scholarly journals A global off-line model of size-resolved aerosol microphysics: I. Model development and prediction of aerosol properties

2005 ◽  
Vol 5 (8) ◽  
pp. 2227-2252 ◽  
Author(s):  
D. V. Spracklen ◽  
K. J. Pringle ◽  
K. S. Carslaw ◽  
M. P. Chipperfield ◽  
G. W. Mann
Keyword(s):  
Boundary Layer ◽  
Sulfuric Acid ◽  
Size Distribution ◽  
Marine Boundary Layer ◽  
Transport Model ◽  
Model Development ◽  
Aerosol Size Distribution ◽  
Chemical Transport Model ◽  
Cloud Processing ◽  
Nucleation Mechanisms

Abstract. A GLObal Model of Aerosol Processes (GLOMAP) has been developed as an extension to the TOMCAT 3-D Eulerian off-line chemical transport model. GLOMAP simulates the evolution of the global aerosol size distribution using a sectional two-moment scheme and includes the processes of aerosol nucleation, condensation, growth, coagulation, wet and dry deposition and cloud processing. We describe the results of a global simulation of sulfuric acid and sea spray aerosol. The model captures features of the aerosol size distribution that are well established from observations in the marine boundary layer and free troposphere. Modelled condensation nuclei (CN>3nm) vary between about 250–500 cm-3 in remote marine boundary layer regions and are generally in good agreement with observations. Modelled continental CN concentrations are lower than observed, which may be due to lack of some primary aerosol sources or the neglect of nucleation mechanisms other than binary homogeneous nucleation of sulfuric acid-water particles. Remote marine CN concentrations increase to around 2000–10 000 cm

scholarly journals A global off-line model of size-resolved aerosol microphysics: I. Model development and prediction of aerosol properties

2005 ◽  
Vol 5 (1) ◽  
pp. 179-215 ◽  
Author(s):  
D. V. Spracklen ◽  
K. J. Pringle ◽  
K. S. Carslaw ◽  
M. P. Chipperfield ◽  
G. W. Mann
Keyword(s):  
Boundary Layer ◽  
Sulfuric Acid ◽  
Size Distribution ◽  
Marine Boundary Layer ◽  
Transport Model ◽  
Cloud Condensation Nuclei ◽  
Aerosol Size Distribution ◽  
Sea Spray ◽  
Condensation Nuclei ◽  
Upper Troposphere

Abstract. A GLObal Model of Aerosol Processes (GLOMAP) has been developed as an extension to the TOMCAT 3-D Eulerian off-line chemical transport model. GLOMAP simulates the evolution of the global aerosol size distribution using a sectional two-moment scheme and includes the processes of aerosol nucleation, condensation, growth, coagulation, wet and dry deposition and cloud processing. We describe the results of a global simulation of sulfuric acid and sea spray aerosol. The model captures features of the aerosol size distribution that are well established from observations in the marine boundary layer and free troposphere. Modelled condensation nuclei (CN>3 nm) vary between about 250–500 cm-3 in remote marine boundary layer regions and between 2000 and 10 000 cm-3 (at standard temperature and pressure) in the upper troposphere. Cloud condensation nuclei (CCN) at 0.2% supersaturation vary between about 1000 cm-3 in polluted regions and between 10 and 500 cm-3 in the remote marine boundary layer. New particle formation through sulfuric acid-water binary nucleation occurs predominantly in the upper troposphere, but the model results show that these particles contribute greatly to aerosol concentrations in the marine boundary layer. It is estimated that sea spray emissions account for only ~10% of CCN in the tropical marine boundary layer, but between 20 and 75% in the mid-latitude Southern Ocean.

scholarly journals Intercomparison of modal and sectional aerosol microphysics representations within the same 3-D global chemical transport model

