Science.gov

Sample records for aerosol condensation nuclei

  1. 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.

  2. 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.

  3. 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.

  4. 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.

  5. 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

  6. 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.

  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. 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 ...

  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. 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.

  11. 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.

  12. 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.

  13. 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.

  14. 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

  15. 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.

  16. 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.

  17. 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.

  18. 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...

  19. 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

  20. 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

  1. 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.

  2. 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%.

  3. 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

  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. 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.

  6. 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

  7. 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.

  8. 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.

  9. 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.

  10. 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.

  11. 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

  12. 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.

  13. 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.

  14. 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.

  15. 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.

  16. 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

  17. 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

  18. 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.

  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. Condensation nuclei and aerosol-scattering extinction measurements at Mauna Loa Observatory: 1974-1985. Data report

    SciTech Connect

    Massey, D.M.; Quakenbush, T.K.; Bodhaine, B.A.

    1987-07-01

    The observatory at Mauna Loa, Hawaii measures the characteristics of surface aerosols under background conditions. The instruments provide data that are representative of the background-aerosol climatology at Mauna Loa. These data can also be used to identify potential local contamination periods. The nephelometer's light-scattering measurements show an annual cycle: a maximum in April and a minimum in November, with a variation of a factor of 5.5. The Condensation Nucleus (CN) counter shows a much smaller annual cycle: a maximum in September and a minimum in March, with a variation of a factor of 1.5. A local decrease in CN concentration occurs in August. The Angstrom exponent minimum occurs in May. This indicates larger aerosol particles within the month as compared with the remainder of the year.

  1. 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 %.

  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. 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%.

  4. 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

  5. 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.

  6. 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.

  7. 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

  8. 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.

  9. 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.

  10. 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.

  11. 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.

  12. 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.

  13. 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.

  14. 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

  15. Origin of Condensation Nuclei in the Springtime Polar Stratosphere

    NASA Technical Reports Server (NTRS)

    Zhao, Jingxia; Toon, Owen B.; Turco, Richard P.

    1995-01-01

    An enhanced sulfate aerosol layer has been observed near 25 km accompanying springtime ozone depletion in the Antarctic stratosphere. We use a one-dimensional aerosol model that includes photochemistry, particle nucleation, condensational growth, coagulation, and sedimentation to study the origin of the layer. Annual cycles of sunlight, temperature, and ozone are incorporated into the model. Our results indicate that binary homogeneous nucleation leads to the formation of very small droplets of sulfuric acid and water under conditions of low temperature and production of H2SO4 following polar sunrise. Photodissociation of carbonyl sulfide (OCS) alone, however, cannot provide sufficient SO2 to create the observed condensation nuclei (CN) layer. When subsidence of SO2 from very high altitudes in the polar night vortex is incorporated into the model, the CN layer is reasonably reproduced. The model predictions, based on the subsidence in polar vortex, agree with in situ measurements of particle concentration, vertical distribution, and persistence during polar spring.

  16. Origin of condensation nuclei in the springtime polar stratosphere

    NASA Technical Reports Server (NTRS)

    Zhao, Jingxia; Toon, Owen B.; Turco, Richard P.

    1995-01-01

    An enhanced sulfate aerosol layer has been observed near 25 km accompanying springtime ozone depletion in the Antarctic stratosphere. We use a one-dimensional aerosol model that includes photochemistry, particle nucleation, condensational growth, coagulation, and sedimentation to study the origin of the layer. Annual cycles of sunlight, temperature, and ozone are incorporated into the model. Our results indicate that binary homogeneous nucleation leads to the formation of very small droplets of sulfuric acid and water under conditions of low temperature and production of H2SO4 following polar sunrise. Photodissociation of carbonyl sulfide (OCS) alone, however, cannot provide sufficient SO2 to create the observed condensation nuclei (CN) layer. When subsidence of SO2 from very high altitudes in the polar night vortex is incorporated into the model, the CN layer is reasonably reproduced. The model predictions, based on the subsidence in polar vortex, agree with in situ measurements of particle concentration, vertical distribution, and persistence during polar spring.

  17. 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.

  18. African Dust Aerosols as Atmospheric Ice Nuclei

    NASA Technical Reports Server (NTRS)

    DeMott, Paul J.; Brooks, Sarah D.; Prenni, Anthony J.; Kreidenweis, Sonia M.; Sassen, Kenneth; Poellot, Michael; Rogers, David C.; Baumgardner, Darrel

    2003-01-01

    Measurements of the ice nucleating ability of aerosol particles in air masses over Florida having sources from North Africa support the potential importance of dust aerosols for indirectly affecting cloud properties and climate. The concentrations of ice nuclei within dust layers at particle sizes below 1 pn exceeded 1/cu cm; the highest ever reported with our device at temperatures warmer than homogeneous freezing conditions. These measurements add to previous direct and indirect evidence of the ice nucleation efficiency of desert dust aerosols, but also confirm their contribution to ice nuclei populations at great distances from source regions.

  19. Optical sensors based on the molecular condensation nuclei detector

    NASA Astrophysics Data System (ADS)

    Kuptsov, Vladimir D.; Katelevsky, Vadim Y.; Valyukhov, Vladimir P.

    2015-05-01

    Molecular condensation nuclei (MCN) detector is a specialized optical sensor which provides for monitoring of various chemicals impurity in the environment and diagnosis of diseases in human exhaled air ("electronic nose" biosensor). Structurally MCN detector is included in the highly sensitive gas analyzers based on MCN method. The article describes the fundamental principles, specific features and application fields of the advanced highly sensitive MCN method. The MCN method is based on the application of various physico-chemical processes to the flow of a gas containing impurities. As a result of these processes aerosol particle that are about 106 times larger than the original molecule of the impurity are produced. The ability of the aerosol particle to scatter incident light also increases ~1014÷1016 times compared with the original molecule and the aerosol particle with the molecule of the impurity in the center is easily detected by light scattering inside a photometer. By measuring of the light scattering intensity is determined concentration of chemical impurities in the air. Aerosol particles in the MCN detector are formed in the condensing devices through overgrowth of the molecule detectable impurity by molecules so-called «developer» substance. At the final stage of the analysis in the MCN detector is measured light scattering by aerosol particles which is proportional to the concentration of determined impurities in the environment. For calculations of the scattered radiation is applicable Mie's theory considering the scattering of light by spherical particles whose size is comparable to the wavelength of light. We have determined that the light scattering by aerosol particles is interferometric and is comparable within an order of magnitude with light scattering by the air inside a photometer. The detection threshold for the target component of the gas analyzer is attained at the spontaneous ionization background level and not at the limiting

  20. 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).

  1. 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.

  2. 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.

  3. Multi-K¯ nuclei and kaon condensation

    NASA Astrophysics Data System (ADS)

    Gazda, D.; Friedman, E.; Gal, A.; Mareš, J.

    2008-04-01

    We extend previous relativistic mean-field (RMF) calculations of multi-K¯ nuclei, using vector boson fields with SU(3) PPV coupling constants and scalar boson fields constrained phenomenologically. For a given core nucleus, the resulting K¯ separation energy BK¯, as well as the associated nuclear and K¯-meson densities, saturate with the number κ of K¯ mesons for κ>κsat~10. Saturation appears robust against a wide range of variations, including the RMF nuclear model used and the type of boson fields mediating the strong interactions. Because BK¯ generally does not exceed 200 MeV, it is argued that multi-K¯ nuclei do not compete with multihyperonic nuclei in providing the ground state of strange hadronic configurations and that kaon condensation is unlikely to occur in strong-interaction self-bound strange hadronic matter. Last, we explore possibly self-bound strange systems made of neutrons and K¯0 mesons, or protons and K- mesons, and study their properties.

  4. The south pole automatic condensation nuclei counter: instrument details and five years of observations

    SciTech Connect

    Murphy, M.E.; Bodhaine, B.A.

    1980-02-01

    An automatic General Electric (G.E.) condensation nuclei counter has been operating continuously at the Amundson-Scott South Pole station since 1974 as part of the Geophysical Monitoring for Climatic Change (GMCC) program. This instrument (calibrated by a Pollak nuclei counter standard), with its high sensitivity and fast response, can provide continuous aerosol climatology and identify periods of contamination from local sources. The annual variation of nuclei concentration is apparent and is repeatably consistent over the five year period. Nuclei concentrations occasionally reach values as low as 7/cu cm during the austral winter (April through September), begin to increase near the time of astronomical sunrise, and reach values as high as about 240/cu cm during summer months. The continuously operating G.E. condensation nuclei counter in conjunction with the Pollak nuclei counter, have produced an excellent data set over the five year period, 1974-1978.

  5. 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.

  6. 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.

  7. 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.

  8. 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.

  9. Stratospheric condensation nuclei variations may relate to solar activity

    NASA Technical Reports Server (NTRS)

    Hofmann, D. J.; Rosen, J. M.

    1982-01-01

    Observations of increases of stratospheric condensation nuclei suggest a photo-initiated sulphuric acid vapour formation process in spring in polar regions. It is proposed that the sulphuric acid rapidly forms condensation nuclei through attachment to negatively charged multi-ion complexes and that the process may be modulated through variations in solar activity.

  10. The threshold sensitivity of the molecular condensation nuclei detector

    NASA Astrophysics Data System (ADS)

    Kuptsov, Vladimir D.; Katelevsky, Vadim Y.; Valyukhov, Vladimir P.

    2015-05-01

    Molecular condensation nuclei (MCN) method is used in production engineering and process monitoring and relates to optical metrology methods of measuring the concentrations of various contaminants in the environment. Ultra high sensitivity of MCN method to a class of substances is determined by measuring the optical scattering aerosol particles, at the centers of which are located the detectable impurities molecules. This article investigates the influence of MCN manifestations coefficient (ratio of the concentration of aerosol particles to the concentration of molecules detectable impurities) on the sensitivity of the MCN detector. The MCN method is based on the application of various physicochemical processes to the flow of a gas containing impurities. As a result of these processes aerosol particle that are about 106 times larger than the original molecule of the impurity are produced. The ability of the aerosol particle to scatter incident light also increases ~1014 ÷1016 times compared with the original molecule and the aerosol particle with the molecule of the impurity in the center is easily detected by light scattering inside a photometer. By measuring of the light scattering intensity is determined concentration of chemical impurities in the air. An application nephelometric optical metrology scheme of light scattering by aerosol particles ensures stable operation of reliable and flexible measuring systems. Light scattering by aerosol particles is calculated on the basis of the Mie's theory as aerosol particle sizes comparable to the wavelength of the optical radiation. The experimental results are shown for detectable impurities of metal carbonyls. Gas analyzers based on the MCN method find application in industries with the possibility of highly toxic emissions into the atmosphere (carbonyl technology of metal coatings and products, destruction of chemical weapons, etc.), during storage and transportation of toxic substances, as well as in the

  11. 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.

  12. 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

  13. 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.

  14. 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

  15. 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

  16. 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

  17. 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.

  18. 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.

  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. Bose condensation of nuclei in heavy ion collisions

    NASA Technical Reports Server (NTRS)

    Tripathi, Ram K.; Townsend, Lawrence W.

    1994-01-01

    Using a fully self-consistent quantum statistical model, we demonstrate the possibility of Bose condensation of nuclei in heavy ion collisions. The most favorable conditions of high densities and low temperatures are usually associated with astrophysical processes and may be difficult to achieve in heavy ion collisions. Nonetheless, some suggestions for the possible experimental verification of the existence of this phenomenon are made.

  1. 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.

  2. 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

  3. Counting Condensation Nuclei in the Antarctic Ozone Mission

    NASA Technical Reports Server (NTRS)

    Wilson, James Charles

    1994-01-01

    The work done on this grant primarily concerns the measurement of aerosol in the stratosphere from NASA ER-2 aircraft in studies of stratospheric ozone depletion in the northern and southern hemispheres. The ER-2 Condensation Nucleus Counter (CNC) measures the number concentration of particles in the diameter range of approximately 0.01 to 1 micron. The Passive Cavity Aerosol Spectrometer measures size distributions in the 0.17 to 3 micron diameter range. This instrument was upgraded during this grant period to a Focused Cavity Aerosol Spectrometer (FCAS). This upgrade permitted the instrument to measure particles as small as 0.05 micron in diameter. The inlet for the PCAS and FCAS was modified and characterized under this grant so that the modifications to the aerosol due to anisokinetic sampling and heating upon sampling and in transport to the measurement location were accounted for in the data analysis. These measurements permitted observations of particle production in the southern hemisphere winter polar vortex and observation of the impact of denitrification on the number concentration of the aerosol in the denitrified air. In the northern polar vortex, the measurements provided a characterization of the sulfate aerosol. Following the eruption of Mount Pinatubo in 1991, the measurements permitted an accurate characterization of the sulfate aerosol enhancements resulting from the eruption. This led to studies of the impact of heterogeneous chemistry on the partitioning of the partitioning of the reactive nitrogen species and the partitioning of the chlorine reservoir.

  4. MULTI-bar K (hyper)nuclei and Kaon Condensation

    NASA Astrophysics Data System (ADS)

    Gazda, D.; Mareš, J.; Friedman, E.; Gal, A.

    We report on recent relativistic mean-field calculations of multi-bar K nuclei1,2 which were performed fully and self-consistently across the periodic table. The bar K separation energy B{bar K} as well as the nuclear and bar K-meson densities were found to saturate with the number of antikaons in the nuclear medium. Saturation appears robust against a wide range of variations, including the nuclear model used and the type of boson fields mediating the strong interactions. In addition, we have explored properties of kaonic hypernuclei — strange systems made of nucleons, hyperons and K- mesons. We observed saturation also in these objects. Since the bar K separation energy B{bar K} does not exceed 200 MeV, multi-bar K nuclei lie energetically well above multi-hyperonic nuclei and it is unlikely that kaon condensation could occur in strong-interaction self-bound hadronic matter.

  5. MULTI-bar K (hyper)nuclei and Kaon Condensation

    NASA Astrophysics Data System (ADS)

    Gazda, D.; Mareš, J.; Friedman, E.; Gal, A.

