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Model test of CCN-cloud albedo climate forcing

Cloud condensation nuclei (CCN) influence cloud albedo through their effect on the cloud droplet size distribution. A number of studies have evaluated the climatic impact of the CCN-cloud albedo feedback, but all have assumed that cloud distributions, cloud thicknesses, and cloud liquid water contents would remain constant as the climate adjusted. This assumption has been tested using the Livermore version of the National Center for Atmospheric Research Community Climate Model. The results indicate that there are no significant compensating changes in cloud properties that would counteract the 1.7 percent global albedo increase resulting from a fourfold increase in marine CCN concentration. Furthermore, when ocean surface temperatures are decreased 4 C in a manner broadly consistent with the enhanced cloud albedos, an increase in cloud fraction of 3.5 percent and a reduction in cloud altitude are predicted, leading to a positive feedback from clouds that would imply a climate impact roughly double that calculated from cloud droplet size distribution change alone.

Ghan, S. J.

Stratospheric CCN sampling program

Two one liter grab samples of stratospheric aerosol were returned from each of six U-2 sampling missions. Cloud condensation nuclei (CCN) spectra from each sample were obtained. Interest was centered on the effects of volcanic activity. Spurious particle generation was found to be a serious problem in container 9 LFT and a much smaller problem in container 9 RT. Initial studies of an option for improved sample containers and values were completed. A CCN spectrometer, able to operate at an internal pressure of 300 mb, was designed.

Rogers, C. F.

The CCN counter of the IOPG of Puy de Dome: Main characterisics and results of measurements

In performing the data analysis of the measurements achieved during the Workshop with the device, a global approach was preferred rather than an individual analysis, in order to illustrate some main characteristics in the behavior of the device with respect to a mean behavior resulting from a general survey of all the equipments involved in each experiment. The device tends generally to overestimate the CCN concentrations measured near the high supersaturations and sometimes underestimates the concentrations close to 0.1% or 0.2% of supersaturation. Despite the fact that it belongs to a type of static diffusion chamber, it shows, however, similar spectra to those obtained with other types of chambers (continuous flow diffusion chamber and haze chamber).

Serpolay, R.

A description of the UK Meteorological Office CCN counter

The chamber is a thermal gradient diffusion type with the upper plate at room temperature and the lower plate thermoelectrically cooled. The light from a 25W projector bulb is focused in a beam of approximations 1x3 mm in the central part of the chamber. The light scattered by drops is viewed in the forward direction (40 deg) by a microscope and a sensitive photodetector. Experiments were performed to relate the peak output from the photocell with the maximum number of drops in the beam recorded photographically. The microscope is used to check the calibration at low concentrations of CCN. The results of the experiments and the performance of the counter are reported.

Kitchen, M.

CCN comparisons of static diffusion chambers

Nine CCN counters of the static diffusion (SDC) type were compared with one another and with continuous flow diffusion (CFD) chambers. The nine SDCs showed a considerable amount of variation, largely attributable to newness and/or lack of prior calibration of some units. The five more consistent instruments agreed quite well, to within at least 20 percent of the NRL mobility analyzer and to within 10 percent at 1 percent supersaturation. There was satisfactory agreement between the more reliable SDC and CFD chambers.

Jiusto, J. E.

UMR dual mode CCN counter (modes: CFD plus haze)

The chamber consists of two vertical plates 100 cm long in the vertical direction and 13 cm wide, with a 0.8 cm spacing between the plates. The haze mode is used for the nuclei active at supersaturations (S) from 0.0133 to 0.173%. In this mode the two plates are kept at the same temperature (25 C). In the CFD mode the supersaturation is determined by the temperature difference between the two plates. About 40 minutes is required to obtain a spectrum (5 values of S in the CFD mode, plus 7 values of S in the haze mode). About half of this time is used to adjust the temperatures and flows; the rest is used in actual counting of the nuclei. Comparisons of the counter to other types of counters are reported.

Alofs, D. J.

