Science.gov

Sample records for aerosol cloud condensation

  1. Cloud condensation nuclei (CCN) activity of aliphatic amine secondary aerosol

    NASA Astrophysics Data System (ADS)

    Tang, X.; Price, D.; Praske, E.; Vu, D. N.; Purvis-Roberts, K.; Silva, P. J.; Cocker, D. R., III; Asa-Awuku, A.

    2014-06-01

    Aliphatic amines can form secondary aerosol via oxidation with atmospheric radicals (e.g., hydroxyl radical and nitrate radical). The particle can contain both secondary organic aerosol (SOA) and inorganic salts. The ratio of organic to inorganic materials in the particulate phase influences aerosol hygroscopicity and cloud condensation nuclei (CCN) activity. SOA formed from trimethylamine (TMA) and butylamine (BA) reactions with hydroxyl radical (OH) is composed of organic material of low hygroscopicity (single hygroscopicity parameter, κ, ≤ 0.25). Secondary aerosol formed from the tertiary aliphatic amine (TMA) with N2O5 (source of nitrate radical, NO3) contains less volatile compounds than the primary aliphatic amine (BA) aerosol. As relative humidity (RH) increases, inorganic amine salts are formed as a result of acid-base reactions. The CCN activity of the humid TMA-N2O5 aerosol obeys Zdanovskii, Stokes, and Robinson (ZSR) ideal mixing rules. The humid BA + N2O5 aerosol products were found to be very sensitive to the temperature at which the measurements were made within the streamwise continuous-flow thermal gradient CCN counter; κ ranges from 0.4 to 0.7 dependent on the instrument supersaturation (ss) settings. The variance of the measured aerosol κ values indicates that simple ZSR rules cannot be applied to the CCN results from the primary aliphatic amine system. Overall, aliphatic amine aerosol systems' κ ranges within 0.2 < κ < 0.7. This work indicates that aerosols formed via nighttime reactions with amines are likely to produce hygroscopic and volatile aerosol, whereas photochemical reactions with OH produce secondary organic aerosol of lower CCN activity. The contributions of semivolatile secondary organic and inorganic material from aliphatic amines must be considered for accurate hygroscopicity and CCN predictions from aliphatic amine systems.

  2. Vertical Profiles of Cloud Condensation Nuclei, Condensation Nuclei, Optical Aerosol, Aerosol Optical Properties, and Aerosol Volatility Measured from Balloons

    NASA Technical Reports Server (NTRS)

    Deshler, T.; Snider, J. R.; Vali, G.

    1998-01-01

    Under the support of this grant a balloon-borne gondola containing a variety of aerosol instruments was developed and flown from Laramie, Wyoming, (41 deg N, 105 deg W) and from Lauder, New Zealand (45 deg S, 170 deg E). The gondola includes instruments to measure the concentrations of condensation nuclei (CN), cloud condensation nuclei (CCN), optically detectable aerosol (OA.) (r greater than or equal to 0.15 - 2.0 microns), and optical scattering properties using a nephelometer (lambda = 530 microns). All instruments sampled from a common inlet which was heated to 40 C on ascent and to 160 C on descent. Flights with the CN counter, OA counter, and nephelometer began in July 1994. The CCN counter was added in November 1994, and the engineering problems were solved by June 1995. Since then the flights have included all four instruments, and were completed in January 1998. Altogether there were 20 flights from Laramie, approximately 5 per year, and 2 from Lauder. Of these there were one or more engineering problems on 6 of the flights from Laramie, hence the data are somewhat limited on those 6 flights, while a complete data set was obtained from the other 14 flights. Good CCN data are available from 12 of the Laramie flights. The two flights from Lauder in January 1998 were successful for all measurements. The results from these flights, and the development of the balloon-bome CCN counter have formed the basis for five conference presentations. The heated and unheated CN and OA measurements have been used to estimate the mass fraction of the aerosol volatile, while comparisons of the nephelometer measurements were used to estimate the light scattering, associated with the volatile aerosol. These estimates were calculated for 0.5 km averages of the ascent and descent data between 2.5 km and the tropopause, near 11.5 km.

  3. Cloud condensation nuclei activity of isoprene secondary organic aerosol

    NASA Astrophysics Data System (ADS)

    Engelhart, Gabriella J.; Moore, Richard H.; Nenes, Athanasios; Pandis, Spyros N.

    2011-01-01

    This work explores the cloud condensation nuclei (CCN) activity of isoprene secondary organic aerosol (SOA), likely a significant source of global organic particulate matter and CCN, produced from the oxidation with OH from HONO/HOOH photolysis in a temperature-controlled SOA chamber. CCN concentrations, activation diameter, and droplet growth kinetic information were monitored as a function of supersaturation (from 0.3% to 1.5%) for several hours using a cylindrical continuous-flow streamwise thermal gradient CCN counter connected to a scanning mobility particle sizer. The initial SOA concentrations ranged from 2 to 30 μg m-3 and presented CCN activity similar to monoterpene SOA with an activation diameter of 35 nm for 1.5% supersaturation and 72 nm for 0.6% supersaturation. The CCN activity improved slightly in some experiments as the SOA aged chemically and did not depend significantly on the level of NOx during the SOA production. The measured activation diameters correspond to a hygroscopicity parameter κ value of 0.12, similar to κ values of 0.1 ± 0.04 reported for monoterpene SOA. Analysis of the water-soluble carbon extracted from filter samples of the SOA suggest that it has a κ of 0.2-0.3 implying an average molar mass between 90 and 150 g mol-1 (assuming a zero and 5% surface tension reduction with respect to water, respectively). These findings are consistent with known oxidation products of isoprene. Using threshold droplet growth analysis, the CCN activation kinetics of isoprene SOA was determined to be similar to pure ammonium sulfate aerosol.

  4. Cloud condensation nuclei activation of limited solubility organic aerosol

    NASA Astrophysics Data System (ADS)

    Huff Hartz, Kara E.; Tischuk, Joshua E.; Chan, Man Nin; Chan, Chak K.; Donahue, Neil M.; Pandis, Spyros N.

    The cloud condensation nuclei (CCN) activation of 19 organic species with water solubilities ( Csat) ranging from 10 -4 to 10 2 g solute 100 g -1 H 2O was measured. The organic particles were generated by nebulization of an aqueous or an alcohol solution. Use of alcohols as solvents enables the measurement of low solubility, non-volatile organic CCN activity and reduces the likelihood of residual water in the aerosol. The activation diameter of organic species with very low solubility in water ( Csat<0.3 g 100 g -1 H 2O) is in agreement with Köhler theory using the bulk solubility (limited solubility case) of the organic in water. Many species, including 2-acetylbenzoic acid, aspartic acid, azelaic acid, glutamic acid, homophthalic acid, phthalic acid, cis-pinonic acid, and salicylic acid are highly CCN active in spite of their low solubility (0.3 g 100 g -1 H 2O< Csat<1 g 100 g -1 H 2O), and activate almost as if completely water soluble. The CCN activity of most species is reduced, if the particles are produced using non-aqueous solvents. The existence of the particles in a metastable state at low RH can explain the observed enhancement in CCN activity beyond the levels suggested by their solubility.

  5. Cloud Condensation Nuclei Activity of Aerosols during GoAmazon 2014/15 Field Campaign Report

    SciTech Connect

    Wang, J.; Martin, S. T.; Kleinman, L.; Thalman, R. M.

    2016-03-01

    Aerosol indirect effects, which represent the impact of aerosols on climate through influencing the properties of clouds, remain one of the main uncertainties in climate predictions (Stocker et al. 2013). Reducing this large uncertainty requires both improved understanding and representation of aerosol properties and processes in climate models, including the cloud activation properties of aerosols. The Atmospheric System Research (ASR) science program plan of January 2010 states that: “A key requirement for simulating aerosol-cloud interactions is the ability to calculate cloud condensation nuclei and ice nuclei (CCN and IN, respectively) concentrations as a function of supersaturation from the chemical and microphysical properties of the aerosol.” The Observations and Modeling of the Green Ocean Amazon (GoAmazon 2014/15) study seeks to understand how aerosol and cloud life cycles are influenced by pollutant outflow from a tropical megacity (Manaus)—in particular, the differences in cloud-aerosol-precipitation interactions between polluted and pristine conditions. One key question of GoAmazon2014/5 is: “What is the influence of the Manaus pollution plume on the cloud condensation nuclei (CCN) activities of the aerosol particles and the secondary organic material in the particles?” To address this question, we measured size-resolved CCN spectra, a critical measurement for GoAmazon2014/5.

  6. Effect of aerosol subgrid variability on aerosol optical depth and cloud condensation nuclei: implications for global aerosol modelling

    NASA Astrophysics Data System (ADS)

    Weigum, Natalie; Schutgens, Nick; Stier, Philip

    2016-11-01

    A fundamental limitation of grid-based models is their inability to resolve variability on scales smaller than a grid box. Past research has shown that significant aerosol variability exists on scales smaller than these grid boxes, which can lead to discrepancies in simulated aerosol climate effects between high- and low-resolution models. This study investigates the impact of neglecting subgrid variability in present-day global microphysical aerosol models on aerosol optical depth (AOD) and cloud condensation nuclei (CCN). We introduce a novel technique to isolate the effect of aerosol variability from other sources of model variability by varying the resolution of aerosol and trace gas fields while maintaining a constant resolution in the rest of the model. We compare WRF-Chem (Weather and Research Forecast model) runs in which aerosol and gases are simulated at 80 km and again at 10 km resolutions; in both simulations the other model components, such as meteorology and dynamics, are kept at the 10 km baseline resolution. We find that AOD is underestimated by 13 % and CCN is overestimated by 27 % when aerosol and gases are simulated at 80 km resolution compared to 10 km. The processes most affected by neglecting aerosol subgrid variability are gas-phase chemistry and aerosol uptake of water through aerosol-gas equilibrium reactions. The inherent non-linearities in these processes result in large changes in aerosol properties when aerosol and gaseous species are artificially mixed over large spatial scales. These changes in aerosol and gas concentrations are exaggerated by convective transport, which transports these altered concentrations to altitudes where their effect is more pronounced. These results demonstrate that aerosol variability can have a large impact on simulating aerosol climate effects, even when meteorology and dynamics are held constant. Future aerosol model development should focus on accounting for the effect of subgrid variability on these

  7. Vertical profiles of cloud condensation nuclei, aerosol hygroscopicity, water uptake, and scattering across the United States

    NASA Astrophysics Data System (ADS)

    Lin, J. J.; Bougiatioti, A.; Nenes, A.; Anderson, B. E.; Beyersdorf, A. J.; Brock, C. A.; Gordon, T. D.; Lack, D.; Law, D. C.; Liao, J.; Middlebrook, A. M.; Richardson, M.; Thornhill, K. L., II; Winstead, E.; Wagner, N. L.; Welti, A.; Ziemba, L. D.

    2014-12-01

    The evolutions of vertical distributions of aerosol chemical, microphysical, hygroscopic, and optical properties present fundamental challenges to the understanding of ground-level air quality and radiative transfer, and few datasets exist to date for evaluation of atmospheric models. Data collected from recent NASA and NOAA field campaigns in the California Central Valley (DISCOVER-AQ), southeast United States (SENEX, SEAC4RS) and Texas (DISCOVER-AQ) allow for a unique opportunity to constrain vertical profiles of climate-relevant aerosol properties. This work presents in-situ aircraft measurements of cloud condensation nuclei (CCN) concentration and derivations of aerosol hygroscopicity, water uptake, and light scattering. Aerosol hygroscopicity is derived from CCN and aerosol measurements. Inorganic water uptake is calculated from aerosol composition using ISORROPIA, a chemical thermodynamic model, while organic water uptake is calculated from organic hygroscopicity. Aerosol scattering closure is performed between scattering from water uptake calculations and in-situ scattering measurements.

  8. Titan's Aerosol and Condensation Cloud Properties in the Far-IR Between 2005 and 2010

    NASA Technical Reports Server (NTRS)

    Anderson, Carrie; Samuelson, Robert

    2011-01-01

    Analyses of far-IR spectra between 20 and 560 cm(exp -1) (500 to 18 micron) recorded by the Cassini Composite Infrared Spectrometer (CIRS) yield the spectral dependence and the vertical distribution of Titan's photochemical aerosol and ice clouds. Titan's aerosol appears to be well mixed between the surface and an altitude of 300 km, with a spectral shape that does not change with latitude or time. The aerosol exhibits an extremely broad emission feature with a spectral peak at 140 cm(exp -1) (71 micron), which is not evident in laboratory simulated Titan aerosols (tholin). This low- energy aerosol emission feature may arise from low-energy molecules such as polycyclic aromatic hydrocarbons and/or nitrogenated aromatics. Unlike the vertically well-mixed aerosol, Titan's condensate clouds are located in highly restricted altitudes in the lower stratosphere, ranging between 60 and 100 km at low and moderate latitudes, to between 150 and 165 km at high northern latitudes during northern winter. Such clouds are located at altitudes where nitrile vapors are expected to condense and appear to be dominated by HCN and HC3N, which are the two most abundant nitriles in Titan's atmosphere. Associated with this ice cloud is a broad emission feature that spectrally peaks near 160 cm(exp -1) (62.5 micron). This ice composite appears to chemically change with altitude and latitude, probably as a result of differences in vapor abundance and condensation temperature, and the ice cloud appears to be global in extent. Both CIRS and the Huygens Descent Imager and Spectral Radiometer (DISR) show evidence of cloud layering in Titan's lower stratosphere. The 15 km difference in cloud altitude indicated by the two instruments suggests a difference in ice composition. CIRS also indicates a second ice cloud that exists at isolated latitudes and is consistent with hydrocarbon condensation above the tropopause. This cloud exhibits an emission feature that spectrally peaks near 80 cm(exp -1

  9. Biogenic sulfur emissions and aerosols over the tropical South Atlantic: 3. Atmospheric dimethylsulfide, aerosols and cloud condensation nuclei

    NASA Astrophysics Data System (ADS)

    Andreae, Meinrat O.; Elbert, Wolfgang; de Mora, Stephen J.

    1995-06-01

    We measured dimethylsulfide in air (DMSa) and the number concentration, size distribution, and chemical composition of atmospheric aerosols, including the concentration of cloud condensation nuclei (CCN), during February-March 1991 over the tropical South Atlantic along 19°S (F/S Meteor, cruise 15/3). Aerosol number/size distributions were determined with a laser-optical particle counter, condensation nuclei (CN) concentrations with a TSI 3020, and cloud condensation nuclei (CCN) with a Hudson-type supersaturation chamber. Aerosol samples were collected on two-stage stacked filters and analyzed by ion chromatography for soluble ion concentrations. Black carbon in aerosols was measured by visible light absorption and used to identify and eliminate periods with anthropogenic pollution from the data set. Meteorological analysis shows that most of the air masses sampled had spent extended periods over remote marine areas in the tropical and subtropical region. DMSa was closely correlated with the sea-to- air DMS flux calculated from DMS concentrations in seawater and meteorological data. Sea salt made the largest contribution to aerosol mass and volume but provided only a small fraction of the aerosol number concentration. The submicron aerosol had a mean composition close to ammonium bisulfate, with the addition of some methanesulfonate. Aerosol (CN and CCN) number and non-sea-salt sulfate concentrations were significantly correlated with DMS concentration and flux. This suggests that DMS oxidation followed by aerosol nucleation and growth in the marine boundary layer is an important, if not dominating, source of CN and possibly CCN. The degree of correlation between DMS and particle concentrations in the marine boundary layer may be strongly influenced by the different time scales of the processes regulating these concentrations. Our results provide strong support for several aspects of the CLAW hypothesis, which proposes the existence of a feedback loop linking DMS

  10. Effects of aerosol organics on cloud condensation nucleus (CCN) concentration and first indirect aerosol effect

    SciTech Connect

    Wang, J. X.; Lee, Y.- N.; Daum, Peter H.; Jayne, John T.; Alexander, M. L.

    2008-11-03

    Abstract. Aerosol microphysics, chemical composition, and CCN properties were measured on the Department of Energy Gulfstream-1 aircraft during the Marine Stratus/ Stratocumulus Experiment (MASE) conducted over the coastal waters between Point Reyes National Seashore and Monterey Bay, California, in July 2005. Aerosols measured during MASE included free tropospheric aerosols, marine boundary layer aerosols, and aerosols with high organic concentration within a thin layer above the cloud. Closure analysis was carried out for all three types of aerosols by comparing the measured CCN concentrations at 0.2% supersaturation to those predicted based on size distribution and chemical composition using K¨ohler theory. The effect of aerosol organic species on predicted CCN concentration was examined using a single hygroscopicity parameterization.

  11. Cloud condensation nuclei activity of aliphatic amine secondary aerosol

    Technology Transfer Automated Retrieval System (TEKTRAN)

    Aliphatic amines can form secondary aerosol via oxidation with atmospheric radicals (e.g. hydroxyl radical and nitrate radical). The resulting particle composition can contain both secondary organic aerosol (SOA) and inorganic salts. The fraction of organic to inorganic materials in the particulate ...

  12. Cloud Condensation Nuclei Prediction Error from Application of Kohler Theory: Importance for the Aerosol Indirect Effect

    NASA Technical Reports Server (NTRS)

    Sotiropoulou, Rafaella-Eleni P.; Nenes, Athanasios; Adams, Peter J.; Seinfeld, John H.

    2007-01-01

    In situ observations of aerosol and cloud condensation nuclei (CCN) and the GISS GCM Model II' with an online aerosol simulation and explicit aerosol-cloud interactions are used to quantify the uncertainty in radiative forcing and autoconversion rate from application of Kohler theory. Simulations suggest that application of Koehler theory introduces a 10-20% uncertainty in global average indirect forcing and 2-11% uncertainty in autoconversion. Regionally, the uncertainty in indirect forcing ranges between 10-20%, and 5-50% for autoconversion. These results are insensitive to the range of updraft velocity and water vapor uptake coefficient considered. This study suggests that Koehler theory (as implemented in climate models) is not a significant source of uncertainty for aerosol indirect forcing but can be substantial for assessments of aerosol effects on the hydrological cycle in climatically sensitive regions of the globe. This implies that improvements in the representation of GCM subgrid processes and aerosol size distribution will mostly benefit indirect forcing assessments. Predictions of autoconversion, by nature, will be subject to considerable uncertainty; its reduction may require explicit representation of size-resolved aerosol composition and mixing state.

  13. Detection of organophosphorus aerosols by a cloud condensation nuclei spectrometer of new design

    NASA Astrophysics Data System (ADS)

    Hudson, James G.; Dong, Ya Y.; Hallet, John; Carlon, Hugh R.; Allan, Craig R.

    1989-03-01

    The Cloud Condensation Nuclei (CCN) Spectrometer is a newly-developed instrument, which was devised and built by the Desert Research Institute (DRI). Unlike other CCN Spectrometers, this one uses droplet size to infer the critical supersaturation (Sc) spectrum of the sampled aerosol. The new instrument obtains simultaneous CCN spectra from the droplet spectra. Since the nuclei can be as small as 0.01 micrometer in diameter and are too small to obtain a size spectrum, they are amplified by water condensation to micrometer sizes that can be easily detected by an optical particle counter. The droplet spectrum is then related to the CCN spectrum through calibration using monodisperse salt aerosol with known Sc's. Droplet size dispersion is achieved by exposing the sample to an increasing Sc as it passes through the chamber. Preliminary studies have shown that the new system can detect and characterize organophosphorus aerosols, such as Malathian, and is useful in measuring and identifying natural or background aerosols against which chemical warfare aerosols would have to be detected. Further work is suggested to improve detection specificity and to permit a wider range of water-insoluble substances to be detected.

  14. Effect of the secondary organic aerosol coatings on black carbon water uptake, cloud condensation nuclei activity, and particle collapse

    EPA Science Inventory

    The ability of black carbon aerosols to absorb water and act as a cloud condensation nuclei (CCN) directly controls their lifetime in the atmosphere as well as their impact on cloud formation, thus impacting the earth’s climate. Black carbon emitted from most combustion pro...

  15. Characterization and parameterization of aerosol cloud condensation nuclei activation under different pollution conditions.

    PubMed

    Che, H C; Zhang, X Y; Wang, Y Q; Zhang, L; Shen, X J; Zhang, Y M; Ma, Q L; Sun, J Y; Zhang, Y W; Wang, T T

    2016-04-14

    To better understand the cloud condensation nuclei (CCN) activation capacity of aerosol particles in different pollution conditions, a long-term field experiment was carried out at a regional GAW (Global Atmosphere Watch) station in the Yangtze River Delta area of China. The homogeneity of aerosol particles was the highest in clean weather, with the highest active fraction of all the weather types. For pollution with the same visibility, the residual aerosol particles in higher relative humidity weather conditions were more externally mixed and heterogeneous, with a lower hygroscopic capacity. The hygroscopic capacity (κ) of organic aerosols can be classified into 0.1 and 0.2 in different weather types. The particles at ~150 nm were easily activated in haze weather conditions. For CCN predictions, the bulk chemical composition method was closer to observations at low supersaturations (≤0.1%), whereas when the supersaturation was ≥0.2%, the size-resolved chemical composition method was more accurate. As for the mixing state of the aerosol particles, in haze, heavy haze, and severe haze weather conditions CCN predictions based on the internal mixing assumption were robust, whereas for other weather conditions, predictions based on the external mixing assumption were more accurate.

  16. Characterization and parameterization of aerosol cloud condensation nuclei activation under different pollution conditions

    NASA Astrophysics Data System (ADS)

    Che, H. C.; Zhang, X. Y.; Wang, Y. Q.; Zhang, L.; Shen, X. J.; Zhang, Y. M.; Ma, Q. L.; Sun, J. Y.; Zhang, Y. W.; Wang, T. T.

    2016-04-01

    To better understand the cloud condensation nuclei (CCN) activation capacity of aerosol particles in different pollution conditions, a long-term field experiment was carried out at a regional GAW (Global Atmosphere Watch) station in the Yangtze River Delta area of China. The homogeneity of aerosol particles was the highest in clean weather, with the highest active fraction of all the weather types. For pollution with the same visibility, the residual aerosol particles in higher relative humidity weather conditions were more externally mixed and heterogeneous, with a lower hygroscopic capacity. The hygroscopic capacity (κ) of organic aerosols can be classified into 0.1 and 0.2 in different weather types. The particles at ~150 nm were easily activated in haze weather conditions. For CCN predictions, the bulk chemical composition method was closer to observations at low supersaturations (≤0.1%), whereas when the supersaturation was ≥0.2%, the size-resolved chemical composition method was more accurate. As for the mixing state of the aerosol particles, in haze, heavy haze, and severe haze weather conditions CCN predictions based on the internal mixing assumption were robust, whereas for other weather conditions, predictions based on the external mixing assumption were more accurate.

  17. Characterization and parameterization of aerosol cloud condensation nuclei activation under different pollution conditions

    PubMed Central

    Che, H. C.; Zhang, X. Y.; Wang, Y. Q.; Zhang, L.; Shen, X. J.; Zhang, Y. M.; Ma, Q. L.; Sun, J. Y.; Zhang, Y. W.; Wang, T. T.

    2016-01-01

    To better understand the cloud condensation nuclei (CCN) activation capacity of aerosol particles in different pollution conditions, a long-term field experiment was carried out at a regional GAW (Global Atmosphere Watch) station in the Yangtze River Delta area of China. The homogeneity of aerosol particles was the highest in clean weather, with the highest active fraction of all the weather types. For pollution with the same visibility, the residual aerosol particles in higher relative humidity weather conditions were more externally mixed and heterogeneous, with a lower hygroscopic capacity. The hygroscopic capacity (κ) of organic aerosols can be classified into 0.1 and 0.2 in different weather types. The particles at ~150 nm were easily activated in haze weather conditions. For CCN predictions, the bulk chemical composition method was closer to observations at low supersaturations (≤0.1%), whereas when the supersaturation was ≥0.2%, the size-resolved chemical composition method was more accurate. As for the mixing state of the aerosol particles, in haze, heavy haze, and severe haze weather conditions CCN predictions based on the internal mixing assumption were robust, whereas for other weather conditions, predictions based on the external mixing assumption were more accurate. PMID:27075947

  18. Composition, size and cloud condensation nuclei activity of biomass burning aerosol from northern Australian savannah fires

    NASA Astrophysics Data System (ADS)

    Mallet, Marc D.; Cravigan, Luke T.; Milic, Andelija; Alroe, Joel; Ristovski, Zoran D.; Ward, Jason; Keywood, Melita; Williams, Leah R.; Selleck, Paul; Miljevic, Branka

    2017-03-01

    The vast majority of Australia's fires occur in the tropical north of the continent during the dry season. These fires are a significant source of aerosol and cloud condensation nuclei (CCN) in the region, providing a unique opportunity to investigate the biomass burning aerosol (BBA) in the absence of other sources. CCN concentrations at 0.5 % supersaturation and aerosol size and chemical properties were measured at the Australian Tropical Atmospheric Research Station (ATARS) during June 2014. CCN concentrations reached over 104 cm-3 when frequent and close fires were burning - up to 45 times higher than periods with no fires. Both the size distribution and composition of BBA appeared to significantly influence CCN concentrations. A distinct diurnal trend in the proportion of BBA activating to cloud droplets was observed, with an activation ratio of 40 ± 20 % during the night and 60 ± 20 % during the day. BBA was, on average, less hygroscopic during the night (κ = 0. 04 ± 0.03) than during the day (κ = 0.07 ± 0.05), with a maximum typically observed just before midday. Size-resolved composition of BBA showed that organics comprised a constant 90 % of the aerosol volume for aerodynamic diameters between 100 and 200 nm. While this suggests that the photochemical oxidation of organics led to an increase in the hygroscopic growth and an increase in daytime activation ratios, it does not explain the decrease in hygroscopicity after midday. Modelled CCN concentrations assuming typical continental hygroscopicities produced very large overestimations of up to 200 %. Smaller, but still significant, overpredictions up to ˜ 100 % were observed using aerosol mass spectrometer (AMS)- and hygroscopicity tandem differential mobility analyser (H-TDMA)-derived hygroscopicities as well as campaign night and day averages. The largest estimations in every case occurred during the night, when the small variations in very weakly hygroscopic species corresponded to large

  19. Impacts of new particle formation on aerosol cloud condensation nuclei (CCN) activity in Shanghai: case study

    NASA Astrophysics Data System (ADS)

    Leng, C.; Zhang, Q.; Zhang, D.; Zhang, H.; Xu, C.; Li, X.; Kong, L.; Tao, J.; Cheng, T.; Zhang, R.; Chen, J.; Qiao, L.; Lou, S.; Wang, H.; Chen, C.

    2014-07-01

    New particle formation (NPF) events and their impacts on cloud condensation nuclei (CCN) were investigated using continuous measurements collected in urban Shanghai from 1 to 30 April 2012. During the campaign, NPF occurred in 8 out of the 30 days and enhanced CCN number concentration (NCCN) by a actor of 1.2-1.8, depending on supersaturation (SS). The NPF event on 3 April 2012 was chosen as an example to investigate the NPF influence on CCN activity. In this NPF event, secondary aerosols were produced continuously and increased PM2.5 mass concentration at a~rate of 4.33 μg cm-3 h-1, and the growth rate (GR) and formation rate (FR) were on average 5 nm h-1 and 0.36 cm-3 s-1, respectively. The newly formed particles grew quickly from nucleation mode (10-20 nm) into CCN size range. NCCN increased rapidly at SS of 0.4-1.0% but weakly at SS of 0.2%. Correspondingly, aerosol CCN activities (fractions of activated aerosol particles in total aerosols, NCCN / NCN) were significantly enhanced from 0.24-0.60 to 0.30-0.91 at SS of 0.2-1.0% due to the NPF. On the basis of the κ-Köhler theory, aerosol size distributions and chemical composition measured simultaneously were used to predict NCCN. There was a good agreement between the predicted and measured NCCN (R2 = 0.96, Npredicted / Nmeasured = 1.04). This study reveals that NPF exerts large impacts on aerosol particle abundance and size spectra, thus significantly promotes NCCN and aerosol CCN activity in this urban environment. The GR of NPF is the key factor controlling the newly formed particles to become CCN at all SS levels, whereas the FR is an effective factor only under high SS (e.g. 1.0%) conditions.

  20. Oxidation of ambient biogenic secondary organic aerosol by hydroxyl radicals: Effects on cloud condensation nuclei activity

    NASA Astrophysics Data System (ADS)

    Wong, J. P. S.; Lee, A. K. Y.; Slowik, J. G.; Cziczo, D. J.; Leaitch, W. R.; Macdonald, A.; Abbatt, J. P. D.

    2011-11-01

    Changes in the hygroscopicity of ambient biogenic secondary organic aerosols (SOA) due to controlled OH oxidation were investigated at a remote forested site at Whistler Mountain, British Columbia during July of 2010. Coupled photo-oxidation and cloud condensation nuclei (CCN) experiments were conducted on: i) ambient particles exposed to high levels of gas-phase OH, and ii) the water-soluble fraction of ambient particles oxidized by aqueous-phase OH. An Aerodyne Aerosol Mass Spectrometer (AMS) monitored the changes in the chemical composition and degree of oxidation (O:C ratio) of the organic component of ambient aerosol due to OH oxidation. The CCN activity of size-selected particles was measured to determine the hygroscopicity parameter ($\\kappa$org,CCN) for particles of various degrees of oxygenation. In both cases, the CCN activity of the oxidized material was higher than that of the ambient particles. In general, $\\kappa$org,CCN of the aerosol increases with its O:C ratio, in agreement with previous laboratory measurements.

  1. Formation and aging of secondary organic aerosol from isoprene photooxidation during cloud condensation-evaporation cycles

    NASA Astrophysics Data System (ADS)

    Giorio, C.; Siekmann, F.; Bregonzio, L.; Temime-Roussel, B.; Ravier, S.; Tapparo, A.; Kalberer, M.; Doussin, J.; Monod, A.

    2013-12-01

    Biogenic volatile organic compounds (BVOCs) can be oxidized in the gas phase to form more water-soluble compounds which could partition into atmospheric water droplets. Oxidation processes in the liquid phase could produce high molecular weight and less volatile compounds which can partly remain in the particle phase after water evaporation (Ervens et al., 2011). This work investigates the formation and composition of secondary organic aerosol (SOA) from the photooxidation of isoprene (the most abundant BVOC) and methacrolein (its main first-generation oxidation product). The experiments were performed during the CUMULUS (CloUd MULtiphase chemistry of organic compoUndS in the troposphere) campaigns at the 4.2 m3 stainless steel CESAM chamber at LISA, specifically designed to investigate multiphase processes (Wang et al., 2011). In each experiment, 500/1000 ppb of isoprene or methacrolein were injected in the chamber together with HONO before irradiation. Gas phase oxidation products have been analyzed on-line by a Proton Transfer Reaction Mass Spectrometer (PTR-MS) and a Fourier Transform Infrared Spectrometer (FTIR) together with NOx and O3 analyzers. SOA formation and composition has been followed on-line with a Scanning Mobility Particle Sizer (SMPS) and an Aerodyne High Resolution Time-Of-Flight Aerosol Mass Spectrometer (HR-TOF-AMS). Particular attention has been focused on the study of SOA formation and aging during cloud condensation-evaporation cycles simulated in the smog chamber. In all experiments, we noted that water soluble gas-phase oxidation products readily partition into cloud droplets accompanied by a prompt SOA production during cloud formation which partly persists after cloud evaporation. Ervens, B. et al. (2011) Atmos. Chem. Phys. 11, 11069 11102. Wang, J. et al. (2011) Atmos. Measur. Tech. 4, 2465 2494.

  2. Ozone oxidation of oleic acid surface films decreases aerosol cloud condensation nuclei activity

    NASA Astrophysics Data System (ADS)

    Schwier, A. N.; Sareen, N.; Lathem, T. L.; Nenes, A.; McNeill, V. F.

    2011-08-01

    Heterogeneous oxidation of aerosols composed of pure oleic acid (C18H34O2, an unsaturated fatty acid commonly found in continental and marine aerosol) by gas-phase O3 is known to increase aerosol hygroscopicity and activity as cloud condensation nuclei (CCN). Whether this trend is preserved when the oleic acid is internally mixed with other electrolytes is unknown and addressed in this study. We quantify the CCN activity of sodium salt aerosols (NaCl and Na2SO4) internally mixed with sodium oleate (SO) and oleic acid (OA). We find that particles containing roughly one monolayer of SO/OA show similar CCN activity to pure salt particles, whereas a tenfold increase in organic concentration slightly depresses CCN activity. O3 oxidation of these multicomponent aerosols has little effect on the critical diameter for CCN activation for unacidified particles at all conditions studied, and the activation kinetics of the CCN are similar in each case to those of pure salts. SO-containing particles which are acidified to atmospherically relevant pH before analysis in order to form oleic acid, however, show depressed CCN activity upon oxidation. This effect is more pronounced at higher organic concentrations. The behavior after oxidation is consistent with the disappearance of the organic surface film, supported by Köhler Theory Analysis (KTA). The κ-Köhler calculations show a small decrease in hygroscopicity after oxidation. The important implication of this finding is that oxidative aging may not always enhance the hygroscopicity of internally mixed inorganic-organic aerosols.

  3. 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

    NASA Technical Reports Server (NTRS)

    Ghan, Stephen J.; Rissman, Tracey A.; Ellman, Robert; Ferrare, Richard A.; Turner, David; Flynn, Connor; Wang, Jian; Ogren, John; Hudson, James; Jonsson, Haflidi H.; VanReken, Timothy; Flagan, Richard C.; Seinfeld, John H.

    2006-01-01

    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.

  4. Aerosol properties and their influences on marine boundary layer cloud condensation nuclei at the ARM mobile facility over the Azores

    NASA Astrophysics Data System (ADS)

    Logan, Timothy; Xi, Baike; Dong, Xiquan

    2014-04-01

    A multiplatform data set from the Clouds, Aerosol, and Precipitation in the Marine Boundary Layer (MBL) Graciosa, Azores, 2009-2010 field campaign was used to investigate how continental aerosols can influence MBL cloud condensation nuclei (CCN) number concentration (NCCN). The seasonal variations of aerosol properties have shown that the winter and early spring months had the highest mean surface wind speed (> 5 m s-1) and greatest contribution of sea salt to aerosol optical depth (AOD), while continental fine mode aerosols were the main contributors to AOD during the warm season months (May-September). Five aerosol events consisting of mineral dust, pollution, biomass smoke, and volcanic ash particles were selected as case studies using Atmospheric Radiation Measurement (ARM) mobile facility measurements. The aerosols in Case I were found to primarily consist of coarse mode, Saharan mineral dust. For Case II, the aerosols were also coarse mode but consisted of volcanic ash. Case III had fine mode biomass smoke and pollution aerosol influences while Cases IV and V consisted of mixtures of North American pollution and Saharan dust that was advected by an extratropical cyclone to the Azores. Cases I, IV, and V exhibited weak correlations between aerosol loading and NCCN due to mineral dust influences, while Cases II and III had a strong relationship with NCCN likely due to the sulfate content in the volcanic ash and pollution particles. The permanent Eastern North Atlantic ARM facility over the Azores will aid in a future long-term study of aerosol effects on NCCN.

  5. Toward Aerosol/Cloud Condensation Nuclei (CCN) Closure during CRYSTAL-FACE

    NASA Technical Reports Server (NTRS)

    VanReken, Timothy M.; Rissman, Tracey, A.; Roberts, Gregory C.; Varutbangkul, Varuntida; Jonsson, Haflidi H.; Flagan, Richard C.; Seinfeld, John H.

    2003-01-01

    During July 2002, measurements of cloud condensation nuclei were made in the vicinity of southwest Florida as part of the Cirrus Regional Study of Tropical Anvils and Cirrus Layers-Florida Area Cirrus Experiment (CRYSTAL-FACE) field campaign. These observations, at supersaturations of 0.2 and 0.85%, are presented here. The performance of each of the two CCN counters was validated through laboratory calibration and an in situ intercomparison. The measurements indicate that the aerosol sampled during the campaign was predominantly marine in character: the median concentrations were 233 cm-3 (at S = 0.2%) and 371 cm(sup -3) (at S = 0.85%). Three flights during the experiment differed from this general trend; the aerosol sampled during the two flights on 18 July was more continental in character, and the observations on 28 July indicate high spatial variability and periods of very high aerosol concentrations. This study also includes a simplified aerosol/CCN closure analysis. Aerosol size distributions were measured simultaneously with the CCN observations, and these data are used to predict a CCN concentration using Kohler theory. For the purpose of this analysis, an idealized composition of pure ammonium sulfate was assumed. The analysis indicates that in this case, there was good general agreement between the predicted and observed CCN concentrations: at S = 0.2%, N(sub predicted)/N(sub observed)= 1.047 (R(sup 2)= 0.911)); at S = 0.85%, N(sub predicted)/N(sub observed)=1.201 (R(sup 2)= 0.835)). The impacts of the compositional assumption and of including in-cloud data in the analysis are addressed. The effect of removing the data from the 28 July flight is also examined; doing so improves the result of the closure analysis at S = 0.85%. When omitting that atypical flight, N(sub predicted)/N(sub observed) = 1.085 (R(sup 2) = 0.770) at S = 0.85%.

  6. Impacts of oxidation aging on secondary organic aerosol formation, particle growth rate, cloud condensation nuclei abundance, and aerosol climate forcing

    NASA Astrophysics Data System (ADS)

    Yu, F.; Luo, G.

    2014-12-01

    Particle composition measurements indicate that organic aerosol (OA) makes up ~20-90% of submicron particulate mass and secondary OA (SOA) accounts for a large fraction (~ 72 ±21%) of these OA masses at many locations around the globe. The volatility changes of secondary organic gases (SOG) associated with oxidation aging as well as the contribution of highly oxidized low volatile SOG (LV-SOG) to the condensational growth of secondary particles have been found to be important in laboratory and field measurements but are poorly represented in global models. A novel scheme to extend the widely used two-product SOA formation model, by adding a third product arising from the oxidation aging (i.e., LV-SOG) and considering the dynamic transfer of mass from higher to lower volatile products, has been developed and implemented into a global chemical transport model (GEOS-Chem) and a community atmosphere model (CESM-CAM5). The scheme requires only minor changes to the existing two-product SOA formation model and is computationally efficient. With the oxidation rate constrained by laboratory measurements, we show that the new scheme predicts a much higher SOA mass concentrations, improving the agreement with aerosol mass spectrometer SOA measurements. The kinetic condensation of LV-SOG on ultrafine particles, simulated by a size-resolved (sectional) advanced particle microphysics (APM) model incorporated into in GEOS-Chem and CAM5, increases the particle growth rate substantially and improves the agreement of simulated cloud condensation nuclei (CCN) concentrations with observations. Based on GEOS-Chem-APM simulations, the new SOA formation scheme increases global mean low troposphere SOA mass concentration by ~130% and CCN abundance by ~ 15%, and optical depth of secondary particles and coated black carbon and primary organic carbon particles by ~10%. As a result, aerosol radiative cooling effect (direct + first indirect) is enhanced by -0.9 W/m2, with large spatial

  7. Cloud condensation nucleus activity of secondary organic aerosol particles mixed with sulfate

    NASA Astrophysics Data System (ADS)

    King, Stephanie M.; Rosenoern, Thomas; Shilling, John E.; Chen, Qi; Martin, Scot T.

    2007-12-01

    The cloud condensation nucleus (CCN) activity of organic-sulfate particles was investigated using a steady-state environmental chamber. The organic component consisted of secondary organic aerosol (SOA) generated in the dark from 24 +/- 2 ppb α-pinene for conditions of 300 +/- 5 ppb ozone, 40 +/- 2% relative humidity, and 25 +/- 1°C, with the organic mass loading in the chamber ranging from 23 to 37 μg m-3. CCN analysis was performed for 80- to 150-nm particles having variable organic-sulfate volume fractions, which were estimated from the diameter of the organic-sulfate particle relative to that of the seed as well as independently from mass spectra. Critical supersaturation, which increased for greater SOA volume fraction and smaller particle diameter, was well predicted by a Köhler model having two components, one for ammonium sulfate and another for SOA. The entire data set could be successfully modeled by a single suite of effective chemical parameters for SOA. The results suggest that the effects of limited organic solubility in mixed SOA-sulfate particles may be reliably omitted in the treatment of cloud droplet formation.

  8. Aerosol Chemistry Resolved by Mass Spectrometry: Linking Field Measurements of Cloud Condensation Nuclei Activity to Organic Aerosol Composition.

    PubMed

    Vogel, Alexander L; Schneider, Johannes; Müller-Tautges, Christina; Phillips, Gavin J; Pöhlker, Mira L; Rose, Diana; Zuth, Christoph; Makkonen, Ulla; Hakola, Hannele; Crowley, John N; Andreae, Meinrat O; Pöschl, Ulrich; Hoffmann, Thorsten

    2016-10-06

    Aerosol hygroscopic properties were linked to its chemical composition by using complementary online mass spectrometric techniques in a comprehensive chemical characterization study at a rural mountaintop station in central Germany in August 2012. In particular, atmospheric pressure chemical ionization mass spectrometry ((-)APCI-MS) provided measurements of organic acids, organosulfates, and nitrooxy-organosulfates in the particle phase at 1 min time resolution. Offline analysis of filter samples enabled us to determine the molecular composition of signals appearing in the online (-)APCI-MS spectra. Aerosol mass spectrometry (AMS) provided quantitative measurements of total submicrometer organics, nitrate, sulfate, and ammonium. Inorganic sulfate measurements were achieved by semionline ion chromatography and were compared to the AMS total sulfate mass. We found that up to 40% of the total sulfate mass fraction can be covalently bonded to organic molecules. This finding is supported by both on- and offline soft ionization techniques, which confirmed the presence of several organosulfates and nitrooxy-organosulfates in the particle phase. The chemical composition analysis was compared to hygroscopicity measurements derived from a cloud condensation nuclei counter. We observed that the hygroscopicity parameter (κ) that is derived from organic mass fractions determined by AMS measurements may overestimate the observed κ up to 0.2 if a high fraction of sulfate is bonded to organic molecules and little photochemical aging is exhibited.

  9. Long-term study of cloud condensation nuclei (CCN) activation of the atmospheric aerosol in Vienna

    PubMed Central

    Burkart, J.; Steiner, G.; Reischl, G.; Hitzenberger, R.

    2011-01-01

    During a total of 11 months, cloud condensation nuclei (CCN at super-saturation S 0.5%) and condensation nuclei (CN) concentrations were measured in the urban background aerosol of Vienna, Austria. For several months, number size distributions between 13.22 nm and 929 nm were also measured with a scanning mobility particle spectrometer (SMPS). Activation ratios (i.e. CCN/CN ratios) were calculated and apparent activation diameters obtained by integrating the SMPS size distributions. Variations in all CCN parameters (concentration, activation ratio, apparent activation diameter) are quite large on timescales of days to weeks. Passages of fronts influenced CCN parameters. Concentrations decreased with the passage of a front. No significant differences were found for fronts from different sectors (for Vienna mainly north to west and south to east). CCN concentrations at 0.5% S ranged from 160 cm−3 to 3600 cm−3 with a campaign average of 820 cm−3. Activation ratios were quite low (0.02–0.47, average: 0.13) and comparable to activation ratios found in other polluted regions (e.g. Cubison et al., 2008). Apparent activation diameters were found to be much larger (campaign average: 169 nm, range: (69–370) nm) than activation diameters for single-salt particles (around 50 nm depending on the salt). Contrary to CN concentrations, which are influenced by source patterns, CCN concentrations did not exhibit distinct diurnal patterns. Activation ratios showed diurnal variations counter-current to the variations of CN concentrations. PMID:21977003

  10. Elemental composition of aerosols in fourteen experiments of the Cloud Condensation Nuclei Workshop

    NASA Technical Reports Server (NTRS)

    Mach, W. H.; Hucek, R. R.

    1981-01-01

    Aeosols were collected with two Ci impactors and analyzed with proton induced X-ray emission (PIXE) for chemical composition and to detect if contamination was present. One of the impactors sampled the generated aerosols; the other impactor sampled droplets from a diffusion cloud chamber. The purpose of the experiments was to test the feasibility of a study of the transfer of chemical elements from the fine particle sizes to the coarse particle sizes, after CCN are activated and cloud droplets are formed. The data indicated that sulfur-containing aerosols did exhibit the expected transfer.

  11. Investigation of the seasonal variations of aerosol physicochemical properties and their impact on cloud condensation nuclei number concentration

    NASA Astrophysics Data System (ADS)

    Logan, Timothy S.

    Aerosols are among the most complex yet widely studied components of the atmosphere not only due to the seasonal variability of their physical and chemical properties but also their effects on climate change. The three main aerosol types that are known to affect the physics and chemistry of the atmosphere are: mineral dust, anthropogenic pollution, and biomass burning aerosols. In order to understand how these aerosols affect the atmosphere, this dissertation addresses the following three scientific questions through a combination of surface and satellite observations: SQ1: What are the seasonal and regional variations of aerosol physico-chemical properties at four selected Asian sites? SQ2: How do these aerosol properties change during transpacific and intra-continental long range transport? SQ3: What are the impacts of aerosol properties on marine boundary layer cloud condensation nuclei number concentration? This dissertation uses an innovative approach to classify aerosol properties by region and season to address SQ1. This is useful because this method provides an additional dimension when investigating the physico-chemical properties of aerosols by linking a regional and seasonal dependence to both the aerosol direct and indirect effects. This method involves isolating the aerosol physico-chemical properties into four separate regions using AERONET retrieved Angstrom exponent (AEAOD) and single scattering co-albedo (o oabs) to denote aerosol size and absorptive properties. The aerosols events are then clustered by season. The method is first applied to four AERONET sites representing single mode aerosol dominant regions: weakly absorbing pollution (NASA Goddard), strongly absorbing pollution (Mexico City), mineral dust (Solar Village), and biomass burning smoke (Alta Floresta). The method is then applied to four Asian sites that represent complicated aerosol components. There are strong regional and seasonal influences of the four aerosol types over the

  12. Secondary organic aerosol formation from isoprene photooxidation during cloud condensation-evaporation cycles

    NASA Astrophysics Data System (ADS)

    Brégonzio-Rozier, L.; Giorio, C.; Siekmann, F.; Pangui, E.; Morales, S. B.; Temime-Roussel, B.; Gratien, A.; Michoud, V.; Cazaunau, M.; DeWitt, H. L.; Tapparo, A.; Monod, A.; Doussin, J.-F.

    2016-02-01

    The impact of cloud events on isoprene secondary organic aerosol (SOA) formation has been studied from an isoprene / NOx / light system in an atmospheric simulation chamber. It was shown that the presence of a liquid water cloud leads to a faster and higher SOA formation than under dry conditions. When a cloud is generated early in the photooxidation reaction, before any SOA formation has occurred, a fast SOA formation is observed with mass yields ranging from 0.002 to 0.004. These yields are 2 and 4 times higher than those observed under dry conditions. When the cloud is generated at a later photooxidation stage, after isoprene SOA is stabilized at its maximum mass concentration, a rapid increase (by a factor of 2 or higher) of the SOA mass concentration is observed. The SOA chemical composition is influenced by cloud generation: the additional SOA formed during cloud events is composed of both organics and nitrate containing species. This SOA formation can be linked to the dissolution of water soluble volatile organic compounds (VOCs) in the aqueous phase and to further aqueous phase reactions. Cloud-induced SOA formation is experimentally demonstrated in this study, thus highlighting the importance of aqueous multiphase systems in atmospheric SOA formation estimations.

  13. A three-dimensional sectional representation of aerosol mixing state for simulating optical properties and cloud condensation nuclei

    SciTech Connect

    Ching, Ping Pui; Zaveri, Rahul A.; Easter, Richard C.; Riemer, Nicole; Fast, Jerome D.

    2016-05-27

    Light absorption by black carbon (BC) particles emitted from fossil fuel combustion depends on the how thickly they are coated with non-refractory species such as ammonium, sulfate, nitrate, organics, and water. The cloud condensation nuclei (CCN) activation property of a particle depends on its dry size and the hygroscopicities of all the individual species mixed together. It is therefore necessary to represent both size and mixing state of aerosols to reliably predict their climate-relevant properties in atmospheric models. Here we describe and evaluate a novel sectional framework in the Model for Simulating Aerosol Interactions and Chemistry, referred to as MOSAIC-mix, that represents the mixing state by resolving aerosol dry size (Ddry), BC dry mass fraction (wBC), and hygroscopicity (κ). Using ten idealized urban plume scenarios in which different types of aerosols evolve over 24 hours under a range of atmospherically relevant environmental conditions, we examine errors in CCN concentrations and optical properties with respect to a more explicit aerosol mixing state representation. We find that only a small number of wBC and κ bins are needed to achieve significant reductions in the errors, and propose a configuration consisting of 24 Ddry bins, 2 wBC bins, and 2 κ bins that gives 24-hour average errors of about 5% or less in CCN concentrations and optical properties, 3-4 times lower than those from size-only-resolved simulations. These results show that MOSAIC-mix is suitable for use in regional and global models to examine the effects of evolving aerosol mixing states on aerosol-radiation-cloud feedbacks.

  14. Characterisation of secondary organic aerosol formed during cloud condensation-evaporation cycles from isoprene photooxidation (CUMULUS project)

    NASA Astrophysics Data System (ADS)

    Giorio, Chiara; Bregonzio, Lola; Siekmann, Frank; Temime-Roussel, Brice; Ravier, Sylvain; Pangui, Edouard; Tapparo, Andrea; Kalberer, Markus; Monod, Anne; Doussin, Jean-François

    2014-05-01

    Biogenic volatile organic compounds (BVOCs) undergo many reactions in the atmosphere and form a wide range of oxidised and water-soluble compounds. These compounds could partition into atmospheric water droplets, and react within the aqueous phase producing higher molecular weight and less volatile compounds which could remain in the particle phase after water evaporation (Ervens et al., 2011). The aim of this work is the characterisation of secondary organic aerosol (SOA) formed from the photooxidation of isoprene and the effect of cloud water on SOA formation and composition. The experiments were performed during the CUMULUS project (CloUd MULtiphase chemistry of organic compoUndS in the troposphere), at the 4.2 m3 stainless steel CESAM chamber at LISA (Wang et al., 2011). In each experiment, isoprene was injected in the chamber together with HONO under dry conditions before irradiation. Gas phase compounds were analyzed on-line by a Proton Transfer Reaction Time of Flight Mass Spectrometer (PTR-ToF-MS), a Fourier Transform Infrared Spectrometer (FTIR), NOx and O3 analyzers. SOA formation and composition were analysed on-line with a Scanning Mobility Particle Sizer (SMPS) and an Aerodyne High Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS). Particular attention has been focused on SOA formation and aging during cloud condensation-evaporation cycles simulated in the smog chamber. In all experiments, we observed that during cloud formation water soluble gas-phase oxidation products readily partitioned into cloud droplets and new SOA was promptly produced which partly persisted after cloud evaporation. Chemical composition, elemental ratios and density of SOA, measured with the HR-ToF-AMS, were compared before, during cloud formation and after cloud evaporation. Experiments with other precursors, i.e. methacrolein, and effects of the presence of seeds were also investigated. Ervens, B. et al. (2011) Atmos. Chem. Phys. 11, 11069 11102. Wang, J. et al

  15. A broad supersaturation scanning (BS2) approach for rapid measurement of aerosol particle hygroscopicity and cloud condensation nuclei activity

    NASA Astrophysics Data System (ADS)

    Su, H.; Cheng, Y.; Ma, N.; Wang, Z.; Wang, X.; Pöhlker, M.; Nillius, B.; Wiedensohler, A.; Pöschl, U.

    2015-09-01

    The activation and hygroscopicity of cloud condensation nuclei (CCN) are key to understand aerosol-cloud interactions and their climate impact. It can be measured by scanning the particle size and supersaturation in CCN measurements. The scanning of supersaturation is often time-consuming and limits the temporal resolution and performance of CCN measurements. Here we present a new approach, termed broad supersaturation scanning (BS2) method, in which a range of supersaturation is simultaneously scanned reducing the time interval between different supersaturation scans. The practical applicability of the BS2 approach is demonstrated with nano-CCN measurements of laboratory-generated aerosol particles. Model simulations show that the BS2 approach is also applicable for measuring CCN activation of ambient mixed particles. Due to its fast response and technical simplicity, the BS2 approach may be well suited for long-term measurements. Since hygroscopicity is closely related to the fraction of organics/inorganics in aerosol particles, a BS2-CCN counter can also serve as a complementary sensor for fast detection/estimation of aerosol chemical compositions.

  16. A broad supersaturation scanning (BS2) approach for rapid measurement of aerosol particle hygroscopicity and cloud condensation nuclei activity

    NASA Astrophysics Data System (ADS)

    Su, Hang; Cheng, Yafang; Ma, Nan; Wang, Zhibin; Wang, Xiaoxiang; Pöhlker, Mira L.; Nillius, Björn; Wiedensohler, Alfred; Pöschl, Ulrich

    2016-10-01

    The activation and hygroscopicity of cloud condensation nuclei (CCN) are key to the understanding of aerosol-cloud interactions and their impact on climate. They can be measured by scanning the particle size and supersaturation in CCN measurements. The scanning of supersaturation is often time-consuming and limits the temporal resolution and performance of CCN measurements. Here we present a new approach, termed the broad supersaturation scanning (BS2) method, in which a range of supersaturation is simultaneously scanned, reducing the time interval between different supersaturation scans. The practical applicability of the BS2 approach is demonstrated with nano-CCN measurements of laboratory-generated aerosol particles. Model simulations show that the BS2 approach may also be applicable for measuring CCN activation of ambient mixed particles. Due to its fast response and technical simplicity, the BS2 approach may be well suited for aircraft and long-term measurements. Since hygroscopicity is closely related to the fraction of organics/inorganics in aerosol particles, a BS2-CCN counter can also serve as a complementary sensor for fast detection/estimation of aerosol chemical compositions.

  17. Aerosol- and updraft-limited regimes of cloud droplet formation: influence of particle number, size and hygroscopicity on the activation of cloud condensation nuclei (CCN)

    NASA Astrophysics Data System (ADS)

    Reutter, P.; Su, H.; Trentmann, J.; Simmel, M.; Rose, D.; Gunthe, S. S.; Wernli, H.; Andreae, M. O.; Pöschl, U.

    2009-09-01

    We have investigated the formation of cloud droplets under pyro-convective conditions using a cloud parcel model with detailed spectral microphysics and with the κ-Köhler model approach for efficient and realistic description of the cloud condensation nucleus (CCN) activity of aerosol particles. Assuming a typical biomass burning aerosol size distribution (accumulation mode centred at 120 nm), we have calculated initial cloud droplet number concentrations (NCD) for a wide range of updraft velocities (w=0.25-20 m s-1) and aerosol particle number concentrations (NCN=200-105 cm-3) at the cloud base. Depending on the ratio between updraft velocity and particle number concentration (w/NCN), we found three distinctly different regimes of CCN activation and cloud droplet formation: (1) An aerosol-limited regime that is characterized by high w/NCN ratios (>≈10-3 m s-1 cm3), high maximum values of water vapour supersaturation (Smax>≈0.5%), and high activated fractions of aerosol particles (NCN/NCN>≈90%). In this regime NCD is directly proportional to NCN and practically independent of w. (2) An updraft-limited regime that is characterized by low w/NCN ratios (<≈10-4 m s-1 cm3), low maximum values of water vapour supersaturation (Smax<≈0.2%), and low activated fractions of aerosol particles (NCD/NCN<≈20%). In this regime NCD is directly proportional to w and practically independent of NCN. (3) An aerosol- and updraft-sensitive regime (transitional regime), which is characterized by parameter values in between the two other regimes and covers most of the conditions relevant for pyro-convection. In this regime NCD depends non-linearly on both NCN and w. In sensitivity studies we have tested the influence of aerosol particle size distribution and hygroscopicity on NCD. Within the range of effective hygroscopicity parameters that is characteristic for continental atmospheric aerosols (κ≈0.05-0.6), we found that NCD depends rather weakly on the actual value of κ

  18. Hygroscopic properties of urban aerosols and their cloud condensation nuclei activities measured in Seoul during the MAPS-Seoul campaign

    NASA Astrophysics Data System (ADS)

    Kim, Najin; Park, Minsu; Yum, Seong Soo; Park, Jong Sung; Song, In Ho; Shin, Hye Jung; Ahn, Joon Young; Kwak, Kyung-Hwan; Kim, Hwajin; Bae, Gwi-Nam; Lee, Gangwoong

    2017-03-01

    Aerosol physical properties, chemical compositions, hygroscopicity and cloud condensation nuclei (CCN) activities were measured in Seoul, the highly populated capital city of Korea, during the Megacity Air Pollution Studies (MAPS-Seoul) campaign, in May-June 2015. The average aerosol concentration for particle diameters >10 nm was 11787 ± 7421 cm-3 with dominant peaks at morning rush hours and in the afternoon due to frequent new particle formation (NPF) events. The average CCN concentration was 4075 ± 1812 cm-3 at 0.6% supersaturation, with little diurnal variation. The average hygroscopicity parameter (κ) value determined using a humidified tandem differential mobility analyzer (HTDMA) ranged 0.17-0.27 for a range of particle diameters (30-150 nm). The κ values derived using the aerosol mass spectrometer (AMS) data with three different methods were 0.32-0.34, significantly higher than those from HTDMA due to the uncertainties in the hygroscopicity values of different chemical compositions, especially organics and black carbon. Factors affecting the aerosol hygroscopicity seemed to be traffic and chemical processes during the NPF events. The CCN concentration predicted based on HTDMA κ data showed very good agreement with the measured one. Because of the overestimation of κ, CCN closure with the predicted CCN concentration based on AMS κ data over-predicted CCN concentration although the linear correlation between measured and predicted CCN concentration was still very good.

  19. Direct Observation of Secondary Organic Aerosol Formation during Cloud Condensation-Evaporation Cycles (SOAaq) in Simulation Chamber Experiments

    NASA Astrophysics Data System (ADS)

    Doussin, J. F.; Bregonzio-Rozier, L.; Giorio, C.; Siekmann, F.; Gratien, A.; Temime-Roussel, B.; Ravier, S.; Pangui, E.; Tapparo, A.; Kalberer, M.; Monod, A.

    2014-12-01

    Biogenic volatile organic compounds (BVOCs) undergo many reactions in the atmosphere and form a wide range of oxidised and water-soluble compounds. These compounds can partition into atmospheric water droplets, and react within the aqueous phase producing higher molecular weight and/or less volatile compounds which can remain in the particle phase after water evaporation and thus increase the organic aerosol mass (Ervens et al., 2011; Altieri et al., 2008; Couvidat et al., 2013). While this hypothesis is frequently discussed in the literature, so far, almost no direct observations of such a process have been provided.The aim of the present work is to study SOA formation from isoprene photooxidation during cloud condensation-evaporation cycles.The experiments were performed during the CUMULUS project (CloUd MULtiphase chemistry of organic compoUndS in the troposphere), in the CESAM simulation chamber located at LISA. CESAM is a 4.2 m3 stainless steel chamber equipped with realistic irradiation sources and temperature and relative humidity (RH) controls (Wang et al., 2011). In each experiment, isoprene was allowed to oxidize during several hours in the presence on nitrogen oxides under dry conditions. Gas phase compounds were analyzed on-line by a Proton Transfer Reaction Time of Flight Mass Spectrometer (PTR-ToF-MS), a Fourier Transform Infrared Spectrometer (FTIR), NOx and O3 analyzers. SOA formation was monitored on-line with a Scanning Mobility Particle Sizer (SMPS) and an Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS). The experimental protocol was optimised to generate cloud events in the simulation chamber, which allowed us to generate clouds lasting for ca. 10 minutes in the presence of light.In all experiments, we observed that during cloud formation, water-soluble gas-phase oxidation products (e.g., methylglyoxal, hydroxyacetone, acetaldehyde, formic acid, acetic acid and glycolaldehyde) readily partitioned into cloud

  20. Thermochemical, cloud condensation nucleation ability and optical properties of alkyl aminium sulfate aerosols

    NASA Astrophysics Data System (ADS)

    Lavi, A.; Bluvshtein, N.; Segre, E.; Segev, L.; Flores, J.; Rudich, Y.

    2013-12-01

    The increased interest in the chemistry of alkylamines and their possible roles in the atmosphere increased recently due to field observations of the correlation between new particle formation and post nucleation growth events and the presence of alkylamines in their cationic form. Due to their high saturation vapor pressure it is unlikely that short chain alkylamines will contribute to particle formation or growth by condensation. Therefore, it was previously suggested that their contribution to particulate phase is the result of acid-base reactions between the basic alkylamines and atmospherically relevant acids such as sulfuric and nitric acid. In this study we present laboratory data on the thermochemical, CCN activity and optical properties of selected atmospherically relevant alkyl aminium sulfate salts: Monomethyl aminium sulfate (MMAS), dimethyaminium sulfate (DMAS), trimethylaminium sulfate, monoethylaminium sulfate (MEAS), diethylaminium sulfate (DEAS) and triethylaminium sulfate (TEAS)). We found that the vapor pressure of these aminium salts is 1-3 orders of magnitude lower than that of ammonium sulfate and as such they can contribute to new aerosols and secondary aerosols formation. We infer that these species have very high CCN activity, with hygroscopicity parameter that is lower but close to that ammonium sulfate. Finally, we present the optical properties of these alkyl aminium sulfate salts between 360 and 420 nm. These compounds are less scattering than ammonium sulfate and show minimal wavelength dependence in this range. These compounds also do not absorb light. These derived parameters can contribute to the better understanding and characterization of the role that these compounds play in atmospheric chemical reactions, gas-solid partitioning and their possible contribution to the microphysical and radiative effects of atmospheric aerosols.

  1. Chemical Aging and Cloud Condensation Nuclei Activity of Biomass Burning Aerosol Proxies in the Presence of OH Radicals

    NASA Astrophysics Data System (ADS)

    Slade, Jonathan H., Jr.

    Biomass burning aerosol (BBA) can adversely impact regional and global air quality and represents a significant source of organic aerosol (OA) to the atmosphere that can affect climate. Aerosol particles can alter the transfer of radiation in earth's atmosphere directly by scattering and absorbing radiation or indirectly via cloud formation. Gas-to-particle, also termed heterogeneous, oxidation reactions can significantly alter the particle's physical and chemical properties. In turn, this can lead to the degradation of biomolecular markers for air quality-related aerosol source apportionment studies, the particles' lifetime, and modify the particles' abilities to serve as cloud condensation nuclei (CCN). However, the rates, mechanisms, and conditions by which these multiphase oxidation reactions occur and influence the CCN activity of OA is not well understood. The work presented here aims to determine the reactivity and products from the interaction of BBA surrogate-particles and trace gas-phase oxidants and to link the effects of OA chemical aging on the particles' ability to nucleate clouds. The reactive uptake of OH by BBA surrogate-substrates and particles, including levoglucosan, nitroguaiacol, abietic acid, and methyl-nitrocatechol, was determined as a function of both OH concentration and relative humidity (RH) using chemical ionization mass spectrometry coupled to various flow reactors. OH reactive uptake decreased with increasing OH concentration, indicative of OH adsorption followed by reaction. OH oxidation led to significant volatilization, i.e. mass loss of the organic material, as determined by application of high resolution proton transfer reaction time-of-flight mass spectrometry. Volatilized reaction products were identified, providing mechanistic insight of the chemical pathways in the heterogeneous OH oxidation of BBA. The reactive uptake of OH by levoglucosan particles increased with RH due to enhanced OH and organic bulk diffusivity. In

  2. Soot Aerosol Particles as Cloud Condensation Nuclei: from Ice Nucleation Activity to Ice Crystal Morphology

    NASA Astrophysics Data System (ADS)

    Pirim, Claire; Ikhenazene, Raouf; Ortega, Isamel Kenneth; Carpentier, Yvain; Focsa, Cristian; Chazallon, Bertrand; Ouf, François-Xavier

    2016-04-01

    Emissions of solid-state particles (soot) from engine exhausts due to incomplete fuel combustion is considered to influence ice and liquid water cloud droplet activation [1]. The activity of these aerosols would originate from their ability to be important centers of ice-particle nucleation, as they would promote ice formation above water homogeneous freezing point. Soot particles are reported to be generally worse ice nuclei than mineral dust because they activate nucleation at higher ice-supersaturations for deposition nucleation and at lower temperatures for immersion freezing than ratios usually expected for homogeneous nucleation [2]. In fact, there are still numerous opened questions as to whether and how soot's physico-chemical properties (structure, morphology and chemical composition) can influence their nucleation ability. Therefore, systematic investigations of soot aerosol nucleation activity via one specific nucleation mode, here deposition nucleation, combined with thorough structural and compositional analyzes are needed in order to establish any association between the particles' activity and their physico-chemical properties. In addition, since the morphology of the ice crystals can influence their radiative properties [3], we investigated their morphology as they grow over both soot and pristine substrates at different temperatures and humidity ratios. In the present work, Combustion Aerosol STandart soot samples were produced from propane using various experimental conditions. Their nucleation activity was studied in deposition mode (from water vapor), and monitored using a temperature-controlled reactor in which the sample's relative humidity is precisely measured with a cryo-hygrometer. Formation of water/ice onto the particles is followed both optically and spectroscopically, using a microscope coupled to a Raman spectrometer. Vibrational signatures of hydroxyls (O-H) emerge when the particle becomes hydrated and are used to characterize ice

  3. Chemical aging of single and multicomponent biomass burning aerosol surrogate particles by OH: implications for cloud condensation nucleus activity

    NASA Astrophysics Data System (ADS)

    Slade, J. H.; Thalman, R.; Wang, J.; Knopf, D. A.

    2015-09-01

    Multiphase OH and O3 oxidation reactions with atmospheric organic aerosol (OA) can influence particle physicochemical properties including composition, morphology, and lifetime. Chemical aging of initially insoluble or low-soluble single-component OA by OH and O3 can increase their water solubility and hygroscopicity, making them more active as cloud condensation nuclei (CCN) and susceptible to wet deposition. However, an outstanding problem is whether the effects of chemical aging on their CCN activity are preserved when mixed with other organic or inorganic compounds exhibiting greater water solubility. In this work, the CCN activity of laboratory-generated biomass burning aerosol (BBA) surrogate particles exposed to OH and O3 is evaluated by determining the hygroscopicity parameter, κ, as a function of particle type, mixing state, and OH and O3 exposure applying a CCN counter (CCNc) coupled to an aerosol flow reactor (AFR). Levoglucosan (LEV), 4-methyl-5-nitrocatechol (MNC), and potassium sulfate (KS) serve as representative BBA compounds that exhibit different hygroscopicity, water solubility, chemical functionalities, and reactivity with OH radicals, and thus exemplify the complexity of mixed inorganic/organic aerosol in the atmosphere. The CCN activities of all of the particles were unaffected by O3 exposure. Following exposure to OH, κ of MNC was enhanced by an order of magnitude, from 0.009 to ~ 0.1, indicating that chemically aged MNC particles are better CCN and more prone to wet deposition than pure MNC particles. No significant enhancement in κ was observed for pure LEV particles following OH exposure. κ of the internally mixed particles was not affected by OH oxidation. Furthermore, the CCN activity of OH-exposed MNC-coated KS particles is similar to the OH unexposed atomized 1 : 1 by mass MNC : KS binary-component particles. Our results strongly suggest that when OA is dominated by water-soluble organic carbon (WSOC) or inorganic ions, chemical

  4. Chemical aging of single and multicomponent biomass burning aerosol surrogate-particles by OH: implications for cloud condensation nucleus activity

    NASA Astrophysics Data System (ADS)

    Slade, J. H.; Thalman, R.; Wang, J.; Knopf, D. A.

    2015-03-01

    Multiphase OH and O3 oxidation reactions with atmospheric organic aerosol (OA) can influence particle physicochemical properties including composition, morphology, and lifetime. Chemical aging of initially insoluble or low soluble single-component OA by OH and O3 can increase their water-solubility and hygroscopicity, making them more active as cloud condensation nuclei (CCN) and susceptible to wet deposition. However, an outstanding problem is whether the effects of chemical aging on their CCN activity are preserved when mixed with other organic or inorganic compounds exhibiting greater water-solubility. In this work, the CCN activity of laboratory-generated biomass burning aerosol (BBA) surrogate-particles exposed to OH and O3 is evaluated by determining the hygroscopicity parameter, κ, as a function of particle type, mixing state, and OH/O3 exposure applying a CCN counter (CCNc) coupled to an aerosol flow reactor (AFR). Levoglucosan (LEV), 4-methyl-5-nitrocatechol (MNC), and potassium sulfate (KS) serve as representative BBA compounds that exhibit different hygroscopicity, water solubility, chemical functionalities, and reactivity with OH radicals, and thus exemplify the complexity of mixed inorganic/organic aerosol in the atmosphere. The CCN activities of all of the particles were unaffected by O3 exposure. Following exposure to OH, κ of MNC was enhanced by an order of magnitude, from 0.009 to ~0.1, indicating that chemically-aged MNC particles are better CCN and more prone to wet deposition than pure MNC particles. No significant enhancement in κ was observed for pure LEV particles following OH exposure. κ of the internally-mixed particles was not affected by OH oxidation. Furthermore, the CCN activity of OH exposed MNC-coated KS particles is similar to the OH unexposed atomized 1 : 1 by mass MNC : KS binary-component particles. Our results strongly suggest that when OA is dominated by water-soluble organic carbon (WSOC) or inorganic ions, chemical aging

  5. Chemical aging of single and multicomponent biomass burning aerosol surrogate-particles by OH: Implications for cloud condensation nucleus activity

    DOE PAGES

    Thalman, R.; Thalman, R.; Wang, J.; ...

    2015-03-06

    Multiphase OH and O₃ oxidation reactions with atmospheric organic aerosol (OA) can influence particle physicochemical properties including composition, morphology, and lifetime. Chemical aging of initially insoluble or low soluble single-component OA by OH and O₃ can increase their water-solubility and hygroscopicity, making them more active as cloud condensation nuclei (CCN) and susceptible to wet deposition. However, an outstanding problem is whether the effects of chemical aging on their CCN activity are preserved when mixed with other organic or inorganic compounds exhibiting greater water-solubility. In this work, the CCN activity of laboratory-generated biomass burning aerosol (BBA) surrogate-particles exposed to OH andmore » O₃ is evaluated by determining the hygroscopicity parameter, κ, as a function of particle type, mixing state, and OH/O₃ exposure applying a CCN counter (CCNc) coupled to an aerosol flow reactor (AFR). Levoglucosan (LEV), 4-methyl-5-nitrocatechol (MNC), and potassium sulfate (KS) serve as representative BBA compounds that exhibit different hygroscopicity, water solubility, chemical functionalities, and reactivity with OH radicals, and thus exemplify the complexity of mixed inorganic/organic aerosol in the atmosphere. The CCN activities of all of the particles were unaffected by O₃ exposure. Following exposure to OH, κ of MNC was enhanced by an order of magnitude, from 0.009 to ~0.1, indicating that chemically-aged MNC particles are better CCN and more prone to wet deposition than pure MNC particles. No significant enhancement in κ was observed for pure LEV particles following OH exposure. κ of the internally-mixed particles was not affected by OH oxidation. Furthermore, the CCN activity of OH exposed MNC-coated KS particles is similar to the OH unexposed atomized 1:1 by mass MNC: KS binary-component particles. Our results strongly suggest that when OA is dominated by water-soluble organic carbon (WSOC) or inorganic ions

  6. Chemical aging of single and multicomponent biomass burning aerosol surrogate particles by OH: implications for cloud condensation nucleus activity

    DOE PAGES

    Slade, J. H.; Thalman, R.; Wang, J.; ...

    2015-09-14

    Multiphase OH and O3 oxidation reactions with atmospheric organic aerosol (OA) can influence particle physicochemical properties including composition, morphology, and lifetime. Chemical aging of initially insoluble or low-soluble single-component OA by OH and O3 can increase their water solubility and hygroscopicity, making them more active as cloud condensation nuclei (CCN) and susceptible to wet deposition. However, an outstanding problem is whether the effects of chemical aging on their CCN activity are preserved when mixed with other organic or inorganic compounds exhibiting greater water solubility. In this work, the CCN activity of laboratory-generated biomass burning aerosol (BBA) surrogate particles exposed tomore » OH and O3 is evaluated by determining the hygroscopicity parameter, κ, as a function of particle type, mixing state, and OH and O3 exposure applying a CCN counter (CCNc) coupled to an aerosol flow reactor (AFR). Levoglucosan (LEV), 4-methyl-5-nitrocatechol (MNC), and potassium sulfate (KS) serve as representative BBA compounds that exhibit different hygroscopicity, water solubility, chemical functionalities, and reactivity with OH radicals, and thus exemplify the complexity of mixed inorganic/organic aerosol in the atmosphere. The CCN activities of all of the particles were unaffected by O3 exposure. Following exposure to OH, κ of MNC was enhanced by an order of magnitude, from 0.009 to ~ 0.1, indicating that chemically aged MNC particles are better CCN and more prone to wet deposition than pure MNC particles. No significant enhancement in κ was observed for pure LEV particles following OH exposure. κ of the internally mixed particles was not affected by OH oxidation. Furthermore, the CCN activity of OH-exposed MNC-coated KS particles is similar to the OH unexposed atomized 1 : 1 by mass MNC : KS binary-component particles. Our results strongly suggest that when OA is dominated by water-soluble organic carbon (WSOC) or inorganic ions

  7. Chemical aging of single and multicomponent biomass burning aerosol surrogate-particles by OH: Implications for cloud condensation nucleus activity

    SciTech Connect

    Thalman, R.; Thalman, R.; Wang, J.; Knopf, D. A.

