scholarly journals A simple analytical model of aerosol properties with account for hygroscopic growth: 1. Equilibrium size spectra and cloud condensation nuclei activity spectra

1999 ◽  
Vol 104 (D2) ◽  
pp. 2175-2184 ◽  
Author(s):  
Vitaly I. Khvorostyanov ◽  
Judith A. Curry
2011 ◽  
Vol 11 (24) ◽  
pp. 12627-12645 ◽  
Author(s):  
J. H. Kim ◽  
S. S. Yum ◽  
S. Shim ◽  
S.-C. Yoon ◽  
J. G. Hudson ◽  
...  

Abstract. Aerosol size distribution, total concentration (i.e. condensation nuclei (CN) concentration, NCN), cloud condensation nuclei (CCN) concentration (NCCN), hygroscopicity at ~90% relative humidity (RH) were measured at a background monitoring site at Gosan, Jeju Island, south of the Korean Peninsula in August 2006, April to May 2007 and August to October 2008. Similar measurements took place in August 2009 at another background site (Baengnyeongdo Comprehensive Monitoring Observatory, BCMO) on the island of Baengnyeongdo, off the west coast of the Korean Peninsula. Both islands were found to be influenced by continental sources regardless of season and year. Average values for all of the measured NCCN at 0.2, 0.6 and 1.0% supersaturations (S), NCN, and geometric mean diameter (Dg) from both islands were in the range of 1043–3051 cm−3, 2076–4360 cm−3, 2713–4694 cm−3, 3890–5117 cm−3 and 81–98 nm, respectively. Although the differences in Dg and NCN were small between Gosan and BCMO, NCCN at various S was much higher at the latter, which is closer to China. Most of the aerosols were internally mixed and no notable differences in hygroscopicity were found between the days of strong pollution influence and the non-pollution days for both islands. During the 2008 and 2009 campaigns, critical supersaturation for CCN nucleation (Sc) for selected particle sizes was measured. Particles of 100 nm diameters had mean Sc of 0.19 ± 0.02% during 2008 and those of 81 and 110 nm diameters had mean Sc of 0.26 ± 0.07% and 0.17 ± 0.04%, respectively, during 2009. The values of the hygroscopicity parameter (κ), estimated from measured Sc, were mostly higher than the κ values obtained from the measured hygroscopic growth at ~90% RH. For the 2008 campaign, NCCN at 0.2, 0.6 and 1.0% S were predicted based on measured dry particle size distributions and various ways of representing particle hygroscopicity. The best closure was obtained when temporally varying and size-resolved hygroscopicity information from the HTDMA was used, for which the average relative deviations from the measured values were 28 ± 20% for 0.2% S (mostly under-prediction), 25 ± 52% for 0.6% (balanced between over- and under-prediction) and 19 ± 15% for 1.0% S (balanced). Prescribing a constant hygroscopicity parameter suggested in the literature (κ = 0.3) for all sizes and times resulted in average relative deviations of 28–41% where over-prediction was dominant. When constant hygroscopicity was assumed, the relative deviation tended to increase with decreasing NCCN, which was accompanied by an increase of the sub-100 nm fraction. These results suggest that hygroscopicity information for particles of diameters smaller than 100 nm is crucial for more accurate predictions of NCCN. For confirmation when κ = 0.17, the average κ for sub-100 nm particles in this study, was applied for sub-100 nm and κ = 0.3 for all other sizes, the CCN closure became significantly better than that with κ = 0.3 for all sizes.


2020 ◽  
Author(s):  
Patricia Quinn ◽  
Tim Bates ◽  
Eric Saltzman ◽  
Tom Bell ◽  
Mike Behrenfeld

<p>The emission of sea spray aerosol (SSA) and dimethylsulfide (DMS) from the ocean results in marine boundary layer aerosol particles that can impact Earth’s radiation balance by directly scattering solar radiation and by acting as cloud condensation nuclei (CCN), thereby altering cloud properties. The surface ocean is projected to warm by 1.3 to 2.8°C globally over the 21<sup>st</sup> century. Impacts of this warming on plankton blooms, ocean ecosystems, and ocean-to-atmosphere fluxes of aerosols and their precursor gases are highly uncertain. A fundamental understanding of linkages between surface ocean ecosystems and ocean-derived aerosols is required to address this uncertainty. One approach for improved understandings of these linkages is simultaneous measurements of relevant surface ocean and aerosol properties in an ocean region with seasonally varying plankton blooms and a minimally polluted overlying atmosphere. The western North Atlantic hosts the largest annual phytoplankton bloom in the global ocean with a large spatial and seasonal variability in plankton biomass and composition. Periods of low aerosol number concentrations associated with unpolluted air masses allow for the detection of linkages between ocean ecosystems and ocean-derived aerosol.</p><p> </p><p>Five experiments were conducted in the western North Atlantic between 2014 and 2018 with the objective of finding links between the bloom and marine aerosols. These experiments include the second Western Atlantic Climate Study (WACS-2) and four North Atlantic Aerosol and Marine Ecosystem Study (NAAMES) cruises. This series of cruises was the first time the western North Atlantic bloom was systematically sampled during every season with extensive ocean and atmosphere measurements able to assess how changes in the state of the bloom might impact ocean-derived aerosol properties. Measurements of unheated and heated number size distributions, cloud condensation nuclei (CCN) concentrations, and aerosol composition were used to identify primary and secondary aerosol components that could be related to the state of the bloom. Only periods of clean marine air, as defined by radon, particle number concentration, aerosol light absorption coefficient, and back trajectories, were included in the analysis.</p><p> </p><p>CCN concentrations at 0.1% supersaturation were best correlated (r<sup>2</sup> = 0.73) with accumulation mode nss SO<sub>4</sub><sup>=</sup>. Sea spray aerosol (SSA) was only correlated with CCN during November when bloom accumulation had not yet occurred and dimethylsulfide (DMS) concentrations were at a minimum. The fraction of CCN attributable to SSA was less than 20% during March, May/June, and September, indicating the limited contribution of SSA to the CCN population of the western North Atlantic atmosphere. The strongest link between the plankton bloom and aerosol and cloud properties appears to be due to biogenic non-seasalt SO<sub>4</sub><sup>=</sup>.</p><p> </p>