An automatic light scattering CCN counter

The counter is a static thermal diffusion chamber which has been modified to include an optical system for the determination of droplet concentration by the measurement of scattered light. The determination of concentration is made by measurement of the peak scattered light signal from the cloud of growing droplets which is a function of both the droplet concentration and chamber supersaturation. Because the formation of the peak is related to the rate of growth of the droplets and sedimentation, both of which are determined by supersaturation, the system calibration can be uniquely determined by comparison with an absolute counter such as a static diffusion chamber with a photographic recording system.

Lala, G. G.

Numerical case study of the aerosol–cloud interactions in warm boundary layer clouds over the eastern North Atlantic with an interactive chemistry module

The presence of warm boundary layer stratiform clouds over the eastern North Atlantic (ENA) region is commonly influenced by the Azores High, especially during the summer season. To investigate comprehensive aerosol–cloud interactions, this study employs the Weather Research and Forecasting model coupled with a chemistry component (WRF-Chem), incorporating aerosol chemical components that are relevant to the formation of cloud condensation nuclei (CCN) and accounting for aerosol spatiotemporal variation. This study focuses on aerosol indirect effects, particularly the long-range transport of aerosols, in the ENA region under three different weather regimes: a ridge with a surface high-pressure system, a post-trough with a surface high-pressure system, and a weak trough. The WRF-Chem simulations conducted at a near-large-eddy scale offer valuable insights into the model's performance, especially in terms of its ability to use high spatial resolution to capture mesoscale cloud features across various weather regimes. Our result shows that introducing 5 times more aerosols to either non-precipitating or precipitating clouds significantly increases ambient CCN numbers, resulting in, to varying degrees, higher liquid water path (LWP) values. The substantial aerosol–cloud interaction especially occurs in the precipitating clouds and demonstrates the susceptibility of the LWP to changes in CCN under different regimes. Conversely, thin, non-rain clouds at the edges of a cloud system are prone to evaporation, exhibiting an aerosol drying effect. The aerosols released during this process transition back to the accumulation mode, facilitating future activation. This dynamic behavior is not adequately represented in prescribed-aerosol simulations.

54 ENVIRONMENTAL SCIENCES

A Study of Direct and Cloud-Mediated Radiative Forcing of Climate Due to Aerosols