    2015-03-06

    Multiphase OH and O₃ oxidation reactions with atmospheric organic aerosol (OA) can influence particle physicochemical properties including composition, morphology, and lifetime. Chemical aging of initially insoluble or low soluble single-component OA by OH and O₃ can increase their water-solubility and hygroscopicity, making them more active as cloud condensation nuclei (CCN) and susceptible to wet deposition. However, an outstanding problem is whether the effects of chemical aging on their CCN activity are preserved when mixed with other organic or inorganic compounds exhibiting greater water-solubility. In this work, the CCN activity of laboratory-generated biomass burning aerosol (BBA) surrogate-particles exposed to OH and O₃ is evaluated by determining the hygroscopicity parameter, κ, as a function of particle type, mixing state, and OH/O₃ exposure applying a CCN counter (CCNc) coupled to an aerosol flow reactor (AFR). Levoglucosan (LEV), 4-methyl-5-nitrocatechol (MNC), and potassium sulfate (KS) serve as representative BBA compounds that exhibit different hygroscopicity, water solubility, chemical functionalities, and reactivity with OH radicals, and thus exemplify the complexity of mixed inorganic/organic aerosol in the atmosphere. The CCN activities of all of the particles were unaffected by O₃ exposure. Following exposure to OH, κ of MNC was enhanced by an order of magnitude, from 0.009 to ~0.1, indicating that chemically-aged MNC particles are better CCN and more prone to wet deposition than pure MNC particles. No significant enhancement in κ was observed for pure LEV particles following OH exposure. κ of the internally-mixed particles was not affected by OH oxidation. Furthermore, the CCN activity of OH exposed MNC-coated KS particles is similar to the OH unexposed atomized 1:1 by mass MNC: KS binary-component particles. Our results strongly suggest that when OA is dominated by water-soluble organic carbon (WSOC) or inorganic ions, chemical

  8. Titan's Stratospheric Aerosols and Condensate Clouds as Observed with Cassini CIRS

    NASA Astrophysics Data System (ADS)

    de Kok, Remco; Irwin, P. G.; Teanby, N. A.; Samuelson, R. E.; Nixon, C. A.; Jennings, D. E.; Fletcher, L.; Howett, C.; Calcutt, S. B.; Bowles, N. E.; Flasar, F. M.; Taylor, F. W.; Cassini/CIRS Team

    2006-09-01

    Four broad spectral features were identified in far-infrared limb spectra from the Cassini Composite Infrared Spectrometer (CIRS). The features are broader than the spectral resolution, which suggests that they are caused by particulates in Titan's stratosphere. We derive here the spectral properties and variations with altitude and latitude for these four features. Titan's main aerosol is called Haze 0 here. It is present at all wavenumbers in the far-infrared and is found to have a fractional scale height between 1.6-1.7 with a small increase in opacity in the north. A second feature around 140 cm-1 (Haze A) has similar spatial properties to Haze 0, but has a smaller fractional scale height of 1.2-1.3. Both Haze 0 and Haze A show an increase in abundance below 100 km, perhaps indicative of a scattering cloud. Two other features (Haze B around 220 cm-1 and Haze C around 190 cm-1) have a large maximum in their density profiles at 140 km and 90 km respectively. Haze B is much more abundant in the northern hemisphere compared to the southern hemisphere. Haze C also shows a large increase towards the north, but then disappears at 85oN. This work is supported by the Prins Bernhard Cultuurfond and Pieter Beijer Fonds.

  9. Surfactant effect on cloud condensation nuclei for two-component internally mixed aerosols

    NASA Astrophysics Data System (ADS)

    Petters, Sarah Suda; Petters, Markus Dirk

    2016-02-01

    This work presents experimental data on the cloud condensation nuclei (CCN) activity of two-component mixtures containing surfactants. Nine binary systems were tested combining strong ionic (sodium dodecyl sulfate) and nonionic surfactants (Zonyl FS-300 and Triton X-100) with nonsurfactant compounds (glucose, ammonium sulfate, or sodium chloride). Control tests were performed for systems combining organic (glucose) and inorganic compounds (ammonium sulfate or sodium chloride). Results show that CCN activity deviates strongly relative to predictions made from measurements of bulk surface tension. Köhler theory accounting for surface tension reduction and surface partitioning underpredicts the CCN activity of particles containing Zonyl FS-300 and Triton X-100. Partitioning theory better describes data for Zonyl FS-300 and Triton X-100 when limiting surface adsorption to 1.5 monolayers of the growing drop. Deviations from predictions were observed. Likely explanations include solute-solute interactions and nonspherical particle shape. The findings presented here examine in detail the perturbation of CCN activity by surfactants and may offer insight into both the success and limitations of physical models describing CCN activity of surface active molecules.

  10. Separating Cloud Forming Nuclei from Interstitial Aerosol

    SciTech Connect

    Kulkarni, Gourihar R.

    2012-09-12

    It has become important to characterize the physicochemical properties of aerosol that have initiated the warm and ice clouds. The data is urgently needed to better represent the aerosol-cloud interaction mechanisms in the climate models. The laboratory and in-situ techniques to separate precisely the aerosol particles that act as cloud condensation nuclei (CCN) and ice nuclei (IN), termed as cloud nuclei (CN) henceforth, have become imperative in studying aerosol effects on clouds and the environment. This review summarizes these techniques, design considerations, associated artifacts and challenges, and briefly discusses the need for improved designs to expand the CN measurement database.

  11. Aerosol generation and distribution system for the Third International Cloud Condensation Nuclei Workshop

    NASA Technical Reports Server (NTRS)

    Katz, U.; Dea, J. Y.

    1981-01-01

    In order to obtain identical samples participating CCN instruments and aerosol characterizing equipment were located along and connected to a 8.2 cm diameter aluminum tube through which the test aerosols were pumped directly from the source at very slight overpressure. Of the total of 29 experiments, 18 were carried out with artificial NaCl or (NH4)2SO4 aerosols. These were generated from salt solutions by pneumatic atomizers of special design to ensure high constancy of the aerosol output concentration. In three experiments with insoluble CCN (AgI, paraffin wax) the aerosols were generated thermally. In some of the tests, an electrostatic classifier was used for narrowing the particle size distributions.

  12. Aerosol measurements at a high-elevation site: composition, size, and cloud condensation nuclei activity

    SciTech Connect

    Friedman, Beth; Zelenyuk, Alla; Beranek, Josef; Kulkarni, Gourihar R.; Pekour, Mikhail S.; Hallar, Anna G.; McCubbin, Ian; Thornton, Joel A.; Cziczo, D. J.

    2013-12-09

    We present measurements of CCN concentrations and associated aerosol composition and size properties at a high-elevation research site in March 2011. CCN closure and aerosol hygroscopicity were assessed using simplified assumptions of bulk aerosol properties as well as a new method utilizing single particle composition and size to assess the importance of particle mixing state in CCN activation. Free troposphere analysis found no significant difference between the CCN activity of free tropospheric aerosol and boundary layer aerosol at this location. Closure results indicate that using only size and number information leads to adequate prediction, in the majority of cases within 50%, of CCN concentrations, while incorporating the hygroscopicity parameters of the individual aerosol components measured by single particle mass spectrometry adds to the agreement, in most cases within 20%, between predicted and measured CCN concentrations. For high-elevation continental sites, with largely aged aerosol and low amounts of local area emissions, a lack of chemical knowledge and hygroscopicity may not hinder models in predicting CCN concentrations. At sites influenced by fresh emissions or more heterogeneous particle types, single particle composition information may be more useful in predicting CCN concentrations and understanding the importance of particle mixing state on CCN activation.

  13. Cloud Condensation Nuclei Activity, Droplet Growth Kinetics and Hygroscopicity of Biogenic and Anthropogenic Secondary Organic Aerosol (SOA)

    NASA Astrophysics Data System (ADS)

    Zhao, Defeng; Buchholz, Angela; Kortner, Birthe; Schlag, Patrick; Rubach, Florian; Hendrik, Fucks; Kiendler-Scharr, Astrid; Tillmann, Ralf; Wahner, Andreas; Hallquist, Mattias; Flores, Michel; Rudich, Yinon; Glasius, Marianne; Kourtchev, Ivan; Kalberer, Markus; Mentel, Thomas

    2015-04-01

    Recent field data and model analysis show that secondary organic aerosol (SOA) formation is enhanced under anthropogenic influences (de Gouw et al. 2005, Spracklen et al. 2011). The interaction of biogenic VOCs (BVOCs) with anthropogenic emissions such as anthropogenic VOCs (AVOCs) could change the particle formation yields and the aerosol properties, as was recently demonstrated (Emanuelsson et al., 2013; Flores et al., 2014). However, the effect of the interaction of BVOCs with AVOCs on cloud condensation nuclei (CCN) activity and hygroscopicity of SOA remains elusive. Characterizing such changes is necessary in order to assess the indirect radiative forcing of biogenic aerosols that form under anthropogenic influence. In this study, we investigated the influence of AVOCs on CCN activation and hygroscopic growth of BSOA. SOA was formed from photooxidation of monoterpenes and aromatics as representatives of BVOCs and AVOCs, respectively. The hygroscopicity and CCN activation of BSOA were studied and compared with that of anthropogenic SOA (ASOA) and the mixture of ASOA and BSOA (ABSOA). We found that ASOA had a significantly higher hygroscopicity than BSOA at similar OH dose, which is attributed to a higher oxidation level of ASOA. While the ASOA fraction had an enhancing effect on the hygroscopicity of ABSOA compared to BSOA, the hygroscopicity of ABSOA cannot be explained by a linear combination of the pure ASOA and BSOA systems, indicating potentially additional non-linear effects such as oligomerization. However, in contrast to hygroscopicity, ASOA showed similar CCN activity as BSOA, in spite of its higher oxidation level. The ASOA fraction did not enhance the CCN activity of ABSOA. The discrepancy between hygroscopicity and CCN activity is discussed. In addition, BSOA, ABSOA and ASOA formed similar droplet size with ammonium sulfate in CCN at a given supersaturation, indicating none of these aerosols had a delay in the water uptake in the supersaturated

  14. Cloud condensation nuclei near marine cumulus

    NASA Technical Reports Server (NTRS)

    Hudson, James G.

    1993-01-01

    Extensive airborne measurements of cloud condensation nucleus (CCN) spectra and condensation nuclei below, in, between, and above the cumulus clouds near Hawaii point to important aerosol-cloud interactions. Consistent particle concentrations of 200/cu cm were found above the marine boundary layer and within the noncloudy marine boundary layer. Lower and more variable CCN concentrations within the cloudy boundary layer, especially very close to the clouds, appear to be a result of cloud scavenging processes. Gravitational coagulation of cloud droplets may be the principal cause of this difference in the vertical distribution of CCN. The results suggest a reservoir of CCN in the free troposphere which can act as a source for the marine boundary layer.

  15. Pre-Cloud Aerosol, Cloud Droplet Concentration, and Cloud Condensation Nuclei from the VAMOS Ocean-Cloud-Atmosphere Land Study (VOCALS) Field Campaign First Quarter 2010 ASR Program Metric Report

    SciTech Connect

    Kleinman, LI; Springston, SR; Daum, PH; Lee, Y-N; Sedlacek, AJ; Senum, G; Wang, J

    2011-08-31

    In this, the first of a series of Program Metric Reports, we (1) describe archived data from the DOE G-1 aircraft, (2) illustrate several relations between sub-cloud aerosol, CCN, and cloud droplets pertinent to determining the effects of pollutant sources on cloud properties, and (3) post to the data archive an Excel spreadsheet that contains cloud and corresponding sub-cloud data.

  16. Characterisation of Secondary Organic Aerosol Formed from the Photooxidation of Isoprene during Cloud Condensation-Evaporation Cycles (CUMULUS Project)

    NASA Astrophysics Data System (ADS)

    Doussin, J. F.; Giorio, C.; Bregonzio-Rozier, L.; Siekmann, F.; Temime-Roussel, B.; Gratien, A.; Ravier, S.; Pangui, E.; Tapparo, A.; Kalberer, M.; Vermeylen, R.; Claeys, M.; Monod, A.

    2014-12-01

    Biogenic volatile organic compounds (BVOCs) undergo many oxidation processes in the atmosphere accompanied by formation of water-soluble compounds. These compounds could partition into atmospheric water droplets, and react within the aqueous phase producing higher molecular weight and less volatile compounds which could form new aerosol (Ervens et al., 2011). This work investigates the formation and composition of secondary organic aerosol (SOA) from the photooxidation of isoprene and methacrolein (its main first-generation oxidation product) and the effect of cloud water on SOA formation and composition. The experiments were performed within the CUMULUS project (CloUd MULtiphase chemistry of organic compoUndS in the troposphere) at the 4.2 m3 stainless steel CESAM chamber (Wang et al., 2011). In each experiment, isoprene or methacrolein was injected in the chamber together with HONO under dry conditions before irradiation. The experimental protocol was optimised to generate cloud events in the chamber, lasting for ca. 10 minutes in the presence of light. Gas phase compounds were analyzed on-line by a Proton Transfer Reaction Time of Flight Mass Spectrometer (PTR-ToF-MS), a Fourier Transform Infrared Spectrometer (FTIR), NOx and O3 analyzers. SOA formation and composition were analysed on-line with a Scanning Mobility Particle Sizer (SMPS) and an Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and off-line through sampling on filters and analysis in GC-MS and LC-MS. We observed that during cloud formation water soluble gas-phase oxidation products readily partitioned into cloud droplets and new SOA was promptly produced. Chemical composition, elemental ratios and density of SOA were compared before, during cloud formation and after cloud evaporation. Ervens, B. et al. (2011) Atmos. Chem. Phys. 11, 11069-11102. Wang, J. et al. (2011) Atmos. Measur. Tech. 4, 2465-2494.

  17. Size-resolved aerosol and cloud condensation nuclei (CCN) properties in the remote marine South China Sea - Part 1: Observations and source classification

    NASA Astrophysics Data System (ADS)

    Atwood, Samuel A.; Reid, Jeffrey S.; Kreidenweis, Sonia M.; Blake, Donald R.; Jonsson, Haflidi H.; Lagrosas, Nofel D.; Xian, Peng; Reid, Elizabeth A.; Sessions, Walter R.; Simpas, James B.

    2017-01-01

    Ship-based measurements of aerosol and cloud condensation nuclei (CCN) properties are presented for 2 weeks of observations in remote marine regions of the South China Sea/East Sea during the southwestern monsoon (SWM) season. Smoke from extensive biomass burning throughout the Maritime Continent advected into this region during the SWM, where it was mixed with anthropogenic continental pollution and emissions from heavy shipping activities. Eight aerosol types were identified using a k-means cluster analysis with data from a size-resolved CCN characterization system. Interpretation of the clusters was supplemented by additional onboard aerosol and meteorological measurements, satellite, and model products for the region. A typical bimodal marine boundary layer background aerosol population was identified and observed mixing with accumulation mode aerosol from other sources, primarily smoke from fires in Borneo and Sumatra. Hygroscopicity was assessed using the κ parameter and was found to average 0.40 for samples dominated by aged accumulation mode smoke; 0.65 for accumulation mode marine aerosol; 0.60 in an anthropogenic aerosol plume; and 0.22 during a short period that was characterized by elevated levels of volatile organic compounds not associated with biomass burning impacts. As a special subset of the background marine aerosol, clean air masses substantially scrubbed of particles were observed following heavy precipitation or the passage of squall lines, with changes in observed aerosol properties occurring on the order of minutes. Average CN number concentrations, size distributions, and κ values are reported for each population type, along with CCN number concentrations for particles that activated at supersaturations between 0.14 and 0.85 %.

  18. AEROSOL, CLOUDS, AND CLIMATE CHANGE

    SciTech Connect

    SCHWARTZ, S.E.

    2005-09-01

    Earth's climate is thought to be quite sensitive to changes in radiative fluxes that are quite small in absolute magnitude, a few watts per square meter, and in relation to these fluxes in the natural climate. Atmospheric aerosol particles exert influence on climate directly, by scattering and absorbing radiation, and indirectly by modifying the microphysical properties of clouds and in turn their radiative effects and hydrology. The forcing of climate change by these indirect effects is thought to be quite substantial relative to forcing by incremental concentrations of greenhouse gases, but highly uncertain. Quantification of aerosol indirect forcing by satellite- or ground-based remote sensing has proved quite difficult in view of inherent large variation in the pertinent observables such as cloud optical depth, which is controlled mainly by liquid water path and only secondarily by aerosols. Limited work has shown instances of large magnitude of aerosol indirect forcing, with local instantaneous forcing upwards of 50 W m{sup 66}-2. Ultimately it will be necessary to represent aerosol indirect effects in climate models to accurately identify the anthropogenic forcing at present and over secular time and to assess the influence of this forcing in the context of other forcings of climate change. While the elements of aerosol processes that must be represented in models describing the evolution and properties of aerosol particles that serve as cloud condensation particles are known, many important components of these processes remain to be understood and to be represented in models, and the models evaluated against observation, before such model-based representations can confidently be used to represent aerosol indirect effects in climate models.

  19. Parameterizing cloud condensation nuclei concentrations during HOPE

    NASA Astrophysics Data System (ADS)

    Hande, Luke B.; Engler, Christa; Hoose, Corinna; Tegen, Ina

    2016-09-01

    An aerosol model was used to simulate the generation and transport of aerosols over Germany during the HD(CP)2 Observational Prototype Experiment (HOPE) field campaign of 2013. The aerosol number concentrations and size distributions were evaluated against observations, which shows satisfactory agreement in the magnitude and temporal variability of the main aerosol contributors to cloud condensation nuclei (CCN) concentrations. From the modelled aerosol number concentrations, number concentrations of CCN were calculated as a function of vertical velocity using a comprehensive aerosol activation scheme which takes into account the influence of aerosol chemical and physical properties on CCN formation. There is a large amount of spatial variability in aerosol concentrations; however the resulting CCN concentrations vary significantly less over the domain. Temporal variability is large in both aerosols and CCN. A parameterization of the CCN number concentrations is developed for use in models. The technique involves defining a number of best fit functions to capture the dependence of CCN on vertical velocity at different pressure levels. In this way, aerosol chemical and physical properties as well as thermodynamic conditions are taken into account in the new CCN parameterization. A comparison between the parameterization and the CCN estimates from the model data shows excellent agreement. This parameterization may be used in other regions and time periods with a similar aerosol load; furthermore, the technique demonstrated here may be employed in regions dominated by different aerosol species.

  20. Improved Cloud Condensation Nucleus Spectrometer

    NASA Technical Reports Server (NTRS)

    Leu, Ming-Taun

    2010-01-01

    An improved thermal-gradient cloud condensation nucleus spectrometer (CCNS) has been designed to provide several enhancements over prior thermal- gradient counters, including fast response and high-sensitivity detection covering a wide range of supersaturations. CCNSs are used in laboratory research on the relationships among aerosols, supersaturation of air, and the formation of clouds. The operational characteristics of prior counters are such that it takes long times to determine aerosol critical supersaturations. Hence, there is a need for a CCNS capable of rapid scanning through a wide range of supersaturations. The present improved CCNS satisfies this need. The improved thermal-gradient CCNS (see Figure 1) incorporates the following notable features: a) The main chamber is bounded on the top and bottom by parallel thick copper plates, which are joined by a thermally conductive vertical wall on one side and a thermally nonconductive wall on the opposite side. b) To establish a temperature gradient needed to establish a supersaturation gradient, water at two different regulated temperatures is pumped through tubes along the edges of the copper plates at the thermally-nonconductive-wall side. Figure 2 presents an example of temperature and supersaturation gradients for one combination of regulated temperatures at the thermally-nonconductive-wall edges of the copper plates. c) To enable measurement of the temperature gradient, ten thermocouples are cemented to the external surfaces of the copper plates (five on the top plate and five on the bottom plate), spaced at equal intervals along the width axis of the main chamber near the outlet end. d) Pieces of filter paper or cotton felt are cemented onto the interior surfaces of the copper plates and, prior to each experimental run, are saturated with water to establish a supersaturation field inside the main chamber. e) A flow of monodisperse aerosol and a dilution flow of humid air are introduced into the main

  1. Measured and modelled cloud condensation nuclei (CCN) concentration in São Paulo, Brazil: the importance of aerosol size-resolved chemical composition on CCNhack concentration prediction

    NASA Astrophysics Data System (ADS)

    Almeida, G. P.; Brito, J.; Morales, C. A.; Andrade, M. F.; Artaxo, P.

    2014-07-01

    Measurements of cloud condensation nuclei (CCN), aerosol size distribution and non-refractory chemical composition were performed from 16 to 31 October 2012 in the São Paulo Metropolitan Area (SPMA), Brazil. CCN measurements were performed at 0.23, 0.45, 0.68, 0.90 and 1.13% water supersaturation and were subsequently compared with the Köhler theory, considering the chemical composition. Real-time chemical composition has been obtained by deploying, for the first time in the SPMA, an aerosol chemical ionization monitor (ACSM). CCN closure analyses were performed considering internal mixtures. Average aerosol composition during the studied period yielded (arithmetic mean~± standard deviation) 4.81 ± 3.05, 3.26 ± 2.10, 0.30 ± 0.27, 0.52 ± 0.32, 0.37 ± 0.21 and 0.04 ± 0.04 μg m-3 for organics, BC, NH4, SO4, NO3 and Cl, respectively. Particle number concentration was 12 813 ± 5350 cm-3, with a dominant nucleation mode. CCN concentrations were on average 1090 ± 328 and 3570 ± 1695 cm-3 at SS = 0.23% and SS = 1.13%, respectively. Results show an increase in aerosol hygroscopicity in the afternoon as a result of aerosol photochemical processing, leading to an enhancement of both organic and inorganic secondary aerosols in the atmosphere, as well as an increase in aerosol average diameter. Considering the bulk composition alone, observed CCN concentrations were substantially overpredicted when compared with the Köhler theory (44.1 ± 47.9% at 0.23% supersaturation and 91.4 ± 40.3% at 1.13% supersaturation). Overall, the impact of composition on the calculated CCN concentration (NCCN) decreases with decreasing supersaturation, partially because using bulk composition introduces less bias for large diameters and lower critical supersaturations, defined as the supersaturation at which the cloud droplet activation will take place. Results suggest that the consideration of only inorganic fraction improves the calculated NCCN. Introducing a size-dependent chemical

  2. Long-term observations of cloud condensation nuclei in the Amazon rain forest - Part 1: Aerosol size distribution, hygroscopicity, and new model parametrizations for CCN prediction

    NASA Astrophysics Data System (ADS)

    Pöhlker, Mira L.; Pöhlker, Christopher; Ditas, Florian; Klimach, Thomas; Hrabe de Angelis, Isabella; Araújo, Alessandro; Brito, Joel; Carbone, Samara; Cheng, Yafang; Chi, Xuguang; Ditz, Reiner; Gunthe, Sachin S.; Kesselmeier, Jürgen; Könemann, Tobias; Lavrič, Jošt V.; Martin, Scot T.; Mikhailov, Eugene; Moran-Zuloaga, Daniel; Rose, Diana; Saturno, Jorge; Su, Hang; Thalman, Ryan; Walter, David; Wang, Jian; Wolff, Stefan; Barbosa, Henrique M. J.; Artaxo, Paulo; Andreae, Meinrat O.; Pöschl, Ulrich

    2016-12-01

    Size-resolved long-term measurements of atmospheric aerosol and cloud condensation nuclei (CCN) concentrations and hygroscopicity were conducted at the remote Amazon Tall Tower Observatory (ATTO) in the central Amazon Basin over a 1-year period and full seasonal cycle (March 2014-February 2015). The measurements provide a climatology of CCN properties characteristic of a remote central Amazonian rain forest site.The CCN measurements were continuously cycled through 10 levels of supersaturation (S = 0.11 to 1.10 %) and span the aerosol particle size range from 20 to 245 nm. The mean critical diameters of CCN activation range from 43 nm at S = 1.10 % to 172 nm at S = 0.11 %. The particle hygroscopicity exhibits a pronounced size dependence with lower values for the Aitken mode (κAit = 0.14 ± 0.03), higher values for the accumulation mode (κAcc = 0.22 ± 0.05), and an overall mean value of κmean = 0.17 ± 0.06, consistent with high fractions of organic aerosol.The hygroscopicity parameter, κ, exhibits remarkably little temporal variability: no pronounced diurnal cycles, only weak seasonal trends, and few short-term variations during long-range transport events. In contrast, the CCN number concentrations exhibit a pronounced seasonal cycle, tracking the pollution-related seasonality in total aerosol concentration. We find that the variability in the CCN concentrations in the central Amazon is mostly driven by aerosol particle number concentration and size distribution, while variations in aerosol hygroscopicity and chemical composition matter only during a few episodes.For modeling purposes, we compare different approaches of predicting CCN number concentration and present a novel parametrization, which allows accurate CCN predictions based on a small set of input data.

  3. Cloud condensation nucleus activity comparison of dry- and wet-generated mineral dust aerosol: the significance of soluble material

    NASA Astrophysics Data System (ADS)

    Garimella, S.; Huang, Y.-w.; Seewald, J. S.; Cziczo, D. J.

    2013-11-01

    This study examines the interaction of clay mineral particles and water vapor to determine the conditions required for cloud droplet formation. Droplet formation conditions are investigated for three clay minerals: illite, sodium-rich montmorillonite, and Arizona Test Dust. Using wet and dry particle generation coupled to a differential mobility analyzer (DMA) and cloud condensation nuclei counter, the critical activation of the clay mineral particles as cloud condensation nuclei is characterized. Electron microscopy (EM) is used to determine non-sphericity in particle shape. EM is also used to determine particle surface area and account for transmission of multiply charged particles by the DMA. Single particle mass spectrometry and ion chromatography are used to investigate soluble material in wet-generated samples and demonstrate that wet and dry generation yield compositionally different particles. Activation results are analyzed in the context of both κ-Köhler theory and Frenkel, Halsey, and Hill (FHH) adsorption activation theory. This study has two main results: (1) κ-Köhler is a suitable framework, less complex than FHH theory, to describe clay mineral nucleation activity despite apparent differences in κ with respect to size. For dry-generated particles the size dependence is likely an artifact of the shape of the size distribution: there is a sharp drop-off in particle concentration at ~300 nm, and a large fraction of particles classified with a mobility diameter less than ~300 nm are actually multiply charged, resulting in a much lower critical supersaturation for droplet activation than expected. For wet-generated particles, deviation from κ-Köhler theory is likely a result of the dissolution and redistribution of soluble material. (2) Wet-generation is found to be unsuitable for simulating the lofting of fresh dry dust because it changes the size-dependent critical supersaturations by fractionating and re-partitioning soluble material.

  4. Modeling sea salt and sulfate aerosol over the global oceans to understand the origins of marine cloud condensation nuclei and the impact of pollution on them

    NASA Astrophysics Data System (ADS)

    Fan, Tianyi

    Over the oceans, anthropogenic aerosols compete with natural aerosols from sea spray and oceanic phytoplankton-derived sulfate to create cloud condensation nuclei (CCN). To understand the impact of pollution on the marine CCN, we need knowledge of both natural and anthropogenic aerosols. In this research, we model sea salt and sulfate aerosol in a coupled climate and sectional microphysical model, CAM/CARMA. We develop a sea salt source function, CMS, based upon several earlier source functions (Clarke, Monahan, and Smith). The CMS source function is capable of reproducing observed sea salt mass, optical depth and number concentration as well as the size distribution better than other source function choices we tried. However, as we note, it is also important to properly set the removal rate of the particles to reproduce the observed abundances. The simulated non-sea-salt sulfate mass agrees well with the observations. Direct emission of sulfate from sea spray is the largest source of marine sulfate aerosol and depends on the sea salt emission. Non-sea-salt sulfate from gas- and aqueous-phase conversion, together with sea salt, contributes to the marine CCN over the mid-latitude Northern Hemisphere, while sea salt dominates the CCN over the Southern Ocean. Human impact on marine CCN extends to 45 oS. Anthropogenic sulfur emissions are responsible for about 35% of the surface layer CCN over the global oceans. With doubling the year 2000 anthropogenic sulfur emissions. Surface layer CCN increases by about 22% over the global oceans if sulfur emissions are doubled from. With no or double anthropogenic emissions, the changes in the surface layer CCN number over the Southern Hemisphere oceans are usually less than 10%.

  5. Cloud Condensation Nuclei in FIRE III

    NASA Technical Reports Server (NTRS)

    Hudson, James G.; Delnore, Victor E. (Technical Monitor)

    2002-01-01

    Yum and Hudson showed that the springtime Arctic aerosol is probably a result of long-range transport at high altitudes. Scavenging of particles by clouds reduces the low level concentrations by a factor of 3. This produces a vertical gradient in particle concentrations when low-level clouds are present. Concentrations are uniform with height when clouds are not present. Low-level CCN (cloud condensation nuclei) spectra are similar to those in other maritime areas as found by previous projects including FIRE 1 and ASTEX, which were also supported on earlier NASA-FIRE grants. Wylie and Hudson carried this work much further by comparing the CCN spectra observed during ACE with back trajectories of air masses and satellite photographs. This showed that cloud scavenging reduces CCN concentrations at all altitudes over the springtime Arctic, with liquid clouds being more efficient scavengers than frozen clouds. The small size of the Arctic Ocean seems to make it more susceptible to continental and thus anthropogenic aerosol influences than any of the other larger oceans.

  6. Sulfate aerosol distributions and cloud variations during El Nino anomalies

    SciTech Connect

    Parungo, F. ); Hicks, B. )

    1993-02-20

    The effects of aerosols on cloud characteristics, albedo, rainfall amount, and overall climate changes were investigated by assessing the qualitative associations and quantitative correlations between the relevant variables during El Nino-Southern Oscillation (ENSO) perturbations. Both historical records and data from recent field measurements for the Pacific Ocean region were used for the investigation. The results show that ENSO perturbations could change sulfate aerosol production and distribution over the surveyed regions. Strong correlations were observed between condensation nucleus concentrations and sulfate aerosol concentrations, and between cloud amount and albedo. Weak but significant correlations were also observed between condensation nucleus concentrations and cloud amounts, and between sulfate aerosol concentrations and rainfall amounts. Although sulfate aerosols appeared to have a strong impact on cloud microphysics, the present data confirm that cloud dynamics play the pivotal role in control of cloud types and cloud amount in the studied regions. 31 refs., 5 figs., 3 tabs.

  7. Cloud condensation nucleus activity comparison of dry- and wet-generated mineral dust aerosol: the significance of soluble material

    NASA Astrophysics Data System (ADS)

    Garimella, S.; Huang, Y.-W.; Seewald, J. S.; Cziczo, D. J.

    2014-06-01

    This study examines the interaction of clay mineral particles and water vapor for determining the conditions required for cloud droplet formation. Droplet formation conditions are investigated for two common clay minerals, illite and sodium-rich montmorillonite, and an industrially derived sample, Arizona Test Dust. Using wet and dry particle generation coupled to a differential mobility analyzer (DMA) and cloud condensation nuclei counter, the critical activation of the clay mineral particles as cloud condensation nuclei is characterized. Electron microscopy (EM) is used in order to determine non-sphericity in particle shape. It is also used in order to determine particle surface area and account for transmission of multiply charged particles by the DMA. Single particle mass spectrometry and ion chromatography are used to investigate soluble material in wet-generated samples and demonstrate that wet and dry generation yield compositionally different particles. Activation results are analyzed in the context of both κ-Köhler theory (κ-KT) and Frenkel-Halsey-Hill (FHH) adsorption activation theory. This study has two main results: (1) κ-KT is the suitable framework to describe clay mineral nucleation activity. Apparent differences in κ with respect to size arise from an artifact introduced by improper size-selection methodology. For dust particles with mobility sizes larger than ~300 nm, i.e., ones that are within an atmospherically relevant size range, both κ-KT and FHH theory yield similar critical supersaturations. However, the former requires a single hygroscopicity parameter instead of the two adjustable parameters required by the latter. For dry-generated particles, the size dependence of κ is likely an artifact of the shape of the size distribution: there is a sharp drop-off in particle concentration at ~300 nm, and a large fraction of particles classified with a mobility diameter less than ~300 nm are actually multiply charged, resulting in a much

  8. Particle-resolved simulation of aerosol size, composition, mixing state, and the associated optical and cloud condensation nuclei activation properties in an evolving urban plume

    SciTech Connect

    Zaveri, Rahul A.; Barnard, James C.; Easter, Richard C.; Riemer, Nicole; West, Matthew

    2010-09-11

    The recently developed particle-resolved aerosol box model PartMC-MOSAIC was used to simulate the evolution of aerosol mixing state and the associated optical and cloud condensation nuclei (CCN) activation properties in an idealized urban plume. The model explicitly resolved the size and composition of individual particles from a number of sources and tracked their evolution due to condensation/evaporation, coagulation, emission, and dilution. The ensemble black carbon (BC) specific absorption cross section increased by 40% over the course of two days as a result of BC aging by condensation and coagulation. Three- and four-fold enhancements in CCN/CN ratios were predicted to occur within 6 hours for 0.2% and 0.5% supersaturations (S), respectively. The particle-resolved results were used to evaluate the errors in the optical and CCN activation properties that would be predicted by a conventional sectional framework that assumes monodisperse, internally-mixed particles within each bin. This assumption artificially increased the ensemble BC specific absorption by 14-30% and decreased the single scattering albedo by 0.03-0.07 while the bin resolution had a negligible effect. In contrast, the errors in CCN/CN ratios were sensitive to the bin resolution, and they depended on the chosen supersaturation. For S = 0.2%, the CCN/CN ratio predicted using 100 internally-mixed bins was up to 25% higher than the particle-resolved results, while it was up to 125% higher using 10 internally-mixed bins. Errors introduced in the predicted optical and CCN properties by neglecting coagulation were also quantified.

  9. First direct observation of secondary organic aerosol formation during cloud condensation-evaporation cycles in isoprene photo-oxidation reacting mixtures (CUMULUS project)

    NASA Astrophysics Data System (ADS)

    Brégonzio-Rozier, Lola; Siekmann, Frank; Giorio, Chiara; Temime-Roussel, Brice; Pangui, Edouard; Morales, Sébastien; Ravier, Sylvain; Monod, Anne; Doussin, Jean-François

    2014-05-01

    Several field observations, laboratory and model studies suggest a potentially important role of cloud droplets in forming additional secondary organic aerosol (SOA) (Sorooshian et al., 2007; Altieri et al., 2008; Couvidat et al., 2013). While this SOAaq hypothesis seems to be robust and is considered quite established, so far, no direct observations of such a process have been provided. Recently a consortium of five laboratories has joined theirs efforts in a series of experimental simulation experiments to try to bring a direct confirmation of this hypothesis: the CUMULUS project (CloUd MULtiphase chemistry of organic compoUndS in the troposphere). The aim of the present work is to study SOA formation from isoprene photo-oxidation during cloud condensation-evaporation cycles. The chemistry occurring in the gaseous, particulate and aqueous phases, and the exchange between these phases were investigated through an original multiphase approach in a simulation chamber. Experiments were performed in the CESAM chamber (Wang et al., 2011) which was designed to investigate multiphase processes under realistic actinic flux, and accurate control of both temperature and relative humidity. A protocol was designed to generate cloud events in the simulation chamber, it has allowed us to generate clouds lasting for ca. 10 minutes in the presence of light and many clouds could be generated in a single experiment. Connected to the chamber, a large panel of instruments was used to monitor the gas-phase and the particulate phase during experiments. Gas-phase composition was analyzed in-situ via a Fourier Transform Infrared Spectrometer (FTIR) and a Proton Transfer Reaction Mass Spectrometer (PTR-TOF-MS) as well as NOx and O3 analyzers. A Scanning Mobility Particle Sizer (SMPS) measured dried SOA size distributions and total concentrations inside the chamber. An Aerodyne High Resolution Time-Of-Flight Aerosol Mass Spectrometer (HR-TOF-AMS) was also used to investigate aerosol

  10. Radiative Importance of Aerosol-Cloud Interaction

    NASA Technical Reports Server (NTRS)

    Tsay, Si-Chee

    1999-01-01

    Aerosol particles are input into the troposphere by biomass burning, among other sources. These aerosol palls cover large expanses of the earth's surface. Aerosols may directly scatter solar radiation back to space, thus increasing the earth's albedo and act to cool the earth's surface and atmosphere. Aerosols also contribute to the earth's energy balance indirectly. Hygroscopic aerosol act as cloud condensation nuclei (CCN) and thus affects cloud properties. In 1977, Twomey theorized that additional available CCN would create smaller but more numerous cloud droplets in a cloud with a given amount of liquid water. This in turn would increase the cloud albedo which would scatter additional radiation back to space and create a similar cooling pattern as the direct aerosol effect. Estimates of the magnitude of the aerosol indirect effect on a global scale range from 0.0 to -4.8 W/sq m. Thus the indirect effect can be of comparable magnitude and opposite in sign to the estimates of global greenhouse gas forcing Aerosol-cloud interaction is not a one-way process. Just as aerosols have an influence on clouds through the cloud microphysics, clouds have an influence on aerosols. Cloud droplets are solutions of liquid water and CCN, now dissolved. When the cloud droplet evaporates it leaves behind an aerosol particle. This new particle does not have to have the same properties as the original CCN. In fact, studies show that aerosol particles that result from cloud processing are larger in size than the original CCN. Optical properties of aerosol particles are dependent on the size of the particles. Larger particles have a smaller backscattering fraction, and thus less incoming solar radiation will be backscattered to space if the aerosol particles are larger. Therefore, we see that aerosols and clouds modify each other to influence the radiative balance of the earth. Understanding and quantifying the spatial and seasonal patterns of the aerosol indirect forcing may have

  11. Putting the clouds back in aerosol-cloud interactions

    NASA Astrophysics Data System (ADS)

    Gettelman, A.

    2015-11-01

    Aerosol-cloud interactions (ACI) are the consequence of perturbed aerosols affecting cloud drop and crystal number, with corresponding microphysical and radiative effects. ACI are sensitive to both cloud microphysical processes (the "C" in ACI) and aerosol emissions and processes (the "A" in ACI). This work highlights the importance of cloud microphysical processes, using idealized and global tests of a cloud microphysics scheme used for global climate prediction. Uncertainties in key cloud microphysical processes examined with sensitivity tests cause uncertainties of nearly -30 to +60 % in ACI, similar to or stronger than uncertainties identified due to natural aerosol emissions (-30 to +30 %). The different dimensions and sensitivities of ACI to microphysical processes identified in previous work are analyzed in detail, showing that precipitation processes are critical for understanding ACI and that uncertain cloud lifetime effects are nearly one-third of simulated ACI. Buffering of different processes is important, as is the mixed phase and coupling of the microphysics to the condensation and turbulence schemes in the model.

  12. Cloud Forming Potential of Aminium Carboxylate Aerosols

    NASA Astrophysics Data System (ADS)

    Gomez Hernandez, M. E.; McKeown, M.; Taylor, N.; Collins, D. R.; Lavi, A.; Rudich, Y.; Zhang, R.

    2014-12-01

    Atmospheric aerosols affect visibility, air quality, human health, climate, and in particular the aerosol direct and indirect forcings represent the largest uncertainty in climate projections. In this paper, we present laboratory measurements of the hygroscopic growth factors (HGf) and cloud condensation nuclei (CCN) activity of a series of aminium carboxylate salt aerosols, utilizing a Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA) coupled to a Condensation Particle Counter (CPC) and a CCN counter. HGf measurements were conducted for size-selected aerosols with diameters ranging from 46 nm to 151 nm and at relative humidity (RH%) values ranging from 10 to 90%. In addition, we have calculated the CCN activation diameters for the aminium carboxylate aerosols and derived the hygroscopicity parameter (k or kappa) values for all species using three methods, i.e., the mixing rule approximation, HGf, and CCN results. Our results show that variations in the ratio of acid to base directly affect the activation diameter, HGf, and (k) values of the aminium carboxylate aerosols. Atmospheric implications of the variations in the chemical composition of aminium carboxylate aerosols on their cloud forming potential will be discussed.

  13. Cloud condensation nuclei in polluted air and biomass burning smoke: Size-resolved measurements and implications for the modeling of aerosol particle hygroscopicity and CCN activity

    NASA Astrophysics Data System (ADS)

    Rose, D.; Achtert, P.; Nowak, A.; Wiedensohler, A.; Hu, M.; Shao, M.; Zhang, Y.; Andreae, M. O.; Pöschl, U.

    2009-04-01

    Atmospheric aerosol particles serving as cloud condensation nuclei (CCN) are key elements of the hydrological cycle and climate, but their abundance, properties and sources are highly variable and not well known. We have measured and characterized CCN in polluted air and biomass burning smoke during the PRIDE-PRD2006 campaign on 1-30 July 2006 at a rural site ~60 km northwest of the mega-city Guangzhou in southeastern China. CCN efficiency spectra (activated fraction vs. dry particle diameter; 20-300 nm) were recorded at water vapor supersaturations (S) in the range of 0.07% to 1.27%. Depending on S, the dry CCN activation diameters were in the range of 30-200 nm, corresponding to effective hygroscopicity parameters kappa in the range of 0.1-0.5. The hygroscopicity of particles in the accumulation size range was generally higher than that of particles in the nucleation and Aitken size range. The campaign average value of kappa for all aerosol particles across the investigated size range was 0.3, which equals the average value of kappa for other continental locations. During a strong local biomass burning event, the activation diameters increased by ~10% and the average value of kappa dropped to 0.2, which can be considered as characteristic for freshly emitted smoke from the burning of agricultural waste. At low S (≤0.27%), the maximum activated fraction remained generally well below one, which indicates substantial proportions of externally mixed CCN-inactive particles with much lower hygroscopicity - most likely soot particles (up to ~60% at ~250 nm). The mean CCN number concentrations (N_CCN,S) ranged from 1100 cm-3 at S=0.07% to 16 000 cm-3 at S=1.27%, representing ~7% to ~85% of the total aerosol particle number concentration. Based on the measurement data, we have tested different model approaches (power laws and kappa-Köhler model) for the approximation/prediction of N_CCN,S as a function of water vapor supersaturation, aerosol particle number

  14. The Effects of Transpacific Transported Aerosol on Clouds in California

    NASA Astrophysics Data System (ADS)

    Suski, K.; Creamean, J.; Rosenfeld, D.; Cazorla, A.; DeMott, P. J.; Sullivan, R. C.; White, A. B.; Ralph, F. M.; Cahill, J.; Tomlinson, J. M.; Chand, D.; Schmid, B.; Prather, K. A.

    2012-12-01

    Atmospheric aerosols are frequently lofted high into the atmosphere and can travel large distances within several days. Long-range transported aerosols can have large impacts on radiative and microphysical cloud properties and can affect precipitation on both regional and global scales. Research flights were conducted out of Sacramento, California onboard the DOE G-1 aircraft during the CalWater 2011 flight campaign, which aimed to understand the effects of aerosols on clouds and precipitation in California. To investigate aerosol effects on clouds, measurements of cloud microphysical properties were coupled with an aircraft aerosol time-of-flight mass spectrometer (A-ATOFMS), which characterized the chemical composition of aerosols and cloud residues. California Central Valley pollution aerosols were hypothesized to have a large impact on orographic clouds in the California Sierra Nevada Mountains; however transpacific transported aerosols were observed in cloud residues on several flights. Our observations indicate that dust from Asia, Africa, and the Middle East initiated ice formation in upper level clouds, while Asian soot from biomass burning served as cloud condensation nuclei in clouds with large concentrations of small liquid droplets. Previous work has linked large concentrations of small droplets to suppression of orographic precipitation, while ice formation has been shown to enhance precipitation. Therefore, the overall impact of these competing effects on precipitation in the Sierra Nevada is highly uncertain. The varying impacts of long-range transported aerosols on clouds and precipitation in California are presented.

  15. Global observations of cloud-sensitive aerosol loadings in low-level marine clouds

    NASA Astrophysics Data System (ADS)

    Andersen, H.; Cermak, J.; Fuchs, J.; Schwarz, K.

    2016-11-01

    Aerosol-cloud interaction is a key component of the Earth's radiative budget and hydrological cycle, but many facets of its mechanisms are not yet fully understood. In this study, global satellite-derived aerosol and cloud products are used to identify at what aerosol loading cloud droplet size shows the greatest sensitivity to changes in aerosol loading (ACSmax). While, on average, cloud droplet size is most sensitive at relatively low aerosol loadings, distinct spatial and temporal patterns exist. Possible determinants for these are identified with reanalysis data. The magnitude of ACSmax is found to be constrained by the total columnar water vapor. Seasonal patterns of water vapor are reflected in the seasonal patterns of ACSmax. Also, situations with enhanced turbulent mixing are connected to higher ACSmax, possibly due to intensified aerosol activation. Of the analyzed aerosol species, dust seems to impact ACSmax the most, as dust particles increase the retrieved aerosol loading without substantially increasing the concentration of cloud condensation nuclei.

  16. Ice-condenser aerosol tests

    SciTech Connect

    Ligotke, M.W.; Eschbach, E.J.; Winegardner, W.K. )

    1991-09-01

    This report presents the results of an experimental investigation of aerosol particle transport and capture using a full-scale height and reduced-scale cross section test facility based on the design of the ice compartment of a pressurized water reactor (PWR) ice-condenser containment system. Results of 38 tests included thermal-hydraulic as well as aerosol particle data. Particle retention in the test section was greatly influenced by thermal-hydraulic and aerosol test parameters. Test-average decontamination factor (DF) ranged between 1.0 and 36 (retentions between {approximately}0 and 97.2%). The measured test-average particle retentions for tests without and with ice and steam ranged between DF = 1.0 and 2.2 and DF = 2.4 and 36, respectively. In order to apparent importance, parameters that caused particle retention in the test section in the presence of ice were steam mole fraction (SMF), noncondensible gas flow rate (residence time), particle solubility, and inlet particle size. Ice-basket section noncondensible flows greater than 0.1 m{sup 3}/s resulted in stable thermal stratification whereas flows less than 0.1 m{sup 3}/s resulted in thermal behavior termed meandering with frequent temperature crossovers between flow channels. 10 refs., 66 figs., 16 tabs.

  17. Aerosol-Cloud-Drizzle-Turbulence Interactions in Boundary Layer Clouds

    DTIC Science & Technology

    2013-09-30

    understanding of the effects of aerosol-cloud interactions and drizzle and entrainment processes in boundary layer clouds for the purpose of developing...thickness, cloud turbulence intensity, and aerosols on precipitation production; 4) study the processing of aerosols by cloud processes ; 5) explore mass...drizzle processes to the artificial introduction of CCN and giant nuclei under differing aerosol backgrounds. In addition, a set of aerosol and cloud

  18. From aerosol-limited to invigoration of warm convective clouds.

    PubMed

    Koren, Ilan; Dagan, Guy; Altaratz, Orit

    2014-06-06

    Among all cloud-aerosol interactions, the invigoration effect is the most elusive. Most of the studies that do suggest this effect link it to deep convective clouds with a warm base and cold top. Here, we provide evidence from observations and numerical modeling of a dramatic aerosol effect on warm clouds. We propose that convective-cloud invigoration by aerosols can be viewed as an extension of the concept of aerosol-limited clouds, where cloud development is limited by the availability of cloud-condensation nuclei. A transition from pristine to slightly polluted atmosphere yields estimated negative forcing of ~15 watts per square meter (cooling), suggesting that a substantial part of this anthropogenic forcing over the oceans occurred at the beginning of the industrial era, when the marine atmosphere experienced such transformation.

  19. The Third International Cloud Condensation Nuclei Workshop. [conference

    NASA Technical Reports Server (NTRS)

    Kocmond, W. C.; Rogers, C. R. (Editor); Rea, S. W. (Editor)

    1981-01-01

    Twenty-five instruments were tested, including size characterization devices and two Aitken counters. The test aerosols were supplied to the instruments by an on-line generation system, thereby eliminating the need for storage bags. Cloud condensation chambers and haze chambers are highlighted.

  20. Rapid Scan Humidified Growth Cloud Condensation Nuclei Counter

    SciTech Connect

    Gregory L. Kok; Athanasios Nenes

    2013-03-13

    This research focused on enhancements to the streamwise thermal gradient cloud condensation nuclei counter to support the rapid scan mode and to enhance the capability for aerosol humidified growth measurements. The research identified the needs for flow system modifications and range of capability for operating the conventional instrument in the rapid scan and humidified growth modes.

  1. Limitations of passive satellite remote sensing to constrain global cloud condensation nuclei

    NASA Astrophysics Data System (ADS)

    Stier, P.

    2015-11-01

    Aerosol-cloud interactions are considered a key uncertainty in our understanding of climate change (Boucher et al., 2013). Knowledge of the global abundance of aerosols suitable to act as cloud condensation nuclei (CCN) is fundamental to determine the strength of the anthropogenic climate perturbation. Direct measurements are limited and sample only a very small fraction of the globe so that remote sensing from satellites and ground based instruments is widely used as a proxy for cloud condensation nuclei (Nakajima et al., 2001; Andreae, 2009; Clarke and Kapustin, 2010; Boucher et al., 2013). However, the underlying assumptions cannot be robustly tested with the small number of measurements available so that no reliable global estimate of cloud condensation nuclei exists. This study overcomes this limitation using a fully self-consistent global model (ECHAM-HAM) of aerosol radiative properties and cloud condensation nuclei. An analysis of the correlation of simulated aerosol radiative properties and cloud condensation nuclei reveals that common assumptions about their relationships are violated for a significant fraction of the globe: 71 % of the area of the globe shows correlation coefficients between CCN0.2% at cloud base and aerosol optical depth (AOD) below 0.5, i.e. AOD variability explains only 25 % of the CCN variance. This has significant implications for satellite based studies of aerosol-cloud interactions. The findings also suggest that vertically resolved remote sensing techniques, such as satellite-based high spectral resolution lidars, have a large potential for global monitoring of cloud condensation nuclei.

  2. Cloud Condensation Nuclei Profile Value-Added Product

    SciTech Connect

    McFarlane, S; Sivaraman, C; Ghan, S

    2012-10-08

    The cloud condensation nuclei (CCN) concentration at cloud base is the most relevant measure of the aerosol that influences droplet formation in clouds. Since the CCN concentration depends on supersaturation, a more general measure of the CCN concentration is the CCN spectrum (values at multiple supersaturations). The CCN spectrum is now measured at the surface at several fixed ARM sites and by the ARM Mobile Facility (AMF), but is not measured at the cloud base. Rather than rely on expensive aircraft measurements for all studies of aerosol effects on clouds, a way to project CCN measurements at the surface to cloud base is needed. Remote sensing of aerosol extinction provides information about the vertical profile of the aerosol, but cannot be directly related to the CCN concentration because the aerosol extinction is strongly influenced by humidification, particularly near cloud base. Ghan and Collins (2004) and Ghan et al. (2006) propose a method to remove the influence of humidification from the extinction profiles and tie the “dry extinction” retrieval to the surface CCN concentration, thus estimating the CCN profile. This methodology has been implemented as the CCN Profile (CCNPROF) value-added product (VAP).

  3. Submicron aerosols at thirteen diversified sites in China: size distribution, new particle formation and corresponding contribution to cloud condensation nuclei production

    NASA Astrophysics Data System (ADS)

    Peng, J. F.; Hu, M.; Wang, Z. B.; Huang, X. F.; Kumar, P.; Wu, Z. J.; Yue, D. L.; Guo, S.; Shang, D. J.; Zheng, Z.; He, L. Y.

    2014-06-01

    site types, suggesting that the NPF events in background area were more influenced by the pollutant transport. In addition, average contributions of NPF events to potential cloud condensation nuclei (CCN) at 0.2% super-saturation in the afternoon of all sampling days were calculated as 11% and 6% at urban sites and regional sites, respectively. On the other hand, NPF events at coastal and cruise measurement sites had little impact on potential production of CCN. This study provides a large dataset of aerosol size distribution in diversified atmosphere of China, improving our general understanding of emission, secondary formation, new particles formation and corresponding CCN activity of submicron aerosols in Chinese environments.

  4. Limitations of passive remote sensing to constrain global cloud condensation nuclei

    NASA Astrophysics Data System (ADS)

    Stier, Philip

    2016-05-01

    Aerosol-cloud interactions are considered a key uncertainty in our understanding of climate change (Boucher et al., 2013). Knowledge of the global abundance of cloud condensation nuclei (CCN) is fundamental to determine the strength of the anthropogenic climate perturbation. Direct measurements are limited and sample only a very small fraction of the globe so that remote sensing from satellites and ground-based instruments is widely used as a proxy for cloud condensation nuclei (Nakajima et al., 2001; Andreae, 2009; Clarke and Kapustin, 2010; Boucher et al., 2013). However, the underlying assumptions cannot be robustly tested with the small number of measurements available so that no reliable global estimate of cloud condensation nuclei exists. This study overcomes this limitation using a self-consistent global model (ECHAM-HAM) of aerosol radiative properties and cloud condensation nuclei. An analysis of the correlation of simulated aerosol radiative properties and cloud condensation nuclei reveals that common assumptions about their relationships are violated for a significant fraction of the globe: 71 % of the area of the globe shows correlation coefficients between CCN0.2 % at cloud base and aerosol optical depth (AOD) below 0.5, i.e. AOD variability explains only 25 % of the CCN variance. This has significant implications for satellite based studies of aerosol-cloud interactions. The findings also suggest that vertically resolved remote-sensing techniques, such as satellite-based high spectral resolution lidars, have a large potential for global monitoring of cloud condensation nuclei.

  5. Cloud condensation nucleus-sulfate mass relationship and cloud albedo

    NASA Technical Reports Server (NTRS)

    Hegg, Dean A.

    1994-01-01

    Analysis of previously published, simultaneous measurements of cloud condensation nucleus number concentration and sulfate mass concentration suggest a nonlinear relationship between the two variables. This nonlinearity reduces the sensitivity of cloud albedo to changes in the sulfur cycle.

  6. Campaign datasets for Holistic Interactions of Shallow Clouds, Aerosols, and Land-Ecosystems (HISCALE)

    SciTech Connect

    Fast,Jerome; Mei,Fan; Hubbe,John; Kalukin,Andrew; Long,Chuck; Matthews,Alyssa; Pekour, Mikhail; Schobesberger,Siegfried; Shilling,John; Springston,Stephen; Tomlinson,Jason; Wang,Jian; Zelenyuk-Imre,Alla

    2016-11-21

    Most of the instruments were deployed on the ARM Aerial Facility (AAF) Gulfstream-159 (G-1) aircraft, including those that measure atmospheric turbulence, cloud water content and drop size distributions, aerosol precursor gases, aerosol chemical composition and size distributions, and cloud condensation nuclei concentrations. Aerosol microphysical property measurements supplemented routine ARM aerosol measurements made at the surface. The G-1 completed transects over the SGP Central Facility at multiple altitudes within the boundary layer, and within and above clouds.

  7. Submicron aerosols at thirteen diversified sites in China: size distribution, new particle formation and corresponding contribution to cloud condensation nuclei production

    NASA Astrophysics Data System (ADS)

    Peng, J. F.; Hu, M.; Wang, Z. B.; Huang, X. F.; Kumar, P.; Wu, Z. J.; Guo, S.; Yue, D. L.; Shang, D. J.; Zheng, Z.; He, L. Y.

    2014-09-01

    , suggesting that the NPF events in background areas were more influenced by the pollutant transport. In addition, average contributions of NPF events to potential cloud condensation nuclei (CCN) at 0.2% super-saturation in the afternoon of all sampling days were calculated as 11% and 6% at urban sites and regional sites, respectively. On the other hand, NPF events at coastal sites and during cruise measurement had little impact on potential production of CCN. This study provides a large data set of particle size distribution in diversified atmosphere of China, improving our general understanding of emission, secondary formation, new particle formation and corresponding CCN activity of submicron aerosols in Chinese environments.

  8. Condensing Organic Aerosols in a Microphysical Model

    NASA Astrophysics Data System (ADS)

    Gao, Y.; Tsigaridis, K.; Bauer, S.

    2015-12-01

    The condensation of organic aerosols is represented in a newly developed box-model scheme, where its effect on the growth and composition of particles are examined. We implemented the volatility-basis set (VBS) framework into the aerosol mixing state resolving microphysical scheme Multiconfiguration Aerosol TRacker of mIXing state (MATRIX). This new scheme is unique and advances the representation of organic aerosols in models in that, contrary to the traditional treatment of organic aerosols as non-volatile in most climate models and in the original version of MATRIX, this new scheme treats them as semi-volatile. Such treatment is important because low-volatility organics contribute significantly to the growth of particles. The new scheme includes several classes of semi-volatile organic compounds from the VBS framework that can partition among aerosol populations in MATRIX, thus representing the growth of particles via condensation of low volatility organic vapors. Results from test cases representing Mexico City and a Finish forrest condistions show good representation of the time evolutions of concentration for VBS species in the gas phase and in the condensed particulate phase. Emitted semi-volatile primary organic aerosols evaporate almost completely in the high volatile range, and they condense more efficiently in the low volatility range.

  9. Aerosol-Cloud-Precipitation Interactions in the Climate System

    NASA Astrophysics Data System (ADS)

    Andreae, M. O.

    2015-12-01

    Aerosols serve as cloud condensation nuclei (CCN) and thus have a powerful effect on cloud properties. Increased aerosol concentrations resulting from pollution lead to higher cloud droplet concentrations, but smaller droplet sizes. This in turn affects the physical processes inside clouds that lead to the initiation of precipitation. Depending on a number of factors, including aerosol composition, atmospheric stability, and cloud water content, increasing CCN concentrations may either decrease or increase rainfall. In convective clouds, early rain formation is suppressed, which makes more water and energy available to rise higher in the atmosphere and form ice particles. This may invigorate the dynamics of convection, encourage the formation of hail and lightning, and enhance the transport of materials to the upper troposphere. In turn, cloud processing also affects the concentrations, composition, and distribution of atmospheric aerosols. In order to understand and quantify the effects of air pollution on climate, and precipitation in particular, knowledge of natural abundance and characteristics of aerosols is as essential as the observation of perturbed conditions. I will present recent advances in the conceptual understanding of aerosol-precipitation interactions, as well as results of measurements on aerosol and cloud characteristics in pristine and polluted conditions.

  10. Effects of aerosol on evaporation, freezing and precipitation in a multiple cloud system

    NASA Astrophysics Data System (ADS)

    Lee, Seoung Soo; Kim, Byung-Gon; Yum, Seong Soo; Seo, Kyong-Hwan; Jung, Chang-Hoon; Um, Jun Shik; Li, Zhanqing; Hong, JinKyu; Chang, Ki-Ho; Jeong, Jin-Yim

    2017-02-01

    Aerosol effects on clouds and precipitation account for a large portion of uncertainties in the prediction of the future course of global hydrologic circulations and climate. As a process of a better understanding of interactions between aerosol, clouds and precipitation, simulations are performed for a mixed-phase convective multiple-cloud system over the tropics. Studies on single-cloud systems have shown that aerosol-induced increases in freezing, associated increases in parcel buoyancy and thus the intensity of clouds (or updrafts) are a main mechanism which controls aerosol-cloud-precipitation interactions in convective clouds. However, in the multiple-cloud system that plays much more important roles in global hydrologic circulations and thus climate than single-cloud systems, aerosol effects on condensation play the most important role in aerosol-induced changes in the intensity of clouds and the effects on freezing play a negligible role in those changes. Aerosol-induced enhancement in evaporation intensifies gust fronts and increases the number of subsequently developing clouds, which leads to the substantial increases in condensation and associated intensity of convection. Although aerosol-induced enhancement in freezing takes part in the increases in condensation by inducing stronger convergence around cloud bottom, the increases in condensation are one order of magnitude larger than those in freezing. It is found that while aerosol-induced increases in freezing create intermittent extremely heavy precipitation, aerosol-induced increases in evaporation enhance light and medium precipitation in the multiple-cloud system here. This increase in light and medium precipitation makes it possible that cumulative precipitation increases with increasing aerosol concentration, although the increase is small. It is interesting that the altitude of the maximum of the time- and domain-averaged hydrometeor mass densities is quite robust to increases in aerosol

  11. CALIPSO Observations of Aerosol Properties Near Clouds

    NASA Technical Reports Server (NTRS)

    Marshak, Alexander; Varnai, Tamas; Yang, Weidong

    2010-01-01

    Clouds are surrounded by a transition zone of rapidly changing aerosol properties. Characterizing this zone is important for better understanding aerosol-cloud interactions and aerosol radiative effects as well as for improving satellite measurements of aerosol properties. We present a statistical analysis of a global dataset of CALIPSO (Cloud-Aerosol Lidar and infrared Pathfinder Satellite Observation) Lidar observations over oceans. The results show that the transition zone extends as far as 15 km away from clouds and it is ubiquitous over all oceans. The use of only high confidence level cloud-aerosol discrimination (CAD) data confirms the findings. However, the results underline the need for caution to avoid biases in studies of satellite aerosol products, aerosol-cloud interactions, and aerosol direct radiative effects.

  12. Aerosol processing in stratiform clouds in ECHAM6-HAM

    NASA Astrophysics Data System (ADS)

    Neubauer, David; Lohmann, Ulrike; Hoose, Corinna

    2013-04-01

    Aerosol processing in stratiform clouds by uptake into cloud particles, collision-coalescence, chemical processing inside the cloud particles and release back into the atmosphere has important effects on aerosol concentration, size distribution, chemical composition and mixing state. Aerosol particles can act as cloud condensation nuclei. Cloud droplets can take up further aerosol particles by collisions. Atmospheric gases may also be transferred into the cloud droplets and undergo chemical reactions, e.g. the production of atmospheric sulphate. Aerosol particles are also processed in ice crystals. They may be taken up by homogeneous freezing of cloud droplets below -38° C or by heterogeneous freezing above -38° C. This includes immersion freezing of already immersed aerosol particles in the droplets and contact freezing of particles colliding with a droplet. Many clouds do not form precipitation and also much of the precipitation evaporates before it reaches the ground. The water soluble part of the aerosol particles concentrates in the hydrometeors and together with the insoluble part forms a single, mixed, larger particle, which is released. We have implemented aerosol processing into the current version of the general circulation model ECHAM6 (Stevens et al., 2013) coupled to the aerosol module HAM (Stier et al., 2005). ECHAM6-HAM solves prognostic equations for the cloud droplet number and ice crystal number concentrations. In the standard version of HAM, seven modes are used to describe the total aerosol. The modes are divided into soluble/mixed and insoluble modes and the number concentrations and masses of different chemical components (sulphate, black carbon, organic carbon, sea salt and mineral dust) are prognostic variables. We extended this by an explicit representation of aerosol particles in cloud droplets and ice crystals in stratiform clouds similar to Hoose et al. (2008a,b). Aerosol particles in cloud droplets are represented by 5 tracers for the

  13. Influence of organic films on the evaporation and condensation of water in aerosol.

    PubMed

    Davies, James F; Miles, Rachael E H; Haddrell, Allen E; Reid, Jonathan P

    2013-05-28

    Uncertainties in quantifying the kinetics of evaporation and condensation of water from atmospheric aerosol are a significant contributor to the uncertainty in predicting cloud droplet number and the indirect effect of aerosols on climate. The influence of aerosol particle surface composition, particularly the impact of surface active organic films, on the condensation and evaporation coefficients remains ambiguous. Here, we report measurements of the influence of organic films on the evaporation and condensation of water from aerosol particles. Significant reductions in the evaporation coefficient are shown to result when condensed films are formed by monolayers of long-chain alcohols [C(n)H(2n+1)OH], with the value decreasing from 2.4 × 10(-3) to 1.7 × 10(-5) as n increases from 12 to 17. Temperature-dependent measurements confirm that a condensed film of long-range order must be formed to suppress the evaporation coefficient below 0.05. The condensation of water on a droplet coated in a condensed film is shown to be fast, with strong coherence of the long-chain alcohol molecules leading to islanding as the water droplet grows, opening up broad areas of uncoated surface on which water can condense rapidly. We conclude that multicomponent composition of organic films on the surface of atmospheric aerosol particles is likely to preclude the formation of condensed films and that the kinetics of water condensation during the activation of aerosol to form cloud droplets is likely to remain rapid.

  14. Evidence for Natural Variability in Marine Stratocumulus Cloud Properties Due to Cloud-Aerosol

    NASA Technical Reports Server (NTRS)

    Albrecht, Bruce; Sharon, Tarah; Jonsson, Haf; Minnis, Patrick; Minnis, Patrick; Ayers, J. Kirk; Khaiyer, Mandana M.

    2004-01-01

    In this study, aircraft observations from the Interdisciplinary Remotely-Piloted Aircraft Studies (CIRPAS) Twin Otter are used to characterize the variability in drizzle, cloud, and aerosol properties associated with cloud rifts and the surrounding solid clouds observed off the coast of California. A flight made on 16 July 1999 provided measurements directly across an interface between solid and rift cloud conditions. Aircraft instrumentation allowed for measurements of aerosol, cloud droplet, and drizzle spectra. CCN concentrations were measured in addition to standard thermodynamic variables and the winds. A Forward Scatter Spectrometer Probe (FSSP) measured size distribution of cloud-sized droplets. A Cloud Imaging Probe (CIP) was used to measure distributions of drizzle-sized droplets. Aerosol distributions were obtained from a Cloud Aerosol Scatterprobe (CAS). The CAS probe measured aerosols, cloud droplets and drizzle-sized drops; for this study. The CAS probe was used to measure aerosols in the size range of 0.5 micron - 1 micron. Smaller aerosols were characterized using an Ultrafine Condensation Particle Counter (CPC) sensor. The CPC was used to measure particles with diameters greater than 0.003 micron. By subtracting different count concentrations measured with the CPC, this probe was capable of identifying ultrafine particles those falling in the size range of 3 nanometers - 7 nanometers that are believed to be associated with new particle production.

  15. Condensed Acids In Antartic Stratospheric Clouds

    NASA Technical Reports Server (NTRS)

    Pueschel, R. F.; Snetsinger, K. G.; Toon, O. B.; Ferry, G. V.; Starr, W. L.; Oberbeck, V. R.; Chan, K. R.; Goodman, J. K.; Livingston, J. M.; Verma, S.; Fong, W.

    1992-01-01

    Report dicusses nitrate, sulfate, and chloride contents of stratospheric aerosols during 1987 Airborne Antarctic Ozone Experiment. Emphasizes growth of HNO3*3H2O particles in polar stratospheric clouds. Important in testing theories concerning Antarctic "ozone hole".

  16. Satellite remote sensing of aerosol and cloud properties over Eurasia

    NASA Astrophysics Data System (ADS)

    Sogacheva, Larisa; Kolmonen, Pekka; Saponaro, Giulia; Virtanen, Timo; Rodriguez, Edith; Sundström, Anu-Maija; Atlaskina, Ksenia; de Leeuw, Gerrit

    2015-04-01

    surface properties, the surface reflectance can be independently retrieved using the AOD for atmospheric correction. For the retrieval of cloud properties, the SACURA algorithm has been implemented in the ADV/ASV aerosol retrieval suite. Cloud properties retrieved from AATSR data are cloud fraction, cloud optical thickness, cloud top height, cloud droplet effective radius, liquid water path. Aerosol and cloud properties are applied for different studies over the Eurasia area. Using the simultaneous retrieval of aerosol and cloud properties allows for study of the transition from the aerosol regime to the cloud regime, such as changes in effective radius or AOD (aerosol optical depth) to COT (cloud optical thickness). The column- integrated aerosol extinction, aerosol optical depth or AOD, which is primarily reported from satellite observations, can be used as a proxy for cloud condensation nuclei (CCN) and hence contains information on the ability of aerosol particles to form clouds. Hence, connecting this information with direct observations of cloud properties provides information on aerosol-cloud interactions.

  17. An Aerosol Condensation Model for Sulfur Trioxide

    SciTech Connect

    Grant, K E

    2008-02-07

    This document describes a model for condensation of sulfuric acid aerosol given an initial concentration and/or source of gaseous sulfur trioxide (e.g. fuming from oleum). The model includes the thermochemical effects on aerosol condensation and air parcel buoyancy. Condensation is assumed to occur heterogeneously onto a preexisting background aerosol distribution. The model development is both a revisiting of research initially presented at the Fall 2001 American Geophysical Union Meeting [1] and a further extension to provide new capabilities for current atmospheric dispersion modeling efforts [2]. Sulfuric acid is one of the most widely used of all industrial chemicals. In 1992, world consumption of sulfuric acid was 145 million metric tons, with 42.4 Mt (mega-tons) consumed in the United States [10]. In 2001, of 37.5 Mt consumed in the U.S., 74% went into producing phosphate fertilizers [11]. Another significant use is in mining industries. Lawuyi and Fingas [7] estimate that, in 1996, 68% of use was for fertilizers and 5.8% was for mining. They note that H{sub 2}SO{sub 4} use has been and should continue to be very stable. In the United States, the elimination of MTBE (methyl tertiary-butyl ether) and the use of ethanol for gasoline production are further increasing the demand for petroleum alkylate. Alkylate producers have a choice of either a hydrofluoric acid or sulfuric acid process. Both processes are widely used today. Concerns, however, over the safety or potential regulation of hydrofluoric acid are likely to result in most of the growth being for the sulfuric acid process, further increasing demand [11]. The implication of sulfuric acid being a pervasive industrial chemical is that transport is also pervasive. Often, this is in the form of oleum tankers, having around 30% free sulfur trioxide. Although sulfuric acid itself is not a volatile substance, fuming sulfuric acid (referred to as oleum) is [7], the volatile product being sulfur trioxide

  18. The Impact of Aerosols on Cloud and Precipitation Processes: Cloud-Resolving Model Simulations

    NASA Technical Reports Server (NTRS)

    Tao, Wei-Kuo; Li, Xiaowen; Khain, Alexander; Matsui, Toshihisa; Lang, Stephen; Simpson, Joanne

    2008-01-01

    Aerosols and especially their effect on clouds are one of the key components of the climate system and the hydrological cycle [Ramanathan et al., 2001]. Yet, the aerosol effect on clouds remains largely unknown and the processes involved not well understood. A recent report published by the National Academy of Science states "The greatest uncertainty about the aerosol climate forcing - indeed, the largest of all the uncertainties about global climate forcing - is probably the indirect effect of aerosols on clouds [NRC, 2001]." The aerosol effect on clouds is often categorized into the traditional "first indirect (i.e., Twomey)" effect on the cloud droplet sizes for a constant liquid water path [Twomey, 1977] and the "semi-direct" effect on cloud coverage [e.g., Ackerman et al ., 2001]." Enhanced aerosol concentrations can also suppress warm rain processes by producing a narrow droplet spectrum that inhibits collision and coalescence processes [e.g., Squires and Twomey, 1961; Warner and Twomey, 1967; Warner, 1968; Rosenfeld, 19991. The aerosol effect on precipitation processes, also known as the second type of aerosol indirect effect [Albrecht, 1989], is even more complex, especially for mixed-phase convective clouds. Table 1 summarizes the key observational studies identifying the microphysical properties, cloud characteristics, thermodynamics and dynamics associated with cloud systems from high-aerosol continental environments. For example, atmospheric aerosol concentrations can influence cloud droplet size distributions, warm-rain process, cold-rain process, cloud-top height, the depth of the mixed phase region, and occurrence of lightning. In addition, high aerosol concentrations in urban environments could affect precipitation variability by providing an enhanced source of cloud condensation nuclei (CCN). Hypotheses have been developed to explain the effect of urban regions on convection and precipitation [van den Heever and Cotton, 2007 and Shepherd, 2005

  19. Explicit Simulation of Aerosol Physics in a Cloud-Resolving Model: Aerosol Transport and Processing in the Free Troposphere.