    2010-10-01

    We report on recent relativistic mean-field calculations of multi-bar K nuclei1,2 which were performed fully and self-consistently across the periodic table. The bar K separation energy B{bar K} as well as the nuclear and bar K-meson densities were found to saturate with the number of antikaons in the nuclear medium. Saturation appears robust against a wide range of variations, including the nuclear model used and the type of boson fields mediating the strong interactions. In addition, we have explored properties of kaonic hypernuclei - strange systems made of nucleons, hyperons and K- mesons. We observed saturation also in these objects. Since the bar K separation energy B{bar K} does not exceed 200 MeV, multi-bar K nuclei lie energetically well above multi-hyperonic nuclei and it is unlikely that kaon condensation could occur in strong-interaction self-bound hadronic matter.

  6. 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.

  7. Modification of laminar flow ultrafine condensation particle counters for the enhanced detection of 1 nm condensation nuclei

    SciTech Connect

    Kuang, C.; Chen, M.; McMurry, P. H.; Wang, J.

    2011-10-01

    This paper describes simple modifications to thermally diffusive laminar flow ultrafine condensation particle counters (UCPCs) that allow detection of {approx}1 nm condensation nuclei with much higher efficiencies than have been previously reported. These nondestructive modifications were applied to a commercial butanol based UCPC (TSI 3025A) and to a diethylene glycol-based UCPC (UMN DEG-UCPC). Size and charge dependent detection efficiencies using the modified UCPCs (BNL 3025A and BNL DEGUCPC) were measured with high resolution mobility classified aerosols composed of NaCl, W, molecular ion standards of tetraalkyl ammonium bromide, and neutralizer-generated ions. With negatively charged NaCl aerosol, the BNL 3025A and BNL DEGUCPC achieved detection efficiencies of 37% (90x increase over TSI 3025A) at 1.68 nm mobility diameter (1.39 nm geometric diameter) and 23% (8x increase over UMN DEG-UCPC) at 1.19 nm mobility diameter (0.89 nm geometric diameter), respectively. Operating conditions for both UCPCs were identified that allowed negatively charged NaCl and W particles, but not negative ions of exactly the same mobility size, to be efficiently detected. This serendipitous material dependence, which is not fundamentally understood, suggests that vapor condensation might sometimes allow for the discrimination between air 'ions' and charged 'particles.' As a detector in a scanning mobility particle spectrometer (SMPS), a UCPC with this strong material dependence would allow for more accurate measurements of sub-2 nm aerosol size distributions due to the reduced interference from neutralizer-generated ions and atmospheric ions, and provide increased sensitivity for the determination of nucleation rates and initial particle growth rates.

  8. 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

  9. 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.

  10. 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

  11. 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.

  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. 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

  15. 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.

  16. Influence of Anthropogenic Sources on the Cloud Condensation Nuclei (CCN) in zones near to Mexico City

    NASA Astrophysics Data System (ADS)

    Frias-Cisneros, M.; Baumgardner, D.; Marin, J.

    2007-05-01

    During March 2006, a field experiment was conducted at the Paso de Cortes site, 60 km SE of Mexico City, at an altitude (4000 m, a.s.l.) where the site is sometimes in the free troposphere and otherwise within the boundary layer. During this experiment, cloud condensation nuclei (CCN) concentrations were measured with a thermal gradient diffusion chamber at applied supersaturations that ranged from 0.2 to 0.7 %. In addition, aerosol size distributions were obtained with a differential mobility analyzer (DMA and concentrations of condensation nuclei (CN) with a TSI Model 3010 CPC. The wind trajectories were computed for the altitude of the observation site from NCEP analysis. In this work the methodological approach was to determine the relationships between CN and CCN concentration and associated size distributions for various air masses arriving at the observation site from different directions according to the potential origin of the anthropogenic particles. Air masses are classified into four principal types: 1) Mexico City (NW), 2) Puebla (SE), 3) Cuernavaca (SW) and 4) local biomass burning. The CCN concentrations clearly depend on the source of the air mass, i.e., the highest concentrations are related to the biomass burning and the lowest from Cuernavaca. Moreover, a typical range can be attributed to each air mass type for the CCN/CN ratio. The objective of this study is to evaluate the evolution of CN and CCN as related to the anthropogenic sources.

  17. 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

  18. Calibration and demonstration of a condensation nuclei counting system for airborne measurements of aircraft exhausted particles

    NASA Astrophysics Data System (ADS)

    Cofer, Wesley R.; Anderson, Bruce E.; Winstead, Edward L.; Bagwell, Donald R.

    A system of multiple continuous-flow condensation nuclei counters (CNC) was assembled, calibrated, and demonstrated on a NASA T-39 Sabreliner jet aircraft. The mission was to penetrate the exhaust plumes and/or contrails of other subsonic jet aircraft and determine the concentrations of submicrometer diameter aerosol particles. Mission criteria required rapid response measurements ( ˜ 1 s) at aircraft cruise altitudes (9-12 km). The CNC sampling system was optimized to operate at 160 Torr. Aerosol samples were acquired through an externally mounted probe. Installed downstream of the probe was a critical flow orifice that provided sample to the CNC system. The orifice not only controlled volumetric flow rate, but also dampened probe pressure/flow oscillations encountered in the turbulent aircraft-wake vortex environment. Laboratory calibrations with NaCl particles under representative conditions are reported that indicate small amounts of particle loss and a maximum measurement efficiency of ˜ 75% for particles with diameters ranging from ⩾ 0.01- ⩽ 0.18 μm Data from exhaust/contrail samplings of a NASA B757 and DC-8 at cruise altitude are discussed. Data include exhaust/contrail measurements made during periods in which the B757 port jet engine burned low-sulfur fuel while the starboard engine simultaneously burned specially prepared high-sulfur fuel. The data discussed highlight the CNC systems performance, and introduce new observations pertinent to the behavior of sulfur in aircraft exhaust aerosol chemistry.

  19. 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.

  20. 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

  1. 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.

  2. 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.

  3. Optical instrumentation systems for environmental and structural health monitoring based on the molecular condensation nuclei (MCN) detector

    NASA Astrophysics Data System (ADS)

    Kuptsov, Vladimir D.; Katelevsky, Vadim Ya.; Valyukhov, Vladimir P.; Aladov, Andrei V.

    2016-04-01

    The foundation of measurement systems for environmental and structural health monitoring based on molecular condensation nuclei (MCN) detector is the measurement of the intensity of light scattered by aerosol particles. Aerosol particles are formed in the condensation chamber around single molecules of detected impurities (harmful and dangerous substances in the case of environmental monitoring and biomarkers in the case of structural health monitoring). The size of an aerosol particle is about 106 times larger than the size of the original impurity molecule. The ability of the aerosol particle to scatter incident light also increases 1014÷1016 times compared with the original molecule. By measuring the light scattering intensity the concentration of chemical impurities in the air is determined. The paper investigates many aspects of the detection process - the optical scattering by aerosol particles inside the photometer of MCN detector; signal conditioning, processing of light scattering measurements results, determination of the criteria for making a decision about the presence of detected impurities in the environment; multi-component sensing of detected impurities and graphical user interface design. Experimental results of the detection of toxic substances in micro-concentrations in the environment are presented.

  4. Airborne cloud condensation nuclei measurements during the 2006 Texas Air Quality Study

    NASA Astrophysics Data System (ADS)

    Asa-Awuku, Akua; Moore, Richard H.; Nenes, Athanasios; Bahreini, Roya; Holloway, John S.; Brock, Charles A.; Middlebrook, Ann M.; Ryerson, Thomas B.; Jimenez, Jose L.; Decarlo, Peter F.; Hecobian, Arsineh; Weber, Rodney J.; Stickel, Robert; Tanner, Dave J.; Huey, Lewis G.

    2011-06-01

    Airborne measurements of aerosol and cloud condensation nuclei (CCN) were conducted aboard the National Oceanic and Atmospheric Administration WP-3D platform during the 2006 Texas Air Quality Study/Gulf of Mexico Atmospheric Composition and Climate Study (TexAQS/GoMACCS). The measurements were conducted in regions influenced by industrial and urban sources. Observations show significant local variability of CCN activity (CCN/CN from 0.1 to 0.5 at s = 0.43%), while variability is less significant across regional scales (˜100 km × 100 km; CCN/CN is ˜0.1 at s = 0.43%). CCN activity can increase with increasing plume age and oxygenated organic fraction. CCN measurements are compared to predictions for a number of mixing state and composition assumptions. Mixing state assumptions that assumed internally mixed aerosol predict CCN concentrations well. Assuming organics are as hygroscopic as ammonium sulfate consistently overpredicted CCN concentrations. On average, the water-soluble organic carbon (WSOC) fraction is 60 ± 14% of the organic aerosol. We show that CCN closure can be significantly improved by incorporating knowledge of the WSOC fraction with a prescribed organic hygroscopicity parameter (κ = 0.16 or effective κ ˜ 0.3). This implies that the hygroscopicity of organic mass is primarily a function of the WSOC fraction. The overall aerosol hygroscopicity parameter varies between 0.08 and 0.88. Furthermore, droplet activation kinetics are variable and 60% of particles are smaller than the size characteristic of rapid droplet growth.

  5. 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.

  6. 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.

  7. 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.; Schmitt, J.; White, D.R.; Hopkins, A.R.; Trueblood, M.B. . Cloud and Aerosol Science Lab.)

    1992-12-01

    This third progress report describes the status of our efforts to develop the instrumentation to collect cloud condensation nuclei (CCN) in amounts sufficient for chemical analysis. During the fall of 1992 we started collecting filter samples of CCN with the laboratory version of the apparatus at Rolla -MO. The mobile version of the apparatus is in the latter stages of construction. This report includes a fairly rigorous discussion of the operation of the CCN sampling system. A statistical model of the operation of the system is presented to show the ability of the system to collect CCN in the two different size ranges for which we plan to determine the chemical composition. A question is raised by the model results about the operation of one of the virtual impactors. It appears to pass a small percent of particles larger than its cut-point that has the potential of contaminating the smallest CCN sample with larger CCN material. Further tests are necessary, but it may be necessary to redesign that impactor. The appendices of the report show pictures of both the laboratory version and the mobile version of the CCN sampling system. The major hardware has been completed, and the mobile version will be in operation within a few weeks.

  8. Meteoric Dust as Condensation Nuclei of Small-Mode Particles in the Upper Haze of Venus

    NASA Astrophysics Data System (ADS)

    Gao, P.; Zhang, X.; Crisp, D.; Bardeen, C.; Yung, Y. L.

    2012-12-01

    Observations by the SPICAV/SOIR instruments aboard Venus Express have revealed that the Upper Haze of Venus is populated by two particle modes, as reported by Wilquet et al. (J. Geophys. Res., 114, E00B42, 2009). In this work, we posit that the large mode is made up of cloud particles that have diffused upwards from the cloud deck below, while the smaller mode is generated by the in situ nucleation of meteoric dust. We test this hypothesis by using version 3.0 of the Community Aerosol and Radiation Model for Atmospheres, first developed by Turco et al. (J. Atmos. Sci., 36, 699-717, 1979) and upgraded to version 3.0 by Bardeen et al. (The CARMA 3.0 microphysics package in CESM, Whole Atmosphere Working Group Meeting, 2011). Using the meteoric dust production profile of Kalashnikova et al. (Geophys. Res. Lett., 27, 3293-3296, 2000), the sulfur/sulfate condensation nuclei production profile of Imamura and Hashimoto (J. Atmos. Sci., 58, 3597-3612, 2001), and sulfuric acid vapor production profile of Zhang et al. (Icarus, 217, 714-739, 2012), we numerically simulate a column of the Venus atmosphere from 40 to 100 km above the surface. Our aerosol number density results agree well with Pioneer Venus data from Knollenberg and Hunten (J. Geophys. Res., 85, 8039-8058, 1980), while our gas distribution results match that of Kolodner and Steffes below 55 km (Icarus, 132, 151-169, 1998). The resulting size distribution of cloud particles shows two distinct modes, qualitatively matching the observations of Pioneer Venus. We also observe a third mode in our results with a size of a few microns at 48 km altitude, which appears to support the existence of the controversial third mode in the Pioneer Venus data. This mode disappears if coagulation is not included in the simulation. The Upper Haze size distribution shows two lognormal-like distributions overlapping each other, possibly indicating the presence of the two distinct modes. We test our hypothesis by simulating the

  9. Delayed production of sulfuric acid condensation nuclei in the polar stratosphere from El Chichon volcanic vapors

    NASA Technical Reports Server (NTRS)

    Hofmann, D. J.; Rosen, J. M.; Gringel, W.

    1985-01-01

    It is pointed out that measurements of the vertical profiles of atmospheric condensation nuclei (CN) have been conducted since 1973. Studies with a new instrument revealed that the CN concentration undergoes a remarkable annual variation in the 30-km region characterized by a large increase in the late winter/early spring period with a subsequent decay during the remainder of the year. The event particles are observed to be volatile at 150 C, suggesting a sulfuric acid-water composition similar to that found in the normal 20 km aerosol layer. The development of about 10 to the 7th metric tons of sulfuric acid aerosol following the injection of sulfurous gases by El Chichon in April 1982, prompted Hofmann and Rosen (1983) to predict a very large CN event for 1983. The present investigation is concerned with the actual observation of the predicted event. Attention is given to the observation of a very large increase of what appear to be small sulfuric acid droplets at 30-km altitude in January 1983 over Laramie, WY, in January 1983.

  10. 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.

  11. 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.

