scholarly journals The importance of interstitial particle scavenging by cloud droplets in shaping the remote aerosol size distribution and global aerosol-climate effects

2015 ◽  
Vol 15 (4) ◽  
pp. 5589-5618
Author(s):  
J. R. Pierce ◽  
B. Croft ◽  
J. K. Kodros ◽  
S. D. D'Andrea ◽  
R. V. Martin

Abstract. In this paper, we investigate the coagulation of interstitial aerosol particles (particles too small to activate to cloud droplets) with cloud drops, a process often ignored in aerosol-climate models. We use the GEOS-Chem-TOMAS global chemical transport model with aerosol microphysics to calculate the changes in the aerosol size distribution, cloud-albedo aerosol indirect effect, and direct aerosol effect due to the interstitial coagulation process. We find that inclusion of interstitial coagulation in clouds lowers total particle number concentrations by 15–21% globally, where the range is due to varying assumptions regarding activation diameter, cloud droplet size, and ice cloud physics. The interstitial coagulation process lowers the concentration of particles with dry diameters larger than 80 nm (a proxy for larger CCN) by 10–12%. These 80 nm particles are not directly removed by the interstitial coagulation, but are reduced in concentration because fewer smaller particles grow to diameters larger than 80 nm. The global aerosol indirect effect of adding interstitial coagulation varies from +0.4 to +1.3 W m−2 where again the range depends on our cloud assumptions. Thus, the aerosol indirect effect of this process is significant, but the magnitude depends greatly on assumptions regarding activation diameter, cloud droplet size, and ice cloud physics. The aerosol direct effect of interstitial coagulation process is minor (<0.01 W m−2) due to the shift in the aerosol size distribution at sizes where scattering is most effective being small. We recommend that this interstitial scavenging process be considered in aerosol models when the size distribution and aerosol indirect effects are important.

2015 ◽  
Vol 15 (11) ◽  
pp. 6147-6158 ◽  
Author(s):  
J. R. Pierce ◽  
B. Croft ◽  
J. K. Kodros ◽  
S. D. D'Andrea ◽  
R. V. Martin

Abstract. In this paper, we investigate the coagulation of interstitial aerosol particles (particles too small to activate to cloud droplets) with cloud drops, a process often ignored in aerosol-climate models. We use the GEOS-Chem-TOMAS (Goddard Earth Observing System-Chemistry TwO-Moment Aerosol Sectional) global chemical transport model with aerosol microphysics to calculate the changes in the aerosol size distribution, cloud-albedo aerosol indirect effect, and direct aerosol effect due to the interstitial coagulation process. We find that inclusion of interstitial coagulation in clouds lowers total particle number concentrations by 15–21% globally, where the range is due to varying assumptions regarding activation diameter, cloud droplet size, and ice cloud physics. The interstitial coagulation process lowers the concentration of particles with dry diameters larger than 80 nm (a proxy for larger CCN) by 10–12%. These 80 nm particles are not directly removed by the interstitial coagulation but are reduced in concentration because fewer smaller particles grow to diameters larger than 80 nm. The global aerosol indirect effect of adding interstitial coagulation varies from +0.4 to +1.3 W m−2 where again the range depends on our cloud assumptions. Thus, the aerosol indirect effect of this process is significant, but the magnitude depends greatly on assumptions regarding activation diameter, cloud droplet size, and ice cloud physics. The aerosol direct effect of the interstitial coagulation process is minor (< 0.01 W m−2) due to the shift in the aerosol size distribution at sizes where scattering is most effective being small. We recommend that this interstitial scavenging process be considered in aerosol models when the size distribution and aerosol indirect effects are important.


2005 ◽  
Vol 5 (9) ◽  
pp. 2561-2570 ◽  
Author(s):  
H. Korhonen ◽  
V.-M. Kerminen ◽  
K. E. J. Lehtinen ◽  
M. Kulmala