    NASA Astrophysics Data System (ADS)

    Ekman, Annica M. L.; Wang, Chien; Ström, Johan; Krejci, Radovan

    2006-02-01

    Large concentrations of small aerosols have been previously observed in the vicinity of anvils of convective clouds. A 3D cloud-resolving model (CRM) including an explicit size-resolving aerosol module has been used to examine the origin of these aerosols. Five different types of aerosols are considered: nucleation mode sulfate aerosols (here defined by 0 d 5.84 nm), Aitken mode sulfate aerosols (here defined by 5.84 nm d 31.0 nm), accumulation mode sulfate aerosols (here defined by d 31.0 nm), mixed aerosols, and black carbon aerosols.The model results suggest that approximately 10% of the initial boundary layer number concentration of Aitken mode aerosols and black carbon aerosols are present at the top of the convective cloud as the cloud reaches its decaying state. The simulated average number concentration of Aitken mode aerosols in the cloud anvil (1.6 × 104 cm-3) is in the same order of magnitude as observations. Thus, the model results strongly suggest that vertical convective transport, particularly during the active period of the convection, is responsible for a major part of the appearance of high concentrations of small aerosols (corresponding to the Aitken mode in the model) observed in the vicinity of cloud anvils.There is some formation of new aerosols within the cloud, but the formation is small. Nucleation mode aerosols are also efficiently scavenged through impaction scavenging by precipitation. Accumulation mode and mixed mode aerosols are efficiently scavenged through nucleation scavenging and their concentrations in the cloud anvil are either very low (mixed mode) or practically zero (accumulation mode).In addition to the 3D CRM, a box model, including important features of the aerosol module of the 3D model, has been used to study the formation of new aerosols after the cloud has evaporated. The possibility of these aerosols to grow to suitable cloud condensation or ice nuclei size is also examined. Concentrations of nucleation mode aerosols

  20. Precipitating Condensation Clouds in Substellar Atmospheres

    NASA Technical Reports Server (NTRS)

    Ackerman, Andrew S.; Marley, Mark S.; Gore, Warren J. (Technical Monitor)

    2000-01-01

    We present a method to calculate vertical profiles of particle size distributions in condensation clouds of giant planets and brown dwarfs. The method assumes a balance between turbulent diffusion and precipitation in horizontally uniform cloud decks. Calculations for the Jovian ammonia cloud are compared with previous methods. An adjustable parameter describing the efficiency of precipitation allows the new model to span the range of predictions from previous models. Calculations for the Jovian ammonia cloud are found to be consistent with observational constraints. Example calculations are provided for water, silicate, and iron clouds on brown dwarfs and on a cool extrasolar giant planet.

  1. Super-droplet method as a versatile numerical approach for representing aerosol-cloud-aerosol interactions.

    NASA Astrophysics Data System (ADS)

    Jaruga, Anna; Arabas, Sylwester; Pawlowska, Hanna

    2013-04-01

    Aerosol interacts with clouds by serving as cloud condensation nuclei (CCN). Its physical and chemical properties are one of the factors defining cloud droplet size distribution. On the other hand, clouds process atmospheric aerosol taking part in its wet deposition and CCN regeneration through evaporation of cloud droplets and drizzle. Physical and chemical properties of the regenerated CCN may be altered if the evaporated droplets go through collisional growth or irreversible chemical reactions. The main challenge of representing these aerosol-cloud interactions in a numerical cloud model stems from the need to track the properties of the drop nuclei throughout the cloud lifecycle. A class of methods allowing such studies is the Lagrangian particle-based simulation technique. In a simulation of cloud, each modeled particle represents a multiplicity of particles of the same nucleus type, position and size. During the simulation particle sizes change in a continuous way from CCN-sized to rain drop particles. Tracking microphysical properties of modeled particles is an inherent feature of the particle-based frameworks, making them suitable for studying aerosol-cloud-aerosol interactions. Super-droplet method is a Lagrangian technique introduced by Shima et al. (2009) featuring an efficient Monte-Carlo type solver for particle coalescence. In this study a new implementation of the super-droplet method, using the kappa-Koehler parametrisation of aerosol composition and an aqueous chemistry module for representing irreversible oxidation, will be presented. Components of the developed model will be discussed using a single-eddy prescribed-flow framework, focusing solely on the microphysical aspects of simulations. Example case will mimic a Stratocumulus cloud and depict cloud-aerosol interactions resolved by the model.

  2. Aerosol and Cloud Microphysical Characteristics of Rifts and Gradients in Maritime Stratocumulus Clouds

    NASA Technical Reports Server (NTRS)

    Sharon, Tarah M.; Albrecht, Bruce A.; Jonsson, Haflidi H.; Minnis, Patrick; Khaiyer, Mandana M.; Van Reken, Timothy; Seinfeld, John; Flagan, Rick

    2008-01-01

    A cloud rift is characterized as a large-scale, persistent area of broken, low reflectivity stratocumulus clouds usually surrounded by a solid deck of stratocumulus. A rift observed off the coast of Monterey Bay, California on 16 July 1999 was studied to compare the aerosol and cloud microphysical properties in the rift with those of the surrounding solid stratus deck. Variables measured from an instrumented aircraft included temperature, water vapor, and cloud liquid water. These measurements characterized the thermodynamic properties of the solid deck and rift areas. Microphysical measurements made included aerosol, cloud drop and drizzle drop concentrations and cloud condensation nuclei (CCN) concentrations. The microphysical characteristics in a solid stratus deck differ substantially from those of a broken, cellular rift where cloud droplet concentrations are a factor of 2 lower than those in the solid cloud. Further, CCN concentrations were found to be about 3 times greater in the solid cloud area compared with those in the rift and aerosol concentrations showed a similar difference as well. Although drizzle was observed near cloud top in parts of the solid stratus cloud, the largest drizzle rates were associated with the broken clouds within the rift area. In addition to marked differences in particle concentrations, evidence of a mesoscale circulation near the solid cloud rift boundary is presented. This mesoscale circulation provides a mechanism for maintaining a rift, but further study is required to understand the initiation of a rift and the conditions that may cause it to fill.

  3. Satellite retrieval of cloud condensation nuclei concentrations by using clouds as CCN chambers.

    PubMed

    Rosenfeld, Daniel; Zheng, Youtong; Hashimshoni, Eyal; Pöhlker, Mira L; Jefferson, Anne; Pöhlker, Christopher; Yu, Xing; Zhu, Yannian; Liu, Guihua; Yue, Zhiguo; Fischman, Baruch; Li, Zhanqing; Giguzin, David; Goren, Tom; Artaxo, Paulo; Barbosa, Henrique M J; Pöschl, Ulrich; Andreae, Meinrat O

    2016-05-24

    Quantifying the aerosol/cloud-mediated radiative effect at a global scale requires simultaneous satellite retrievals of cloud condensation nuclei (CCN) concentrations and cloud base updraft velocities (Wb). Hitherto, the inability to do so has been a major cause of high uncertainty regarding anthropogenic aerosol/cloud-mediated radiative forcing. This can be addressed by the emerging capability of estimating CCN and Wb of boundary layer convective clouds from an operational polar orbiting weather satellite. Our methodology uses such clouds as an effective analog for CCN chambers. The cloud base supersaturation (S) is determined by Wb and the satellite-retrieved cloud base drop concentrations (Ndb), which is the same as CCN(S). Validation against ground-based CCN instruments at Oklahoma, at Manaus, and onboard a ship in the northeast Pacific showed a retrieval accuracy of ±25% to ±30% for individual satellite overpasses. The methodology is presently limited to boundary layer not raining convective clouds of at least 1 km depth that are not obscured by upper layer clouds, including semitransparent cirrus. The limitation for small solar backscattering angles of <25° restricts the satellite coverage to ∼25% of the world area in a single day.

  4. Satellite retrieval of cloud condensation nuclei concentrations by using clouds as CCN chambers

    NASA Astrophysics Data System (ADS)

    Rosenfeld, Daniel; Zheng, Youtong; Hashimshoni, Eyal; Pöhlker, Mira L.; Jefferson, Anne; Pöhlker, Christopher; Yu, Xing; Zhu, Yannian; Liu, Guihua; Yue, Zhiguo; Fischman, Baruch; Li, Zhanqing; Giguzin, David; Goren, Tom; Artaxo, Paulo; Barbosa, Henrique M. J.; Pöschl, Ulrich; Andreae, Meinrat O.

    2016-05-01

    Quantifying the aerosol/cloud-mediated radiative effect at a global scale requires simultaneous satellite retrievals of cloud condensation nuclei (CCN) concentrations and cloud base updraft velocities (Wb). Hitherto, the inability to do so has been a major cause of high uncertainty regarding anthropogenic aerosol/cloud-mediated radiative forcing. This can be addressed by the emerging capability of estimating CCN and Wb of boundary layer convective clouds from an operational polar orbiting weather satellite. Our methodology uses such clouds as an effective analog for CCN chambers. The cloud base supersaturation (S) is determined by Wb and the satellite-retrieved cloud base drop concentrations (Ndb), which is the same as CCN(S). Validation against ground-based CCN instruments at Oklahoma, at Manaus, and onboard a ship in the northeast Pacific showed a retrieval accuracy of ±25% to ±30% for individual satellite overpasses. The methodology is presently limited to boundary layer not raining convective clouds of at least 1 km depth that are not obscured by upper layer clouds, including semitransparent cirrus. The limitation for small solar backscattering angles of <25° restricts the satellite coverage to ˜25% of the world area in a single day.

  5. Satellite retrieval of cloud condensation nuclei concentrations by using clouds as CCN chambers

    SciTech Connect

    Rosenfeld, Daniel; Zheng, Youtong; Hashimshoni, Eyal; Pöhlker, Mira L.; Jefferson, Anne; Pöhlker, Christopher; Yu, Xing; Zhu, Yannian; Liu, Guihua; Yue, Zhiguo; Fischman, Baruch; Li, Zhanqing; Giguzin, David; Goren, Tom; Artaxo, Paulo; Barbosa, Henrique M. J.; Pöschl, Ulrich; Andreae, Meinrat O.

    2016-03-04

    Quantifying the aerosol/cloud-mediated radiative effect at a global scale requires simultaneous satellite retrievals of cloud condensation nuclei (CCN) concentrations and cloud base updraft velocities (Wb). Hitherto, the inability to do so has been a major cause of high uncertainty regarding anthropogenic aerosol/cloud-mediated radiative forcing. This can be addressed by the emerging capability of estimating CCN and Wb of boundary layer convective clouds from an operational polar orbiting weather satellite. In this paper, our methodology uses such clouds as an effective analog for CCN chambers. The cloud base supersaturation (S) is determined by Wb and the satellite-retrieved cloud base drop concentrations (Ndb), which is the same as CCN(S). Validation against ground-based CCN instruments at Oklahoma, at Manaus, and onboard a ship in the northeast Pacific showed a retrieval accuracy of ±25% to ±30% for individual satellite overpasses. The methodology is presently limited to boundary layer not raining convective clouds of at least 1 km depth that are not obscured by upper layer clouds, including semitransparent cirrus. Finally, the limitation for small solar backscattering angles of <25° restricts the satellite coverage to ~25% of the world area in a single day.

  6. Satellite retrieval of cloud condensation nuclei concentrations by using clouds as CCN chambers

    DOE PAGES

    Rosenfeld, Daniel; Zheng, Youtong; Hashimshoni, Eyal; ...

    2016-03-04

    Quantifying the aerosol/cloud-mediated radiative effect at a global scale requires simultaneous satellite retrievals of cloud condensation nuclei (CCN) concentrations and cloud base updraft velocities (Wb). Hitherto, the inability to do so has been a major cause of high uncertainty regarding anthropogenic aerosol/cloud-mediated radiative forcing. This can be addressed by the emerging capability of estimating CCN and Wb of boundary layer convective clouds from an operational polar orbiting weather satellite. In this paper, our methodology uses such clouds as an effective analog for CCN chambers. The cloud base supersaturation (S) is determined by Wb and the satellite-retrieved cloud base drop concentrationsmore » (Ndb), which is the same as CCN(S). Validation against ground-based CCN instruments at Oklahoma, at Manaus, and onboard a ship in the northeast Pacific showed a retrieval accuracy of ±25% to ±30% for individual satellite overpasses. The methodology is presently limited to boundary layer not raining convective clouds of at least 1 km depth that are not obscured by upper layer clouds, including semitransparent cirrus. Finally, the limitation for small solar backscattering angles of <25° restricts the satellite coverage to ~25% of the world area in a single day.« less

  7. Satellite retrieval of cloud condensation nuclei concentrations by using clouds as CCN chambers

    PubMed Central

    Rosenfeld, Daniel; Zheng, Youtong; Hashimshoni, Eyal; Pöhlker, Mira L.; Jefferson, Anne; Pöhlker, Christopher; Yu, Xing; Zhu, Yannian; Liu, Guihua; Yue, Zhiguo; Fischman, Baruch; Li, Zhanqing; Giguzin, David; Goren, Tom; Artaxo, Paulo; Pöschl, Ulrich

    2016-01-01

    Quantifying the aerosol/cloud-mediated radiative effect at a global scale requires simultaneous satellite retrievals of cloud condensation nuclei (CCN) concentrations and cloud base updraft velocities (Wb). Hitherto, the inability to do so has been a major cause of high uncertainty regarding anthropogenic aerosol/cloud-mediated radiative forcing. This can be addressed by the emerging capability of estimating CCN and Wb of boundary layer convective clouds from an operational polar orbiting weather satellite. Our methodology uses such clouds as an effective analog for CCN chambers. The cloud base supersaturation (S) is determined by Wb and the satellite-retrieved cloud base drop concentrations (Ndb), which is the same as CCN(S). Validation against ground-based CCN instruments at Oklahoma, at Manaus, and onboard a ship in the northeast Pacific showed a retrieval accuracy of ±25% to ±30% for individual satellite overpasses. The methodology is presently limited to boundary layer not raining convective clouds of at least 1 km depth that are not obscured by upper layer clouds, including semitransparent cirrus. The limitation for small solar backscattering angles of <25° restricts the satellite coverage to ∼25% of the world area in a single day. PMID:26944081

  8. Observations of anthropogenic cloud condensation nuclei

    NASA Technical Reports Server (NTRS)

    Hudson, James G.

    1990-01-01

    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.

  9. Characterisation of aerosol combustible mixtures generated using condensation process

    NASA Astrophysics Data System (ADS)

    Saat, Aminuddin; Dutta, Nilabza; Wahid, Mazlan A.

    2012-06-01

    An accidental release of a liquid flammable substance might be formed as an aerosol (droplet and vapour mixture). This phenomenon might be due to high pressure sprays, pressurised liquid leaks and through condensation when hot vapour is rapidly cooled. Such phenomena require a fundamental investigation of mixture characterisation prior to any subsequent process such as evaporation and combustion. This paper describes characterisation study of droplet and vapour mixtures generated in a fan stirred vessel using condensation technique. Aerosol of isooctane mixtures were generated by expansion from initially a premixed gaseous fuel-air mixture. The distribution of droplets within the mixture was characterised using laser diagnostics. Nearly monosized droplet clouds were generated and the droplet diameter was defined as a function of expansion time. The effect of changes in pressure, temperature, fuel-air fraction and expansion ratio on droplet diameter was evaluated. It is shown that aerosol generation by expansion was influenced by the initial pressure and temperature, equivalence ratio and expansion rates. All these parameters affected the onset of condensation which in turn affected the variation in droplet diameter.

  10. Cloud Condensation in Titan's Lower Stratosphere

    NASA Technical Reports Server (NTRS)

    Romani, Paul N.; Anderson, Carrie M.

    2011-01-01

    A 1-D condensation model is developed for the purpose of reproducing ice clouds in Titan's lower stratosphere observed by the Composite Infrared Spectrometer (CIRS) onboard Cassini. Hydrogen cyanide (HCN), cyanoacetylene (HC3N), and ethane (C2H6) vapors are treated as chemically inert gas species that flow from an upper boundary at 500 km to a condensation sink near Titan's tropopause (-45 km). Gas vertical profiles are determined from eddy mixing and a downward flux at the upper boundary. The condensation sink is based upon diffusive growth of the cloud particles and is proportional to the degree of supersaturation in the cloud formation regIOn. Observations of the vapor phase abundances above the condensation levels and the locations and properties of the ice clouds provide constraints on the free parameters in the model. Vapor phase abundances are determined from CIRS mid-IR observations, whereas cloud particle sizes, altitudes, and latitudinal distributions are derived from analyses of CIRS far-IR observations of Titan. Specific cloud constraints include: I) mean particle radii of2-3 J.lm inferred from the V6 506 cm- band of HC3N, 2) latitudinal abundance distributions of condensed nitriles, inferred from a composite emission feature that peaks at 160/cm , and 3) a possible hydrocarbon cloud layer at high latitudes, located near an altitude of 60 km, which peaks between 60 and 80 cm l . Nitrile abundances appear to diminish substantially at high northern latitudes over the time period 2005 to 2010 (northern mid winter to early spring). Use of multiple gas species provides a consistency check on the eddy mixing coefficient profile. The flux at the upper boundary is the net column chemical production from the upper atmosphere and provides a constraint on chemical pathways leading to the production of these compounds. Comparison of the differing lifetimes, vapor phase transport, vapor phase loss rate, and particle sedimentation, sheds light on temporal stability

  11. Properties of aerosol processed by ice clouds

    NASA Astrophysics Data System (ADS)

    Rudich, Y.; Adler, G.; Moise, T.; Erlick-Haspel, C.

    2012-12-01

    We suggest that highly porous aerosol (HPA) can form in the upper troposphere/lower stratosphere when ice particles encounter sub-saturation leading to ice sublimation similar to freeze drying. This process can occur at the lower layers of cirrus clouds (few km), at anvils of high convective clouds and thunderstorms, in clouds forming in atmospheric gravitational waves, in contrails and in high convective clouds injecting to the stratosphere. A new experimental system that simulates freeze drying of proxies for atmospheric aerosol at atmospheric pressure was constructed and various proxies for atmospheric soluble aerosol were studied. The properties of resulting HPA were characterized by various methods. It was found that the resulting aerosol have larger sizes (extent depends on substance and mixing), lower density (largevoid fraction), lower optical extinction and higher CCN activity and IN activity. Implication of HPA's unique properties and their atmospheric consequences to aerosol processing in ice clouds and to cloud cycles will be discussed.

  12. On the Effect of Dust Particles on Global Cloud Condensation Nuclei and Cloud Droplet Number

    NASA Technical Reports Server (NTRS)

    Karydis, V. A.; Kumar, P.; Barahona, D.; Sokolik, I. N.; Nenes, A.

    2011-01-01

    Aerosol-cloud interaction studies to date consider aerosol with a substantial fraction of soluble material as the sole source of cloud condensation nuclei (CCN). Emerging evidence suggests that mineral dust can act as good CCN through water adsorption onto the surface of particles. This study provides a first assessment of the contribution of insoluble dust to global CCN and cloud droplet number concentration (CDNC). Simulations are carried out with the NASA Global Modeling Initiative chemical transport model with an online aerosol simulation, considering emissions from fossil fuel, biomass burning, marine, and dust sources. CDNC is calculated online and explicitly considers the competition of soluble and insoluble CCN for water vapor. The predicted annual average contribution of insoluble mineral dust to CCN and CDNC in cloud-forming areas is up to 40 and 23.8%, respectively. Sensitivity tests suggest that uncertainties in dust size distribution and water adsorption parameters modulate the contribution of mineral dust to CDNC by 23 and 56%, respectively. Coating of dust by hygroscopic salts during the atmospheric aging causes a twofold enhancement of the dust contribution to CCN; the aged dust, however, can substantially deplete in-cloud supersaturation during the initial stages of cloud formation and can eventually reduce CDNC. Considering the hydrophilicity from adsorption and hygroscopicity from solute is required to comprehensively capture the dust-warm cloud interactions. The framework presented here addresses this need and can be easily integrated in atmospheric models.

  13. Precipitation effects of giant cloud condensation nuclei artificially introduced into stratocumulus clouds

    NASA Astrophysics Data System (ADS)

    Jung, E.; Albrecht, B. A.; Jonsson, H. H.; Chen, Y.-C.; Seinfeld, J. H.; Sorooshian, A.; Metcalf, A. R.; Song, S.; Fang, M.; Russell, L. M.

    2015-01-01

    To study the effect of giant cloud condensation nuclei (GCCN) on precipitation processes in stratocumulus clouds, 1-10 μm diameter salt particles (salt powder) were released from an aircraft while flying near cloud top on 3 August 2011 off the central coast of California. The seeded area was subsequently sampled from the aircraft that was equipped with aerosol, cloud, and precipitation probes and an upward-facing cloud radar. During post-seeding sampling, made 30-60 min after seeding, the mean cloud droplet size increased, the droplet number concentration decreased, and large drop (e.g., diameter larger than 10 μm) concentration increased. Average drizzle rates increased from about 0.05 to 0.20 mm h-1, and liquid water path decreased from about 52 to 43 g m-2. Strong radar returns associated with drizzle were observed on the post-seeding cloud-base level-leg flights and were accompanied by a substantial depletion of the cloud liquid water content. The changes were large enough to suggest that the salt particles with concentrations estimated to be 10-2 to 10-4 cm-3 resulted in a four-fold increase in the cloud base rainfall rate and depletion of the cloud water due to rainout. In contrast, a case is shown where the cloud was already precipitating (on 10 August) and the effect of adding GCCN to the cloud was insignificant.

  14. Precipitation effects of giant cloud condensation nuclei artificially introduced into stratocumulus clouds

    NASA Astrophysics Data System (ADS)

    Jung, E.; Albrecht, B. A.; Jonsson, H. H.; Chen, Y.-C.; Seinfeld, J. H.; Sorooshian, A.; Metcalf, A. R.; Song, S.; Fang, M.; Russell, L. M.

    2015-05-01

    To study the effect of giant cloud condensation nuclei (GCCN) on precipitation processes in stratocumulus clouds, 1-10 μm diameter salt particles (salt powder) were released from an aircraft while flying near the cloud top on 3 August 2011 off the central coast of California. The seeded area was subsequently sampled from the aircraft that was equipped with aerosol, cloud, and precipitation probes and an upward-facing cloud radar. During post-seeding sampling, made 30-60 min after seeding, the mean cloud droplet size increased, the droplet number concentration decreased, and large drop (e.g., diameter larger than 10 μm) concentration increased. Average drizzle rates increased from about 0.05 to 0.20 mm h-1, and the liquid water path decreased from about 52 to 43 g m-2. Strong radar returns associated with drizzle were observed on the post-seeding cloud-base level-leg flights and were accompanied by a substantial depletion of the cloud liquid water content. The changes were large enough to suggest that the salt particles with concentrations estimated to be 10-2 to 10-4 cm-3 resulted in a four-fold increase in the cloud-base rainfall rate and depletion of the cloud water due to rainout. In contrast, a case is shown where the cloud was already precipitating (on 10 August) and the effect of adding GCCN to the cloud was insignificant.

  15. The Impact of Aerosols on Cloud and Precipitation Processes: Cloud-Resolving Model Simulations

    NASA Technical Reports Server (NTRS)

    Tao, Wei-Kuo; Li, X.; Khain, A.; Simpson, S.

    2005-01-01

    Cloud microphysics are inevitable affected by the smoke particle (CCN, cloud condensation nuclei) size distributions below the clouds, Therefore, size distributions parameterized as spectral bin microphysics are needed to explicitly study the effect of atmospheric aerosol concentration on cloud development, rainfall production, and rainfall rates for convective clouds. Recently, a detailed spectral-bin microphysical scheme was implemented into the the Goddard Cumulus Ensemble (GCE) model. The formulation for the explicit spectral-bim microphysical processes is based on solving stochastic kinetic equations for the size distribution functions of water droplets (i.e., cloud droplets and raindrops), and several types of ice particles [i.e., pristine ice crystals (columnar and plate-like), snow (dendrites and aggregates), graupel and frozen drops/hail]. Each type is described by a special size distribution function containing many categories (i.e., 33 bins). Atmospheric aerosols are also described using number density size-distribution functions.

  16. Aerosol indirect effect dictated by liquid clouds

    NASA Astrophysics Data System (ADS)

    Christensen, Matthew W.; Chen, Yi-Chun; Stephens, Graeme L.

    2016-12-01

    Anthropogenic aerosols have been shown to enhance the solar reflection from warm liquid clouds and mask part of the warming due to the buildup of greenhouse gases. However, very little is known about the effects of aerosol on mixed-phase stratiform clouds as well as other cloud regimes including cumulus, altocumulus, nimbostratus, deep convection, and anvil cirrus. These additional cloud categories are ubiquitous and typically overlooked in satellite-based assessments of the global aerosol indirect forcing. Here we provide their contribution to the aerosol indirect forcing estimate using satellite data collected from several colocated sensors in the A-train for the period 2006-2010. Cloud type is determined according to the 2B-CLDCLASS-LIDAR CloudSat product, and the observations are matched to the radiative flux measurements from CERES (Clouds and the Earth's Radiant Energy System) and aerosol retrievals from MODIS (MODerate resolution Imaging Spectroradiometer). The oceanic mean aerosol indirect forcing is estimated to be -0.20 ± 0.31 W m-2 with warm low-level cloud largely dictating the strength of the response (-0.36 ± 0.21 W m-2) due to their abundance and strong cloud albedo effect. Contributions from mixed-phase low-level cloud (0.01 ± 0.06 W m-2) and convective cloud (0.15 ± 0.23 W m-2) are positive and buffer the system due to strong aerosol-cloud feedbacks that reduce the cloud albedo effect and/or lead to convective invigoration causing a countering positive longwave warming response. By combining all major cloud categories together, aerosol indirect forcing decreases and now contains positive values in the uncertainty estimate.

  17. The Aerosol/Cloud/Ecosystems Mission (ACE)

    NASA Technical Reports Server (NTRS)

    Schoeberl, Mark

    2008-01-01

    The goals and measurement strategy of the Aerosol/Cloud/Ecosystems Mission (ACE) are described. ACE will help to answer fundamental science questions associated with aerosols, clouds, air quality and global ocean ecosystems. Specifically, the goals of ACE are: 1) to quantify aerosol-cloud interactions and to assess the impact of aerosols on the hydrological cycle and 2) determine Ocean Carbon Cycling and other ocean biological processes. It is expected that ACE will: narrow the uncertainty in aerosol-cloud-precipitation interaction and quantify the role of aerosols in climate change; measure the ocean ecosystem changes and precisely quantify ocean carbon uptake; and, improve air quality forecasting by determining the height and type of aerosols being transported long distances. Overviews are provided of the aerosol-cloud community measurement strategy, aerosol and cloud observations over South Asia, and ocean biology research goals. Instruments used in the measurement strategy of the ACE mission are also highlighted, including: multi-beam lidar, multiwavelength high spectra resolution lidar, the ocean color instrument (ORCA)--a spectroradiometer for ocean remote sensing, dual frequency cloud radar and high- and low-frequency micron-wave radiometer. Future steps for the ACE mission include refining measurement requirements and carrying out additional instrument and payload studies.

  18. Impact of volcanic ash plume aerosol on cloud microphysics

    NASA Astrophysics Data System (ADS)

    Martucci, G.; Ovadnevaite, J.; Ceburnis, D.; Berresheim, H.; Varghese, S.; Martin, D.; Flanagan, R.; O'Dowd, C. D.

    2012-03-01

    This study focuses on the dispersion of the Eyjafjallajökull volcanic ash plume over the west of Ireland, at the Mace Head Supersite, and its influence on cloud formation and microphysics during one significant event spanning May 16th and May 17th, 2010. Ground-based remote sensing of cloud microphysics was performed using a K a-band Doppler cloud RADAR, a LIDAR-ceilometer and a multi-channel microwave-radiometer combined with the synergistic analysis scheme SYRSOC ( Synergistic Remote Sensing Of Cloud). For this case study of volcanic aerosol interaction with clouds, cloud droplet number concentration (CDNC), liquid water content (LWC), and droplet effective radius ( reff) and the relative dispersion were retrieved. A unique cloud type formed over Mace Head characterized by layer-averaged maximum, mean and standard deviation values of the CDNC, reff and LWC: Nmax = 948 cm -3, N¯=297cm, σ=250cm, reff max = 35.5 μm, r¯=4.8μm, σ=4.4μm, LWC=0.23gm, LWC¯=0.055gm, σ=0.054gm, respectively. The high CDNC, for marine clean air, were associated with large accumulation mode diameter (395 nm) and a hygroscopic growth factor consistent with sulphuric acid aerosol, despite being almost exclusively internally mixed in submicron sizes. Additionally, the Condensation Nuclei (CN, d > 10 nm) to Cloud Condensation Nuclei (CCN) ratio, CCN:CN ˜1 at the moderately low supersaturation of 0.25%. This case study illustrates the influence of volcanic aerosols on cloud formation and microphysics and shows that volcanic aerosol can be an efficient CCN.

  19. Improvement of MODIS aerosol retrievals near clouds

    NASA Astrophysics Data System (ADS)

    Wen, Guoyong; Marshak, Alexander; Levy, Robert C.; Remer, Lorraine A.; Loeb, Norman G.; Várnai, Tamás.; Cahalan, Robert F.

    2013-08-01

    retrieval of aerosol properties near clouds from reflected sunlight is challenging. Sunlight reflected from clouds can effectively enhance the reflectance in nearby clear regions. Ignoring cloud 3-D radiative effects can lead to large biases in aerosol retrievals, risking an incorrect interpretation of satellite observations on aerosol-cloud interaction. Earlier, we developed a simple model to compute the cloud-induced clear-sky radiance enhancement that is due to radiative interaction between boundary layer clouds and the molecular layer above. This paper focuses on the application and implementation of the correction algorithm. This is the first time that this method is being applied to a full Moderate Resolution Imaging Spectroradiometer (MODIS) granule. The process of the correction includes converting Clouds and the Earth's Radiant Energy System broadband flux to visible narrowband flux, computing the clear-sky radiance enhancement, and retrieving aerosol properties. We find that the correction leads to smaller values in aerosol optical depth (AOD), Ångström exponent, and the small mode aerosol fraction of the total AOD. It also makes the average aerosol particle size larger near clouds than far away from clouds, which is more realistic than the opposite behavior observed in operational retrievals. We discuss issues in the current correction method as well as our plans to validate the algorithm.

  20. Global Analysis of Aerosol Properties Above Clouds

    NASA Technical Reports Server (NTRS)

    Waquet, F.; Peers, F.; Ducos, F.; Goloub, P.; Platnick, S. E.; Riedi, J.; Tanre, D.; Thieuleux, F.

    2013-01-01

    The seasonal and spatial varability of Aerosol Above Cloud (AAC) properties are derived from passive satellite data for the year 2008. A significant amount of aerosols are transported above liquid water clouds on the global scale. For particles in the fine mode (i.e., radius smaller than 0.3 m), including both clear sky and AAC retrievals increases the global mean aerosol optical thickness by 25(+/- 6%). The two main regions with man-made AAC are the tropical Southeast Atlantic, for biomass burning aerosols, and the North Pacific, mainly for pollutants. Man-made AAC are also detected over the Arctic during the spring. Mineral dust particles are detected above clouds within the so-called dust belt region (5-40 N). AAC may cause a warming effect and bias the retrieval of the cloud properties. This study will then help to better quantify the impacts of aerosols on clouds and climate.

  1. Clouds and aerosols on Venus: an overview

    NASA Astrophysics Data System (ADS)

    Titov, Dmitri; Ignatiev, Nikolay; McGouldrick, Kevin; Wilquet, Valerie; Wilson, Colin

    2015-04-01

    size distributions found in the literature, with an effective radius below 0.3 μm and a variance of about 2. The scale height of the upper haze is found to be 6.9 ± 5.1 km. The lower and middle cloud layers - those at 48 - 60 km altitudes - are difficult to observe, as they are hidden by upper clouds. Nevertheless, both nightside near-IR sounding and radio occultation has provided valuable insight into cloud processes in this region. Near IR sounding reveals the morphology of the lower/middle clouds 'backlit' by thermally emitted photons from the lower atmosphere. The morphology of these clouds changes on timescales of order of 24 hours. The vertically integrated cloud optical depth is twice as great in the polar collar (at 75 degrees latitude) compared to low latitudes. Spectral band ratio analysis, if interpreted strictly in terms of Mode 1 / 2 / 2' / 3 particles of H2SO4:H2O mixtures, suggests that the acidity of the cloud particles is higher near the polar collar and in regions of optically thick cloud. Particles in the centre of the polar vortex exhibit anomalously high band ratios so are significantly larger and/or of different composition than those at low latitudes. Radio occultation from Venus Express confirms that the atmosphere is in convective equilibrium from 50-60 km. Sulphuric acid vapour profiles calculated from the absorption of the radio signals show an atmosphere saturated with sulphuric acid in the cloud layer. Both of these results are consistent with the understanding of convective condensational cloud at altitudes of 50-60 km. Microphysical simulations of the aerosol populations in the atmosphere of Venus have received a boost from the recent exploration of particle properties carried out by various teams using Venus Express over the last decade or so. Numerous groups are applying separate models to the coupled problems of the Venus clouds. Quasi-periodic variability of aerosol population properties has been found in model simulations by

  2. Clouds and aerosols on Venus: an overview

    NASA Astrophysics Data System (ADS)

    Titov, D. V.; Ignatiev, N. I.; McGouldrick, K.; Wilquet, V.; Wilson, C. F.

    2014-04-01

    concentration with a decreasing altitude (from 70-75% at about 90 km to 85% at 70 km of altitude) and (2) Many SOIR/SPICAV data cannot be fitted when using size distributions found in the literature, with an effective radius below 0.3 μm and a variance of about 2. The scale height of the upper haze is found to be 6.9 ± 5.1 km. The lower & middle cloud layers - those at 48 - 60 km altitudes - are difficult to observe, as they are hidden by upper clouds. Nevertheless, both nightside near-IR sounding and radio occultation has provided valuable insight into cloud processes in this region. Near IR sounding reveals the morphology of the lower/middle clouds 'backlit' by thermally emitted photons from the lower atmosphere. The morphology of these clouds changes on timescales of order of 24 hours [7]. The vertically integrated cloud optical depth is twice as great in the polar collar (at 75 degrees latitude) compared to low latitudes. Spectral band ratio analysis, if interpreted strictly in terms of Mode 1 / 2 / 2' / 3 particles of H2SO4:H2O mixtures, the acidity of the cloud particles is found to be higher near the polar collar and in regions of optically thick cloud [8]. Particles in the centre of the polar vortex exhibit anomalously high band ratios so are significantly larger and/or of different composition than those at low latitudes [9]. Radio occultation from Venus Express confirms that the atmosphere is in convective equilibrium from 50-60 km [10]. Sulphuric acid vapour profiles calculated from the absorption of the radio signals show an atmosphere saturated with sulphuric acid in the cloud layer [11]. Both of these results are consistent with the understanding of convective condensational cloud at altitudes of 50-60 km. Microphysical simulations of the aerosol populations in the atmosphere of Venus have received a boost from the recent exploration of particle properties carried out by various teams using Venus Express over the last decade or so. Numerous groups are applying

  3. Aerosol cloud processing with the global model ECHAM5-HAM-SALSA

    NASA Astrophysics Data System (ADS)

    Bergman, T.; Korhonen, H.; Zubair, M.; Romakkaniemi, S.; Lehtinen, K.; Kokkola, H.

    2012-04-01

    Atmospheric aerosols and their interactions with clouds constitute the largest uncertainty in the radiative forcing of the Earth's atmosphere. Increasing aerosol number concentrations increases the cloud droplet concentration and droplet surface and hence the cloud albedo. This mechanism is called the aerosol indirect effect on climate. Understanding the changes in cloud droplet number concentrations and size by anthropogenic aerosols are the key factors in the study of future climate change. Therefore the aerosols' formation and growth from nanoparticles to cloud condensation nuclei (CCN) must be described accurately. The formation and growth of aerosols are shown to be described more accurately with sectional representations than with bulk (total aerosol mass only), modal (lognormal modes describing mass and number size distribution) or moment (processes tied to different moments of particle number size distribution) approaches. Recently the sectional aerosol models have been implemented to global climate models. However, the resolution of sectional models must be optimised to reduce the computational cost. We have implemented the sectional aerosol model SALSA in ECHAM5-HAM. SALSA describes the aerosol population with 20 size sections. The dynamics are optimised for large scale applications and the model includes an improved moving center sectional method. The particulate mass consists of five compounds: sulphate, organic carbon, black carbon, sea salt and dust. The aerosol processing has been studied extensively and there are many numerical models used to predict CCN number concentrations. However, due to computational limitations many of them are not suitable for utilisation in global climate models. Therefore in most global climate studies on aerosol activation to CCN is examined using cloud activation parameterisations. We study the aerosol cloud processing and its affect on transport of aerosols using Abdul-Razzak-Ghan aerosol cloud activation

  4. Measurements of cloud condensation nuclei spectra within maritime cumulus cloud droplets: Implications for mixing processes

    NASA Technical Reports Server (NTRS)

    Twohy, Cynthia H.; Hudson, James G.

    1995-01-01

    In a cloud formed during adiabatic expansion, the droplet size distribution will be systematically related to the critical supersaturation of the cloud condensation nuclei (CNN), but this relationship can be complicated in entraining clouds. Useful information about cloud processes, such as mixing, can be obtained from direct measurements of the CNN involved in droplet nucleation. This was accomplished by interfacing two instruments for a series of flights in maritime cumulus clouds. One instrument, the counterflow virtual impactor, collected cloud droplets, and the nonvolatile residual nuclei of the droplets was then passed to a CCN spectrometer, which measured the critical supersaturation (S(sub c)) spectrum of the droplet nuclei. The measured S(sub c) spectra of the droplet nuclei were compared with the S(sub c) spectra of ambient aerosol particles in order to identify which CCN were actually incorporated into droplets and to determine when mixing processes were active at different cloud levels. The droplet nuclei nearly always exhibited lower median S(sub c)'s than the ambient aerosol, as expected since droplets nucleate perferentially on particles with lower critical supersaturations. Critical supersaturation spectra from nuclei of droplets near cloud base were similar to those predicted for cloud regions formed adiabatically, but spectra of droplet nuclei from middle cloud levels showed some evidence that mixing had occurred. Near cloud top, the greatest variation in the spectra of the droplet nuclei was observed, and nuclei with high S(sub c)'s were sometimes present even within relatively large droplets. This suggests that the extent of mixing increases with height in cumulus clouds and that inhomogeneous mixing may be important near cloud top. These promising initial results suggest improvements to the experimental technique that will permit more quantitative results in future experiments.

  5. Impact of Aerosol Processing on Orographic Clouds

    NASA Astrophysics Data System (ADS)

    Pousse-Nottelmann, Sara; Zubler, Elias M.; Lohmann, Ulrike

    2010-05-01

    Aerosol particles undergo significant modifications during their residence time in the atmosphere. Physical processes like coagulation, coating and water uptake, and aqueous surface chemistry alter the aerosol size distribution and composition. At this, clouds play a primary role as physical and chemical processing inside cloud droplets contributes considerably to the changes in aerosol particles. A previous study estimates that on global average atmospheric particles are cycled three times through a cloud before being removed from the atmosphere [1]. An explicit and detailed treatment of cloud-borne particles has been implemented in the regional weather forecast and climate model COSMO-CLM. The employed model version includes a two-moment cloud microphysical scheme [2] that has been coupled to the aerosol microphysical scheme M7 [3] as described by Muhlbauer and Lohmann, 2008 [4]. So far, the formation, transfer and removal of cloud-borne aerosol number and mass were not considered in the model. Following the parameterization for cloud-borne particles developed by Hoose et al., 2008 [5], distinction between in-droplet and in-crystal particles is made to more physically account for processes in mixed-phase clouds, such as the Wegener-Bergeron-Findeisen process and contact and immersion freezing. In our model, this approach has been extended to allow for aerosol particles in five different hydrometeors: cloud droplets, rain drops, ice crystals, snow flakes and graupel. We account for nucleation scavenging, freezing and melting processes, autoconversion, accretion, aggregation, riming and selfcollection, collisions between interstitial aerosol particles and hydrometeors, ice multiplication, sedimentation, evaporation and sublimation. The new scheme allows an evaluation of the cloud cycling of aerosol particles by tracking the particles even when scavenged into hydrometeors. Global simulations of aerosol processing in clouds have recently been conducted by Hoose et al

  6. Aerosols, clouds, and precipitation in the North Atlantic trades observed during the Barbados aerosol cloud experiment - Part 1: Distributions and variability

    NASA Astrophysics Data System (ADS)

    Jung, Eunsil; Albrecht, Bruce A.; Feingold, Graham; Jonsson, Haflidi H.; Chuang, Patrick; Donaher, Shaunna L.

    2016-07-01

    Shallow marine cumulus clouds are by far the most frequently observed cloud type over the Earth's oceans; but they are poorly understood and have not been investigated as extensively as stratocumulus clouds. This study describes and discusses the properties and variations of aerosol, cloud, and precipitation associated with shallow marine cumulus clouds observed in the North Atlantic trades during a field campaign (Barbados Aerosol Cloud Experiment- BACEX, March-April 2010), which took place off Barbados where African dust periodically affects the region. The principal observing platform was the Center for Interdisciplinary Remotely Piloted Aircraft Studies (CIRPAS) Twin Otter (TO) research aircraft, which was equipped with standard meteorological instruments, a zenith pointing cloud radar and probes that measured aerosol, cloud, and precipitation characteristics.The temporal variation and vertical distribution of aerosols observed from the 15 flights, which included the most intense African dust event during all of 2010 in Barbados, showed a wide range of aerosol conditions. During dusty periods, aerosol concentrations increased substantially in the size range between 0.5 and 10 µm (diameter), particles that are large enough to be effective giant cloud condensation nuclei (CCN). The 10-day back trajectories showed three distinct air masses with distinct vertical structures associated with air masses originating in the Atlantic (typical maritime air mass with relatively low aerosol concentrations in the marine boundary layer), Africa (Saharan air layer), and mid-latitudes (continental pollution plumes). Despite the large differences in the total mass loading and the origin of the aerosols, the overall shapes of the aerosol particle size distributions were consistent, with the exception of the transition period.The TO was able to sample many clouds at various phases of growth. Maximum cloud depth observed was less than ˜ 3 km, while most clouds were less than 1 km

  7. Black carbon mixing state impacts on cloud microphysical properties: effects of aerosol plume and environmental conditions

    SciTech Connect

    Ching, Ping Pui; Riemer, Nicole; West, Matthew

    2016-05-27

    Black carbon (BC) is usually mixed with other aerosol species within individual aerosol particles. This mixture, along with the particles' size and morphology, determines the particles' optical and cloud condensation nuclei properties, and hence black carbon's climate impacts. In this study the particle-resolved aerosol model PartMC-MOSAIC was used to quantify the importance of black carbon mixing state for predicting cloud microphysical quantities. Based on a set of about 100 cloud parcel simulations a process level analysis framework was developed to attribute the response in cloud microphysical properties to changes in the underlying aerosol population ("plume effect") and the cloud parcel cooling rate ("parcel effect"). It shows that the response of cloud droplet number concentration to changes in BC emissions depends on the BC mixing state. When the aerosol population contains mainly aged BC particles an increase in BC emission results in increasing cloud droplet number concentrations ("additive effect"). In contrast, when the aerosol population contains mainly fresh BC particles they act as sinks for condensable gaseous species, resulting in a decrease in cloud droplet number concentration as BC emissions are increased ("competition effect"). Additionally, we quantified the error in cloud microphysical quantities when neglecting the information on BC mixing state, which is often done in aerosol models. The errors ranged from -12% to +45% for the cloud droplet number fraction, from 0% to +1022% for the nucleation-scavenged black carbon (BC) mass fraction, from -12% to +4% for the effective radius, and from -30% to +60% for the relative dispersion.

  8. Dimethylsulfide/cloud condensation nuclei/climate system - Relevant size-resolved measurements of the chemical and physical properties of atmospheric aerosol particles

    NASA Technical Reports Server (NTRS)

    Quinn, P. K.; Covert, D. S.; Bates, T. S.; Kapustin, V. N.; Ramsey-Bell, D. C.; Mcinnes, L. M.

    1993-01-01

    The mass and number relationships occurring within the atmospheric dimethylsulfide/cloud condensation nuclei (CCN)/climate system, using simultaneous measurements of particulate phase mass size distributions of nss SO4(2-), methanesulfonic acid (MSA), and NH4(+); number size distributions of particles having diameters between 0.02 and 9.6 microns; CCN concentrations at a supersaturation of 0.3 percent; relative humidity; and temperature, obtained for the northeastern Pacific Ocean in April and May 1991. Based on these measurements, particulate nss SO4(2-), MSA, and NH4(+) mass appeared to be correlated with both particle effective surface area and number in the accumulation mode size range (0.16 to 0.5 micron). No correlations were found in the size range below 0.16 micron. A correlation was also found between nss SO4(2-) mass and the CCN number concentration, such that a doubling of the SO4(2-) mass corresponded to a 40 percent increase in the CCN number concentration. However, no correlation was found between MSA mass and CCN concentration.

  9. Model simulations of the first aerosol indirect effect and comparison of cloud susceptibility fo satellite measurements

    SciTech Connect

    Chuang, C; Penner, J E; Kawamoto, K

    2002-03-08

    Present-day global anthropogenic emissions contribute more than half of the mass in submicron particles primarily due to sulfate and carbonaceous aerosol components derived from fossil fuel combustion and biomass burning. These anthropogenic aerosols modify the microphysics of clouds by serving as cloud condensation nuclei (CCN) and enhance the reflectivity of low-level water clouds, leading to a cooling effect on climate (the Twomey effect or first indirect effect). The magnitude of the first aerosol indirect effect is associated with cloud frequency as well as a quantity representing the sensitivity of cloud albedo to changes in cloud drop number concentration. This quantity is referred to as cloud susceptibility [Twomey, 1991]. Analysis of satellite measurements demonstrates that marine stratus clouds are likely to be of higher susceptibility than continental clouds because of their lower number concentrations of cloud drops [Platnick and Twomey, 1994]. Here, we use an improved version of the fully coupled climate/chemistry model [Chuang et al., 1997] to calculate the global concentrations Of sulfate, dust, sea salt, and carbonaceous aerosols (biomass smoke and fossil fuel organic matter and black carbon). We investigated the impact of anthropogenic aerosols on cloud susceptibility and calculated the associated changes of shortwave radiative fluxes at the top of the atmosphere. We also examined the correspondence between the model simulation of cloud susceptibility and that inferred from satellite measurements to test whether our simulated aerosol concentrations and aerosol/cloud interactions give a faithful representation of these features.

  10. The role of aerosols in cloud drop parameterizations and its applications in global climate models

    SciTech Connect

    Chuang, C.C.; Penner, J.E.

    1996-04-01

    The characteristics of the cloud drop size distribution near cloud base are initially determined by aerosols that serve as cloud condensation nuclei and the updraft velocity. We have developed parameterizations relating cloud drop number concentration to aerosol number and sulfate mass concentrations and used them in a coupled global aerosol/general circulation model (GCM) to estimate the indirect aerosol forcing. The global aerosol model made use of our detailed emissions inventories for the amount of particulate matter from biomass burning sources and from fossil fuel sources as well as emissions inventories of the gas-phase anthropogenic SO{sub 2}. This work is aimed at validating the coupled model with the Atmospheric Radiation Measurement (ARM) Program measurements and assessing the possible magnitude of the aerosol-induced cloud effects on climate.

  11. Assessment of aerosol-cloud interactions during southern African biomass burning activity, employing cloud parameterizations

    NASA Astrophysics Data System (ADS)

    Wiston, Modise; McFiggans, Gordon; Schultz, David

    2015-04-01

    In this study, we perform a simulation of the spatial distributions of particle and gas concentrations from a significantly large source of pollution event during a dry season in southern Africa and their interactions with cloud processes. Specific focus is on the extent to which cloud-aerosol interactions are affected by various inputs (i.e. emissions) and parameterizations and feedback mechanisms in a coupled mesoscale chemistry-meteorology model -herein Weather Research and Forecasting model with chemistry (WRF-Chem). The southern African dry season (May-Sep) is characterised by biomass burning (BB) type of pollution. During this period, BB particles are frequently observed over the subcontinent, at the same time a persistent deck of stratocumulus covers the south West African coast, favouring long-range transport over the Atlantic Ocean of aerosols above clouds. While anthropogenic pollutants tend to spread more over the entire domain, biomass pollutants are concentrated around the burning areas, especially the savannah and tropical rainforest of the Congo Basin. BB is linked to agricultural practice at latitudes south of 10° N. During an intense burning event, there is a clear signal of strong interactions of aerosols and cloud microphysics. These species interfere with the radiative budget, and directly affect the amount of solar radiation reflected and scattered back to space and partly absorbed by the atmosphere. Aerosols also affect cloud microphysics by acting as cloud condensation nuclei (CCN), modifying precipitation pattern and the cloud albedo. Key area is to understand the role of pollution on convective cloud processes and its impacts on cloud dynamics. The hypothesis is that an environment of potentially high pollution enables the probability of interactions between co-located aerosols and cloud layers. To investigate this hypothesis, we outline an approach to integrate three elements: i) focusing on regime(s) where there are strong indications of

  12. Constraining the aerosol influence on cloud fraction

    NASA Astrophysics Data System (ADS)

    Gryspeerdt, E.; Quaas, J.; Bellouin, N.

    2016-04-01

    Aerosol-cloud interactions have the potential to modify many different cloud properties. There is significant uncertainty in the strength of these aerosol-cloud interactions in analyses of observational data, partly due to the difficulty in separating aerosol effects on clouds from correlations generated by local meteorology. The relationship between aerosol and cloud fraction (CF) is particularly important to determine, due to the strong correlation of CF to other cloud properties and its large impact on radiation. It has also been one of the hardest to quantify from satellites due to the strong meteorological covariations involved. This work presents a new method to analyze the relationship between aerosol optical depth (AOD) and CF. By including information about the cloud droplet number concentration (CDNC), the impact of the meteorological covariations is significantly reduced. This method shows that much of the AOD-CF correlation is explained by relationships other than that mediated by CDNC. By accounting for these, the strength of the global mean AOD-CF relationship is reduced by around 80%. This suggests that the majority of the AOD-CF relationship is due to meteorological covariations, especially in the shallow cumulus regime. Requiring CDNC to mediate the AOD-CF relationship implies an effective anthropogenic radiative forcing from an aerosol influence on liquid CF of -0.48 W m-2 (-0.1 to -0.64 W m-2), although some uncertainty remains due to possible biases in the CDNC retrievals in broken cloud scenes.

  13. Analysis of Arctic Cloud Thermodynamic Phase Susceptibility to Aerosols.

    NASA Astrophysics Data System (ADS)

    Coopman, Q.; Garrett, T. J.; Riedi, J.; Eckhardt, S.; Stohl, A.

    2014-12-01

    Even if Arctic is remote from industrialized areas, this region is influenced by elevated concentration of aerosols from mid-latitude, especially during winter. This is mainly due to the decrease of wet scavenging and the surface temperature inversion, both acting as a trap for the atmospheric particles. Aerosols play a key role on cloud's microphysics, because they act as Cloud Condensation Nuclei (CCN) or Ice Nuclei (IN). Both nuclei influence directly on cloud's presence and formation, potentially impacting also thermodynamic phase transition through different mechanisms, which in turn affect cloud radiative properties and forcing. In our study we used two sets of data: i) A combination of POLDER-3/PARASOL and MODIS/AQUA satellite measurements to retrieve cloud properties; ii) The numerical transport model FLEXPART which use carbon monoxide tracer to inform on concentration of biomass burning and anthropogenic aerosols. The main advantage of combining these two sets of data is to obtain large statistics about clouds that have been potentially influenced by varied concentrations of aerosol. We report here results of a study in which we analyze potential interaction between clouds and aerosols from biomass burning and anthropogenic sources. We first analyzed the temperature at which thermodynamic phase transition is most likely to occur according to the types and concentrations of aerosols. It is shown a correlation between the temperature of thermodynamic phase transition and aerosols concentrations and type. Unlike we could have expected from previous studies, preliminary analyses suggest that aerosols from anthropogenic sources accelerate the liquid-ice transition whereas aerosols from biomass burning inhibit the transition from water to ice. Different hypotheses can be responsible for this observation and we analyze parameters that can play a role on the transition temperature shift and how aerosols act as an inhibitor or activator of the phase transition, for

  14. Aerosol-cloud interaction using AATSR

    NASA Astrophysics Data System (ADS)

    Sogacheva, Larisa; Kolmonen, Pekka; Virtanen, Timo H.; Saponaro, Giulia; Kokhanovsky, Alexander; de Leeuw, Gerrit

    2014-05-01

    Aerosols and clouds play an important role in terrestrial atmospheric dynamics, thermodynamics, chemistry, and radiative transfer and are key elements of the water and energy cycles. The interactions between aerosol particles and cloud drops is critical to identifying how much they reflect solar radiation. Accurate evaluation of the effects of aerosols and clouds on climate requires global information on aerosol properties. Such global information can only be provided using satellite remote sensing. Among the satellite instruments used for aerosol and cloud retrieval is the Advanced Along-Track Scanning Radiometer (AATSR) on board the European Space Agency (ESA) satellite ENVISAT. Many instruments and retrieval techniques have been developed and applied to satellite data to derive cloud data products (Kokhanonsky et al., 2009). However, many problems still remain to be solved. They are mostly related to the usage of homogeneous, single-layered cloud model. Further issues exist for studies of thin clouds, where both cloud inhomogeniety, cloud fraction and the underlying surface bi-directional reflectance must be accounted for in the retrieval process. The aerosol retrieval algorithm (dual-view over land and single-view over ocean) was constructed for ATSR-2 data (e.g. Veefkind et al. 1998). The most recent version of ADV (AATSR Dual View) is described in Kolmenen et al. (2013). The ATSR dual-view allows retrieval without prior information about land surface reflectance. A semi-analytical cloud retrieval algorithm using backscattered radiation in 0.4-2.4 μm spectral region has been implemented to ADV for the determination of the optical thickness, the liquid water path, and the effective size of droplets from spectral measurements of the intensity of light reflected from water clouds with large optical thickness. In AacDV (AATSR aerosol and cloud Dual View) aerosol and cloud retrievals are combined. Cloud retrieval starts when cloud tests for aerosol retrieval show

  15. Effects of Ocean Ecosystem on Marine Aerosol-Cloud Interaction

    DOE PAGES

    Meskhidze, Nicholas; Nenes, Athanasios

    2010-01-01

    Using smore » atellite data for the surface ocean, aerosol optical depth (AOD), and cloud microphysical parameters, we show that statistically significant positive correlations exist between ocean ecosystem productivity, the abundance of submicron aerosols, and cloud microphysical properties over different parts of the remote oceans. The correlation coefficient for remotely sensed surface chlorophyll a concentration ([Chl- a ]) and liquid cloud effective radii over productive areas of the oceans varies between − 0.2 and − 0.6 . Special attention is given to identifying (and addressing) problems from correlation analysis used in the previous studies that can lead to erroneous conclusions. A new approach (using the difference between retrieved AOD and predicted sea salt aerosol optical depth, AOD diff ) is developed to explore causal links between ocean physical and biological systems and the abundance of cloud condensation nuclei (CCN) in the remote marine atmosphere. We have found that over multiple time periods, 550 nm AOD diff (sensitive to accumulation mode aerosol, which is the prime contributor to CCN) correlates well with [Chl- a ] over the productive waters of the Southern Ocean. Since [Chl- a ] can be used as a proxy of ocean biological productivity, our analysis demonstrates the role of ocean ecology in contributing CCN, thus shaping the microphysical properties of low-level marine clouds.« less

  16. Determining the chemical composition of cloud condensation nuclei

    SciTech Connect

    Williams, A.L.; Rothert, J.E.; McClure, K.E. ); Alofs, D.J.; Hagen, D.E.; White, D.R.; Hopkins, A.R.; Trueblood, M.B. . Cloud and Aerosol Science Lab.)

    1992-02-01

    This second progress report describes the status of the project one and one-half years after the start. The goal of the project is to develop the instrumentation to collect cloud condensation nuclei (CCN) in sufficient amounts to determine their chemical composition, and to survey the CCN composition in different climates through a series of field measurements. Our approach to CCN collection is to first form droplets on the nuclei under simulated cloud humidity conditions, which is the only known method of identifying CCN from the background aerosol. Under cloud chamber conditions, the droplets formed become larger than the surrounding aerosol, and can then be removed by inertial impaction. The residue of the evaporated droplets represents the sample to be chemically analyzed. Two size functions of CCN particles are collected by first forming droplets on the large particles are collected by first forming droplets on the large CCN in a haze chamber at 100% relative humidity, and then activating the remaining CCN at 1% supersaturation in a cloud chamber. The experimental apparatus is a serious flow arrangement consisting of an impactor to remove the large aerosol particles, a haze chamber to form droplets on the remaining larger CCN, another impactor to remove the haze droplets containing the larger CCN particles for chemical analysis, a continuous flow diffusion (CFD) cloud chamber to form droplets on the remaining smaller CCN, and a third impactor to remove the droplets for the small CCN sample. Progress is documented here on the development of each of the major components of the flow system. Chemical results are reported on tests to determine suitable wicking material for the different plates. Results of computer modeling of various impactor flows are discussed.

  17. Effects of aerosol sources and chemical compositions on cloud drop sizes and glaciation temperatures

    NASA Astrophysics Data System (ADS)

    Zipori, Assaf; Rosenfeld, Daniel; Tirosh, Ofir; Teutsch, Nadya; Erel, Yigal

    2015-09-01

    The effect of aerosols on cloud properties, such as its droplet sizes and its glaciation temperatures, depends on their compositions and concentrations. In order to examine these effects, we collected rain samples in northern Israel during five winters (2008-2011 and 2013) and determined their chemical composition, which was later used to identify the aerosols' sources. By combining the chemical data with satellite-retrieved cloud properties, we linked the aerosol types, sources, and concentrations with the cloud glaciation temperatures (Tg). The presence of dust increased Tg from -26°C to -12°C already at relatively low dust concentrations. This result is in agreement with the conventional wisdom that desert dust serves as good ice nuclei (INs). With higher dust concentrations, Tg saturated at -12°C, even though cloud droplet sizes decreased as a result of the cloud condensation nucleating (CCN) activity of the dust. Marine air masses also encouraged freezing, but in this case, freezing was enhanced by the larger cloud droplet sizes in the air masses (caused by low CCN concentrations) and not by IN concentrations or by aerosol type. An increased fraction of anthropogenic aerosols in marine air masses caused a decrease in Tg, indicating that these aerosols served as poor IN. Anthropogenic aerosols reduced cloud droplet sizes, which further decreased Tg. Our results could be useful in climate models for aerosol-cloud interactions, as we investigated the effects of aerosols of different sources on cloud properties. Such parameterization can simplify these models substantially.

  18. Aerosol-cloud closure study using RPAS measurements

    NASA Astrophysics Data System (ADS)

    Calmer, R.; Roberts, G.; Sanchez, K. J.; Nicoll, K.; Preissler, J.; Ovadnevaite, J.; Sciare, J.; Bronz, M.; Hattenberger, G.; Rosenfeld, D.; Lauda, S.; Hashimshoni, E.

    2015-12-01

    Enhancements in Remotely Piloted Aircraft Systems (RPAS) have increased their possible uses in many fields for the past two decades. For atmospheric research, ultra-light RPAS (< 2.5kg) are now able to fly at altitudes greater than 3 km and even in cloud, which opens new opportunities to understand aerosol-cloud interactions. We are deploying the RPAS as part of the European project BACCHUS (Impact of Biogenic versus Anthropogenic Emissions on Clouds and Climate: towards a Holistic Understanding). Field experiments in Cyprus and Ireland have already been conducted to study aerosol-cloud interactions in climatically different environments. The RPAS are being utilized in this study with the purpose of complementing ground-based observations of cloud condensation nuclei (CCN) to conduct aerosol-cloud closure studies Cloud microphysical properties such as cloud drop number concentration and size can be predicted directly from the measured CCN spectrum and the observed updraft, the vertical component of the wind vector [e.g., Conant et al, 2004]. On the RPAS, updraft measurements are obtained from a 5-hole probe synchronized with an Inertial Measurement Unit (IMU). The RPA (remotely piloted aircraft) are programmed to fly at a level leg just below cloud base to measure updraft measurements while a scanning CCN counter is stationed at ground level. Vertical profiles confirm that CCN measurements on the ground are representative to those at cloud base. An aerosol-cloud parcel model is implemented to model the cloud droplet spectra associated with measured updraft velocities. The model represents the particle size domain with internally mixed chemical components, using a fixed-sectional approach [L. M. Russell and Seinfeld, 1998]. The model employs a dual moment (number and mass) algorithm to calculate growth of particles from one section to the next for non-evaporating species. Temperature profiles, cloud base, updraft velocities and aerosol size and composition, all

  19. The Aerosol, Clouds and Ecosystem (ACE) Mission

    NASA Astrophysics Data System (ADS)

    Schoeberl, M.; Remer, L.; Kahn, R.; Starr, D.; Hildebrand, P.; Colarco, P.; Diner, D.; Vane, D.; Im, E.; Behrenfeld, M.; Stephens, G.; Maring, H.; Bontempi, P.; Martins, J. V.

    2008-12-01

    The Aerosol, Clouds and Ecosystem (ACE) Mission is a second tier Decadal Survey mission designed to characterize the role of aerosols in climate forcing, especially their impact on precipitation and cloud formation. ACE also includes ocean biosphere measurements (chlorophyll and dissolved organic materials) which will be greatly improved by simultaneous measurements of aerosols. The nominal ACE payload includes lidar and multiangle spectropolarimetric polarimetric measurements of aerosols, radar measurements of clouds and multi-band spectrometer for the measurement of ocean ecosystems. An enhancement to ACE payload under consideration includes µ-wave radiometer measurements of cloud ice and water outside the nadir path of the radar/lidar beams. This talk will cover ACE instrument and science options, updates on the science team definition activity and science potential.

  20. Reformulating Aerosol Thermodynamics and Cloud Microphysics

    NASA Astrophysics Data System (ADS)

    Metzger, S.

    2006-12-01

    Modeling aerosol composition and cloud microphysics is rather complex due to the required thermodynamics, even if chemical and thermodynamical equilibrium is assumed. We show, however, that for deliquescent atmospheric aerosols thermodynamics can be considerably simplified, if we reformulate chemical equilibrium to include water purely based on thermodynamic principles. In chemical and thermodynamical equilibrium, the relative humidity (RH) fixes the molality of atmospheric aerosols. Although this fact is in theory well known, it has hardly been utilized in aerosol modeling nor has been the fact that for the same reason also the aerosol activity (including activity coefficients) and water content are fixed (by RH) for a given aerosol concentration and type. The only model that successfully utilizes this fact is the computationally very efficient EQuilibrium Simplified thermodynamic gas/Aerosol partitioning Model, EQSAM (Metzger et al., 2002a), EQSAM2 (Metzger et al., 2006). In both versions the entire gas/liquid/solid aerosol equilibrium partitioning is solved analytically and hence non-iteratively a substantial advantage in aerosol composition modeling. Here we briefly present the theoretical framework of EQSAM2, which differs from EQSAM in a way that the calculation of the water activity of saturated binary or mixed inorganic/organic salt solutions of multi-component aerosols has been generalized by including the Kelvin-term, thus allowing for any solute activity above the deliquescence relative humidity, including supersaturation. With application of our new concept to a numerical whether prediction (NWP) model, we demonstrate its wide implications for the computation of various aerosol and cloud properties, as our new concept allows to consistently and efficiently link the modeling of aerosol thermodynamics and cloud microphysics through the aerosol water mass, which therefore deserves special attention in atmospheric chemistry, air pollution, NWP and climate

  1. Applying super-droplets as a compact representation of warm-rain microphysics for aerosol-cloud-aerosol interactions

    NASA Astrophysics Data System (ADS)

    Arabas, S.; Jaruga, A.; Pawlowska, H.; Grabowski, W. W.

    2012-12-01

    Clouds may influence aerosol characteristics of their environment. The relevant processes include wet deposition (rainout or washout) and cloud condensation nuclei (CCN) recycling through evaporation of cloud droplets and drizzle drops. Recycled CCN physicochemical properties may be altered if the evaporated droplets go through collisional growth or irreversible chemical reactions (e.g. SO2 oxidation). The key challenge of representing these processes in a numerical cloud model stems from the need to track properties of activated CCN throughout the cloud lifecycle. Lack of such "memory" characterises the so-called bulk, multi-moment as well as bin representations of cloud microphysics. In this study we apply the particle-based scheme of Shima et al. 2009. Each modelled particle (aka super-droplet) is a numerical proxy for a multiplicity of real-world CCN, cloud, drizzle or rain particles of the same size, nucleus type,and position. Tracking cloud nucleus properties is an inherent feature of the particle-based frameworks, making them suitable for studying aerosol-cloud-aerosol interactions. The super-droplet scheme is furthermore characterized by linear scalability in the number of computational particles, and no numerical diffusion in the condensational and in the Monte-Carlo type collisional growth schemes. The presentation will focus on processing of aerosol by a drizzling stratocumulus deck. The simulations are carried out using a 2D kinematic framework and a VOCALS experiment inspired set-up (see http://www.rap.ucar.edu/~gthompsn/workshop2012/case1/).

  2. New approaches to quantifying aerosol influence on the cloud radiative effect.

    PubMed

    Feingold, Graham; McComiskey, Allison; Yamaguchi, Takanobu; Johnson, Jill S; Carslaw, Kenneth S; Schmidt, K Sebastian

    2016-05-24

    The topic of cloud radiative forcing associated with the atmospheric aerosol has been the focus of intense scrutiny for decades. The enormity of the problem is reflected in the need to understand aspects such as aerosol composition, optical properties, cloud condensation, and ice nucleation potential, along with the global distribution of these properties, controlled by emissions, transport, transformation, and sinks. Equally daunting is that clouds themselves are complex, turbulent, microphysical entities and, by their very nature, ephemeral and hard to predict. Atmospheric general circulation models represent aerosol-cloud interactions at ever-increasing levels of detail, but these models lack the resolution to represent clouds and aerosol-cloud interactions adequately. There is a dearth of observational constraints on aerosol-cloud interactions. We develop a conceptual approach to systematically constrain the aerosol-cloud radiative effect in shallow clouds through a combination of routine process modeling and satellite and surface-based shortwave radiation measurements. We heed the call to merge Darwinian and Newtonian strategies by balancing microphysical detail with scaling and emergent properties of the aerosol-cloud radiation system.

  3. New approaches to quantifying aerosol influence on the cloud radiative effect

    NASA Astrophysics Data System (ADS)

    Feingold, Graham; McComiskey, Allison; Yamaguchi, Takanobu; Johnson, Jill S.; Carslaw, Kenneth S.; Schmidt, K. Sebastian

    2016-05-01

    The topic of cloud radiative forcing associated with the atmospheric aerosol has been the focus of intense scrutiny for decades. The enormity of the problem is reflected in the need to understand aspects such as aerosol composition, optical properties, cloud condensation, and ice nucleation potential, along with the global distribution of these properties, controlled by emissions, transport, transformation, and sinks. Equally daunting is that clouds themselves are complex, turbulent, microphysical entities and, by their very nature, ephemeral and hard to predict. Atmospheric general circulation models represent aerosol-cloud interactions at ever-increasing levels of detail, but these models lack the resolution to represent clouds and aerosol-cloud interactions adequately. There is a dearth of observational constraints on aerosol-cloud interactions. We develop a conceptual approach to systematically constrain the aerosol-cloud radiative effect in shallow clouds through a combination of routine process modeling and satellite and surface-based shortwave radiation measurements. We heed the call to merge Darwinian and Newtonian strategies by balancing microphysical detail with scaling and emergent properties of the aerosol-cloud radiation system.

  4. New approaches to quantifying aerosol influence on the cloud radiative effect

    DOE PAGES

    Feingold, Graham; McComiskey, Allison; Yamaguchi, Takanobu; ...

    2016-02-01

    The topic of cloud radiative forcing associated with the atmospheric aerosol has been the focus of intense scrutiny for decades. The enormity of the problem is reflected in the need to understand aspects such as aerosol composition, optical properties, cloud condensation, and ice nucleation potential, along with the global distribution of these properties, controlled by emissions, transport, transformation, and sinks. Equally daunting is that clouds themselves are complex, turbulent, microphysical entities and, by their very nature, ephemeral and hard to predict. Atmospheric general circulation models represent aerosol-cloud interactions at ever-increasing levels of detail, but these models lack the resolution tomore » represent clouds and aerosol-cloud interactions adequately. There is a dearth of observational constraints on aerosol-cloud interactions. We develop a conceptual approach to systematically constrain the aerosol-cloud radiative effect in shallow clouds through a combination of routine process modeling and satellite and surface-based shortwave radiation measurements. We heed the call to merge Darwinian and Newtonian strategies by balancing microphysical detail with scaling and emergent properties of the aerosol-cloud radiation system.« less

  5. Aerosol and cloud retrieval using AATSR

    NASA Astrophysics Data System (ADS)

    Sogacheva, Larisa; Kolmonen, Pekka; Virtanen, Timo; Saponaro, Giulia; Kokhanovsky, Alexander; de Leeuw, Gerrit

    2013-04-01

    Aerosols and clouds play an important role in terrestrial atmospheric dynamics, thermodynamics, chemistry, and radiative transfer and are key elements of the water and energy cycles. Accurate evaluation of the effects of aerosols and clouds on climate requires global information on aerosol properties. Such global information can only be provided using satellite remote sensing. Among the satellite instruments used for aerosol and cloud retrieval is the Advanced Along-Track Scanning Radiometer (AATSR) on board the European Space Agency (ESA) satellite ENVISAT. Many instruments and retrieval techniques have been developed and applied to satellite data to derive cloud data products (Kokhanonsky et al., 2009). However, many problems still remain to be solved. They are mostly related to the usage of homogeneous, single-layered cloud model. Further issues exist for studies of thin clouds, where both cloud inhomogeniety, cloud fraction and the underlying surface bi-directional reflectance must be accounted for in the retrieval process. The aerosol retrieval algorithm (dual-view over land and single-view over ocean) was constructed for ATSR-2 data (e.g. Veefkind et al. 1998). The most recent version of ADV (AATSR Dual View) is described in Kolmenen et al. (2012). The ATSR dual-view allows retrieval without prior information about land surface reflectance. A semi-analytical cloud retrieval algorithm using backscattered radiation in 0.4-2.4 μm spectral region has recently been implemented to ADV for the determination of the optical thickness, the liquid water path, and the effective size of droplets from spectral measurements of the intensity of light reflected from water clouds with large optical thickness. In AacDV (AATSR aerosol and cloud Dual View) aerosol and cloud retrievals are combined. Cloud retrieval starts when cloud tests for aerosol retrieval show the presence of clouds. The algorithm was early introduced in Kokhanovsky et al. (2003). It works well for thick

  6. Arctic Aerosol-­Cloud Interactions during ASCOS

    NASA Astrophysics Data System (ADS)

    Stevens, R.; Hill, A. A.; Shipway, B. J.; Field, P.; Carslaw, K. S.

    2015-12-01

    A decrease in Arctic sea ice extent and thickness has been observed within recent decades. Further decreases are expected to increase the fluxes aerosol and precursor gases from the open ocean surface within the Arctic. The resulting increase in cloud condensation nuclei (CCN) concentrations would be expected to result in increased cloud albedo (Struthers et al, 2011), leading to potentially large changes in radiative forcings.However, Browse et al. (2014) have shown that these increases in condensable material could also result in the growth of existing particles to sizes where they are more efficiently removed by wet deposition in drizzling stratocumulus clouds, ultimately decreasing CCN concentrations in the high Arctic. The study of Browse et al (2014) was limited in that it did not simulate alterations of dynamics or cloud properties due to either changes in heat and moisture fluxes following sea­-ice loss or changing aerosol concentrations.Taken together, the results of Struthers et al (2011) and Browse et al (2014) show that significant uncertainties remain in trying to quantify aerosol­-cloud processes in the poorly understood Arctic system. It is likely that the CCN response to sea-­ice loss is controlled by many interrelated processes and unlikely that the current representation of these processes in global climate models include is sufficient to realistically simulate long­-term changes.Using the Met Office Unified Model (UM) including Cloud AeroSol Interactions Microphysics (CASIM), we perform a case study of summertime high Arctic (>80N) clouds in order to better understand the processes currently governing Arctic clouds, and how they may change in the future. We compare our results with observations obtained during the 2008 ASCOS campaign. We then perform sensitivity studies to assess the changes in cloud properties to reductions in sea­-ice, through either changes in fluxes of surface heat and moisture or changes in fluxes of aerosol and

  7. Aerosol impacts on radiative and microphysical properties of clouds and precipitation formation

    NASA Astrophysics Data System (ADS)

    Alizadeh-Choobari, O.; Gharaylou, M.

    2017-03-01

    Through modifying the number concentration and size of cloud droplets, aerosols have intricate impacts on radiative and microphysical properties of clouds, which together influence precipitation processes. Aerosol-cloud interactions for a mid-latitude convective cloud system are investigated using a two-moment aerosol-aware bulk microphysical scheme implemented into the Weather Research and Forecasting (WRF) model. Three sensitivity experiments with initial identical dynamic and thermodynamic conditions, but different cloud-nucleating aerosol concentrations were conducted. Increased aerosol number concentration has resulted in more numerous cloud droplets of overall smaller sizes, through which the optical properties of clouds have been changed. While the shortwave cloud forcing is significantly increased in more polluted experiments, changes in the aerosol number concentration have negligible impacts on the longwave cloud forcing. For the first time, it is found that polluted clouds have higher cloud base heights, the feature that is caused by more surface cooling due to a higher shortwave cloud forcing, as well as a drier boundary layer in the polluted experiment compared to the clean. The polluted experiment was also associated with a higher liquid water content (LWC), caused by an increase in the number of condensation of water vapor due to higher concentration of hygroscopic aerosols acting as condensation nuclei. The domain-averaged accumulated precipitation is little changed under both polluted and clean atmosphere. Nevertheless, changes in the rate of precipitation are identified, such that under polluted atmosphere light rain is reduced, while both moderate and heavy rain are intensified, confirming the fact that if an ample influx of water vapor exists, an increment of hygroscopic aerosols can increase the amount of precipitation.