  12. Feasibility of using multiwavelength lidar measurements to measure cloud condensation nuclei

    SciTech Connect

    Feingold, G.; Grund, C.J. |

    1994-12-01

    This paper addresses the feasibility of using multiwavelength lidar measurements to differentiate both qualitatively and quantitatively between the relative concentrations of hygroscopic and nonhygroscopic aerosol particles. The proposed technique utilizes the fact that hygroscopic particles undergo a size increase and refractive-index change with increasing relative humidity and that different wavelengths respond to these changes in different ways. The lidar wavelengths considered are 0.289, 0.355, 0.532, 0.694, 1.064, and 2.02 micrometer and the 9-11.5-micrometer range. It is shown that under certain conditions, a judicious choice of lidar wavelengths can provide a differential backscatter, sufficient to provide information on the size and percentage number concentration of the hygroscopic aerosol and, consequently, cloud condensation nuclei concentration. The presence of a mode of coarse particles (median radius greater than 0.3 micrometer) produces ambiguous results and limits application of the technique to regions sufficiently distant from coarse mode sources (e.g., in the free troposphere). The authors have identified a pair of wavelengths in the infrared region that provides a clear indication of the existence of these particles. The potential benefits of distinguishing hygroscopic particle concentration from nonhygroscopic particle concentration are great since remote measurement can provide good temporal and spatial coverage of these properties and valuable information for climate monitoring.

  13. 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.

  14. 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

  15. 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

  16. 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.

  17. 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

  18. 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.

  19. Cloud condensation nuclei closure study on long-term observation data

    NASA Astrophysics Data System (ADS)

    Schmale, Julia; Henning, Silvia; Stratmann, Frank; Henzing, Bas; Kos, Gerard; Schlag, Patrick; Holzinger, Ruprecht; Aalto, Pasi; Keskinen, Helmi; Paramonov, Mikhail; Poulain, Laurent; Ovadnevaite, Jurgita; Krüger, Mira; Carbone, Samara; Brito, Joel; Fröhlich, Roman; Herrmann, Erik; Hammer, Emanuel; Baltensperger, Urs; Gysel, Martin

    2016-04-01

    Aerosol-cloud interactions (ACI) are currently the least understood influence on climate change (IPCC, 2013). ACI are largely controlled by the relative change in cloud condensation nuclei (CCN) and ice nuclei (IN) number concentrations. As direct CCN and IN measurements are not always at hand, being able to predict their concentrations is important. Focusing on CCN, we use monitoring type data from 5 stations within the ACTRIS network in Europe (http://www.actris.net/) and the ATTO site in Brazil to compare measured CCN concentrations at various supersaturations with predicted concentrations based on kappa-Köhler theory. The locations represent a variety of different environments including the rain and boreal forests, and continental-remote, marine and high-alpine conditions. At all sites, at least one full year of CCN concentrations, size distribution and chemical composition data were available for the period between 2012 and 2014. Submicron particle chemical composition data were provided by either Aerodyne aerosol mass spectrometers (AMS) or aerosol chemical speciation monitors (ACSM) and used to derive the hygroscopicity parameter kappa. We explore how well standard kappa-Köhler theory can be applied in the different environments. We find kappa ranging between 0.2 (median) for forest environments, 0.35 for continental-remote and high-alpine conditions, and 0.75 for the marine site. Generally, theory can predict actual CCN concentration within ± 25 % with relatively high correlation coefficients > 0.8 for all supersaturations and throughout all seasons. Applying a fixed kappa of 0.3 instead of hourly derived values yields similarly good results in most cases, while it leads to a discrepancy mismatch for the marine site and a slight difference for the rain forest aerosol. In addition, we find a number of mismatches that can be explained by data quality issues rather than deficiencies in the theory. A sensitivity study shows that only unrealistic assumptions

  20. 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.

  1. Cloud condensation nuclei activity and droplet activation kinetics of wet processed regional dust samples and minerals

    NASA Astrophysics Data System (ADS)

    Kumar, P.; Sokolik, I. N.; Nenes, A.

    2011-08-01

    This study reports laboratory measurements of particle size distributions, cloud condensation nuclei (CCN) activity, and droplet activation kinetics of wet generated aerosols from clays, calcite, quartz, and desert soil samples from Northern Africa, East Asia/China, and Northern America. The dependence of critical supersaturation, sc, on particle dry diameter, Ddry, is used to characterize particle-water interactions and assess the ability of Frenkel-Halsey-Hill adsorption activation theory (FHH-AT) and Köhler theory (KT) to describe the CCN activity of the considered samples. Wet generated regional dust samples produce unimodal size distributions with particle sizes as small as 40 nm, CCN activation consistent with KT, and exhibit hygroscopicity similar to inorganic salts. Wet generated clays and minerals produce a bimodal size distribution; the CCN activity of the smaller mode is consistent with KT, while the larger mode is less hydrophilic, follows activation by FHH-AT, and displays almost identical CCN activity to dry generated dust. Ion Chromatography (IC) analysis performed on regional dust samples indicates a soluble fraction that cannot explain the CCN activity of dry or wet generated dust. A mass balance and hygroscopicity closure suggests that the small amount of ions (from low solubility compounds like calcite) present in the dry dust dissolve in the aqueous suspension during the wet generation process and give rise to the observed small hygroscopic mode. Overall these results identify an artifact that may question the atmospheric relevance of dust CCN activity studies using the wet generation method. Based on the method of threshold droplet growth analysis, wet generated mineral aerosols display similar activation kinetics compared to ammonium sulfate calibration aerosol. Finally, a unified CCN activity framework that accounts for concurrent effects of solute and adsorption is developed to describe the CCN activity of aged or hygroscopic dusts.

  2. 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.

  3. 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

  4. Recent Field Measurements of Ice Nuclei Concentration Relation to Aerosol Properties

    NASA Astrophysics Data System (ADS)

    DeMott, P. J.; Sullivan, R. C.; McMeeking, G.; Prenni, A. J.; Hill, T. C.; Franc, G. D.; Sullivan, A. P.; Garcia, E.; Tobo, Y.; Prather, K. A.; Suski, K.; Cazorla, A.; Anderson, J. R.; Kreidenweis, S. M.

    2011-12-01

    It is expected that atmospheric variability of ice nuclei concentrations is governed by a variety of factors related to aerosol physical and chemical properties. Not all particles contribute equally due to the special nature of ice nuclei. The "size requirement" of ice nuclei (Pruppacher and Klett, 1997), partly related to the typical aerosol compositions known to act as ice nuclei (e.g., mineral dust particles, certain biological particles), leads to the relation of ice nuclei number concentrations to larger aerosol concentrations in some cases, but we emphasize here the additional relation to aerosol chemistry. Recent atmospheric ice nuclei measurements focused on biomass burning, mineral dust, pollution and biological particles will be discussed to highlight new assessment of their source contributions on the basis of physical, chemical and biological analysis. Pruppacher, H. R., and J. D. Klett, 1997: Microphysics of Clouds and Precipitation (2nd Edition), Kluwer Academic Press, Dordrecht, 954 pp.

  5. Water adsorption and cloud condensation nuclei activity of calcite and calcite coated with model humic and fulvic acids

    NASA Astrophysics Data System (ADS)

    Hatch, Courtney D.; Gierlus, Kelly M.; Schuttlefield, Jennifer D.; Grassian, Vicki H.

    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 insoluble nuclei, such as mineral dust aerosol. A large fraction of unidentified organic material in aerosol particles is composed of poly-acidic compounds resembling humic substances. The presence of these humic-like substances (HULIS) can alter the water adsorption and CCN activity of mineral dust aerosol. We have measured the CCN activity of model humic and fulvic acids and of mineral dust particles coated with these substances in the laboratory. We find that coatings of humic and fulvic acids on calcite particles significantly increases water adsorption compared to uncoated particles. CCN measurements indicate that humic- or fulvic acid-coated calcite particles are more CCN active than uncoated calcite particles. Additionally, thicker coatings of humic or fulvic acids appear to result in more efficient CCN activity. Thus, mineral dust particles coated with high molecular weight organic materials will take up more water and become more efficient CCN in the atmosphere than uncoated mineral dust particles, potentially altering the effect of mineral dust on the Earth's climate. In addition to the experimental results, we have explored a newly modified Köhler theory for predicting the CCN activity of insoluble, wettable particles based on multi layer water adsorption measurements of calcite.

  6. Direct Measurement of Cloud Condensation Nuclei Chemistry using a New Microfluidic Instrument During the CalWater 2011 Campaign

    NASA Astrophysics Data System (ADS)

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

    2011-12-01

    The CalWater 2011 campaign took place in the California Sierra Nevada with the objective of determining the effects atmospheric rivers and aerosols have on California precipitation. To meet this goal, the role of chemistry on atmospheric aerosols' ability to act as cloud condensation nuclei (CCN) needed to be evaluated because not all aerosols are CCN active. To date, direct measurement of ambient CCN chemistry has been difficult or unobtainable because of the difficulty in obtaining a well-defined CCN population, small aerosol masses, and low measurement flow rates. To address this need, a miniature CCN collector was employed that directly deposits CCN-active aerosol into an aqueous sample solution in a microfluidic device. Microchip electrophoresis (MCE) then performs chemical analysis on the soluble CCN components, and concentrations of water-soluble inorganic anions were obtained. Additional instruments were run alongside the CCN-MCE system to obtain a more complete characterization of the aerosol, including MCE coupled to a collector for all water condensation nuclei (WCN), two aerosol time-of-flight mass spectrometers (ATOFMS), optical CCN counters, condensation particle counters, and aerosol sizing instrumentation. The work discussed here will describe the operation of the CCN-MCE instrument and show the preliminary results obtained for CCN chemistry measurements at the Sugar Pine Reservoir during CalWater 2011. The prototype CCN-MCE analyzer permits online monitoring at a single, constant supersaturation. The outlet stream of the CCN system inertially impacts wetted CCN particles into a buffer-filled sample reservoir for immediate electrophoretic analysis, requiring <1 min per run. The integrated CCN-MCE system collects aerosols at ~0.05 lpm and deposits them into ~20 μL of solution, providing detection limits of ~0.1 μg per cubic meter with 10 min of sampling. Because of the low (mostly rural) aerosol concentrations monitored at the Sugar Pine Reservoir

  7. 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.

  8. 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.

  9. Size-dependent hygroscopicity parameter (κ) and chemical composition of secondary organic cloud condensation nuclei

    NASA Astrophysics Data System (ADS)

    Zhao, D. F.; Buchholz, A.; Kortner, B.; Schlag, P.; Rubach, F.; Kiendler-Scharr, A.; Tillmann, R.; Wahner, A.; Flores, J. M.; Rudich, Y.; Watne, À. K.; Hallquist, M.; Wildt, J.; Mentel, Th. F.

    2015-12-01

    Secondary organic aerosol components (SOA) contribute significantly to the activation of cloud condensation nuclei (CCN) in the atmosphere. The CCN activity of internally mixed submicron SOA particles is often parameterized assuming a size-independent single-hygroscopicity parameter κ. In the experiments done in a large atmospheric reactor (SAPHIR, Simulation of Atmospheric PHotochemistry In a large Reaction chamber, Jülich), we consistently observed size-dependent κ and particle composition for SOA from different precursors in the size range of 50 nm-200 nm. Smaller particles had higher κ and a higher degree of oxidation, although all particles were formed from the same reaction mixture. Since decreasing volatility and increasing hygroscopicity often covary with the degree of oxidation, the size dependence of composition and hence of CCN activity can be understood by enrichment of higher oxygenated, low-volatility hygroscopic compounds in smaller particles. Neglecting the size dependence of κ can lead to significant bias in the prediction of the activated fraction of particles during cloud formation.

  10. 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.

  11. 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

  12. 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.

  13. Biogenic sulphur emissions and inferred non-sea-salt-sulphate cloud condensation nuclei in and around Antarctica

    NASA Astrophysics Data System (ADS)

    O'Dowd, Colin D.; Lowe, Jason A.; Smith, Michael H.; Davison, Brian; Hewitt, C. Nicholas; Harrison, Roy M.

    1997-06-01

    Accumulation mode aerosol properties and biogenic sulphur emissions over the South Atlantic and Antarctic Oceans are examined. Two contrasting air masses, polar and maritime, each possessing distinct aerosol properties, were encountered during the summer months. By examining aerosol volatile properties, polar air masses arriving from the Antarctic continent were shown to consist primarily Of H2SO4 in the accumulation mode size range, with inferred NH+4 to SO=4 molar ratios close to zero. By comparison, air masses of temperate maritime origin were significantly neutralized with molar ratios of ≈1. These results suggest a deficit of ammonia in polar air masses compared with that in maritime air masses. Dimethyl sulphide (DMS) exhibited no correlation with its putative aerosol oxidation products, although spatial coherence in atmospheric concentrations of DMS, methane sulphonic acid (MSA), and non-sea-salt (nss)-sulphate mass was observed. Volatility analysis, used to infer nss-sulphate cloud condensation nuclei (nss-sCCN) active at a supersaturation of ≈0.2%, indicates that nss-sCCN mass and number concentration were best correlated with MSA mass (r≈0.63). Aerosol volatility identified the presence of MSA in submicron non-sea-salt aerosol; however, its contribution to the aerosol mass was small relative to the contribution of sulphuric acid and ammonium bisulphate/sulphate aerosol. The marine sulphur cycle appears strongly coupled to the sea-salt cycle with, typically, 80-90% of nss-sulphate thought to be internally mixed with sea-salt aerosol. During the austral Summer of 1992/1993, a period of strong biological productivity in the Weddell Sea and sub-Antarctic Ocean, particularly during ice-melt, the cruise-average DMS flux of 61 μg m-2 d-1 corresponded to a very modest average nss-sCCN concentration of 21 cm-3. Observed peak values of DMS flux and inferred nss-CCN concentrations during the cruise were 477 μg m-2 d-1 and 64 cm-3, respectively. Events of new

  14. Measurements of cloud condensation nuclei in the stratosphere around the plume of Mount St. Helens

    SciTech Connect

    Rogers, C.F.; Hudson, J.G.; Kocmond, W.C.

    1981-01-01

    Measurements of cloud condensation nuclei were made from small samples of stratospheric air taken from a U-2 aircraft at altitudes ranging from 13 to 19 kilometers. The measured concentrations of nuclei both in and outside the plume from the May and June 1980 eruptions of Mount St. Helens were higher than expected, ranging from about 100 to about 1000 per cubic centimeter active at 1 percent supersaturation.