2012 ◽  
Vol 12 (1) ◽  
pp. 623-689 ◽  
Author(s):  
G. W. Mann ◽  
K. S. Carslaw ◽  
D. A. Ridley ◽  
D. V. Spracklen ◽  
K. J. Pringle ◽  
...  
Keyword(s):  
Size Distribution ◽  
Transport Model ◽  
Cloud Condensation Nuclei ◽  
Particle Growth ◽  
Free Troposphere ◽  
Chemical Transport Model ◽  
Condensation Nuclei ◽  
Chemistry Transport Model ◽  
Surface Mass ◽  
Cloud Processing

Abstract. A global modal aerosol microphysics module (GLOMAP-mode) is evaluated and improved by comparing against a sectional version (GLOMAP-bin) and observations in the same 3-D global offline chemistry transport model. With both schemes, the model captures the main features of the global particle size distribution, with sub-micron aerosol approximately unimodal in continental regions and bi-modal in marine regions. Initial bin-mode comparisons showed that various size distribution parameter settings (mode widths and inter-modal separation sizes) resulted in clear biases compared to the sectional scheme. By adjusting these parameters in the modal scheme, much better agreement is achieved against the bin scheme and observations. Surface mass of sulphate, sea-salt, black carbon (BC) and organic carbon (OC) are, on the annual mean, within 25 % in the two schemes in nearly all regions. On the annual mean, surface level concentrations of condensation nuclei (CN), cloud condensation nuclei (CCN), surface area density and condensation sink also compare within 25 % in most regions. However, marine CCN concentrations between 30° N and 30° S are systematically higher in the modal scheme, by 25–60 %, which we attribute to differences in size-resolved particle growth or cloud-processing. Larger differences also exist in regions or seasons dominated by biomass burning and in free-troposphere and high-latitude regions. Indeed, in the free-troposphere, GLOMAP-mode BC is a factor 2–4 higher than GLOMAP-bin, likely due to differences in size-resolved scavenging. Nevertheless, in most parts of the atmosphere, we conclude that bin-mode differences are much less than model-observation differences, although some processes are missing in these runs which may pose a bigger challenge to modal schemes (e.g. boundary layer nucleation, ultra-fine sea-spray). The findings here underline the need for a spectrum of complexity in global models, with size-resolved aerosol properties predicted by modal schemes needing to be continually benchmarked and improved against freely evolving sectional schemes and observations.

scholarly journals Assessing the potential efficacy of marine cloud brightening for cooling Earth using a simple heuristic model

2021 ◽  
Vol 21 (19) ◽  
pp. 14507-14533
Author(s):  
Robert Wood
Keyword(s):  
Boundary Layer ◽  
Size Distribution ◽  
Radiative Forcing ◽  
Marine Boundary Layer ◽  
Cloud Droplet ◽  
Aerosol Size Distribution ◽  
Heuristic Model ◽  
Droplet Concentration ◽  
Salt Mass ◽  
Large Eddy