  8. Cloud condensation nuclei in polluted air and biomass burning smoke near the mega-city Guangzhou, China - Part 1: Size-resolved measurements and implications for the modeling of aerosol particle hygroscopicity and CCN activity

    NASA Astrophysics Data System (ADS)

    Rose, D.; Nowak, A.; Achtert, P.; Wiedensohler, A.; Hu, M.; Shao, M.; Zhang, Y.; Andreae, M. O.; Pöschl, U.

    2008-09-01

    Atmospheric aerosol particles serving as cloud condensation nuclei (CCN) are key elements of the hydrological cycle and climate, but their abundance, properties and sources are highly variable and not well known. We have measured and characterized CCN in polluted air and biomass burning smoke during the PRIDE-PRD2006 campaign on 1 30 July 2006 at a rural site ~60 km northwest of the mega-city Guangzhou in southeastern China. CCN efficiency spectra (activated fraction vs. dry particle diameter; 20 300 nm) were recorded at water vapor supersaturations (S) in the range of 0.07% to 1.27%. Depending on S, the dry CCN activation diameters were in the range of 30 200 nm, corresponding to effective hygroscopicity parameters κ in the range of 0.1 0.5. The hygroscopicity of particles in the accumulation size range was generally higher than that of particles in the nucleation and Aitken size range. The campaign average value of κ for all aerosol particles across the investigated size range was 0.3, which equals the average value of κ for other continental locations. During a strong local biomass burning event, the activation diameters increased by ~10% and the average value of κ dropped to 0.2, which can be considered as characteristic for freshly emitted smoke from the burning of agricultural waste. At low S (≤0.27%), the maximum activated fraction remained generally well below one, which indicates substantial proportions of externally mixed CCN-inactive particles with much lower hygroscopicity most likely soot particles (up to ~60% at ~250 nm). The mean CCN number concentrations (NCCN,S) ranged from 1100 cm-3 at S=0.07% to 16 000 cm-3 at S=1.27%, representing ~7% to ~85% of the total aerosol particle number concentration. Based on the measurement data, we have tested different model approaches (power laws and κ-Köhler model) for the approximation/prediction of NCCN,S as a function of water vapor supersaturation, aerosol particle number concentration, size

  9. Impact of Aerosols on Convective Clouds and Precipitation

    NASA Technical Reports Server (NTRS)

    Tao, Wei-Kuo; Chen, Jen-Ping; Li, Zhanqing; Wang, Chien; Zhang, Chidong; Li, Xiaowen

    2012-01-01

    Aerosols are a critical.factor in the atmospheric hydrological cycle and radiation budget. As a major agent for clouds to form and a significant attenuator of solar radiation, aerosols affect climate in several ways. Current research suggests that aerosols have a major impact on the dynamics, microphysics, and electrification properties of continental mixed-phase convective clouds. In addition, high aerosol concentrations in urban environments could affect precipitation variability by providing a significant source of cloud condensation nuclei (CCN). Such pollution . effects on precipitation potentially have enormous climatic consequences both in terms of feedbacks involving the land surface via rainfall as well as the surface energy budget and changes in latent heat input to the atmosphere. Basically, aerosol concentrations can influence cloud droplet size distributions, the warm-rain process, the cold-rain process, cloud-top heights, the depth of the mixed-phase region, and the occurrence of lightning. Recently, many cloud resolution models (CRMs) have been used to examine the role of aerosols on mixed-phase convective clouds. These modeling studies have many differences in terms of model configuration (two- or three-dimensional), domain size, grid spacing (150-3000 m), microphysics (two-moment bulk, simple or sophisticated spectral-bin), turbulence (1st or 1.5 order turbulent kinetic energy (TKE)), radiation, lateral boundary conditions (i.e., closed, radiative open or cyclic), cases (isolated convection, tropical or midlatitude squall lines) and model integration time (e.g., 2.5 to 48 hours). Among these modeling studies, the most striking difference is that cumulative precipitation can either increase or decrease in response to higher concentrations of CCN. In this presentation, we review past efforts and summarize our current understanding of the effect of aerosols on convective precipitation processes. Specifically, this paper addresses the following topics

  10. Distinct Impacts of Aerosols on an Evolving Continental Cloud Complex during the RACORO Field Campaign

    DOE PAGES

    Lin, Yun; Wang, Yuan; Pan, Bowen; ...

    2016-08-26

    In this study, a continental cloud complex, consisting of shallow cumuli, a deep convective cloud (DCC), and stratus, is simulated by a cloud-resolving Weather Research and Forecasting Model to investigate the aerosol microphysical effect (AME) and aerosol radiative effect (ARE) on the various cloud regimes and their transitions during the Department of Energy Routine Atmospheric Radiation Measurement Aerial Facility Clouds with Low Optical Water Depths Optical Radiative Observations (RACORO) campaign. Under an elevated aerosol loading with AME only, a reduced cloudiness for the shallow cumuli and stratus resulted from more droplet evaporation competing with suppressed precipitation, but an enhanced cloudinessmore » for the DCC is attributed to more condensation. With the inclusion of ARE, the shallow cumuli are suppressed owing to the thermodynamic effects of light-absorbing aerosols. The responses of DCC and stratus to aerosols are monotonic with AME only but nonmonotonic with both AME and ARE. The DCC is invigorated because of favorable convection and moisture conditions at night induced by daytime ARE, via the so-called aerosol-enhanced conditional instability mechanism. Finally, the results reveal that the overall aerosol effects on the cloud complex are distinct from the individual cloud types, highlighting that the aerosol–cloud interactions for diverse cloud regimes and their transitions need to be evaluated to assess the regional and global climatic impacts.« less

  11. Distinct Impacts of Aerosols on an Evolving Continental Cloud Complex during the RACORO Field Campaign

    SciTech Connect

    Lin, Yun; Wang, Yuan; Pan, Bowen; Hu, Jiaxi; Liu, Yangang; Zhang, Renyi

    2016-08-26

    In this study, a continental cloud complex, consisting of shallow cumuli, a deep convective cloud (DCC), and stratus, is simulated by a cloud-resolving Weather Research and Forecasting Model to investigate the aerosol microphysical effect (AME) and aerosol radiative effect (ARE) on the various cloud regimes and their transitions during the Department of Energy Routine Atmospheric Radiation Measurement Aerial Facility Clouds with Low Optical Water Depths Optical Radiative Observations (RACORO) campaign. Under an elevated aerosol loading with AME only, a reduced cloudiness for the shallow cumuli and stratus resulted from more droplet evaporation competing with suppressed precipitation, but an enhanced cloudiness for the DCC is attributed to more condensation. With the inclusion of ARE, the shallow cumuli are suppressed owing to the thermodynamic effects of light-absorbing aerosols. The responses of DCC and stratus to aerosols are monotonic with AME only but nonmonotonic with both AME and ARE. The DCC is invigorated because of favorable convection and moisture conditions at night induced by daytime ARE, via the so-called aerosol-enhanced conditional instability mechanism. Finally, the results reveal that the overall aerosol effects on the cloud complex are distinct from the individual cloud types, highlighting that the aerosol–cloud interactions for diverse cloud regimes and their transitions need to be evaluated to assess the regional and global climatic impacts.

  12. A Balloon-Borne Cloud Condensation Nuclei Counter

    NASA Technical Reports Server (NTRS)

    Delene, David J.; Deshler, Terry; Wechsler, Perry; Vali, Gabor A.

    1997-01-01

    A balloon-borne instrument was constructed for observations of vertical profiles of cloud condensation nucleus (CCN) concentrations, active at 1% supersaturation. Droplet concentration in the static thermal-gradient diffusion chamber is deduced from the amount of scattered laser light detected by a photodetector. The photodetector is calibrated using a video camera and computer system to count the number of droplets produced from NaCl aerosol. Preliminary data are available from nine early morning profiles obtained at Laramie, Wyoming, between June 1995 and January 1997. To complement the CCN measurements, instruments that measure condensation nuclei (CN) and aerosols with diameter greater than 0.30 micrometers (D(sub 0.3) were also included on the balloon package. CCN concentrations exhibited a general decrease from the surface to the top of the boundary layers, were generally uniform through well-mixed layers, and show variability above well-mixed layers. In general, the structure of the CCN profile appears to be closely related to the structure in the CN and D(sub 0.3) profiles. Summer profiles generally have CCN concentration greater than 200/cu cm up to 500 mbar, whereas winter profiles are less than 200/cu cm at all levels.

  13. Cloud condensation nuclei in polluted air and biomass burning smoke near the mega-city Guangzhou, China - Part 1: Size-resolved measurements and implications for the modeling of aerosol particle hygroscopicity and CCN activity

    NASA Astrophysics Data System (ADS)

    Rose, D.; Nowak, A.; Achtert, P.; Wiedensohler, A.; Hu, M.; Shao, M.; Zhang, Y.; Andreae, M. O.; Pöschl, U.

    2010-04-01

    Atmospheric aerosol particles serving as Cloud Condensation Nuclei (CCN) are key elements of the hydrological cycle and climate. We measured and characterized CCN in polluted air and biomass burning smoke during the PRIDE-PRD2006 campaign from 1-30 July 2006 at a rural site ~60 km northwest of the mega-city Guangzhou in southeastern China. CCN efficiency spectra (activated fraction vs. dry particle diameter; 20-290 nm) were recorded at water vapor supersaturations (S) in the range of 0.068% to 1.27%. The corresponding effective hygroscopicity parameters describing the influence of particle composition on CCN activity were in the range of κ≍0.1-0.5. The campaign average value of κ=0.3 equals the average value of κ for other continental locations. During a strong local biomass burning event, the average value of κ dropped to 0.2, which can be considered as characteristic for freshly emitted smoke from the burning of agricultural waste. At low S (≤0.27%), the maximum activated fraction remained generally well below one, indicating substantial portions of externally mixed CCN-inactive particles with much lower hygroscopicity - most likely soot particles (up to ~60% at ~250 nm). The mean CCN number concentrations (NCCN,S) ranged from 1000 cm-3 at S=0.068% to 16 000 cm-3 at S=1.27%, which is about two orders of magnitude higher than in pristine air. Nevertheless, the ratios between CCN concentration and total aerosol particle concentration (integral CCN efficiencies) were similar to the ratios observed in pristine continental air (~6% to ~85% at S=0.068% to 1.27%). Based on the measurement data, we have tested different model approaches for the approximation/prediction of NCCN,S. Depending on S and on the model approach, the relative deviations between observed and predicted NCCN,S ranged from a few percent to several hundred percent. The largest deviations occurred at low S with a simple power law. With a Köhler model using variable κ values obtained from

  14. Effect of CALIPSO Cloud Aerosol Discrimination (CAD) Confidence Levels on Observations of Aerosol Properties near Clouds

    NASA Technical Reports Server (NTRS)

    Yang, Weidong; Marshak, Alexander; Varnai, Tamas; Liu, Zhaoyan

    2012-01-01

    CALIPSO aerosol backscatter enhancement in the transition zone between clouds and clear sky areas is revisited with particular attention to effects of data selection based on the confidence level of cloud-aerosol discrimination (CAD). The results show that backscatter behavior in the transition zone strongly depends on the CAD confidence level. Higher confidence level data has a flatter backscatter far away from clouds and a much sharper increase near clouds (within 4 km), thus a smaller transition zone. For high confidence level data it is shown that the overall backscatter enhancement is more pronounced for small clear-air segments and horizontally larger clouds. The results suggest that data selection based on CAD reduces the possible effects of cloud contamination when studying aerosol properties in the vicinity of clouds.

  15. Response of Cloud Condensation Nuclei (> 50 nm) to changes in ion-nucleation

    NASA Astrophysics Data System (ADS)

    Pedersen, J. O.; Enghoff, M. B.; Svensmark, H.

    2012-12-01

    The role of ionization in the formation of clouds and aerosols has been debated for many years. A body of evidence exists that correlates cloud properties to galactic cosmic ray ionization; however these results are still contested. In recent years experimental evidence has also been produced showing that ionization can promote the nucleation of small aerosols at atmospheric conditions. The experiments showed that an increase in ionization leads to an increase in the formation of ultrafine aerosols (~3 nm), but in the real atmosphere such small particles have to grow by coagulation and condensation to become cloud condensation nuclei (CCN) in order to have an effect on clouds. However, numerical studies predict that variations in the count of ultra-fine aerosols will lead only to an insignificant change in the count of CCN. This is due to 1) the competition between the additional ultra-fine aerosols for the limited supply of condensable gases leading to a slower growth and 2) the increased loss rates of the additional particles during the longer growth-time. We investigated the growth of aerosols to CCN sizes using an 8 m3 reaction chamber made from electro-polished stainless steel. One side was fitted with a Teflon foil to allow ultraviolet light to illuminate the chamber, which was continuously flushed with dry purified air. Variable concentrations of water vapor, ozone, and sulfur dioxide could be added to the chamber. UV-lamps initiated photochemistry producing sulfuric acid. Ionization could be enhanced with two Cs-137 gamma sources (30 MBq), mounted on each side of the chamber. Figure 1 shows the evolution of the aerosols, following a nucleation event induced by the gamma sources. Previous to the event the aerosols were in steady state. Each curve represents a size bin: 3-10 nm (dark purple), 10-20 nm (purple), 20-30 nm (blue), 30-40 nm (light blue), 40-50 nm (green), 50-60 nm (yellow), and 60-68 nm (red). Black curves show a ~1 hour smoothing. The initial

  16. The Dependence of Cloud Particle Size on Non-Aerosol-Loading Related Variables

    SciTech Connect

    Shao, H.; Liu, G.

    2005-03-18

    An enhanced concentration of aerosol may increase the number of cloud drops by providing more cloud condensation nuclei (CCN), which in turn results in a higher cloud albedo at a constant cloud liquid water path. This process is often referred to as the aerosol indirect effect (AIE). Many in situ and remote sensing observations support this hypothesis (Ramanathan et al. 2001). However, satellite observed relations between aerosol concentration and cloud drop size are not always in agreement with the AIE. Based on global analysis of cloud effective radius (r{sub e}) and aerosol number concentration (N{sub a}) derived from satellite data, Sekiguchi et al. (2003) found that the correlations between the two variables can be either negative, or positive, or none, depending on the location of the clouds. They discovered that significantly negative r{sub e} - N{sub a} correlation can only be identified along coastal regions of the continents where abundant continental aerosols inflow from land, whereas Feingold et al. (2001) found that the response of r{sub e} to aerosol loading is the greatest in the region where aerosol optical depth ({tau}{sub a}) is the smallest. The reason for the discrepancy is likely due to the variations in cloud macroscopic properties such as geometrical thickness (Brenguier et al. 2003). Since r{sub e} is modified not only by aerosol but also by cloud geometrical thickness (H), the correlation between re and {tau}{sub a} actually reflects both the aerosol indirect effect and dependence of H. Therefore, discussing AIE based on the r{sub e}-{tau}{sub a} correlation without taking into account variations in cloud geometrical thickness may be misleading. This paper is motivated to extract aerosols' effect from overall effects using the independent measurements of cloud geometrical thickness, {tau}{sub a} and r{sub e}.

  17. Cloud Condensation Nuclei in Cumulus Humilis — selected Case Study During the CHAPS Campaign

    SciTech Connect

    Yu, X.; Lee, Y.; Berg, L.; Berkowitz, C.; Alexander, L.; Laskin, A.; Ogren, J.; Andrews, E.

    2010-03-15

    The Cumulus Humilis Aerosol Processing Study (CHAPS) provided a unique opportunity to study aerosol and cloud processing. Clouds play an active role in the processing and cycling of atmospheric constituents. Gases and particles can partition to cloud droplets by absorption and condensation as well as activation and impact scavenging. The U.S. Department of Energy (DOE) G-1 aircraft was used as one of the main platforms in CHAPS. Flight tracks were designed and implemented to characterize freshly emitted aerosols at cloud top and cloud base as well as within the cloud, i.e., cumulus humilis (or fair-weather cumulus), in the vicinity of Oklahoma City. Measurements of interstitial aerosols and residuals of activated condensation cloud nuclei were conducted simultaneously. The interstitial aerosols were measured downstream of an isokinetic inlet, and the activated particles downstream of a counter-flow virtual impactor (CVI). The sampling line to the Aerodyne Aerosol Mass Spectrometer (AMS) was switched between the isokinetic inlet and the CVI to allow characterization of non-activated interstitial particles outside of clouds in contrast to particles activated in clouds. Trace gases including ozone, carbon monoxide, sulfur dioxide, and a series of volatile organic compounds (VOCs) were also measured, as were key meteorological state parameters including liquid water content, cloud drop size, and dew point. We will report on the CCN properties in cumulus humilis. Several approaches will be taken. The first is single-particle analysis of particles collected by the Time-Resolved Aerosol Sampler (TRAC) by scanning electron microscopy (SEM) and transmission electron microscopy (TEM) coupled with energy disperse X-ray spectroscopy (EDX). Specifically, we examine differences between activated and interstitial ones, such as differences in chemical composition and morphology. The second analysis will link in situ measurements by AMS and PTRMS with the observations by TRAC. For

  18. Marine Aerosols: Hygroscopocity and Aerosol-Cloud Relationships

    DTIC Science & Technology

    2012-09-30

    MSc) clouds. A CIRPAS Twin Otter field experiment took place in July-August 2011 over the eastern Pacific Ocean off the coast of Monterey, CA...large eddy simulation (LES) and field measurements, the latter including Twin Otter missions such as MASE I and MASE II and those involving other...properties in ship tracks, which have continued to serve as a well-defined example of marine aerosol-cloud perturbations. The Twin Otter payload has

  19. Smoke and Pollution Aerosol Effect on Cloud Cover

    NASA Technical Reports Server (NTRS)

    Kaufman, Yoram J.; Koren, Ilan

    2006-01-01

    Pollution and smoke aerosols can increase or decrease the cloud cover. This duality in the effects of aerosols forms one of the largest uncertainties in climate research. Using solar measurements from Aerosol Robotic Network sites around the globe, we show an increase in cloud cover with an increase in the aerosol column concentration and an inverse dependence on the aerosol absorption of sunlight. The emerging rule appears to be independent of geographical location or aerosol type, thus increasing our confidence in the understanding of these aerosol effects on the clouds and climate. Preliminary estimates suggest an increase of 5% in cloud cover.

  20. Effect of aerosol number concentration on cloud droplet dispersion: An LES study and implications for aerosol indirect forcing

    NASA Astrophysics Data System (ADS)

    Lu, M.; Seinfeld, J. H.

    2005-12-01

    Through three-dimensional LES simulations of marine stratocumulus we explore the factors that control the cloud spectral relative dispersion (ratio of cloud droplet spectral width to the mean radius of the distribution) as a function of aerosol number concentration and the extent to which the relative dispersion either enhances or mitigates the Twomey effect. We find that relative dispersion decreases with increasing aerosol number concentration (for aerosol number concentrations less than about 1000 cm- 3) because smaller droplets resulting from higher aerosol number concentrations inhibit precipitation and lead to: (1) less spectral broadening by suppressed collision and coalescence processes; and (2) more spectral narrowing by droplet condensational growth at higher updraft velocity, because reduced drizzle latent heating at cloud top results in increased boundary layer turbulent kinetic energy production by buoyancy and thereby stronger turbulence. Increased spectral broadening owing to increased cloud-top entrainment mixing, also as a result of increased boundary layer turbulence, is relatively insignificant compared with (1) and (2). The coefficient k, an important parameter that relates cloud droplet effective radius and volume mean radius in large-scale models, is a function of skewness and relative dispersion of the distribution and is negatively correlated with relative dispersion. Increasing k with increasing aerosol number concentration leads to maximum enhancement of the cloud susceptibility (the change of cloud optical depth due to change of cloud droplet number concentration) over that attributable to the Twomey effect alone by about 4.2% and 39% for simulated FIRE and ASTEX cases, respectively.

  1. Global synthesis of long-term cloud condensation nuclei observations

    NASA Astrophysics Data System (ADS)

    Schmale, Julia; Henning, Silvia; Stratmann, Frank; Henzing, Bas; Schlag, Patrick; Aalto, Pasi; Keskinen, Helmi; Sellegri, Karine; Ovadnevaite, Jurgita; Krüger, Mira; Jefferson, Anne; Whitehead, James; Carslaw, Ken; Yum, Seong Soo; Kristensson, Adam; Baltensperger, Urs; Gysel, Martin

    2016-04-01

    Cloud condensation nuclei (CCN) are aerosol particles with the ability to activate into droplets at a given super saturation and therefore influence the microphysical and optical properties of clouds. To predict cloud radiative properties understanding the spatial and temporal variability of CCN concentrations in different environments is important. However, currently, the effects of atmospheric particles on changes in cloud radiative forcing are still the largest contribution of uncertainty in climate forcing prediction (IPCC, 2013). Numerous intensive field campaigns have already explored detailed characteristics of CCN in many locations around the world. However, these rather short-term observations can generally not address seasonal or inter-annual variations and a comparison between campaign sites is difficult due to the higher influence of specific environmental circumstances on short-term measurements results. Here, we present results of more long-term CCN and aerosol number concentrations as well as size distribution data covering at least one full year between 2006 and 2014. The 12 locations include ACTRIS stations (http://www.actris.net/) in Europe, and further sites in North America, Brazil and Korea. The sites are located in different environments allowing for temporal and spatial characterization of CCN variability in different atmospheric regimes. Those include marine, remote-continental, boreal forest, rain forest, Arctic and monsoon-influenced environments, as well as boundary layer and free tropospheric conditions. The aerosol populations and their activation behavior show significant differences across the stations. While peak concentrations of CCN are observed in summer at the high altitude sites, in the Arctic the highest concentrations occur during the Haze period in spring. The rural-marine and rural-continental sites exhibit similar CCN concentration characteristics with a relatively flat annual cycle. At some stations, e.g. in the boreal

  2. Cloud Condensation Nuclei in Fire-3

    NASA Technical Reports Server (NTRS)

    2000-01-01

    The centerpiece of this research was the cloud condensation nuclei (CCN) measurements of the Desert Research Institute (DRI) CCN spectrometers on board the NCAR C-130 aircraft during the Arctic Cloud Experiment (ACE) in May, 1998. These instruments operated successfully throughout all eight 10-hour research flights based in Fairbanks and the two ferry flights between Colorado and Fairbanks. Within a few months of completion of ACE the CCN data was edited and put into the archives. A paper was completed and published on the CCN climatology during the previous two FIRE field projects-FIRE 1 based in San Diego in June and July, 1987 and ASTEX based in the Azores Islands in June, 1992. This showed distinct contrasts in concentrations and spectra between continental and maritime CCN concentrations, which depended on air mass trajectories. Pollution episodes from Europe had distinct influences on particle concentrations at low altitudes especially within the boundary layer. At higher altitudes concentrations were similar in the two air mass regimes. Cloudier atmospheres showed lower concentrations especially below the clouds, which were a result mostly of coalescence scavenging.

  3. The Impact of Aerosols on Cloud and Precipitation Processes: Cloud-Resolving Model Simulations

    NASA Technical Reports Server (NTRS)

    Tao, Wei-Kuo; Li, X.; Khain, A.; Simpson, S.; Johnson, D.; Remer, L.

    2004-01-01

    Cloud microphysics is inevitably affected by the smoke particle (CCN, cloud condensation nuclei) size distributions below the clouds. Therefore, size distributions parameterized as spectral bin microphysics are needed to explicitly study the effects of atmospheric aerosol concentration on cloud development, rainfall production, and rainfall rates for convective clouds. Recently, two detailed spectral-bin microphysical schemes were implemented into the Goddard Cumulus Ensembel (GCE) model. The formulation for the explicit spectral-bin microphysical processes is based on solving stochastic kinetic equations for the size distribution functions of water droplets (i.e., cloud droplets and raindrops), and several types of ice particles [i.e. pristine ice crystals (columnar and plate-like), snow (dendrites and aggregates), graupel and frozen drops/hail]. Each type is described by a special size distribution function containing many categories (i.e. 33 bins). Atmospheric aerosols are also described using number density size distribution functions. A spectral-bin microphysical model is very expensive from a computational point of view and has only been implemented into the 2D version of the GCE at the present time. The model is tested by studying the evolution of deep tropical clouds in the west Pacific warm pool region and in the mid-latitude continent with different concentrations of CCN: a low "c1ean"concentration and a high "dirty" concentration. In addition, differences and similarities between bulk microphysics and spectral-bin microphysical schemes will be examined and discussed.

  4. The Impact of Aerosols on Cloud and Precipitation Processes: Cloud-resolving Model Simulations

    NASA Technical Reports Server (NTRS)

    Tao, Wei-Kuo; Li, X.; Khain, A.; Simpson, S.; Johnson, D.; Remer, L.

    2004-01-01

    Cloud microphysics is inevitably affected by the smoke particle (CCN, cloud condensation nuclei) size distributions below the clouds. Therefore, size distributions parameterized as spectral bin microphysics are needed to explicitly study the effects of atmospheric aerosol concentration on cloud development, r d a U production, and rainfall rates for convective clouds. Recently, two detailed spectral-bin microphysical schemes were implemented into the Goddard Cumulus Ensembe1 (GCE) model. The formulation for the explicit spectral-bin microphysical processes is based on solving stochastic kinetic equations for the size distribution functions of water droplets (i.e., cloud droplets and raindrops), and several types of ice particles [i.e. pristine ice crystals (columnar and platelike), snow (dendrites and aggregates), graupel and frozen drops/hail]. Each type is described by a special size distribution function containing many categories (i.e. 33 bins). Atmospheric aerosols are also described using number density size-distribution functions. A spectral-bin microphysical model is very expensive from a computational point of view and has only been implemented into the 2D version of the GCE at the present time. The model is tested by studying the evolution of deep tropical clouds in the west Pacific warm pool region and in the mid-latitude continent with different concentrations of CCN: a low "c1ean"concentration and a high "dirty" concentration. In addition, differences and similarities between bulk microphysics and spectral-bin microphysical schemes will be examined and discussed.

  5. The Impact of Aerosols on Cloud and Precipitation Processes: Cloud-Resolving Model Simulations

    NASA Technical Reports Server (NTRS)

    Tao, Wei-Kuo; Li, X.; Khain, A.; Simpson, S.

    2004-01-01

    Cloud microphysics are inevitably affected by the smoke particle (CCN, cloud condensation nuclei) size distributions below the clouds. Therefore, size distributions parameterized as spectral bin microphysics are needed to explicitly study the effects of atmospheric aerosol concentration on cloud development, rainfall production, and rainfall rates for convective clouds. Recently, two detailed spectral-bin microphysical schemes were implemented into the Goddard Cumulus Ensemble (GCE) model. The formulation for the explicit spectral-bin microphysical processes is based on solving stochastic kinetic equations for the size distribution functions of water droplets (i.e., cloud droplets and raindrops), and several types of ice particles (i.e., pristine ice crystals (columnar and plate-like), snow (dendrites and aggregates), graupel and frozen drops/hail). Each type is described by a special size distribution function containing many categories (i.e. 33 bins). Atmospheric aerosols are also described using number density size-distribution functions. A spectral-bin microphysical model is very expensive from a computational point of view and has only been implemented into the 2D version of the GCE at the present time. The model is tested by studying the evolution of deep cloud systems in the west Pacific warm pool region, in the sub-tropics (Florida) and in the mid-latitude using identical thermodynamic conditions but with different concentrations of CCN: a low 'clean' concentration and a high 'dirty' concentration.

  6. Development of a thermal gradient cloud condensation nucleus spectrometer

    NASA Technical Reports Server (NTRS)

    Leu, Ming-Taun; Friedl, R.

    2004-01-01

    Droplet clouds are one of the most important factors controlling the albedo and hence the temperature of out planet. Anthropogenic aerosols, such as black carbon (BC) organic carbon (OC) and sulfate, have a strong influence on cloud albedo. IPCC (2001) has estimated the global mean forcing from aerosols to be potentially as large as that of green house gases but opposite in sign. However, the uncertainties associated with the indirect aerosol forcing preclude a quantitative estimate. An additional impact on the indirect aerosol forcing, not quantified by IPCC, arises from recently identified chemical factors, for examples, interactions of atmospheric soluble gases, slightly soluble solutes, and organic substance with aerosols, which may influence the formation of cloud droplets. Recent studies suggest that inclusion of chemical effects on aerosol droplets. We plan to conduct several critical laboratory experiments that will reduce the uncertainty associated with indirect radiative forcing due to chemical modification of sulfate and BC aerosols by ambient gases.

  7. Clouds and aerosols in Puerto Rico - a new evaluation

    NASA Astrophysics Data System (ADS)

    Allan, J. D.; Baumgardner, D.; Raga, G. B.; Mayol-Bracero, O. L.; Morales-García, F.; García-García, F.; Montero-Martínez, G.; Borrmann, S.; Schneider, J.; Mertes, S.; Walter, S.; Gysel, M.; Dusek, U.; Frank, G. P.; Krämer, M.

    2008-03-01

    The influence of aerosols, both natural and anthropogenic, remains a major area of uncertainty when predicting the properties and behaviour of clouds and their influence on climate. In an attempt to better understand warm cloud formation in a tropical marine environment, a period of intensive measurements took place in December 2004 in Puerto Rico, using some of the latest developments in online instrumentation such as aerosol mass spectrometers, cloud condensation nuclei counters and a hygroscopicity tandem differential mobility analyser. Simultaneous online measurements of aerosol size distributions, composition, hygroscopicity and optical properties were made near the lighthouse of Cape San Juan in the north-eastern corner of the island and at the top of East Peak mountain (1040 m a.s.l.), the two sites separated by 17 km. Additional measurements of the cloud droplet residual and interstitial aerosol properties were made at the mountain site, accompanied by measurements of cloud droplet size distributions, liquid water content and the chemical composition of cloud and rain water samples. Both aerosol composition and cloud properties were found to be sensitive to wind sector. Air from the east-northeast (ENE) was mostly free of anthropogenic influences, the submicron fraction being mainly composed of non-sea salt sulphate, while that from the east-southeast (ESE) was found to be moderately influenced by populated islands upwind, adding smaller (<100 nm), externally mixed, carbonaceous particles to the aerosol that increased the number concentrations by over a factor of 3. This change in composition was also accompanied with a reduction in the measured hygroscopicity and fractional cloud activation potential of the aerosol. At the mountain site, the average cloud droplet concentrations increased from 193 to 519 cm-3, median volume diameter decreased from 20 to 14 μm and the liquid water content increased from 0.24 to 0.31 g m-3 when the winds shifted from the ENE

  8. Impact of Asian aerosols on air quality over the United States: A perspective from aerosol-cloud-radiation coupling

    NASA Astrophysics Data System (ADS)

    Tao, Z.; Yu, H.; Chin, M.

    2013-12-01

    It has well been established, through satellite/ground observations, that dust and aerosols from various Asian sources can travel across the Pacific and reach North America (NA) at least on episode bases. Once reaching NA, these inflow aerosols would compete with local emissions to influence atmospheric composition and air quality over the United States (US). The previous studies, typically based on one or multiple satellite measurements in combination with global/regional model simulations, suggest that the impact of Asian dust/aerosols on US air quality tend to be small since most inflow aerosols stay aloft. On the other hand, aerosols affect many key meteorological processes that will ultimately channel down to impact air quality. Aerosols absorb and scatter solar radiation that change the atmospheric stability, thus temperature, wind, and planetary boundary layer structure that would directly alter air quality. Aerosols can serve as cloud condensation nuclei and ice nuclei to modify cloud properties and precipitation that would also affect aerosol removal and concentration. This indirect impact of Asian aerosol inflow on US air quality may be substantial and need to be investigated. This study employs the NASA Unified WRF (NU-WRF) to address the question from the aerosol-radiation-cloud interaction perspective. The simulation period was selected from April to June of 2010 during which the Asian dust continuously reached NA based on CALIPSO satellite observation. The preliminary results show that the directly-transported Asian aerosol increases surface PM2.5 concentration by less than 2 μg/m3 over the west coast areas of US, and the aerosol-radiation-cloud feedback has a profound effect on air quality over the central to eastern US. A more detailed analysis links this finding to a series of meteorological conditions modified by aerosol effects.

  9. Microphysical processing of aerosol particles in orographic clouds

    NASA Astrophysics Data System (ADS)

    Pousse-Nottelmann, S.; Zubler, E. M.; Lohmann, U.

    2015-01-01

    An explicit and detailed treatment of cloud-borne particles allowing for the consideration of aerosol cycling in clouds has been implemented in the regional weather forecast and climate model COSMO. The effects of aerosol scavenging, cloud microphysical processing and regeneration upon cloud evaporation on the aerosol population and on subsequent cloud formation are investigated. For this, two-dimensional idealized simulations of moist flow over two bell-shaped mountains were carried out varying the treatment of aerosol scavenging and regeneration processes for a warm-phase and a mixed-phase orographic cloud. The results allowed to identify different aerosol cycling mechanisms. In the simulated non-precipitating warm-phase cloud, aerosol mass is incorporated into cloud droplets by activation scavenging and released back to the atmosphere upon cloud droplet evaporation. In the mixed-phase cloud, a first cycle comprises cloud droplet activation and evaporation via the Wegener-Bergeron-Findeisen process. A second cycle includes below-cloud scavenging by precipitating snow particles and snow sublimation and is connected to the first cycle via the riming process which transfers aerosol mass from cloud droplets to snow flakes. In the simulated mixed-phase cloud, only a negligible part of the total aerosol mass is incorporated into ice crystals. Sedimenting snow flakes reaching the surface remove aerosol mass from the atmosphere. The results show that aerosol processing and regeneration lead to a vertical redistribution of aerosol mass and number. However, the processes not only impact the total aerosol number and mass, but also the shape of the aerosol size distributions by enhancing the internally mixed/soluble accumulation mode and generating coarse mode particles. Concerning subsequent cloud formation at the second mountain, accounting for aerosol processing and regeneration increases the cloud droplet number concentration with possible implications for the ice

  10. Microphysical processing of aerosol particles in orographic clouds

    NASA Astrophysics Data System (ADS)

    Pousse-Nottelmann, S.; Zubler, E. M.; Lohmann, U.

    2015-08-01

    An explicit and detailed treatment of cloud-borne particles allowing for the consideration of aerosol cycling in clouds has been implemented into COSMO-Model, the regional weather forecast and climate model of the Consortium for Small-scale Modeling (COSMO). The effects of aerosol scavenging, cloud microphysical processing and regeneration upon cloud evaporation on the aerosol population and on subsequent cloud formation are investigated. For this, two-dimensional idealized simulations of moist flow over two bell-shaped mountains were carried out varying the treatment of aerosol scavenging and regeneration processes for a warm-phase and a mixed-phase orographic cloud. The results allowed us to identify different aerosol cycling mechanisms. In the simulated non-precipitating warm-phase cloud, aerosol mass is incorporated into cloud droplets by activation scavenging and released back to the atmosphere upon cloud droplet evaporation. In the mixed-phase cloud, a first cycle comprises cloud droplet activation and evaporation via the Wegener-Bergeron-Findeisen (WBF) process. A second cycle includes below-cloud scavenging by precipitating snow particles and snow sublimation and is connected to the first cycle via the riming process which transfers aerosol mass from cloud droplets to snowflakes. In the simulated mixed-phase cloud, only a negligible part of the total aerosol mass is incorporated into ice crystals. Sedimenting snowflakes reaching the surface remove aerosol mass from the atmosphere. The results show that aerosol processing and regeneration lead to a vertical redistribution of aerosol mass and number. Thereby, the processes impact the total aerosol number and mass and additionally alter the shape of the aerosol size distributions by enhancing the internally mixed/soluble Aitken and accumulation mode and generating coarse-mode particles. Concerning subsequent cloud formation at the second mountain, accounting for aerosol processing and regeneration increases

  11. Constraining cloud lifetime effects of aerosols using A-Train satellite observations

    NASA Astrophysics Data System (ADS)

    Wang, Minghuai; Ghan, Steven; Liu, Xiaohong; L'Ecuyer, Tristan S.; Zhang, Kai; Morrison, Hugh; Ovchinnikov, Mikhail; Easter, Richard; Marchand, Roger; Chand, Duli; Qian, Yun; Penner, Joyce E.

    2012-08-01

    Aerosol indirect effects have remained the largest uncertainty in estimates of the radiative forcing of past and future climate change. Observational constraints on cloud lifetime effects are particularly challenging since it is difficult to separate aerosol effects from meteorological influences. Here we use three global climate models, including a multi-scale aerosol-climate model PNNL-MMF, to show that the dependence of the probability of precipitation on aerosol loading, termed the precipitation frequency susceptibility (Spop), is a good measure of the liquid water path response to aerosol perturbation (λ), as both Spop and λ strongly depend on the magnitude of autoconversion, a model representation of precipitation formation via collisions among cloud droplets. This provides a method to use satellite observations to constrain cloud lifetime effects in global climate models. Spop in marine clouds estimated from CloudSat, MODIS and AMSR-E observations is substantially lower than that from global climate models and suggests a liquid water path increase of less than 5% from doubled cloud condensation nuclei concentrations. This implies a substantially smaller impact on shortwave cloud radiative forcing over ocean due to aerosol indirect effects than simulated by current global climate models (a reduction by one-third for one of the conventional aerosol-climate models). Further work is needed to quantify the uncertainties in satellite-derived estimates of Spop and to examine Spop in high-resolution models.

  12. Cloud Condensation Nuclei Measurements in Tropical Cyclones

    NASA Astrophysics Data System (ADS)

    Hudson, J. G.; Simpson, J.

    2002-05-01

    The first measurements of cloud condensation nuclei (CCN) within and around tropical cyclones were made with the Desert Research Institute (DRI) CCN spectrometer (Hudson 1989) from a NOAA P-3 Hurricane Hunter aircraft throughout the 2001 season. Two penetrations of the closed eye of Hurricane Erin off the northeast US coast on Sept. 10 showed concentrations consistently well in excess of 1000 per cubic cm at approximately 1.4% supersaturation. Simultaneous condensation nuclei (CN--total particle) concentrations were consistently well in excess of 2000 per cubic cm throughout these closed eye penetrations. These within eye measurements at 4 km altitude far exceeded CCN and CN measurements just outside of the storm at similar altitudes--300 and 600 per cubic cm respectively. These CCN and CN concentrations within this closed eye were far above concentrations in maritime air masses; they are characteristic of continental or polluted air masses. Although there was a possibility that Saharan dust may have gotten into this storm these sub tenth micrometer particles are much too small and much too numerous to be dust. Such high concentrations may have originated from European air pollution, which may have been transported by similar airflow patterns to those that carry Saharan dust across the Atlantic. These high concentrations may be a manifestation of descending air that brings higher concentrations that are often characteristic of the upper troposphere (Clarke and Kapustin 2002). Later in the month measurements in Humberto showed highly variable CCN and CN concentrations that ranged from less than 5 per cubic cm to more than 1000 per cubic cm over km scale distances within and around the open eye of this tropical storm/hurricane. These very low concentrations suggest strong cloud scavenging. Clarke, A.D. and V.N. Kapustin, J. Atmos. Sci., 59, 363-382, 2002. Hudson, J.G., J. Atmos. & Ocean. Tech., 6, 1055-1065, 1989.

  13. Cloud Condensation Nuclei Measurements in Tropical Cyclones

    NASA Technical Reports Server (NTRS)

    Hudson, J. G.; Simpson, J.

    2002-01-01

    The first measurements of cloud condensation nuclei (CCN) within and around tropical cyclones were made with the Desert Research Institute (DRI) CCN spectrometer (Hudson 1909) from a NOAA P-3 Hurricane Hunter aircraft throughout the 2001 season. Two penetrations of the closed eye of Hurricane Erin off the northeast US coast on Sept. 10 showed concentrations consistently well in excess of 1000 per cubic cm at approximately 1.4% supersaturation. Simultaneous condensation nuclei (CN--total particle) concentrations were consistently well in excess of 2000 per cubic cm throughout these closed eye penetrations. These within eye measurements at 4 km altitude for exceeded CCN and CN measurements just outside of the storm at similar altitudes--300 and 600 per cubic cm respectively. These CCN and CN concentrations within this closed eye were far above concentrations in maritime air masses; they are characteristic of continental or polluted air masses. Although there was a possibility that Saharan duct may have gotten into this storm these sub tenth micrometer particles are much too small and much too numerous to be dust. Such high concentrations may have originated from European air pollution, which may have been transported by similar airflow patterns to those that carry Saharan dust across the Atlantic. These high concentrations may be a manifestation of descending air that brings higher concentrations that are often characteristic of the upper troposphere (Clarke and Kapustin 2002). Later in the month measurements in Humberto showed highly variable CCN and CN concentrations that ranged from lots than 5 per cubic cm to more than 1000 per Cubic cm over km scale distances within and around the open eye of this tropical storm/hurricane. These very low concentrations suggest strong cloud scavenging.

  14. Parameterization of bulk condensation in numerical cloud models

    NASA Technical Reports Server (NTRS)

    Kogan, Yefim L.; Martin, William J.

    1994-01-01

    The accuracy of the moist saturation adjustment scheme has been evaluated using a three-dimensional explicit microphysical cloud model. It was found that the error in saturation adjustment depends strongly on the Cloud Condensation Nucleii (CCN) concentration in the ambient atmosphere. The scheme provides rather accurate results in the case where a sufficiently large number of CCN (on the order of several hundred per cubic centimeter) is available. However, under conditions typical of marine stratocumulus cloud layers with low CCN concentration, the error in the amounts of condensed water vapor and released latent heat may be as large as 40%-50%. A revision of the saturation adjustment scheme is devised that employs the CCN concentration, dynamical supersaturation, and cloud water content as additional variables in the calculation of the condensation rate. The revised condensation model reduced the error in maximum updraft and cloud water content in the climatically significant case of marine stratocumulus cloud layers by an order of magnitude.

  15. Contrasting the Evaporation and Condensation of Water from Glassy and Amorphous Aerosol Particles

    NASA Astrophysics Data System (ADS)

    Reid, J. P.; Bones, D. L.; Power, R.; Lienhard, D.; Krieger, U. K.

    2012-04-01

    The partitioning of water between the condensed and gas phases in atmospheric aerosol is usually assumed to occur instantaneously and to be regulated by solution thermodynamics. However, the persistence of high viscosity, glassy and amorphous aerosol to low relative humidity without crystallisation occurring is now widely recognised, suggesting that the timescale for water transport to or from the particle during condensation or evaporation may be significant. A kinetic limitation on water transport could have important implications for understanding hygroscopic growth measurements made on ambient particles, the ability of particles to act as ice nuclei or cloud condensation nuclei, the kinetics of chemical aging/heterogeneous chemistry, and the rate or condensation/evaporation of semi-volatile organic components. In this study we will report on measurements of the timescale of water transport to and from glassy aerosol and ultra-high viscosity solution droplets using aerosol optical tweezers to investigate the time-response of single particles to changes in relative humidity. As a benchmark system, mixed component aerosol particles containing sucrose and sodium chloride have been used; varying the mole fractions of the two solutes allows a wide range of solution viscosities to be studied. We will show that coarse particles can take many thousands of seconds to equilibrate in size and that the timescale correlates with the estimated bulk viscosity of the particle. We will also confirm that significant inhomogeneities in particle composition can be established during evaporation or condensation. Using the experimental data to benchmark a model for equilibration time, predictions can be made of the timescale for the equilibration of accumulation mode particles during water condensation or evaporation and these predictions will be described and their significance explored. Finally, the coalescence dynamics of highly viscous aerosol particles will be reported

  16. Sources and evolution of cloud-active aerosol in California's Sierra Nevada Mountains

    NASA Astrophysics Data System (ADS)

    Roberts, G. C.; Corrigan, C.; Noblitt, S.; Creamean, J.; Collins, D. B.; Cahill, J. F.; Prather, K. A.; Collett, J. L.; Henry, C.

    2011-12-01

    To assess the sources of cloud-active aerosol and their influence on the hydrological cycle in California, the CalWater Experiment took place in winter 2011 in the foothills of the Sierra Nevada Mountains. During this experiment, we coupled the capabilities of demonstrated miniaturized instrumentation - cloud condensation nuclei (CCN), water condensation nuclei (WCN) and microchip capillary electrophoresis (MCE) - to provide direct chemical measurements of cloud active aerosols. Ion concentrations of CCN droplets attribute the anthropogenic, marine and secondary organic contributions to cloud-active aerosols. Detailed spectra from an Aerosol-Time-of-Flight Mass Spectrometer provide additional information on the sources of aerosol. Storm fronts and changes in atmospheric boundary layer brought aerosol and anions associated with Central Valley pollution to the field site with CCN concentrations reaching several thousand cm-3. Hygroscopicity parameters indicate aging of the organic fraction during aerosol transport from the Central Valley to the mountains. Otherwise, CCN concentrations were low when high pressure systems prevented boundary layer development and intrusion of the Central Valley pollution to the site. MCE results show that nitrates and sulfates comprise most of the fraction of the aerosol anion mass (PM1). During the passage of storm fronts, which transported pollution from the Central Valley upslope, nitrate concentrations peaked at several μ g m-3. Low supersaturation CCN concentrations coincide with increases in aerosol nitrate, which suggests that nitrate has a role in cloud formation of giant CCN and, furthermore, in precipitation processes in the Sierra Nevada. CCN spectra show large variations depending on the aerosol sources and sometimes exhibit bi-modal distributions with minima at 0.3% Sc -- similar to the so-called 'Hoppel minima' associated to number size distributions. During these bi-modal events, sulfate also increases supporting the

  17. Vertical microphysical profiles of convective clouds as a tool for obtaining aerosol cloud-mediated climate forcings

    SciTech Connect

    Rosenfeld, Daniel

    2015-12-23

    Quantifying the aerosol/cloud-mediated radiative effect at a global scale requires simultaneous satellite retrievals of cloud condensation nuclei (CCN) concentrations and cloud base updraft velocities (Wb). Hitherto, the inability to do so has been a major cause of high uncertainty regarding anthropogenic aerosol/cloud-mediated radiative forcing. This can be addressed by the emerging capability of estimating CCN and Wb of boundary layer convective clouds from an operational polar orbiting weather satellite. Our methodology uses such clouds as an effective analog for CCN chambers. The cloud base supersaturation (S) is determined by Wb and the satellite-retrieved cloud base drop concentrations (Ndb), which is the same as CCN(S). Developing and validating this methodology was possible thanks to the ASR/ARM measurements of CCN and vertical updraft profiles. Validation against ground-based CCN instruments at the ARM sites in Oklahoma, Manaus, and onboard a ship in the northeast Pacific showed a retrieval accuracy of ±25% to ±30% for individual satellite overpasses. The methodology is presently limited to boundary layer not raining convective clouds of at least 1 km depth that are not obscured by upper layer clouds, including semitransparent cirrus. The limitation for small solar backscattering angles of <25º restricts the satellite coverage to ~25% of the world area in a single day. This methodology will likely allow overcoming the challenge of quantifying the aerosol indirect effect and facilitate a substantial reduction of the uncertainty in anthropogenic climate forcing.

  18. On COBACC (COntinental Biosphere-Aerosol-Cloud-Climate) feedback

    NASA Astrophysics Data System (ADS)

    Kulmala, Markku

    2016-04-01

    Anthropogenic emissions of GHGs have increased substantially during the past century. Elevated concentrations of CO2 and methane are the most important forcing agents causing global warming. However, it is not straightforward to attribute or predict the climate change in detail, as the internal variability of climate is only partially understood, aerosol forcings are still highly uncertain, and there are many feedback mechanisms that are difficult to quantify. It has been recognized for decades that the biosphere plays an important role in climate. For example, Kulmala et al. (2004) suggested a negative climate feedback mechanism whereby higher temperatures and CO2-levels boost continental biomass production, leading to increased biogenic secondary organic aerosol (BSOA) and cloud condensation nuclei (CCN) concentrations, tending to cause cooling. This COBACC (COntinental Biosphere-Aerosol-Cloud-Climate) feedback is similar to the so-called CLAW-hypothesis by Charlson et al. (1987) which connects the ocean biochemistry and climate via a negative feedback loop involving CCN production due to sulphur emissions from plankton. The first quantification of the COBACC feedback loop (Kulmala et al. 2014) was based on continuous comprehensive observations at SMEAR II (Station for Measuring Forest Ecosystem-Atmosphere Relations) station in Hyytiälä, Finland, and showed that a 10 ppm increase in atmospheric CO2 concentration leads to a significant (several percent) increase in both carbon sink and aerosol source. These effects operate through changes in gross primary production, volatile organic compound (VOC) emissions and secondary aerosol formation associated with atmospheric oxidation of VOCs. Here we will describe the present knowledge from processes level understanding to whole COBACC feedback including some hints on biogenic and anthropogenic contributions to global aerosol number load. References: Charlson, R. J. et al. Nature 326, 655 1987 Kulmala, M. et al. Atmos

  19. Cloud residues and interstitial aerosols from non-precipitating clouds over an industrial and urban area in northern China

    NASA Astrophysics Data System (ADS)

    Li, Weijun; Li, Peiren; Sun, Guode; Zhou, Shengzhen; Yuan, Qi; Wang, Wenxing

    2011-05-01

    Most studies of aerosol-cloud interactions have been conducted in remote locations; few have investigated the characterization of cloud condensation nuclei (CCN) over highly polluted urban and industrial areas. The present work, based on samples collected at Mt. Tai, a site in northern China affected by nearby urban and industrial air pollutant emissions, illuminates CCN properties in a polluted atmosphere. High-resolution transmission electron microscopy (TEM) was used to obtain the size, composition, and mixing state of individual cloud residues and interstitial aerosols. Most of the cloud residues displayed distinct rims which were found to consist of soluble organic matter (OM). Nearly all (91.7%) cloud residues were attributed to sulfate-related salts (the remainder was mostly coarse crustal dust particles with nitrate coatings). Half the salt particles were internally mixed with two or more refractory particles (e.g., soot, fly ash, crustal dust, CaSO 4, and OM). A comparison between cloud residues and interstitial particles shows that the former contained more salts and were of larger particle size than the latter. In addition, a somewhat high number scavenging ratio of 0.54 was observed during cloud formation. Therefore, the mixtures of salts with OMs account for most of the cloud-nucleating ability of the entire aerosol population in the polluted air of northern China. We advocate that both size and composition - the two influential, controlling factors for aerosol activation - should be built into all regional climate models of China.

  20. Holistic Interactions of Shallow Clouds, Aerosols, and Land-Ecosystems (HI-SCALE) Science Plan

    SciTech Connect

    Fast, JD; Berg, LK

    2015-12-01

    Cumulus convection is an important component in the atmospheric radiation budget and hydrologic cycle over the Southern Great Plains and over many regions of the world, particularly during the summertime growing season when intense turbulence induced by surface radiation couples the land surface to clouds. Current convective cloud parameterizations contain uncertainties resulting in part from insufficient coincident data that couples cloud macrophysical and microphysical properties to inhomogeneities in boundary layer and aerosol properties. The Holistic Interactions of Shallow Clouds, Aerosols, and Land-Ecosystems (HI-SCALE) campaign is designed to provide a detailed set of measurements that are needed to obtain a more complete understanding of the life cycle of shallow clouds by coupling cloud macrophysical and microphysical properties to land surface properties, ecosystems, and aerosols. HI-SCALE consists of 2, 4-week intensive observational periods, one in the spring and the other in the late summer, to take advantage of different stages and distribution of “greenness” for various types of vegetation in the vicinity of the Atmospheric Radiation and Measurement (ARM) Climate Research Facility’s Southern Great Plains (SGP) site as well as aerosol properties that vary during the growing season. Most of the proposed instrumentation will be deployed on the ARM Aerial Facility (AAF) Gulfstream 1 (G-1) aircraft, including those that measure atmospheric turbulence, cloud water content and drop size distributions, aerosol precursor gases, aerosol chemical composition and size distributions, and cloud condensation nuclei concentrations. Routine ARM aerosol measurements made at the surface will be supplemented with aerosol microphysical properties measurements. The G-1 aircraft will complete transects over the SGP Central Facility at multiple altitudes within the boundary layer, within clouds, and above clouds.

  1. Challenges in constraining anthropogenic aerosol effects on cloud radiative forcing using present-day spatiotemporal variability.

    PubMed

    Ghan, Steven; Wang, Minghuai; Zhang, Shipeng; Ferrachat, Sylvaine; Gettelman, Andrew; Griesfeller, Jan; Kipling, Zak; Lohmann, Ulrike; Morrison, Hugh; Neubauer, David; Partridge, Daniel G; Stier, Philip; Takemura, Toshihiko; Wang, Hailong; Zhang, Kai

    2016-05-24

    A large number of processes are involved in the chain from emissions of aerosol precursor gases and primary particles to impacts on cloud radiative forcing. Those processes are manifest in a number of relationships that can be expressed as factors dlnX/dlnY driving aerosol effects on cloud radiative forcing. These factors include the relationships between cloud condensation nuclei (CCN) concentration and emissions, droplet number and CCN concentration, cloud fraction and droplet number, cloud optical depth and droplet number, and cloud radiative forcing and cloud optical depth. The relationship between cloud optical depth and droplet number can be further decomposed into the sum of two terms involving the relationship of droplet effective radius and cloud liquid water path with droplet number. These relationships can be constrained using observations of recent spatial and temporal variability of these quantities. However, we are most interested in the radiative forcing since the preindustrial era. Because few relevant measurements are available from that era, relationships from recent variability have been assumed to be applicable to the preindustrial to present-day change. Our analysis of Aerosol Comparisons between Observations and Models (AeroCom) model simulations suggests that estimates of relationships from recent variability are poor constraints on relationships from anthropogenic change for some terms, with even the sign of some relationships differing in many regions. Proxies connecting recent spatial/temporal variability to anthropogenic change, or sustained measurements in regions where emissions have changed, are needed to constrain estimates of anthropogenic aerosol impacts on cloud radiative forcing.

  2. Spatial and Temporal Patterns of Aerosol-Cloud Interactions

    NASA Astrophysics Data System (ADS)

    Fuchs, Julia; Cermak, Jan

    2014-05-01

    This study determines the spatial and temporal distribution of regions with frequent aerosol-cloud interactions (aci) and identifies their meteorological determinants based on CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations) and ECMWF (European Centre for Medium-Range Weather Forecasts) data products. Atmospheric aerosols influence the microphysical structure of clouds, while both also respond to meteorological conditions. The potential radiative adjustments to changes in a cloud system associated with aerosol-cloud interactions are grouped and termed as effective radiative forcing due to aerosol-cloud interactions (ERFaci). It is difficult to distinguish, to what extent radiative forcing and precipitation patterns of clouds are a result of cloud feedbacks to aerosols or the existing meteorological conditions. A complete understanding of aerosol-cloud-meteorology interactions is crucial as the uncertainty range of ERFaci in climate change modeling could be significantly reduced. In the present study it is suggested that presence of hydrated aerosols is an implication for aci. Knowledge of their vertical and horizontal distribution and frequency over the globe would be important for understanding ERFaci. To identify regions with aerosol-cloud transitions the CAD score (cloud-aerosol discrimination) of the CALIOP (Cloud-Aerosol LIdar with Orthogonal Polarization) instrument on the CALIPSO satellite is used. It separates aerosols and clouds according to the probability distribution functions of 5 parameters (attenuated backscatter, total color ratio, volume depolarization ratio, altitude and latitude) and assigns the likelihood of cloud or aerosol presence. This parameter is used to calculate relative frequencies of aci on a global scale from 2006 to 2013.

  3. Dark Targets, Aerosols, Clouds and Toys

    NASA Astrophysics Data System (ADS)

    Remer, L. A.

    2015-12-01

    Today if you use the Thomson-Reuters Science Citations Index to search for "aerosol*", across all scientific disciplines and years, with no constraints, and you sort by number of citations, you will find a 2005 paper published in the Journal of the Atmospheric Sciences in the top 20. This is the "The MODIS Aerosol Algorithm, Products and Validation". Although I am the first author, there are in total 12 co-authors who each made a significant intellectual contribution to the paper or to the algorithm, products and validation described. This paper, that algorithm, those people lie at the heart of a lineage of scientists whose collaborations and linked individual pursuits have made a significant contribution to our understanding of radiative transfer and climate, of aerosol properties and the global aerosol system, of cloud physics and aerosol-cloud interaction, and how to measure these parameters and maximize the science that can be obtained from those measurements. The 'lineage' had its origins across the globe, from Soviet Russia to France, from the U.S. to Israel, from the Himalayas, the Sahel, the metropolises of Sao Paulo, Taipei, and the cities of east and south Asia. It came together in the 1990s and 2000s at the NASA Goddard Space Flight Center, using cultural diversity as a strength to form a common culture of scientific creativity that continues to this day. The original algorithm has spawned daughter algorithms that are being applied to new satellite and airborne sensors. The original MODIS products have been fundamental to analyses as diverse as air quality monitoring and aerosol-cloud forcing. AERONET, designed originally for the need of validation, is now its own thriving institution, and the lineage continues to push forward to provide new technology for the coming generations.

  4. A Study of Cloud Processing of Organic Aerosols Using Models and CHAPS Data

    SciTech Connect

    Ervens, Barbara

    2012-01-17

    The main theme of our work has been the identification of parameters that mostly affect the formation and modification of aerosol particles and their interaction with water vapor. Our detailed process model studies led to simplifications/parameterizations of these effects that bridge detailed aerosol information from laboratory and field studies and the need for computationally efficient expressions in complex atmospheric models. One focus of our studies has been organic aerosol mass that is formed in the atmosphere by physical and/or chemical processes (secondary organic aerosol, SOA) and represents a large fraction of atmospheric particulate matter. Most current models only describe SOA formation by condensation of low volatility (or semivolatile) gas phase products and neglect processes in the aqueous phase of particles or cloud droplets that differently affect aerosol size and vertical distribution and chemical composition (hygroscopicity). We developed and applied models of aqueous phase SOA formation in cloud droplets and aerosol particles (aqSOA). Placing our model results into the context of laboratory, model and field studies suggests a potentially significant contribution of aqSOA to the global organic mass loading. The second focus of our work has been the analysis of ambient data of particles that might act as cloud condensation nuclei (CCN) at different locations and emission scenarios. Our model studies showed that the description of particle chemical composition and mixing state can often be greatly simplified, in particular in aged aerosol. While over the past years many CCN studies have been successful performed by using such simplified composition/mixing state assumptions, much more uncertainty exists in aerosol-cloud interactions in cold clouds (ice or mixed-phase). Therefore we extended our parcel model that describes warm cloud formation by ice microphysics and explored microphysical parameters that determine the phase state and lifetime of

  5. Aerosol/Cloud Measurements Using Coherent Wind Doppler Lidars

    NASA Astrophysics Data System (ADS)

    Royer, Philippe; Boquet, Matthieu; Cariou, Jean-Pierre; Sauvage, Laurent; Parmentier, Rémy

    2016-06-01

    The accurate localization and characterization of aerosol and cloud layers is crucial for climate studies (aerosol indirect effect), meteorology (Planetary Boundary Layer PBL height), site monitoring (industrial emissions, mining,…) and natural hazards (thunderstorms, volcanic eruptions). LEOSPHERE has recently developed aerosol/cloud detection and characterization on WINDCUBE long range Coherent Wind Doppler Lidars (CWDL). These new features combine wind and backscatter intensity informations (Carrier-to-Noise Ratio CNR) in order to detect (aerosol/cloud base and top, PBL height) and to characterize atmospheric structures (attenuated backscatter, depolarization ratio). For each aerosol/cloud functionality the method is described, limitations are discussed and examples are given to illustrate the performances.

  6. Aerosol and Plasma Measurements in Noctilucent Clouds

    NASA Technical Reports Server (NTRS)

    Robertson, Scott

    2000-01-01

    The purpose of this project was to develop rocket-borne probes to detect charged aerosol layers in the mesosphere. These include sporadic E layers, which have their origin in meteoric dust, and noctilucent clouds, which form in the arctic summer and are composed of ice crystals. The probe being developed consists of a charge collecting patch connected to a sensitive electrometer which measures the charge deposited on the patch by impacting aerosols. The ambient electrons and light ions in the mesosphere are prevented from being collected by a magnetic field. The magnetic force causes these lighter particles to turn so that they miss the collecting patch.

  7. The impact of humidity above stratiform clouds on indirect aerosol climate forcing.

    PubMed

    Ackerman, Andrew S; Kirkpatrick, Michael P; Stevens, David E; Toon, Owen B

    2004-12-23

    Some of the global warming from anthropogenic greenhouse gases is offset by increased reflection of solar radiation by clouds with smaller droplets that form in air polluted with aerosol particles that serve as cloud condensation nuclei. The resulting cooling tendency, termed the indirect aerosol forcing, is thought to be comparable in magnitude to the forcing by anthropogenic CO2, but it is difficult to estimate because the physical processes that determine global aerosol and cloud populations are poorly understood. Smaller cloud droplets not only reflect sunlight more effectively, but also inhibit precipitation, which is expected to result in increased cloud water. Such an increase in cloud water would result in even more reflective clouds, further increasing the indirect forcing. Marine boundary-layer clouds polluted by aerosol particles, however, are not generally observed to hold more water. Here we simulate stratocumulus clouds with a fluid dynamics model that includes detailed treatments of cloud microphysics and radiative transfer. Our simulations show that the response of cloud water to suppression of precipitation from increased droplet concentrations is determined by a competition between moistening from decreased surface precipitation and drying from increased entrainment of overlying air. Only when the overlying air is humid or droplet concentrations are very low does sufficient precipitation reach the surface to allow cloud water to increase with droplet concentrations. Otherwise, the response of cloud water to aerosol-induced suppression of precipitation is dominated by enhanced entrainment of overlying dry air. In this scenario, cloud water is reduced as droplet concentrations increase, which diminishes the indirect climate forcing.

  8. Aerosol-Cloud Interactions in the South-East Atlantic

    NASA Astrophysics Data System (ADS)

    Andersen, Hendrik; Cermak, Jan

    2014-05-01

    In this contribution, a satellite-based study on aerosol-cloud interactions (ACI) in the South-East Atlantic with explicit consideration of meteorological conditions is presented. Aerosol-Cloud Interactions remain difficult to quantify and contribute the largest uncertainty to global radiative forcing. These uncertainties make them one of the most important factors for anthropogenic climate perturbations. Interactions are highly complex as microphysical and macrostructural cloud adjustments to aerosol perturbations do not transpire in a black box but are highly dependent on a variety of factors like cloud regime, meteorology and aerosol properties. To gain understanding of the processes that govern ACI in order to increase accuracy of climate models and predictions of future changes in the climate system is thus of great importance. This process study uses multiple statistical approaches to untangle the various influences on ACI. Stratocumulus clouds in the South-East Atlantic are investigated over a time span of 10 years using daily Terra MODIS L3 data for aerosol and cloud parameters. Together with ERA-Interim reanalysis data of cloud-relevant meteorological parameters, statistical relationships between aerosol and cloud properties are derived for different weather types on the basis of a kmeans cluster analysis, in addition to bivariate relationships. Also, the influence of aerosol loading on aerosol-cloud relationships is investigated. Relationships between aerosol and cloud microphysical properties are established. Macrostructural cloud adjustments are more ambiguous, as the observed positive relationship between aerosol and cloud liquid water path (LWP) is inconsistent with the Albrecht hypothesis (more cloud water due to drizzle suppression). Adjustments of cloud optical thickness (COT) to aerosol perturbations are negligible as COT is highly dependent on LWP. Strong relationships between aerosol and cloud fraction are identified, but might be spurious and

  9. Condensed nitrate, sulfate, and chloride in Antarctic stratospheric aerosols

    NASA Technical Reports Server (NTRS)

    Pueschel, R. F.; Snetsinger, K. G.; Toon, O. B.; Ferry, G. V.; Oberbeck, V. R.; Starr, W. L.; Chan, K. R.; Goodman, J. K.

    1989-01-01

    The 1987 Airborne Antarctic Ozone Experiment, in which the NO3, Cl, and SO4 contents of stratospheric aerosols were estimated, is discussed. The aerosol size and chemical composition measurements were carried out on samples collected during August 17 to September 4, 1987. The data indicate that condensed nitrate is found below a threshold temperature of 193.6 + or - 3.0 K, which is generally found at latitudes exceeding 64 deg S. A negative correlation exists between condensed nitrate and ozone correlation.

  10. Aerosol-Cloud-Drizzle-Turbulence Interactions in Boundary Layer Clouds

    DTIC Science & Technology

    2012-09-30

    provide a means for evaluating and developing parameterizations for models that predict cloud microphysical processes. Observations of the...observed during BACEX was associated with African dust above the boundary layer. On two days when convection was completely suppressed, an African... dust event associated with record Aerosol Optical Depths (AODs) for Barbados during this time of the year was observed. The vertical structure of the

  11. Global CALIPSO Observations of Aerosol Changes Near Clouds

    NASA Technical Reports Server (NTRS)

    Varnai, Tamas; Marshak, Alexander

    2011-01-01

    Several recent studies have found that clouds are surrounded by a transition zone of rapidly changing aerosol optical properties and particle size. Characterizing this transition zone is important for better understanding aerosol-cloud interactions and aerosol radiative effects, and also for improving satellite retrievals of aerosol properties. This letter presents a statistical analysis of a monthlong global data set of Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) lidar observations over oceans. The results show that the transition zone is ubiquitous over all oceans and extends up to 15 km away from clouds. They also show that near-cloud enhancements in backscatter and particle size are strongest at low altitudes, slightly below the top of the nearest clouds. Also, the enhancements are similar near illuminated and shadowy cloud sides, which confirms that the asymmetry of Moderate Resolution Imaging Spectroradiometer reflectances found in an earlier study comes from 3-D radiative processes and not from differences in aerosol properties. Finally, the effects of CALIPSO aerosol detection and cloud identification uncertainties are discussed. The findings underline the importance of accounting for the transition zone to avoid potential biases in studies of satellite aerosol products, aerosol-cloud interactions, and aerosol direct radiative effects.

  12. Boreal forests, aerosols and the impacts on clouds and climate.

    PubMed

    Spracklen, Dominick V; Bonn, Boris; Carslaw, Kenneth S

    2008-12-28

    Previous studies have concluded that boreal forests warm the climate because the cooling from storage of carbon in vegetation and soils is cancelled out by the warming due to the absorption of the Sun's heat by the dark forest canopy. However, these studies ignored the impacts of forests on atmospheric aerosol. We use a global atmospheric model to show that, through emission of organic vapours and the resulting condensational growth of newly formed particles, boreal forests double regional cloud condensation nuclei concentrations (from approx. 100 to approx. 200 cm(-3)). Using a simple radiative model, we estimate that the resulting change in cloud albedo causes a radiative forcing of between -1.8 and -6.7 W m(-2) of forest. This forcing may be sufficiently large to result in boreal forests having an overall cooling impact on climate. We propose that the combination of climate forcings related to boreal forests may result in an important global homeostasis. In cold climatic conditions, the snow-vegetation albedo effect dominates and boreal forests warm the climate, whereas in warmer climates they may emit sufficiently large amounts of organic vapour modifying cloud albedo and acting to cool climate.

  13. How much water can pollution aerosols hold in the cloud by suppressing warm rain?

    NASA Astrophysics Data System (ADS)

    Rosenfeld, D.

    2009-12-01

    Vertical profiles of aerosols, cloud drop size distribution and hydrometeors were measured by cloud physics airplanes in a wide range of locations in the world and a wide range of aerosol properties. This includes tropical clouds in the Amazon and Indian Monsoon, severe convective clouds in Argentina and the USA, and winter clouds in California and Israel. The aerosol conditions span from pristine maritime to heavy air pollution and smoke from forest fires, and includes large aerosols such as desert dust and sea spray. It is found that heavy air pollution that is dominated by small cloud condensation nuclei (CCN) can suppress the warm rain processes in warm base clouds (cloud base temperature >20C) up to heights of more than 5 km above cloud base, which is well above the freezing level. The warm rain is formed as supercooled rain that freezes and gets rimed into graupel. Such clouds have intense electrical activity. In microphysically highly continental vigorous convective clouds with cold base of 12C, warm rain is also delayed to 5 km above base. The onset of warm rain in these clouds occur at temperatures close to the homogeneous ice nucleation isotherm of -35C and colder. The resultant drizzle forms the embryos of ice hydrometeors. Giant CCN from dust and sea salt initiate the rain faster than would have been expected based on the concentration of small CCN. A relation between CCN concentration and cloud depth for onset of warm rain can be formulated and applied to cloud parameterization in models that do not calculate explicitly the rain forming processes in clouds.

  14. Cloud Condensation Nucleus Activity of calcite and calcite coated with model humic and fulvic acids

    NASA Astrophysics Data System (ADS)

    Hatch, C. D.; Gierlus, K. M.; Schuttlefield, J. D.; Grassian, V. H.

    2007-12-01

    Many recent studies have shown that organics can alter the water adsorption and cloud condensation nuclei (CCN) activity of common deliquescent species in the Earth's atmosphere. However, very little is known about the effect of organics on water adsorption and CCN activity of common inactive cloud nuclei, such as mineral aerosol. As many studies have shown that a large fraction of unidentified organic material in aerosol particles is composed of polycarboxylic acids resembling humic substances, the presence of these large molecular weight Humic-Like Substances (HULIS) may also alter the water adsorption and CCN activity of mineral aerosol. Thus, we have measured the water adsorption and CCN activity of model humic and fulvic acids. Additionally, the water adsorption and CCN activity of mineral aerosol particles coated with humic and fulvic acids have been studied. We find that humic and fulvic acids show continual multilayer water adsorption as the relative humidity is raised. Additionally, we find that calcite particles mixed with humic and fulvic acids take up more water by mass, by a factor of two, compared to the uncoated calcite particles at approximately 70% RH. CCN measurements also indicate that internally mixed calcite-humic or fulvic acid aerosols are more CCN active than the otherwise inactive, uncoated calcite particles. Our results suggest that mineral aerosol particles coated with high molecular weight organic materials will take up more water and become more efficient CCN in the Earth's atmosphere than single-component mineral aerosol.

  15. Cloud droplet nucleation and its connection to aerosol properties

    SciTech Connect

    Schwartz, S.E.

    1996-04-01

    Anthropogenic aerosols influence the earth`s radiation balance and climate directly, by scattering shortwave (solar) radiation in cloud-free conditions and indirectly, by increasing concentrations of cloud droplets thereby enhancing cloud shortwave reflectivity. These effects are thought to be significant in the context of changes in the earth radiation budget over the industrial period, exerting a radiative forcing that is of comparable magnitude to that of increased concentrations of greenhouse gases over this period but opposite in sign. However the magnitudes of both the direct and indirect aerosol effects are quite uncertain. Much of the uncertainty of the indirect effect arises from incomplete ability to describe changes in cloud properties arising from anthropogenic aerosols. This paper examines recent studies pertaining to the influence of anthropogenic aerosols on loading and properties of aerosols affecting their cloud nucleating properties and indicative of substantial anthropogenic influence on aerosol and cloud properties over the North Atlantic.

  16. The Impact of Aerosols on Cloud and Precipitation Processes: Cloud-Resolving Model Simulations

    NASA Technical Reports Server (NTRS)

    Tao, Wei-Kuo; Khain, A.; Simpson, S.; Johnson, D.; Li, X.; Remer, L.