The Intergovernmental Panel on Climate Change (IPCC) has reported that in the southeastern US and eastern China, the general greenhouse warming due to anthropogenic gaseous emissions is dominated by the cooling effect of anthropogenic aerosols. To verify this model prediction in eastern China and southeastern US, we analyzed regional patterns of climate changes at 72 stations in eastern China during 1951- 94 (44 years), and at 52 stations in the southeastern US during 1949-94 (46 years) to detect the fingerprint of aerosol radiative forcing. It was found that the mean rates of change of annual mean daily, maximum, minimum temperatures and diurnal temperature range (DTR) in eastern China were 0.8, -0.2, 1.8, and -2.0 C/100 years respectively, while the mean rates of change of annual mean daily, maximum, minimum temperatures and DTR in the southeastern US were -0.2, -0.6, 0.2, and -0.8 C/100 years, respectively. This indicates that the high rate of increase in annual mean minimum temperature in eastern China results in a slightly warming trend of daily temperature, while the high rate of decrease in annual mean maximum temperature and low rate of increase in annual mean minimum temperature lead to the cooling trend of daily temperature in the southeastern US. We found that the warming from the longwave forcing due to both greenhouse gases and aerosols was completely counteracted by the shortwave aerosol forcing in the southeastern US in the past 46 years. A slightly overall warming trend in eastern China is evident; winters have become milder. This finding is explained by hypothesizing that increasing energy usage during the past 44 years has resulted in more coal and biomass burning, thus increasing the emission of absorbing soot and organic aerosols in eastern China. Such emissions, in addition to well-known Asia dust and greenhouse gases, may be responsible for the winter warming trend in eastern China that we have reported here. The sensitivity of aerosol radiative properties to aerosol composition, size distribution, relative humidity (RH) is examined for the following aerosol systems: inorganic and organic ions (Cl-, Br-, NO3 -, SO4 2-, Na+, NH4 +, K+, Ca2+, Mg2+, HCOO-, CH3COO-, CH3CH2COO-, CH3COCOO-, OOCCOO2-, MSA-1); water-insoluble inorganic and organic compounds (elemental carbon, n-alkanes, SiO2, Al2O3, Fe2O3 and other organic compounds). The partial molar refraction method was used to calculate the real part of the refractive index. It was found that the asymmetry factor increased by approximately 48% with the real part varying from 1.40 to 1.65, and the single scattering albedo decreased by 24% with the imaginary part varying from -0.005 to -0.1. The asymmetry factor increased by 5.4 times with the geometric standard deviation varying from 1.2 to 3.0. The radiation transmission is very sensitive to the change in size distribution; other factors are not as significant. To determine the aerosol direct radiative forcing (ADRF), the aerosol optical depth (AOD) values at the three operational wavelengths (415, 500 and 673 nm) were determined at a regionally representative site, namely, Mt. Gibbs (35.78 deg N, 82.29 deg W, elevation 2006 m) in Mt. Mitchell State Park, NC, and a site located in an adjacent valley (Black Mountain, 35.66 deg N, 82.38 deg W, elevation 951 m) in the southeastern US. The two sites are separated horizontally by 10 km and vertically by 1 km. It was found that the representative total AOD values at 500 nm at the valley site for highly polluted (HP), marine (M) and continental (C) air masses were 0.68 +/- 0.33, 0.29 +/- 0.19 and 0.10 +/- 0.04, respectively. A search-graph method was used to retrieve the columnar size distribution (number concentration N, effective radius reff and geometric standard deviation=?g) from the optical depth observations at three operational wavelengths. The ground albedo, single scattering albedo and imaginary part of the refractive index were calculated using a mathematically unique procedure involving a Mie code and a radiative transfer code in conjunction with the retrieved aerosol size distribution, AOD, and diffuse-direct irradiance ratio. It was found that N, r(eff) and sigma(g) were in the ranges of 10 to 1.7 x 10(exp 4)/cubic cm, 0.09 to 0.68 micrometers and 1.12 to 2.95, respectively. The asymmetry factor and single scattering albedo were in the ranges of 0.63 to 0.75 and 0.74 to 0.97 respectively. The ground albedo for the forested terrain and imaginary part of refractive index were found to be in the ranges of 0.06 to 0.29 and 0.005 to 0.051 respectively. On the basis of these aerosol radiative properties obtained at the research sites and computations using the Column Radiation Model (CRM) of National Center of Atmospheric Research (NCAR) Community Climate Model (CCM3), it was found that the average cloud-free 24-hour ADRF values were -13 +/- 8, -8 +/- 3, -33 +/- 16 W/square m for marine, continental, and polluted air masses, respectively. On the assumption that the fractional coverage of clouds is 0.61, it was estimated that the annual mean ADRF was 7 +/- 2 W/square m in the southeastern US. The review with respect to the current knowledge of organic acids shows that aerosol formate and acetate concentrations range from 0.02 to 5.3 nmol/cubic m and from 0.03 to 12.4 nmol/cubic m respectively, and that between 34% to 77% of formate and between 21% to 66% of acetate are present in the fine fraction of aerosols. It was found that although most (98-99%) of these volatile organic acids were present in the gas phase, their concentrations in the aerosol particles were sufficient to make them a good candidate for cloud condensation nuclei (CCN). It is hypothesized that organic acids are at least one of the primary sources of CCN in the atmosphere due to their ubiquitous presence in the troposphere, especially over the continental forested areas. The results of our measurements at Palmer Station, Antarctica show that the daily average CCN concentrations at 0.3% and 1% supersaturations ranged from 0.3 to 160/cubic cm and from 4 to 168/cubic cm, respectively, during the period from 17 January to 26 February, 1994. New evidence for substantial and definitive CCN enhancement near and within cloud has been observed at Mt. Mitchell, North Carolina. The results show that the average monthly CCN concentrations were 460 +/- 217, 386 +/- 286, 429 +/- 228 and 238 +/- 134/cubic cm for in-cloud, overcast, clear and rainy conditions, respectively. The typical CCN spectra show that there were a lot of small CCN produced and the ion concentrations (especially H+ and SO4 2-) were very high during the CCN enhancement period. The significantly positive correlation between black carbon (BC) and CCN at 1% supersaturation indicates that a percentage of the BC measured at the site may be in the form of an internal mixture and participated in the formation of CCN.