Abstract. A simple heuristic model is described to assess the potential for increasing solar reflection by augmenting the aerosol population below marine low clouds, which nominally leads to increased cloud droplet concentration and albedo. The model estimates the collective impact of many point source particle sprayers, each of which generates a plume of injected particles that affects clouds over a limited area. A look-up table derived from simulations of an explicit aerosol activation scheme is used to derive cloud droplet concentration as a function of the sub-cloud aerosol size distribution and updraft speed, and a modified version of Twomey's formulation is used to estimate radiative forcing. Plume overlap is accounted for using a Poisson distribution, assuming idealized elongated cuboid plumes that have a length driven by aerosol lifetime and wind speed, a width consistent with satellite observations of ship track broadening, and a depth equal to an assumed boundary layer depth. The model is found to perform favorably against estimates of brightening from large eddy simulation studies that explicitly model cloud responses to aerosol injections over a range of conditions. Although the heuristic model does not account for cloud condensate or coverage adjustments to aerosol, in most realistic ambient remote marine conditions these tend to augment the Twomey effect in the large eddy simulations, with the result being a modest underprediction of brightening in the heuristic model. The heuristic model is used to evaluate the potential for global radiative forcing from marine cloud brightening as a function of the quantity, size, and lifetime of salt particles injected per sprayer and the number of sprayers deployed. Radiative forcing is sensitive to both the background aerosol size distribution in the marine boundary layer into which particles are injected and the assumed updraft speed. Given representative values from the literature, radiative forcing sufficient to offset a doubling of carbon dioxide ΔF2×CO2 is possible but would require spraying 50 % or more of the ocean area. This is likely to require at least 104 sprayers to avoid major losses of particles due to near-sprayer coagulation. The optimal dry diameter of injected particles, for a given salt mass injection rate, is 30–60 nm. A major consequence is that the total salt emission rate (50–70 Tg yr−1) required to offset ΔF2×CO2 is a factor of five lower than the emissions rates required to generate significant forcing in previous studies with climate models, which have mostly assumed dry diameters for injected particles in excess of 200 nm. With the lower required emissions, the salt mass loading in the marine boundary layer for ΔF2×CO2 is dominated by natural salt aerosol, with injected particles only contributing ∼ 10 %. When using particle sizes optimized for cloud brightening, the aerosol direct radiative forcing is shown to make a minimal contribution to the overall radiative forcing.

scholarly journals Assessing the potential efficacy of marine cloud brightening for cooling Earth using a simple heuristic model

2021 ◽  
Author(s):  
Robert Wood
Keyword(s):  
Boundary Layer ◽  
Size Distribution ◽  
Radiative Forcing ◽  
Marine Boundary Layer ◽  
Cloud Droplet ◽  
Aerosol Size Distribution ◽  
Heuristic Model ◽  
Droplet Concentration ◽  
Salt Mass ◽  
Large Eddy

Abstract. A simple heuristic model is described to assess the potential for increasing solar reflection by augmenting the aerosol population below marine low clouds, which nominally leads to increased cloud droplet concentration and albedo. The model estimates the collective impact of many point-source particle sprayers, each of which generates a plume of injected particles that affects clouds over a limited area. A widely-used aerosol activation scheme is used to derive cloud droplet concentration as a function of the sub-cloud aerosol size distribution and updraft speed, and a modified version of Twomey's formulation is used to estimate radiative forcing. Plume overlap is accounted for using a Poisson distribution assuming idealized elongated cuboid plumes that have a length driven by aerosol lifetime and wind speed, a width consistent with satellite observations of ship track broadening, and a depth equal to an assumed boundary layer depth. The model is found to perform favorably against estimates of brightening from large eddy simulation studies that explicitly model cloud responses to aerosol injections over a range of conditions. Although the heuristic model does not account for cloud condensate or coverage adjustments to aerosol, in most realistic ambient remote marine conditions these tend to augment the Twomey effect in the large eddy simulations, with the resulting being a modest underprediction of brightening in the heuristic model. The heuristic model is used to evaluate the potential for global radiative forcing from marine cloud brightening as a function of the quantity, size, and lifetime of salt particles injected per sprayer and the number of sprayers deployed. Radiative forcing is sensitive to both the background aerosol size distribution in the marine boundary layer into which particles are injected, and the assumed updraft speed. Given representative values from the literature, radiative forcing sufficient to offset a doubling of carbon dioxide ΔF2xCO2 is possible but would require spraying over 50% or more of the ocean area. This is likely to require at least 104 sprayers to avoid major losses of particles due to near-sprayer coagulation. The optimal dry diameter of injected particles, for a given salt mass injection rate, is 30–60 nm. A major consequence is that the total salt emission rate (50–70 Tg/yr) required to offset F2xCO2 is a factor of five lower than the emissions rates required to generate significant forcing in previous studies with climate models, which have mostly assumed dry diameters for injected particles in excess of 200 nm. With the lower required emissions, the salt mass loading in the marine boundary layer for F2xCO2 is dominated by natural salt aerosol, with injected particles only contributing ~ 10%. When using particle sizes optimized for cloud brightening, the aerosol direct radiative forcing is shown to make a minimal contribution to the overall radiative forcing.