2020 ◽  
Author(s):  
Tim Bates ◽  
Patricia Quinn

<p>The fair-weather cumulus clouds, that cover much of the low-latitude oceans, affect the radiation balance of the planet by reflecting incoming solar radiation and absorbing outgoing longwave radiation.  These clouds also drive atmospheric circulation by mixing the lower atmosphere in a process called shallow convection.  This mixing, in turn, affects sea surface temperature and salinity by moderating the air-sea exchange of energy and moisture.  Marine boundary layer (MBL) atmospheric aerosols play a role in the processes described above by scattering and absorbing solar radiation and by serving as cloud condensation nuclei (CCN) thereby influencing cloud droplet concentrations and size; the extent, lifetime, and albedo of clouds; and the frequency and intensity of precipitation. Quantifying the role of aerosols over the Northwest Tropical Atlantic is critical to advance understanding of shallow convection and air-sea interactions.</p><p>MBL aerosol properties were measured aboard the RV Ronald H. Brown during the EUREC4A and ATOMIC field studies in January/February 2020.  Aerosols encountered during the study include background sulfate/sea spray particles and African dust/biomass burning particles.  Aerosol physical, chemical, optical and cloud condensation nuclei properties will be presented and their interaction with local and regional circulation.</p>


2005 ◽  
Vol 5 (12) ◽  
pp. 3233-3250 ◽  
Author(s):  
D. V. Spracklen ◽  
K. J. Pringle ◽  
K. S. Carslaw ◽  
M. P. Chipperfield ◽  
G. W. Mann

Abstract. We use the new GLOMAP model of global aerosol microphysics to investigate the sensitivity of modelled sulfate and sea salt aerosol properties to uncertainties in the driving microphysical processes and compare these uncertainties with those associated with aerosol and precursor gas emissions. Overall, we conclude that uncertainties in microphysical processes have a larger effect on global sulfate and sea salt derived condensation nuclei (CN) and cloud condensation nuclei (CCN) concentrations than uncertainties in present-day sulfur emissions. Our simulations suggest that uncertainties in predicted sulfate and sea salt CCN abundances due to poorly constrained microphysical processes are likely to be of a similar magnitude to long-term changes in sulfate and sea salt CCN due to changes in anthropogenic emissions. A microphysical treatment of the global sulfate aerosol allows the uncertainty in climate-relevant aerosol properties to be attributed to specific processes in a way that has not been possible with simpler aerosol schemes. In particular we conclude that: (1) changes in the binary H2SO4-H2O nucleation rate and condensation rate of gaseous H2SO4 cause a shift in the vertical location of the upper tropospheric CN layer by as much as 3 km, while the shape of the CN profile is essentially pre-served (2) uncertainties in the binary H2SO4-H2O nucleation rate have a relatively insignificant effect on marine boundary layer (MBL) aerosol properties; (3) emitting a fraction of anthropogenic SO2 as particulates (to represent production of sulfate particles in power plant plumes below the scale of the model grid (which is of the order of 300 km)) has the potential to change the global mean MBL sulfate-derived CN concentrations by up to 72%, and changes of up to a factor 20 can occur in polluted continental regions; (4) predicted global mean MBL sulfate and sea salt CCN concentrations change by 10 to 60% when several microphysical processes are changed within reasonable uncertainty ranges; (5) sulfate and sea salt derived CCN concentrations are particularly sensitive to primary particle emissions, with global mean MBL sulfate and sea salt CCN changing by up to 27% and local concentrations over continental regions changing by more than 100% when the percentage of anthropogenic SO2 emitted as particulates is changed from 0 to 5%; (6) large changes in sea spray flux have insignificant effects on global sulfate aerosol except when the mass accommodation coefficient of sulfuric acid on the salt particles is set unrealistically low.