Yu, Shao-Cai

Evaluation of Global Simulations of Aerosol Particle and Cloud Condensation Nuclei Number, with Implications for Cloud Droplet Formation

A total of 16 global chemistry transport models and general circulation models have participated in this study; 14 models have been evaluated with regard to their ability to reproduce the near-surface observed number concentration of aerosol particles and cloud condensation nuclei (CCN), as well as derived cloud droplet number concentration (CDNC). Model results for the period 2011-2015 are compared with aerosol measurements (aerosol particle number, CCN and aerosol particle composition in the submicron fraction) from nine surface stations located in Europe and Japan. The evaluation focuses on the ability of models to simulate the average across time state in diverse environments and on the seasonal and short-term variability in the aerosol properties. There is no single model that systematically performs best across all environments represented by the observations. Models tend to underestimate the observed aerosol particle and CCN number concentrations, with average normalized mean bias (NMB) of all models and for all stations, where data are available, of -24% and -35% for particles with dry diameters > 50 and > 120nm, as well as -36% and -34% for CCN at supersaturations of 0.2% and 1.0%, respectively. However, they seem to behave differently for particles activating at very low supersaturations (< 0.1%) than at higher ones. A total of 15 models have been used to produce ensemble annual median distributions of relevant parameters. The model diversity (defined as the ratio of standard deviation to mean) is up to about 3 for simulated N3 (number concentration of particles with dry diameters larger than 3 nm) and up to about 1 for simulated CCN in the extra-polar regions. A global mean reduction of a factor of about 2 is found in the model diversity for CCN at a supersaturation of 0.2% (CCN(0.2)) compared to that for N3, maximizing over regions where new particle formation is important. An additional model has been used to investigate potential causes of model diversity in CCN and bias compared to the observations by performing a perturbed parameter ensemble (PPE) accounting for uncertainties in 26 aerosol-related model input parameters. This PPE suggests that biogenic secondary organic aerosol formation and the hygroscopic properties of the organic material are likely to be the major sources of CCN uncertainty in summer, with dry deposition and cloud processing being dominant in winter. Models capture the relative amplitude of the seasonal variability of the aerosol particle number concentration for all studied particle sizes with available observations (dry diameters larger than 50, 80 and 120nm). The short-term persistence time (on the order of a few days) of CCN concentrations, which is a measure of aerosol dynamic behavior in the models, is underestimated on average by the models by 40% during winter and 20% in summer.

cloud droplets

Impacts of Varying Concentrations of Cloud Condensation Nuclei On Deep Convective Cloud Updrafts – A Multimodel Assessment

This study presents results from a model intercomparison project, focusing on the range of responses in deep convective cloud updrafts to varying cloud condensation nuclei (CCN) concentrations amongst seven, state-of-the-art, cloud-resolving models. Simulations of scattered convective clouds near Houston, Texas are conducted, after being initialized with both relatively low and high CCN concentrations. Deep convective updrafts are identified, and trends in the updraft intensity and frequency are assessed. The factors contributing to the vertical velocity tendencies are examined to identify the physical processes associated with the CCN-induced, updraft changes. The models show several consistent trends. In general, the changes between the High- CCN and Low-CCN simulations in updraft magnitudes throughout the depth of the troposphere are within 15% for all of the models. All models produce stronger (~+5-15%) mean updrafts from ~4–7 km above ground level (AGL) in the High-CCN simulations, followed by a waning response up to ~8 km AGL in most of the models. Thermal buoyancy was more sensitive than condensate loading to varying CCN concentrations in most of the models and more impactful in the mean updraft responses. However, there are also differences between the models. The change in the amount of deep convective updrafts varies significantly. Furthermore, approximately half the models demonstrate neutral-to-weaker (~-5-0%) updrafts above ~8 km AGL, while the other models show stronger (~+10%) updrafts in the High-CCN simulations. The combination of the CCN-induced impacts on the buoyancy and vertical perturbation pressure gradient terms better explains these middle- and upper-tropospheric updraft trends than the buoyancy terms alone.