    2003-01-01

    Cloud microphysics are inevitably affected by the smoke particle (CCN, cloud condensation nuclei) size distributions below the clouds. Therefore, size distributions parameterized as spectral bin microphysics are needed to explicitly study the effects of atmospheric aerosol concentration on cloud development, rainfall production, and rainfall rates for convective clouds. Recently, two detailed spectral-bin microphysical schemes were implemented into the Goddard Cumulus Ensemble (GCE) model. The formulation for the explicit spectral-bin microphysical processes is based on solving stochastic kinetic equations for the size distribution functions of water droplets (i.e., cloud droplets and raindrops), and several types of ice particles [i.e.,pristine ice crystals (columnar and plate-like), snow (dendrites and aggregates), graupel and frozen drops/hail]. Each type is described by a special size distribution function containing many categories (i.e. 33 bins). Atmospheric aerosols are also described using number density size-distribution functions.A spectral-bin microphysical model is very expensive from a from a computational point of view and has only been implemented into the 2D version of the GCE at the present time. The model is tested by studying the evolution of deep tropical clouds in the west Pacific warm pool region using identical thermodynamic conditions but with different concentrations of CCN: a low "clean" concentration and a high "dirty" concentration. Besides the initial differences in aerosol concentration, preliminary results indicate that the low CCN concentration case produces rainfall at the surface sooner than the high CCN case but has less cloud water mass aloft. Because the spectral-bin model explicitly calculates and allows for the examination of both the mass and number concentration of species in each size categor, a detailed analysis of the instantaneous size spectrum can be obtained for the two cases. It is shown that since the low CCN case

  17. Process-model simulations of cloud albedo enhancement by aerosols in the Arctic.

    PubMed

    Kravitz, Ben; Wang, Hailong; Rasch, Philip J; Morrison, Hugh; Solomon, Amy B

    2014-12-28

    A cloud-resolving model is used to simulate the effectiveness of Arctic marine cloud brightening via injection of cloud condensation nuclei (CCN), either through geoengineering or other increased sources of Arctic aerosols. An updated cloud microphysical scheme is employed, with prognostic CCN and cloud particle numbers in both liquid and mixed-phase marine low clouds. Injection of CCN into the marine boundary layer can delay the collapse of the boundary layer and increase low-cloud albedo. Albedo increases are stronger for pure liquid clouds than mixed-phase clouds. Liquid precipitation can be suppressed by CCN injection, whereas ice precipitation (snow) is affected less; thus, the effectiveness of brightening mixed-phase clouds is lower than for liquid-only clouds. CCN injection into a clean regime results in a greater albedo increase than injection into a polluted regime, consistent with current knowledge about aerosol-cloud interactions. Unlike previous studies investigating warm clouds, dynamical changes in circulation owing to precipitation changes are small. According to these results, which are dependent upon the representation of ice nucleation processes in the employed microphysical scheme, Arctic geoengineering is unlikely to be effective as the sole means of altering the global radiation budget but could have substantial local radiative effects.

  18. Aerosol-cloud interactions in the ECHAM6-HAM2 GCM and Aerosol_cci/Cloud_cci satellite products

    NASA Astrophysics Data System (ADS)

    Neubauer, David; Lohmann, Ulrike

    2015-04-01

    The first indirect aerosol effect or cloud albedo effect can be estimated as a radiative forcing. While the sign of this forcing is agreed to be negative, model-based estimates of its magnitude show a large variability. The responses of cloud liquid water content and cloud cover to aerosol increases also referred to as secondary indirect aerosol effects or fast adjustments are uncertain as well. In studies that use the variability in the present day satellite data to infer aerosol-cloud interactions (ACI), or that constrain model parameterizations to better agree with satellite observations a less negative ACI radiative forcing is found. The projects of the Climate Change Initiative (CCI) programme of ESA aim at producing long time series of satellite data of essential climate variables with specific information on errors and uncertainties. The quantification of uncertainty in satellite retrievals provides an opportunity to get insights in the discrepancy between model based and satellite based estimates of ACI. Within the Aerosol_cci project susceptibilities of cloud properties from Cloud_cci to aerosol properties from Aerosol_cci datasets are to be compared to susceptibilities from the aerosol climate model ECHAM6-HAM2. Particularly interesting relationships for the first indirect aerosol effect and the second aerosol indirect effect will be investigated. Satellite studies show a strong effect of aerosol on cloud amount, which could be a methodological artefact such as aerosol swelling or meteorological covariation. The immediate vicinity of clouds needs to be excluded due to these potential cloud contaminations although it would be the most interesting region for associations between aerosol and clouds. As the resolution of the data can have an impact on statistical correlations between cloud and aerosol properties, the assessment will be done on different scales. First results will be presented at the conference.

  19. Some Technical Aspects of a CALIOP and MODIS Data Analysis that Examines Near-Cloud Aerosol Properties as a Function of Cloud Fraction

    NASA Technical Reports Server (NTRS)

    Varnai, Tamas; Yang, Weidong; Marshak, Alexander

    2016-01-01

    CALIOP shows stronger near-cloud changes in aerosol properties at higher cloud fractions. Cloud fraction variations explain a third of near-cloud changes in overall aerosol statistics. Cloud fraction and aerosol particle size distribution have a complex relationship.

  20. Technical Note: Estimating Aerosol Effects on Cloud Radiative Forcing

    SciTech Connect

    Ghan, Steven J.

    2013-10-09

    Estimating anthropogenic aerosol effects on the planetary energy balance through the aerosol influence on clouds using the difference in cloud radiative forcing from simulations with and without anthropogenic emissions produces estimates that are positively biased. A more representative method is suggested using the difference in cloud radiative forcing calculated with aerosol radiative effects neglected. The method also yields an aerosol radiative forcing decomposition that includes a term quantifying the impact of changes in surface albedo. The method requires only two additional diagnostic calculations: the whole-sky and clear-sky top-of-atmosphere radiative flux with aerosol radiative effects neglected.

  1. Comparing the relationships between aerosol optical depth and cloud properties in observations and global models

    NASA Astrophysics Data System (ADS)

    Gryspeerdt, Edward; Quaas, Johannes

    2016-04-01

    Aerosols impact the climate both directly, through their interaction with radiation and indirectly, via their ability to act as cloud condensation nuclei (CCN), modifying cloud properties. The influence of aerosols on cloud properties is highly uncertain. Many relationships between aerosol optical depth (AOD) and cloud properties have been observed using satellite data, but previous work has shown that some of these relationships are the product of the strong AOD-cloud fraction (CF) relationship. The confounding influence of local meteorology obscures the magnitude of any aerosol impact on CF, and so also the impact of aerosol on other cloud properties. For example, both AOD and CF are strongly influenced by relative humidity, which can generate a correlation between them. Previous studies have used reanalysis data to account for confounding meteorological variables. This requires knowledge of the relevant meteorological variables and is limited by the accuracy of the reanalysis data. Recent work has shown that by using the cloud droplet number concentration (CDNC) to mediate the AOD-CF relationship, the impact of relative humidity can be significantly reduced. This method removes the limitations imposed by the finite accuracy of reanalysis data. In this work we investigate the impact of the CDNC mediation on the AOD-CF relationship and on the relationship between AOD and other cloud properties in global atmospheric models. By comparing pre-industrial and present day runs, we investigate the success of the CDNC mediated AOD-CF relationship to predict the change in CF from the pre-industrial to the present day using only observations of the present day relationships between clouds and aerosol properties. This helps to determine whether the satellite-derived relationship provides a constraint on the aerosol indirect forcing due to changes in CF.

  2. Cloud condensation nuclei over the Arctic Ocean in early spring

    SciTech Connect

    Hegg, D.A.; Ferek, R.J.; Hobbs, P.V.

    1995-09-01

    Cloud condensation nucleus (CCN) spectral data are presented for the Arctic in spring, which considerably augment the existing meager CCN database for the Arctic. Concurrent measurements of sulfate mass suggest that most of the CCN were commonly not sulfate. Sulfate was more closely associated with particles below the CCN size range. Some measurements of the microphysical structure of Arctic Stratus clouds are also described.

  3. CALIPSO observations of near-cloud aerosol properties as a function of cloud fraction

    NASA Astrophysics Data System (ADS)

    Yang, Weidong; Marshak, Alexander; Várnai, Tamás.; Wood, Robert

    2014-12-01

    This paper uses spaceborne lidar data to study how near-cloud aerosol statistics of attenuated backscatter depend on cloud fraction. The results for a large region around the Azores show that (1) far-from-cloud aerosol statistics are dominated by samples from scenes with lower cloud fractions, while near-cloud aerosol statistics are dominated by samples from scenes with higher cloud fractions; (2) near-cloud enhancements of attenuated backscatter occur for any cloud fraction but are most pronounced for higher cloud fractions; (3) the difference in the enhancements for different cloud fractions is most significant within 5 km from clouds; (4) near-cloud enhancements can be well approximated by logarithmic functions of cloud fraction and distance to clouds. These findings demonstrate that if variability in cloud fraction across the scenes used for composite aerosol statistics is not considered, a sampling artifact will affect these statistics calculated as a function of distance to clouds. For the Azores region data set examined here, this artifact occurs mostly within 5 km from clouds and exaggerates the near-cloud enhancements of lidar backscatter and color ratio by about 30%. This shows that for accurate characterization of the changes in aerosol properties with distance to clouds, it is important to account for the impact of changes in cloud fraction.

  4. CALIPSO Observations of Near-Cloud Aerosol Properties as a Function of Cloud Fraction

    NASA Technical Reports Server (NTRS)

    Yang, Weidong; Marshak, Alexander; Varnai, Tamas; Wood, Robert

    2015-01-01

    This paper uses spaceborne lidar data to study how near-cloud aerosol statistics of attenuated backscatter depend on cloud fraction. The results for a large region around the Azores show that: (1) far-from-cloud aerosol statistics are dominated by samples from scenes with lower cloud fractions, while near-cloud aerosol statistics are dominated by samples from scenes with higher cloud fractions; (2) near-cloud enhancements of attenuated backscatter occur for any cloud fraction but are most pronounced for higher cloud fractions; (3) the difference in the enhancements for different cloud fractions is most significant within 5km from clouds; (4) near-cloud enhancements can be well approximated by logarithmic functions of cloud fraction and distance to clouds. These findings demonstrate that if variability in cloud fraction across the scenes used to composite aerosol statistics are not considered, a sampling artifact will affect these statistics calculated as a function of distance to clouds. For the Azores-region dataset examined here, this artifact occurs mostly within 5 km from clouds, and exaggerates the near-cloud enhancements of lidar backscatter and color ratio by about 30. This shows that for accurate characterization of the changes in aerosol properties with distance to clouds, it is important to account for the impact of changes in cloud fraction.

  5. The influence of small aerosol particles on the properties of water and ice clouds.

    PubMed

    Choularton, T W; Bower, K N; Weingartner, E; Crawford, I; Coe, H; Gallagher, M W; Flynn, M; Crosier, J; Connolly, P; Targino, A; Alfarra, M R; Baltensperger, U; Sjogren, S; Verheggen, B; Cozic, J; Gysel, M

    2008-01-01

    In this paper, results are presented of the influence of small organic- and soot-containing particles on the formation of water and ice clouds. There is strong evidence that these particles have grown from nano particle seeds produced by the combustion of oil products. Two series of field experiments are selected to represent the observations made. The first is the CLoud-Aerosol Characterisation Experiment (CLACE) series of experiments performed at a high Alpine site (Jungfraujoch), where cloud was in contact with the ground and the measuring station. Both water and ice clouds were examined at different times of the year. The second series of experiments is the CLOud Processing of regional Air Pollution advecting over land and sea (CLOPAP) series, where ageing pollution aerosol from UK cities was observed, from an airborne platform, to interact with warm stratocumulus cloud in a cloud-capped atmospheric boundary layer. Combining the results it is shown that aged pollution aerosol consists of an internal mixture of organics, sulfate, nitrate and ammonium, the organic component is dominated by highly oxidized secondary material. The relative contributions and absolute loadings of the components vary with location and season. However, these aerosols act as Cloud Condensation Nuclei (CCN) and much of the organic material, along with the other species, is incorporated into cloud droplets. In ice and mixed phase cloud, it is observed that very sharp transitions (extending over just a few metres) are present between highly glaciated regions and regions consisting of supercooled water. This is a unique finding; however, aircraft observations in cumulus suggest that this kind of structure may be found in these cloud types too. It is suggested that this sharp transition is caused by ice nucleation initiated by oxidised organic aerosol coated with sulfate in more polluted regions of cloud, sometimes enhanced by secondary ice particle production in these regions.

  6. Improving aerosol interaction with clouds and precipitation in a regional chemical weather modeling system

    NASA Astrophysics Data System (ADS)

    Zhou, C.; Zhang, X.; Gong, S.; Wang, Y.; Xue, M.

    2015-06-01

    A comprehensive aerosol-cloud-precipitation interaction (ACI) scheme has been developed under CMA chemical weather modeling system GRAPES/CUACE. Calculated by a sectional aerosol activation scheme based on the information of size and mass from CUACE and the thermal-dynamic and humid states from the weather model GRAPES at each time step, the cloud condensation nuclei (CCN) is fed online interactively into a two-moment cloud scheme (WDM6) and a convective parameterization to drive the cloud physics and precipitation formation processes. The modeling system has been applied to study the ACI for January 2013 when several persistent haze-fog events and eight precipitation events occurred. The results show that interactive aerosols with the WDM6 in GRAPES/CUACE obviously increase the total cloud water, liquid water content and cloud droplet number concentrations while decrease the mean diameter of cloud droplets with varying magnitudes of the changes in each case and region. These interactive micro-physical properties of clouds improve the calculation of their collection growth rates in some regions and hence the precipitation rate and distributions in the model, showing 24 to 48% enhancements of TS scoring for 6 h precipitation in almost all regions. The interactive aerosols with the WDM6 also reduce the regional mean bias of temperature by 3 °C during certain precipitation events, but the monthly means bias is only reduced by about 0.3 °C.

  7. Long-term impacts of aerosols on the vertical development of clouds and precipitation

    SciTech Connect

    Li, Zhanqing; Niu, F.; Fan, Jiwen; Liu, Yangang; Rosenfeld, Daniel; Ding, Yanni

    2011-12-01

    Aerosol has complex effects on clouds and precipitation that may augment or offset each other contingent upon a variety of variables. As a result, its long-term impact on climate is largely unknown. Using 10 years of the US Atmospheric Radiation Measurement (ARM) measurements, strong aerosol effects of climatologically significance are detected. With increasing total aerosol number concentration (condensation nucleus, CN) measured near the ground, both cloud top height and precipitation change systematically for mix-phase clouds of warm-base (cloud base <1km) and cold-top (above the freezing level), but not for pure liquid and ice clouds. Cloud thickness can increase systematically with the CN concentration by up to a factor of 2. The response of precipitation to CN depends on cloud liquid water path (LWP). As CN increases, rain occurs more frequently for high LWP but less frequently for low LWP. Such strong signals of aerosol long-term impact on cloud and precipitation have not been reported and have significant implications for climate change studies, especially concerning regional and global climate change induced by pollution.

  8. Improving aerosol interaction with clouds and precipitation in a regional chemical weather modeling system

    NASA Astrophysics Data System (ADS)

    Zhou, C.; Zhang, X.; Gong, S.

    2015-12-01

    A comprehensive aerosol-cloud-precipitation interaction (ACI) scheme has been developed under CMA chemical weather modeling system GRAPES/CUACE. Calculated by a sectional aerosol activation scheme based on the information of size and mass from CUACE and the thermal-dynamic and humid states from the weather model GRAPES at each time step, the cloud condensation nuclei (CCN) is fed online interactively into a two-moment cloud scheme (WDM6) and a convective parameterization to drive the cloud physics and precipitation formation processes. The modeling system has been applied to study the ACI for January 2013 when several persistent haze-fog events and eight precipitation events occurred. The results show that interactive aerosols with the WDM6 in GRAPES/CUACE obviously increase the total cloud water, liquid water content and cloud droplet number concentrations while decrease the mean diameter of cloud droplets with varying magnitudes of the changes in each case and region. These interactive micro-physical properties of clouds improve the calculation of their collection growth rates in some regions and hence the precipitation rate and distributions in the model, showing 24% to 48% enhancements of TS scoring for 6-h precipitation in almost all regions. The interactive aerosols with the WDM6 also reduce the regional mean bias of temperature by 3 °C during certain precipitation events, but the monthly means bias is only reduced by about 0.3°C.

  9. MATRIX-VBS Condensing Organic Aerosols in an Aerosol Microphysics Model

    NASA Technical Reports Server (NTRS)

    Gao, Chloe Y.; Tsigaridis, Konstas; Bauer, Susanne E.

    2015-01-01

    The condensation of organic aerosols is represented in a newly developed box-model scheme, where its effect on the growth and composition of particles are examined. We implemented the volatility-basis set (VBS) framework into the aerosol mixing state resolving microphysical scheme Multiconfiguration Aerosol TRacker of mIXing state (MATRIX). This new scheme is unique and advances the representation of organic aerosols in models in that, contrary to the traditional treatment of organic aerosols as non-volatile in most climate models and in the original version of MATRIX, this new scheme treats them as semi-volatile. Such treatment is important because low-volatility organics contribute significantly to the growth of particles. The new scheme includes several classes of semi-volatile organic compounds from the VBS framework that can partition among aerosol populations in MATRIX, thus representing the growth of particles via condensation of low volatility organic vapors. Results from test cases representing Mexico City and a Finish forrest condistions show good representation of the time evolutions of concentration for VBS species in the gas phase and in the condensed particulate phase. Emitted semi-volatile primary organic aerosols evaporate almost completely in the high volatile range, and they condense more efficiently in the low volatility range.

  10. An Investigation into Cloud Condensation Nuclei (CCN) Activation in the Southwestern United States

    NASA Astrophysics Data System (ADS)

    Crosbie, E. C.; Youn, J.; Wonaschuetz, A.; Sorooshian, A.

    2013-12-01

    Cloud condensation nuclei (CCN) comprise a key component of the total aerosol with critical influences on weather and climate. The importance of CCN concentration is often linked to radiative feedbacks associated with cloud albedo, which has important consequences for climate sensitivity, however the importance of CCN may also extend to cloud dynamics in convective environments and atmospheric electricity. We present data from fifteen months of field measurements taken in an urban environment on a rooftop of a building at the University of Arizona campus in Tucson, Arizona. CCN were measured at high temporal resolution concurrently with measurements of particle size distributions, meteorological parameters, and the composition of the organic fraction of the aerosol. We investigate monthly, weekly, and diurnal patterns in the data along with activation ratio and apparent activation diameter, which provide important insight into the micro-scale dependencies of cloud activation. Furthermore, we examine the relationship between CCN and local and regional meteorology, with particular focus on the North American Monsoon season, to investigate feedback and response mechanisms relating to dynamics, microphysics, and chemistry. Monsoon aerosol are shown to have favorable composition to allow for higher CCN activity and thus lower apparent activation diameters. This finding coincides with enhanced aqueous-phase chemistry to produce more hygroscopic aerosol constituents such as sulfate and water-soluble organic compounds.

  11. Modeling aerosol growth by aqueous chemistry in nonprecipitating stratiform cloud

    SciTech Connect

    Ovchinnikov, Mikhail; Easter, Richard C.

    2010-07-29

    A new microphysics module based on a two-dimensional (2D) joint size distribution function representing both interstitial and cloud particles is developed and applied to studying aerosol processing in non-precipitating stratocumulus clouds. The module is implemented in a three-dimensional dynamical framework of a large-eddy simulation (LES) model and in a trajectory ensemble model (TEM). Both models are used to study the modification of sulfate aerosol by the activation - aqueous chemistry - resuspension cycle in shallow marine stratocumulus clouds. The effect of particle mixing and different size-distribution representations on modeled aerosol processing are studied in a comparison of the LES and TEM simulations with the identical microphysics treatment exposes and a comparison of TEM simulations with a 2D fixed and moving bin microphysics. Particle mixing which is represented in LES and neglected in the TEM leads to the mean relative per particle dry mass change in the TEM simulations being about 30% lower than in analogous subsample of LES domain. Particles in the final LES spectrum are mixed in from different “parcels”, some of which have experienced longer in-cloud residence times than the TEM parcels, all of which originated in the subcloud layer, have. The mean relative per particle dry mass change differs by 14% between TEM simulations with fixed and moving bin microphysics. Finally, the TEM model with the moving bin microphysics is used to evaluate assumptions about liquid water mass partitioning among activated cloud condensation nuclei (CCN) of different dry sizes. These assumptions are used in large-scale models to map the bulk aqueous chemistry sulfate production, which is largely proportional to the liquid water mass, to the changes in aerosol size distribution. It is shown that the commonly used assumptions that the droplet mass is independent of CCN size or that the droplet mass is proportional to the CCN size to the third power do not perform

  12. Quantifying compositional impacts of ambient aerosol on cloud droplet formation

    NASA Astrophysics Data System (ADS)

    Lance, Sara

    It has been historically assumed that most of the uncertainty associated with the aerosol indirect effect on climate can be attributed to the unpredictability of updrafts. In Chapter 1, we analyze the sensitivity of cloud droplet number density, to realistic variations in aerosol chemical properties and to variable updraft velocities using a 1-dimensional cloud parcel model in three important environmental cases (continental, polluted and remote marine). The results suggest that aerosol chemical variability may be as important to the aerosol indirect effect as the effect of unresolved cloud dynamics, especially in polluted environments. We next used a continuous flow streamwise thermal gradient Cloud Condensation Nuclei counter (CCNc) to study the water-uptake properties of the ambient aerosol, by exposing an aerosol sample to a controlled water vapor supersaturation and counting the resulting number of droplets. In Chapter 2, we modeled and experimentally characterized the heat transfer properties and droplet growth within the CCNc. Chapter 3 describes results from the MIRAGE field campaign, in which the CCNc and a Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA) were deployed at a ground-based site during March, 2006. Size-resolved CCN activation spectra and growth factor distributions of the ambient aerosol in Mexico City were obtained, and an analytical technique was developed to quantify a probability distribution of solute volume fractions for the CCN in addition to the aerosol mixing-state. The CCN were shown to be much less CCN active than ammonium sulfate, with water uptake properties more consistent with low molecular weight organic compounds. The pollution outflow from Mexico City was shown to have CCN with an even lower fraction of soluble material. "Chemical Closure" was attained for the CCN, by comparing the inferred solute volume fraction with that from direct chemical measurements. A clear diurnal pattern was observed for the CCN solute

  13. LES simulation of cloud-aerosols-chemistry interactions in Western Africa

    NASA Astrophysics Data System (ADS)

    Leriche, M.; Brosse, F.; Mari, C. H.; Couvreux, F.

    2014-12-01

    Low clouds have a major impact on the radiative balance of the earth, in particular in tropical areas. The Southern West Africa (SWA) area encounters during boreal summer frequent formations of stratus and/or cumulus clouds over a large extent. These cloud bands, still badly represented in climatic models, can lead to large errors in the estimation of the cloud radiative forcing. Moreover, these cloud bands can evolve or not in cumulus congestus clouds leading to precipitations. The SWA area is characterized by a large diversity of natural and anthropic emissions of gaseous chemical species and aerosol particles. These emissions have a potential large impact on the number concentration and chemical composition of aerosol particles over the SWA zone. This impact is direct through emissions of primary particles, and indirect through the formation of secondary particles from gaseous precursors. A part of these particles will act as cloud condensation nuclei, thus, influencing the cloud microphysics characteristics. In order to improve our understanding of these complex processes, an airborne campaign is planed in summer 2015 over SWA zone in the framework of the European project DACCIWA (Dynamics-aerosol-chemistry-cloud interactions in West Africa). To prepare the campaign and begin to investigate the cloud-chemistry-aerosols interactions, a LES simulation on a case study designed from an AMMA (African Monsoon Multidisciplinary Analyses) case has been performed with the 3D online-chemistry Meso-NH model. The LES simulation captures the chemical segregation due to thermals in the rising convective boundary layer. Comparing simulation with or without cloud chemistry highlights the effect of aqueous phase chemistry on gaseous precursors of aerosol particles.

  14. Parameterizations of Cloud Microphysics and Indirect Aerosol Effects

    SciTech Connect

    Tao, Wei-Kuo

    2014-05-19

    1. OVERVIEW Aerosols and especially their effect on clouds are one of the key components of the climate system and the hydrological cycle [Ramanathan et al., 2001]. Yet, the aerosol effect on clouds remains largely unknown and the processes involved not well understood. A recent report published by the National Academy of Science states "The greatest uncertainty about the aerosol climate forcing - indeed, the largest of all the uncertainties about global climate forcing - is probably the indirect effect of aerosols on clouds [NRC, 2001]." The aerosol effect on clouds is often categorized into the traditional "first indirect (i.e., Twomey)" effect on the cloud droplet sizes for a constant liquid water path [Twomey, 1977] and the "semi-direct" effect on cloud coverage [e.g., Ackerman et al., 2000]. Enhanced aerosol concentrations can also suppress warm rain processes by producing a narrow droplet spectrum that inhibits collision and coalescence processes [e.g., Squires and Twomey, 1961; Warner and Twomey, 1967; Warner, 1968; Rosenfeld, 1999]. The aerosol effect on precipitation processes, also known as the second type of aerosol indirect effect [Albrecht, 1989], is even more complex, especially for mixed-phase convective clouds. Table 1 summarizes the key observational studies identifying the microphysical properties, cloud characteristics, thermodynamics and dynamics associated with cloud systems from high-aerosol continental environments. For example, atmospheric aerosol concentrations can influence cloud droplet size distributions, warm-rain process, cold-rain process, cloud-top height, the depth of the mixed phase region, and occurrence of lightning. In addition, high aerosol concentrations in urban environments could affect precipitation variability by providing an enhanced source of cloud condensation nuclei (CCN). Hypotheses have been developed to explain the effect of urban regions on convection and precipitation [van den Heever and Cotton, 2007 and Shepherd

  15. The Impact of humidity above stratiform clouds on indirect aerosol climate forcing

    SciTech Connect

    Ackerman, A S; Kirkpatrick, M P; Stevens, D E; Toon, O B

    2004-12-20

    Some of the global warming effect of anthropogenic greenhouse gases is offset by increased solar reflection from clouds with smaller droplets that form on increased numbers of cloud condensation nuclei in polluted air. The global magnitude of the resulting indirect aerosol climate forcing is estimated to be comparable (and opposed) to the anthropogenic carbon dioxide forcing, but estimates are highly uncertain because of complexities in characterizing the physical process that determine global aerosol and cloud populations and their interactions. Beyond reflecting sunlight more effectively, smaller droplets are less efficient at producing precipitation, and decreased precipitation is expected to result in increased cloud water and cloud cover, further increasing the indirect forcing. Yet polluted marine boundary-layer clouds are not generally observed to hold more water. Here we use model simulations of stratocumulus clouds to show that suppression of precipitation from increased droplet concentrations leads to increased cloud water only when sufficient precipitation reaches the surface, a condition favored when the overlying air is moist. Otherwise, aerosol induced suppression of precipitation enhances entrainment of overlying dry air, thereby reducing cloud water and diminishing the indirect climate forcing.

  16. Cloud-Resolving Model Simulations of Aerosol-Cloud Interactions Triggered by Strong Aerosol Emissions in the Arctic

    NASA Astrophysics Data System (ADS)

    Wang, H.; Kravitz, B.; Rasch, P. J.; Morrison, H.; Solomon, A.

    2014-12-01

    Previous process-oriented modeling studies have highlighted the dependence of effectiveness of cloud brightening by aerosols on cloud regimes in warm marine boundary layer. Cloud microphysical processes in clouds that contain ice, and hence the mechanisms that drive aerosol-cloud interactions, are more complicated than in warm clouds. Interactions between ice particles and liquid drops add additional levels of complexity to aerosol effects. A cloud-resolving model is used to study aerosol-cloud interactions in the Arctic triggered by strong aerosol emissions, through either geoengineering injection or concentrated sources such as shipping and fires. An updated cloud microphysical scheme with prognostic aerosol and cloud particle numbers is employed. Model simulations are performed in pure super-cooled liquid and mixed-phase clouds, separately, with or without an injection of aerosols into either a clean or a more polluted Arctic boundary layer. Vertical mixing and cloud scavenging of particles injected from the surface is still quite efficient in the less turbulent cold environment. Overall, the injection of aerosols into the Arctic boundary layer can delay the collapse of the boundary layer and increase low-cloud albedo. The pure liquid clouds are more susceptible to the increase in aerosol number concentration than the mixed-phase clouds. Rain production processes are more effectively suppressed by aerosol injection, whereas ice precipitation (snow) is affected less; thus the effectiveness of brightening mixed-phase clouds is lower than for liquid-only clouds. Aerosol injection into a clean boundary layer results in a greater cloud albedo increase than injection into a polluted one, consistent with current knowledge about aerosol-cloud interactions. Unlike previous studies investigating warm clouds, the impact of dynamical feedback due to precipitation changes is small. According to these results, which are dependent upon the representation of ice nucleation

  17. Cloud Scavenging Effects on Aerosol Radiative and Cloud-nucleating Properties - Final Technical Report

    SciTech Connect

    Ogren, John A.; Sheridan, Patrick S.; Andrews, Elisabeth

    2009-03-05

    The optical properties of aerosol particles are the controlling factors in determining direct aerosol radiative forcing. These optical properties depend on the chemical composition and size distribution of the aerosol particles, which can change due to various processes during the particles’ lifetime in the atmosphere. Over the course of this project we have studied how cloud processing of atmospheric aerosol changes the aerosol optical properties. A counterflow virtual impactor was used to separate cloud drops from interstitial aerosol and parallel aerosol systems were used to measure the optical properties of the interstitial and cloud-scavenged aerosol. Specifically, aerosol light scattering, back-scattering and absorption were measured and used to derive radiatively significant parameters such as aerosol single scattering albedo and backscatter fraction for cloud-scavenged and interstitial aerosol. This data allows us to demonstrate that the radiative properties of cloud-processed aerosol can be quite different than pre-cloud aerosol. These differences can be used to improve the parameterization of aerosol forcing in climate models.

  18. Organic Aerosol Nucleation and Growth at the CERN CLOUD chamber

    NASA Astrophysics Data System (ADS)

    Tröstl, Jasmin; Lethipalo, Katrianne; Bianchi, Federico; Sipilä, Mikko; Nieminen, Tuomo; Wagner, Robert; Frege, Carla; Simon, Mario; Weingartner, Ernest; Gysel, Martin; Dommen, Josef; Baltensperger, Urs

    2014-05-01

    It is well known that atmospheric aerosols influence the climate by changing Earth's radiation balance (IPCC 2007 and 2013). Recent models have shown (Merikanto et al. 2009) that aerosol nucleation is one of the biggest sources of low level cloud condensation nuclei. Still, aerosol nucleation and growth are not fully understood. The driving force of nucleation and growth is sulfuric acid. However ambient nucleation and growth rates cannot be explained by solely sulfuric acid as precursor. Recent studies have shown that only traces of precursors like ammonia and dimethylamine enhance the nucleation rates dramatically (Kirkby et al. 2011, Almeida et al., 2013). Thus the role of different aerosol precursor needs to be studied not only in ambient but also in very well controlled chamber experiments. The CLOUD (Cosmics Leaving OUtdoor Droplets) experiment enables conducting experiments very close to atmospheric conditions and with a very low contaminant background. The latest CLOUD experiments focus on the role of organics in aerosol nucleation and growth. For this purpose, numerous experiments with alpha-pinene have been conducted at the CERN CLOUD chamber. Several state-of-the-art instruments were used to cover the whole complexity of the experiment. Chamber conditions were set to 40% relative humidity and 5° C. Atmospheric concentrations of SO2, O3, HONO, H2O and alpha-pinene were injected to the chamber. Different oxidation conditions were used, yielding different levels of oxidized organics: (1) OH radicals, (2) Ozone with the OH scavenger H2 (pure ozonolysis) and (3) both. SO2 was injected to allow for sulfuric acid production. Optical UV fibers were used to enable photochemical reactions. A high field cage (30 kV) can be turned on to remove all charged particles in the chamber to enable completely neutral conditions. Comparing neutral conditions to the beam conditions using CERN's proton synchrotron, the fraction of ion-induced nucleation can be studied. Using

  19. The Southern Ocean Clouds, Radiation, Aerosol Transport Experimental Study (SOCRATES): An Observational Campaign for Determining Role of Clouds, Aerosols and Radiation in Climate System

    NASA Astrophysics Data System (ADS)

    McFarquhar, G. M.; Wood, R.; Bretherton, C. S.; Alexander, S.; Jakob, C.; Marchand, R.; Protat, A.; Quinn, P.; Siems, S. T.; Weller, R. A.

    2014-12-01

    The Southern Ocean (SO) region is one of the cloudiest on Earth, and as such clouds determine its albedo and play a major role in climate. Evidence shows Earth's climate sensitivity and the Intertropical Convergence Zone location depend upon SO clouds. But, climate models are challenged by uncertainties and biases in the simulation of clouds, aerosols, and air-sea exchanges in this region which trace back to a poor process-level understanding. Due to the SO's remote location, there have been sparse observations of clouds, aerosols, precipitation, radiation and the air-sea interface apart from those from satellites. Plans for an upcoming observational program, SOCRATES, are outlined. Based on feedback on observational and modeling requirements from a 2014 workshop conducted at the University of Washington, a plan is described for obtaining a comprehensive dataset on the boundary-layer structure and associated vertical distributions of liquid and mixed-phase cloud and aerosol properties across a range of synoptic settings, especially in the cold sector of cyclonic storms. Four science themes are developed: improved climate model simulation of SO cloud and boundary layer structure in a rapidly varying synoptic setting; understanding seasonal and synoptic variability in SO cloud condensation and ice nucleus concentration and the role of local biogenic sources; understanding supercooled liquid and mixed-phase clouds and their impacts; and advancing retrievals of clouds, precipitation, aerosols, radiation and surface fluxes. Testable hypotheses for each theme are identified. The observational strategy consists of long-term ground-based observations from Macquarie Island and Davis, continuous data collection onboard Antarctic supply ships, satellite retrievals, and a dedicated field campaign covering 2 distinct seasons using in-situ and remote sensors on low- and high-altitude aircraft, UAVs, and a ship-borne platform. A timeline for these activities is proposed.

  20. Approaches to Observe Anthropogenic Aerosol-Cloud Interactions.

    PubMed

    Quaas, Johannes

    Anthropogenic aerosol particles exert an-quantitatively very uncertain-effective radiative forcing due to aerosol-cloud interactions via an immediate altering of cloud albedo on the one hand and via rapid adjustments by alteration of cloud processes and by changes in thermodynamic profiles on the other hand. Large variability in cloud cover and properties and the therefore low signal-to-noise ratio for aerosol-induced perturbations hamper the identification of effects in observations. Six approaches are discussed as a means to isolate the impact of anthropogenic aerosol on clouds from natural cloud variability to estimate or constrain the effective forcing. These are (i) intentional cloud modification, (ii) ship tracks, (iii) differences between the hemispheres, (iv) trace gases, (v) weekly cycles and (vi) trends. Ship track analysis is recommendable for detailed process understanding, and the analysis of weekly cycles and long-term trends is most promising to derive estimates or constraints on the effective radiative forcing.

  1. Cloud forming potential of oligomers relevant to secondary organic aerosols

    NASA Astrophysics Data System (ADS)

    Xu, Wen; Guo, Song; Gomez-Hernandez, Mario; Zamora, Misti L.; Secrest, Jeremiah; Marrero-Ortiz, Wilmarie; Zhang, Annie L.; Collins, Don R.; Zhang, Renyi

    2014-09-01

    The hygroscopic growth factor (HGF) and cloud condensation nuclei (CCN) activity are measured for surrogates that mimic atmospherically relevant oligomers, including glyoxal trimer dihydrate, methyl glyoxal trimer dihydrate, sucrose, methyl glyoxal mixtures with sulfuric acid and glycolic acid, and 2,4-hexandienal mixtures with sulfuric acid and glycolic acid. For the single-component aerosols, the measured HGF ranges from 1.3 to 1.4 at a relative humidity of 90%, and the hygroscopicity parameter (κ) is in the range of 0.06 to 0.19 on the basis of the measured CCN activity and 0.13 to 0.22 on the basis of the measured HGF, compared to the calculated values of 0.08 to 0.16. Large differences exist in the κ values derived using the measured HGF and CCN data for the multi-component aerosols. Our results reveal that, in contrast to the oxidation process, oligomerization decreases particle hygroscopicity and CCN activity and provides guidance for analyzing the organic species in ambient aerosols.

  2. Clouds, Aerosol, and Precipitation in the Marine Boundary Layer (CAP-MBL) Final Campaign Report

    SciTech Connect

    Wood, R.

    2016-01-01

    The extensive coverage of low clouds over the subtropical eastern oceans greatly impacts the current climate. In addition, the response of low clouds to changes in atmospheric greenhouse gases and aerosols is a major source of uncertainty, which thwarts accurate prediction of future climate change. Low clouds are poorly simulated in climate models, partly due to inadequate long-term simultaneous observations of their macrophysical and microphysical structure, radiative effects, and associated aerosol distribution in regions where their impact is greatest. The thickness and extent of subtropical low clouds is dependent on tight couplings between surface fluxes of heat and moisture, radiative cooling, boundary layer turbulence, and precipitation (much of which evaporates before reaching the ocean surface and is closely connected to the abundance of cloud condensation nuclei). These couplings have been documented as a result of past field programs and model studies. However, extensive research is still required to achieve a quantitative understanding sufficient for developing parameterizations, which adequately predict aerosol indirect effects and low cloud response to climate perturbations. This is especially true of the interactions between clouds, aerosol, and precipitation. These processes take place in an ever-changing synoptic environment that can confound interpretation of short time period observations.

  3. Hemispheric aerosol vertical profiles: anthropogenic impacts on optical depth and cloud nuclei.

    PubMed

    Clarke, Antony; Kapustin, Vladimir

    2010-09-17

    Understanding the effect of anthropogenic combustion upon aerosol optical depth (AOD), clouds, and their radiative forcing requires regionally representative aerosol profiles. In this work, we examine more than 1000 vertical profiles from 11 major airborne campaigns in the Pacific hemisphere and confirm that regional enhancements in aerosol light scattering, mass, and number are associated with carbon monoxide from combustion and can exceed values in unperturbed regions by more than one order of magnitude. Related regional increases in a proxy for cloud condensation nuclei (CCN) and AOD imply that direct and indirect aerosol radiative effects are coupled issues linked globally to aged combustion. These profiles constrain the influence of combustion on regional AOD and CCN suitable for challenging climate model performance and informing satellite retrievals.

  4. Photoreactivity of condensed species on Titan's aerosols analogues

    NASA Astrophysics Data System (ADS)

    Fleury, Benjamin; Gudipati, Murthy; Carrasco, Nathalie

    2016-10-01

    Titan's aerosols formation is initiated in the upper atmospheric layers at about 1000 km by the dissociation and the ionization of N2 and CH4 by the VUV solar photons [1]. Then, they aggregate and sediment to the surface. The temperatures of the stratosphere and the troposphere [3] (measured by the HASI instrument onboard the Huygens probe [2]) allow the condensation of many volatile organics on the solid aerosols, forming organic ice coating on the aerosol polymers. We will present an experimental study simulating this process and discuss the photoreactivity of condensed species on Titan's aerosols analogues in the atmosphere and on the surface. We demonstrated experimentally that the organic aerosols, which cover the Titan's surface, drive the photoreactivity of condensed species such as acetylene when they are irradiated with long wavelength photons (λ > 300 nm). This result highlights that Titan's surface remains active despite the absorption of the most energetic photons by the atmosphere.AcknowledgmentsThis work is supported by NASA Solar System Workings grant " Photochemistry in Titan's Lower Atmosphere". The research work has been carried out at the Jet Propulsion Laboratory, California Institute of Technology under a contract with the National Aeronautics and Space Administration. NC acknowledges the European Research Council for their financial support (ERC Starting Grant PRIMCHEM, grant agreement n°636829).References[1] Waite, J. H., et al., The process of Tholin formation in Titan's upper atmosphere, (2007), Science 316, 870-875.[2] Fulchignoni, M., et al., In situ measurements of the physical characteristics of Titan's environment, (2005), Nature 438, 785-791[3] Lavvas, P., et al., Condensation in Titan's atmosphere at the Huygens landing site, (2011), Icarus 215, 732-750.

  5. Aerosol-CAPE-Cloud Interactions over Gangetic Basin

    NASA Astrophysics Data System (ADS)

    Tripathi, S. N.; Sarangi, C.

    2015-12-01

    In the last few decades exponential growth of population and rapid industrialization has resulted in high aerosol loading over Gangetic basin (GB) in Northern India. Gangetic basin is the food basket of India and its agricultural yield is mainly dependent on South Asian summer monsoon. Hence, understanding the aerosol-cloud-rainfall interactions is crucial and demand utmost attention. In this study, we have used more than a decade (2002-2013) of Radiosonde measurements from 5 WMO stations over the GB to illustrate enhancement of CAPE and cloud thickness with increase in AOD under deep cloudy conditions. Enhancement in mean atmospheric temperature below cloud layer at higher aerosol loading was also observed. These observations suggest that increase in aerosols increases the atmospheric temperature below cloud base and causes increase in CAPE, which, in turn, invigorates the cloud dynamics and eventually resultsin deeper cloud systems. Simultaneously, analysis of decade long satellite and in-situ observational datasets provided compelling evidence of aerosol-induced cloud invigoration, from cloud macrophysical as well as microphysical observations, which fostered a net atmospheric cooling nearly twice compared to the aerosol direct effect. Moreover, a striking positive association between aerosol loading and daily surface rainfall during Indian summer monsoon was found. The observed aerosol-induced heating of lower atmosphere, intensification of cloud dynamics, deepening of clouds, intensification of precipitation rate and daily rainfall coherently suggested an increase in surface water with increase in aerosol loading. Hence, this study not only demonstrates the importance of aerosol-induced microphysical perturbations during Indian summer monsoon but also is a major step forward in understanding the impact of aerosols on surface water under continental conditions.

  6. A Study of Aerosol Effect on Marine Water Clouds with Long-term Satellite Climate Data Records

    NASA Astrophysics Data System (ADS)

    Zhao, X.; Heidinger, A. K.; Walther, A.

    2015-12-01

    Cloud microphysical structures and properties provide a critical link between the energy and hydrological cycles of Earth's climate system. A change of cloud microphysical properties related to anthropogenic activities may result in distressing climate consequence and changes. Since atmospheric aerosol is the major source of cloud condensation nuclei (CNN) that is critical for the formation of cloud microphysical structures and properties, aerosol changes due to anthropogenic emissions will result in the modification of CCN and cloud microphysical properties and eventually cause the changes of Earth's climate. In this study, we will investigate the effect of aerosol on the microphysical properties, including cloud particle effective radius, cloud water path, and cloud optical depth, of marine stratus clouds by using more than 30-years climate data records (CDRs) of aerosols and clouds derived from NOAA operational AVHRR satellite observations. The correlation between satellite derived cloud and aerosol microphysical parameters will be determined and the statistics significance will be examined using the long-term AVHRR satellite CDRs.

  7. STORMVEX. Ice Nuclei and Cloud Condensation Nuclei Characterization Field Campaign Report

    SciTech Connect

    Cziczo, D.

    2016-03-01

    The relationship between aerosol particles and the formation of clouds is among the most uncertain aspects in our current understanding of climate change. Warm clouds have been the most extensively studied, in large part because they are normally close to the Earth’s surface and only contain large concentrations of liquid droplets. Ice and mixed-phase clouds have been less studied even though they have extensive global coverage and dominate precipitation formation. Because they require low temperatures to form, both cloud types are infrequently found at ground level, resulting in more difficult field studies. Complex mixtures of liquid and ice elements, normally at much lower concentrations than found in warm clouds, require precise separation techniques and accurate identification of phase. Because they have proved so difficult to study, the climatic impact of ice-containing clouds remains unresolved. In this study, cloud condensation nuclei (CCN) concentrations and associated single particles’ composition and size were measured at a high-elevation research site—Storm Peak Lab, east of Steamboat Springs, Colorado, operated by the Desert Research Institute. Detailed composition analyses were presented to compare CCN activation with single-particle composition. In collaboration with the scientists of the Storm Peak Lab Cloud Property Validation Experiment (STORMVEX), our goal was to relate these findings to the cloud characteristics and the effect of anthropogenic activities.

  8. Aerosols in polluted versus nonpolluted air masses Long-range transport and effects on clouds

    NASA Technical Reports Server (NTRS)

    Pueschel, R. F.; Van Valin, C. C.; Castillo, R. C.; Kadlecek, J. A.; Ganor, E.

    1986-01-01

    To assess the influence of anthropogenic aerosols on the physics and chemistry of clouds in the northeastern United States, aerosol and cloud-drop size distributions, elemental composition of aerosols as a function of size, and ionic content of cloud water were measured on Whiteface Mountain, NY, during the summers of 1981 and 1982. In several case studies, the data were cross-correlated with different air mass types - background continental, polluted continental, and maritime - that were advected to the sampling site. The results are the following: (1) Anthropogenic sources hundreds of kilometers upwind cause the small-particle (accumulation) mode number to increase from hundreds of thousands per cubic centimeter and the mass loading to increase from a few to several tens of micrograms per cubic meter, mostly in the form of sulfur aerosols. (2) A significant fraction of anthropogenic sulfur appears to act as cloud condensation nuclei (CCN) to affect the cloud drop concentration. (3) Clouds in Atlantic maritime air masses have cloud drop spectra that are markedly different from those measured in continental clouds. The drop concentration is significantly lower, and the drop size spectra are heavily skewed toward large drops. (4) Effects of anthropogenic pollutants on cloud water ionic composition are an increase of nitrate by a factor of 50, an increase of sulfate by more than one order of magnitude, and an increase of ammonium ion by a factor of 7. The net effect of the changes in ionic concentrations is an increase in cloud water acidity. An anion deficit even in maritime clouds suggests an unknown, possibly biogenic, source that could be responsible for a pH below neutral, which is frequently observed in nonpolluted clouds.

  9. The Impact of Aerosols on Cloud and Precipitation Processes: Cloud-Resolving Model Simulations

    NASA Technical Reports Server (NTRS)

    Tao, Wei-Kuo; Khain, A.; Simpson, S.; Johnson, D.; Li, X.; Remer, L.

    2003-01-01

    Cloud microphysics are inevitable affected by the smoke particle (CCN, cloud condensation nuclei) size distributions below the clouds. Therefore, size distribution parameterized as spectral bin microphysics are needed to explicitly study the effect of atmospheric aerosol concentration on cloud development, rainfall production, and rainfall rates convective clouds. Recently, two detailed spectral-bin microphysical schemes were implemented into the Goddard Cumulus Ensembel (GCE) model. The formulation for the explicit spectral-bim microphysical processes is based on solving stochastic kinetic equations for the size distribution functions of water droplets (i.e., cloud droplets and raindrops), and several types of ice particles [i.e., pristine ice crystals (columnar and plate-like), snow (dendrites and aggregates), groupel and frozen drops/hall] Each type is described by a special size distribution function containing many categories (i.e., 33 bins). Atmospheric aerosols are also described using number density size-distribution functions.A spectral-bin microphysical model is very expensive from a computational point of view and has only been implemented into the 2D version of the GCE at the present time. The model is tested by studying the evolution of deep cloud systems in the west Pacific warm pool region and in the mid-latitude using identical thermodynamic conditions but with different concentrations of CCN: a low "clean" concentration and a high "dirty" concentration. Besides the initial differences in aerosol concentration, preliminary results indicate that the low CCN concentration case produces rainfall at the surface sooner than the high CCN case but has less cloud water mass aloft. Because the spectral-bim model explicitly calculates and allows for the examination of both the mass and number concentration of cpecies in each size category, a detailed analysis of the instantaneous size spectrum can be obtained for the two cases. It is shown that since the low

  10. Space-borne observations of aerosol - cloud relations for cloud systems of different heights

    NASA Astrophysics Data System (ADS)

    Stathopoulos, S.; Georgoulias, A. K.; Kourtidis, K.

    2017-01-01

    Here, we examine the aerosol - cloud relations over three major urban clusters of China, representative of three different climatic regimes, under different water vapor conditions and cloud heights, using Aerosol Optical Depth at 550 nm (AOD), Cloud Fraction (CC), Cloud Optical Depth (COD), Water Vapor (WV) and Cloud Top Pressure (CTP) data from the MODIS instrument. Over all regions and for all seasons, CC is found to increase with increasing AOD, WV and cloud height. Aerosols, at low WV environments and under constant CTP, have less impact on CC than at high WV environments. Furthermore, AOD has a varying influence on COD depending on CTP. Finally, COD is found to increase with height for low and middle height clouds, and with increasing AOD, especially at low AOD. Our results demonstrate that the role of WV in the observed satellite-based aerosol - cloud relations is significant for all cloud heights.

  11. Fog and Cloud Induced Aerosol Modification Observed by AERONET

    NASA Technical Reports Server (NTRS)

    Eck, T. F.; Holben, B. N.; Reid, J. S.; Giles, D. M.; Rivas, M. A.; Singh, R. P.; Tripathi, S. N.; Bruegge, C. J.; Platnick, S. E.; Arnold, G. T.; Krotkov, N. A.; Carn, S. A.; Sinyuk, A.; Dubovik, O.; Arola, A.; Schafer, J. S.; Artaxo, P.; Smirnov, A.; Chen, H.; Goloub, P.

    2011-01-01

    Large fine mode (sub-micron radius) dominated aerosols in size distributions retrieved from AERONET have been observed after fog or low-altitude cloud dissipation events. These column-integrated size distributions have been obtained at several sites in many regions of the world, typically after evaporation of low altitude cloud such as stratocumulus or fog. Retrievals with cloud processed aerosol are sometimes bimodal in the accumulation mode with the larger size mode often approx.0.4 - 0.5 microns radius (volume distribution); the smaller mode typically approx.0.12 to aprrox.0.20 microns may be interstitial aerosol that were not modified by incorporation in droplets and/or aerosol that are less hygroscopic in nature. Bimodal accumulation mode size distributions have often been observed from in situ measurements of aerosols that have interacted with clouds, and AERONET size distribution retrievals made after dissipation of cloud or fog are in good agreement with particle sizes measured by in situ techniques for cloud-processed aerosols. Aerosols of this type and large size range (in lower concentrations) may also be formed by cloud processing in partly cloudy conditions and may contribute to the shoulder of larger size particles in the accumulation mode retrievals, especially in regions where sulfate and other soluble aerosol are a significant component of the total aerosol composition. Observed trends of increasing aerosol optical depth (AOD) as fine mode radius increased suggests higher AOD in the near cloud environment and therefore greater aerosol direct radiative forcing than typically obtained from remote sensing, due to bias towards sampling at low cloud fraction.

  12. Collocated observations of cloud condensation nuclei, particle size distributions, and chemical composition.

    PubMed

    Schmale, Julia; Henning, Silvia; Henzing, Bas; Keskinen, Helmi; Sellegri, Karine; Ovadnevaite, Jurgita; Bougiatioti, Aikaterini; Kalivitis, Nikos; Stavroulas, Iasonas; Jefferson, Anne; Park, Minsu; Schlag, Patrick; Kristensson, Adam; Iwamoto, Yoko; Pringle, Kirsty; Reddington, Carly; Aalto, Pasi; Äijälä, Mikko; Baltensperger, Urs; Bialek, Jakub; Birmili, Wolfram; Bukowiecki, Nicolas; Ehn, Mikael; Fjæraa, Ann Mari; Fiebig, Markus; Frank, Göran; Fröhlich, Roman; Frumau, Arnoud; Furuya, Masaki; Hammer, Emanuel; Heikkinen, Liine; Herrmann, Erik; Holzinger, Rupert; Hyono, Hiroyuki; Kanakidou, Maria; Kiendler-Scharr, Astrid; Kinouchi, Kento; Kos, Gerard; Kulmala, Markku; Mihalopoulos, Nikolaos; Motos, Ghislain; Nenes, Athanasios; O'Dowd, Colin; Paramonov, Mikhail; Petäjä, Tuukka; Picard, David; Poulain, Laurent; Prévôt, André Stephan Henry; Slowik, Jay; Sonntag, Andre; Swietlicki, Erik; Svenningsson, Birgitta; Tsurumaru, Hiroshi; Wiedensohler, Alfred; Wittbom, Cerina; Ogren, John A; Matsuki, Atsushi; Yum, Seong Soo; Myhre, Cathrine Lund; Carslaw, Ken; Stratmann, Frank; Gysel, Martin

    2017-03-14

    Cloud condensation nuclei (CCN) number concentrations alongside with submicrometer particle number size distributions and particle chemical composition have been measured at atmospheric observatories of the Aerosols, Clouds, and Trace gases Research InfraStructure (ACTRIS) as well as other international sites over multiple years. Here, harmonized data records from 11 observatories are summarized, spanning 98,677 instrument hours for CCN data, 157,880 for particle number size distributions, and 70,817 for chemical composition data. The observatories represent nine different environments, e.g., Arctic, Atlantic, Pacific and Mediterranean maritime, boreal forest, or high alpine atmospheric conditions. This is a unique collection of aerosol particle properties most relevant for studying aerosol-cloud interactions which constitute the largest uncertainty in anthropogenic radiative forcing of the climate. The dataset is appropriate for comprehensive aerosol characterization (e.g., closure studies of CCN), model-measurement intercomparison and satellite retrieval method evaluation, among others. Data have been acquired and processed following international recommendations for quality assurance and have undergone multiple stages of quality assessment.

  13. Collocated observations of cloud condensation nuclei, particle size distributions, and chemical composition

    PubMed Central

    Schmale, Julia; Henning, Silvia; Henzing, Bas; Keskinen, Helmi; Sellegri, Karine; Ovadnevaite, Jurgita; Bougiatioti, Aikaterini; Kalivitis, Nikos; Stavroulas, Iasonas; Jefferson, Anne; Park, Minsu; Schlag, Patrick; Kristensson, Adam; Iwamoto, Yoko; Pringle, Kirsty; Reddington, Carly; Aalto, Pasi; Äijälä, Mikko; Baltensperger, Urs; Bialek, Jakub; Birmili, Wolfram; Bukowiecki, Nicolas; Ehn, Mikael; Fjæraa, Ann Mari; Fiebig, Markus; Frank, Göran; Fröhlich, Roman; Frumau, Arnoud; Furuya, Masaki; Hammer, Emanuel; Heikkinen, Liine; Herrmann, Erik; Holzinger, Rupert; Hyono, Hiroyuki; Kanakidou, Maria; Kiendler-Scharr, Astrid; Kinouchi, Kento; Kos, Gerard; Kulmala, Markku; Mihalopoulos, Nikolaos; Motos, Ghislain; Nenes, Athanasios; O’Dowd, Colin; Paramonov, Mikhail; Petäjä, Tuukka; Picard, David; Poulain, Laurent; Prévôt, André Stephan Henry; Slowik, Jay; Sonntag, Andre; Swietlicki, Erik; Svenningsson, Birgitta; Tsurumaru, Hiroshi; Wiedensohler, Alfred; Wittbom, Cerina; Ogren, John A.; Matsuki, Atsushi; Yum, Seong Soo; Myhre, Cathrine Lund; Carslaw, Ken; Stratmann, Frank; Gysel, Martin

    2017-01-01

    Cloud condensation nuclei (CCN) number concentrations alongside with submicrometer particle number size distributions and particle chemical composition have been measured at atmospheric observatories of the Aerosols, Clouds, and Trace gases Research InfraStructure (ACTRIS) as well as other international sites over multiple years. Here, harmonized data records from 11 observatories are summarized, spanning 98,677 instrument hours for CCN data, 157,880 for particle number size distributions, and 70,817 for chemical composition data. The observatories represent nine different environments, e.g., Arctic, Atlantic, Pacific and Mediterranean maritime, boreal forest, or high alpine atmospheric conditions. This is a unique collection of aerosol particle properties most relevant for studying aerosol-cloud interactions which constitute the largest uncertainty in anthropogenic radiative forcing of the climate. The dataset is appropriate for comprehensive aerosol characterization (e.g., closure studies of CCN), model-measurement intercomparison and satellite retrieval method evaluation, among others. Data have been acquired and processed following international recommendations for quality assurance and have undergone multiple stages of quality assessment. PMID:28291234

  14. Physical and Optical/Radiative Characteristics of Aerosol and Cloud Particles in Tropical Cirrus: Importance in Radiation Balance

    NASA Technical Reports Server (NTRS)

    Pueschel, R. F.; Howard, S. D.; Foster, T. C.; Hallett, J.; Arnott, W. P.; Condon, Estelle P. (Technical Monitor)

    1996-01-01

    Whether cirrus clouds heat or cool the Earth-atmosphere system depends on the relative importance of the cloud shortwave albedo effect and the cloud thermal greenhouse effect. Both are determined by the distribution of ice condensate with cloud particle size. The microphysics instrument package flown aboard the NASA DC-8 in TOGA/COARE included an ice crystal replicator, a 2D Greyscale Cloud Particle Probe and a Forward Scattering Spectrometer Aerosol Probe. In combination, the electro-optical instruments permitted particle size measurements between 0.5 micrometer and 2.6 millimeter diameter. Ice crystal replicas were used to validate signals from the electrooptical instruments. Both optical and scanning electron microscopy were utilized to analyze aerosol and ice particle replicas between 0.1 micrometer and several 100 micrometer diameter. In first approximation, the combined aerosol-cloud particle spectrum in several clouds followed a power law N alpha D(sup -2.5). Thus, large cloud particles carried most of the condensate mass, while small cloud and aerosol particles determined the surface area. The mechanism of formation of small particles is growth of (hygroscopic, possibly ocean-derived) aerosol particles along the Kohler curves. The concentration of small particles is higher and less variable in space and time, and their tropospheric residence time is longer, than those of large cloud particles because of lower sedimentation velocities. Small particles shift effective cloud particle radii to sizes much smaller than the mean diameter of the cloud particles. This causes an increase in shortwave reflectivity and IR emissivity, and a decrease in transmissivity. Occasionally, the cloud reflectivity increased with altitude (decreasing temperature) stronger than did cloud emissivity, yielding enhanced radiative cooling at higher altitudes. Thus, cirrus produced by deep convection in the tropics may be critical in controlling processes whereby energy from warm

  15. Aerosol Impacts on Microphysical and Radiative Properties of Stratocumulus Clouds in the Southeast Pacific

    NASA Astrophysics Data System (ADS)

    Twohy, C. H.; Toohey, D. W.; Andrejczuk, M.; Anderson, J. R.; Adams, A.; Lytle, M.; George, R.; Wood, R.; Zuidema, P.; Leon, D.

    2011-12-01

    The southeast Pacific Ocean is covered by the world's largest stratocumulus cloud layer, which has a strong impact on ocean temperatures and climate in the region. The effect of anthropogenic sources of aerosol particles was investigated during the VOCALS field experiment. Aerosol measurements below and above cloud were made with a ultra-high sensitivity aerosol spectrometer and analytical electron microscopy. In addition to more standard in-cloud measurements, cloud droplets were collected and evaporated using a counterflow virtual impactor (CVI), and the non-volatile residual particles were analyzed. Many flights focused on the gradient in cloud properties along an E-W track from near the Chilean coast to remote areas offshore. Mean statistics from seven flights were compiled. Consistent with a continental source of cloud condensation nuclei, below-cloud accumulation-mode aerosol and droplet number concentration generally decreased from near shore to offshore. The effect extends ~800 to 1000 km from shore. The additional particles are mainly sulfates from anthropogenic sources. Liquid water content and drizzle concentration tended to increase with distance from shore, but exhibited much greater variability. Analysis of the droplet residual measurements showed that not only were there more residual nuclei near shore, but that they tended to be larger than those offshore. Single particle analysis over a broad particle size range was used to reveal types and sources of CCN, which were primarily sulfates near shore. Differences in the size distribution of droplet residual particles and ambient aerosol particles were observed due to the preferential activation of large aerosol particles. By progressively excluding small droplets from the CVI sample, we were able to show that the larger drops, which initiate drizzle, contain the largest aerosol particles. However, the scavenging efficiency is not sharp as expected from a simple parcel activation model. A wide range of

  16. The role of organic compounds in cloud formation: Relative importance of entrainment, co-condensation and particle-phase properties

    NASA Astrophysics Data System (ADS)

    Lowe, Samuel; Partridge, Daniel; Topping, David; Riipinen, Ilona

    2016-04-01

    The organic fraction of atmospheric aerosols is widely acknowledged to affect the cloud nucleating potential of aerosols. Cloud droplet formation through activation of non-volatile CCN is considered to be relatively well understood, however, there are fewer systematic studies on the activation of aerosols containing semi-volatile organic compounds that co-condense alongside water vapour, thus enhancing CCN activity. Although the significance of co-condensation of organic vapours for cloud droplet number concentration predictions has recently been identified, it remains uncertain how this process may interact with atmospheric dynamics. In addition to co-condensation of existing in-cloud material, additional semi-volatile mass can be entrained from the surrounding environment. Reduced cloud droplet number concentrations are expected as the parcel is diluted with clean air; however, additional soluble mass in the particle phase promotes droplet activation. The extent of increased droplet activation due to co-condensation relies also on the physiochemical properties of the organic compounds, as seen in several other phase partitioning sensitivity studies. In this work we study the simultaneous impact of entrainment and co-condensation, the relative importance of these two processes at different atmospheric conditions, their interactions with each other, and the particle-phase chemistry in terms of cloud microphysical properties and their parametric sensitivities. To assess the importance of the entrainment of semi-volatile materials as compared with their co-condensation and chemical properties, a pseudo-adiabatic cloud parcel model with a detailed description of bin microphysics is employed. We have added the co-condensation process to the model such that it is coupled with the parametric entrainment representation. The effects of entrainment and co-condensation are benchmarked independently and simultaneously against a control simulation. Furthermore, we probe the

  17. New approaches to quantifying aerosol influence on the cloud radiative effect

    PubMed Central

    Feingold, Graham; McComiskey, Allison; Yamaguchi, Takanobu; Johnson, Jill S.; Carslaw, Kenneth S.; Schmidt, K. Sebastian

    2016-01-01

    The topic of cloud radiative forcing associated with the atmospheric aerosol has been the focus of intense scrutiny for decades. The enormity of the problem is reflected in the need to understand aspects such as aerosol composition, optical properties, cloud condensation, and ice nucleation potential, along with the global distribution of these properties, controlled by emissions, transport, transformation, and sinks. Equally daunting is that clouds themselves are complex, turbulent, microphysical entities and, by their very nature, ephemeral and hard to predict. Atmospheric general circulation models represent aerosol−cloud interactions at ever-increasing levels of detail, but these models lack the resolution to represent clouds and aerosol−cloud interactions adequately. There is a dearth of observational constraints on aerosol−cloud interactions. We develop a conceptual approach to systematically constrain the aerosol−cloud radiative effect in shallow clouds through a combination of routine process modeling and satellite and surface-based shortwave radiation measurements. We heed the call to merge Darwinian and Newtonian strategies by balancing microphysical detail with scaling and emergent properties of the aerosol−cloud radiation system. PMID:26831092

  18. CHASER: An Innovative Satellite Mission Concept to Measure the Effects of Aerosols on Clouds and Climate

    NASA Astrophysics Data System (ADS)

    Renno, N.; Williams, E.; Rosenfeld, D.; Fischer, D.; Fischer, J.; Kremic, T.; Agrawal, A.; Andreae, M.; Bierbaum, R.; Blakeslee, R.; Boerner, A.; Bowles, N.; Christian, H.; Dunion, J.; Horvath, A.; Huang, X.; Khain, A.; Kinne, S.; Lemos, M.-C.; Penner, J.

    2012-04-01

    The formation of cloud droplets on aerosol particles, technically known as the activation of cloud condensation nuclei (CCN), is the fundamental process driving the interactions of aerosols with clouds and precipitation. Knowledge of these interactions is foundational to our understanding of weather and climate. The Intergovernmental Panel on Climate Change (IPCC) and the Decadal Survey (NRC 2007) indicate that the uncertainty in how clouds adjust to aerosol perturbations dominates the uncertainty in the overall quantification of the radiative forcing attributable to human activities. The Clouds, Hazards, and Aerosols Survey for Earth Researchers (CHASER) mission concept responds to the IPCC and Decadal Survey concerns by studying the activation of CCN and their interactions with clouds and storms. CHASER proposes to revolutionize our understanding of the interactions of aerosols with clouds by making the first global measurements of the fundamental physical entity linking them: activated cloud condensation nuclei. The CHASER mission was conceptualized to measure all quantities necessary for determining the interactions of aerosols with clouds and storms. Measurements by current satellites allow the determination of crude profiles of cloud particle size but not of the activated CCN that seed them. CHASER uses a new technique (Freud et al. 2011; Rosenfeld et al. 2012) and high-heritage instruments to produce the first global maps of activated CCN and the properties of the clouds associated with them. CHASER measures the CCN concentration and cloud thermodynamic forcing simultaneously, allowing their effects to be distinguished. Changes in the behavior of a group of weather systems in which only one of the quantities varies (a partial derivative of the intensity with the desirable quantity) allow the determination of each effect statistically. The high uncertainties of current climate predictions limit their much-needed use in decision-making. CHASER mitigates this

  19. Science Plan Biogenic Aerosols – Effects on Clouds and Climate (BAECC)

    SciTech Connect

    Petäjä, T

    2013-12-01

    Atmospheric aerosol particles impact human health in urban environments, while on regional and global scales they can affect climate patterns, the hydrological cycle, and the intensity of radiation that reaches the Earth’s surface. In spite of recent advances in the understanding of aerosol formation processes and the links between aerosol dynamics and biosphere-atmosphere-climate interactions, great challenges remain in the analysis of related processes on a global scale. Boreal forests, situated in a circumpolar belt in the northern latitudes throughout the United States, Canada, Russia and Scandinavia, are among the most active areas of atmospheric aerosol formation among all biomes. The formation of aerosol particles and their growth to the sizes of cloud condensation nuclei in these areas are associated with biogenic volatile organic emissions from vegetation and soil.

  20. Primary marine aerosol-cloud interactions off the coast of California

    NASA Astrophysics Data System (ADS)

    Modini, R. L.; Frossard, A. A.; Ahlm, L.; Russell, L. M.; Corrigan, C. E.; Roberts, G. C.; Hawkins, L. N.; Schroder, J. C.; Bertram, A. K.; Zhao, R.; Lee, A. K. Y.; Abbatt, J. P. D.; Lin, J.; Nenes, A.; Wang, Z.; Wonaschütz, A.; Sorooshian, A.; Noone, K. J.; Jonsson, H.; Seinfeld, J. H.; Toom-Sauntry, D.; MacDonald, A. M.; Leaitch, W. R.

    2015-05-01

    Primary marine aerosol (PMA)-cloud interactions off the coast of California were investigated using observations of marine aerosol, cloud condensation nuclei (CCN), and stratocumulus clouds during the Eastern Pacific Emitted Aerosol Cloud Experiment (E-PEACE) and the Stratocumulus Observations of Los-Angeles Emissions Derived Aerosol-Droplets (SOLEDAD) studies. Based on recently reported measurements of PMA size distributions, a constrained lognormal-mode-fitting procedure was devised to isolate PMA number size distributions from total aerosol size distributions and applied to E-PEACE measurements. During the 12 day E-PEACE cruise on the R/V Point Sur, PMA typically contributed less than 15% of total particle concentrations. PMA number concentrations averaged 12 cm-3 during a relatively calmer period (average wind speed 12 m/s1) lasting 8 days, and 71 cm-3 during a period of higher wind speeds (average 16 m/s1) lasting 5 days. On average, PMA contributed less than 10% of total CCN at supersaturations up to 0.9% during the calmer period; however, during the higher wind speed period, PMA comprised 5-63% of CCN (average 16-28%) at supersaturations less than 0.3%. Sea salt was measured directly in the dried residuals of cloud droplets during the SOLEDAD study. The mass fractions of sea salt in the residuals averaged 12 to 24% during three cloud events. Comparing the marine stratocumulus clouds sampled in the two campaigns, measured peak supersaturations were 0.2 ± 0.04% during E-PEACE and 0.05-0.1% during SOLEDAD. The available measurements show that cloud droplet number concentrations increased with >100 nm particles in E-PEACE but decreased in the three SOLEDAD cloud events.

  1. Process-model Simulations of Cloud Albedo Enhancement by Aerosols in the Arctic

    SciTech Connect

    Kravitz, Benjamin S.; Wang, Hailong; Rasch, Philip J.; Morrison, H.; Solomon, Amy

    2014-11-17

    A cloud-resolving model is used to simulate the effectiveness of Arctic marine cloud brightening via injection of cloud condensation nuclei (CCN). An updated cloud microphysical scheme is employed, with prognostic CCN and cloud particle numbers in both liquid and mixed-phase marine low clouds. Injection of CCN into the marine boundary layer can delay the collapse of the boundary layer and increase low-cloud albedo. Because nearly all of the albedo effects are in the liquid phase due to the removal of ice water by snowfall when ice processes are involved, albedo increases are stronger for pure liquid clouds than mixed-phase clouds. Liquid precipitation can be suppressed by CCN injection, whereas ice precipitation (snow) is affected less; thus the effectiveness of brightening mixed-phase clouds is lower than for liquid-only clouds. CCN injection into a clean regime results in a greater albedo increase than injection into a polluted regime, consistent with current knowledge about aerosol-cloud interactions. Unlike previous studies investigating warm clouds, dynamical changes in circulation due to precipitation changes are small.

  2. Process-model simulations of cloud albedo enhancement by aerosols in the Arctic

    PubMed Central

    Kravitz, Ben; Wang, Hailong; Rasch, Philip J.; Morrison, Hugh; Solomon, Amy B.

    2014-01-01

    A cloud-resolving model is used to simulate the effectiveness of Arctic marine cloud brightening via injection of cloud condensation nuclei (CCN), either through geoengineering or other increased sources of Arctic aerosols. An updated cloud microphysical scheme is employed, with prognostic CCN and cloud particle numbers in both liquid and mixed-phase marine low clouds. Injection of CCN into the marine boundary layer can delay the collapse of the boundary layer and increase low-cloud albedo. Albedo increases are stronger for pure liquid clouds than mixed-phase clouds. Liquid precipitation can be suppressed by CCN injection, whereas ice precipitation (snow) is affected less; thus, the effectiveness of brightening mixed-phase clouds is lower than for liquid-only clouds. CCN injection into a clean regime results in a greater albedo increase than injection into a polluted regime, consistent with current knowledge about aerosol–cloud interactions. Unlike previous studies investigating warm clouds, dynamical changes in circulation owing to precipitation changes are small. According to these results, which are dependent upon the representation of ice nucleation processes in the employed microphysical scheme, Arctic geoengineering is unlikely to be effective as the sole means of altering the global radiation budget but could have substantial local radiative effects. PMID:25404677

  3. A Simple Model for the Cloud Adjacency Effect and the Apparent Bluing of Aerosols Near Clouds

    NASA Technical Reports Server (NTRS)

    Marshak, Alexander; Wen, Guoyong; Coakley, James A., Jr.; Remer, Lorraine A.; Loeb,Norman G.; Cahalan, Robert F.

    2008-01-01

    In determining aerosol-cloud interactions, the properties of aerosols must be characterized in the vicinity of clouds. Numerous studies based on satellite observations have reported that aerosol optical depths increase with increasing cloud cover. Part of the increase comes from the humidification and consequent growth of aerosol particles in the moist cloud environment, but part comes from 3D cloud-radiative transfer effects on the retrieved aerosol properties. Often, discerning whether the observed increases in aerosol optical depths are artifacts or real proves difficult. The paper provides a simple model that quantifies the enhanced illumination of cloud-free columns in the vicinity of clouds that are used in the aerosol retrievals. This model is based on the assumption that the enhancement in the cloud-free column radiance comes from enhanced Rayleigh scattering that results from the presence of the nearby clouds. The enhancement in Rayleigh scattering is estimated using a stochastic cloud model to obtain the radiative flux reflected by broken clouds and comparing this flux with that obtained with the molecules in the atmosphere causing extinction, but no scattering.

  4. A numerical study of the effect of different aerosol types on East Asian summer clouds and precipitation

    SciTech Connect

    Jiang, Yiquan; Liu, Xiaohong; Yang, Xiuqun; Wang, Minghuai

    2013-05-01

    The impact of anthropogenic aerosol on the East Asian summer monsoon (EASM) is investigated with NCAR CAM5, a state-of-the-art climate model with aerosol’s direct and indirect effects. Results indicate that anthropogenic aerosol tends to cause a weakened EASM with a southward shift of precipitation in East Asia mostly by its radiative effect. Anthropogenic aerosol induced surface cooling stabilizes the boundary layer, suppresses the convection and latent heat release in northern China, and reduces the tropospheric temperature over land and land-sea thermal contrast, thus leading to a weakened EASM. Meanwhile, acting as cloud condensation nuclei (CCN), anthropogenic aerosol can significantly increase the cloud droplet number concentration but decrease the cloud droplet effective radius over Indochina and Indian Peninsulas as well as over southwestern and northern China, inhibiting the precipitation in these regions. Thus, anthropogenic aerosol tends to reduce Southeast and South Asian summer monsoon precipitation by its indirect effect.

  5. Characteristics-based sectional modeling of aerosol nucleation and condensation

    NASA Astrophysics Data System (ADS)

    Frederix, E. M. A.; Stanic, M.; Kuczaj, A. K.; Nordlund, M.; Geurts, B. J.

    2016-12-01

    A new numerical method for the solution of an internally mixed spatially homogeneous sectional model for aerosol nucleation and condensation is proposed. The characteristics method is used to predict droplet sizes within a discrete time step. The method is designed such that 1) a pre-specified number of moments of the droplet size distribution may be preserved, 2) there exists no time step stability restriction related to the condensation rate and section size, 3) highly skewed fixed sectional distributions may be used and 4) it is straightforward to extend to spatially inhomogeneous settings and to incorporate droplet coagulation and break-up. We derive, starting from mass conservation, a consistent internally mixed multi-species aerosol model. For certain condensational growth laws analytical solutions exist, against which the method is validated. Using two-moment and four-moment-preserving schemes, we find first order convergence of the numerical solution to the analytical result, as a function of the number of sections. As the four-moment-preserving scheme does not guarantee positivity of the solution, a hybrid scheme is proposed, which, when needed, locally reverts back to two-moment preservation, to prevent negativity. As an illustration, the method is applied to a complete multi-species homogeneous nucleation and condensation problem.