  15. Measurements of cloud condensation nuclei in the stratosphere around the plume of mount st. Helens.

    PubMed

    Rogers, C F; Hudson, J G; Kocmond, W C

    1981-02-20

    Measurements of cloud condensation nuclei were made from small samples of stratospheric air taken from a U-2 aircraft at altitudes ranging from 13 to 19 kilometers. The measured concentrations of nuclei both in and outside the plume from the May and June 1980 eruptions of Mount St. Helens were higher than expected, ranging from about 100 to about 1000 per cubic centimeter active at 1 percent supersaturation.

  16. 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.

  17. 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.

  18. 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

  19. Measurements of cloud condensation nuclei activity and droplet activation kinetics of fresh unprocessed regional dust samples and minerals

    NASA Astrophysics Data System (ADS)

    Kumar, P.; Sokolik, I. N.; Nenes, A.

    2010-12-01

    This study reports laboratory measurements of cloud condensation nuclei (CCN) activity and droplet activation kinetics of aerosols dry-generated from clays, calcite, quartz, and desert soil samples from Northern Africa, East Asia/China, and Northern America. Based on the observed dependence of critical supersaturation, sc, with particle dry diameter, Ddry, we find that FHH adsorption activation theory is a far more suitable framework for describing fresh dust CCN activity than Köhler theory. One set of FHH parameters (AFFH ~ 2.25 ± 0.75, BFFH ~ 1.20 ± 0.10) can adequately reproduce the measured CCN activity for all species considered, and also explains the large range of hygroscopicities reported in the literature. Based on threshold droplet growth analysis, mineral dust aerosols were found to display retarded activation kinetics compared to ammonium sulfate. Comprehensive simulations of mineral dust activation and growth in the CCN instrument suggest that this retardation is equivalent to a reduction of the water vapor uptake coefficient (relative to that for calibration ammonium sulfate aerosol) by 30-80%. These results suggest that dust particles do not require deliquescent material to act as CCN in the atmosphere.

  20. Measurements of cloud condensation nuclei activity and droplet activation kinetics of fresh unprocessed regional dust samples and minerals

    NASA Astrophysics Data System (ADS)

    Kumar, P.; Sokolik, I. N.; Nenes, A.

    2011-04-01

    This study reports laboratory measurements of cloud condensation nuclei (CCN) activity and droplet activation kinetics of aerosols dry generated from clays, calcite, quartz, and desert soil samples from Northern Africa, East Asia/China, and Northern America. Based on the observed dependence of critical supersaturation, sc, with particle dry diameter, Ddry, we found that FHH (Frenkel, Halsey and Hill) adsorption activation theory is a far more suitable framework for describing fresh dust CCN activity than Köhler theory. One set of FHH parameters (AFHH ∼ 2.25 ± 0.75, BFHH ∼ 1.20 ± 0.10) can adequately reproduce the measured CCN activity for all species considered, and also explains the large range of hygroscopicities reported in the literature. Based on a threshold droplet growth analysis, mineral dust aerosols were found to display retarded activation kinetics compared to ammonium sulfate. Comprehensive simulations of mineral dust activation and growth in the CCN instrument suggest that this retardation is equivalent to a reduction of the water vapor uptake coefficient (relative to that for calibration ammonium sulfate aerosol) by 30-80%. These results suggest that dust particles do not require deliquescent material to act as CCN in the atmosphere.

  1. DESIGN AND PERFORMANCE CHARACTERISTICS OF A TURBULENT MIXING CONDENSATION NUCLEI COUNTER. (R826654)

    EPA Science Inventory

    The design and optimization of operation parameters of a Turbulent Mixing Condensation Nuclei Counter (TMCNC) are discussed as well as its performance using dibutylphthalate (DBP) as the working fluid. A detection limit of 3 nm has been achieved at a flow rate of 2.8 lmin-1<...

  2. Application of the string method to the study of critical nuclei in capillary condensation.

    PubMed

    Qiu, Chunyin; Qian, Tiezheng; Ren, Weiqing

    2008-10-21

    We adopt a continuum description for liquid-vapor phase transition in the framework of mean-field theory and use the string method to numerically investigate the critical nuclei for capillary condensation in a slit pore. This numerical approach allows us to determine the critical nuclei corresponding to saddle points of the grand potential function in which the chemical potential is given in the beginning. The string method locates the minimal energy path (MEP), which is the most probable transition pathway connecting two metastable/stable states in configuration space. From the MEP, the saddle point is determined and the corresponding energy barrier also obtained (for grand potential). Moreover, the MEP shows how the new phase (liquid) grows out of the old phase (vapor) along the most probable transition pathway, from the birth of a critical nucleus to its consequent expansion. Our calculations run from partial wetting to complete wetting with a variable strength of attractive wall potential. In the latter case, the string method presents a unified way for computing the critical nuclei, from film formation at solid surface to bulk condensation via liquid bridge. The present application of the string method to the numerical study of capillary condensation shows the great power of this method in evaluating the critical nuclei in various liquid-vapor phase transitions.

  3. 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.

  4. Mitotic chromatin condensation in vitro using somatic cell extracts and nuclei with variable levels of endogenous topoisomerase II

    PubMed Central

    1990-01-01

    We report the development of a new method for producing mitotic extracts from tissue culture cells. These extracts reproducibly promote the condensation of chromatin in vitro when incubated with purified interphase nuclei. This condensation reaction is not species specific, since nuclei from chicken, human, and hamster cell lines all undergo chromatin condensation upon incubation with the extract. We have used this extract to investigate the role of DNA topoisomerase II (topo II) in the chromosome condensation process. Chromatin condensation does not require the presence of soluble topo II in the mitotic extract. However, the extent of formation of discrete chromosome-like structures correlates with the level of endogenous topo II present in the interphase nuclei. Our results further suggest that chromatin condensation in this extract may involve two processes: chromatin compaction and resolution into discrete chromosomes. PMID:2176652

  5. Measurements of cloud condensation nuclei activity and droplet activation kinetics of wet processed regional dust samples and minerals

    NASA Astrophysics Data System (ADS)

    Kumar, P.; Sokolik, I. N.; Nenes, A.

    2011-04-01

    This study reports laboratory measurements of particle size distributions, cloud condensation nuclei (CCN) activity, and droplet activation kinetics of wet generated aerosols from clays, calcite, quartz, and desert soil samples from Northern Africa, East Asia/China, and Northern America. The dependence of critical supersaturation, sc, on particle dry diameter, Ddry, is used to characterize particle-water interactions and assess the ability of Frenkel-Halsey-Hill adsorption activation theory (FHH-AT) and Köhler theory (KT) to describe the CCN activity of the considered samples. Regional dust samples produce unimodal size distributions with particle sizes as small as 40 nm, CCN activation consistent with KT, and exhibit hygroscopicity similar to inorganic salts. Clays and minerals produce a bimodal size distribution; the CCN activity of the smaller mode is consistent with KT, while the larger mode is less hydrophilic, follows activation by FHH-AT, and displays almost identical CCN activity to dry generated dust. Ion Chromatography (IC) analysis performed on regional dust samples indicates a soluble fraction that cannot explain the CCN activity of dry or wet generated dust. A mass balance and hygroscopicity closure suggests that the small amount of ions (of low solubility compounds like calcite) present in the dry dust dissolve in the aqueous suspension during the wet generation process and give rise to the observed small hygroscopic mode. Overall these results identify an artifact that may question the atmospheric relevance of dust CCN activity studies using the wet generation method. Based on a threshold droplet growth analysis, wet generated mineral aerosols display similar activation kinetics compared to ammonium sulfate calibration aerosol. Finally, a unified CCN activity framework that accounts for concurrent effects of solute and adsorption is developed to describe the CCN activity of aged or hygroscopic dusts.

  6. Comparing the mechanism of water condensation and evaporation in glassy aerosol.

    PubMed

    Bones, David L; Reid, Jonathan P; Lienhard, Daniel M; Krieger, Ulrich K

    2012-07-17

    Atmospheric models generally assume that aerosol particles are in equilibrium with the surrounding gas phase. However, recent observations that secondary organic aerosols can exist in a glassy state have highlighted the need to more fully understand the kinetic limitations that may control water partitioning in ambient particles. Here, we explore the influence of slow water diffusion in the condensed aerosol phase on the rates of both condensation and evaporation, demonstrating that significant inhibition in mass transfer occurs for ultraviscous aerosol, not just for glassy aerosol. Using coarse mode (3-4 um radius) ternary sucrose/sodium chloride/aqueous droplets as a proxy for multicomponent ambient aerosol, we demonstrate that the timescale for particle equilibration correlates with bulk viscosity and can be ≫10(3) s. Extrapolation of these timescales to particle sizes in the accumulation mode (e.g., approximately 100 nm) by applying the Stokes-Einstein equation suggests that the kinetic limitations imposed on mass transfer of water by slow bulk phase diffusion must be more fully investigated for atmospheric aerosol. Measurements have been made on particles covering a range in dynamic viscosity from < 0.1 to > 10(13) Pa s. We also retrieve the radial inhomogeneities apparent in particle composition during condensation and evaporation and contrast the dynamics of slow dissolution of a viscous core into a labile shell during condensation with the slow percolation of water during evaporation through a more homogeneous viscous particle bulk.

  7. Condensational growth and trace species scavenging in stratospheric sulfuric acid/water aerosol droplets

    NASA Technical Reports Server (NTRS)

    Tompson, Robert V., Jr.

    1991-01-01

    Stratospheric aerosols play a significant role in the environment. The composition of aerosols is believed to be a liquid solution of sulfuric acid and water with numerous trace species. Of these trace species, ozone in particular was recognized as being very important in its role of shielding the environment from harmful ultraviolet radiation. Also among the trace species are HCl and ClONO2, the so called chlorine reservoir species and various oxides of nitrogen. The quantity of stratospheric aerosol and its particle size distribution determines, to a large degree, the chemistry present in the stratosphere. Aerosols experience 3 types of growth: nucleation, condensation, and coagulation. The application of condensation investigations to the specific problem of stratospheric aerosols is discussed.

  8. Atmospheric Aerosol Scattering Background Observations

    DTIC Science & Technology

    1988-06-14

    condensation nuclei in the atmosphere, Nature 51:1259- 1267. 16. Whitby , K.T. (1975) Modeling of Atmospheric Aerosol Particle Size Distribution, Prog. Rep...Meteorol. 18:501-509. 33 15. Went, F.W. (1964) The nature of Aitkin condensation nuclei In the atmosphere, Nature 51:1259- 1267. 16. Whitby . K.T. (1975

  9. Condensin I and II behaviour in interphase nuclei and cells undergoing premature chromosome condensation.

    PubMed

    Zhang, Tao; Paulson, James R; Bakhrebah, Muhammed; Kim, Ji Hun; Nowell, Cameron; Kalitsis, Paul; Hudson, Damien F

    2016-05-01

    Condensin is an integral component of the mitotic chromosome condensation machinery, which ensures orderly segregation of chromosomes during cell division. In metazoans, condensin exists as two complexes, condensin I and II. It is not yet clear what roles these complexes may play outside mitosis, and so we have examined their behaviour both in normal interphase and in premature chromosome condensation (PCC). We find that a small fraction of condensin I is retained in interphase nuclei, and our data suggests that this interphase nuclear condensin I is active in both gene regulation and chromosome condensation. Furthermore, live cell imaging demonstrates condensin II dramatically increases on G1 nuclei following completion of mitosis. Our PCC studies show condensins I and II and topoisomerase II localise to the chromosome axis in G1-PCC and G2/M-PCC, while KIF4 binding is altered. Individually, condensins I and II are dispensable for PCC. However, when both are knocked out, G1-PCC chromatids are less well structured. Our results define new roles for the condensins during interphase and provide new information about the mechanism of PCC.

  10. Quantifying the sources of atmospheric ice nuclei from carbonaceous combustion aerosol

    NASA Astrophysics Data System (ADS)

    Schill, G. P.; Jathar, S.; Galang, A.; Farmer, D.; Friedman, B.; Levin, E. J.; DeMott, P. J.; Kreidenweis, S. M.

    2015-12-01

    Ice nucleation on particles is a fundamental atmospheric process, which governs precipitation, cloud lifetimes, and climate. Despite being a basic atmospheric process, our current understanding of ice nucleation in the atmosphere is low. One reason for this low understanding is that ice nuclei concentrations are low (only ~1 in 105 particles in the free troposphere nucleate ice), making it challenging to identify both the composition and sources of ambient ice nuclei. Carbonaceous combustion aerosol produced from biomass and fossil fuel combustion are one potential source of these ice nuclei, as they contribute to over one-third of all aerosol in the North American free troposphere. Unfortunately, previous results from field measurements in-cloud, aircraft measurements, and laboratory studies are in conflict, with estimates of the impact of combustion aerosol ranging from no effect to rivaling the well-known atmospheric ice nuclei mineral dust. It is, however, becoming clear that aerosols from combustion processes are more complex than model particles, and their ice activity depends greatly on both fuel type and combustion conditions. Given these dependencies, we propose that sampling from real-world biomass burning and fossil fuel sources would provide the most useful new information on the contribution of carbonaceous combustion aerosols to atmospheric ice nuclei particles. To determine the specific contribution of refractory black carbon (rBC) to ice nuclei concentrations, we have coupled the Single Particle Soot Photometer (SP2) to the Colorado State University Continuous Flow Diffusion Chamber (CFDC). The SP2 utilizes laser-induced incandescence to quantify rBC mass on a particle-by-particle basis; in doing so, it also selectively destroys rBC particles by heating them to their vaporization temperature. Thus, the SP2 can be used as a selective pre-filter for rBC into the CFDC. In this work, we will present recent results looking at contribution of diesel

  11. Condensation nuclei measurement in the stratosphere for the NASA ACE program

    NASA Technical Reports Server (NTRS)

    Wilson, James Charles

    1994-01-01

    A condensation nucleus counter which operated at stratospheric pressures was developed, designed, and constructed. It was calibrated in the laboratory. Its response as a function of particle size and concentration was reported. This was the first time that the response of such an instrument was verified in the laboratory. An inlet was constructed which provided near isokinetic sampling. The resulting instrument, the U-2 CNC, was deployed on NASA U-2 aircraft in the study of the climatic effects of aerosol. These studies occurred in March, April, May, July, November, and December of 1992 and in April, May, June, and December of 1983. The U-2 CNC was used in the study of the aerosol cloud resulting from the eruption of El Chichon. It permitted the observation of new particle formation in the stratosphere.