scholarly journals Seasonal features and origins of carbonaceous aerosols at Syowa Station, coastal Antarctica

2019 ◽  
Vol 19 (11) ◽  
pp. 7817-7837 ◽  
Author(s):  
Keiichiro Hara ◽  
Kengo Sudo ◽  
Takato Ohnishi ◽  
Kazuo Osada ◽  
Masanori Yabuki ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Marine Boundary Layer ◽  
Transport Model ◽  
Model Simulation ◽  
Chemical Transport ◽  
Chemical Transport Model ◽  
Backward Trajectory ◽  
Syowa Station ◽  
The Antarctic ◽  
Measurement Period

Abstract. We have measured black carbon (BC) concentrations at Syowa Station, Antarctica, since February 2005. The measured BC concentrations in 2005–2016 were corrected to equivalent BC (EBC) concentrations using Weingartner's method. Seasonal features of EBC concentrations, long-range transport from mid-latitudes to the Antarctic coast, and their origins were characterized. Results show that daily median EBC concentrations were below the detection limit (0.2 ng m−3) to 63.8 ng m−3 at Syowa Station (median, 1.8 ng m−3; mean, 2.7 ng m−3 during the measurement period of February 2005–December 2016). Although seasonal features and year-to-year variations in EBC concentrations were observed, no long-term trend of EBC concentrations was clear during our measurement period. Seasonal features of EBC concentrations showed a spring maximum during September–October at Syowa Station. To elucidate EBC transport processes, origins, and the potential source area (PSA), we compared EBC data to backward trajectory analysis and chemical transport model simulation. From comparison with backward trajectory, high EBC concentrations were found in air masses from the marine boundary layer. This finding implies that transport via the marine boundary layer was the most important transport pathway to EBC concentrations at Antarctic coasts. Some EBC was supplied to the Antarctic region by transport via the upper free troposphere. Chemical transport model simulation demonstrated that the most important origins and PSA of EBC at Syowa Station were biomass burning in South America and southern Africa. Fossil fuel combustion in South America and southern Africa also have important contributions. The absorption Ångström exponent (AAE) showed clear seasonal features with 0.5–1.0 during April–October and maximum (1.0–1.5) in December–February. The AAE features might be associated with organic aerosols and mixing states of EBC.

scholarly journals Ammonia in the summertime Arctic marine boundary layer: sources, sinks and implications

2015 ◽  
Vol 15 (21) ◽  
pp. 29973-30016 ◽  
Author(s):  
G. R. Wentworth ◽  
J. G. Murphy ◽  
B. Croft ◽  
R. V. Martin ◽  
J. R. Pierce ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Marine Boundary Layer ◽  
Transport Model ◽  
Canadian Arctic ◽  
Atmospheric Composition ◽  
Chemical Transport Model ◽  
Baffin Bay ◽  
Melt Ponds ◽  
Ambient Nh3 ◽  
The Impact