  6. Clouds Aerosols Internal Affaires: Increasing Cloud Fraction and Enhancing the Convection

    NASA Technical Reports Server (NTRS)

    Koren, Ilan; Kaufman, Yoram; Remer, Lorraine; Rosenfeld, Danny; Rudich, Yinon

    2004-01-01

    Clouds developing in a polluted environment have more numerous, smaller cloud droplets that can increase the cloud lifetime and liquid water content. Such changes in the cloud droplet properties may suppress low precipitation allowing development of a stronger convection and higher freezing level. Delaying the washout of the cloud water (and aerosol), and the stronger convection will result in higher clouds with longer life time and larger anvils. We show these effects by using large statistics of the new, 1km resolution data from MODIS on the Terra satellite. We isolate the aerosol effects from meteorology by regression and showing that aerosol microphysical effects increases cloud fraction by average of 30 presents for all cloud types and increases convective cloud top pressure by average of 35mb. We analyze the aerosol cloud interaction separately for high pressure trade wind cloud systems and separately for deep convective cloud systems. The resultant aerosol radiative effect on climate for the high pressure cloud system is: -10 to -13 W/sq m at the top of the atmosphere (TOA) and -11 to -14 W/sq m at the surface. For deeper convective clouds the forcing is: -4 to -5 W/sq m at the TOA and -6 to -7 W/sq m at the surface.

  7. HCl in rocket exhaust clouds - Atmospheric dispersion, acid aerosol characteristics, and acid rain deposition

    NASA Technical Reports Server (NTRS)

    Pellett, G. L.; Sebacher, D. I.; Bendura, R. J.; Wornom, D. E.

    1983-01-01

    Both measurements and model calculations of the temporal dispersion of peak HCl (g + aq) concentration in Titan III exhaust clouds are found to be well characterized by one-term power-law decay expressions. The respective coefficients and decay exponents, however, are found to vary widely with meteorology. The HCl (g), HCl (g + aq), dewpoint, and temperature-pressure-altitude data for Titan III exhaust clouds are consistent with accurately calculated HCl/H2O vapor-liquid compositions for a model quasi-equilibrated flat surface aqueous aerosol. Some cloud evolution characteristics are also defined. Rapid and extensive condensation of aqueous acid clearly occurs during the first three min of cloud rise. Condensation is found to be intensified by the initial entrainment of relatively moist ambient air from lower levels, that is, from levels below eventual cloud stabilization. It is pointed out that if subsequent dilution air at stabilization altitude is significantly drier, a state of maximum condensation soon occurs, followed by an aerosol evaporation phase.

  8. Aerosol Indirect Forcing Dictated by Warm Low-Cloud

    NASA Astrophysics Data System (ADS)

    Christensen, M.; Chen, Y. C.; Stephens, G. L.

    2014-12-01

    Aerosol indirect forcing is one of the largest sources of uncertainty in estimating the extent of global warming. Increased aerosol levels can enhance the solar reflection from warm liquid clouds countering greenhouse gas warming. However, very little is actually known about the strength of the indirect effects for mixed-phase stratiform clouds as well as other cloud types such as cumulus, altocumulus, nimbostratus, deep convection, and cirrus. These mixed-phase cloud types are ubiquitous and typically overlooked in satellite estimates of the indirect forcing. In this study we assess the responses of each major cloud type to changes in aerosol loading and provide an estimate of their contribution to the global mean indirect forcing. Satellite data is collected from several co-located sensors in the A-train for the period starting in January of 2007 - 2010. Cloud layers are classified according to the 2B-CLDCLASS-LIDAR CloudSat product. Radiative fluxes are obtained from CERES (Clouds and the Earth's Radiant Energy System) and examined as a function of the aerosol loading obtained from MODIS (MODerate resolution Imaging Spectroradiometer) data. For low-level cloud regimes (e.g., stratus, stratocumulus, cumulus) we show that the longwave contribution to the net indirect effect is insignificant and dominated by changes in reflected shortwave radiation which also becomes insignificant as cloud top temperature decreases below 0°C. An increase in the aerosol loading in mixed-phase stratocumulus leads to more ice and precipitation that depletes cloud water and limits cloud brightening. For the more convective type clouds (e.g., altocumulus, nimbostratus, deep convection), increased aerosol loading can invigorate deep convection and promote deeper clouds with higher cloud albedo (cooling effect) and cloud tops that emit less longwave radiation to space (warming effect). As a consequence, the shortwave and longwave indirect radiative effects tend to cancel for the

  9. Evaluating aerosol indirect effect through marine stratocumulus clouds

    SciTech Connect

    Kogan, Z.N.; Kogan, Y.L.; Lilly, D.K.

    1996-04-01

    During the last decade much attention has been focused on anthropogenic aerosols and their radiative influence on the global climate. Charlson et al. and Penner et al. have demonstrated that tropospheric aerosols and particularly anthropogenic sulfate aerosols may significantly contribute to the radiative forcing exerting a cooling influence on climate (-1 to -2 W/m{sup 2}) which is comparable in magnitude to greenhouse forcing, but opposite in sign. Aerosol particles affect the earth`s radiative budget either directly by scattering and absorption of solar radiation by themselves or indirectly by altering the cloud radiative properties through changes in cloud microstructure. Marine stratocumulus cloud layers and their possible cooling influence on the atmosphere as a result of pollution are of special interest because of their high reflectivity, durability, and large global cover. We present an estimate of thet aerosol indirect effect, or, forcing due to anthropogenic sulfate aerosols.

  10. A Novel Tool for Simulating Aerosol-cloud Interactions with a Sectional Model Implemented to a Large-Eddy Simulator

    NASA Astrophysics Data System (ADS)

    Tonttila, J.; Romakkaniemi, S.; Kokkola, H.; Maalick, Z.; Korhonen, H.; Liqing, H.

    2015-12-01

    A new cloud-resolving model setup for studying aerosol-cloud interactions, with a special emphasis on partitioning and wet deposition of semi-volatile aerosol species, is presented. The model is based on modified versions of two well-established model components: the Large-Eddy Simulator (LES) UCLALES, and the sectional aerosol model SALSA, previously employed in the ECHAM climate model family. Implementation of the UCLALES-SALSA is described in detail. As the basis for this work, SALSA has been extended to include a sectional representation of the size distributions of cloud droplets and precipitation. Microphysical processes operating on clouds and precipitation have also been added. Given our main motivation, the cloud droplet size bins are defined according to the dry particle diameter. The droplet wet diameter is solved dynamically through condensation equations, but represents an average droplet diameter inside each size bin. This approach allows for accurate tracking of the aerosol properties inside clouds, but minimizes the computational cost. Since the actual cloud droplet diameter is not fully resolved inside the size bins, processes such as precipitation formation rely on parameterizations. For realistic growth of drizzle drops to rain, which is critical for the aerosol wet deposition, the precipitation size bins are defined according to the actual drop size. With these additions, the implementation of the SALSA model replaces most of the microphysical and thermodynamical components within the LES. The cloud properties and aerosol-cloud interactions simulated by the model are analysed and evaluated against detailed cloud microphysical boxmodel results and in-situ aerosol-cloud interaction observations from the Puijo measurement station in Kuopio, Finland. The ability of the model to reproduce the impacts of wet deposition on the aerosol population is demonstrated.

  11. Challenges in constraining anthropogenic aerosol effects on cloud radiative forcing using present-day spatiotemporal variability

    PubMed Central

    Ghan, Steven; Wang, Minghuai; Zhang, Shipeng; Ferrachat, Sylvaine; Gettelman, Andrew; Griesfeller, Jan; Kipling, Zak; Lohmann, Ulrike; Morrison, Hugh; Neubauer, David; Partridge, Daniel G.; Stier, Philip; Takemura, Toshihiko; Wang, Hailong; Zhang, Kai

    2016-01-01

    A large number of processes are involved in the chain from emissions of aerosol precursor gases and primary particles to impacts on cloud radiative forcing. Those processes are manifest in a number of relationships that can be expressed as factors dlnX/dlnY driving aerosol effects on cloud radiative forcing. These factors include the relationships between cloud condensation nuclei (CCN) concentration and emissions, droplet number and CCN concentration, cloud fraction and droplet number, cloud optical depth and droplet number, and cloud radiative forcing and cloud optical depth. The relationship between cloud optical depth and droplet number can be further decomposed into the sum of two terms involving the relationship of droplet effective radius and cloud liquid water path with droplet number. These relationships can be constrained using observations of recent spatial and temporal variability of these quantities. However, we are most interested in the radiative forcing since the preindustrial era. Because few relevant measurements are available from that era, relationships from recent variability have been assumed to be applicable to the preindustrial to present-day change. Our analysis of Aerosol Comparisons between Observations and Models (AeroCom) model simulations suggests that estimates of relationships from recent variability are poor constraints on relationships from anthropogenic change for some terms, with even the sign of some relationships differing in many regions. Proxies connecting recent spatial/temporal variability to anthropogenic change, or sustained measurements in regions where emissions have changed, are needed to constrain estimates of anthropogenic aerosol impacts on cloud radiative forcing. PMID:26921324

  12. Effects of Aerosol Pollution on Clouds over Megacities

    NASA Astrophysics Data System (ADS)

    Sechrist, B.; Jacobson, M. Z.

    2013-12-01

    The correlation between aerosol optical depth (AOD) and cloud properties - principally cloud fraction and cloud optical depth (COD) - is examined using satellite retrievals from the MODIS satellites over Los Angeles and Beijing. Ten Hoeve et al. (2011, Atmos. Chem. Phys, 11(7), 3021-3036) used satellite data to examine the impact of aerosols on warm clouds around Rondonia, Brazil, during the biomass burning season. They found that the COD-AOD relationship exhibits a 'boomerang' shape in which COD initially increases with increasing AOD but then decreases as AOD continues to increase beyond some critical level. This result is thought to reflect the balance between the microphysical and radiative components of a cloud's response to aerosols. The microphysical process dominates at low AOD, while the radiative process dominates at high AOD. This study is analogous to Ten Hoeve et al., but for aerosols derived primarily from fossil fuel combustion rather than biomass burning. Preliminary results will be presented.

  13. Interpretation of FRESCO cloud retrievals in case of absorbing aerosol events

    NASA Astrophysics Data System (ADS)

    Wang, P.; Tuinder, O. N. E.; Tilstra, L. G.; de Graaf, M.; Stammes, P.

    2012-10-01

    Cloud and aerosol information is needed in trace gas retrievals from satellite measurements. The Fast REtrieval Scheme for Clouds from the Oxygen A band (FRESCO) cloud algorithm employs reflectance spectra of the O2 A band around 760 nm to derive cloud pressure and effective cloud fraction. In general, clouds contribute more to the O2 A band reflectance than aerosols. Therefore, the FRESCO algorithm does not correct for aerosol effects in the retrievals and attributes the retrieved cloud information entirely to the presence of clouds, and not to aerosols. For events with high aerosol loading, aerosols may have a dominant effect, especially for almost cloud free scenes. We have analysed FRESCO cloud data and Absorbing Aerosol Index (AAI) data from the Global Ozone Monitoring Experiment (GOME-2) instrument on the Metop-A satellite for events with typical absorbing aerosol types, such as volcanic ash, desert dust and smoke. We find that the FRESCO effective cloud fractions are correlated with the AAI data for these absorbing aerosol events and that the FRESCO cloud pressure contains information on aerosol layer pressure. For cloud free scenes, the derived FRESCO cloud pressure is close to the aerosol layer pressure, especially for optically thick aerosol layers. For cloudy scenes, if the strongly absorbing aerosols are located above the clouds, then the retrieved FRESCO cloud pressure may represent the height of the aerosol layer rather than the height of the clouds. Combining FRESCO and AAI data, an estimate for the aerosol layer pressure can be given.

  14. Representing Cloud Processing of Aerosol in Numerical Models

    SciTech Connect

    Mechem, D.B.; Kogan, Y.L.

    2005-03-18

    The satellite imagery in Figure 1 provides dramatic examples of how aerosol influences the cloud field. Aerosol from ship exhaust can serve as nucleation centers in otherwise cloud-free regions, forming ship tracks (top image), or can enhance the reflectance/albedo in already cloudy regions. This image is a demonstration of the first indirect effect, in which changes in aerosol modulate cloud droplet radius and concentration, which influences albedo. It is thought that, through the effects it has on precipitation (drizzle), aerosol can also affect the structure and persistence of planetary boundary layer (PBL) clouds. Regions of cellular convection, or open pockets of cloudiness (bottom image) are thought to be remnants of strongly drizzling PBL clouds. Pockets of Open Cloudiness (POCs) (Stevens et al. 2005) or Albrecht's ''rifts'' are low cloud fraction regions characterized by anomalously low aerosol concentrations, implying they result from precipitation. These features may in fact be a demonstration of the second indirect effect. To accurately represent these clouds in numerical models, we have to treat the coupled cloud-aerosol system. We present the following series of mesoscale and large eddy simulation (LES) experiments to evaluate the important aspects of treating the coupled cloud-aerosol problem. 1. Drizzling and nondrizzling simulations demonstrate the effect of drizzle on a mesoscale forecast off the California coast. 2. LES experiments with explicit (bin) microphysics gauge the relative importance of the shape of the aerosol spectrum on the 3D dynamics and cloud structure. 3. Idealized mesoscale model simulations evaluate the relative roles of various processes, sources, and sinks.

  15. Using OMI Observations to Measure Aerosol Absorption of Biomass Burning Aerosols Above Clouds

    NASA Technical Reports Server (NTRS)

    Torres, Omar; Bhartia, P. K.; Jethva, Hiren

    2011-01-01

    The presence of absorbing aerosol layers above clouds is unambiguously detected by the TOMS/OMI UV Aerosol Index (AI) that uses satellite observations at two near-UV channels. A sensitivity study using radiative transfer calculations shows that the AI signal of resulting from the presence of aerosols above clouds is mainly driven by the aerosol absorption optical depth and the optical depth of the underlying cloud. Based on these results, an inversion algorithm has been developed to retrieve the aerosol optical depth (AOD) of aerosol layers above clouds. In this presentation we will discuss the sensitivity analysis, describe the retrieval approach, and present results of applications of the retrieval method to OMI observations over the South Atlantic Ocean. Preliminary error analyses, to be discussed, indicate that the AOD can be underestimated (up to -30%) or overestimated (up to 60%) depending on algorithmic assumptions.

  16. Potential Impacts of Pollution Aerosol and Dust Acting As Cloud-Nucleating Aerosol on Precipitation in the Colorado River Basin

    NASA Astrophysics Data System (ADS)

    Jha, V.; Cotton, W. R.; Carrio, G. G.

    2014-12-01

    The southwest US has huge demands on water resources. The Colorado River Basin (CRB) is potentially affected by anthropogenic aerosol pollution and dust acting as cloud-nucleating aerosol as well as impacting snowpack albedo.The specific objective of this research is to quantify the impacts of both dust and pollution aerosols on wintertime precipitation in the Colorado Mountains for the years 2005-2006. We examine the combined effects of anthropogenic pollution aerosol and dust serving as cloud condensation nuclei (CCN), ice nuclei (IN) and giant CCN(GCCN) on precipitation in the CRB. Anthropogenic pollution can enhance droplet concentrations, and decrease collision and coalescence and ice particle riming largely via the "spillover" effect. Dust can serve as IN and enhance precipitation in wintertime orographic clouds. Dust coated with sulfates or originating over dry lake beds can serve as GCCN which when wetted can result in larger cloud droplets and thereby enhance the warm-rain collision and coalescence process and ice particle riming. But smaller dust particles coated with sulfates, can decrease collision and coalescence and ice particle riming similar to anthropogenic pollution aerosols. The Colorado State University (CSU) Regional Atmospheric Modeling System (RAMS) version 6.0 is used for this study. RAMS was modified to ingest GEOS-CHEM output data and periodically update aerosol fields. GEOS-CHEM is a chemical transport model which uses assimilated meteorological data from the NASA Goddard Earth Observation System (GEOS). The aerosol data comprise a sum of hydrophobic and hydrophilic black carbon and organic aerosol, hydrophilic SOAs, hydrocarbon oxidation and inorganic aerosols (nitrate, sulfate and ammonium). In addition, a RAMS-based dust source and transport model is used. Preliminary analysis suggests pollution dominates over dust resulting in a decrease in precipitation via the spillover effect. Dust serving as GCCN and IN tend to enhance ice

  17. Role of clouds, aerosols, and aerosol-cloud interaction in 20th century simulations with GISS ModelE2

    NASA Astrophysics Data System (ADS)

    Nazarenko, L.; Rind, D. H.; Bauer, S.; Del Genio, A. D.

    2015-12-01

    Simulations of aerosols, clouds and their interaction contribute to the major source of uncertainty in predicting the changing Earth's energy and in estimating future climate. Anthropogenic contribution of aerosols affects the properties of clouds through aerosol indirect effects. Three different versions of NASA GISS global climate model are presented for simulation of the twentieth century climate change. All versions have fully interactive tracers of aerosols and chemistry in both the troposphere and stratosphere. All chemical species are simulated prognostically consistent with atmospheric physics in the model and the emissions of short-lived precursors [Shindell et al., 2006]. One version does not include the aerosol indirect effect on clouds. The other two versions include a parameterization of the interactive first indirect aerosol effect on clouds following Menon et al. [2010]. One of these two models has the Multiconfiguration Aerosol Tracker of Mixing state (MATRIX) that permits detailed treatment of aerosol mixing state, size, and aerosol-cloud activation. The main purpose of this study is evaluation of aerosol-clouds interactions and feedbacks, as well as cloud and aerosol radiative forcings, for the twentieth century climate under different assumptions and parameterizations for aerosol, clouds and their interactions in the climate models. The change of global surface air temperature based on linear trend ranges from +0.8°C to +1.2°C between 1850 and 2012. Water cloud optical thickness increases with increasing temperature in all versions with the largest increase in models with interactive indirect effect of aerosols on clouds, which leads to the total (shortwave and longwave) cloud radiative cooling trend at the top of the atmosphere. Menon, S., D. Koch, G. Beig, S. Sahu, J. Fasullo, and D. Orlikowski (2010), Black carbon aerosols and the third polar ice cap, Atmos. Chem. Phys., 10,4559-4571, doi:10.5194/acp-10-4559-2010. Shindell, D., G. Faluvegi

  18. Cloud condensation nuclei characteristics of Asian dust particles over the western and central North Pacific

    NASA Astrophysics Data System (ADS)

    Uematsu, M.; Furutani, H.; Kawata, R.; Nakayama, H.

    2015-12-01

    Marine aerosols, such as sea salt particles, and sulfate and organic particles originated from marine biotas, exist in the marine atmosphere. Additionally, continental aerosols, such as dust and anthropogenic substances are transported over the open oceans. Variation of number concentration of cloud condensation nuclei (CCN) depends on the number-size distribution and chemical compositions of aerosols, and affects the lifetime and the reflectivity of clouds over the open oceans. During the R/V Hakuho Maru KH-12-1 cruise from Callao to Tokyo via Honolulu in the Pacific Ocean (23 January - 7 March 2012), aerosol number-size distribution and CCN number concentration were continuously measured, and the marine aerosols for chemical analysis were collected on shipboard. In the marine atmosphere over the Pacific, averaged aerosol total number concentration (TN) was 280 cm-3. Bimodal number-size distributions were observed frequently with peaks at 40-60 nm (Aitken mode) and 160-230 nm (accumulation mode). CCN concentrations were categorized by assuming three types of particles by chemical compositions (i.e., NaCl; a major component of sea salt particles, (NH4)2SO4; a sulfur oxide originated from the marine biotas, and Oxalic acid; a major component among organic carbon (OC) originated from the marine biotas). Activation Rate (AR), which is defined as the ratio of the number concentrations of CCN against TN, varied mainly because of the number-size distribution. Chemical composition was the factor that determined AR values. However, the AR variations caused by changes of the chemical composition were much smaller than those caused changes of the particle size distribution even when Asian dust were observed over the region on 27-29 February. During the long range transport, rapid coagulation among mineral dust, organics and sea salt particles may accelerate the gravitational setting of marine aerosols and supplies the terrestrial substances to the ocean environment.

  19. A Scientific Cloud Computing Platform for Condensed Matter Physics

    NASA Astrophysics Data System (ADS)

    Jorissen, K.; Johnson, W.; Vila, F. D.; Rehr, J. J.

    2013-03-01

    Scientific Cloud Computing (SCC) makes possible calculations with high performance computational tools, without the need to purchase or maintain sophisticated hardware and software. We have recently developed an interface dubbed SC2IT that controls on-demand virtual Linux clusters within the Amazon EC2 cloud platform. Using this interface we have developed a more advanced, user-friendly SCC Platform configured especially for condensed matter calculations. This platform contains a GUI, based on a new Java version of SC2IT, that permits calculations of various materials properties. The cloud platform includes Virtual Machines preconfigured for parallel calculations and several precompiled and optimized materials science codes for electronic structure and x-ray and electron spectroscopy. Consequently this SCC makes state-of-the-art condensed matter calculations easy to access for general users. Proof-of-principle performance benchmarks show excellent parallelization and communication performance. Supported by NSF grant OCI-1048052

  20. Influence of particle size and chemistry on the cloud nucleating properties of aerosols

    NASA Astrophysics Data System (ADS)

    Quinn, P. K.; Bates, T. S.; Coffman, D. J.; Covert, D. S.

    2008-02-01

    The ability of an aerosol particle to act as a cloud condensation nuclei (CCN) is a function of the size of the particle, its composition and mixing state, and the supersaturation of the cloud. In-situ data from field studies provide a means to assess the relative importance of these parameters. During the 2006 Texas Air Quality - Gulf of Mexico Atmospheric Composition and Climate Study (TexAQS-GoMACCS), the NOAA RV Ronald H. Brown encountered a wide variety of aerosol types ranging from marine near the Florida panhandle to urban and industrial in the Houston-Galveston area. These varied sources provided an opportunity to investigate the role of aerosol sources and chemistry in the potential activation of particles to form cloud droplets. Measurements were made of CCN concentrations, aerosol chemical composition in the size range relevant for particle activation in warm clouds, and aerosol size distributions. Variability in aerosol composition was parameterized by the mass fraction of Hydrocarbon-like Organic Aerosol (HOA) for particle diameters less than 200 nm (vacuum aerodynamic). The HOA mass fraction in this size range was lowest for marine aerosol and highest for aerosol sampled close to anthropogenic sources. Combining all data from the experiment reveals that composition (defined by HOA mass fraction) explains 40% of the variance in the critical diameter for particle activation at the instrumental supersaturation (S) of 0.44%. Correlations between HOA mass fraction and aerosol mean diameter show that these two parameters are essentially independent of one another for this data set. We conclude that, based on the variability of the HOA mass fraction observed during TexAQS-GoMACCS, variability in particle composition played a significant role in determining the fraction of particles that could activate to form cloud droplets. Using a simple model based on Köhler theory and the assumption that HOA is insoluble, we estimate the degree to which calculated CCN

  1. Impact of Aerosols on Convective Clouds and Precipitation

    NASA Technical Reports Server (NTRS)

    Tao, Wei-Kuo; Chen, Jen-Ping; Li, Zhanqing; Wang, Chien; Zhang, Chidong

    2012-01-01

    Aerosols are a critical factor in the atmospheric hydrological cycle and radiation budget. As a major agent for clouds to form and a significant attenuator of solar radiation, aerosols affect climate in several ways. Current research suggests that aerosol effects on clouds could further extend to precipitation, both through the formation of cloud particles and by exerting persistent radiative forcing on the climate system that disturbs dynamics. However, the various mechanisms behind these effects, in particular the ones connected to precipitation, are not yet well understood. The atmospheric and climate communities have long been working to gain a better grasp of these critical effects and hence to reduce the significant uncertainties in climate prediction resulting from such a lack of adequate knowledge. Here we review past efforts and summarize our current understanding of the effect of aerosols on convective precipitation processes from theoretical analysis of microphysics, observational evidence, and a range of numerical model simulations. In addition, the discrepancy between results simulated by models, as well as that between simulations and observations, are presented. Specifically, this paper addresses the following topics: (1) fundamental theories of aerosol effects on microphysics and precipitation processes, (2) observational evidence of the effect of aerosols on precipitation processes, (3) signatures of the aerosol impact on precipitation from largescale analyses, (4) results from cloud-resolving model simulations, and (5) results from large-scale numerical model simulations. Finally, several future research directions for gaining a better understanding of aerosol--cloud-precipitation interactions are suggested.

  2. Models to support active sensing of biological aerosol clouds

    NASA Astrophysics Data System (ADS)

    Brown, Andrea M.; Kalter, Jeffrey M.; Corson, Elizabeth C.; Chaudhry, Zahra; Boggs, Nathan T.; Brown, David M.; Thomas, Michael E.; Carter, Christopher C.

    2013-05-01

    Elastic backscatter LIght Detection And Ranging (LIDAR) is a promising approach for stand-off detection of biological aerosol clouds. Comprehensive models that explain the scattering behavior from the aerosol cloud are needed to understand and predict the scattering signatures of biological aerosols under varying atmospheric conditions and against different aerosol backgrounds. Elastic signatures are dependent on many parameters of the aerosol cloud, with two major components being the size distribution and refractive index of the aerosols. The Johns Hopkins University Applied Physics Laboratory (JHU/APL) has been in a unique position to measure the size distributions of released biological simulant clouds using a wide assortment of aerosol characterization systems that are available on the commercial market. In conjunction with the size distribution measurements, JHU/APL has also been making a dedicated effort to properly measure the refractive indices of the released materials using a thin-film absorption technique and laboratory characterization of the released materials. Intimate knowledge of the size distributions and refractive indices of the biological aerosols provides JHU/APL with powerful tools to build elastic scattering models, with the purpose of understanding, and ultimately, predicting the active signatures of biological clouds.

  3. Shortwave and longwave radiative forcings of aerosols depending on the vertical stratification of aerosols and clouds

    NASA Astrophysics Data System (ADS)

    Oikawa, Eiji; Suzuki, Kentaroh; Nakajima, Teruyuki; Nishizawa, Tomoaki

    2017-02-01

    We investigate four scenarios for estimating shortwave (SW) and longwave (LW) direct aerosol radiative forcing (DARF) at the top of atmosphere (TOA) using the global data set of the vertical distributions for aerosols and clouds of CALIPSO and CloudSat Level 2 products. One scenario is clear-sky (cloud-free) condition and three scenarios are cloudy-sky condition: the case that aerosols exists above clouds (AAC case), and the case that aerosols exist below high clouds such as cirrus, but without clouds below the aerosol layers (ABC case), and the case that aerosols are not observed in cloudy-sky condition. In clear-sky and ABC cases, aerosols mainly scatter sunlight and SWDARFs show negative values, except for bright surfaces, such as desert regions and the North and South Poles. In AAC case, aerosols absorb the reflected light from underlying low-level clouds to TOA, so that SWDARF at TOA shows positive value. Mineral dust absorbs the Earth's radiation and LWDARF indicates strong positive over Saharan and Arabian deserts. The global mean values of SW plus LW DARFs are -2.77, -0.77, and -1.40 Wm-2 under clear-sky, cloudy-sky, and all-sky conditions.

  4. Aerosol Impacts on Clouds and Precipitation in Eastern China: Results from Bin and Bulk Microphysics

    SciTech Connect

    Fan, Jiwen; Leung, Lai-Yung R.; Li, Zhanqing; Morrison, H.; Chen, Hongbin; Zhou, Yuquan; Qian, Yun; Wang, Yuan

    2012-01-19

    Using the Weather Research and Forecasting (WRF) model coupled with a 3 spectral-bin microphysics ('SBM') and measurements from the Atmospheric Radiation 4 Measurement (ARM) Mobile Facility field campaign in China (AMF-China), the authors 5 examine aerosol indirect effects (AIE) in the typical cloud regimes of the warm and cold 6 seasons in Southeast China: deep convective clouds (DCC) and stratus clouds (SC), 7 respectively. Comparisons with a two-moment bulk microphysics ('Bulk') are performed 8 to gain insights for improving bulk schemes in estimating AIE in weather and climate 9 simulations. For the first time, measurements of aerosol and cloud properties acquired in 10 China are used to evaluate model simulations to better understand AIE in China. It is 11 found that changes in cloud condensation nuclei (CCN) concentration significantly 12 change the timing of storms, the spatial and temporal distributions of precipitation, the 13 frequency distribution of precipitation rate, as well as cloud base and top heights for the 14 DCC, but not for the SC. CCN increase cloud droplet number (Nc) and mass 15 concentrations, decrease raindrop number concentration (Nr), and delay the onset of 16 precipitation. It is indicated much higher Nc and the opposite CCN effects on convection 17 and heavy rain with Bulk compared to SBM stem from the fixed CCN prescribed in Bulk. 18 CCN have a significant effect on ice microphysical properties with SBM but not Bulk 19 and different condensation/deposition freezing parameterizations employed could be the 20 main reason. This study provided insights to further improve the bulk scheme to better 21 account for aerosol-cloud interactions in regional and global climate simulations, which 22 will be the focus for a follow-on paper.

  5. Phytoplankton blooms weakly influence the cloud forming ability of sea spray aerosol

    NASA Astrophysics Data System (ADS)

    Collins, Douglas B.; Bertram, Timothy H.; Sultana, Camille M.; Lee, Christopher; Axson, Jessica L.; Prather, Kimberly A.

    2016-09-01

    After many field studies, the establishment of connections between marine microbiological processes, sea spray aerosol (SSA) composition, and cloud condensation nuclei (CCN) has remained an elusive challenge. In this study, we induced algae blooms to probe how complex changes in seawater composition impact the ability of nascent SSA to act as CCN, quantified by using the apparent hygroscopicity parameter (κapp). Throughout all blooms, κapp ranged between 0.7 and 1.4 (average 0.95 ± 0.15), consistent with laboratory investigations using algae-produced organic matter, but differing from climate model parameterizations and in situ SSA generation studies. The size distribution of nascent SSA dictates that changes in κapp associated with biological processing induce less than 3% change in expected CCN concentrations for typical marine cloud supersaturations. The insignificant effect of hygroscopicity on CCN concentrations suggests that the SSA production flux and/or secondary aerosol chemistry may be more important factors linking ocean biogeochemistry and marine clouds.

  6. Aerosol and Cloud-Nucleating Particle Observations during an Atmospheric River Event

    NASA Astrophysics Data System (ADS)

    DeMott, P. J.; McCluskey, C. S.; Petters, M.; Suski, K. J.; Levin, E. J.; Hill, T. C. J.; Atwood, S. A.; Schill, G. P.; Rocci, K.; Boose, Y.; Martin, A.; Cornwell, G.; Al-Mashat, H.; Moore, K.; Prather, K. A.; Rothfuss, N.; Taylor, H.; Leung, L. R.; Tomlinson, J. M.; Mei, F.; Hubbe, J. M.; Rosenfeld, D.; Spackman, J. R.; Fairall, C. W.; Creamean, J.; White, A. B.; Kreidenweis, S. M.

    2015-12-01

    The multi-agency CalWater 2015 project occurred over North Central CA and the Eastern Pacific during January to March 2015 (Spackman et al., this session). The goals of the campaign were to document the structure of atmospheric rivers (ARs) that deliver much of the water vapor associated with major winter storms along the U.S. West Coast and to investigate the modulating effect of aerosols on precipitation. Aerosol sources that may influence orographic cloud properties for air lifted over the mountains in California in winter include pollution, biomass burning, soil dusts and marine aerosols, but their roles will also be influenced by transport, vertical stratification, and scavenging processes. We present results from a comprehensive study of aerosol distributions, compositions, and cloud nucleating properties during an intense winter storm during February 2015, including data from an NSF-supported measurement site at Bodega Bay, from the DOE-ARM Cloud Aerosol Precipitation Experiment that included sampling on the NOAA RV Ron Brown offshore and the G-1 aircraft over ocean and land, and with context provided by other NOAA aircraft and remote sensing facilities. With a special focus on the coastal site, we discuss changes in aerosol distributions, aerosol hygroscopicity, and number concentrations of fluorescent particles, cloud condensation nuclei (CCN), and ice nucleating particles (INPs) during the AR event. We compare with periods preceding and following the event. For example, total aerosol number and surface area concentrations at below 0.5 μm diameter decreased from typical values of a few thousand cm-3 and 100 μm2 cm-3, respectively, to a few hundred cm-3 and 10 μm2cm-3 at Bodega Bay during the AR event. CCN concentrations were similarly lower, but hygroscopicity parameter (kappa) increased from typical values of 0.2 to values > 0.5 during the AR.INP and fluorescent particle number concentrations were generally lower during the AR event than at any other

  7. Integrated approach towards understanding interactions of mineral dust aerosol with warm clouds

    NASA Astrophysics Data System (ADS)

    Kumar, Prashant

    2011-12-01

    Mineral dust is ubiquitous in the atmosphere and represents a dominant type of particulate matter by mass. Dust particles can serve as cloud condensation nuclei (CCN), giant CCN (GCCN), or ice nuclei (IN), thereby, affecting cloud microphysics, albedo, and lifetime. Despite its well-recognized importance, assessments of dust impacts on clouds and climate remain highly uncertain. This thesis addresses the role of dust as CCN and GCCN with the goal of improving our understanding of dust-warm cloud interactions and their representation in climate models. Most studies to date focus on the soluble fraction of aerosol particles when describing cloud droplet nucleation, and overlook the interactions of the hydrophilic insoluble fraction with water vapor. A new approach to include such interactions (expressed by the process of water vapor adsorption) is explored, by combining multilayer Frenkel-Halsey-Hill (FHH) physical adsorption isotherm and curvature (Kelvin) effects. The importance of adsorption activation theory (FHH-AT) is corroborated by measurements of CCN activity of mineral aerosols generated from clays, calcite, quartz, and desert soil samples from Northern Africa, East Asia/China, and Northern America. A new aerosol generation setup for CCN measurements was developed based on a dry generation technique capable of reproducing natural dust aerosol emission. Based on the dependence of critical supersaturation with particle dry diameter, it is found that the FHH-AT is a better framework for describing fresh (and unprocessed) dust CCN activity than the classical Kohler theory (KT). Ion Chromatography (IC) measurements performed on fresh regional dust samples indicate negligible soluble fraction, and support that water vapor adsorption is the prime source of CCN activity in the dust. CCN measurements with the commonly used wet generated mineral aerosol (from atomization of a dust aqueous suspension) are also carried out. Results indicate that the method is subject

  8. GCM Simulations of the Aerosol Indirect Effect: Sensitivity to Cloud Parameterization and Aerosol Burden

    NASA Technical Reports Server (NTRS)

    Menon, Surabi; DelGenio, Anthony D.; Koch, Dorothy; Tselioudis, George; Hansen, James E. (Technical Monitor)

    2001-01-01

    We describe the coupling of the Goddard Institute for Space Studies (GISS) general circulation model (GCM) to an online sulfur chemistry model and source models for organic matter and sea-salt that is used to estimate the aerosol indirect effect. The cloud droplet number concentration is diagnosed empirically from field experiment datasets over land and ocean that observe droplet number and all three aerosol types simultaneously; corrections are made for implied variations in cloud turbulence levels. The resulting cloud droplet number is used to calculate variations in droplet effective radius, which in turn allows us to predict aerosol effects on cloud optical thickness and microphysical process rates. We calculate the aerosol indirect effect by differencing the top-of-the-atmosphere net cloud radiative forcing for simulations with present-day vs. pre-industrial emissions. Both the first (radiative) and second (microphysical) indirect effects are explored. We test the sensitivity of our results to cloud parameterization assumptions that control the vertical distribution of cloud occurrence, the autoconversion rate, and the aerosol scavenging rate, each of which feeds back significantly on the model aerosol burden. The global mean aerosol indirect effect for all three aerosol types ranges from -1.55 to -4.36 W m(exp -2) in our simulations. The results are quite sensitive to the pre-industrial background aerosol burden, with low pre-industrial burdens giving strong indirect effects, and to a lesser extent to the anthropogenic aerosol burden, with large burdens giving somewhat larger indirect effects. Because of this dependence on the background aerosol, model diagnostics such as albedo-particle size correlations and column cloud susceptibility, for which satellite validation products are available, are not good predictors of the resulting indirect effect.

  9. GCM Simulations of the Aerosol Indirect Effect: Sensitivity to Cloud Parameterization and Aerosol Burden

    NASA Technical Reports Server (NTRS)

    Menon, Surabi; DelGenio, Anthony D.; Koch, Dorothy; Tselioudis, George; Hansen, James E. (Technical Monitor)

    2001-01-01

    We describe the coupling of the Goddard Institute for Space Studies (GISS) general circulation model (GCM) to an online sulfur chemistry model and source models for organic matter and sea-salt that is used to estimate the aerosol indirect effect. The cloud droplet number concentration is diagnosed empirically from field experiment datasets over land and ocean that observe droplet number and all three aerosol types simultaneously; corrections are made for implied variations in cloud turbulence levels. The resulting cloud droplet number is used to calculate variations in droplet effective radius, which in turn allows us to predict aerosol effects on cloud optical thickness and microphysical process rates. We calculate the aerosol indirect effect by differencing the top-of-the-atmosphere net cloud radiative forcing for simulations with present-day vs. pre-industrial emissions. Both the first (radiative) and second (microphysical) indirect effects are explored. We test the sensitivity of our results to cloud parameterization assumptions that control the vertical distribution of cloud occurrence, the autoconversion rate, and the aerosol scavenging rate, each of which feeds back significantly on the model aerosol burden. The global mean aerosol indirect effect for all three aerosol types ranges from -1.55 to -4.36 W/sq m in our simulations. The results are quite sensitive to the pre-industrial background aerosol burden, with low pre-industrial burdens giving strong indirect effects, and to a lesser extent to the anthropogenic aerosol burden, with large burdens giving somewhat larger indirect effects. Because of this dependence on the background aerosol, model diagnostics such as albedo-particle size correlations and column cloud susceptibility, for which satellite validation products are available, are not good predictors of the resulting indirect effect.

  10. Airborne measurements of cloud forming nuclei and aerosol particles at Kennedy Space Center, Florida

    NASA Technical Reports Server (NTRS)

    Radke, L. F.; Langer, G.; Hindman, E. E., II

    1978-01-01

    Results of airborne measurements of the sizes and concentrations of aerosol particles, ice nuclei, and cloud condensation nuclei that were taken at Kennedy Space Center, Florida, are presented along with a detailed description of the instrumentation and measuring capabilities of the University of Washington airborne measuring facility (Douglas B-23). Airborne measurements made at Ft. Collins, Colorado, and Little Rock, Arkansas, during the ferry of the B-23 are presented. The particle concentrations differed significantly between the clean air over Ft. Collins and the hazy air over Little Rock and Kennedy Space Center. The concentrations of cloud condensation nuclei over Kennedy Space Center were typical of polluted eastern seaboard air. Three different instruments were used to measure ice nuclei: one used filters to collect the particles, and the others used optical and acoustical methods to detect ice crystals grown in portable cloud chambers. A comparison of the ice nucleus counts, which are in good agreement, is presented.

  11. Aerosol effect on the evolution of the thermodynamic properties of warm convective cloud fields

    PubMed Central

    Dagan, Guy; Koren, Ilan; Altaratz, Orit; Heiblum, Reuven H.

    2016-01-01

    Convective cloud formation and evolution strongly depend on environmental temperature and humidity profiles. The forming clouds change the profiles that created them by redistributing heat and moisture. Here we show that the evolution of the field’s thermodynamic properties depends heavily on the concentration of aerosol, liquid or solid particles suspended in the atmosphere. Under polluted conditions, rain formation is suppressed and the non-precipitating clouds act to warm the lower part of the cloudy layer (where there is net condensation) and cool and moisten the upper part of the cloudy layer (where there is net evaporation), thereby destabilizing the layer. Under clean conditions, precipitation causes net warming of the cloudy layer and net cooling of the sub-cloud layer (driven by rain evaporation), which together act to stabilize the atmosphere with time. Previous studies have examined different aspects of the effects of clouds on their environment. Here, we offer a complete analysis of the cloudy atmosphere, spanning the aerosol effect from instability-consumption to enhancement, below, inside and above warm clouds, showing the temporal evolution of the effects. We propose a direct measure for the magnitude and sign of the aerosol effect on thermodynamic instability. PMID:27929097

  12. Aerosol effect on the evolution of the thermodynamic properties of warm convective cloud fields

    NASA Astrophysics Data System (ADS)

    Dagan, Guy; Koren, Ilan; Altaratz, Orit; Heiblum, Reuven H.

    2016-12-01

    Convective cloud formation and evolution strongly depend on environmental temperature and humidity profiles. The forming clouds change the profiles that created them by redistributing heat and moisture. Here we show that the evolution of the field’s thermodynamic properties depends heavily on the concentration of aerosol, liquid or solid particles suspended in the atmosphere. Under polluted conditions, rain formation is suppressed and the non-precipitating clouds act to warm the lower part of the cloudy layer (where there is net condensation) and cool and moisten the upper part of the cloudy layer (where there is net evaporation), thereby destabilizing the layer. Under clean conditions, precipitation causes net warming of the cloudy layer and net cooling of the sub-cloud layer (driven by rain evaporation), which together act to stabilize the atmosphere with time. Previous studies have examined different aspects of the effects of clouds on their environment. Here, we offer a complete analysis of the cloudy atmosphere, spanning the aerosol effect from instability-consumption to enhancement, below, inside and above warm clouds, showing the temporal evolution of the effects. We propose a direct measure for the magnitude and sign of the aerosol effect on thermodynamic instability.

  13. Aerosol effect on the evolution of the thermodynamic properties of warm convective cloud fields.

    PubMed

    Dagan, Guy; Koren, Ilan; Altaratz, Orit; Heiblum, Reuven H

    2016-12-08

    Convective cloud formation and evolution strongly depend on environmental temperature and humidity profiles. The forming clouds change the profiles that created them by redistributing heat and moisture. Here we show that the evolution of the field's thermodynamic properties depends heavily on the concentration of aerosol, liquid or solid particles suspended in the atmosphere. Under polluted conditions, rain formation is suppressed and the non-precipitating clouds act to warm the lower part of the cloudy layer (where there is net condensation) and cool and moisten the upper part of the cloudy layer (where there is net evaporation), thereby destabilizing the layer. Under clean conditions, precipitation causes net warming of the cloudy layer and net cooling of the sub-cloud layer (driven by rain evaporation), which together act to stabilize the atmosphere with time. Previous studies have examined different aspects of the effects of clouds on their environment. Here, we offer a complete analysis of the cloudy atmosphere, spanning the aerosol effect from instability-consumption to enhancement, below, inside and above warm clouds, showing the temporal evolution of the effects. We propose a direct measure for the magnitude and sign of the aerosol effect on thermodynamic instability.

  14. Airborne measurements of cloud-forming nuclei and aerosol particles in stabilized ground clouds produced by solid rocket booster firings

    NASA Technical Reports Server (NTRS)

    Hindman, E. E., II; Ala, G. G.; Parungo, F. P.; Willis, P. T.; Bendura, R. J.; Woods, D.

    1978-01-01

    Airborne measurements of cloud volumes, ice nuclei and cloud condensation nuclei, liquid particles, and aerosol particles were obtained from stabilized ground clouds (SGCs) produced by Titan 3 launches at Kennedy Space Center, 20 August and 5 September 1977. The SGCs were bright, white, cumulus clouds early in their life and contained up to 3.5 g/m3 of liquid in micron to millimeter size droplets. The measured cloud volumes were 40 to 60 cu km five hours after launch. The SGCs contained high concentrations of cloud condensation nuclei active at 0.2%, 0.5%, and 1.0% supersaturation for periods of three to five hours. The SGCs also contained high concentrations of submicron particles. Three modes existed in the particle population: a 0.05 to 0.1 micron mode composed of aluminum-containing particles, a 0.2 to 0.8 micron mode, and a 2.0 to 10 micron mode composed of particles that contained primarily aluminum.

  15. Global estimation of above-cloud aerosols using spaceborne LIDAR

    NASA Astrophysics Data System (ADS)

    Chand, D.; Wood, R.; Anderson, T. L.; Satheesh, S. K.; Leahy, L.

    2008-12-01

    Estimates of global mean direct climate forcing by absorbing aerosols located above boundary layer clouds are large, uncertain, and almost entirely unconstrained by observations. Spaceborne lidar offers a new opportunity of estimating the aerosols at global scale. Here we use two recently available techniques quantifying the above-cloud aerosols using liquid water clouds as lidar targets from Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) [Chand et al., 2008]. Both methods can quantify aerosols above clouds and are based on their self-calibrating techniques. We used one year of global data between 70N-70S to show that day time calibration constants are different than night time calibrations constants. A clear latitudinal dependence is observed in the calibrations constants in CALIPSO observations. Using these 'self-calibration' constants, aerosol optical depth (AOD) and angstrom exponent (AE) of 'above- cloud' aerosols are quantified. Biomass burning is a major source of fine mode aerosols in different regions of world. For example, it is observed that June is the onset of the biomass burning fires in Southern Africa, peaking in August and September and then slowly decreasing until November, with a corresponding signature in aerosol optical depth. Layers with aerosol optical depth greater than 0.3 are commonly observed up to several thousand kilometers away from Africa over the Atlantic Ocean. The 'above-cloud' AOD as high as 1.5 is observed in the peak months. Despite of large variations is AOD, mean AE of these aerosols is about 1.6, without any systematic variability away from the source region. The results estimating the aerosols above clouds, including other regions at global scale, will be presented in the AGU meeting. Chand, D., T. L. Anderson, R. Wood, R. J. Charlson, Y. Hu, Z. Liu, and M. Vaughan (2008), Quantifying above-cloud aerosol using spaceborne lidar for improved understanding of cloudy-sky direct climate forcing, J

  16. Pollen as atmospheric cloud condensation nuclei

    NASA Astrophysics Data System (ADS)

    Steiner, Allison L.; Brooks, Sarah D.; Deng, Chunhua; Thornton, Daniel C. O.; Pendleton, Michael W.; Bryant, Vaughn

    2015-05-01

    Anemophilous (wind-dispersed) pollen grains are emitted in large quantities by vegetation in the midlatitudes for reproduction. Pollen grains are coarse particles (5-150 µm) that can rupture when wet to form submicron subpollen particles (SPP) that may have a climatic role. Laboratory CCN experiments of six fresh pollen samples show that SPP activate as CCN at a range of sizes, requiring supersaturations from 0.81 (± 0.07)% for 50 nm particles, 0.26 (± 0.03)% for 100 nm particles, and 0.12 (± 0.00)% for 200 nm particles. Compositional analyses indicate that SPP contain carbohydrates and proteins. The SPP contribution to global CCN is uncertain but could be important depending on pollen concentrations outside the surface layer and the number of SPP generated from a single pollen grain. The production of hygroscopic SPP from pollen represents a novel, biologically driven cloud formation pathway that may influence cloud optical properties and lifetimes, thereby influencing climate.

  17. Aerosol effects on deep convective clouds: impact of changes in aerosol size distribution and aerosol activation parameterization

    NASA Astrophysics Data System (ADS)

    Ekman, A. M. L.; Engström, A.; Söderberg, A.

    2010-03-01

    A cloud-resolving model including explicit aerosol physics and chemistry is used to study the impact of aerosols on deep convective strength. More specifically, by conducting six sensitivity series we examine how the complexity of the aerosol model, the size of the aerosols and the aerosol activation parameterization influence the aerosol-induced deep convective cloud sensitivity. Only aerosol effects on liquid droplet formation are considered. We find that an increased aerosol concentration generally results in stronger convection, which for the simulated case is in agreement with the conceptual model presented by Rosenfeld et al. (2008). However, there are two sensitivity series that do not display a monotonic increase in updraft velocity with increasing aerosol concentration. These exceptions illustrate the need to: 1) account for changes in evaporation processes and subsequent cooling when assessing aerosol effects on deep convective strength, 2) better understand graupel impaction scavenging of aerosols which may limit the number of CCN at a critical stage of cloud development and thereby dampen the convection, 3) increase our knowledge of aerosol recycling due to evaporation of cloud droplets. Furthermore, we find a significant difference in the aerosol-induced deep convective cloud sensitivity when using different complexities of the aerosol model and different aerosol activation parameterizations. For the simulated case, a 100% increase in aerosol concentration results in a difference in average updraft between the various sensitivity series which is as large as the average updraft increase itself. The model simulations also show that the change in graupel and rain formation is not necessarily directly proportional to the change in updraft velocity. For example, several of the sensitivity series display a decrease of the rain amount at the lowest model level with increasing updraft velocity. Finally, an increased number of aerosols in the Aitken mode (here

  18. Modeling aerosol-cloud interactions with a self-consistent cloud scheme in a general circulation model

    SciTech Connect

    Ming, Y; Ramaswamy, V; Donner, L J; Phillips, V T; Klein, S A; Ginoux, P A; Horowitz, L H

    2005-05-02

    This paper describes a self-consistent prognostic cloud scheme that is able to predict cloud liquid water, amount and droplet number (N{sub d}) from the same updraft velocity field, and is suitable for modeling aerosol-cloud interactions in general circulation models (GCMs). In the scheme, the evolution of droplets fully interacts with the model meteorology. An explicit treatment of cloud condensation nuclei (CCN) activation allows the scheme to take into account the contributions to N{sub d} of multiple types of aerosol (i.e., sulfate, organic and sea-salt aerosols) and kinetic limitations of the activation process. An implementation of the prognostic scheme in the Geophysical Fluid Dynamics Laboratory (GFDL) AM2 GCM yields a vertical distribution of N{sub d} characteristic of maxima in the lower troposphere differing from that obtained through diagnosing N{sub d} empirically from sulfate mass concentrations. As a result, the agreement of model-predicted present-day cloud parameters with satellite measurements is improved compared to using diagnosed N{sub d}. The simulations with pre-industrial and present-day aerosols show that the combined first and second indirect effects of anthropogenic sulfate and organic aerosols give rise to a global annual mean flux change of -1.8 W m{sup -2} consisting of -2.0 W m{sup -2} in shortwave and 0.2 W m{sup -2} in longwave, as model response alters cloud field, and subsequently longwave radiation. Liquid water path (LWP) and total cloud amount increase by 19% and 0.6%, respectively. Largely owing to high sulfate concentrations from fossil fuel burning, the Northern Hemisphere mid-latitude land and oceans experience strong cooling. So does the tropical land which is dominated by biomass burning organic aerosol. The Northern/Southern Hemisphere and land/ocean ratios are 3.1 and 1.4, respectively. The calculated annual zonal mean flux changes are determined to be statistically significant, exceeding the model's natural variations

  19. Improving aerosol distributions below clouds by assimilating satellite-retrieved cloud droplet number

    PubMed Central

    Saide, Pablo E.; Carmichael, Gregory R.; Spak, Scott N.; Minnis, Patrick; Ayers, J. Kirk

    2012-01-01

    Limitations in current capabilities to constrain aerosols adversely impact atmospheric simulations. Typically, aerosol burdens within models are constrained employing satellite aerosol optical properties, which are not available under cloudy conditions. Here we set the first steps to overcome the long-standing limitation that aerosols cannot be constrained using satellite remote sensing under cloudy conditions. We introduce a unique data assimilation method that uses cloud droplet number (Nd) retrievals to improve predicted below-cloud aerosol mass and number concentrations. The assimilation, which uses an adjoint aerosol activation parameterization, improves agreement with independent Nd observations and with in situ aerosol measurements below shallow cumulus clouds. The impacts of a single assimilation on aerosol and cloud forecasts extend beyond 24 h. Unlike previous methods, this technique can directly improve predictions of near-surface fine mode aerosols responsible for human health impacts and low-cloud radiative forcing. Better constrained aerosol distributions will help improve health effects studies, atmospheric emissions estimates, and air-quality, weather, and climate predictions. PMID:22778436

  20. Improving aerosol distributions below clouds by assimilating satellite-retrieved cloud droplet number.

    PubMed

    Saide, Pablo E; Carmichael, Gregory R; Spak, Scott N; Minnis, Patrick; Ayers, J Kirk

    2012-07-24

    Limitations in current capabilities to constrain aerosols adversely impact atmospheric simulations. Typically, aerosol burdens within models are constrained employing satellite aerosol optical properties, which are not available under cloudy conditions. Here we set the first steps to overcome the long-standing limitation that aerosols cannot be constrained using satellite remote sensing under cloudy conditions. We introduce a unique data assimilation method that uses cloud droplet number (N(d)) retrievals to improve predicted below-cloud aerosol mass and number concentrations. The assimilation, which uses an adjoint aerosol activation parameterization, improves agreement with independent N(d) observations and with in situ aerosol measurements below shallow cumulus clouds. The impacts of a single assimilation on aerosol and cloud forecasts extend beyond 24 h. Unlike previous methods, this technique can directly improve predictions of near-surface fine mode aerosols responsible for human health impacts and low-cloud radiative forcing. Better constrained aerosol distributions will help improve health effects studies, atmospheric emissions estimates, and air-quality, weather, and climate predictions.

  1. The Role of Aerosols on Precipitation Processes: Cloud Resolving Model Simulations

    NASA Technical Reports Server (NTRS)

    Tao, Wei-Kuo; Li, X.; Matsui, T.

    2012-01-01

    Cloud microphysics is inevitably affected by the smoke particle (CCN, cloud condensation nuclei) size distributions below the clouds. Therefore, size distributions parameterized as spectral bin microphysics are needed to explicitly study the effects of atmospheric aerosol concentration on cloud development, rainfall production, and rainfall rates for convective clouds. Recently, a detailed spectral-bin microphysical scheme was implemented into the Goddard Cumulus Ensemble (GCE) model. The formulation for the explicit spectral bin microphysical processes is based on solving stochastic kinetic equations for the size distribution functions of water droplets (i.e., cloud droplets and raindrops), and several types of ice particles [i.e. pristine ice crystals (columnar and plate-like), snow (dendrites and aggregates), graupel and frozen drops/hail]. Each type is described by a special size distribution function containing many categories (i.e., 33 bins). Atmospheric aerosols are also described using number density size-distribution functions. The model is tested by studying the evolution of deep cloud systems in the west Pacific warm pool region, the sub-tropics (Florida) and midlatitudes using identical thermodynamic conditions but with different concentrations of CCN: a low "clean" concentration and a high "dirty" concentration. Results indicate that the low CCN concentration case produces rainfall at the surface sooner than the high CeN case but has less cloud water mass aloft. Because the spectral-bin model explicitly calculates and allows for the examination of both the mass and number concentration of species in each size category, a detailed analysis of the instantaneous size spectrum can be obtained for these cases. It is shown that since the low (CN case produces fewer droplets, larger sizes develop due to greater condensational and collection growth, leading to a broader size spectrum in comparison to the high CCN case. Sensitivity tests were performed to

  2. Impact of Aerosols on Convective Clouds and Precipitation

    NASA Technical Reports Server (NTRS)

    Tao, Wei-Kuo; Chen, Jen-Ping; Li, Zhanqing; Wang, Chien; Zhang, Chidong

    2011-01-01

    Aerosols are a critical factor in the atmospheric hydrological cycle and radiation budget. As a major reason for clouds to form and a significant attenuator of solar radiation, aerosols affect climate in several ways. Current research suggests that aerosol effects on clouds could further extend to precipitation, both through the formation of cloud particles and by exerting persistent radiative forcing on the climate system that disturbs dynamics. However, the various mechanisms behind these effects, in particular the ones connected to precipitation, are not yet well understood. The atmospheric and climate communities have long been working to gain a better grasp of these critical effects and hence to reduce the significant uncertainties in climate prediction resulting from such a lack of adequate knowledge. The central theme of this paper is to review past efforts and summarize our current understanding of the effect of aerosols on precipitation processes from theoretical analysis of microphysics, observational evidence, and a range of numerical model simulations. In addition, the discrepancy between results simulated by models, as well as that between simulations and observations will be presented. Specifically, this paper will address the following topics: (1) fundamental theories of aerosol effects on microphysics and precipitation processes, (2) observational evidence of the effect of aerosols on precipitation processes, (3) signatures of the aerosol impact on precipitation from large-scale analyses, (4) results from cloud-resolving model simulations, and (5) results from large-scale numerical model simulations. Finally, several future research directions on aerosol - precipitation interactions are suggested.

  3. Improving aerosol interaction with clouds and precipitation in a regional chemical weather modeling system

    NASA Astrophysics Data System (ADS)

    Zhou, C.; Zhang, X.; Gong, S.; Wang, Y.; Xue, M.

    2016-01-01

    A comprehensive aerosol-cloud-precipitation interaction (ACI) scheme has been developed under a China Meteorological Administration (CMA) chemical weather modeling system, GRAPES/CUACE (Global/Regional Assimilation and PrEdiction System, CMA Unified Atmospheric Chemistry Environment). Calculated by a sectional aerosol activation scheme based on the information of size and mass from CUACE and the thermal-dynamic and humid states from the weather model GRAPES at each time step, the cloud condensation nuclei (CCN) are interactively fed online into a two-moment cloud scheme (WRF Double-Moment 6-class scheme - WDM6) and a convective parameterization to drive cloud physics and precipitation formation processes. The modeling system has been applied to study the ACI for January 2013 when several persistent haze-fog events and eight precipitation events occurred.

    The results show that aerosols that interact with the WDM6 in GRAPES/CUACE obviously increase the total cloud water, liquid water content, and cloud droplet number concentrations, while decreasing the mean diameters of cloud droplets with varying magnitudes of the changes in each case and region. These interactive microphysical properties of clouds improve the calculation of their collection growth rates in some regions and hence the precipitation rate and distributions in the model, showing 24 to 48 % enhancements of threat score for 6 h precipitation in almost all regions. The aerosols that interact with the WDM6 also reduce the regional mean bias of temperature by 3 °C during certain precipitation events, but the monthly means bias is only reduced by about 0.3 °C.

  4. A Framework for Aerosol-Cloud Interactions Monitoring

    NASA Astrophysics Data System (ADS)

    Russchenberg, H. W. J.; Sarna, K.

    2014-12-01

    A broad range of strategies have been used to study Aerosol-Cloud Interactions (ACI). However, the wide scope of methods and scales used makes it difficult to quantitatively compare result from different studies. In this paper, we propose a method of aerosol-cloud interaction monitoring based on widely available remote sensing instruments and easily applicable at many different observatories. This method provides a way of identifying cases where a change in the aerosol environment causes a change in the cloud. In this scheme we attempt to use (as far as possible) the observed signal from lidar and radar. For an aerosol proxy we use the attenuated backscatter (sensitive to aerosol concentration) and to obtain information about changes in the cloud we use the radar reflectivity factor (sensitive to cloud droplet size and concentration). Assuming a positive dependence between the number concentration of cloud droplets and the number concentration of aerosol we expect that an increase of the attenuated backscatter coefficient will correspond to a small increase of the radar reflectivity factor (due to the increase of cloud droplets concentration). However, the slope of this correlation will vary. A number of factors, such as meteorology or cloud drop microphysical properties, can influence changes in a cloud. For that reason we put a constraint on the liquid water content using liquid water path information from microwave radiometers. This limitation ensures that the variability in the cloud will be primarily due to changes in microphysical properties associated with the variation in aerosols. Further, we limit the cases only to non-precipitating, low-level stratiform and stratocumulus clouds without drizzle. Although this method is based on a synergy of instruments, we use widely available systems for an efficient evaluation of the aerosol influence on the cloud. The main advantages of this scheme are the use of direct observables from widely spread remote sensing

  5. Determining the chemical composition of cloud condensation nuclei. Second progress report

    SciTech Connect

    Williams, A.L.; Rothert, J.E.; McClure, K.E.; Alofs, D.J.; Hagen, D.E.; White, D.R.; Hopkins, A.R.; Trueblood, M.B.

    1992-02-01

    This second progress report describes the status of the project one and one-half years after the start. The goal of the project is to develop the instrumentation to collect cloud condensation nuclei (CCN) in sufficient amounts to determine their chemical composition, and to survey the CCN composition in different climates through a series of field measurements. Our approach to CCN collection is to first form droplets on the nuclei under simulated cloud humidity conditions, which is the only known method of identifying CCN from the background aerosol. Under cloud chamber conditions, the droplets formed become larger than the surrounding aerosol, and can then be removed by inertial impaction. The residue of the evaporated droplets represents the sample to be chemically analyzed. Two size functions of CCN particles are collected by first forming droplets on the large particles are collected by first forming droplets on the large CCN in a haze chamber at 100% relative humidity, and then activating the remaining CCN at 1% supersaturation in a cloud chamber. The experimental apparatus is a serious flow arrangement consisting of an impactor to remove the large aerosol particles, a haze chamber to form droplets on the remaining larger CCN, another impactor to remove the haze droplets containing the larger CCN particles for chemical analysis, a continuous flow diffusion (CFD) cloud chamber to form droplets on the remaining smaller CCN, and a third impactor to remove the droplets for the small CCN sample. Progress is documented here on the development of each of the major components of the flow system. Chemical results are reported on tests to determine suitable wicking material for the different plates. Results of computer modeling of various impactor flows are discussed.

  6. Aerosol-Cloud-Drizzle-Turbulence Interactions in Boundary Layer Clouds

    DTIC Science & Technology

    2012-09-30

    and cloud observations in trade wind cumulus clouds using the CIRPAS aircraft with the cloud radar was designed and carried out. The observational...gradients in cloud properties off the coast. Further from the South Florida area of fair-weather cumulus clouds (Jan. 2008) where clouds with both...marine and continental characteristics were observed. This was followed by a set of observations made in 2010 of cumulus clouds in off of Barbados

  7. Individual aerosol particles in and below clouds along a Mt. Fuji slope: Modification of sea-salt-containing particles by in-cloud processing

    NASA Astrophysics Data System (ADS)

    Ueda, S.; Hirose, Y.; Miura, K.; Okochi, H.

    2014-02-01

    Sizes and compositions of atmospheric aerosol particles can be altered by in-cloud processing by absorption/adsorption of gaseous and particulate materials and drying of aerosol particles that were formerly activated as cloud condensation nuclei. To elucidate differences of aerosol particles before and after in-cloud processing, aerosols were observed along a slope of Mt. Fuji, Japan (3776 m a.s.l.) during the summer in 2011 and 2012 using a portable laser particle counter (LPC) and an aerosol sampler. Aerosol samples for analyses of elemental compositions were obtained using a cascade impactor at top-of-cloud, in-cloud, and below-cloud altitudes. To investigate composition changes via in-cloud processing, individual particles (0.5-2 μm diameter) of samples from five cases (days) collected at different altitudes under similar backward air mass trajectory conditions were analyzed using a transmission electron microscope (TEM) equipped with an energy dispersive X-ray analyzer. For most cases (four cases), most particles at all altitudes mainly comprised sea salts: mainly Na with some S and/or Cl. Of those, in two cases, sea-salt-containing particles with Cl were found in below-cloud samples, although sea-salt-containing particles in top-of-cloud samples did not contain Cl. This result suggests that Cl in the sea salt was displaced by other cloud components. In the other two cases, sea-salt-containing particles on samples at all altitudes were without Cl. However, molar ratios of S to Na (S/Na) of the sea-salt-containing particles of top-of-cloud samples were higher than those of below-cloud samples, suggesting that sulfuric acid or sulfate was added to sea-salt-containing particles after complete displacement of Cl by absorption of SO2 or coagulation with sulfate. The additional volume of sulfuric acid in clouds for the two cases was estimated using the observed S/Na values of sea-salt-containing particles. The estimation revealed that size changes by in-cloud

  8. Aerosol and cloud microphysics covariability in the northeast Pacific boundary layer estimated with ship-based and satellite remote sensing observations: NE Pacific Aerosol-Cloud Interactions

    DOE PAGES

    Painemal, David; Chiu, J. -Y. Christine; Minnis, Patrick; ...

    2017-02-27

    We utilized ship measurements collected over the northeast Pacific along transects between the port of Los Angeles (33.7°N, 118.2°W) and Honolulu (21.3°N, 157.8°W) during May to August 2013 in order to investigate the covariability between marine low cloud microphysical and aerosol properties. Ship-based retrievals of cloud optical depth (τ) from a Sun photometer and liquid water path (LWP) from a microwave radiometer were combined to derive cloud droplet number concentration Nd and compute a cloud-aerosol interaction (ACI) metric defined as ACICCN=∂ ln(Nd)/∂ ln(CCN), with CCN denoting the cloud condensation nuclei concentration measured at 0.4% (CCN0.4) and 0.3% (CCN0.3) supersaturation. Analysismore » of CCN0.4, accumulation mode aerosol concentration (Na), and extinction coefficient (σext) indicates that Na and σext can be used as CCN0.4 proxies for estimating ACI. ACICCN derived from 10 min averaged Nd and CCN0.4 and CCN0.3, and CCN0.4 regressions using Na and σext, produce high ACICCN: near 1.0, that is, a fractional change in aerosols is associated with an equivalent fractional change in Nd. ACICCN computed in deep boundary layers was small (ACICCN=0.60), indicating that surface aerosol measurements inadequately represent the aerosol variability below clouds. Satellite cloud retrievals from MODerate-resolution Imaging Spectroradiometer and GOES-15 data were compared against ship-based retrievals and further analyzed to compute a satellite-based ACICCN. We found that the satellite data correlated well with their ship-based counterparts with linear correlation coefficients equal to or greater than 0.78. Combined satellite Nd and ship-based CCN0.4 and Na yielded a maximum ACICCN=0.88–0.92, a value slightly less than the ship-based ACICCN, but still consistent with aircraft-based studies in the eastern Pacific.« less

  9. Evaluating Global Aerosol Models and Aerosol and Water Vapor Properties Near Clouds

    SciTech Connect

    Richard A. Ferrare; David D. Turner

    2011-09-01

    Project goals: (1) Use the routine surface and airborne measurements at the ARM SGP site, and the routine surface measurements at the NSA site, to continue our evaluations of model aerosol simulations; (2) Determine the degree to which the Raman lidar measurements of water vapor and aerosol scattering and extinction can be used to remotely characterize the aerosol humidification factor; (3) Use the high temporal resolution CARL data to examine how aerosol properties vary near clouds; and (4) Use the high temporal resolution CARL and Atmospheric Emitted Radiance Interferometer (AERI) data to quantify entrainment in optically thin continental cumulus clouds.

  10. Venus: Halide cloud condensation and volatile element inventories

    NASA Technical Reports Server (NTRS)

    Lewis, J. S.; Fegley, B., Jr.

    1982-01-01

    Several Venus cloud condensates, including A12C16 as well as halides, oxides and sulfides of arsenic and antimony, are assessed for their thermodynamic and geochemical plausibility. Aluminum chloride can confidently be ruled out, and condensation of arsenic sulfides on the surface will cause arsenic compounds to be too rare to produce the observed clouds. Antimony may conceivably be sufficiently volatile, but the expected molecular form is gaseous SbS, not the chloride. Arsenic and antimony compounds in the atmosphere will be regulated at very low levels by sulfide precipitation, irrespective of the planetary inventory of As and Sb. Thus the arguments for a volatile-deficient origin for Venus based on the depletion of water and mercury (relative to Earth) cannot be tested by a search for atmospheric arsenic or antimony.

  11. Aerosol concentration and size distribution measured below, in, and above cloud from the DOE G-1 during VOCALS-REx

    SciTech Connect

    Kleinman L. I.; Daum, P. H.; Lee, Y.-N.; Lewis, E. R.; Sedlacek III, A. J.; Senum, G. I.; Springston, S. R.; Wang, J.; Hubbe, J.; Jayne, J.; Min, Q.; Yum, S. S.; Allen, G.

    2012-01-04

    During the VOCALS Regional Experiment, the DOE G-1 aircraft was used to sample a varying aerosol environment pertinent to properties of stratocumulus clouds over a longitude band extending 800 km west from the Chilean coast at Arica. Trace gas and aerosol measurements are presented as a function of longitude, altitude, and dew point in this study. Spatial distributions are consistent with an upper atmospheric source for O{sub 3} and South American coastal sources for marine boundary layer (MBL) CO and aerosol, most of which is acidic sulfate. Pollutant layers in the free troposphere (FT) can be a result of emissions to the north in Peru or long range transport from the west. At a given altitude in the FT (up to 3 km), dew point varies by 40 C with dry air descending from the upper atmospheric and moist air having a boundary layer (BL) contribution. Ascent of BL air to a cold high altitude results in the condensation and precipitation removal of all but a few percent of BL water along with aerosol that served as CCN. Thus, aerosol volume decreases with dew point in the FT. Aerosol size spectra have a bimodal structure in the MBL and an intermediate diameter unimodal distribution in the FT. Comparing cloud droplet number concentration (CDNC) and pre-cloud aerosol (D{sub p} > 100 nm) gives a linear relation up to a number concentration of {approx}150 cm{sup -3}, followed by a less than proportional increase in CDNC at higher aerosol number concentration. A number balance between below cloud aerosol and cloud droplets indicates that {approx}25 % of aerosol with D{sub p} > 100 nm are interstitial (not activated). A direct comparison of pre-cloud and in-cloud aerosol yields a higher estimate. Artifacts in the measurement of interstitial aerosol due to droplet shatter and evaporation are discussed. Within each of 102 constant altitude cloud transects, CDNC and interstitial aerosol were anti-correlated. An examination of one cloud as a case study shows that the

  12. Cloud and Aerosol Characterization During CAEsAR 2014

    NASA Astrophysics Data System (ADS)

    Zieger, P.; Tesche, M.; Krejci, R.; Baumgardner, D.; Walther, A.; Rosati, B.; Widequist, U.; Tunved, P.; O'Connor, E.; Ström, J.

    2015-12-01

    The Cloud and Aerosol Experiment at Åre (CAEsAR 2014) campaign took place from June to October 2014 at Mt. Åreskutan, Sweden, a remote mountain site in Northern Sweden. The campaign was designed to study the physical and chemical properties of clouds and aerosols under orographic forcing. A unique and comprehensive set-up allowed an in-situ characterization of both constituents at a mountain top station at 1200 m a.s.l. including instruments to measure cloud droplet size distribution, meteorological parameters, cloud residual properties (using a counterflow virtual impactor inlet), cloud water composition and various aerosol chemical and microphysical properties (e.g. size, optical and hygroscopic properties). At the same time, a remote sensing site was installed below the mountain site at 420 m a.s.l. in the immediate vicinity (< 3 km horizontally), with vertical profiling from an aerosol lidar, winds and turbulence from a scanning Doppler lidar, a Sun photometer measuring aerosol columnar optical properties, and a precipitation sampler taking rain water for chemical analysis. In addition, regular radiosoundings were performed from the valley. Here, we present the results of this intensive campaign which includes approx. 900 hours of in-cloud sampling. Various unique cloud features were frequently observed such as dynamically-driven droplet growth, bimodal droplet distributions, and the activation of particles down to approx. 20 nm in dry particle diameter. During the campaign, a forest fire smoke plume was transported over the site with measureable impacts on the cloud properties. This data will be used to constrain cloud and aerosol models, as well as to validate satellite retrievals. A first comparison to VIIRS and MODIS satellite retrievals will also be shown.

  13. Numerical simulations of stratocumulus cloud response to aerosol perturbation

    NASA Astrophysics Data System (ADS)

    Andrejczuk, Miroslaw; Gadian, Alan; Blyth, Alan

    2010-05-01

    Geoengineering of the Earth clouds is proposed as a one of the methods to offset global warming. Idealized climate model simulations indicate that such an approach may work and stratocumulus cloud seeding may delay global warming by as much as 25 years. However cloud-aerosol interaction is not fully understood yet, and its representation in climate model are very simplified, what may lead to significant uncertainty in climate model predictions. Problem with quantifying aerosol distribution/composition/concentration -> cloud droplet number relation is more general and even higher resolution model models with more sophisticated microphysics have problem with capturing this relation. Stratocumulus clouds are especially difficult to model because these are long living clouds and aerosol can affect these clouds significantly both locally and globally. Before investigating effect of aerosol perturbation on stratocumulus clouds, models should be able to capture observed relation between aerosol and cloud droplets. Although there are indications that cloud seeding may effect cloud albedo based on results from parcel model(1), assumption made in this type of models about homogeneity and neglected effect of dynamics may affect model results. In the presentation new approach to microphysics, which is represented in Lagrangian framework, with two way coupling between Lagrangian parcels and Large Eddy Simulations model dynamics and theromodynamics(2) will be discussed. Results from this model will be presented and validated against observations from VOCALS field campaign. Model response to aerosol perturbation and its effect on cloud albedo will be shown for cases with high and low initial cloud droplet concentration. (1) Bower, K. N., Choularton, T. W., Latham, J., Sahraei, J. and Salter, S. H. (2006), Computational assessment of a proposed technique for global warming mitigation via albedo-enhancement of marine stratocumulus clouds. Atmos. Res. 82, 328-336. (2) M. Andrejczuk

  14. Cloud Regimes as a Tool for Systematic Study of Various Aerosol-Cloud-Precipitation Interactions

    NASA Technical Reports Server (NTRS)

    Oreopoulos, Lazaros; Cho, Nayeong; Lee, Dongmin

    2016-01-01

    Systematic changes of clouds and precipitation are notoriously difficult to ascribe to aerosols. This presentation will showcase yet one more attempt to at least credibly detect the signal of aerosol-cloud-precipitation interactions. We surmise that the concept of cloud regimes (CRs) is appropriate to conduct such an investigation. Previous studies focused on what we call here dynamical CRs, and while we continue to adopt those too for our analysis, we have found that a different way of organizing cloud systems, namely via microphysical regimes is also promising. Our analysis relies on MODIS Collection 6 Level-3 data for clouds and aerosols, and TRMM-TMPA data for precipitation. The regimes are derived by applying clustering analysis on MODIS joint histograms, and once each grid cell is assigned a regime, aerosol and precipitation data can be spatiotemporally matched and composited by regime. The composites of various cloud and precipitation variables for high (upper quartile of distribution) and low (lower quartile) aerosol loadings can then be contrasted. We seek evidence of aerosol effects both in regimes with large fractions of deep ice-rich clouds, as well as regimes where low liquid phase clouds dominate. Signals can be seen, especially when the analysis is broken by land-ocean and when additional filters are applied, but there are of course caveats which will be discussed.