Abstract. We investigate the influence of low size resolution, typical to sectional aerosol models in large scale applications, on cloud droplet activation and cloud processing of aerosol particles. A simplified cloud model with five approaches to determine the fraction of activated particles is compared with a detailed reference model under different atmospheric conditions. In general, activation approaches which assume a distribution profile within the critical model size sections predict the cloud droplet concentration most accurately under clean and moderately polluted conditions. In such cases, the deviation from the reference simulations is below 15% except for very low updraft velocities. In highly polluted cases, the concentration of cloud droplets is significantly overestimated due to the inability of the simplified model to account for the kinetic limitations of the droplet growth. Of the profiles examined, taking into account the local shape of the particle size distribution is the most accurate although in most cases the shape of the profile has little relevance. While the low resolution cloud model cannot reproduce the details of the out-of-the-cloud aerosol size distribution, it captures well the amount of sulphate produced in aqueous-phase reactions as well as the distribution of the sulphate between the cloud droplets. Overall, the simplified cloud model with low size resolution performs well for clean and moderately polluted regions that cover most of the Earth's surface and is therefore suitable for large scale models. It can, however, show uncertainties in areas with strong pollution from anthropogenic sources.


2005 ◽  
Vol 5 (4) ◽  
pp. 4871-4892
Author(s):  
H. Korhonen ◽  
V.-M. Kerminen ◽  
K. E. J. Lehtinen ◽  
M. Kulmala

Abstract. We investigate the influence of low size resolution, typical to sectional aerosol models in large scale applications, on cloud droplet activation and cloud processing of aerosol particles. A simplified cloud scheme with five approaches to determine the fraction of activated particles is compared with a detailed reference model under different atmospheric conditions. In general, activation approaches which assume a distribution profile within the critical model size sections predict the cloud droplet concentration most accurately under clean and moderately polluted conditions. In such cases, the deviation from the reference simulations is below 15% except for very low updraft velocities. In highly polluted cases, the concentration of cloud droplets is significantly overestimated due to the inability of the simplified scheme to account for the kinetic limitations of the droplet growth. Of the profiles examined, taking into account the local shape of the particle size distribution is the most accurate although in most cases the shape of the profile has little relevance. While the low resolution cloud model cannot reproduce the details of the out-of-the-cloud aerosol size distribution, it captures well the amount of sulphate produced in aqueous-phase reactions as well as the distribution of the sulphate between the cloud droplets. Overall, the simplified cloud scheme with low size resolution performs well for clean and moderately polluted regions that cover most of the Earth's surface and is therefore suitable for large scale models.


2014 ◽  
Vol 14 (13) ◽  
pp. 18943-18960 ◽  
Author(s):  
S. Li ◽  
E. Joseph ◽  
Q. Min ◽  
B. Yin

Abstract. Long-term ground-based observations (2006 to 2010) of aerosol and cloud properties derived from passive radiometric sensors deployed at an atmospheric measurement field station in the Baltimore–Washington corridor operated by Howard University were used to examine aerosol indirect effect on cloud optical depth (COD), liquid water path (LWP), cloud droplets effective radius (Re) and cloud droplets number concentration (Nd). A higher frequency of clouds with large COD (> 20) and small Re (< 7 m) was found during summer of 2006 and 2007 along with higher frequency of abundant aerosol loading. The five-year data are screened for summer months only and are separated into clean and polluted cases based on aerosol particulate matter with aerodynamic diameter ≤ 2.5 m (PM2.5) value. Evidence of aerosol indirect effect is found where for polluted cases the mean and median values of COD and Nd distributions were elevated while the mean and median values of Re were decreased. Further reinforcing this conclusion is the result that the mean and median values of LWP distributions did not show prominent difference between clean and polluted cases, this implies that differences between the two cases of influential factors on cloud properties were relatively controlled. Moreover aerosol indirect effects were found insignificant when LWP was small but significant when LWP was large through the analysis of sensitivity of Nd to LWP under different aerosol loading and the measurements of aerosol size distribution.


2004 ◽  
Vol 4 (5) ◽  
pp. 1255-1263 ◽  
Author(s):  
B. Mayer ◽  
M. Schröder ◽  
R. Preusker ◽  
L. Schüller

Abstract. Cloud single scattering properties are mainly determined by the effective radius of the droplet size distribution. There are only few exceptions where the shape of the size distribution affects the optical properties, in particular the rainbow and the glory directions of the scattering phase function. Using observations by the Compact Airborne Spectrographic Imager (CASI) in 180° backscatter geometry, we found that high angular resolution aircraft observations of the glory provide unique new information which is not available from traditional remote sensing techniques: Using only one single wavelength, 753nm, we were able to determine not only optical thickness and effective radius, but also the width of the size distribution at cloud top. Applying this novel technique to the ACE-2 CLOUDYCOLUMN experiment, we found that the size distributions were much narrower than usually assumed in radiation calculations which is in agreement with in-situ observations during this campaign. While the shape of the size distribution has only little relevance for the radiative properties of clouds, it is extremely important for understanding their formation and evolution.