deep convective cloud updrafts

Observations of anthropogenic cloud condensation nuclei

Cloud Condensation Nuclei (CCN) concentrations and spectral measurements obtained with the DRI instantaneous CCN spectrometer (Hudson, 1989) over the last few years are presented. The climatic importance of cloud microphysics has been pointed out. The particles which affect cloud microphysics are cloud condensation nuclei (CCN). The commonly-observed order of magnitude difference in cloud droplet concentrations between maritime and continental air masses (i.e., Squires, 1958) was determined to be caused by systematic differences in the concentrations of CCN between continental and maritime air masses (e.g., Twomey and Wojciechowski, 1969). Twomey (1977) first pointed out that cloud microphysics also affects the radiative properties of clouds. Thus continental and anthropogenic CCN could affect global temperature. Resolution of this Twomey effect requires answers to two questions - whether antropogenic CCN are a significant contribution to atmospheric CCN, and whether they are actually affecting cloud microphysics to an extent which is of climatic importance. The reasons for the contrast between continental and maritime CCN concentration are not understood. The question of the relative importance of anthropogenic CCN is addressed. These observations should shed light on this complex question although further research is being conducted in order to produce more quantitative answers. Accompanying CN measurements made with a TSI 3020 condensation nucleus (CN) counter are also presented.

Hudson, James G.

Interpretable ensemble learning unveils main aerosol optical properties in predicting cloud condensation nuclei number concentration

Variations in cloud condensation nuclei number concentration (N CCN ) significantly influence cloud microphysics, yet direct N CCN measurements remain challenging. Here, we present an N CCN ensemble learning (NEL) model utilizing ensemble learning and interpretability analysis on aerosol optical parameters. Validated at two land sites, two ocean sites and one polar site within the Atmospheric Radiation Measurement program, the mean absolute percentage error range of the NEL model across different environments is from 12% to 36%, demonstrating high accuracy. Key findings reveal that aerosol optical parameters can serve as predictors for N CCN . Aerosol scattering and backscattering coefficients, absorption coefficient, backscatter fraction (BSF), and Ångström exponent (AE) are positively correlated with N CCN , while single scattering albedo shows negative correlations. N CCN prediction at land sites is highly sensitive to BSF, largely driven by the backscattering coefficient, as fine particles dominate in these sites. At ocean sites, N CCN prediction is more sensitive to AE, primarily influenced by the scattering coefficient, due to the higher proportion of larger particles. At the polar site, N CCN prediction shows sensitivity to both BSF and AE, mainly driven by the scattering coefficient, as polar sites are cleaner and contain larger particles. These differences reflect the variation in particle size and number concentration across different environments.

Atmospheric science

Use of In Situ Cloud Condensation Nuclei, Extinction, and Aerosol Size Distribution Measurements to Test a Method for Retrieving Cloud Condensation Nuclei Profiles From Surface Measurements

If the aerosol composition and size distribution below cloud are uniform, the vertical profile of cloud condensation nuclei (CCN) concentration can be retrieved entirely from surface measurements of CCN concentration and particle humidification function and surface-based retrievals of relative humidity and aerosol extinction or backscatter. This provides the potential for long-term measurements of CCN concentrations near cloud base. We have used a combination of aircraft, surface in situ, and surface remote sensing measurements to test various aspects of the retrieval scheme. Our analysis leads us to the following conclusions. The retrieval works better for supersaturations of 0.1% than for 1% because CCN concentrations at 0.1% are controlled by the same particles that control extinction and backscatter. If in situ measurements of extinction are used, the retrieval explains a majority of the CCN variance at high supersaturation for at least two and perhaps five of the eight flights examined. The retrieval of the vertical profile of the humidification factor is not the major limitation of the CCN retrieval scheme. Vertical structure in the aerosol size distribution and composition is the dominant source of error in the CCN retrieval, but this vertical structure is difficult to measure from remote sensing at visible wavelengths.

Ghan, Stephen J.