  15. Aerosol-Cloud Interactions Measured at Puijo Measurement Station: The effect of surrounding terrain

    NASA Astrophysics Data System (ADS)

    Romakkaniemi, Sami; Hellsten, Antti; Ahmad, Irshad; Tonttila, Juha; Jaatinen, Antti; Portin, Harri; Leskinen, Ari; Hao, Liqing; Virtanen, Annele; Komppula, Mika

    2015-04-01

    Puijo measurement station has provided continuous data on aerosol-cloud interactions since 2006. The station is located on top of the Puijo observation tower (tower height 75m, measurement altitude 224 m above the surrounding lake level) in Kuopio, Finland. The top of the tower is covered by low altitude cloud about 15 % of days, offering perfect conditions for studying aerosol-cloud interactions. In the measurements, a twin-inlet setup (total and interstitial inlets) is used to separate the activated particles from the interstitial (non-activated) particles. The continuous twin-inlet measurements include aerosol size distribution, scattering and absorption. In addition weather parameters and cloud droplet size distribution are measured continuously. During the campaigns the twin-inlet system is additionally equipped with aerosol mass spectrometer (AMS) and cloud condensation nuclei counter (CCNC). This way we were able to define the differences in chemical composition of the activated and non-activated particles, and the number of potential cloud condensation nuclei (CCN) in different supersaturations. As the tower is located on the top of a hill, it is possible that updrafts created by the hill are affecting the cloud droplet formation. In this study the terrain effect on wind fields around the measurement station was modelled using PALM Large Eddy Simulation model. The LES domain covered 15 km x 8 km area around the Puijo tower and extended up to 1 km height while the boundary-layer depth was about 370 m. The LES grid spacing was 5 m in the mean wind direction and 4 m in both cross-wind and vertical directions. The terrain topography needed was obtained from the National Land Survey of Finland with spatial resolution of 2 meters. Results from this work show that in some conditions the updrafts caused by the hill are affecting cloud droplet number concentration measured at the station. This is dependent on the wind speed and direction, and cloud base height. In

  16. On the source of organic acid aerosol layers above clouds.

    PubMed

    Sorooshian, Armin; Lu, Miao-Ling; Brechtel, Fred J; Jonsson, Haflidi; Feingold, Graham; Flagan, Richard C; Seinfeld, John H

    2007-07-01

    During the July 2005 Marine Stratus/Stratocumulus Experiment (MASE) and the August-September 2006 Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS), the Center for Interdisciplinary Remotely-Piloted Aircraft Studies (CIRPAS) Twin Otter probed aerosols and cumulus clouds in the eastern Pacific Ocean off the coast of northern California and in southeastern Texas, respectively. An on-board particle-into-liquid sampler (PILS) quantified inorganic and organic acid species with < or = 5-min time resolution. Ubiquitous organic aerosol layers above cloud with enhanced organic acid levels were observed in both locations. The data suggest that aqueous-phase reactions to produce organic acids, mainly oxalic acid, followed by droplet evaporation is a source of elevated organic acid aerosol levels above cloud. Oxalic acid is observed to be produced more efficiently relative to sulfate as the cloud liquid water content increases, corresponding to larger and less acidic droplets. As derived from large eddy simulations of stratocumulus underthe conditions of MASE, both Lagrangian trajectory analysis and diurnal cloudtop evolution provide evidence that a significant fraction of the aerosol mass concentration above cloud can be accounted for by evaporated droplet residual particles. Methanesulfonate data suggest that entrainment of free tropospheric aerosol can also be a source of organic acids above boundary layer clouds.

  17. The cloud-aerosol-radiation (CAR) ensemble modeling system

    NASA Astrophysics Data System (ADS)

    Liang, X.-Z.; Zhang, F.

    2013-08-01

    A cloud-aerosol-radiation (CAR) ensemble modeling system has been developed to incorporate the largest choices of alternate parameterizations for cloud properties (cover, water, radius, optics, geometry), aerosol properties (type, profile, optics), radiation transfers (solar, infrared), and their interactions. These schemes form the most comprehensive collection currently available in the literature, including those used by the world's leading general circulation models (GCMs). CAR provides a unique framework to determine (via intercomparison across all schemes), reduce (via optimized ensemble simulations), and attribute specific key factors for (via physical process sensitivity analyses) the model discrepancies and uncertainties in representing greenhouse gas, aerosol, and cloud radiative forcing effects. This study presents a general description of the CAR system and illustrates its capabilities for climate modeling applications, especially in the context of estimating climate sensitivity and uncertainty range caused by cloud-aerosol-radiation interactions. For demonstration purposes, the evaluation is based on several CAR standalone and coupled climate model experiments, each comparing a limited subset of the full system ensemble with up to 896 members. It is shown that the quantification of radiative forcings and climate impacts strongly depends on the choices of the cloud, aerosol, and radiation schemes. The prevailing schemes used in current GCMs are likely insufficient in variety and physically biased in a significant way. There exists large room for improvement by optimally combining radiation transfer with cloud property schemes.

  18. Cloud-Aerosol-Radiation (CAR) ensemble modeling system

    NASA Astrophysics Data System (ADS)

    Liang, X.-Z.; Zhang, F.

    2013-04-01

    A Cloud-Aerosol-Radiation (CAR) ensemble modeling system has been developed to incorporate the largest choices of alternative parameterizations for cloud properties (cover, water, radius, optics, geometry), aerosol properties (type, profile, optics), radiation transfers (solar, infrared), and their interactions. These schemes form the most comprehensive collection currently available in the literature, including those used by the world leading general circulation models (GCMs). The CAR provides a unique framework to determine (via intercomparison across all schemes), reduce (via optimized ensemble simulations), and attribute specific key factors for (via physical process sensitivity analyses) the model discrepancies and uncertainties in representing greenhouse gas, aerosol and cloud radiative forcing effects. This study presents a general description of the CAR system and illustrates its capabilities for climate modeling applications, especially in the context of estimating climate sensitivity and uncertainty range caused by cloud-aerosol-radiation interactions. For demonstration purpose, the evaluation is based on several CAR standalone and coupled climate model experiments, each comparing a limited subset of the full system ensemble with up to 896 members. It is shown that the quantification of radiative forcings and climate impacts strongly depends on the choices of the cloud, aerosol and radiation schemes. The prevailing schemes used in current GCMs are likely insufficient in variety and physically biased in a significant way. There exists large room for improvement by optimally combining radiation transfer with cloud property schemes.

  19. Effect of Carbonaceous Aerosols on Clouds and Precipitation in Asia

    NASA Astrophysics Data System (ADS)

    v, V.; Wang, H.; Ganguly, D.; Minghuai, W.; Rasch, P. J.

    2010-12-01

    Carbonaceous aerosols enhance scattering and absorption of solar radiation (i.e., direct radiative effect) in the atmosphere and also affect clouds and precipitation through indirect effects, thus heating the atmosphere but reducing the amount of solar radiation that reaches the earth’s surface. These effects through dynamic feedbacks can also have remote impact over regions far away from their emission sources and hence demand special scientific attention. Previous modeling studies have revealed that large amount of anthropogenic carbonaceous aerosols over the Asian region can alter monsoon circulation and precipitation patterns and thereby influence its strength by varying degrees spatially. Most of the studies focused on the direct radiative effect of aerosols and their subsequent effect on monsoon precipitation. We evaluate the changes in clouds and precipitation in Asia due to carbonaceous aerosols using the community atmospheric model (CAM5) which accounts for not only aerosol direct effects, but also aerosol indirect effects on warm, mixed-phase and cirrus clouds. This study focuses on the precipitation efficiency with emphasis on aerosol indirect effects. In addition to carbonaceous aerosol emissions over Asia, the effect of emissions from other regions like North America, North Africa and Europe are also investigated for their influence on precipitation in the Asian region. In addition to the focus on the aerosol effect on monsoon, we also study the seasonality in aerosol induced changes to precipitation efficiency. We present the quantitative estimates of changes in precipitation efficiency related to changes in aerosol loading and compare them with those estimated from satellite observations, and further explore the potential role of aerosol indirect effects to changes in precipitation efficiency.

  20. Eye safe short range standoff aerosol cloud finder.

    SciTech Connect

    Bambha, Ray P.; Schroder, Kevin L.; Reichardt, Thomas A.

    2005-02-01

    Because many solid objects, both stationary and mobile, will be present in an indoor environment, the design of an indoor aerosol cloud finding lidar (light detection and ranging) instrument presents a number of challenges. The cloud finder must be able to discriminate between these solid objects and aerosol clouds as small as 1-meter in depth in order to probe suspect clouds. While a near IR ({approx}1.5-{micro}m) laser is desirable for eye-safety, aerosol scattering cross sections are significantly lower in the near-IR than at visible or W wavelengths. The receiver must deal with a large dynamic range since the backscatter from solid object will be orders of magnitude larger than for aerosol clouds. Fast electronics with significant noise contributions will be required to obtain the necessary temporal resolution. We have developed a laboratory instrument to detect aerosol clouds in the presence of solid objects. In parallel, we have developed a lidar performance model for performing trade studies. Careful attention was paid to component details so that results obtained in this study could be applied towards the development of a practical instrument. The amplitude and temporal shape of the signal return are analyzed for discrimination of aerosol clouds in an indoor environment. We have assessed the feasibility and performance of candidate approaches for a fieldable instrument. With the near-IR PMT and a 1.5-{micro}m laser source providing 20-{micro}J pulses, we estimate a bio-aerosol detection limit of 3000 particles/l.

  1. The NASA Decadal Survey Aerosol, Cloud, Ecosystems Mission

    NASA Technical Reports Server (NTRS)

    McClain, Charles R.; Bontempi, Paula; Maring, Hal

    2011-01-01

    In 2007, the National Academy of Sciences delivered a Decadal Survey (Earth Science and Applications from Space: National Imperatives for the Next Decade and Beyond) for NASA, NOAA, and USGS, which is a prioritization of future satellite Earth observations. The recommendations included 15 missions (13 for NASA, two for NOAA), which were prioritized into three groups or tiers. One of the second tier missions is the Aerosol, Cloud, (ocean) Ecosystems (ACE) mission, which focuses on climate forcing, cloud and aerosol properties and interactions, and ocean ecology, carbon cycle science, and fluxes. The baseline instruments recommended for ACE are a cloud radar, an aerosol/cloud lidar, an aerosol/cloud polarimeter, and an ocean radiometer. The instrumental heritage for these measurements are derived from the Cloudsat, CALIPSO, Glory, SeaWiFS and Aqua (MODIS) missions. In 2008, NASA HQ, lead by Hal Maring and Paula Bontempi, organized an interdisciplinary science working group to help formulate the ACE mission by refining the science objectives and approaches, identifying measurement (satellite and field) and mission (e.g., orbit, data processing) requirements, technology requirements, and mission costs. Originally, the disciplines included the cloud, aerosol, and ocean biogeochemistry communities. Subsequently, an ocean-aerosol interaction science working group was formed to ensure the mission addresses the broadest range of science questions possible given the baseline measurements, The ACE mission is a unique opportunity for ocean scientists to work closely with the aerosol and cloud communities. The science working groups are collaborating on science objectives and are defining joint field studies and modeling activities. The presentation will outline the present status of the ACE mission, the science questions each discipline has defined, the measurement requirements identified to date, the current ACE schedule, and future opportunities for broader community

  2. Interactions between aerosol absorption, thermodynamics, dynamics, and microphysics and their impacts on a multiple-cloud system

    NASA Astrophysics Data System (ADS)

    Lee, Seoung Soo; Li, Zhanqing; Mok, Jungbin; Ahn, Myoung-Hwan; Kim, Byung-Gon; Choi, Yong-Sang; Jung, Chang-Hoon; Yoo, Hye Lim

    2017-02-01

    This study investigates how the increasing concentration of black carbon aerosols, which act as radiation absorbers as well as agents for the cloud-particle nucleation, affects stability, dynamics and microphysics in a multiple-cloud system using simulations. Simulations show that despite increases in stability due to increasing concentrations of black carbon aerosols, there are increases in the averaged updraft mass fluxes (over the whole simulation domain and period). This is because aerosol-enhanced evaporative cooling intensifies convergence near the surface. This increase in the intensity of convergence induces an increase in the frequency of updrafts with the low range of speeds, leading to the increase in the averaged updraft mass fluxes. The increase in the frequency of updrafts induces that in the number of condensation entities and this leads to more condensation and cloud liquid that acts to be a source of the accretion of cloud liquid by precipitation. Hence, eventually, there is more accretion that offsets suppressed autoconversion, which results in negligible changes in cumulative precipitation as aerosol concentrations increase. The increase in the frequency of updrafts with the low range of speeds alters the cloud-system organization (represented by cloud-depth spatiotemporal distributions and cloud-cell population) by supporting more low-depth clouds. The altered organization in turn alters precipitation spatiotemporal distributions by generating more weak precipitation events. Aerosol-induced reduction in solar radiation that reaches the surface induces more occurrences of small-value surface heat fluxes, which in turn supports the more low-depth clouds and weak precipitation together with the greater occurrence of low-speed updrafts.

  3. Aerosol Indirect Effects on Cirrus Clouds in Global Aerosol-Climate Models

    NASA Astrophysics Data System (ADS)

    Liu, X.; Zhang, K.; Wang, Y.; Neubauer, D.; Lohmann, U.; Ferrachat, S.; Zhou, C.; Penner, J.; Barahona, D.; Shi, X.

    2015-12-01

    Cirrus clouds play an important role in regulating the Earth's radiative budget and water vapor distribution in the upper troposphere. Aerosols can act as solution droplets or ice nuclei that promote ice nucleation in cirrus clouds. Anthropogenic emissions from fossil fuel and biomass burning activities have substantially perturbed and enhanced concentrations of aerosol particles in the atmosphere. Global aerosol-climate models (GCMs) have now been used to quantify the radiative forcing and effects of aerosols on cirrus clouds (IPCC AR5). However, the estimate uncertainty is very large due to the different representation of ice cloud formation and evolution processes in GCMs. In addition, large discrepancies have been found between model simulations in terms of the spatial distribution of ice-nucleating aerosols, relative humidity, and temperature fluctuations, which contribute to different estimates of the aerosol indirect effect through cirrus clouds. In this presentation, four GCMs with the start-of-the art representations of cloud microphysics and aerosol-cloud interactions are used to estimate the aerosol indirect effects on cirrus clouds and to identify the causes of the discrepancies. The estimated global and annual mean anthropogenic aerosol indirect effect through cirrus clouds ranges from 0.1 W m-2 to 0.3 W m-2 in terms of the top-of-the-atmosphere (TOA) net radiation flux, and 0.5-0.6 W m-2 for the TOA longwave flux. Despite the good agreement on global mean, large discrepancies are found at the regional scale. The physics behind the aerosol indirect effect is dramatically different. Our analysis suggests that burden of ice-nucleating aerosols in the upper troposphere, ice nucleation frequency, and relative role of ice formation processes (i.e., homogeneous versus heterogeneous nucleation) play key roles in determining the characteristics of the simulated aerosol indirect effects. In addition to the indirect effect estimate, we also use field campaign

  4. Aerosols and clouds in chemical transport models and climate models.

    SciTech Connect

    Lohmann,U.; Schwartz, S. E.

    2008-03-02

    Clouds exert major influences on both shortwave and longwave radiation as well as on the hydrological cycle. Accurate representation of clouds in climate models is a major unsolved problem because of high sensitivity of radiation and hydrology to cloud properties and processes, incomplete understanding of these processes, and the wide range of length scales over which these processes occur. Small changes in the amount, altitude, physical thickness, and/or microphysical properties of clouds due to human influences can exert changes in Earth's radiation budget that are comparable to the radiative forcing by anthropogenic greenhouse gases, thus either partly offsetting or enhancing the warming due to these gases. Because clouds form on aerosol particles, changes in the amount and/or composition of aerosols affect clouds in a variety of ways. The forcing of the radiation balance due to aerosol-cloud interactions (indirect aerosol effect) has large uncertainties because a variety of important processes are not well understood precluding their accurate representation in models.

  5. The CalWater 2 - ARM Cloud Aerosol Precipitation Experiment (ACAPEX)

    NASA Astrophysics Data System (ADS)

    Leung, L. Y.; Prather, K. A.; Ralph, F. M.; Rosenfeld, D.; Spackman, J. R.; Fairall, C. W.; DeMott, P. J.; Fan, J.; Zhao, C.

    2014-12-01

    modeling experiments to investigate long range transport of aerosols to the western U.S. and the influence of cloud condensation nuclei and ice nuclei on precipitation.

  6. Indirect and semi-direct aerosol campaign: The impact of Arctic aerosols on clouds

    SciTech Connect

    McFarquhar, Greg M.; Ghan, Steven; Verlinde, Johannes; Korolev, Alexei; Strapp, J. Walter; Schmid, Beat; Tomlinson, Jason M.; Wolde, Menqistu; Brooks, Sarah D.; Cziczo, Dan; Dubey, Manvendra K.; Fan, Jiwen; Flynn, Connor; Gultepe, Ismail; Hubbe, John; Gilles, Mary K.; Laskin, Alexander; Lawson, Paul; Leaitch, W. Richard; Liu, Peter; Liu, Xiaohong; Lubin, Dan; Mazzoleni, Claudio; Macdonald, Ann -Marie; Moffet, Ryan C.; Morrison, Hugh; Ovchinnikov, Mikhail; Ronfeld, Debbie; Shupe, Matthew D.; Xie, Shaocheng; Zelenyuk, Alla; Bae, Kenny; Freer, Matt; Glen, Andrew

    2011-02-01

    A comprehensive dataset of microphysical and radiative properties of aerosols and clouds in the boundary layer in the vicinity of Barrow, Alaska, was collected in April 2008 during the Indirect and Semi-Direct Aerosol Campaign (ISDAC). ISDAC's primary aim was to examine the effects of aerosols, including those generated by Asian wildfires, on clouds that contain both liquid and ice. ISDAC utilized the Atmospheric Radiation Measurement Pro- gram's permanent observational facilities at Barrow and specially deployed instruments measuring aerosol, ice fog, precipitation, and radiation. The National Research Council of Canada Convair-580 flew 27 sorties and collected data using an unprecedented 41 stateof- the-art cloud and aerosol instruments for more than 100 h on 12 different days. Aerosol compositions, including fresh and processed sea salt, biomassburning particles, organics, and sulfates mixed with organics, varied between flights. Observations in a dense arctic haze on 19 April and above, within, and below the single-layer stratocumulus on 8 and 26 April are enabling a process-oriented understanding of how aerosols affect arctic clouds. Inhomogeneities in reflectivity, a close coupling of upward and downward Doppler motion, and a nearly constant ice profile in the single-layer stratocumulus suggests that vertical mixing is responsible for its longevity observed during ISDAC. Data acquired in cirrus on flights between Barrow and Fairbanks, Alaska, are improving the understanding of the performance of cloud probes in ice. Furthermore, ISDAC data will improve the representation of cloud and aerosol processes in models covering a variety of spatial and temporal scales, and determine the extent to which surface measurements can provide retrievals of aerosols, clouds, precipitation, and radiative heating.

  7. Indirect and semi-direct aerosol campaign: The impact of Arctic aerosols on clouds

    DOE PAGES

    McFarquhar, Greg M.; Ghan, Steven; Verlinde, Johannes; ...

    2011-02-01

    A comprehensive dataset of microphysical and radiative properties of aerosols and clouds in the boundary layer in the vicinity of Barrow, Alaska, was collected in April 2008 during the Indirect and Semi-Direct Aerosol Campaign (ISDAC). ISDAC's primary aim was to examine the effects of aerosols, including those generated by Asian wildfires, on clouds that contain both liquid and ice. ISDAC utilized the Atmospheric Radiation Measurement Pro- gram's permanent observational facilities at Barrow and specially deployed instruments measuring aerosol, ice fog, precipitation, and radiation. The National Research Council of Canada Convair-580 flew 27 sorties and collected data using an unprecedented 41more » stateof- the-art cloud and aerosol instruments for more than 100 h on 12 different days. Aerosol compositions, including fresh and processed sea salt, biomassburning particles, organics, and sulfates mixed with organics, varied between flights. Observations in a dense arctic haze on 19 April and above, within, and below the single-layer stratocumulus on 8 and 26 April are enabling a process-oriented understanding of how aerosols affect arctic clouds. Inhomogeneities in reflectivity, a close coupling of upward and downward Doppler motion, and a nearly constant ice profile in the single-layer stratocumulus suggests that vertical mixing is responsible for its longevity observed during ISDAC. Data acquired in cirrus on flights between Barrow and Fairbanks, Alaska, are improving the understanding of the performance of cloud probes in ice. Furthermore, ISDAC data will improve the representation of cloud and aerosol processes in models covering a variety of spatial and temporal scales, and determine the extent to which surface measurements can provide retrievals of aerosols, clouds, precipitation, and radiative heating.« less

  8. Influence of non-ideality on condensation to aerosol

    NASA Astrophysics Data System (ADS)

    Compernolle, S.; Ceulemans, K.; Müller, J.-F.

    2009-02-01

    Secondary organic aerosol (SOA) is a complex mixture of water and organic molecules. Its composition is determined by the presence of semi-volatile or non-volatile compounds, their saturation vapor pressure and activity coefficient. The activity coefficient is a non-ideality effect and is a complex function of SOA composition. In a previous publication, the detailed chemical mechanism (DCM) for α-pinene oxidation and subsequent aerosol formation BOREAM was presented. In this work, we investigate with this DCM the impact of non-ideality by simulating smog chamber experiments for α-pinene degradation and aerosol formation and taking the activity coefficient into account of all molecules in the aerosol phase. Several versions of the UNIFAC method are tested for this purpose, and missing parameters for e.g. hydroperoxides and nitrates are inferred from fittings to activity coefficient data generated using the SPARC model. Alternative approaches to deal with these missing parameters are also tested, as well as an activity coefficient calculation method based on Hansen solubility parameters (HSP). It turns out that for most experiments, non-ideality has only a limited impact on the interaction between the organic molecules, and therefore on SOA yields and composition, when water uptake is ignored. The reason is that often, the activity coefficient is on average close to 1 and, specifically for high-VOC experiments, partitioning is not very sensitive on the activity coefficient because the equilibrium is shifted strongly towards condensation. Still, for ozonolysis experiments with low amounts of volatile organic carbon (low-VOC), the UNIFAC parameterization of Raatikainen et al. leads to significantly higher SOA yields (by up to a factor 1.6) compared to the ideal case and to other parameterizations. Water uptake is model dependent, in the order: ideal > UNIFAC-Raatikainen > UNIFAC-Peng > UNIFAC-Hansen ≍ UNIFAC-Magnussen ≍ UNIFAC-Ming. In the absence of salt

  9. Aerosol concentration and size distribution measured below, in, and above cloud from the DOE G-1 during VOCALS-REx

    SciTech Connect

    Kleinman, L.I.; Daum, P. H.; Lee, Y.-N.; Lewis, E. R.; Sedlacek III, A. J.; Senum, G. I.; Springston, S. R.; Wang, J.; Hubbe, J.; Jayne, J.; Min, Q.; Yum, S. S.; Allen, G.

    2011-06-21

    During the VOCALS Regional Experiment, the DOE G-1 aircraft was used to sample a varying aerosol environment pertinent to properties of stratocumulus clouds over a longitude band extending 800 km west from the Chilean coast at Arica. Trace gas and aerosol measurements are presented as a function of longitude, altitude, and dew point in this study. Spatial distributions are consistent with an upper atmospheric source for O{sub 3} and South American coastal sources for marine boundary layer (MBL) CO and aerosol, most of which is acidic sulfate in agreement with the dominant pollution source being SO{sub 2} from Cu smelters and power plants. Pollutant layers in the free troposphere (FT) can be a result of emissions to the north in Peru or long range transport from the west. At a given altitude in the FT (up to 3 km), dew point varies by 40 C with dry air descending from the upper atmospheric and moist air having a BL contribution. Ascent of BL air to a cold high altitude results in the condensation and precipitation removal of all but a few percent of BL water along with aerosol that served as CCN. Thus, aerosol volume decreases with dew point in the FT. Aerosol size spectra have a bimodal structure in the MBL and an intermediate diameter unimodal distribution in the FT. Comparing cloud droplet number concentration (CDNC) and pre-cloud aerosol (Dp > 100 nm) gives a linear relation up to a number concentration of {approx}150 cm{sup -3}, followed by a less than proportional increase in CDNC at higher aerosol number concentration. A number balance between below cloud aerosol and cloud droplets indicates that {approx}25% of aerosol in the PCASP size range are interstitial (not activated). One hundred and two constant altitude cloud transects were identified and used to determine properties of interstitial aerosol. One transect is examined in detail as a case study. Approximately 25 to 50% of aerosol with D{sub p} > 110 nm were not activated, the difference between the two

  10. Aerosol concentration and size distribution measured below, in, and above cloud from the DOE G-1 during VOCALS-REx

    NASA Astrophysics Data System (ADS)

    Kleinman, L. I.; Daum, P. H.; Lee, Y.-N.; Lewis, E. R.; Sedlacek, A. J., III; Senum, G. I.; Springston, S. R.; Wang, J.; Hubbe, J.; Jayne, J.; Min, Q.; Yum, S. S.; Allen, G.

    2011-06-01

    During the VOCALS Regional Experiment, the DOE G-1 aircraft was used to sample a varying aerosol environment pertinent to properties of stratocumulus clouds over a longitude band extending 800 km west from the Chilean coast at Arica. Trace gas and aerosol measurements are presented as a function of longitude, altitude, and dew point in this study. Spatial distributions are consistent with an upper atmospheric source for O3 and South American coastal sources for marine boundary layer (MBL) CO and aerosol, most of which is acidic sulfate in agreement with the dominant pollution source being SO2 from Cu smelters and power plants. Pollutant layers in the free troposphere (FT) can be a result of emissions to the north in Peru or long range transport from the west. At a given altitude in the FT (up to 3 km), dew point varies by 40 °C with dry air descending from the upper atmospheric and moist air having a BL contribution. Ascent of BL air to a cold high altitude results in the condensation and precipitation removal of all but a few percent of BL water along with aerosol that served as CCN. Thus, aerosol volume decreases with dew point in the FT. Aerosol size spectra have a bimodal structure in the MBL and an intermediate diameter unimodal distribution in the FT. Comparing cloud droplet number concentration (CDNC) and pre-cloud aerosol (Dp > 100 nm) gives a linear relation up to a number concentration of ~150 cm-3, followed by a less than proportional increase in CDNC at higher aerosol number concentration. A number balance between below cloud aerosol and cloud droplets indicates that ~25 % of aerosol in the PCASP size range are interstitial (not activated). One hundred and two constant altitude cloud transects were identified and used to determine properties of interstitial aerosol. One transect is examined in detail as a case study. Approximately 25 to 50 % of aerosol with Dp > 110 nm were not activated, the difference between the two approaches possibly representing

  11. Impacts of aerosol particles on the microphysical and radiative properties of stratocumulus clouds over the southeast Pacific Ocean

    NASA Astrophysics Data System (ADS)

    Twohy, C. H.; Anderson, J. R.; Toohey, D. W.; Andrejczuk, M.; Adams, A.; Lytle, M.; George, R. C.; Wood, R.; Saide, P.; Spak, S.; Zuidema, P.; Leon, D.

    2013-03-01

    The southeast Pacific Ocean is covered by the world's largest stratocumulus cloud layer, which has a strong impact on ocean temperatures and climate in the region. The effect of anthropogenic sources of aerosol particles on the stratocumulus deck was investigated during the VOCALS field experiment. Aerosol measurements below and above cloud were made with a ultra-high sensitivity aerosol spectrometer and analytical electron microscopy. In addition to more standard in-cloud measurements, droplets were collected and evaporated using a counterflow virtual impactor (CVI), and the non-volatile residual particles were analyzed. Many flights focused on the gradient in cloud properties on an E-W track along 20° S from near the Chilean coast to remote areas offshore. Mean statistics, including their significance, from eight flights and many individual legs were compiled. Consistent with a continental source of cloud condensation nuclei, below-cloud accumulation-mode aerosol and droplet number concentration generally decreased from near shore to offshore. Single particle analysis was used to reveal types and sources of the enhanced particle number that influence droplet concentration. While a variety of particle types were found throughout the region, the dominant particles near shore were partially neutralized sulfates. Modeling and chemical analysis indicated that the predominant source of these particles in the marine boundary layer along 20° S was anthropogenic pollution from central Chilean sources, with copper smelters a relatively small contribution. Cloud droplets were smaller in regions of enhanced particles near shore. However, physically thinner clouds, and not just higher droplet number concentrations from pollution, both contributed to the smaller droplets. Satellite measurements were used to show that cloud albedo was highest 500-1000 km offshore, and actually slightly lower closer to shore due to the generally thinner clouds and lower liquid water paths

  12. Implementation of an Aerosol-Cloud Microphysics-Radiation Coupling into the NASA Unified WRF: Simulation Results for the 6-7 August 2006 AMMA Special Observing Period

    NASA Technical Reports Server (NTRS)

    Shi, J. J.; Matsui, T.; Tao, W.-K.; Tan, Q.; Peters-Lidard, C.; Chin, M.; Pickering, K.; Guy, N.; Lang, S.; Kemp, E. M.

    2014-01-01

    Aerosols affect the Earth's radiation balance directly and cloud microphysical processes indirectly via the activation of cloud condensation and ice nuclei. These two effects have often been considered separately and independently, hence the need to assess their combined impact given the differing nature of their effects on convective clouds. To study both effects, an aerosol-microphysics-radiation coupling, including Goddard microphysics and radiation schemes, was implemented into the NASA Unified Weather Research and Forecasting model (NU-WRF). Fully coupled NU-WRF simulations were conducted for a mesoscale convective system (MCS) that passed through the Niamey, Niger area on 6-7 August 2006 during an African Monsoon Multidisciplinary Analysis (AMMA) special observing period. The results suggest that rainfall is reduced when aerosol indirect effects are included, regardless of the aerosol direct effect. Daily mean radiation heating profiles in the area traversed by the MCS showed the aerosol (mainly mineral dust) direct effect had the largest impact near cloud tops just above 200 hectopascals where short-wave heating increased by about 0.8 Kelvin per day; the weakest long-wave cooling was at around 250 hectopascals. It was also found that more condensation and ice nuclei as a result of higher aerosol/dust concentrations led to increased amounts of all cloud hydrometeors because of the microphysical indirect effect, and the radiation direct effect acts to reduce precipitating cloud particles (rain, snow and graupel) in the middle and lower cloud layers while increasing the non-precipitating particles (ice) in the cirrus anvil. However, when the aerosol direct effect was activated, regardless of the indirect effect, the onset of MCS precipitation was delayed about 2 hours, in conjunction with the delay in the activation of cloud condensation and ice nuclei. Overall, for this particular environment, model set-up and physics configuration, the effect of aerosol

  13. Meteorological and aerosol effects on marine cloud microphysical properties

    NASA Astrophysics Data System (ADS)

    Sanchez, K. J.; Russell, L. M.; Modini, R. L.; Frossard, A. A.; Ahlm, L.; Corrigan, C. E.; Roberts, G. C.; Hawkins, L. N.; Schroder, J. C.; Bertram, A. K.; Zhao, R.; Lee, A. K. Y.; Lin, J. J.; Nenes, A.; Wang, Z.; Wonaschütz, A.; Sorooshian, A.; Noone, K. J.; Jonsson, H.; Toom, D.; Macdonald, A. M.; Leaitch, W. R.; Seinfeld, J. H.

    2016-04-01

    Meteorology and microphysics affect cloud formation, cloud droplet distributions, and shortwave reflectance. The Eastern Pacific Emitted Aerosol Cloud Experiment and the Stratocumulus Observations of Los-Angeles Emissions Derived Aerosol-Droplets studies provided measurements in six case studies of cloud thermodynamic properties, initial particle number distribution and composition, and cloud drop distribution. In this study, we use simulations from a chemical and microphysical aerosol-cloud parcel (ACP) model with explicit kinetic drop activation to reproduce observed cloud droplet distributions of the case studies. Four cases had subadiabatic lapse rates, resulting in fewer activated droplets, lower liquid water content, and higher cloud base height than an adiabatic lapse rate. A weighted ensemble of simulations that reflect measured variation in updraft velocity and cloud base height was used to reproduce observed droplet distributions. Simulations show that organic hygroscopicity in internally mixed cases causes small effects on cloud reflectivity (CR) (<0.01), except for cargo ship and smoke plumes, which increased CR by 0.02 and 0.07, respectively, owing to their high organic mass fraction. Organic hygroscopicity had larger effects on droplet concentrations for cases with higher aerosol concentrations near the critical diameter (namely, polluted cases with a modal peak near 0.1 µm). Differences in simulated droplet spectral widths (k) caused larger differences in CR than organic hygroscopicity in cases with organic mass fractions of 60% or less for the cases shown. Finally, simulations from a numerical parameterization of cloud droplet activation suitable for general circulation models compared well with the ACP model, except under high organic mass fraction.

  14. Indirect and Semi-Direct Aerosol Campaign: The Impact of Arctic Aerosols on Clouds

    SciTech Connect

    McFarquhar, Greg; Ghan, Steven J.; Verlinde, J.; Korolev, Alexei; Strapp, J. Walter; Schmid, Beat; Tomlinson, Jason M.; Wolde, Mengistu; Brooks, Sarah D.; Cziczo, Daniel J.; Dubey, Manvendra K.; Fan, Jiwen; Flynn, Connor J.; Gultepe, Ismail; Hubbe, John M.; Gilles, Mary K.; Laskin, Alexander; Lawson, Paul; Leaitch, W. R.; Liu, Peter S.; Liu, Xiaohong; Lubin, Dan; Mazzoleni, Claudio; Macdonald, A. M.; Moffet, Ryan C.; Morrison, H.; Ovchinnikov, Mikhail; Shupe, Matthew D.; Turner, David D.; Xie, Shaocheng; Zelenyuk, Alla; Bae, Kenny; Freer, Matthew; Glen, Andrew

    2011-02-01

    A comprehensive dataset of microphysical and radiative properties of aerosols and clouds in the arctic boundary layer in the vicinity of Barrow, Alaska was collected in April 2008 during the Indirect and Semi-Direct Aerosol Campaign (ISDAC) sponsored by the Department of Energy Atmospheric Radiation Measurement (ARM) and Atmospheric Science Programs. The primary aim of ISDAC was to examine indirect effects of aerosols on clouds that contain both liquid and ice water. The experiment utilized the ARM permanent observational facilities at the North Slope of Alaska (NSA) in Barrow. These include a cloud radar, a polarized micropulse lidar, and an atmospheric emitted radiance interferometer as well as instruments specially deployed for ISDAC measuring aerosol, ice fog, precipitation and spectral shortwave radiation. The National Research Council of Canada Convair-580 flew 27 sorties during ISDAC, collecting data using an unprecedented 42 cloud and aerosol instruments for more than 100 hours on 12 different days. Data were obtained above, below and within single-layer stratus on 8 April and 26 April 2008. These data enable a process-oriented understanding of how aerosols affect the microphysical and radiative properties of arctic clouds influenced by different surface conditions. Observations acquired on a heavily polluted day, 19 April 2008, are enhancing this understanding. Data acquired in cirrus on transit flights between Fairbanks and Barrow are improving our understanding of the performance of cloud probes in ice. Ultimately the ISDAC data will be used to improve the representation of cloud and aerosol processes in models covering a variety of spatial and temporal scales, and to determine the extent to which long-term surface-based measurements can provide retrievals of aerosols, clouds, precipitation and radiative heating in the Arctic.

  15. Aerosol properties, source identification, and cloud processing in orographic clouds measured by single particle mass spectrometry on a central European mountain site during HCCT-2010

    NASA Astrophysics Data System (ADS)

    Roth, A.; Schneider, J.; Klimach, T.; Mertes, S.; van Pinxteren, D.; Herrmann, H.; Borrmann, S.

    2016-01-01

    Cloud residues and out-of-cloud aerosol particles with diameters between 150 and 900 nm were analysed by online single particle aerosol mass spectrometry during the 6-week study Hill Cap Cloud Thuringia (HCCT)-2010 in September-October 2010. The measurement location was the mountain Schmücke (937 m a.s.l.) in central Germany. More than 160 000 bipolar mass spectra from out-of-cloud aerosol particles and more than 13 000 bipolar mass spectra from cloud residual particles were obtained and were classified using a fuzzy c-means clustering algorithm. Analysis of the uncertainty of the sorting algorithm was conducted on a subset of the data by comparing the clustering output with particle-by-particle inspection and classification by the operator. This analysis yielded a false classification probability between 13 and 48 %. Additionally, particle types were identified by specific marker ions. The results from the ambient aerosol analysis show that 63 % of the analysed particles belong to clusters having a diurnal variation, suggesting that local or regional sources dominate the aerosol, especially for particles containing soot and biomass burning particles. In the cloud residues, the relative percentage of large soot-containing particles and particles containing amines was found to be increased compared to the out-of-cloud aerosol, while, in general, organic particles were less abundant in the cloud residues. In the case of amines, this can be explained by the high solubility of the amines, while the large soot-containing particles were found to be internally mixed with inorganics, which explains their activation as cloud condensation nuclei. Furthermore, the results show that during cloud processing, both sulfate and nitrate are added to the residual particles, thereby changing the mixing state and increasing the fraction of particles with nitrate and/or sulfate. This is expected to lead to higher hygroscopicity after cloud evaporation, and therefore to an increase of

  16. Implications of using transmitted vs. reflected light for determining cloud properties, cloud radiative effects and aerosol-cloud-interactions

    NASA Astrophysics Data System (ADS)

    LeBlanc, S. E.; Redemann, J.; Segal-Rosenhaimer, M.; Kacenelenbogen, M. S.; Shinozuka, Y.; Flynn, C. J.; Schmidt, S.; Pilewskie, P.; Song, S.; Woods, S.; Lawson, P.; Nenes, A.; Lin, J. J.; Ziemba, L. D.

    2015-12-01

    Light transmitted through clouds is sensitive to a different cloud volume than reflected light at cloud top. This difference in sampling volumes has implications when calculating the radiative effects of clouds (CRE) and aerosol-cloud-interactions (ACI). We present a comparison of retrieved cloud properties and the corresponding CRE and ACI based on transmitted and reflected light for a cloud sampled during the Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS, 2013) field campaign. Measurements of zenith radiances were obtained from the NASA DC-8 aircraft using the Spectrometer for Sky-Scanning, Sun-Tracking Atmospheric Research (4STAR) instrument. 4STAR was deployed on an airborne platform during SEAC4RS alongside the Solar Spectral Flux Radiometer (SSFR). To retrieve cloud properties from transmitted shortwave radiation, we use a retrieval utilizing spectrally resolved measurements. Spectral features in shortwave radiation transmitted through clouds are sensitive to changes in cloud optical thickness, effective radius, and thermodynamic phase. The spectral features due to absorption and scattering processes by liquid water and ice cloud particles include shifts in spectral slopes, curvatures, maxima, and minima of cloud-transmitted radiance. These spectral features have been quantified by 15 parameters used to retrieve cloud properties from the 4STAR zenith radiances. Retrieved cloud optical thicknesses and effective radii based on transmitted shortwave radiation are compared to their counterparts obtained from reflected shortwave radiation measured above cloud with MODIS and with the enhanced MODIS Airborne Simulator (eMAS), the Research Scanning Polarimeter (RSP), and SSFR operating aboard the NASA ER-2 aircraft. Remotely sensed cloud particle effective radius are combined with in situ measurements of cloud and aerosol particles from the NASA Langley Aerosol Research Group Experiment (LARGE) CCN Counter

  17. Cloud droplet activity changes of soot aerosol upon smog chamber ageing

    NASA Astrophysics Data System (ADS)

    Wittbom, C.; Eriksson, A. C.; Rissler, J.; Carlsson, J. E.; Roldin, P.; Nordin, E. Z.; Nilsson, P. T.; Swietlicki, E.; Pagels, J. H.; Svenningsson, B.

    2014-09-01

    Particles containing soot, or black carbon, are generally considered to contribute to global warming. However, large uncertainties remain in the net climate forcing resulting from anthropogenic emissions of black carbon (BC), to a large extent due to the fact that BC is co-emitted with gases and primary particles, both organic and inorganic, and subject to atmospheric ageing processes. In this study, diesel exhaust particles and particles from a flame soot generator spiked with light aromatic secondary organic aerosol (SOA) precursors were processed by UV radiation in a 6 m3 Teflon chamber in the presence of NOx. The time-dependent changes of the soot nanoparticle properties were characterised using a Cloud Condensation Nuclei Counter, an Aerosol Particle Mass Analyzer and a Soot Particle Aerosol Mass Spectrometer. The results show that freshly emitted soot particles do not activate into cloud droplets at supersaturations ≤2%, i.e. the BC core coated with primary organic aerosol (POA) from the exhaust is limited in hygroscopicity. Before the onset of UV radiation it is unlikely that any substantial SOA formation is taking place. An immediate change in cloud-activation properties occurs at the onset of UV exposure. This change in hygroscopicity is likely attributed to SOA formed from intermediate volatility organic compounds (IVOCs) in the diesel engine exhaust. The change of cloud condensation nuclei (CCN) properties at the onset of UV radiation implies that the lifetime of soot particles in the atmosphere is affected by the access to sunlight, which differs between latitudes. The ageing of soot particles progressively enhances their ability to act as cloud condensation nuclei, due to changes in: (I) organic fraction of the particle, (II) chemical properties of this fraction (e.g. primary or secondary organic aerosol), (III) particle size, and (IV) particle morphology. Applying κ-Köhler theory, using a κSOA value of 0.13 (derived from independent input

  18. Explicit numerical study of aerosol-cloud interactions in boundary layer clouds

    NASA Astrophysics Data System (ADS)

    Paunova, Irena T.

    Aerosol-cloud interactions, the mechanisms by which aerosols impact clouds and precipitation and clouds impact aerosols as they are released upon droplet evaporation, are investigated by means of explicit high-resolution (3 km) numerical simulations with the Mesoscale Compressible Community (MC2) model. This model, which is non-hydrostatic and compressible, was extended by including separate continuity equations for dry and activated multi-modal aerosol, and for chemical species. The sources and sinks include: particle activation, solute transfer between drops, generation of extra soluble material in clouds via oxidation of dissolved SO2, and particle regeneration. The cloud processes are represented by an advanced double-moment bulk microphysical parameterization. Three summertime cases have been evaluated: a marine stratus and a cold frontal system over the Bay of Fundy near Nova Scotia, formed on 1 Sep 1995 and extensively sampled as a part of the Radiation, Aerosol, and Cloud Experiment (RACE); and a continental stratocumulus, formed over the southern coast of Lake Erie on 11 July 2001. The marine stratus and the frontal system have been examined for the effects of aerosol on cloud properties and thoroughly evaluated against the available observations. The frontal system and the continental stratocumulus have been evaluated for the effects of cloud processing on the aerosol spectrum. The marine stratus simulations suggest a significant impact of the aerosol on cloud properties. A simulation with mechanistic activation and a uni-modal aerosol showed the best agreement with observations in regards to cloud-base and cloud-top height, droplet concentration, and liquid water content. A simulation with a simple activation parameterization failed to simulate essential bulk cloud properties: droplet concentration was significantly underpredicted and the vertical structure of the cloud was inconsistent with the observations. A simulation with a mechanistic

  19. Spectral signatures of polar stratospheric clouds and sulfate aerosol

    SciTech Connect

    Massie, S.T.; Bailey, P.L.; Gille, J.C.; Lee, E.C.; Mergenthaler, J.L.; Roche, A.E.; Kumer, J.B.; Fishbein, E.F.; Waters, J.W.; Lahoz, W.A.

    1994-10-15

    Multiwavelength observations of Antarctic and midlatitude aerosol by the Cryogenic Limb Array Etalon Spectrometer (CLAES) experiment on the Upper Atmosphere Research Satellite are used to demonstrate a technique that identifies the location of polar stratospheric clouds. The technique discussed uses the normalized area of the triangle formed by the aerosol extinctions at 925, 1257, and 1605 cm{sup {minus}1} (10.8, 8.0, and 6.2 {mu}m) to derive a spectral aerosol measure M of the aerosol spectrum. Mie calculations for spherical particles and T-matrix calculations for spheroidal particles are used to generate theoretical spectral extinction curves for sulfate and polar stratospheric cloud particles. The values of the spectral aerosol measure M for the sulfate and polar stratospheric cloud particles are shown to be different. Aerosol extinction data, corresponding to temperatures between 180 and 220 K at a pressure of 46 hPa (near 21-km altitude) for 18 August 1992, are used to demonstrate the technique. Thermodynamic calculations, based upon frost-point calculation and laboratory phase-equilibrium studies of nitric acid trihydrate, are used to predict the location of nitric acid trihydrate cloud particles. 47 refs., 22 figs., 3 tabs.

  20. Spectral signatures of polar stratospheric clouds and sulfate aerosol

    NASA Technical Reports Server (NTRS)

    Massie, S. T.; Bailey, P. L.; Gille, J. C.; Lee, E. C.; Mergenthaler, J. L.; Roche, A. E.; Kumer, J. B.; Fishbein, E. F.; Waters, J. W.; Lahoz, W. A.

    1994-01-01

    Multiwavelength observations of Antarctic and midlatitude aerosol by the Cryogenic Limb Array Etalon Spectrometer (CLAES) experiment on the Upper Atmosphere Research Satellite (UARS) are used to demonstrate a technique that identifies the location of polar stratospheric clouds. The technique discussed uses the normalized area of the triangle formed by the aerosol extinctions at 925, 1257, and 1605/cm (10.8, 8.0, and 6.2 micrometers) to derive a spectral aerosol measure M of the aerosol spectrum. Mie calculations for spherical particles and T-matrix calculations for spheriodal particles are used to generate theoretical spectral extinction curves for sulfate and polar stratospheric cloud particles. The values of the spectral aerosol measure M for the sulfate and polar stratospheric cloud particles are shown to be different. Aerosol extinction data, corresponding to temperatures between 180 and 220 K at a pressure of 46 hPa (near 21-km altitude) for 18 August 1992, are used to demonstrate the technique. Thermodynamic calculations, based upon frost-point calculations and laboratory phase-equilibrium studies of nitric acid trihydrate, are used to predict the location of nitric acid trihydrate cloud particles.

  1. Comprehensive mapping and characteristic regimes of aerosol effects on the formation and evolution of pyro-convective clouds

    DOE PAGES

    Chang, D.; Cheng, Y.; Reutter, P.; ...

    2015-09-21

    Here, a recent parcel model study (Reutter et al., 2009) showed three deterministic regimes of initial cloud droplet formation, characterized by different ratios of aerosol concentrations (NCN) to updraft velocities. This analysis, however, did not reveal how these regimes evolve during the subsequent cloud development. To address this issue, we employed the Active Tracer High Resolution Atmospheric Model (ATHAM) with full microphysics and extended the model simulation from the cloud base to the entire column of a single pyro-convective mixed-phase cloud. A series of 2-D simulations (over 1000) were performed over a wide range of NCN and dynamic conditions. Themore » integrated concentration of hydrometeors over the full spatial and temporal scales was used to evaluate the aerosol and dynamic effects. The results show the following. (1) The three regimes for cloud condensation nuclei (CCN) activation in the parcel model (namely aerosol-limited, updraft-limited, and transitional regimes) still exist within our simulations, but net production of raindrops and frozen particles occurs mostly within the updraft-limited regime. (2) Generally, elevated aerosols enhance the formation of cloud droplets and frozen particles. The response of raindrops and precipitation to aerosols is more complex and can be either positive or negative as a function of aerosol concentrations. The most negative effect was found for values of NCN of ~ 1000 to 3000 cm–3. (3) The nonlinear properties of aerosol–cloud interactions challenge the conclusions drawn from limited case studies in terms of their representativeness, and ensemble studies over a wide range of aerosol concentrations and other influencing factors are strongly recommended for a more robust assessment of the aerosol effects.« less

  2. Comprehensive mapping and characteristic regimes of aerosol effects on the formation and evolution of pyro-convective clouds

    SciTech Connect

    Chang, D.; Cheng, Y.; Reutter, P.; Trentmann, J.; Burrows, S. M.; Spichtinger, P.; Nordmann, S.; Andreae, M. O.; Poschl, U.; Su, H.

    2015-09-21

    Here, a recent parcel model study (Reutter et al., 2009) showed three deterministic regimes of initial cloud droplet formation, characterized by different ratios of aerosol concentrations (NCN) to updraft velocities. This analysis, however, did not reveal how these regimes evolve during the subsequent cloud development. To address this issue, we employed the Active Tracer High Resolution Atmospheric Model (ATHAM) with full microphysics and extended the model simulation from the cloud base to the entire column of a single pyro-convective mixed-phase cloud. A series of 2-D simulations (over 1000) were performed over a wide range of NCN and dynamic conditions. The integrated concentration of hydrometeors over the full spatial and temporal scales was used to evaluate the aerosol and dynamic effects. The results show the following. (1) The three regimes for cloud condensation nuclei (CCN) activation in the parcel model (namely aerosol-limited, updraft-limited, and transitional regimes) still exist within our simulations, but net production of raindrops and frozen particles occurs mostly within the updraft-limited regime. (2) Generally, elevated aerosols enhance the formation of cloud droplets and frozen particles. The response of raindrops and precipitation to aerosols is more complex and can be either positive or negative as a function of aerosol concentrations. The most negative effect was found for values of NCN of ~ 1000 to 3000 cm–3. (3) The nonlinear properties of aerosol–cloud interactions challenge the conclusions drawn from limited case studies in terms of their representativeness, and ensemble studies over a wide range of aerosol concentrations and other influencing factors are strongly recommended for a more robust assessment of the aerosol effects.

  3. BAECC Biogenic Aerosols - Effects on Clouds and Climate

    SciTech Connect

    Petäjä, Tuukka; Moisseev, Dmitri; Sinclair, Victoria; O'Connor, Ewan J.; Manninen, Antti J.; Levula, Janne; Väänänen, Riikka; Heikkinen, Liine; Äijälä, Mikko; Aalto, Juho; Bäck, Jaana

    2015-11-01

    “Biogenic Aerosols - Effects on Clouds and Climate (BAECC)”, featured the U.S. Department of Energy’s Atmospheric Radiation Measurement (ARM) Program’s 2nd Mobile Facility (AMF2) in Hyytiälä, Finland. It operated for an 8-month intensive measurement campaign from February to September 2014. The main research goal was to understand the role of biogenic aerosols in cloud formation. One of the reasons to perform BAECC study in Hyytiälä was the fact that it hosts SMEAR-II (Station for Measuring Forest Ecosystem-Atmosphere Relations), which is one of the world’s most comprehensive surface in-situ observation sites in a boreal forest environment. The station has been measuring atmospheric aerosols, biogenic emissions and an extensive suite of parameters relevant to atmosphere-biosphere interactions continuously since 1996. The BAECC enables combining vertical profiles from AMF2 with surface-based in-situ SMEAR-II observations and allows the processes at the surface to be directly related to processes occurring throughout the entire tropospheric column. With the inclusion of extensive surface precipitation measurements, and intensive observation periods involving aircraft flights and novel radiosonde launches, the complementary observations of AMF2 and SMEAR-II provide a unique opportunity for investigating aerosol-cloud interactions, and cloud-to-precipitation processes. The BAECC dataset will initiate new opportunities for evaluating and improving models of aerosol sources and transport, cloud microphysical processes, and boundary-layer structures.

  4. Coupling Between Oceanic Upwelling and Cloud-aerosol Properties at the AMF Point Reyes Site

    SciTech Connect

    Dunn, M.; Jensen, M.; Miller, M.; Kollias, P.; Bartholomew, M. J.; Turner, D.; Andrews, E.; Jefferson, A.; Daum, P.

    2008-03-10

    Cloud microphysical properties measured at the ARM Mobile Facility site located on the northern coast of California near Point Reyes, during the 2005 Marine Stratus Radiation, Aerosol and Drizzle experiment, were analyzed to determine their relationship to the coastal sea surface temperature (SST) which was characterized using measurements acquired from a National Oceanic and Atmospheric Administration offshore buoy. An increase in SST resulting from a relaxation of upwelling, occurring in the eastern Pacific Ocean off the coast of California in summer is observed to strongly correlate with nearby ground measured cloud microphysical properties and cloud condensation nuclei (CCN) concentrations. Correlations between these atmospheric and oceanic features provide insight into the interplay between the ocean and cloud radiative properties. We present evidence of this robust correlation and examine the factors controlling these features. The marine boundary layer is in direct contact with the sea surface and is strongly influenced by SST. Moisture and vertical motion are crucial ingredients for cloud development and so we examine the role of SST in providing these key components to the atmosphere. Although upwelling of cold subsurface waters is conventionally thought to increase aerosols in the region, thus increasing clouds, here we observed a relaxation of upwelling associated with changes in the structure of marine stratus clouds. As upwelling relaxes, the SST get warmer, thick clouds with high liquid water paths are observed and persist for a few days. This cycle is repeated throughout the summer upwelling season. A concomitant cyclic increase and decrease of CCN concentration is also observed. Forcing mechanisms and large-scale atmospheric features are discussed. Marine stratocumulus clouds are a critical component of the earth's radiation budget and this site provides an excellent opportunity to study the influence of SST on these clouds.

  5. Cloud droplet activation through oxidation of organic aerosol influenced by temperature and particle phase state

    NASA Astrophysics Data System (ADS)

    Slade, Jonathan H.; Shiraiwa, Manabu; Arangio, Andrea; Su, Hang; Pöschl, Ulrich; Wang, Jian; Knopf, Daniel A.

    2017-02-01

    Chemical aging of organic aerosol (OA) through multiphase oxidation reactions can alter their cloud condensation nuclei (CCN) activity and hygroscopicity. However, the oxidation kinetics and OA reactivity depend strongly on the particle phase state, potentially influencing the hydrophobic-to-hydrophilic conversion rate of carbonaceous aerosol. Here, amorphous Suwannee River fulvic acid (SRFA) aerosol particles, a surrogate humic-like substance (HULIS) that contributes substantially to global OA mass, are oxidized by OH radicals at different temperatures and phase states. When oxidized at low temperature in a glassy solid state, the hygroscopicity of SRFA particles increased by almost a factor of two, whereas oxidation of liquid-like SRFA particles at higher temperatures did not affect CCN activity. Low-temperature oxidation appears to promote the formation of highly-oxygenated particle-bound fragmentation products with lower molar mass and greater CCN activity, underscoring the importance of chemical aging in the free troposphere and its influence on the CCN activity of OA.

  6. Aerosol Cloud-Precipitation Interaction: Facts and Fiction

    NASA Astrophysics Data System (ADS)

    Cotton, W. R.; Levin, Z.

    2006-12-01

    In this talk we summarize the major findings and conclusions made in the WMO International Aerosol Precipitation Science Assessment Group (IAPSAG) report on aerosol impacts on precipitation. At the time of writing this abstract external reviews of the report have been received and by the time of the fall AGU meeting the final draft should be completed. The objective of the report is to stress the potential importance to the hydrological cycle of the effects of pollution on clouds and precipitation. We emphasize that once the precipitation cycle is altered in clouds by varying amounts of CCN, GCCN, and IN concentrations, the cloud responses can be vary nonlinear. Thus in some cases precipitation is decreased with increasing aerosols and others it is increased. Examples from modeling studies suggest that increased concentrations of CCN can lead to vertical redistributions in latent heating that can invigorate the updrafts of convective clouds and lead to large heavier raining storm systems. Other modeling studies indicate the opposite response and the indication is that it is due to the complex interplay of cold pools produced by storms and their mesoscale or large-scale environment. Thus it is dangerous to generalize that aerosols will always decrease or increase precipitation as the cloud response is a function of the variable large scale environment and the detailed nature of the cloud systems that form in those environments.

  7. Why do general circulation models overestimate the aerosol cloud lifetime effect? A case study comparing CAM5 and a CRM

    DOE PAGES

    Zhou, Cheng; Penner, Joyce E.

    2017-01-02

    Observation-based studies have shown that the aerosol cloud lifetime effect or the increase of cloud liquid water path (LWP) with increased aerosol loading may have been overestimated in climate models. Here, we simulate shallow warm clouds on 27 May 2011 at the southern Great Plains (SGP) measurement site established by the Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) program using a single-column version of a global climate model (Community Atmosphere Model or CAM) and a cloud resolving model (CRM). The LWP simulated by CAM increases substantially with aerosol loading while that in the CRM does not. The increase of LWP inmore » CAM is caused by a large decrease of the autoconversion rate when cloud droplet number increases. In the CRM, the autoconversion rate is also reduced, but this is offset or even outweighed by the increased evaporation of cloud droplets near the cloud top, resulting in an overall decrease in LWP. Our results suggest that climate models need to include the dependence of cloud top growth and the evaporation/condensation process on cloud droplet number concentrations.« less

  8. Why do general circulation models overestimate the aerosol cloud lifetime effect? A case study comparing CAM5 and a CRM

    NASA Astrophysics Data System (ADS)

    Zhou, Cheng; Penner, Joyce E.

    2017-01-01

    Observation-based studies have shown that the aerosol cloud lifetime effect or the increase of cloud liquid water path (LWP) with increased aerosol loading may have been overestimated in climate models. Here, we simulate shallow warm clouds on 27 May 2011 at the southern Great Plains (SGP) measurement site established by the Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) program using a single-column version of a global climate model (Community Atmosphere Model or CAM) and a cloud resolving model (CRM). The LWP simulated by CAM increases substantially with aerosol loading while that in the CRM does not. The increase of LWP in CAM is caused by a large decrease of the autoconversion rate when cloud droplet number increases. In the CRM, the autoconversion rate is also reduced, but this is offset or even outweighed by the increased evaporation of cloud droplets near the cloud top, resulting in an overall decrease in LWP. Our results suggest that climate models need to include the dependence of cloud top growth and the evaporation/condensation process on cloud droplet number concentrations.

  9. From hygroscopic aerosols to cloud droplets: The HygrA-CD campaign in the Athens basin - An overview.

    PubMed

    Papayannis, A; Argyrouli, A; Bougiatioti, A; Remoundaki, E; Vratolis, S; Nenes, A; Solomos, S; Komppula, M; Giannakaki, E; Kalogiros, J; Banks, R; Eleftheriadis, K; Mantas, E; Diapouli, E; Tzanis, C G; Kazadzis, S; Binietoglou, I; Labzovskii, L; Vande Hey, J; Zerefos, C S

    2017-01-01

    The international experimental campaign Hygroscopic Aerosols to Cloud Droplets (HygrA-CD), organized in the Greater Athens Area (GAA), Greece from 15 May to 22 June 2014, aimed to study the physico-chemical properties of aerosols and their impact on the formation of clouds in the convective Planetary Boundary Layer (PBL). We found that under continental (W-NW-N) and Etesian (NE) synoptic wind flow and with a deep moist PBL (~2-2.5km height), mixed hygroscopic (anthropogenic, biomass burning and marine) particles arrive over the GAA, and contribute to the formation of convective non-precipitating PBL clouds (of ~16-20μm mean diameter) with vertical extent up to 500m. Under these conditions, high updraft velocities (1-2ms(-1)) and cloud condensation nuclei (CCN) concentrations (~2000cm(-3) at 1% supersaturation), generated clouds with an estimated cloud droplet number of ~600cm(-3). Under Saharan wind flow conditions (S-SW) a shallow PBL (<1-1.2km height) develops, leading to much higher CCN concentrations (~3500-5000cm(-3) at 1% supersaturation) near the ground; updraft velocities, however, were significantly lower, with an estimated maximum cloud droplet number of ~200cm(-3) and without observed significant PBL cloud formation. The largest contribution to cloud droplet number variance is attributed to the updraft velocity variability, followed by variances in aerosol number concentration.

  10. On the determination of a cloud condensation nuclei from satellite: Challenges and possibilities

    NASA Astrophysics Data System (ADS)

    Kapustin, V. N.; Clarke, A. D.; Shinozuka, Y.; Howell, S.; Brekhovskikh, V.; Nakajima, T.; Higurashi, A.

    2006-02-01

    We use aerosol size distributions measured in the size range from 0.01 to 10+ μm during Transport and Chemical Evolution over the Pacific (TRACE-P) and Aerosol Characterization Experiment-Asia (ACE-Asia), results of chemical analysis, measured/modeled humidity growth, and stratification by air mass types to explore correlations between aerosol optical parameters and aerosol number concentration. Size distributions allow us to integrate aerosol number over any size range expected to be effective cloud condensation nuclei (CCN) and to provide definition of a proxy for CCN (CCNproxy). Because of the internally mixed nature of most accumulation mode aerosol and the relationship between their measured volatility and solubility, this CCNproxy can be linked to the optical properties of these size distributions at ambient conditions. This allows examination of the relationship between CCNproxy and the aerosol spectral radiances detected by satellites. Relative increases in coarse aerosol (e.g., dust) generally add only a few particles to effective CCN but significantly increase the scattering detected by satellite and drive the Angstrom exponent (α) toward zero. This has prompted the use of a so-called aerosol index (AI) on the basis of the product of the aerosol optical depth and the nondimensional α, both of which can be inferred from satellite observations. This approach biases the AI to be closer to scattering values generated by particles in the accumulation mode that dominate particle number and is therefore dominated by sizes commonly effective as CCN. Our measurements demonstrate that AI does not generally relate well to a measured proxy for CCN unless the data are suitably stratified. Multiple layers, complex humidity profiles, dust with very low α mixed with pollution, and size distribution differences in pollution and biomass emissions appear to contribute most to method limitations. However, we demonstrate that these characteristic differences result in

  11. Aerosol properties, source identification, and cloud processing in orographic clouds measured by single particle mass spectrometry on a Central European mountain site during HCCT-2010

    NASA Astrophysics Data System (ADS)

    Roth, A.; Schneider, J.; Klimach, T.; Mertes, S.; van Pinxteren, D.; Herrmann, H.; Borrmann, S.

    2015-09-01

    Cloud residues and out-of-cloud aerosol particles with diameters between 150 and 900 nm have been analysed by on-line single particle aerosol mass spectrometry during the six-week study HCCT-2010 in September/October 2010. The measurement location was the mountain Schmücke (937 m a.s.l.) in Central Germany. More than 170 000 bipolar mass spectra from out-of-cloud aerosol particles and more than 14 000 bipolar mass spectra from cloud residual particles were obtained and were classified using a fuzzy c-means clustering algorithm. Analysis of the uncertainty of the sorting algorithm was conducted on a subset of the data by comparing the clustering output with particle-by-particle inspection and classification by the operator. This analysis yielded a false classification probability between 13 and 48 %. Additionally, particle types were identified by specific marker ions. The results from the ambient aerosol analysis show that 63 % of the analysed particles belong to clusters indicating a diurnal variation, suggesting that local or regional sources dominate the aerosol, especially for particles containing soot and biomass burning particles. In the cloud residues the relative percentage of large soot-containing particles and particles containing amines was found to be increased compared to the out-of-cloud aerosol, while in general organic particles were less abundant in the cloud residues. In the case of amines this can be explained by the high solubility of the amines, while the large soot-containing particles were found to be internally mixed with inorganics, which explains their activation as cloud condensation nuclei. Furthermore, the results show that during cloud processing, both sulphate and nitrate are added to the residual particles, thereby changing the mixing state and increasing the fraction of particles with nitrate and/or sulphate. This is expected to lead to higher hygroscopicity after cloud evaporation, and therefore to an increase of the particles

  12. Organic peroxide and OH formation in aerosol and cloud water: laboratory evidence for this aqueous chemistry

    NASA Astrophysics Data System (ADS)

    Lim, Y. B.; Turpin, B. J.

    2015-06-01

    Aqueous chemistry in atmospheric waters (e.g., cloud droplets or wet aerosols) is well accepted as an atmospheric pathway to produce secondary organic aerosol (SOAaq). Water-soluble organic compounds with small carbon numbers (C2-C3) are precursors for SOAaq and products include organic acids, organic sulfates, and high molecular weight compounds/oligomers. Fenton reactions and the uptake of gas-phase OH radicals are considered to be the major oxidant sources for aqueous organic chemistry. However, the sources and availability of oxidants in atmospheric waters are not well understood. The degree to which OH is produced in the aqueous phase affects the balance of radical and non-radical aqueous chemistry, the properties of the resulting aerosol, and likely its atmospheric behavior. This paper demonstrates organic peroxide formation during aqueous photooxidation of methylglyoxal using ultra high resolution Fourier Transform Ion Cyclotron Resonance electrospray ionization mass spectrometry (FTICR-MS). Organic peroxides are known to form through gas-phase oxidation of volatile organic compounds. They contribute secondary organic aerosol (SOA) formation directly by forming peroxyhemiacetals, and epoxides, and indirectly by enhancing gas-phase oxidation through OH recycling. We provide simulation results of organic peroxide/peroxyhemiacetal formation in clouds and wet aerosols and discuss organic peroxides as a source of condensed-phase OH radicals and as a contributor to aqueous SOA.

  13. Quantification of Feedbacks in Aerosol-Cloud-Precipitation Interactions of Mixed-Phase Clouds

    NASA Astrophysics Data System (ADS)

    Glassmeier, F.; Herger, N.; Ramelli, F.; Lohmann, U.

    2014-12-01

    The notion of clouds as buffered or resilient systems implies that generalized feedback processes unaccounted for in climate simulations may lead to an overestimation of the effective radiative forcing due to aerosol-cloud interactions, i.e. cloud lifetime effects. In this contribution, we study the importance of microphysical feedback processes in response to anthropogenic aerosols in orographic mixed-phase clouds. Our methods can be extended to other cloud regimes as well as dynamical and thermodynamical feedbacks. For our simulations, we use the regional atmospheric model COSMO-ART-M7 in a 2D setup with an idealized mountain. To capture major processes from aerosol emission to precipitation, the model is coupled to a modal aerosol scheme and includes aerosol activation and heterogeneous freezing as well as two-moment cold and warm cloud microphysics. We perform simulations with aerosol conditions that vary in amount and chemical composition and thus perturb the warm- and ice-phase pathways of precipitation formation and their mixed-phase interactions. Our analysis is based on quantifying the interaction strength between aerosol, cloud and precipitation variables by susceptibilities, i.e. relative sensitivities d ln(Y) / d ln(X), where the change in variable Y is a response to a perturbation in variable X. We describe how to decompose susceptibilities into a direct response expected from the parameterization and a contribution from feedbacks. Resilience features similar magnitudes but opposite signs for those contributions, resulting in an overall small susceptibility. We find considerable contributions from feedbacks, which appear more important for warm-phase than for cold-phase processes. We do not observe, however, a trend for resilience in mixed-phase cloud microphysics. Moreover, feedback contributions seem of secondary importance when compared to the strong dependence of susceptibilities on the microphysical state of the cloud.

  14. Interpretation of FRESCO cloud retrievals in case of absorbing aerosol events

    NASA Astrophysics Data System (ADS)

    Wang, P.; Tuinder, O. N. E.; Tilstra, L. G.; Stammes, P.

    2011-12-01

    Cloud and aerosol information is needed in trace gas retrievals from satellite measurements. The Fast REtrieval Scheme for Clouds from the Oxygen A band (FRESCO) cloud algorithm employs reflectance spectra of the O2 A band around 760 nm to derive cloud pressure and effective cloud fraction. In general, clouds contribute more to the O2 A band reflectance than aerosols. Therefore, the FRESCO algorithm does not correct for aerosol effects in the retrievals and attributes the retrieved cloud information entirely to the presence of clouds, and not to aerosols. For events with high aerosol loading, aerosols may have a dominant effect, especially for almost cloud-free scenes. We have analysed FRESCO cloud data and Absorbing Aerosol Index (AAI) data from the Global Ozone Monitoring Experiment (GOME-2) instrument on the Metop-A satellite for events with typical absorbing aerosol types, such as volcanic ash, desert dust and smoke. We find that the FRESCO effective cloud fractions are correlated with the AAI data for these absorbing aerosol events and that the FRESCO cloud pressures contain information on aerosol layer pressure. For cloud-free scenes, the derived FRESCO cloud pressures are close to those of the aerosol layer for optically thick aerosols. For cloudy scenes, if the strongly absorbing aerosols are located above the clouds, then the retrieved FRESCO cloud pressures may represent the height of the aerosol layer rather than the height of the clouds. Combining FRESCO cloud data and AAI, an estimate for the aerosol layer pressure can be given, which can be beneficial for aviation safety and operations in case of e.g. volcanic ash plumes.

  15. multi-dimensional Cloud-aERosol Exploratory Study using RPAS (mCERES): Bottom-up and top-down closure of aerosol-cloud interactions

    NASA Astrophysics Data System (ADS)

    Roberts, Greg; Calmer, Radiance; Sanchez, Kevin; Cayez, Grégoire; Nicoll, Kerianne; Hashimshoni, Eyal; Rosenfeld, Daniel; Ansmann, Albert; Sciare, Jean; Ovadneite, Jurgita; Bronz, Murat; Hattenberger, Gautier; Preissler, Jana; Buehl, Johannes; Ceburnis, Darius; O'Dowd, Colin

    2016-04-01

    Clouds are omnipresent in earth's atmosphere and constitute an important role in regulating the radiative budget of the planet. However, the response of clouds to climate change remains uncertain, in particular, with respect to aerosol-cloud interactions and feedback mechanisms between the biosphere and atmosphere. Aerosol-cloud interactions and their feedbacks are the main themes of the European project FP7 BACCHUS (Impact of Biogenic versus Anthropogenic Emissions on Clouds and Climate: towards a Holistic Understanding). The National Center for Meteorological Research (CNRM-GAME, Toulouse, France) conducted airborne experiments in Cyprus and Ireland in March and August 2015 respectively to link ground-based and satellite observations. Multiple RPAS (remotely piloted aircraft systems) were instrumented for a specific scientific focus to characterize the vertical distribution of aerosol, cloud microphysical properties, radiative fluxes, 3D wind vectors and meteorological state parameters. Flights below and within clouds were coordinated with satellite overpasses to perform 'top-down' closure of cloud micro-physical properties. Measurements of cloud condensation nuclei spectra at the ground-based site have been used to determine cloud microphyical properties using wind vectors and meteorological parameters measured by the RPAS at cloud base. These derived cloud properties have been validated by in-situ RPAS measurements in the cloud and compared to those derived by the Suomi-NPP satellite. In addition, RPAS profiles in Cyprus observed the layers of dust originating from the Arabian Peninsula and the Sahara Desert. These profiles generally show a well-mixed boundary layer and compare well with ground-based LIDAR observations.

  16. Towards Bottom-up and Top-down Closures of Aerosol-cloud Interactions: multi-dimensional Cloud-aERosol Exploratory Study using RPAS

    NASA Astrophysics Data System (ADS)

    Roberts, G. C.; Calmer, R.; Sanchez, K. J.; Nicoll, K.; Hashimshoni, E.; Rosenfeld, D.; Ansmann, A.; Sciare, J.; Ovadnevaite, J.; Bronz, M.; Hattenberger, G.; Preissler, J.; Buehl, J.; Ceburnis, D.; O'Dowd, C. D. D.

    2015-12-01

    Clouds are omnipresent in earth's atmosphere and constitute an important role in regulating the radiative budget of the planet. However, the response of clouds to climate change remains uncertain, in particular, with respect to aerosol-cloud interactions and feedback mechanisms between the biosphere and atmosphere. Aerosol-cloud interactions and their feedbacks are the main themes of the European project FP7 BACCHUS (Impact of Biogenic versus Anthropogenic Emissions on Clouds and Climate: towards a Holistic Understanding). The National Center for Meteorological Research (CNRM-GAME, Toulouse, France) conducted airborne experiments in Cyprus and Ireland in March and August 2015 respectively to link ground-based and satellite observations. Multiple RPAS (remotely piloted aircraft systems) were instrumented for a specific scientific focus to characterize the vertical distribution of aerosol, cloud microphysical properties, radiative fluxes, 3D wind vectors and meteorological state parameters. Flights below and within clouds were coordinated with satellite overpasses to perform 'top-down' closure of cloud micro-physical properties. Measurements of cloud condensation nuclei spectra at the ground-based site have been used to determine cloud microphyical properties using wind vectors and meteorological parameters mesured by the RPAS at cloud base. These derived cloud properties have been validated by in-situ RPAS measurements in the cloud and compared to those derived by the Suomi-NPP satellite. In addition, RPAS profiles in Cyprus observed the layers of dust originating from the Arabian Peninsula and the Sahara Desert. These profiles generally show a well-mixed boundary layer and compare well with ground-based LIDAR observations.