2012 ◽  
Vol 5 (9) ◽  
pp. 2237-2260 ◽  
Author(s):  
J. K. Spiegel ◽  
P. Zieger ◽  
N. Bukowiecki ◽  
E. Hammer ◽  
E. Weingartner ◽  
...  

Abstract. Droplet size spectra measurements are crucial to obtain a quantitative microphysical description of clouds and fog. However, cloud droplet size measurements are subject to various uncertainties. This work focuses on the error analysis of two key measurement uncertainties arising during cloud droplet size measurements with a conventional droplet size spectrometer (FM-100): first, we addressed the precision with which droplets can be sized with the FM-100 on the basis of the Mie theory. We deduced error assumptions and proposed a new method on how to correct measured size distributions for these errors by redistributing the measured droplet size distribution using a stochastic approach. Second, based on a literature study, we summarized corrections for particle losses during sampling with the FM-100. We applied both corrections to cloud droplet size spectra measured at the high alpine site Jungfraujoch for a temperature range from 0 °C to 11 °C. We showed that Mie scattering led to spikes in the droplet size distributions using the default sizing procedure, while the new stochastic approach reproduced the ambient size distribution adequately. A detailed analysis of the FM-100 sampling efficiency revealed that particle losses were typically below 10% for droplet diameters up to 10 μm. For larger droplets, particle losses can increase up to 90% for the largest droplets of 50 μm at ambient wind speeds below 4.4 m s−1 and even to >90% for larger angles between the instrument orientation and the wind vector (sampling angle) at higher wind speeds. Comparisons of the FM-100 to other reference instruments revealed that the total liquid water content (LWC) measured by the FM-100 was more sensitive to particle losses than to re-sizing based on Mie scattering, while the total number concentration was only marginally influenced by particle losses. Consequently, for further LWC measurements with the FM-100 we strongly recommend to consider (1) the error arising due to Mie scattering, and (2) the particle losses, especially for larger droplets depending on the set-up and wind conditions.


2009 ◽  
Vol 9 (1) ◽  
pp. 3207-3241 ◽  
Author(s):  
K. J. Pringle ◽  
K. S. Carslaw ◽  
D. V. Spracklen ◽  
G. M. Mann ◽  
M. P. Chipperfield

Abstract. Empirical relationships that link cloud droplet number (CDN) to aerosol number or mass are commonly used to calculate global fields of CDN for climate forcing assessments. In this work we use a sectional global model of sulfate and sea-salt aerosol coupled to a mechanistic aerosol activation scheme to explore the limitations of this approach. We find that a given aerosol number concentration produces a wide range of CDN concentrations due to variations in the shape of the aerosol size distribution. On a global scale, the dependence of CDN on the size distribution results in regional biases in predicted CDN (for a given aerosol number). Empirical relationships between aerosol number and CDN are often derived from regional data but applied to the entire globe. In an analogous process, we derive regional "correlation-relations" between aerosol number and CDN and apply these regional relations to calculations of CDN on the global scale. The global mean percentage error in CDN caused by using regionally derived CDN-aerosol relations is 20 to 26%, which is about half the global mean percentage change in CDN caused by doubling the updraft velocity. However, the error is as much as 25–75% in the Southern Ocean, the Arctic and regions of persistent stratocumulus when an aerosol-CDN correlation relation from the North Atlantic is used. These regions produce much higher CDN concentrations (for a given aerosol number) than predicted by the globally uniform empirical relations. CDN-aerosol number relations from different regions also show very different sensitivity to changing aerosol. The magnitude of the rate of change of CDN with particle number, a measure of the aerosol efficacy, varies by a factor 4. CDN in cloud processed regions of persistent stratocumulus is particularly sensitive to changing aerosol number. It is therefore likely that the indirect effect will be underestimated in these important regions.


2016 ◽  
Vol 113 (50) ◽  
pp. 14243-14248 ◽  
Author(s):  
Kamal Kant Chandrakar ◽  
Will Cantrell ◽  
Kelken Chang ◽  
David Ciochetto ◽  
Dennis Niedermeier ◽  
...  