Abstract. Continuous hourly measurements of gas-phase ammonia (NH3(g)) were taken from 13 July to 7 August 2014 on a research cruise throughout Baffin Bay and the eastern Canadian Arctic Archipelago. Concentrations ranged from 30–650 ng m−3 (40–870 pptv) with the highest values recorded in Lancaster Sound (74°13' N, 84°00' W). Simultaneous measurements of total ammonium ([NHx]), pH and temperature in the ocean and in melt ponds were used to compute the compensation point (χ), which is the ambient NH3(g) concentration at which surface–air fluxes change direction. Ambient NH3(g) was usually several orders of magnitude larger than both χocean and χMP (< 0.4–10 ng m3) indicating these surface pools are net sinks of NH3(g). Flux calculations estimate average net downward fluxes of 1.4 and 1.1 ng m-2 s-1 for the open ocean and melt ponds, respectively. Sufficient NH3(g) was present to neutralize non-sea salt sulphate (nss-SO42-) in the boundary layer during most of the study. This finding was corroborated with a historical dataset of PM2.5 composition from Alert, NU (82°30' N, 62°20' W) wherein the median ratio of NH4+/nss-SO42- equivalents was greater than 0.75 in June, July and August. The GEOS-Chem chemical transport model was employed to examine the impact of NH3(g) emissions from seabird guano on boundary-layer composition and nss-SO42- neutralization. A GEOS-Chem simulation without seabird emissions underestimated boundary layer NH3(g) by several orders of magnitude and yielded highly acidic aerosol. A simulation that included seabird NH3 emissions was in better agreement with observations for both NH3(g) concentrations and nss-SO42- neutralization. This is strong evidence that seabird colonies are significant sources of NH3(g) in the summertime Arctic, and are ubiquitous enough to impact atmospheric composition across the entire Baffin Bay region. Large wildfires in the Northwest Territories were likely an important source of NH3(g), but their influence was probably limited to the Central Canadian Arctic. Implications of seabird-derived N-deposition to terrestrial and aquatic ecosystems are also discussed.

scholarly journals Combining airborne in situ and ground-based lidar measurements for attribution of aerosol layers

2018 ◽  
Author(s):  
Anna Nikandrova ◽  
Ksenia Tabakova ◽  
Antti Manninen ◽  
Riikka Väänänen ◽  
Tuukka Petäjä ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Size Distribution ◽  
Aerosol Size Distribution ◽  
Long Range Transport ◽  
Back Trajectories ◽  
Clear Sky ◽  
Temporal And Spatial Variability ◽  
Range Transport ◽  
Temporal And Spatial

Abstract. Understanding the distribution of aerosol layers is important for determining long range transport and aerosol radiative forcing. In this study we combine airborne in situ measurements of aerosol with data obtained by a ground-based High Spectral Resolution Lidar (HSRL) and radiosonde profiles to investigate the temporal and vertical variability of aerosol properties in the lower troposphere. The HSRL was deployed in Hyytiälä, Southern Finland, from January to September 2014 as a part of the US DoE ARM (Atmospheric Radiation Measurement) mobile facility during the BAECC (Biogenic Aerosols – Effects on Cloud and Climate) Campaign. Two flight campaigns took place in April and August 2014 with instruments measuring the aerosol size distribution from 10 nm to 10 µm at altitudes up to 3800 m. Two case studies from the flight campaigns, when several aerosol layers were identified, were selected for further investigation: one clear sky case, and one partly cloudy case. During the clear sky case, turbulent mixing ensured low temporal and spatial variability in the measured aerosol size distribution in the boundary layer whereas mixing was not as homogeneous in the boundary layer during the partly cloudy case. The elevated layers exhibited greater temporal and spatial variability in aerosol size distribution, indicating a lack of mixing. New particle formation was observed in the boundary layer during the clear sky case, and nucleation mode particles were also seen in the elevated layers that were not mixing with the boundary layer. Interpreting local measurements of elevated layers in terms of long-range transport can be achieved using back trajectories from Lagrangian models, but care should be taken in selecting appropriate arrival heights, since the modelled and observed layer heights did not always coincide. We conclude that higher confidence in attributing elevated aerosol layers with their air mass origin is attained when back trajectories are combined with lidar and radiosonde profiles.

Prediction and observation of cloud processing of the aerosol size distribution by a band of cumulus

2006 ◽  
Vol 132 (616) ◽  
pp. 845-863 ◽  
Author(s):  
J. R. Peter ◽  
S. T. Siems ◽  
J. B. Jensen ◽  
J. L. Gras ◽  
Y. Ishizaka ◽  
...  
Keyword(s):  
Size Distribution ◽  
Aerosol Size Distribution ◽  
Cloud Processing
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