  17. Aerosol-radiation-cloud interactions in a regional coupled model: the effects of convective parameterisation and resolution

    NASA Astrophysics Data System (ADS)

    Archer-Nicholls, Scott; Lowe, Douglas; Schultz, David M.; McFiggans, Gordon

    2016-05-01

    The Weather Research and Forecasting model with Chemistry (WRF-Chem) has been used to simulate a region of Brazil heavily influenced by biomass burning. Nested simulations were run at 5 and 1 km horizontal grid spacing for three case studies in September 2012. Simulations were run with and without fire emissions, convective parameterisation on the 5 km domain, and aerosol-radiation interactions in order to explore the differences attributable to the parameterisations and to better understand the aerosol direct effects and cloud responses. Direct aerosol-radiation interactions due to biomass burning aerosol resulted in a net cooling, with an average short-wave direct effect of -4.08 ± 1.53 Wm-2. However, around 21.7 Wm-2 is absorbed by aerosol in the atmospheric column, warming the atmosphere at the aerosol layer height, stabilising the column, inhibiting convection, and reducing cloud cover and precipitation. The changes to clouds due to radiatively absorbing aerosol (traditionally known as the semi-direct effects) increase the net short-wave radiation reaching the surface by reducing cloud cover, producing a secondary warming that counters the direct cooling. However, the magnitude of the semi-direct effect was found to be extremely sensitive to the model resolution and the use of convective parameterisation. Precipitation became organised in isolated convective cells when not using a convective parameterisation on the 5 km domain, reducing both total cloud cover and total precipitation. The SW semi-direct effect varied from 6.06 ± 1.46 with convective parameterisation to 3.61 ± 0.86 Wm-2 without. Convective cells within the 1 km domain are typically smaller but with greater updraft velocity than equivalent cells in the 5 km domain, reducing the proportion of the domain covered by cloud in all scenarios and producing a smaller semi-direct effect. Biomass burning (BB) aerosol particles acted as cloud condensation nuclei (CCN), increasing the droplet number

  18. Role of Clouds, Aerosols, and Aerosol-Cloud Interaction in 20th Century Simulations with GISS ModelE2

    NASA Technical Reports Server (NTRS)

    Nazarenko, Larissa; Rind, David; Bauer, Susanne; Del Genio, Anthony

    2015-01-01

    We use the new version of NASA Goddard Institute for Space Studies (GISS) climate model, modelE2 with 2º by 2.5º horizontal resolution and 40 vertical layers, with the model top at 0.1 hPa [Schmidt et al., 2014]. We use two different treatments of the atmospheric composition and aerosol indirect effect: (1) TCAD(I) version has fully interactive Tracers of Aerosols and Chemistry in both the troposphere and stratosphere. This model predicts total aerosol number and mass concentrations [Shindell et al., 2013]; (2) TCAM is the aerosol microphysics and chemistry model based on the quadrature methods of moments [Bauer et al., 2008]. Both TCADI and TCAM models include the first indirect effect of aerosols on clouds [Menon et al., 2010]; the TCAD model includes only the direct aerosol effect. We consider the results of the TCAD, TCADI and TCAM models coupled to "Russell ocean model" [Russell et al., 1995], E2-R. We examine the climate response for the "historical period" that include the natural and anthropogenic forcings for 1850 to 2012. The effect of clouds, their feedbacks, as well as the aerosol-cloud interactions are assessed for the transient climate change.

  19. Direct Numerical Simulation of Turbulent Condensation in Clouds

    NASA Technical Reports Server (NTRS)

    Shariff, K.; Paoli, R.

    2004-01-01

    In this brief, we investigate the turbulent condensation of a population of droplets by means of a direct numerical simulation. To that end, a coupled Navier-Stokes/Lagrangian solver is used where each particle is tracked and its growth by water vapor condensation is monitored exactly. The main goals of the study are to find out whether turbulence broadens the droplet size distribution, as observed in in situ measurements. The second issue is to understand if and for how long a correlation between the droplet radius and the local supersaturation exists for the purpose of modeling sub-grid scale microphysics in cloud-resolving codes. This brief is organized as follows. In Section 2 the governing equations are presented, including the droplet condensation model. The implementation of the forcing procedure is described in Section 3. The simulation results are presented in Section 4 together with a sketch of a simple stochastic model for turbulent condensation. Conclusions and the main outcomes of the study are given in Section 5.

  20. Organic aerosols

    SciTech Connect

    Penner, J.E.

    1994-01-01

    Organic aerosols scatter solar radiation. They may also either enhance or decrease concentrations of cloud condensation nuclei. This paper summarizes observed concentrations of aerosols in remote continental and marine locations and provides estimates for the sources of organic aerosol matter. The anthropogenic sources of organic aerosols may be as large as the anthropogenic sources of sulfate aerosols, implying a similar magnitude of direct forcing of climate. The source estimates are highly uncertain and subject to revision in the future. A slow secondary source of organic aerosols of unknown origin may contribute to the observed oceanic concentrations. The role of organic aerosols acting as cloud condensation nuclei (CCN) is described and it is concluded that they may either enhance or decrease the ability of anthropogenic sulfate aerosols to act as CCN.

  1. Observed aerosol effects on marine cloud nucleation and supersaturation

    NASA Astrophysics Data System (ADS)

    Russell, Lynn M.; Sorooshian, Armin; Seinfeld, John H.; Albrecht, Bruce A.; Nenes, Athanasios; Leaitch, W. Richard; Macdonald, Anne Marie; Ahlm, Lars; Chen, Yi-Chun; Coggon, Matthew; Corrigan, Ashley; Craven, Jill S.; Flagan, Richard C.; Frossard, Amanda A.; Hawkins, Lelia N.; Jonsson, Haflidi; Jung, Eunsil; Lin, Jack J.; Metcalf, Andrew R.; Modini, Robin; Mülmenstädt, Johannes; Roberts, Greg C.; Shingler, Taylor; Song, Siwon; Wang, Zhen; Wonaschütz, Anna

    2013-05-01

    Aerosol particles in the marine boundary layer include primary organic and salt particles from sea spray and combustion-derived particles from ships and coastal cities. These particle types serve as nuclei for marine cloud droplet activation, although the particles that activate depend on the particle size and composition as well as the supersaturation that results from cloud updraft velocities. The Eastern Pacific Emitted Aerosol Cloud Experiment (EPEACE) 2011 was a targeted aircraft campaign to assess how different particle types nucleate cloud droplets. As part of E-PEACE 2011, we studied the role of marine particles as cloud droplet nuclei and used emitted particle sources to separate particle-induced feedbacks from dynamical variability. The emitted particle sources included shipboard smoke-generated particles with 0.05-1 μm diameters (which produced tracks measured by satellite and had drop composition characteristic of organic smoke) and combustion particles from container ships with 0.05-0.2 μm diameters (which were measured in a variety of conditions with droplets containing both organic and sulfate components) [1]. Three central aspects of the collaborative E-PEACE results are: (1) the size and chemical composition of the emitted smoke particles compared to ship-track-forming cargo ship emissions as well as background marine particles, with particular attention to the role of organic particles, (2) the characteristics of cloud track formation for smoke and cargo ships, as well as the role of multi-layered low clouds, and (3) the implications of these findings for quantifying aerosol indirect effects. For comparison with the E-PEACE results, the preliminary results of the Stratocumulus Observations of Los-Angeles Emissions Derived Aerosol-Droplets (SOLEDAD) 2012 provided evidence of the cloud-nucleating roles of both marine organic particles and coastal urban pollution, with simultaneous measurements of the effective supersaturations of the clouds in the

  2. Picosecond laser-induced water condensation in a cloud chamber.

    PubMed

    Sun, Haiyi; Liu, Yonghong; Ju, Jingjing; Tian, Ye; Bai, Yafeng; Liu, Yaoxiang; Du, Shengzhe; Wang, Cheng; Wang, Tiejun; Liu, Jiansheng; Chin, See Leang; Li, Ruxin; Xu, Zhizhan

    2016-09-05

    We investigated water condensation in a laboratory cloud chamber induced by picosecond (ps) laser pulses at ~350 ps (800 nm/1-1000 Hz) with a maximum peak power of ~25 MW. The peak power was much lower than the critical power for self-focusing in air (~3-10 GW depending on the pulse duration). Sparks, airflow and snow formation were observed under different laser energies or repetition rates. It was found that weaker ps laser pulses can also induce water condensation by exploding and breaking down ice crystals and/or water droplets into tiny particles although there was no formation of laser filament. These tiny particles would grow until precipitation in a super-saturation zone due to laser-induced airflow in a cold region with a large temperature gradient.

  3. Marine microgels as a source of cloud condensation nuclei in the high Arctic.

    PubMed

    Orellana, Mónica V; Matrai, Patricia A; Leck, Caroline; Rauschenberg, Carlton D; Lee, Allison M; Coz, Esther

    2011-08-16

    Marine microgels play an important role in regulating ocean basin-scale biogeochemical dynamics. In this paper, we demonstrate that, in the high Arctic, marine gels with unique physicochemical characteristics originate in the organic material produced by ice algae and/or phytoplankton in the surface water. The polymers in this dissolved organic pool assembled faster and with higher microgel yields than at other latitudes. The reversible phase transitions shown by these Arctic marine gels, as a function of pH, dimethylsulfide, and dimethylsulfoniopropionate concentrations, stimulate the gels to attain sizes below 1 μm in diameter. These marine gels were identified with an antibody probe specific toward material from the surface waters, sized, and quantified in airborne aerosol, fog, and cloud water, strongly suggesting that they dominate the available cloud condensation nuclei number population in the high Arctic (north of 80°N) during the summer season. Knowledge about emergent properties of marine gels provides important new insights into the processes controlling cloud formation and radiative forcing, and links the biology at the ocean surface with cloud properties and climate over the central Arctic Ocean and, probably, all oceans.

  4. Marine microgels as a source of cloud condensation nuclei in the high Arctic

    PubMed Central

    Orellana, Mónica V.; Matrai, Patricia A.; Leck, Caroline; Rauschenberg, Carlton D.; Lee, Allison M.; Coz, Esther

    2011-01-01

    Marine microgels play an important role in regulating ocean basin-scale biogeochemical dynamics. In this paper, we demonstrate that, in the high Arctic, marine gels with unique physicochemical characteristics originate in the organic material produced by ice algae and/or phytoplankton in the surface water. The polymers in this dissolved organic pool assembled faster and with higher microgel yields than at other latitudes. The reversible phase transitions shown by these Arctic marine gels, as a function of pH, dimethylsulfide, and dimethylsulfoniopropionate concentrations, stimulate the gels to attain sizes below 1 μm in diameter. These marine gels were identified with an antibody probe specific toward material from the surface waters, sized, and quantified in airborne aerosol, fog, and cloud water, strongly suggesting that they dominate the available cloud condensation nuclei number population in the high Arctic (north of 80°N) during the summer season. Knowledge about emergent properties of marine gels provides important new insights into the processes controlling cloud formation and radiative forcing, and links the biology at the ocean surface with cloud properties and climate over the central Arctic Ocean and, probably, all oceans. PMID:21825118

  5. Characteristics of Interstitial Aerosol in Cold and Warm Clouds during the Ice-T Campaign

    NASA Astrophysics Data System (ADS)

    Dhaniyala, S.; He, M.; Moharreri, A.; Craig, L.

    2012-12-01

    Accurate calculation of the contribution of aerosols to the radiative forcing budget requires an understanding of the aerosol role in cloud formation. From a global climate perspective, aerosol-cloud processes must be represented by simple parametric models that can relate aerosol properties to the characteristics of the clouds formed. The development and testing of such simple models requires aerosol-cloud data from a large number of clouds systems. While reasonably accurate cloud data is currently available from a large number of well-established cloud probes, information about aerosol particles in clouds is largely unavailable because of the problem of artifacts in aerosol measurements from the shatter of cloud droplets. During the recent ICE-T campaign (Summer 2011), several different interstitial aerosol inlets were deployed and aerosol measurements were made in a variety of tropical convective clouds, focused particularly on conditions that permit the formation of ice within these systems. The flight operations were based in St. Croix, U.S. Virgin Islands and sampling was largely conducted within ~ 600 miles of this location. The use of new samplers that permit shatter-free sampling of aerosol particles in cold and clouds has allowed for the collection of significant data on interstitial aerosol in tropical convective clouds. Of particular interest are measurements of aerosol size distributions inside and outside clouds made with a fast mobility spectrometer. Size distributions were obtained at 20-30 second resolution, permitting direct measurements of the scavenged aerosol population in clouds and the differences in the scavenged fraction as a function of cloud properties. As part of this presentation, the characteristics of interstitial aerosol in various cloud conditions will be presented and the transformation of aerosol population during cloud processing will be discussed.

  6. Biomass Burning Aerosol Impact on Orographic Cloud Formation on Kilimanjaro

    NASA Astrophysics Data System (ADS)

    Nair, U. S.; Wu, Y.; Christopher, S. A.

    2014-12-01

    In addition to large scale climate change impacts, regional climate forcing due to land cover and land use change and biomass burning aerosols may also be relevant in understanding observed changes at Kilimanjaro. Analysis of satellite detected fires conducted for 2007 show substantial biomass burning in the vicinity of Kilimanjaro and maximum mid visible MODIS retrieved aerosol optical depth over Kilimanjaro during the month of July. For selected case days in 2007, numerical simulations were conducted using WRF Chem to assess the impact of biomass burning aerosols on orographic cloud formation on Kilimanjaro. Numerical modeling experiments with and without smoke emissions were conducted. Satellite derived smoke emissions are utilized in numerical model experiments considering biomass burning aerosol effects. Nested grid configuration was used in the experiments to establish a fine grid of 100 km x 100 km domain and 1 km grid spacing over the complex terrain of Kilimanjaro. For case days considered, numerical model simulations show substantial impact of biomass burning aerosols on orographic cloud formation. There is a net increase in cloud liquid water path with maximum increase in excess of 10%. Orographic precipitation also show increase in rainfall of up to 10% at higher elevations. Whereas there is average reduction in downwelling solar radiation 18 Wm-2 up to elevations of 5000m, impacts at the mountain peaks are minimal. Processes leading to the differences in cloud formation and results from numerical simulations are conducted for additional case study days during other seasons and will be discussed

  7. Evaluating Global Aerosol Models and Aerosol and Water Vapor Properties Near Clouds

    SciTech Connect

    Turner, David, D.; Ferrare, Richard, A.

    2011-07-06

    The 'Evaluating Global Aerosol Models and Aerosol and Water Vapor Properties Near Clouds' project focused extensively on the analysis and utilization of water vapor and aerosol profiles derived from the ARM Raman lidar at the Southern Great Plains ARM site. A wide range of different tasks were performed during this project, all of which improved quality of the data products derived from the lidar or advanced the understanding of atmospheric processes over the site. These activities included: upgrading the Raman lidar to improve its sensitivity; participating in field experiments to validate the lidar aerosol and water vapor retrievals; using the lidar aerosol profiles to evaluate the accuracy of the vertical distribution of aerosols in global aerosol model simulations; examining the correlation between relative humidity and aerosol extinction, and how these change, due to horizontal distance away from cumulus clouds; inferring boundary layer turbulence structure in convective boundary layers from the high-time-resolution lidar water vapor measurements; retrieving cumulus entrainment rates in boundary layer cumulus clouds; and participating in a field experiment that provided data to help validate both the entrainment rate retrievals and the turbulent profiles derived from lidar observations.

  8. Clouds, aerosols, and photochemistry in the Jovian atmosphere

    NASA Technical Reports Server (NTRS)

    West, R. A.; Strobel, D. F.; Tomasko, M. G.

    1986-01-01

    An assessment is made of the development status of concepts for cloud and aerosol compositions, vertical and horizontal distributions, and microphysical properties, in the Jovian upper troposphere and stratosphere. Attention is given to several key photochemical species' relationships to aerosol formation as well as their transport process implications, treating photochemistry in the context of comparative planetology and noting differences and similarities among the outer planet atmospheres; since this approach emphasizes observational data, a variegated assortment of ground-based and spacecraft observations is assembled. Current views on the tropospheric distribution of clouds are challenged, and a rationale is presented for alternative accounts.

  9. Clouds, aerosols, and photochemistry in the Jovian atmosphere

    NASA Astrophysics Data System (ADS)

    West, R. A.; Strobel, D. F.; Tomasko, M. G.

    1986-03-01

    An assessment is made of the development status of concepts for cloud and aerosol compositions, vertical and horizontal distributions, and microphysical properties, in the Jovian upper troposphere and stratosphere. Attention is given to several key photochemical species' relationships to aerosol formation as well as their transport process implications, treating photochemistry in the context of comparative planetology and noting differences and similarities among the outer planet atmospheres; since this approach emphasizes observational data, a variegated assortment of ground-based and spacecraft observations is assembled. Current views on the tropospheric distribution of clouds are challenged, and a rationale is presented for alternative accounts.

  10. Cloud droplet activity changes of soot aerosol upon smog chamber ageing

    NASA Astrophysics Data System (ADS)

    Wittbom, C.; Pagels, J. H.; Rissler, J.; Eriksson, A. C.; Carlsson, J. E.; Roldin, P.; Nordin, E. Z.; Nilsson, P. T.; Swietlicki, E.; Svenningsson, B.

    2014-04-01

    Particles containing soot, or black carbon, are generally considered to contribute to global warming. However, large uncertainties remain in the net climate forcing resulting from anthropogenic emissions of black carbon (BC), to a large extent due to the fact that BC is co-emitted with gases and primary particles, both organic and inorganic, and subject to atmospheric ageing processes. In this study, diesel exhaust particles and particles from a flame soot generator spiked with light aromatic secondary organic aerosol (SOA) precursors were processed by UV-radiation in a 6 m3 Teflon chamber in the presence of NOx. The time-dependent changes of the soot nanoparticle properties were characterised using a Cloud Condensation Nuclei Counter, an Aerosol Particle Mass Analyzer and a Soot Particle Aerosol Mass Spectrometer. The results show that freshly emitted soot particles do not activate into cloud droplets at supersaturations ≤ 2%, i.e. the black carbon core coated with primary organic aerosol (POA) from the exhaust is limited in hygroscopicity. Before the onset of UV radiation it is unlikely that any substantial SOA formation is taking place. An immediate change in cloud-activation properties occurs at the onset of UV exposure. This change in hygroscopicity is likely attributed to SOA formed from intermediate volatile organic compounds (IVOC) in the diesel engine exhaust. The change of cloud condensation nuclei (CCN) properties at the onset of UV radiation implies that the lifetime of soot particles in the atmosphere is affected by the access to sunlight, which differs between latitudes. The ageing of soot particles progressively enhances their ability to act as cloud condensation nuclei, due to changes in: (I) organic fraction of the particle, (II) chemical properties of this fraction (POA or SOA), (III) particle size, and (IV) particle morphology. Applying κ-Köhler theory, using a κSOA value of 0.13 (derived from independent input parameters describing the

  11. Effect of aerosol number concentration on cloud droplet dispersion: A large-eddy simulation study and implications for aerosol indirect forcing

    NASA Astrophysics Data System (ADS)

    Lu, Miao-Ling; Seinfeld, John H.

    2006-01-01

    Through three-dimensional large-eddy simulations of marine stratocumulus we explore the factors that control the cloud spectral relative dispersion (ratio of cloud droplet spectral width to the mean radius of the distribution) as a function of aerosol number concentration and the extent to which the relative dispersion either enhances or mitigates the Twomey effect. We find that relative dispersion decreases with increasing aerosol number concentration (for aerosol number concentrations less than about 1000 cm-3) because smaller droplets resulting from higher aerosol number concentrations inhibit precipitation and lead to (1) less spectral broadening by suppressed collision and coalescence processes and (2) more spectral narrowing by droplet condensational growth at higher updraft velocity because reduced drizzle latent heating at cloud top results in increased boundary layer turbulent kinetic energy production by buoyancy and thereby stronger turbulence. Increased spectral broadening owing to increased cloud-top entrainment mixing, also as a result of increased boundary layer turbulence, is relatively insignificant compared with outcomes 1 and 2. The coefficient k, an important parameter that relates cloud droplet effective radius and volume mean radius in large-scale models, is a function of skewness and relative dispersion of the distribution and is negatively correlated with relative dispersion. Increasing k with increasing aerosol number concentration leads to maximum enhancement of the cloud susceptibility (the change of cloud optical depth due to change of cloud droplet number concentration) over that attributable to the Twomey effect alone by about 4.2% and 39% for simulated FIRE and ASTEX cases, respectively.

  12. Campaign datasets for ARM Cloud Aerosol Precipitation Experiment (ACAPEX)

    SciTech Connect

    Leung, L. Ruby; Mei, Fan; Comstock, Jennifer; DeMott, Paul; Gero, Jonathan; Hubee, John; Matthews, Alyssa; Nalli, Nicholas; Pekour, Mikhail; Prather, Kimberly; Sedlackek, Arthur; Springston, Stephen; Tomlinson, Jason; Chand, Duli

    2015-08-12

    This campaign consisted of the deployment of the DOE ARM Mobile Facility 2 (AMF2) and the ARM Aerial Facility (AAF) G-1 in a field campaign called ARM Cloud Aerosol Precipitation Experiment (ACAPEX), which took place in conjunction with CalWater 2- a NOAA field campaign. The joint CalWater 2/ACAPEX field campaign aimed to improve understanding and modeling of large-scale dynamics and cloud and precipitation processes associated with ARs and aerosol-cloud interactions that influence precipitation variability and extremes in the western U.S. The observational strategy consisted of the use of land and offshore assets to monitor: 1. the evolution and structure of ARs from near their regions of development 2. the long-range transport of aerosols in the eastern North Pacific and potential interactions with ARs 3. how aerosols from long-range transport and local sources influence cloud and precipitation in the U.S. West Coast where ARs make landfall and post-frontal clouds are frequent.

  13. Dimethyl sulfide as a source of cloud condensation nuclei

    SciTech Connect

    Warren, S.

    1995-09-01

    Cloud condensation nuclei (CCN) are predominantly sulfate particles, and over the oceans the major source of sulfur for these particles appears to be dimethyl sulfide, a gas produced by marine biota. The reflection of sunlight by marine stratiform clouds is a major feature of the Earth`s radiation budget, and these clouds will reflect more sunlight if their liquid water is distributed among more CCN, thus forming more (and smaller) droplets. These facts form the basis of a proposal that marine biogenic sulfur may be an important factor in determining the Earth`s climate. Key implications of this proposal are (1) the possibility of a biota-climate feedback loop if the production of biogenic sulfur is sensitive to changes in climate, (2) the possibility that anthropogenic sulfur emissions may be altering the global climate through this cloud-mediated mechanism, and (3) the possibility that anthropogenic pollution could alter climate by perturbing the sulfur-producing marine organisms. 3 refs., 1 fig.

  14. Final Report for LDRD Project ''A New Era of Research in Aerosol/Cloud/Climate Interactions at LLNL''

    SciTech Connect

    Chuang, C; Bergman, D J; Dignon, J E; Connell, P S

    2002-01-31

    Observations of global temperature records seem to show less warming than predictions of global warming brought on by increasing concentrations of CO{sub 2} and other greenhouse gases. One of the reasonable explanations for this apparent inconsistency is that the increasing concentrations of anthropogenic aerosols may be partially counteracting the effects of greenhouse gases. Aerosols can scatter or absorb the solar radiation, directly change the planetary albedo. Aerosols, unlike CO{sub 2}, may also have a significant indirect effect by serving as cloud condensation nuclei (CCN). Increases in CCN can result in clouds with more but smaller droplets, enhancing the reflection of solar radiation. Aerosol direct and indirect effects are a strong function of the distributions of all aerosol types and the size distribution of the aerosol in question. However, the large spatial and temporal variabilities in the concentration, chemical characteristics, and size distribution of aerosols have made it difficult to assess the magnitude of aerosol effects on atmospheric radiation. These variabilities in aerosol characteristics as well as their effects on clouds are the leading sources of uncertainty in predicting future climate variation. Inventory studies have shown that the present-day anthropogenic emissions contribute more than half of fine particle mass primarily due to sulfate and carbonaceous aerosols derived from fossil fuel combustion and biomass burning. Parts of our earlier studies have been focused on developing an understanding of global sulfate and carbonaceous aerosol abundances and investigating their climate effects [Chuang et al., 1997; Penner et al., 1998]. We have also modeled aerosol optical properties to account for changes in the refractive indices with relative humidity and dry aerosol composition [Grant et al., 1999]. Moreover, we have developed parameterizations of cloud response to aerosol abundance for use in global models to evaluate the importance

  15. An Observational Study of the Relationship between Cloud, Aerosol and Meteorology in Broken Low-Level Cloud Conditions

    NASA Technical Reports Server (NTRS)

    Loeb, Norman G.; Schuster, Gregory L.

    2008-01-01

    Global satellite analyses showing strong correlations between aerosol optical depth and 3 cloud cover have stirred much debate recently. While it is tempting to interpret the results as evidence of aerosol enhancement of cloud cover, other factors such as the influence of meteorology on both the aerosol and cloud distributions can also play a role, as both aerosols and clouds depend upon local meteorology. This study uses satellite observations to examine aerosol-cloud relationships for broken low-level cloud regions off the coast of Africa. The analysis approach minimizes the influence of large-scale meteorology by restricting the spatial and temporal domains in which the aerosol and cloud properties are compared. While distributions of several meteorological variables within 5deg 5deg latitude-longitude regions are nearly identical under low and high aerosol optical depth, the corresponding distributions of single-layer low cloud properties and top-of-atmosphere radiative fluxes differ markedly, consistent with earlier studies showing increased cloud cover with aerosol optical depth. Furthermore, fine-mode fraction and Angstrom Exponent are also larger in conditions of higher aerosol optical depth, even though no evidence of systematic latitudinal or longitudinal gradients between the low and high aerosol optical depth populations are observed. When the analysis is repeated for all 5deg 5deg latitude-longitude regions over the global oceans (after removing cases in which significant meteorological differences are found between the low and high aerosol populations), results are qualitatively similar to those off the coast of Africa.

  16. Enhanced shortwave cloud radiative forcing due to anthropogenic aerosols

    SciTech Connect

    Schwartz, S.E.; Slingo, A.

    1995-05-01

    It has been suggested that anthropogenic aerosols in the troposphere can influence the microphysical properties of clouds and in turn their reflectivity, thereby exerting a radiative influence on climate. This article presents the theoretical basis for of this so-called indirect forcing and reviews pertinent observational evidence and climate model calculations of its magnitude and geographical distribution. We restrict consideration to liquid-water clouds.

  17. Aerosol-Cloud-Radiation Interactions in Atmospheric Forecast Models

    DTIC Science & Technology

    2007-09-30

    combustion, biomass burning, and biogenic activity are sources of particulate oxalic acid ; photooxidation of volatile organic compounds (VOCs...acids are likely particle-phase compounds formed by cloud and fog processing. Oxalic acid , which has also been shown to be formed by aqueous-phase...chemistry in cloud droplets, remains in the aerosol phase after subsequent droplet evaporation. In the aqueous phase, oxalic acid is formed by oxidation

  18. The global aerosol-cloud first indirect effect estimated using MODIS, MERRA, and AeroCom

    NASA Astrophysics Data System (ADS)

    McCoy, D. T.; Bender, F. A.-M.; Mohrmann, J. K. C.; Hartmann, D. L.; Wood, R.; Grosvenor, D. P.

    2017-02-01

    Aerosol-cloud interactions (ACI) represent a significant source of forcing uncertainty in global climate models (GCMs). Estimates of radiative forcing due to ACI in Fifth Assessment Report range from -0.5 to -2.5 W m-2. A portion of this uncertainty is related to the first indirect, or Twomey, effect whereby aerosols act as nuclei for cloud droplets to condense upon. At constant liquid water content this increases the number of cloud droplets (Nd) and thus increases the cloud albedo. In this study we use remote-sensing estimates of Nd within stratocumulus regions in combination with state-of-the-art aerosol reanalysis from Modern-Era Retrospective Analysis for Research and Applications version 2 (MERRA2) to diagnose how aerosols affect Nd. As in previous studies, Nd is related to sulfate mass through a power law relationship. The slope of the log-log relationship between Nd and SO4 in maritime stratocumulus is found to be 0.31, which is similar to the range of 0.2-0.8 from previous in situ studies and remote-sensing studies in the pristine Southern Ocean. Using preindustrial emissions models, the change in Nd between preindustrial and present day is estimated. Nd is inferred to have more than tripled in some regions. Cloud properties from Moderate Resolution Imaging Spectroradiometer (MODIS) are used to estimate the radiative forcing due to this change in Nd. The Twomey effect operating in isolation is estimated to create a radiative forcing of -0.97 ± 0.23 W m-2 relative to the preindustrial era.

  19. Prediction of cloud condensation nuclei activity for organic compounds using functional group contribution methods

    DOE PAGES

    Petters, M. D.; Kreidenweis, S. M.; Ziemann, P. J.

    2016-01-19

    A wealth of recent laboratory and field experiments demonstrate that organic aerosol composition evolves with time in the atmosphere, leading to changes in the influence of the organic fraction to cloud condensation nuclei (CCN) spectra. There is a need for tools that can realistically represent the evolution of CCN activity to better predict indirect effects of organic aerosol on clouds and climate. This work describes a model to predict the CCN activity of organic compounds from functional group composition. Following previous methods in the literature, we test the ability of semi-empirical group contribution methods in Köhler theory to predict themore » effective hygroscopicity parameter, kappa. However, in our approach we also account for liquid–liquid phase boundaries to simulate phase-limited activation behavior. Model evaluation against a selected database of published laboratory measurements demonstrates that kappa can be predicted within a factor of 2. Simulation of homologous series is used to identify the relative effectiveness of different functional groups in increasing the CCN activity of weakly functionalized organic compounds. Hydroxyl, carboxyl, aldehyde, hydroperoxide, carbonyl, and ether moieties promote CCN activity while methylene and nitrate moieties inhibit CCN activity. The model can be incorporated into scale-bridging test beds such as the Generator of Explicit Chemistry and Kinetics of Organics in the Atmosphere (GECKO-A) to evaluate the evolution of kappa for a complex mix of organic compounds and to develop suitable parameterizations of CCN evolution for larger-scale models.« less

  20. Prediction of cloud condensation nuclei activity for organic compounds using functional group contribution methods

    NASA Astrophysics Data System (ADS)

    Petters, M. D.; Kreidenweis, S. M.; Ziemann, P. J.

    2016-01-01

    A wealth of recent laboratory and field experiments demonstrate that organic aerosol composition evolves with time in the atmosphere, leading to changes in the influence of the organic fraction to cloud condensation nuclei (CCN) spectra. There is a need for tools that can realistically represent the evolution of CCN activity to better predict indirect effects of organic aerosol on clouds and climate. This work describes a model to predict the CCN activity of organic compounds from functional group composition. Following previous methods in the literature, we test the ability of semi-empirical group contribution methods in Köhler theory to predict the effective hygroscopicity parameter, kappa. However, in our approach we also account for liquid-liquid phase boundaries to simulate phase-limited activation behavior. Model evaluation against a selected database of published laboratory measurements demonstrates that kappa can be predicted within a factor of 2. Simulation of homologous series is used to identify the relative effectiveness of different functional groups in increasing the CCN activity of weakly functionalized organic compounds. Hydroxyl, carboxyl, aldehyde, hydroperoxide, carbonyl, and ether moieties promote CCN activity while methylene and nitrate moieties inhibit CCN activity. The model can be incorporated into scale-bridging test beds such as the Generator of Explicit Chemistry and Kinetics of Organics in the Atmosphere (GECKO-A) to evaluate the evolution of kappa for a complex mix of organic compounds and to develop suitable parameterizations of CCN evolution for larger-scale models.

  1. Cloud water measurements of glyoxal and methylglyoxal during the Whistler Aerosol and Cloud Study (WACS)

    NASA Astrophysics Data System (ADS)

    Herckes, P.; Ervens, B.; Wang, Y.; Eagar, J.; Leaitch, R.; Macdonald, A.; Sjostedt, S.; Abbatt, J.

    2011-12-01

    Glyoxal and methylglyoxal are produced in high yields from both anthropogenic (aromatics) and biogenic (isoprene) precursors. The role of glyoxal and methylglyoxal in secondary organic aerosol (SOA) formation in the aqueous phase of cloud water and aerosols has received great attention over the past years. In addition, gas phase oxidation and photolysis of these compounds yield radicals and, thus, impact the oxidant budgets. While the reactivity of methylglyoxal and glyoxal in both the gas and aqueous phases is nearly identical, the much higher solubility of glyoxal leads to its more efficient removal in the presence of clouds. Thus, the amount of cloud water (liquid water content, LWC) and cloud processing time will affect the concentration ratios and thus the reaction rates of oxidation processes in the gas and aqueous phase, respectively. The Whistler Aerosol and Cloud Study (WACS) investigated the interactions between clouds and biogenic aerosol in summer 2010 in Whistler (Canada). During this study, cloud samples were collected at two locations, Whistler peak and a mid mountain station Raven's Nest. Cloud samples were extensively chemically characterized including the measurements of glyoxal and methylglyoxal using liquid chromatography coupled to UV and mass spectrometric detection after derivatization. Concentrations were variable on the order of micromoles, accounting for 1% of the dissolved organic matter in clouds. Glyoxal and methylglyoxal concentrations at both locations are predicted by means of model studies using VOC measurements and liquid water contents as input data. These concentrations and their ratios are compared to those in different regions. It will be discussed how cloud liquid water content, cloud processing time and amount and mixture of precursors (emissions) affect these concentration ratios. Finally, the role of different emission scenarios and the presence of clouds for SOA formation and radical budgets will be briefly assessed.

  2. Regime-based analysis of aerosol-cloud interactions

    NASA Astrophysics Data System (ADS)

    Gryspeerdt, Edward; Stier, Philip

    2012-11-01

    Previous global satellite studies into the indirect aerosol effect have relied on determining the sensitivity of derived Cloud Droplet Number Concentration (Nd) to co-located Aerosol Optical Depth (AOD). These studies generally find a positive Nd sensitivity to AOD changes over ocean, but some find a negative sensitivity over land, in contrast to that predicted by models and theory. Here we investigate the Nd sensitivity to AOD in different cloud regimes, determined using a k-means clustering process on retrieved cloud properties. We find the strongest positive Nd sensitivity in the stratiform regimes over both land and ocean, providing the majority of the total sensitivity. The negative sensitivity previously observed over land is generated by the low cloud fraction regimes, suggesting that it is due to the difficulty of retrieving Nd at low cloud fractions. When considering a mean sensitivity, weighted by liquid cloud fraction to account for sampling biases, we find an increased sensitivity over land, in some regions becoming positive. This highlights the importance of regime based analysis when studying aerosol indirect effects.

  3. Examination of the potential impacts of dust and pollution aerosol acting as cloud nucleating aerosol on water resources in the Colorado River Basin

    NASA Astrophysics Data System (ADS)

    Jha, Vandana

    In this study we examine the cumulative effect of dust acting as cloud nucleating aerosol (cloud condensation nuclei (CCN), giant cloud condensation nuclei (GCCN), and ice nuclei (IN)) along with anthropogenic aerosol pollution acting primarily as CCN, over the entire Colorado Rocky Mountains from the months of October to April in the year 2004-2005; the snow year. This ˜6.5 months analysis provides a range of snowfall totals and variability in dust and anthropogenic aerosol pollution. The specific objectives of this research is to quantify the impacts of both dust and pollution aerosols on wintertime precipitation in the Colorado Mountains using the Regional Atmospheric Modeling System (RAMS). In general, dust enhances precipitation primarily by acting as IN, while aerosol pollution reduces water resources in the CRB via the so-called "spill-over" effect, by enhancing cloud droplet concentrations and reducing riming rates. Dust is more episodic and aerosol pollution is more pervasive throughout the winter season. Combined response to dust and aerosol pollution is a net reduction of water resources in the CRB. The question is by how much are those water resources affected? Our best estimate is that total winter-season precipitation loss for for the CRB the 2004-2005 winter season due to the combined influence of aerosol pollution and dust is 5,380,00 acre-feet of water. Sensitivity studies for different cases have also been run for the specific cases in 2004-2005 winter season to analyze the impact of changing dust and aerosol ratios on precipitation in the Colorado River Basin. The dust is varied from 3 to 10 times in the experiments and the response is found to be non monotonic and depends on various environmental factors. The sensitivity studies show that adding dust in a wet system increases precipitation when IN affects are dominant. For a relatively dry system high concentrations of dust can result in over-seeding the clouds and reductions in precipitation

  4. New capabilities for space-based cloud and aerosols measurements: The Cloud-Aerosol Transport System (CATS)

    NASA Astrophysics Data System (ADS)

    Yorks, J. E.; McGill, M. J.; Hlavka, D. L.; Palm, S. P.; Hart, W. D.; Nowottnick, E. P.; Vaughan, M.; Rodier, S. D.; Colarco, P. R.; da Silva, A.; Buchard-Marchant, V.

    2013-12-01

    Current uncertainties in cloud and aerosol properties limit our ability to accurately model the Earth's climate system and predict climate change. These limitations are due primarily to difficulties in adequately measuring aerosols and clouds on a global scale. NASA's A-Train satellites provide an unprecedented opportunity to address these uncertainties. In particular, the Cloud-Aerosol Lidar Infrared Pathfinder Spaceborne Observations (CALIPSO) satellite provides vertical profiles of cloud and aerosol properties. The CALIOP lidar onboard CALIPSO has reached its seventh year of operation, well past its expected lifetime. The ATLID lidar on EarthCARE is not expected to launch until 2016 or later. If the CALIOP lidar fails before a new mission is operational, there will be a gap in global lidar measurements. The Cloud-Aerosol Transport System (CATS), built at NASA Goddard Space Flight Center as a payload for the International Space Station (ISS), is set to launch in the summer of 2014. CATS is an elastic backscatter lidar with three wavelengths (1064, 532, 355 nm) and HSRL capability at 532 nm. Depolarization measurements will be made at all three wavelengths. The ISS orbit is a 51 degree inclination orbit at an altitude of about 405 km. This orbit provides more comprehensive coverage of the tropics and mid-latitudes than sun-synchronous orbiting sensors, with nearly a three day repeat cycle. Thus, science applications of CATS include cloud and aerosol climate studies, air quality monitoring, and smoke/volcanic plume tracking. The primary science objectives of CATS include: continuing the CALIPSO aerosol and cloud vertical profile data record, providing near real time data to support operational applications such as air quality modeling, and advancing technology in support of future mission development using the HSRL channel. Furthermore, the vertical profiles of cloud and aerosol properties provided by CATS will complement current and future passive satellite

  5. Distinct Impacts of Aerosols on an Evolving Continental Cloud System during the RACORO Field Campaign

    NASA Astrophysics Data System (ADS)

    Lin, Y.; Wang, Y.; Zhang, R.; Liu, Y.

    2015-12-01

    Aerosol-cloud interactions have been investigated extensively but still remain high uncertainty due to the complexity of cloud microphysical processes under various dynamic and thermodynamic environments. Cloud-resolving Weather Research and Forecast (CR-WRF) model implemented with a two-moment bulk microphysics and a modified Goddard radiation scheme is employed to investigate aerosol effects on different cloud regimes and their transitions associated with a continental cloud system occurring from 25 May to 27 May, 2009 during the Department of Energy Atmospheric Radiation Measurement Routine AAF Clouds with Low Optical Water Depths Optical Radiative Observations (RACORO) field campaign. The simulated cloud properties and precipitation for the three different cloud regimes, including shallow cumuli, a deep convective cloud (DCC), and a stratus exhibit overall agreements with airborne and ground-based observations. Sensitivity studies with different aerosol scenarios reveal that the responses of cloud micro- and macrophysics to aerosol loading depend on the cloud regimes with monotonic or non-monotonic trend. Aerosol radiative effects modify the atmospheric thermodynamic condition and change the atmospheric stability, which induce different response from aerosol indirect effects. Our results also indicate that the overall aerosol effects on a cloud complex are distinct from those of the individual cloud types. The aerosol-cloud interaction for the different cloud regimes should be evaluated to assess the aerosol direct and indirect radiative forcings on regional and global climate.

  6. Cloud Condensation Nuclei Activity Associated with Chemical Composition and Precipitation Events

    NASA Astrophysics Data System (ADS)

    Corrigan, C.; Roberts, G. C.; Zauscher, M.; Suski, K.; Noblitts, S.; Sullivan, A. P.; Collett, J. L.

    2010-12-01

    Measurements of ambient cloud condensation nuclei (CCN) concentrations can be improved by simultaneously collecting information on the activation size of the CCN along with chemical composition of the ambient aerosol. A size scanning CCN instrument developed at Scripps Institution of Oceanography was deployed as part of the Calwater project in the Sierra Nevada foothills of California during February and March of 2010. The instrument was capable of determining the critical diameter of activation for the ambient aerosol during a 20 minute scan. During the study period, the CCN activation size increased after each rain event and the activity slowly returned over the next few days. The critical diameter of the overall aerosol was largest (least active) immediately following precipitation events. The average critical diameter would typically decrease by 20% in the time between major precipitation events. This regeneration of the CCN activity can be partially attributed to the transport of sulfate and nitrate pollution to replace the particles that were washed out by the rain, but it may also be due to chemical changes via aging and oxidation mechanisms. Since CCN activity is determined by the particles size and chemical composition, the changes in critical diameter indicate a change in the chemical composition of the available CCN particles. By comparing the critical diameters with aerosol chemical data from a semi-real time aerosol ion chromatograph, the CCN activity was generally correlated with the mass loading of sulfate and nitrate. Deviations from the expected activity of sulfate and nitrate indicate the existence of other compounds that contribute to activity through additional dissolution and by reducing the surface tension. The contribution to CCN activity from additional compounds, including organic surfactants, can be estimated by observing the deviation of the measured critical diameters from values calculated using only the measured nitrate+sulfate mass

  7. Aerosol-Cloud-Precipitation Interactions over Indo-Gangetic Basin

    NASA Technical Reports Server (NTRS)

    Tsay, S.-C.; Lau, K. .; Holben, B. N.; Hsu, N. C.; Bhartia, P. K.

    2005-01-01

    About 60% of world population reside in Asia, in term of which sheer population density presents a major environmental stress. Economic expansion in this region is, in fact, accompanied by increases in bio-fuel burning, industrial pollution, and land cover and land use changes. With a growth rate of approx. 8%/yr for Indian economy, more than 600 million people from Lahore, Pakistan to Calcutta, India over the Indo-Gangetic Basin have particularly witnessed increased frequencies of floods and droughts as well as a dramatic increase in atmospheric loading of aerosols (i.e., anthropogenic and natural aerosol) in recent decades. This regional change (e.g., aerosol, cloud, precipitation, etc.) will constitute a vital part of the global change in the 21st century. Better understanding of the impacts of aerosols in affecting monsoon climate and water cycles is crucial in providing the physical basis to improve monsoon climate prediction and for disaster mitigation. Based on climate model simulations, absorbing aerosols (dust and black carbon) play a critical role in affecting interannual and intraseasonal variability of the Indian monsoon. An initiative on the integrated (aerosols, clouds, and precipitation) measurements approach over the Indo-Gangetic Basin will be discussed. An array of ground-based (e.g., AERONET, MPLNET, SMART-COMMIT, etc.) and satellite (e.g., Terra, A-Train, etc.) sensors will be utilized to acquire aerosol characteristics, sources/sinks, and transport processes during the pre-monsoon (April-May, aerosol forcing) season, and to obtain cloud and precipitation properties during the monsoon (May-June, water cycle response) season. Close collaboration with other international programs, such as ABC, CLIVAR, GEWEX, and CEOP in the region is anticipated.

  8. Cloud activation properties of organic aerosols observed at an urban site during CalNex-LA

    NASA Astrophysics Data System (ADS)

    Mei, F.; Hayes, P. L.; Ortega, A. M.; Jimenez, J.; Wang, J.

    2010-12-01

    Atmospheric aerosols strongly influence the global energy budget by scattering and absorbing sunlight (direct effects) and by changing the microphysical structure, lifetime, and coverage of clouds (indirect effects). Currently, the indirect effects of aerosols remain the most uncertain components in forcing of climate change over the industrial period. This large uncertainty is in part due to our incomplete understanding of the ability of aerosol particles to form cloud droplets under climatically relevant supersaturations. During CalNex study, size-resolved cloud condensation nuclei (CCN) spectrum and aerosol chemical composition were measured at an urban supersite in Pasadena, California from May 15 to June 6, 2010. Monodispersed aerosol particles are first classified using a differential mobility analyzer at sizes ranging from 25 to 320 nm. The activation efficiency of the classified aerosol, defined as the ratio of its CCN concentration (characterized by a DMT CCN counter) to total CN concentration (measured by a condensation particle counter, TSI 3771), is derived as a function of both particle size and supersaturation, which ranges from 0.08% to 0.39%. Aerosol chemical composition was characterized using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). In most of days, increases in aerosol mode diameter, organics mass loading, and aerosol organics volume fraction were observed from 10:00 AM to 15:00 PM. These increases are attributed to formation of secondary organic aerosols through photochemical reactions. On average, the aerosol was dominated by organics (~65% by volume), with the contribution from ammonium sulfate (~20%) and ammonium nitrate (~15%), and the balance being made up of elemental carbon. Positive matrix factorization (PMF) analysis shows the oxygenated organic aerosol (OOA) (~75%) was the dominant organics component. Additionally, the organics O:C ratio was within a narrow range of 0.50±0.12. Particle overall

  9. New particle formation events as a source for cloud condensation nuclei in an urban environment

    NASA Astrophysics Data System (ADS)

    Wonaschütz, Anna; Burkart, Julia; Wagner, Robert; Reischl, Georg; Steiner, Gerhard; Hitzenberger, Regina

    2014-05-01

    Nucleation and growth events have been observed in many remote, urban and rural environments. The new particles can contribute significantly to cloud condensation nuclei concentrations, after growing into the appropriate size range (Kerminen et al., 2012). Several studies have attempted to quantify this contribution (e.g. Asmi et al., 2011, Matsui et al., 2013), but only a limited number of them to date have used simultaneous measurements of CCN concentrations and particle size distributions for this purpose (e.g. Levin et al., 2012). In this study, a data set from an urban background station, consisting of 22 months of size distribution and 12 months of CCN concentration measurements (Burkart et al., 2011, Burkart et al., 2012) with 10 months of overlapping measurements is combined to explore the variability of CCN concentrations, their possible causes, and the contribution of nucleation and growth events to CCN concentrations. Consistent with observations in many other locations, nucleation and growth events occur on 30% of all days in spring and summer, on 11% of days in fall and on 4% of days in winter. This suggests a potentially large source of CCN from nucleation and growth events, particularly in the warm season. We acknowledge funding from FWF (Austrian Science Fund) P19515-N20 References: Asmi E., Kivekas, N., Kerminen, V. M., Komppula, M., Hyvarinen, A. P., Hatakka, J., Viisanen, Y., and Lihavainen, H.: Secondary new particle formation in Northern Finland Pallas site between the years 2000 and 2010, Atmos. Chem. Phys., 11, 12959-12972, doi: 10.5194/acp-11-12959-2011, 2011 Burkart J., Steiner, G., Reischl, G., and Hitzenberger, R.: Long-term study of cloud condensation nuclei (CCN) acticvation of the atmospheric aerosol in Vienna, Atmos. Environ., 45, 5751-5759, doi: 10.1016/j.atmosenv.2011.07.022, 2011. Burkart J., Hitzenberger, R., Reischl, G., Bauer, H., Leder, K., and Puxbaum, H.: Activation of "synthetic ambient" aerosols - relation to chemical

  10. Nitric acid in polar stratospheric clouds - Similar temperature of nitric acid condensation and cloud formation

    NASA Technical Reports Server (NTRS)

    Pueschel, Rudolf F.; Snetsinger, Kenneth G.; Hamill, Patrick; Goodman, Jindra K.; Mccormick, M. Patrick

    1990-01-01

    As shown independently by two different techniques, nitric acid aerosols and polar stratospheric clouds (PSCs) both form below similar threshold temperatures. This supports the idea that the PSC particles involved in chlorine activation and ozone depletion in the winter polar stratosphere are composed of nitric acid. One technique used to show this is the inertial impaction of nitric acid aerosols using an Er-2 aircraft; the other method is remote sensing of PSCs by the Stratospheric Aerosol Measurement (SAM II) satellite borne optical sensor. Both procedures were in operation during the Arctic Airborne Stratospheric Expedition in 1989, and the Airborne Antarctic Ozone Experiment in 1987. Analysis of Arctic particles gathered in situ indicates the presence of nitric acid below a 'first appearance' temperature Tfa = 202 K. This is the same highest temperature at which PSCs are seen by the SAM II satellite. In comparison, a 'first appearance' temperature Tfa = 198 K as found for the Antarctic samples.

  11. Cloud-Aerosol Interactions: Retrieving Aerosol Ångström Exponents from Calipso Measurements of Opaque Water Clouds

    NASA Astrophysics Data System (ADS)

    Vaughan, Mark; Liu, Zhaoyan; Hu, Yong-Xiang; Powell, Kathleen; Omar, Ali; Rodier, Sharon; Hunt, William; Kar, Jayanta; Tackett, Jason; Getzewich, Brian; Lee, Kam-Pui

    2016-06-01

    Backscatter and extinction from water clouds are well-understood, both theoretically and experimentally, and thus changes to the expected measurement of layer-integrated attenuated backscatter can be used to infer the optical properties of overlying layers. In this paper we offer a first look at a new retrieval technique that uses CALIPSO measurements of opaque water clouds to derive optical depths and Ångström exponents for overlying aerosol layers.

  12. The influence of marine monoterpene emissions on cloud condensation nuclei concentrations over the Southern Hemisphere oceans

    NASA Astrophysics Data System (ADS)

    Walker, Hannah; Arnold, Steve; Spracklen, Dominick; Rap, Alexandru; Scott, Catherine; Hackenberg, Sina; Carpenter, Lucy

    2016-04-01

    Changes in the concentration of cloud condensation nuclei (CCN) can affect Earth's climate by altering cloud properties such as lifetime, spatial extent, and brightness. Cloud properties are most sensitive to changes in CCN at the low concentrations typical of the remote marine environment. Underestimation of remote marine water-soluble organic carbon aerosol suggests that a source of secondary organic aerosol is missing from current model mechanisms. Oxidation products of oceanic reactive carbon are a candidate for this missing source, and have the potential to contribute to new particle formation and particle growth. Marine phytoplankton are known to produce monoterpenes (C10H16) and elevated monoterpene concentrations have been observed in regions of enhanced biological activity. A top-down estimate places the global oceanic monoterpene source in the region of 30 TgC a-1 but it remains very uncertain. In this study we use a global model of aerosol processes (GLOMAP) to investigate the potential impacts of oceanic monoterpenes on CCN concentrations over remote ocean regions. Satellite observations of chlorophyll-a inform the spatial distribution of oceanic monoterpene emission in the model. Using comparisons with new observations of atmospheric monoterpene concentrations from cruises in the North and South Atlantic oceans, we determine the optimum emission for marine monoterpenes. GLOMAP is implemented within the global chemistry-transport model TOMCAT and includes a detailed aerosol microphysics scheme, simulating size- and composition-resolved aerosol. Oxidation products of monoterpenes contribute to new particle formation. Oxidation products of both monoterpenes and isoprene contribute to particle growth. We find that oceanic monoterpene emission rates of 1-35 Tg a-1 (approximately 0.7-24 % of the estimated terrestrial source) lead to average annual global increases in CCN (particles having a dry diameter greater than 50 nm) of 1.6-31 % at the surface. The

  13. Long-term impacts of aerosols on vertical development of cloud and precipitation

    SciTech Connect

    Li Z.; Liu Y.; Niu, F.; Fan, J.; Rosenfeld, D.; Ding, Y.

    2011-11-13

    Aerosols alter cloud density and the radiative balance of the atmosphere. This leads to changes in cloud microphysics and atmospheric stability, which can either suppress or foster the development of clouds and precipitation. The net effect is largely unknown, but depends on meteorological conditions and aerosol properties. Here, we examine the long-term impact of aerosols on the vertical development of clouds and rainfall frequencies, using a 10-year dataset of aerosol, cloud and meteorological variables collected in the Southern Great Plains in the United States. We show that cloud-top height and thickness increase with aerosol concentration measured near the ground in mixed-phase clouds-which contain both liquid water and ice-that have a warm, low base. We attribute the effect, which is most significant in summer, to an aerosol-induced invigoration of upward winds. In contrast, we find no change in cloud-top height and precipitation with aerosol concentration in clouds with no ice or cool bases. We further show that precipitation frequency and rain rate are altered by aerosols. Rain increases with aerosol concentration in deep clouds that have a high liquid-water content, but declines in clouds that have a low liquid-water content. Simulations using a cloud-resolving model confirm these observations. Our findings provide unprecedented insights of the long-term net impacts of aerosols on clouds and precipitation.

  14. Modeling Electrical Structure of the Artificial Charged Aerosol Cloud

    NASA Astrophysics Data System (ADS)

    Davydenko, S.; Iudin, D.; Klimashov, V.; Kostinskiy, A. J.; Syssoev, V.

    2014-12-01

    The electric structure of the unipolar charged aerosol cloud is considered. The cloud of the volume about 30 cubic meters is generated in the open atmosphere by the original aeroelectrical facility consisting of the source of the aquated ions and the high-voltage discharger. Representing the charge density distribution as a superposition of regular and irregular parts, a model of the electrical structure of the cloud is developed. The regular part is calculated under the stationary current approximation taking into account the source current structure, the shape of the cloud, and results of the multi-point measurements of the electric field and conductivity in the vicinity of the cloud. The irregular part describes random spatiotemporal fluctuations of the charge density which are assumed to be proportional to the aerosol number density. It is shown that a quasi-electrostatic field of the charged aerosol is characterized by significant spatial fluctuations showing the scale invariance. The mean-square fluctuations of the voltage between different parts of the cloud are proportional to the square root of its linear dimensions and may reach significant values even in the absence of the regular field. The basic parameters of the fluctuating spatial structure of the electric field inside the charged aerosol cloud are estimated. It is shown that the charge density fluctuations could lead to a significant (up to 2,5 times) local enhancement of the electric field as compared to the field of the regular part of the charge density. The above effect could serve as one of the important mechanisms of the spark initiation.

  15. ARM Cloud-Aerosol-Precipitation Experiment (ACAPEX) Field Campaign Report

    SciTech Connect

    Leung, L Ruby

    2016-03-01

    The U.S. Department of Energy (DOE)’s Atmospheric Radiation Measurement (ARM) Climate Research Facility’s ARM Cloud-Aerosol-Precipitation Experiment (ACAPEX) field campaign contributes to CalWater 2015, a multi-agency field campaign that aims to improve understanding of atmospheric rivers and aerosol sources and transport that influence cloud and precipitation processes. The ultimate goal is to reduce uncertainties in weather predictions and climate projections of droughts and floods in California. With the DOE G-1 aircraft and ARM Mobile Facility 2 (AMF2) well equipped for making aerosol and cloud measurements, ACAPEX focuses specifically on understanding how aerosols from local pollution and long-range transport affect the amount and phase of precipitation associated with atmospheric rivers. ACAPEX took place between January 12, 2015 and March 8, 2015 as part of CalWater 2015, which included four aircraft (DOE G-1, National Oceanic and Atmospheric Administration [NOAA] G-IV and P-3, and National Aeronautics and Space Administration [NASA] ER-2), the NOAA research ship Ron Brown, carrying onboard the AMF2, National Science Foundation (NSF)-sponsored aerosol and precipitation measurements at Bodega Bay, and the California Department of Water Resources extreme precipitation network.

  16. Pathfinder Instruments for Cloud and Aerosol Spaceborne Observations (PICASSO)

    NASA Technical Reports Server (NTRS)

    McCormick, M. Patrick; Winker, David M.

    1998-01-01

    This paper will describe the planned 3-year Pathfinder Instruments for Cloud and Aerosol Spaceborne Observations (PICASSO) mission, its instrumentation and implementation. It will use LITE and other data, plus analyses, to show the feasibility of such a mission. PICASSO is being proposed for NASA's Earth System Science Pathfinder (ESSP) program with launch predicted in 2003.

  17. Biological aerosol effects on clouds and precipitation

    NASA Astrophysics Data System (ADS)

    Hallar, A. Gannet; Huffman, J. Alex; Fridlind, Ann

    2012-12-01

    Bioaerosol Effects on Clouds Workshop;Steamboat Springs, Colorado, 5-6August 2012 Bioaerosols such as bacteria have been proposed as significant contributors to cloud ice nucleation, but too little is known about the properties and impacts of bioaerosol and other ice nuclei to make reliable conclusions about their wide-scale impact on clouds and precipitation. During late summer an international group of 40 participants met at a Steamboat Springs ski resort to share perspectives on bioaerosol sources, activity, and influence on clouds. Participants who were invited collectively spanned a broad range of expertise, including atmospheric chemistry, microbiology, micrometeorology, and cloud physics, as well as a broad range of research approaches, including laboratory measurement, field measurement, and modeling. Tours of Storm Peak Laboratory (http://www.stormpeak.dri.edu) were offered before and after the workshop.

  18. How much does sea spray aerosol organic matter impact clouds and radiation? Sensitivity studies in the Community Atmosphere Model

    NASA Astrophysics Data System (ADS)

    Burrows, S. M.; Liu, X.; Elliott, S.; Easter, R. C.; Singh, B.; Rasch, P. J.

    2015-12-01

    Submicron marine aerosol particles are frequently observed to contain substantial fractions of organic material, hypothesized to enter the atmosphere as part of the primary sea spray aerosol formed through bubble bursting. This organic matter in sea spray aerosol may affect cloud condensation nuclei and ice nuclei concentrations in the atmosphere, particularly in remote marine regions. Members of our team have developed a new, mechanistic representation of the enrichment of sea spray aerosol with organic matter, the OCEANFILMS parameterization (Burrows et al., 2014). This new representation uses fields from an ocean biogeochemistry model to predict properties of the emitted aerosol. We have recently implemented the OCEANFILMS representation of sea spray aerosol composition into the Community Atmosphere Model (CAM), and performed sensitivity experiments and comparisons with alternate formulations. Early results from these sensitivity simulations will be shown, including impacts on aerosols, clouds, and radiation. References: Burrows, S. M., Ogunro, O., Frossard, A. A., Russell, L. M., Rasch, P. J., and Elliott, S. M.: A physically based framework for modeling the organic fractionation of sea spray aerosol from bubble film Langmuir equilibria, Atmos. Chem. Phys., 14, 13601-13629, doi:10.5194/acp-14-13601-2014, 2014.

  19. Insights into aerosols, chemistry, and clouds from NETCARE: Observations from the Canadian Arctic in summer 2014

    NASA Astrophysics Data System (ADS)

    Abbatt, J.

    2015-12-01

    The Canadian Network on Aerosols and Climate: Addressing Key Uncertainties in Remote Canadian Regions (or NETCARE) was established in 2013 to study the interactions between aerosols, chemistry, clouds and climate. The network brings together Canadian academic and government researchers, along with key international collaborators. Attention is being given to observations and modeling of Arctic aerosol, with the goal to understand underlying processes and so improve predictions of aerosol climate forcing. Motivation to understand the summer Arctic atmosphere comes from the retreat of summer sea ice and associated increase in marine influence. To address these goals, a suite of measurements was conducted from two platforms in summer 2014 in the Canadian Arctic, i.e. an aircraft-based campaign on the Alfred Wegener Institute POLAR 6 and an ocean-based campaign from the CGCS Amundsen icebreaker. NETCARE-POLAR was based out of Resolute Bay, Nunavut during an initial period of little transport and cloud-free conditions and a later period characterized by more transport with potentially biomass burning influence. Measurements included particle and cloud droplet numbers and size distributions, aerosol composition, cloud nuclei, and levels of gaseous tracers. Ultrafine particle events were more frequently observed in the marine boundary layer than above, with particle growth observed in some cases to cloud condensation nucleus sizes. The influence of biological processes on atmospheric constituents was also assessed from the ship during NETCARE-AMUNDSEN, as indicated by high measured levels of gaseous ammonia, DMS and oxygenated VOCs, as well as isolated particle formation and growth episodes. The cruise took place in Baffin Bay and through the Canadian archipelago. Interpretation of the observations from both campaigns is enhanced through the use of chemical transport and particle dispersion models. This talk will provide an overview of NETCARE Arctic observational and

  20. Global aerosol formation and revised radiative forcing based on CERN CLOUD data

    NASA Astrophysics Data System (ADS)

    Gordon, H.; Carslaw, K. S.; Sengupta, K.; Dunne, E. M.; Kirkby, J.

    2015-12-01

    New particle formation in the atmosphere accounts for 40-70% of global cloud condensation nuclei (CCN). It is a complex process involving many precursors: sulphuric acid, ions, ammonia, and a wide range of natural and anthropogenic organic molecules. The CLOUD laboratory chamber experiment at CERN allows the contributions of different compounds to be disentangled in a uniquely well-controlled environment. To date, CLOUD has measured over 500 formation rates (Riccobono 2014, Kirkby 2015, Dunne 2015), under conditions representative of the planetary boundary layer and free troposphere. To understand the sensitivity of the climate to anthropogenic atmospheric aerosols, we must quantify historical aerosol radiative forcing. This requires an understanding of pre-industrial aerosol sources. Here we show pre-industrial nucleation over land usually involves organic molecules in the very first steps of cluster formation. The complexity of the organic vapors is a major challenge for theoretical approaches. Furthermore, with fewer sulphuric acid and ammonia molecules available to stabilize nucleating clusters in the pre-industrial atmosphere, ions from radon or galactic cosmic rays were probably more important than they are today. Parameterizations of particle formation rates determined in CLOUD as a function of precursor concentrations, temperature and ions are being used to refine the GLOMAP aerosol model (Spracklen 2005). The model simulates the growth, transport and loss of particles, translating nucleation rates to CCN concentrations. This allows us to better understand the effects of pre-industrial and present-day particle formation. I will present new results on global CCN based on CLOUD data, including estimates of anthropogenic aerosol radiative forcing, currently the most uncertain driver of climate change (IPCC 2013). References: Riccobono, F. et al, Science 344 717 (2014); Kirkby, J. et al, in review; Dunne, E. et al, in preparation; Spracklen, D. et al, Atmos

  1. Impacts of aerosol particles on the microphysical and radiative properties of stratocumulus clouds over the Southeast Pacific ocean

    NASA Astrophysics Data System (ADS)

    Twohy, C. H.; Anderson, J. R.; Toohey, D. W.; Andrejczuk, M.; Adams, A.; Lytle, M.; George, R. C.; Wood, R.; Saide, P.; Spak, S.; Zuidema, P.; Leon, D.

    2012-08-01

    The Southeast Pacific Ocean is covered by the world's largest stratocumulus cloud layer, which has a strong impact on ocean temperatures and climate in the region. The effect of anthropogenic sources of aerosol particles such as power plants, urban pollution and smelters on the stratocumulus deck was investigated during the VOCALS field experiment. Aerosol measurements below and above cloud were made with a ultra-high sensitivity aerosol spectrometer and analytical electron microscopy. In addition to more standard in-cloud measurements, droplets were collected and evaporated using a counterflow virtual impactor (CVI), and the non-volatile residual particles were analyzed. Many flights focused on the gradient in cloud properties on an E-W track along 20° S from near the Chilean coast to remote areas offshore. Mean statistics from seven flights and many individual legs were compiled. Consistent with a continental source of cloud condensation nuclei, below-cloud accumulation-mode aerosol and droplet number concentration generally decreased from near shore to offshore. Single particle analysis was used to reveal types and sources of the enhanced particle number. While a variety of particle types were found throughout the region, the dominant particles near shore were partially neutralized sulfates. Modeling and chemical analysis indicated that the predominant source of these particles in the marine boundary layer along 20° S was anthropogenic pollution from central Chilean sources, with copper smelters a relatively small contribution. Cloud droplets were more numerous and smaller near shore, and there was less drizzle. Higher droplet number concentration and physically thinner clouds both contributed to the smaller droplets near shore. Satellite measurements were used to show that cloud albedo was highest 500-1000 km offshore, and actually lower closer to shore due to the generally thinner clouds and lower liquid water paths there. Differences in the size

  2. Detrainment and aerosol redistribution in shallow convective clouds (Invited)

    NASA Astrophysics Data System (ADS)

    Chuang, P. Y.; Norgren, M.; Wonaschuetz, A.; Small, J. D.; Sorooshian, A.; Jonsson, H. H.; Feingold, G.; Ervens, B.; Murphy, S. M.

    2013-12-01

    Vertical transport associated with cumulus clouds is important to the redistribution of aerosol particles, gases and energy, with subsequent consequences for many aspects of the climate system. Previous studies have suggested that detrainment from clouds can be comparable to the updraft mass flux, and thus contribute to vertical transport. In this study, we describe a new method to deduce the amounts of gross detrainment and entrainment experienced by non-precipitating cumulus clouds using aircraft observations. The method is applied to aircraft observations from the Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS) which took place in the Houston, Texas region during which 176 small, non-precipitating cumulus were sampled. Our analysis suggests that, on average, these clouds were comprised of 30 to 70% mixed-layer air, with entrained air comprising most of the remainder. The mass fraction of detrained air was less than 2% for a majority of the clouds, although 15% of them did exhibit detrained air fractions larger than 10%. Entrained and detrained air mass fractions both increased with altitude, and the largest detrainment events were almost all associated with air that was at their level of neutral buoyancy, findings that are all consistent with previous studies. To address aerosol redistribution more specifically, aerosol size distributions on clear and cloudy days are compared, with substantial enhancements at higher altitudes found for cloudy days due to a combination of vertical transport and in situ sulfate and organic chemistry.

  3. Global and regional modeling of clouds and aerosols in the marine boundary layer during VOCALS: the VOCA intercomparison

    SciTech Connect

    Wyant, M. C.; Bretherton, Christopher S.; Wood, Robert; Carmichael, Gregory; Clarke, A. D.; Fast, Jerome D.; George, R.; Gustafson, William I.; Hannay, Cecile; Lauer, Axel; Lin, Yanluan; Morcrette, J. -J.; Mulcahay, Jane; Saide, Pablo; Spak, S. N.; Yang, Qing

    2015-01-09

    A diverse collection of models are used to simulate the marine boundary layer in the southeast Pacific region during the period of the October–November 2008 VOCALS REx (VAMOS Ocean Cloud Atmosphere Land Study Regional Experiment) field campaign. Regional models simulate the period continuously in boundary-forced free-running mode, while global forecast models and GCMs (general circulation models) are run in forecast mode. The models are compared to extensive observations along a line at 20° S extending westward from the South American coast. Most of the models simulate cloud and aerosol characteristics and gradients across the region that are recognizably similar to observations, despite the complex interaction of processes involved in the problem, many of which are parameterized or poorly resolved. Some models simulate the regional low cloud cover well, though many models underestimate MBL (marine boundary layer) depth near the coast. Most models qualitatively simulate the observed offshore gradients of SO2, sulfate aerosol, CCN (cloud condensation nuclei) concentration in the MBL as well as differences in concentration between the MBL and the free troposphere. Most models also qualitatively capture the decrease in cloud droplet number away from the coast. However, there are large quantitative intermodel differences in both means and gradients of these quantities. Many models are able to represent episodic offshore increases in cloud droplet number and aerosol concentrations associated with periods of offshore flow. Most models underestimate CCN (at 0.1% supersaturation) in the MBL and free troposphere. The GCMs also have difficulty simulating coastal gradients in CCN and cloud droplet number concentration near the coast. The overall performance of the models demonstrates their potential utility in simulating aerosol–cloud interactions in the MBL, though quantitative estimation of aerosol–cloud interactions and aerosol indirect effects of MBL

  4. Global and regional modeling of clouds and aerosols in the marine boundary layer during VOCALS: the VOCA intercomparison

    DOE PAGES

    Wyant, M. C.; Bretherton, Christopher S.; Wood, Robert; ...

    2015-01-09

    A diverse collection of models are used to simulate the marine boundary layer in the southeast Pacific region during the period of the October–November 2008 VOCALS REx (VAMOS Ocean Cloud Atmosphere Land Study Regional Experiment) field campaign. Regional models simulate the period continuously in boundary-forced free-running mode, while global forecast models and GCMs (general circulation models) are run in forecast mode. The models are compared to extensive observations along a line at 20° S extending westward from the South American coast. Most of the models simulate cloud and aerosol characteristics and gradients across the region that are recognizably similar tomore » observations, despite the complex interaction of processes involved in the problem, many of which are parameterized or poorly resolved. Some models simulate the regional low cloud cover well, though many models underestimate MBL (marine boundary layer) depth near the coast. Most models qualitatively simulate the observed offshore gradients of SO2, sulfate aerosol, CCN (cloud condensation nuclei) concentration in the MBL as well as differences in concentration between the MBL and the free troposphere. Most models also qualitatively capture the decrease in cloud droplet number away from the coast. However, there are large quantitative intermodel differences in both means and gradients of these quantities. Many models are able to represent episodic offshore increases in cloud droplet number and aerosol concentrations associated with periods of offshore flow. Most models underestimate CCN (at 0.1% supersaturation) in the MBL and free troposphere. The GCMs also have difficulty simulating coastal gradients in CCN and cloud droplet number concentration near the coast. The overall performance of the models demonstrates their potential utility in simulating aerosol–cloud interactions in the MBL, though quantitative estimation of aerosol–cloud interactions and aerosol indirect effects of MBL clouds

  5. Multistatic aerosol-cloud lidar in space: A theoretical perspective

    NASA Astrophysics Data System (ADS)

    Mishchenko, Michael I.; Alexandrov, Mikhail D.; Cairns, Brian; Travis, Larry D.

    2016-11-01

    Accurate aerosol and cloud retrievals from space remain quite challenging and typically involve solving a severely ill-posed inverse scattering problem. In this Perspective, we formulate in general terms an aerosol and aerosol-cloud interaction space mission concept intended to provide detailed horizontal and vertical profiles of aerosol physical characteristics as well as identify mutually induced changes in the properties of aerosols and clouds. We argue that a natural and feasible way of addressing the ill-posedness of the inverse scattering problem while having an exquisite vertical-profiling capability is to fly a multistatic (including bistatic) lidar system. We analyze theoretically the capabilities of a formation-flying constellation of a primary satellite equipped with a conventional monostatic (backscattering) lidar and one or more additional platforms each hosting a receiver of the scattered laser light. If successfully implemented, this concept would combine the measurement capabilities of a passive multi-angle multi-spectral polarimeter with the vertical profiling capability of a lidar; address the ill-posedness of the inverse problem caused by the highly limited information content of monostatic lidar measurements; address the ill-posedness of the inverse problem caused by vertical integration and surface reflection in passive photopolarimetric measurements; help relax polarization accuracy requirements; eliminate the need for exquisite radiative-transfer modeling of the atmosphere-surface system in data analyses; yield the day-and-night observation capability; provide direct characterization of ground-level aerosols as atmospheric pollutants; and yield direct measurements of polarized bidirectional surface reflectance. We demonstrate, in particular, that supplementing the conventional backscattering lidar with just one additional receiver flown in formation at a scattering angle close to 170° can dramatically increase the information content of the

  6. A Process-Modeling Study of Aerosol-Cloud-Precipitation Interactions in Response to Controlled Seawater Spray in Marine Boundary Layer (Invited)

    NASA Astrophysics Data System (ADS)

    Wang, H.; Rasch, P. J.; Feingold, G.

    2010-12-01

    Vast areas of the oceanic surface are covered by stratocumulus (Sc) clouds. They significantly enhance the reflection of incoming solar radiation back to space, leading to a considerable cooling of the Earth-atmosphere system. It has been argued that a 4% increase in the areal coverage or a 0.06 increase in cloud albedo of Sc clouds can offset the warming by atmospheric CO2 doubling (Randall et al. 1984; Latham et al. 2008). Acting as cloud condensation nuclei (CCN), aerosol particles can modify cloud albedo, cloud longevity and precipitation efficiency. Recent observational and modeling studies have suggested that aerosol, through its effect on precipitation, can alter cloud cellular structures in marine Sc region, representing a powerful modification of clouds by aerosol. The possibility of mitigating global warming by spraying sea-salt particles into marine boundary layer to brighten Sc clouds was raised by Latham (1990). The idea has been evaluated by several global climate model studies but their inability to represent cloud-scale dynamics and microphysics raises ques