  12. Simulating collisions of thick nuclei in the color glass condensate framework

    NASA Astrophysics Data System (ADS)

    Gelfand, Daniil; Ipp, Andreas; Müller, David

    2016-07-01

    We present our work on the simulation of the early stages of heavy-ion collisions with finite longitudinal thickness in the laboratory frame in 3 +1 dimensions. In particular we study the effects of nuclear thickness on the production of a glasma state in the McLerran-Venugopalan model within the color glass condensate framework. A finite thickness enables us to describe nuclei at lower energies, but forces us to abandon boost invariance. As a consequence, random classical color sources within the nuclei have to be included in the simulation, which is achieved by using the colored particle-in-cell method. We show that the description in the laboratory frame agrees with boost-invariant approaches as a limiting case. Furthermore we investigate collisions beyond boost invariance, in particular the pressure anisotropy in the glasma.

  13. Discrimination of ionic pollutants except condensation nuclei of acid fog using an ultrasonic humidifier.

    PubMed

    Yoshimura, Keiji; Kikuchi, Ryoei; Kimoto, Takashi; Ozeki, Toru; Imano, Kazuhiko; Kajikawa, Masahiro; Ogawa, Nobuaki

    2006-06-01

    Fog droplets in the atmosphere are first produced by the activation of cloud condensation nuclei (CCN), which are originally some ionic compound. Subsequently, the nuclei grow by vapor diffusion. Fog droplets are polluted through the activation process and successive diffusion growth and residence (post activation). We cannot distinguish the effects of the two pollution processes of natural fog water samples. We found that fog droplets can be produced artificially without CCN using an ultrasonic humidifier. Because the artificial fog droplets are not polluted by CCN, the movement of the fog droplets in natural air will take up some pollutants in the air. Consequently, the two pollution processes of fog (the activation of CCN and the post activation process) can be discriminated using data from field experiments. This sampling analytical method is extremely important for further research regarding fog, clouds and environmental chemistry.

  14. Size-resolved cloud condensation nuclei concentration measurements in the Arctic: two case studies from the summer of 2008

    NASA Astrophysics Data System (ADS)

    Zábori, J.; Rastak, N.; Yoon, Y. J.; Riipinen, I.; Ström, J.

    2015-02-01

    The Arctic is one of the most vulnerable regions affected by climate change. Extensive measurement data are needed to understand the atmospheric processes governing this vulnerability. Among these, data describing cloud formation potential are of particular interest, since the indirect effect of aerosols on the climate system is still poorly understood. In this paper we present, for the first time, size-resolved cloud condensation nuclei (CCN) data obtained in the Arctic. The measurements were conducted during two periods in the summer of 2008: one in June, and one in August, at the Zeppelin research station (78°54' N, 11°53' E) in Svalbard. Trajectory analysis indicates that during the measurement period in June 2008, air masses predominantly originated from the Arctic, whereas the measurements from August 2008 were characteristic of mid-latitude air masses. CCN supersaturation (SS) spectra obtained on the 27 June, before size-resolved measurements were begun, and spectra from the 21 and 24 August, conducted before and after the measurement period, revealed similarities between the two months. From the ratio between CCN concentration and the total particle number concentration (CN) as a function of dry particle diameter (Dp) at a SS of 0.4%, the activation diameter (D50), corresponding to CCN / CN = 0.50, was estimated. D50 was found to be 60 and 67 nm for the examined periods in June and August 2008, respectively. Corresponding D50 hygroscopicity parameter (κ) values were estimated to be 0.4 and 0.3 for June and August 2008, respectively. These values can be compared to hygroscopicity values estimated from bulk chemical composition, where κ was calculated to be 0.5 for both June and August 2008. While the agreement between the two months is reasonable, the difference in κ between the different methods indicates a size-dependence in the particle composition, which is likely explained by a higher fraction of sea salt in the bulk aerosol samples.

  15. Size-resolved cloud condensation nuclei concentration measurements in the Arctic: two case studies from the summer of 2008

    NASA Astrophysics Data System (ADS)

    Zábori, J.; Rastak, N.; Yoon, Y. J.; Riipinen, I.; Ström, J.

    2015-12-01

    The Arctic is one of the most vulnerable regions affected by climate change. Extensive measurement data are needed to understand the atmospheric processes governing this vulnerability. Among these, data describing cloud formation potential are of particular interest, since the indirect effect of aerosols on the climate system is still poorly understood. In this paper we present, for the first time, size-resolved cloud condensation nuclei (CCN) data obtained in the Arctic. The measurements were conducted during two periods in the summer of 2008: one in June and one in August, at the Zeppelin research station (78°54´ N, 11°53´ E) in Svalbard. Trajectory analysis indicates that during the measurement period in June 2008, air masses predominantly originated from the Arctic, whereas the measurements from August 2008 were influenced by mid-latitude air masses. CCN supersaturation (SS) spectra obtained on the 27 June, before size-resolved measurements were begun, and spectra from the 21 and 24 August, conducted before and after the measurement period, revealed similarities between the 2 months. From the ratio between CCN concentration and the total particle number concentration (CN) as a function of dry particle diameter (Dp) at a SS of 0.4 %, the activation diameter (D50), corresponding to CCN / CN = 0.50, was estimated. D50 was found to be 60 and 67 nm for the examined periods in June and August 2008, respectively. Corresponding D50 hygroscopicity parameter (κ) values were estimated to be 0.4 and 0.3 for June and August 2008, respectively. These values can be compared to hygroscopicity values estimated from bulk chemical composition, where κ was calculated to be 0.5 for both June and August 2008. While the agreement between the 2 months is reasonable, the difference in κ between the different methods indicates a size dependence in the particle composition, which is likely explained by a higher fraction of inorganics in the bulk aerosol samples.

  16. Cloud condensation nuclei and ice nucleation activity of hydrophobic and hydrophilic soot particles.

    PubMed

    Koehler, Kirsten A; DeMott, Paul J; Kreidenweis, Sonia M; Popovicheva, Olga B; Petters, Markus D; Carrico, Christian M; Kireeva, Elena D; Khokhlova, Tatiana D; Shonija, Natalia K

    2009-09-28

    Cloud condensation nuclei (CCN) activity and ice nucleation behavior (for temperaturesaerosols relevant for atmospheric studies were investigated. Soots were chosen to represent a range of physico-chemical properties, from hydrophobic through a range of hydrophilicity, to hygroscopic. These characteristics were achieved through generation by three different combustion sources; three soots from natural gas pyrolysis (original: TS; graphitized: GTS; and oxidized: TOS), soot from a diffusion flame in an oil lamp burning aviation kerosene (TC1), and soot from a turbulent diffusion flame in an aircraft engine combustor (AEC). All of the samples exhibited some heterogeneity in our experiments, which showed evidence of two or more particle sub-types even within a narrow size cut. The heterogeneity could have resulted from both chemical and sizing differences, the latter attributable in part to particle non-sphericity. Neither GTS nor TS, hydrophobic particles distinguished only by the lower porosity and polarity of the GTS surface, showed CCN activity at or below water supersaturations required for wettable, insoluble particles (the Kelvin limit). TC1 soot particles, despite classification as hydrophilic, did not show CCN activity at or below the Kelvin limit. We attribute this result to the microporosity of this soot. In contrast, oxidized, non-porous, and hydrophilic TOS particles exhibited CCN activation at very near the Kelvin limit, with a small percentage of these particles CCN-active even at lower supersaturations. Due to containing a range of surface coverage of organic and inorganic hydrophilic and hygroscopic compounds, up to approximately 35% of hygroscopic AEC particles were active as CCN, with a small percentage of these particles CCN-active at lower supersaturations. In ice nucleation experiments below -40 degrees C, AEC particles nucleated ice near the expected condition for homogeneous freezing of water from aqueous solutions. In

  17. Test results from a comparative evaluation of a condensation nuclei fire detector

    NASA Technical Reports Server (NTRS)

    Bricker, R. W.

    1985-01-01

    The fire/smoke alarm response of a condensation nuclei fire detector (CNFD) was compared with photoelectric and ionization detectors. Tests were conducted in a former control room 8.5 m by 8.9 with a 2.7 m ceiling. The room had air supplied from above the ceiling and under the floor with return air exiting from ceiling grills. The environment was varied from 278 to 305 K and relative humidities from 8 to 65%. Four detection zones were located in the room. Each zone contained a sampling head for the CNDF, a photodetector, and an ionization detector so that each detector system had four opportunities to alarm during tests. The particle level in the test room was also monitored during tests with a condensation nuclei particle counter. The CNFD responded to 90% of exposures to smoldering plastic and 84% of exposures to visible fire. The photoelectric response was 43 and 12.5% respectively for the same conditions. The ionization response was 9 and 48 respectively.

  18. Electrical Mobility Spectrometer Using a Diethylene Glycol Condensation Particle Counter for Measurement of Aerosol Size Distributions Down to 1 nm

    SciTech Connect

    Jiang, J.; Kuang, C.; Chen, M.; Attoui, M.; McMurry, P. H.

    2011-02-01

    We report a new scanning mobility particle spectrometer (SMPS) for measuring number size distributions of particles down to {approx}1 nm mobility diameter. This SMPS includes an aerosol charger, a TSI 3085 nano differential mobility analyzer (nanoDMA), an ultrafine condensation particle counter (UCPC) using diethylene glycol (DEG) as the working fluid, and a conventional butanol CPC (the 'booster') to detect the small droplets leaving the DEG UCPC. The response of the DEG UCPC to negatively charged sodium chloride particles with mobility diameters ranging from 1-6 nm was measured. The sensitivity of the DEG UCPC to particle composition was also studied by comparing its response to positively charged 1.47 and 1.70 nm tetra-alkyl ammonium ions, sodium chloride, and silver particles. A high resolution differential mobility analyzer was used to generate the test particles. These results show that the response of this UCPC to sub-2 nm particles is sensitive to particle composition. The applicability of the new SMPS for atmospheric measurement was demonstrated during the Nucleation and Cloud Condensation Nuclei (NCCN) field campaign (Atlanta, Georgia, summer 2009). We operated the instrument at saturator and condenser temperatures that allowed the efficient detection of sodium chloride particles but not of air ions having the same mobility. We found that particles as small as 1 nm were detected during nucleation events but not at other times. Factors affecting size distribution measurements, including aerosol charging in the 1-10 nm size range, are discussed. For the charger used in this study, bipolar charging was found to be more effective for sub-2 nm particles than unipolar charging. No ion induced nucleation inside the charger was observed during the NCCN campaign.

  19. A modelling methodology to predict the range of organic components expected to condense to atmospheric aerosol: Sensitivities to fundamental properties and routes for reduced complexity parameterisations

    NASA Astrophysics Data System (ADS)

    Topping, D. O.; McFiggans, G. B.; Barley, M.; Jenkin, M.

    2009-12-01

    Atmospheric aerosol particles are an important yet uncertain component of climate change and air quality. Influencing climate directly by the scattering and absorption of solar radiation and indirectly through their role as cloud condensation nuclei, their radiatively important properties are determined by the chemical composition, mass loading, mixing state and size distribution, as are their impacts on human health. Mechanistic understanding and knowledge of individual compounds involved in the chemical evolution of aerosol particles is far from complete. A full chemical analysis of the organic component of atmospheric aerosols is not available. Whilst explicit hydrocarbon oxidation mechanisms that track many thousands of degradation products of volatile organic compounds (VOC) have been developed, aerosol schemes in large-scale models neglect the majority of chemical components predicted to occur in the organic mixture and will continue to do so in the future. This is a result of prohibitive computational expense of explicit mechanisms which must be avoided via a reduction in complexity (numerical, chemical or both). Reduction mechanisms that neglect compositional information are widely used to derive those parameters deemed important for climatic and health impacts. However, it is possible to make detailed predictions of the range of organic components expected to condense to atmospheric aerosol by combining a gas/particle partitioning model with a detailed gas phase chemical mechanism. Provided they are of sufficient skill, these predictions can be used as the basis for process and composition complexity reduction whilst retaining mechanistic understanding. Here we present development of compound selection methodologies that combine detailed gas phase mechanisms, pure component vapour pressure calculations, thermodynamic properties and a gas/aerosol partition model. As an example, we combine the methodology with the master chemical mechanism (MCM) to simulate

  20. 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.

  1. LIMA (v1.0): A quasi two-moment microphysical scheme driven by a multimodal population of cloud condensation and ice freezing nuclei

    NASA Astrophysics Data System (ADS)

    Vié, B.; Pinty, J.-P.; Berthet, S.; Leriche, M.