The influence of aerosol concentration on the cloud-droplet size distribution is investigated in a laboratory chamber that enables turbulent cloud formation through moist convection. The experiments allow steady-state microphysics to be achieved, with aerosol input balanced by cloud-droplet growth and fallout. As aerosol concentration is increased, the cloud-droplet mean diameter decreases, as expected, but the width of the size distribution also decreases sharply. The aerosol input allows for cloud generation in the limiting regimes of fast microphysics (τc<τt) for high aerosol concentration, and slow microphysics (τc>τt) for low aerosol concentration; here, τc is the phase-relaxation time and τt is the turbulence-correlation time. The increase in the width of the droplet size distribution for the low aerosol limit is consistent with larger variability of supersaturation due to the slow microphysical response. A stochastic differential equation for supersaturation predicts that the standard deviation of the squared droplet radius should increase linearly with a system time scale defined as τs−1=τc−1+τt−1, and the measurements are in excellent agreement with this finding. The result underscores the importance of droplet size dispersion for aerosol indirect effects: increasing aerosol concentration changes the albedo and suppresses precipitation formation not only through reduction of the mean droplet diameter but also by narrowing of the droplet size distribution due to reduced supersaturation fluctuations. Supersaturation fluctuations in the low aerosol/slow microphysics limit are likely of leading importance for precipitation formation.


2009 ◽  
Vol 23 (28n29) ◽  
pp. 5434-5443 ◽  
Author(s):  
ANTONIO CELANI ◽  
ANDREA MAZZINO ◽  
MARCO TIZZI

A new model to study the effect of turbulence on the cloud droplets in the condensation phase is proposed and its behavior investigated by direct numerical simulations. The model is a generalization of the one by Celani, Mazzino, Tizzi, New J. Phys.10, 075021 (2008), where the droplet feedback on vapor is now explicitly taken into account. Physically, it amounts to considering the fact that when a cloud droplet increases its size, vapor is subtracted from the ambient with the net result of a local reduction in the supersaturation field. It is shown how this effect plays to reduce the broadening of droplet size spectra in the condensation stage and thus to produce results in closer agreement with observations.


2018 ◽  
Vol 11 (6) ◽  
pp. 3627-3643 ◽  
Author(s):  
Céline Cornet ◽  
Laurent C.-Labonnote ◽  
Fabien Waquet ◽  
Frédéric Szczap ◽  
Lucia Deaconu ◽  
...  

Abstract. Simulations of total and polarized cloud reflectance angular signatures such as the ones measured by the multi-angular and polarized radiometer POLDER3/PARASOL are used to evaluate cloud heterogeneity effects on cloud parameter retrievals. Effects on optical thickness, albedo, effective radius and variance of the cloud droplet size distribution and aerosol parameters above cloud are analyzed. Three different clouds that have the same mean optical thicknesses were generated: the first with a flat top, the second with a bumpy top and the last with a fractional cloud cover. At small scale (50 m), for oblique solar incidence, the illumination effects lead to higher total but also polarized reflectances. The polarized reflectances even reach values that cannot be predicted by the 1-D homogeneous cloud assumption. At the POLDER scale (7 km × 7 km), the angular signature is modified by a combination of the plane–parallel bias and the shadowing and illumination effects. In order to quantify effects of cloud heterogeneity on operational products, we ran the POLDER operational algorithms on the simulated reflectances to retrieve the cloud optical thickness and albedo. Results show that the cloud optical thickness is greatly affected: biases can reach up to −70, −50 or +40 % for backward, nadir and forward viewing directions, respectively. Concerning the albedo of the cloudy scenes, the errors are smaller, between −4.7 % for solar incidence angle of 20∘ and up to about +8 % for solar incidence angle of 60∘. We also tested the heterogeneity effects on new algorithms that allow retrieving cloud droplet size distribution and cloud top pressures and also aerosol above clouds. Contrary to the bi-spectral method, the retrieved cloud droplet size parameters are not significantly affected by the cloud heterogeneity, which proves to be a great advantage of using polarized measurements. However, the cloud top pressure obtained from molecular scattering in the forward direction can be biased up to about 60 hPa (around 550 m). Concerning the aerosol optical thickness (AOT) above cloud, the results are different depending on the available angular information. Above the fractional cloud, when only side scattering angles between 100 and 130∘ are available, the AOT is underestimated because of the plane–parallel bias. However, for solar zenith angle of 60∘ it is overestimated because the polarized reflectances are increased in forward directions.


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