2004 ◽  
Vol 4 (8) ◽  
pp. 2119-2143 ◽  
Author(s):  
J. Rissler ◽  
E. Swietlicki ◽  
J. Zhou ◽  
G. Roberts ◽  
M. O. Andreae ◽  
...  

Abstract. Sub-micrometer atmospheric aerosol particles were studied in the Amazon region, 125 km northeast of Manaus, Brazil (-1°55.2'S, 59°28.1'W). The measurements were performed during the wet-to-dry transition period, 4-28 July 2001 as part of the LBA (Large-Scale Biosphere Atmosphere Experiment in Amazonia) CLAIRE-2001 (Cooperative LBA Airborne Regional Experiment) experiment. The number size distribution was measured with two parallel differential mobility analyzers, the hygroscopic growth at 90% RH with a Hygroscopic Tandem Mobility Analyzer (H-TDMA) and the concentrations of cloud condensation nuclei (CCN) with a cloud condensation nuclei counter. A model was developed that uses the H-TDMA data to predict the number of soluble molecules or ions in the individual particles and the corresponding minimum particle diameter for activation into a cloud droplet at a certain supersaturation. Integrating the number size distribution above this diameter, CCN concentrations were predicted with a time resolution of 10 min and compared to the measured concentrations. During the study period, three different air masses were identified and compared: clean background, air influenced by aged biomass burning, and moderately polluted air from recent local biomass burning. For the clean period 2001, similar number size distributions and hygroscopic behavior were observed as during the wet season at the same site in 1998, with mostly internally mixed particles of low diameter growth factor (~1.3 taken from dry to 90% RH). During the periods influenced by biomass burning the hygroscopic growth changed slightly, but the largest difference was seen in the number size distribution. The CCN model was found to be successful in predicting the measured CCN concentrations, typically within 25%. A sensitivity study showed relatively small dependence on the assumption of which model salt that was used to predict CCN concentrations from H-TDMA data. One strength of using H-TDMA data to predict CCN concentrations is that the model can also take into account soluble organic compounds, insofar as they go into solution at 90% RH. Another advantage is the higher time resolution compared to using size-resolved chemical composition data.


2011 ◽  
Vol 11 (7) ◽  
pp. 19683-19727 ◽  
Author(s):  
J. H. Kim ◽  
S. S. Yum ◽  
S. Shim ◽  
S.-C. Yoon ◽  
J. G. Hudson ◽  
...  

Abstract. Aerosol size distribution, total concentration (i.e., condensation nuclei (CN) concentration, NCN), cloud condensation nuclei (CCN) concentration (NCCN), hygroscopicity at ~90 % relative humidity (RH) were measured at a background monitoring site at Gosan, Jeju Island, south of the Korea Peninsula in August 2006, April to May 2007 and August to October 2008. Similar measurement took place in August 2009 at another background site (Baengnyeongdo Comprehensive Monitoring Observatory, BCMO) on the island of Baengnyeongdo, off the west coast of the Korean Peninsula. Both islands were found to be influenced by continental sources regardless of season and year. Average values for all of the measured NCCN at 0.2, 0.6 and 1.0 % supersaturations (S), NCN, and geometric mean diameter (Dg) from both islands were in the range of 1043–3051 cm−3, 2076–4360 cm−3, 2713–4694 cm−3, 3890–5117 cm−3 and 81–98 nm, respectively. Although the differences in Dg and NCN were small between Gosan and BCMO, NCCN at various S was much higher at the latter, which is closer to China. Most of the aerosols were internally mixed and no notable differences in hygroscopicity were found between the days of strong pollution influence and the non-pollution days for both islands. During the 2008 and 2009 campaigns, critical supersaturation for cloud nucleation (Sc) for selected particle sizes was measured. Particles of 100 nm diameters had mean Sc of 0.19 ± 0.02 % during 2008 and those of 81 and 110 nm diameters had mean Sc of 0.26 ± 0.07 % and 0.17 ± 0.04 %, respectively, during 2009. Hygroscopicity parameters estimated from the measured Sc were mostly higher than the ones from the measured hygroscopic growth at ~90 % RH. For the 2008 campaign, NCCN at 0.2, 0.6 and 1.0 % S were predicted based on the measured dry particle size distribution and various ways of representing aerosol hygroscopicity. The best closure was obtained when temporally varying and size-resolved hygroscopicity information from HTDMA was used, for which the average relative deviations from the measured values were 19 % for 1.0 % S and 28 % for 0.2 % S. Prescribing a constant hygroscopicity parameter suggested in literature (κ = 0.3) for all sizes and time resulted in the average relative deviations, 25–40 %. When constant hygroscopicity was assumed, the relative deviation tended to increase with decreasing NCCN, which was accompanied by increase of sub-100 nm fraction. These results suggest that hygroscopicity information for aerosols of diameters smaller than 100 nm is crucial for more accurate prediction of NCCN.


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