucleation (ranging between 31–49% taking into account uncertainties in primary emissions and nucleation rates), with the remainder from primary emissions. The model suggests that 35% of CCN (0.2%) in global low-level clouds were created in the free and upper troposphere. In the marine boundary layer 55% of CCN (0.2%) are from nucleation, with 45% entrained from the free troposphere and 10% nucleated directly in the boundary layer. Combinations of model runs show that primary and nucleated CCN are non-linearly coupled. In particular, boundary layer nucleated CCN are strongly suppressed by both primary emissions and entrainment of particles nucleated in the free troposphere. Elimination of all primary emissions reduces global CCN (0.2%) by only 20% and elimination of upper tropospheric nucleation reduces CCN (0.2%) by only 12% because of the increased contribution from boundary layer nucleation.
    Atmospheric Chemistry and Physics. 01/2009;
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    Article: Explaining global surface aerosol number concentrations in terms of primary emissions and particle formation
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    ABSTRACT: 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.
    Atmospheric Chemistry and Physics Discussions. 01/2009;