    2016-02-01

    The paper describes the LIMA (Liquid Ice Multiple Aerosols) quasi two-moment microphysical scheme, which relies on the prognostic evolution of an aerosol population, and the careful description of the nucleating properties that enable cloud droplets and pristine ice crystals to form from aerosols. Several modes of cloud condensation nuclei (CCN) and ice freezing nuclei (IFN) are considered individually. A special class of partially soluble IFN is also introduced. These "aged" IFN act first as CCN and then as IFN by immersion nucleation at low temperatures. All the CCN modes are in competition with each other, as expressed by the single equation of maximum supersaturation. The IFN are insoluble aerosols that nucleate ice in several ways (condensation, deposition and immersion freezing) assuming the singular hypothesis. The scheme also includes the homogeneous freezing of cloud droplets, the Hallett-Mossop ice multiplication process and the freezing of haze at very low temperatures. LIMA assumes that water vapour is in thermodynamic equilibrium with the population of cloud droplets (adjustment to saturation in warm clouds). In ice clouds, the prediction of the number concentration of the pristine ice crystals is used to compute explicit deposition and sublimation rates (leading to free under/supersaturation over ice). The autoconversion, accretion and self-collection processes shape the raindrop spectra. The initiation of the large crystals and aggregates category is the result of the depositional growth of large crystals beyond a critical size. Aggregation and riming are computed explicitly. Heavily rimed crystals (graupel) can experience a dry or wet growth mode. An advanced version of the scheme includes a separate hail category of particles forming and growing exclusively in the wet growth mode. The sedimentation of all particle types is included. The LIMA scheme is inserted into the Meso-NH cloud-resolving mesoscale model. The flexibility of LIMA is illustrated

  2. Increased delivery of condensation nuclei during the Late Heavy Bombardment to the terrestrial and martian atmospheres

    NASA Astrophysics Data System (ADS)

    Losiak, Anna

    2014-05-01

    During the period of the Late Heavy Bombardment (LHB), between 4.1 and 3.8 Ga, the impact rate within the entire Solar System was up to a few thousand times higher than the current value (Ryder 2002, Bottke et al. 2012, Fassett and Minton 2013). Multiple basin-forming events on inner planets that occurred during this time had a strong but short-lasting (up to few thousands of years) effect on atmospheres of Earth and Mars (Sleep et al. 1989, Segura et al. 2002, 2012). However, the role of the continuous flux of smaller impactors has not been assessed so far. We calculated the amount of meteoric material in the 10^-3 kg to 106 kg size range delivered to Earth and Mars during the LHB based on the impact flux at the top of the Earth's atmosphere based on results from Bland and Artemieva (2006). Those values were recalculated for Mars based on Ivanov and Hartmann (2009) and then recalculated to the LHB peak based on estimates from Ryder (2002), Bottke et al. (2012), Fassett and Minton (2013). During the LHB, the amount of meteoritic material within this size range delivered to Earth was up to ~1.7*10^10 kg/year and 1.4*10^10 kg/year for Mars. The impactors that ablate and are disrupted during atmospheric entry can serve as cloud condensation nuclei (Rosen 1968, Hunten et al. 1980, Ogurtsov and Raspopov 2011). The amount of material delivered during LHB to the upper stratosphere and lower mezosphere (Hunten et al. 1980, Bland and Artemieva 2006) is comparable to the current terrestrial annual emission of mineral cloud condensation nuclei of 0.5-8*10^12 kg/year (Tegen 2003). On Mars, the availability of condensation nuclei is one of the main factors guiding water-ice cloud formation (Montmessin et al. 2004), which is in turn one of the main climatic factors influencing the hydrological cycle (Michaels et al. 2006) and radiative balance of the planet (Haberle et al. 1999, Wordsworth et al. 2013, Urata and Toon 2013). Increased delivery of condensation nuclei during the

  3. Droplet Size Distributions as a function of rainy system type and Cloud Condensation Nuclei concentrations

    NASA Astrophysics Data System (ADS)

    Cecchini, Micael A.; Machado, Luiz A. T.; Artaxo, Paulo

    2014-06-01

    This work aims to study typical Droplet Size Distributions (DSDs) for different types of precipitation systems and Cloud Condensation Nuclei concentrations over the Vale do Paraíba region in southeastern Brazil. Numerous instruments were deployed during the CHUVA (Cloud processes of tHe main precipitation systems in Brazil: a contribUtion to cloud resolVing modeling and to the GPM) Project in Vale do Paraíba campaign, from November 22, 2011 through January 10, 2012. Measurements of CCN (Cloud Condensation Nuclei) and total particle concentrations, along with measurements of rain DSDs and standard atmospheric properties, including temperature, pressure and wind intensity and direction, were specifically made in this study. The measured DSDs were parameterized with a gamma function using the moment method. The three gamma parameters were disposed in a 3-dimensional space, and subclasses were classified using cluster analysis. Seven DSD categories were chosen to represent the different types of DSDs. The DSD classes were useful in characterizing precipitation events both individually and as a group of systems with similar properties. The rainfall regime classification system was employed to categorize rainy events as local convective rainfall, organized convection rainfall and stratiform rainfall. Furthermore, the frequencies of the seven DSD classes were associated to each type of rainy event. The rainfall categories were also employed to evaluate the impact of the CCN concentration on the DSDs. In the stratiform rain events, the polluted cases had a statistically significant increase in the total rain droplet concentrations (TDCs) compared to cleaner events. An average concentration increase from 668 cm- 3 to 2012 cm- 3 for CCN at 1% supersaturation was found to be associated with an increase of approximately 87 m- 3 in TDC for those events. For the local convection cases, polluted events presented a 10% higher mass weighted mean diameter (Dm) on average. For the

  4. Monodisperse aerosol generator

    DOEpatents

    Ortiz, Lawrence W.; Soderholm, Sidney C.

    1990-01-01

    An aerosol generator is described which is capable of producing a monodisperse aerosol within narrow limits utilizing an aqueous solution capable of providing a high population of seed nuclei and an organic solution having a low vapor pressure. The two solutions are cold nebulized, mixed, vaporized, and cooled. During cooling, particles of the organic vapor condense onto the excess seed nuclei, and grow to a uniform particle size.

  5. Modeling immersion freezing with aerosol-dependent prognostic ice nuclei in Arctic mixed-phase clouds

    NASA Astrophysics Data System (ADS)

    Paukert, M.; Hoose, C.

    2014-07-01

    While recent laboratory experiments have thoroughly quantified the ice nucleation efficiency of different aerosol species, the resulting ice nucleation parameterizations have not yet been extensively evaluated in models on different scales. Here the implementation of an immersion freezing parameterization based on laboratory measurements of the ice nucleation active surface site density of mineral dust and ice nucleation active bacteria, accounting for nucleation scavenging of ice nuclei, into a cloud-resolving model with two-moment cloud microphysics is presented. We simulated an Arctic mixed-phase stratocumulus cloud observed during Flight 31 of the Indirect and Semi-Direct Aerosol Campaign near Barrow, Alaska. Through different feedback cycles, the persistence of the cloud strongly depends on the ice number concentration. It is attempted to bring the observed cloud properties, assumptions on aerosol concentration, and composition and ice formation parameterized as a function of these aerosol properties into agreement. Depending on the aerosol concentration and on the ice crystal properties, the simulated clouds are classified as growing, dissipating, and quasi-stable. In comparison to the default ice nucleation scheme, the new scheme requires higher aerosol concentrations to maintain a quasi-stable cloud. The simulations suggest that in the temperature range of this specific case, mineral dust can only contribute to a minor part of the ice formation. The importance of ice nucleation active bacteria and possibly other ice formation modes than immersion freezing remains poorly constrained in the considered case, since knowledge on local variations in the emissions of ice nucleation active organic aerosols in the Arctic is scarce.

  6. Heterogeneous oxidation of pesticides on aerosol condensed phase

    NASA Astrophysics Data System (ADS)

    Socorro, Joanna; Durand, Amandine; Temime-Roussel, Brice; Ravier, Sylvain; Gligorovski, Sasho; Wortham, Henri; Quivet, Etienne

    2015-04-01

    Pesticides are widely used all over the world. It is known that they exhibit adverse health effects and environmental risks due to their physico-chemical properties and their extensive use which is growing every year. They are distributed in the atmosphere, an important vector of dissemination, over long distances away from the target area. The partitioning of pesticides between the gas and particulate phases influences their atmospheric fate. Most of the pesticides are semi-volatile compounds, emphasizing the importance of assessing their heterogeneous reactivity towards atmospheric oxidants. These reactions are important because they are involved in, among others, direct and indirect climate changes, adverse health effects from inhaled particles, effects on cloud chemistry and ozone production. In this work, the importance of atmospheric degradation of pesticides is evaluated on the surface of aerosol deliquescent particles. The photolysis processing and heterogeneous reactivity towards O3 and OH, was evaluated of eight commonly used pesticides (cyprodinil, deltamethrin, difenoconazole, fipronil, oxadiazon, pendimethalin, permethrin, tetraconazole) adsorbed on silica particles. Silicate particles are present in air-borne mineral dust in atmospheric aerosols, and heterogeneous reactions can be different in the presence of these mineral particles. Depending on their origin and conditioning, aerosol particles containing pesticides can have complex and highly porous microstructures, which are influenced by electric charge effects and interaction with water vapour. Therefore, the kinetic experiments and consecutive product studies were performed at atmospherically relevant relative humidity (RH) of 55 %. The identification of surface bound products was performed using GC-(QqQ)-MS/MS and LC-(Q-ToF)-MS/MS and the gas-phase products were on-line monitored by PTR-ToF-MS. Based on the detected and identified reaction products, it was observed that water plays a crucial

  7. Atmospheric Condensational Properties of Ultrafine Chain and Fractal Aerosol Particles

    NASA Technical Reports Server (NTRS)

    Marlow, William H.

    1997-01-01

    The purpose for the research sponsored by this grant was to lay the foundations for qualitative understanding and quantitative description of the equilibrium vapor pressure of water vapor over the irregularly shaped, carbonaceous particles that are present in the atmosphere. This work apparently was the first systematic treatment of the subject. Research was conducted in two complementary components: 1. Calculations were performed of the equilibrium vapor pressure of water over particles comprised of aggregates of spheres in the 50-200 nm radius range. The purposes of this work were two-fold. First, since no systematic treatment of this subject had previously been conducted, its availability would be directly useful for quantitative treatment for a limited range of atmospheric aerosols. Second, it would provide qualitative indications of the effects of highly irregular particle shape on equilibrium vapor pressure of aggregates comprised of smaller spheres.

  8. Condensed-Phase Photochemical Processes in Titan's Aerosols and Surface: The Role of Longer Wavelength Photochemistry

    NASA Technical Reports Server (NTRS)

    Gudipati, Murthy S.; Jacovi, Ronen; Lignell, Antti; Couturier, Isabelle

    2011-01-01

    We will discuss photochemical properties of Titan's organic molecules in the condensed phase as solid aerosols or surface material, from small linear polyyenes (polyacetylenes and polycyanoacetylenes) such as C2H2, C4N2, HC5N, etc. In particular we will focus on photochemistry caused by longer wavelength UV-VIS photons (greater than 250 nm) photons that make it through Titan's atmosphere to the haze region (approximately 100 km) and on to the surface of Titan.

  9. Solid ammonium sulfate aerosols as ice nuclei: a pathway for cirrus cloud formation.

    PubMed

    Abbatt, J P D; Benz, S; Cziczo, D J; Kanji, Z; Lohmann, U; Möhler, O

    2006-09-22

    Laboratory measurements support a cirrus cloud formation pathway involving heterogeneous ice nucleation by solid ammonium sulfate aerosols. Ice formation occurs at low ice-saturation ratios consistent with the formation of continental cirrus and an interhemispheric asymmetry observed for cloud onset. In a climate model, this mechanism provides a widespread source of ice nuclei and leads to fewer but larger ice crystals as compared with a homogeneous freezing scenario. This reduces both the cloud albedo and the longwave heating by cirrus. With the global ammonia budget dominated by agricultural practices, this pathway might further couple anthropogenic activity to the climate system.

  10. MELCOR 1.8.1 assessment: PNL Ice Condenser Aerosol Experiments

    SciTech Connect

    Gross, R.J.

    1993-06-01

    The MELCOR code was used to simulate PNL`s Ice Condenser Experiments 11-6 and 16-11. In these experiments, ZnS was injected into a mixing chamber, and the combined steam/air/aerosol mixture flowed into an ice condenser which was l4.7m tall. Experiment 11-6 was a low flow test; Experiment l6-1l was a high flow test. Temperatures in the ice condenser region and particle retention were measured in these tests. MELCOR predictions compared very well to the experimental data. The MELCOR calculations were also compared to CONTAIN code calculations for the same tests. A number of sensitivity studies were performed. It as found that simulation time step, aerosol parameters such as the number of MAEROS components and sections used and the particle density, and ice condenser parameters such as the energy capacity of the ice, ice heat transfer coefficient multiplier, and ice heat structure characteristic length all could affect the results. Thermal/hydraulic parameters such as control volume equilibrium assumptions, flow loss coefficients, and the bubble rise model were found to affect the results less significantly. MELCOR results were not machine dependent for this problem.

  11. 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

  12. 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

  13. 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

  14. 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

  15. 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

  16. Determining the chemical composition of cloud condensation nuclei. Third progress report

    SciTech Connect

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

    1992-12-01

    This third progress report describes the status of our efforts to develop the instrumentation to collect cloud condensation nuclei (CCN) in amounts sufficient for chemical analysis. During the fall of 1992 we started collecting filter samples of CCN with the laboratory version of the apparatus at Rolla -MO. The mobile version of the apparatus is in the latter stages of construction. This report includes a fairly rigorous discussion of the operation of the CCN sampling system. A statistical model of the operation of the system is presented to show the ability of the system to collect CCN in the two different size ranges for which we plan to determine the chemical composition. A question is raised by the model results about the operation of one of the virtual impactors. It appears to pass a small percent of particles larger than its cut-point that has the potential of contaminating the smallest CCN sample with larger CCN material. Further tests are necessary, but it may be necessary to redesign that impactor. The appendices of the report show pictures of both the laboratory version and the mobile version of the CCN sampling system. The major hardware has been completed, and the mobile version will be in operation within a few weeks.

  17. Performance of TSI 3760 condensation nuclei counter at reduced pressures and flow rates

    SciTech Connect

    Zhiqun Zhang; Liu, B.Y.H. )

    1991-01-01

    This article describes an experimental study of the performance of the TSI model 3760 clean room condensation nuclei counter (CNC) at various pressures and flow rates. Studies were made to determine the counting efficiency of the instrument in the pressure range of 0.1-1 atom and flow rate range of 0.15-1.4 L/min. The counting efficiency curves were found to be shifted to larger particle sizes as the pressure or flow rate was reduced. The low pressure and low flow rate limits of the instrument were also determined. The numerical model developed in a previous study was used to predict the performance of the CNC. The numerical results were compared with the experimental data and found to agree well in the pressure range of 0.2-1.0 atm and flow rate range of 0.3-1.4 L/min. Discrepancies were found to be more significant at the lower pressures and flow rates.

  18. 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

  19. Measurements of the hygroscopic and deliquescence properties of organic compounds of different solubilities in water and their relationship with cloud condensation nuclei activities.

    PubMed

    Chan, Man Nin; Kreidenweis, Sonia M; Chan, Chak K

    2008-05-15

    The initial phase (solid or aqueous droplet) of aerosol particles prior to activation is among the critical factors in determining their cloud condensation nuclei (CCN) activity. Single-particle levitation in an electrodynamic balance (EDB)was used to measure the phase transitions and hygroscopic properties of aerosol particles of 11 organic compounds with different solubilities (10(-1) to 102 g solute/100 g water). We use these data and other literature data to relate the CCN activity and hygroscopicity of organic compounds with different solubilities. The EDB data show that glyoxylic acid, 4-methylphthalic acid, monosaccharides (fructose and mannose), and disaccharides (maltose and lactose) did not crystallize and existed as metastable droplets at low relative humidity (RH). Hygroscopic data from this work and in the literature support earlier studies showing that the CCN activities of compounds with solubilities down to the order of 10(-1) g solute/100 g water can be predicted by standard Köhler theory with the assumption of complete dissolution of the solute at activation. We also demonstrate the use of evaporation data (or efflorescence data), which provides information on the water contents of metastable solutions below the compound deliquescence RH that can be extrapolated to higher dilutions, to predict the CCN activity of organic particles, particularly for sparingly soluble organic compounds that do not deliquesce at RH achievable in the EDB and in the hygroscopic tandem differential mobility analyzer.

  20. Size-resolved cloud condensation nuclei (CCN) activity and closure analysis at the HKUST Supersite in Hong Kong

    NASA Astrophysics Data System (ADS)

    Meng, J. W.; Yeung, M. C.; Li, Y. J.; Lee, B. Y. L.; Chan, C. K.

    2014-09-01

    The cloud condensation nuclei (CCN) properties of atmospheric aerosols were measured on 1-30 May 2011 at the HKUST (Hong Kong University of Science and Technology) Supersite, a coastal site in Hong Kong. Size-resolved CCN activation curves, the ratio of number concentration of CCN (NCCN) to aerosol concentration (NCN) as a function of particle size, were obtained at supersaturation (SS) = 0.15, 0.35, 0.50, and 0.70% using a DMT (Droplet Measurement Technologies) CCN counter (CCNc) and a TSI scanning mobility particle sizer (SMPS). The mean bulk size-integrated NCCN ranged from ~500 cm-3 at SS = 0.15% to ~2100 cm-3 at SS = 0.70%, and the mean bulk NCCN / NCN ratio ranged from 0.16 at SS = 0.15% to 0.65 at SS = 0.70%. The average critical mobility diameters (D50) at SS = 0.15, 0.35, 0.50, and 0.70% were 116, 67, 56, and 46 nm, respectively. The corresponding average hygroscopic parameters (κCCN) were 0.39, 0.36, 0.31, and 0.28. The decrease in κCCN can be attributed to the increase in organic to inorganic volume ratio as particle size decreases, as measured by an Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). The κCCN correlates reasonably well with κAMS_SR based on size-resolved AMS measurements: κAMS_SR = κorg × forg + κinorg × finorg, where forg and finorg are the organic and inorganic volume fractions, respectively, κorg = 0.1 and κinorg = 0.6, with a R2 of 0.51. In closure analysis, NCCN was estimated by integrating the measured size-resolved NCN for particles larger than D50 derived from κ assuming internal mixing state. Estimates using κAMS_SR show that the measured and predicted NCCN were generally within 10% of each other at all four SS. The deviation increased to 26% when κAMS was calculated from bulk PM1 AMS measurements of particles because PM1 was dominated by particles of 200 to 500 nm in diameter, which had a larger inorganic fraction than those of D50 (particle diameter < 200 nm). A constant κ = 0

  1. Efficient Formation of Stratospheric Aerosol for Climate Engineering by Emission of Condensible Vapor from Aircraft

    NASA Technical Reports Server (NTRS)

    Pierce, Jeffrey R.; Weisenstein, Debra K.; Heckendorn, Patricia; Peter. Thomas; Keith, David W.

    2010-01-01

    Recent analysis suggests that the effectiveness of stratospheric aerosol climate engineering through emission of non-condensable vapors such as SO2 is limited because the slow conversion to H2SO4 tends to produce aerosol particles that are too large; SO2 injection may be so inefficient that it is difficult to counteract the radiative forcing due to a CO2 doubling. Here we describe an alternate method in which aerosol is formed rapidly in the plume following injection of H2SO4, a condensable vapor, from an aircraft. This method gives better control of particle size and can produce larger radiative forcing with lower sulfur loadings than SO2 injection. Relative to SO2 injection, it may reduce some of the adverse effects of geoengineering such as radiative heating of the lower stratosphere. This method does not, however, alter the fact that such a geoengineered radiative forcing can, at best, only partially compensate for the climate changes produced by CO2.

  2. Method for producing monodisperse aerosols

    DOEpatents

    Ortiz, Lawrence W.; Soderholm, Sidney C.

    1990-01-01

    An aerosol generator is described which is capable of producing a monodisperse aerosol within narrow limits utilizing an aqueous solution capable of providing a high population of seed nuclei and an organic solution having a low vapor pressure. The two solutions are cold nebulized, mixed, vaporized, and cooled. During cooling, particles of the organic vapor condense onto the excess seed nuclei, and grow to a uniform particle size.

  3. Biological aerosol particles as a key determinant of ice nuclei populations in a forest ecosystem

    NASA Astrophysics Data System (ADS)

    Tobo, Yutaka; Prenni, Anthony J.; DeMott, Paul J.; Huffman, J. Alex; McCluskey, Christina S.; Tian, Guoxun; Pöhlker, Christopher; Pöschl, Ulrich; Kreidenweis, Sonia M.

    2013-09-01

    primary biological aerosol particles (PBAPs) are known to have very high ice nucleating ability under mixed-phase cloud conditions. However, since the abundances of ice nucleation active PBAPs in the atmosphere are generally thought to be extremely small, their importance has remained uncertain. Here we present evidence for the role of PBAPs as atmospheric ice nuclei (IN) active at temperatures ranging from about -34°C to -9°C in a midlatitude ponderosa pine forest ecosystem in summertime. Our measurements show that the number concentrations of IN active at these temperatures were positively correlated with number concentrations of ambient fluorescent biological aerosol particles (FBAPs). Notably, the number concentrations of IN active at warmer temperatures increased quite rapidly in response to increases in the number concentrations of FBAPs. Moreover, we show that a newly-proposed parameterization related to the number concentrations of FBAPs can better reproduce the number concentrations of IN active over the entire temperature range examined, as compared with parameterizations related solely to the number concentrations of total aerosol particles with diameters larger than 0.5 µm as proposed previously. These results suggest that certain PBAPs released from forest biota can indeed play a key role in determining atmospheric IN populations in this ecosystem, especially at warmer temperatures, potentially leading to ice initiation in nearby mixed-phase clouds.

  4. Hygroscopic properties and cloud condensation nuclei activation of limonene-derived organosulfates and their mixtures with ammonium sulfate

    NASA Astrophysics Data System (ADS)

    Hansen, A. M. K.; Hong, J.; Raatikainen, T.; Kristensen, K.; Ylisirniö, A.; Virtanen, A.; Petäjä, T.; Glasius, M.; Prisle, N. L.

    2015-06-01

    Even though organosulfates have been observed as constituents of atmospheric aerosols in a wide range of environments spanning from the subtropics to the high Arctic, their hygroscopic properties have not been investigated prior to this study. Here, limonene-derived organosulfates with a molecular weight of 250 Da (L-OS 250) were synthesized and used for simultaneous measurements with a Hygroscopicity Tandem Differential Mobility Analyzer (H-TDMA) and a Cloud Condensation Nuclei Counter (CCNC) to determine the hygroscopicity parameter, κ, for pure L-OS 250 and mixtures of L-OS 250 with ammonium sulfate (AS) over a wide range of humidity conditions. The κ values derived from measurements with H-TDMA decreased with increasing particle dry size for all chemical compositions investigated, indicating size dependency and/or surface effects. For pure L-OS 250, κ was found to increase with increasing relative humidity, indicating dilution/solubility effects to be significant. Discrepancies in κ between the sub- and supersaturated measurements were observed for L-OS 250, whereas κ of AS and mixed L-OS 250/AS were similar. This discrepancy was primarily ascribed to limited dissolution of L-OS 250 at subsaturated conditions. In general, hygroscopic growth factor, critical activation diameter and κ for the mixed L-OS 250/AS particles converged towards the values of pure AS for mixtures with ≥ 20 % w/w AS. Surface tension measurements of bulk aqueous L-OS 250/AS solutions showed that L-OS 250 was indeed surface active, as expected from its molecular structure, decreasing the surface tension of solutions with 24 % from the pure water-value at a L-OS 250 concentration of 0.0025 mol L-1. Based on these surface tension measurements, we present the first concentration-dependent parametrisation of surface tension for aqueous L-OS 250, which was implemented to different process-level models of L-OS 250 hygroscopicity and CCN activation. The values of κ obtained from the

  5. Hygroscopic properties and cloud condensation nuclei activation of limonene-derived organosulfates and their mixtures with ammonium sulfate

    NASA Astrophysics Data System (ADS)

    Hansen, A. M. K.; Hong, J.; Raatikainen, T.; Kristensen, K.; Ylisirniö, A.; Virtanen, A.; Petäjä, T.; Glasius, M.; Prisle, N. L.

    2015-12-01

    Organosulfates have been observed as constituents of atmospheric aerosols in a wide range of environments; however their hygroscopic properties remain uncharacterised. Here, limonene-derived organosulfates with a molecular weight of 250 Da (L-OS 250) were synthesised and used for simultaneous measurements with a hygroscopicity tandem differential mobility analyser (H-TDMA) and a cloud condensation nuclei counter (CCNC) to determine the hygroscopicity parameter, κ, for pure L-OS 250 and mixtures of L-OS 250 with ammonium sulfate (AS) over a wide range of humidity conditions. The κ values derived from measurements with H-TDMA decreased with increasing particle dry diameter for all chemical compositions investigated, indicating that κH-TDMA depends on particle diameter and/or surface effects; however, it is not clear if this trend is statistically significant. For pure L-OS 250, κ was found to increase with increasing relative humidity, indicating dilution/solubility effects to be significant. Discrepancies in κ between the sub- and supersaturated measurements were observed for L-OS 250, whereas κ of AS and mixed L-OS 250/AS were similar. This discrepancy was primarily ascribed to limited dissolution of L-OS 250 at subsaturated conditions. In general, hygroscopic growth factor, critical particle diameter and κ for the mixed L-OS 250/AS particles converged towards the values of pure AS for mixtures with ≥ 20 % w / w AS. Surface tension measurements of bulk aqueous L-OS 250/AS solutions showed that L-OS 250 was indeed surface active, as expected from its molecular structure, decreasing the surface tension of solutions with 24 % from the pure water value at a L-OS 250 concentration of 0.0025 mol L-1. Based on these surface tension measurements, we present the first concentration-dependent parametrisation of surface tension for aqueous L-OS 250, which was implemented to different process-level models of L-OS 250 hygroscopicity and CCN activation. The values of κ

  6. Dependence of Ice Formation in Sierra Winter Orographic Clouds on the Mixing State of Aerosols Serving as Ice Nuclei

    NASA Astrophysics Data System (ADS)

    DeMott, P. J.; Prather, K. A.; Sullivan, R. C.; Suski, K.; Comstock, J. M.; Tomlinson, J. M.; Rosenfeld, D.; Prenni, A. J.; Cazorla, A.

    2011-12-01

    The CalWater study of February to March 2011 offered the opportunity for observations of aerosols from local, regional and long distance sources as they were integrated into clouds and precipitation in the Sierra Nevada. Single particle chemical analysis of cloud particle residual nuclei and surface precipitation, and their association with changes in cloud microphysical differences, suggest that ice initiation and precipitation formation were strongly affected by intrusions of Asian dust. This is consistent with coincident processing of aerosols present in ambient air and cloud particle residuals as ice nuclei. Elevated ice nuclei concentrations were associated with the presence of dust detected in cloud particle residuals, and dust particles dominated ice nuclei chemical compositions assessed by transmission electron microscopy x-ray analyses at these same times. Evidence of the role of Asian dust as ice nuclei during 2011 are consistent with back trajectory analyses and with recently published observational findings from CalWater Early Start data from 2009. The relative roles of aerosols from the marine boundary layer, biomass burning, and pollution as ice nuclei will also be discussed.

  7. Effect of vehicular traffic, remote sources and new particle formation on the activation properties of cloud condensation nuclei in the megacity of São Paulo, Brazil

    NASA Astrophysics Data System (ADS)

    Souto-Oliveira, Carlos Eduardo; de Fátima Andrade, Maria; Kumar, Prashant; Juliano da Silva Lopes, Fábio; Babinski, Marly; Landulfo, Eduardo

    2016-11-01

    Atmospheric aerosol is the primary source of cloud condensation nuclei (CCN). The microphysics and chemical composition of aerosols can affect cloud development and the precipitation process. Among studies conducted in Latin America, only a handful have reported the impact of urban aerosol on CCN activation parameters such as activation ratio (AR) and activation diameter (Dact). With over 20 million inhabitants, the Metropolitan Area of São Paulo (MASP) is the largest megacity in South America. To our knowledge, this is the first study to assess the impact that remote sources and new particle formation (NPF) events have on CCN activation properties in a South American megacity. The measurements were conducted in the MASP between August and September 2014. We measured the CCN within the 0.2-1.0 % range of supersaturation, together with particle number concentration (PNC) and particle number distribution (PND), as well as trace-element concentrations and black carbon (BC). NPF events were identified on 35 % of the sampling days. Combining multivariate analysis in the form of positive matrix factorization (PMF) with an aerosol profile from lidar and HYSPLIT model analyses allowed us to identify the main contribution of vehicular traffic on all days and sea salt and biomass burning from remote regions on 28 and 21 % of the sampling days, respectively. The AR and Dact parameters showed distinct patterns for daytime with intense vehicular traffic and nighttime periods. For example, CCN activation was lower during the daytime than during the nighttime periods, a pattern that was found to be associated mainly with local road-traffic emissions. A decrease in CCN activation was observed on the NPF event days, mainly due to high concentrations of particles with smaller diameters. We also found that aerosols from sea salt, industrial emissions, and biomass burning had minor effects on Dact. For example, nights with biomass burning and vehicular emissions showed slightly lower

  8. Laboratory Testing and Calibration of the Nuclei-Mode Aerosol Size Spectrometer

    NASA Technical Reports Server (NTRS)

    Brock, Charles A.

    1999-01-01

    This grant was awarded to complete testing and calibration of a new instrument, the nuclei-mode aerosol size spectrometer (N-MASS), following its use in the WB-57F Aerosol Measurement (WAM) campaign in early 1998. The N-MASS measures the size distribution of particles in the 4-60 nm diameter range with 1-Hz response at typical free tropospheric conditions. Specific tasks to have been completed under the auspices of this award were: 1) to experimentally determine the instrumental sampling efficiency; 2) to determine the effects of varying temperatures and flows on N-MASS performance; and 3) to calibrate the N-MASS at typical flight conditions as operated in WAM. The work outlined above has been completed, and a journal manuscript based on this work and that describes the performance of the N-MASS is in preparation. Following a brief description of the principles of operation of the instrument, the major findings of this study are described.

  9. Particulate matter and trace-gas changes at Beltsville, MD, and influences on cloud condensation nuclei

    NASA Astrophysics Data System (ADS)

    Doughty, David

    This dissertation seeks to further our understanding of how rainfall processes are affected by the 3 complex interactions among trace gases, aerosols, and clouds in semi-urban areas. (Abstract shortened by ProQuest.).

  10. Comparison of the DiSCmini aerosol monitor to a handheld condensation particle counter and a scanning mobility particle sizer for submicrometer sodium chloride and metal aerosols

    PubMed Central

    Mills, Jessica B.; Park, Jae Hong; Peters, Thomas M.

    2016-01-01

    We evaluated the robust, lightweight DiSCmini (DM) aerosol monitor for its ability to measure the concentration and mean diameter of submicrometer aerosols. Tests were conducted with monodispersed and polydispersed aerosols composed of two particle types (sodium chloride, NaCl, and spark generated metal particles, which simulate particles found in welding fume) at three different steady-state concentration ranges (Low, <103; Medium, 103–104; and High, >104 particles/cm3). Particle number concentration, lung deposited surface area (LDSA) concentration, and mean size measured with the DM were compared to those measured with reference instruments, a scanning mobility particle sizer (SMPS) and a handheld condensation particle counter (CPC). Particle number concentrations measured with the DM were within 21% of those measured by reference instruments for polydisperse aerosols. Poorer agreement was observed for monodispersed aerosols (±35% for most tests and +130% for 300-nm NaCl). LDSA concentrations measured by the DM were 96% to 155% of those estimated with the SMPS. The geometric mean diameters measured with the DM were within 30% of those measured with the SMPS for monodispersed aerosols and within 25% for polydispersed aerosols (except for the case when the aerosol contained a substantial number of particles larger than 300 nm). The accuracy of the DM is reasonable for particles smaller than 300 nm but caution should be exercised when particles larger than 300 nm are present. PMID:23473056

  11. Theory of fermion condensation as an analog of the liquid-drop theory of atomic nuclei

    SciTech Connect

    Khodel, V. A.

    2015-01-15

    We discuss problems of theory of systems with a fermion condensate or, in different words, systems with flat bands pinned to the Fermi surface, employing the duality of the momentum distribution n(p) and the density distribution ρ(r). We propose that the Lifshitz topological phase transition associated with the formation of additional pockets of the Fermi surface is the precursor of fermion condensation.

  12. Studies of ice nuclei at the Leipzig Aerosol Cloud Interaction Simulator and their implications

    NASA Astrophysics Data System (ADS)

    Wex, Heike

    2013-04-01

    Ice containing clouds permanently cover 40% of the earth's surface. Ice formation processes have a large impact on the formation of precipitation, cloud radiative properties, cloud electrification and hence influence both, weather and climate. Our understanding of the physical and chemical processes underlying ice formation is limited. However what we know is that the two main pathways of atmospheric ice formation are homogeneous and heterogeneous ice nucleation. The latter involves aerosol particles that act as ice nuclei inducing cloud droplet freezing at temperatures significantly above the homogeneous freezing threshold temperature. Particles acting as IN are e.g. dust particles, but also biological particles like bacteria, pollen and fungal spores. Different heterogeneous freezing mechanisms do exit, with their relative importance for atmospheric clouds still being debated. However, there are strong indications that immersion freezing is the most important mechanism when considering mixed phase clouds. What we are still lacking is a) the fundamental process understanding on how aerosol particles induce ice nucleation and b) means to quantify ice nucleation in atmospheric models. Concerning a) there most likely is not only one answer, considering the variety of IN found in the atmosphere. With respect to b) different approaches based on either the stochastic or singular hypotheses have been suggested. However it is still being debated which would be a suitable way to parameterize laboratory data for use in atmospheric modeling. In this presentation, both topics will be addressed. Using the Leipzig Aerosol Cloud Interaction Simulator (LACIS) (Hartmann et al., 2011), we examined different types of dust particles with and without coating, and biological particles such as bacteria and pollen, with respect to their immersion freezing behaviour. We will summarize our findings concerning the properties controlling the ice nucleation behaviour of these particles and

  13. 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.

  14. THE INFLUENCE OF WEATHER ON SALT DISTRIBUTIONS AND AEROSOLS ON BEACHES,

    DTIC Science & Technology

    MARINE METEOROLOGY, NUCLEATION), (* SODIUM , MARINE METEOROLOGY), (*BEACHES, SODIUM ), (*ATMOSPHERES, SODIUM ), CALIFORNIA, COASTAL REGIONS...GEOCHEMISTRY, TRANSPORT PROPERTIES, AEROSOLS, SALTS , ATMOSPHERIC CONDENSATION, NUCLEI, AIR POLLUTION, RADIOACTIVE CONTAMINATION, TACTICAL WEAPONS, NUCLEAR WEAPONS, EXPERIMENTAL DATA

  15. Measurements of condensation nuclei in the Airborne Arctic Stratospheric Expedition - Observations of particle production in the polar vortex

    NASA Technical Reports Server (NTRS)

    Wilson, J. C.; Stolzenburg, M. R.; Clark, W. E.; Loewenstein, M.; Ferry, G. V.; Chan, K. R.

    1990-01-01

    The ER-2 Condensation Nucleus Counter (ER-2 CNC) was operated in the Airborne Arctic Stratospheric Expedition (AASE) in January and February 1989. The ER-2 CNC measures the mixing ratio of particles, CN, with diameters from approximately 0.02 to approximately 1 micron. The spatial distribution of CN in the Arctic polar vortex was found to resemble that measured in the Antarctic in the Spring of 1987. The vertical profile of CN in the vortex was lowered by subsidence. At altitudes above the minimum in the CN mixing ratio profile, CN mixing ratios correlated negatively with that of N2O, demonstrating new particle production. CN serve as nuclei in the formation of Polar Stratospheric Clouds (PSCs) and the concentration of CN can affect PSC properties.

  16. Proton-neutron pairing and alpha-type condensation in nuclei

    SciTech Connect

    Sandulescu, N.; Negrea, D.; Gambacurta, D.

    2015-10-15

    We summarize a recent work (N. Sandulescu et al, arXiv:1507.04144) on isoscalar and isovector proton-neutron pairing treated in a formalism which conserves exactly the particle number and the isospin. The formalism is designed for self-conjugate (N=Z) systems of nucleons moving in an axially deformed mean field and interacting through the most general isovector and isoscalar pairing interactions. The ground state of these systems is described by a superposition of two types of condensates, i.e., condensates of isovector quartets, built by two isovector pairs coupled to the total isospin T=0, and condensates of isoscalar proton-neutron pairs. The comparison with the exact solutions of realistic isovector-isoscalar pairing Hamiltonians shows that this formalism is able to describe accurately the pairing correlations energies. It is also shown that, contrary to the majority of HFB calculations, in the present formalism the isovector and isoscalar pairing correlations coexist together for any pairing interactions.

  17. Spatially Resolved Quantification of Chromatin Condensation through Differential Local Rheology in Cell Nuclei Fluorescence Lifetime Imaging.

    PubMed

    Spagnol, Stephen T; Dahl, Kris Noel

    2016-01-01

    The linear sequence of DNA encodes access to the complete set of proteins that carry out cellular functions. Yet, much of the functionality appropriate for each cell is nested within layers of dynamic regulation and organization, including a hierarchy of chromatin structural states and spatial arrangement within the nucleus. There remain limitations in our understanding of gene expression within the context of nuclear organization from an inability to characterize hierarchical chromatin organization in situ. Here we demonstrate the use of fluorescence lifetime imaging microscopy (FLIM) to quantify and spatially resolve chromatin condensation state using cell-permeable, DNA-binding dyes (Hoechst 33342 and PicoGreen). Through in vitro and in situ experiments we demonstrate the sensitivity of fluorescence lifetime to condensation state through the mechanical effects that accompany the structural changes and are reflected through altered viscosity. The establishment of FLIM for resolving and quantifying chromatin condensation state opens the door for single-measurement mechanical studies of the nucleus and for characterizing the role of genome structure and organization in nuclear processes that accompany physiological and pathological changes.

  18. Warming-induced increase in aerosol number concentration likely to moderate climate change

    NASA Astrophysics Data System (ADS)

    Paasonen, Pauli; Asmi, Ari; Petäjä, Tuukka; Kajos, Maija K.; Äijälä, Mikko; Junninen, Heikki; Holst, Thomas; Abbatt, Jonathan P. D.; Arneth, Almut; Birmili, Wolfram; van der Gon, Hugo Denier; Hamed, Amar; Hoffer, András; Laakso, Lauri; Laaksonen, Ari; Richard Leaitch, W.; Plass-Dülmer, Christian; Pryor, Sara C.; Räisänen, Petri; Swietlicki, Erik; Wiedensohler, Alfred; Worsnop, Douglas R.; Kerminen, Veli-Matti; Kulmala, Markku

    2013-06-01

    Atmospheric aerosol particles influence the climate system directly by scattering and absorbing solar radiation, and indirectly by acting as cloud condensation nuclei. Apart from black carbon aerosol, aerosols cause a negative radiative forcing at the top of the atmosphere and substantially mitigate the warming caused by greenhouse gases. In the future, tightening of controls on anthropogenic aerosol and precursor vapour emissions to achieve higher air quality may weaken this beneficial effect. Natural aerosols, too, might affect future warming. Here we analyse long-term observations of concentrations and compositions of aerosol particles and their biogenic precursor vapours in continental mid- and high-latitude environments. We use measurements of particle number size distribution together with boundary layer heights derived from reanalysis data to show that the boundary layer burden of cloud condensation nuclei increases exponentially with temperature. Our results confirm a negative feedback mechanism between the continental biosphere, aerosols and climate: aerosol cooling effects are strengthened by rising biogenic organic vapour emissions in response to warming, which in turn enhance condensation on particles and their growth to the size of cloud condensation nuclei. This natural growth mechanism produces roughly 50% of particles at the size of cloud condensation nuclei across Europe. We conclude that biosphere-atmosphere interactions are crucial for aerosol climate effects and can significantly influence the effects of anthropogenic aerosol emission controls, both on climate and air quality.

  19. Comparison of the DiSCmini aerosol monitor to a handheld condensation particle counter and a scanning mobility particle sizer for submicrometer sodium chloride and metal aerosols.

    PubMed

    Mills, Jessica B; Park, Jae Hong; Peters, Thomas M

    2013-01-01

    We evaluated the robust, lightweight DiSCmini (DM) aerosol monitor for its ability to measure the concentration and mean diameter of submicrometer aerosols. Tests were conducted with monodispersed and polydispersed aerosols composed of two particle types (sodium chloride [NaCl] and spark-generated metal particles, which simulate particles found in welding fume) at three different steady-state concentration ranges (Low, <10(3); Medium, 10(3)-10(4); and High, >10(4) particles/cm(3)). Particle number concentration, lung deposited surface area (LDSA) concentration, and mean size measured with the DM were compared with those measured with reference instruments, a scanning mobility particle sizer (SMPS), and a handheld condensation particle counter (CPC). Particle number concentrations measured with the DM were within 16% of those measured by the CPC for polydispersed aerosols. Poorer agreement was observed for monodispersed aerosols (±35% for most tests and +101% for 300-nm NaCl). LDSA concentrations measured by the DM were 96% to 155% of those estimated with the SMPS. The geometric mean diameters measured with the DM were within 30% of those measured with the SMPS for monodispersed aerosols and within 25% for polydispersed aerosols (except for the case when the aerosol contained a substantial number of particles larger than 300 nm). The accuracy of the DM is reasonable for particles smaller than 300 nm, but caution should be exercised when particles larger than 300 nm are present. [Supplementary materials are available for this article. Go to the publisher's online edition of the Journal of Occupational and Environmental Hygiene for the following free supplemental resources: manufacturer-reported capabilities of instruments used, and information from the SMPS measurements for polydispersed test particles.].

  20. 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.

  1. An overview of the Ice Nuclei Research Unit Jungfraujoch/Cloud and Aerosol Characterization Experiment 2013 (INUIT-JFJ/CLACE-2013)

    NASA Astrophysics Data System (ADS)

    Schneider, Johannes

    2014-05-01

    Ice formation in mixed phase tropospheric clouds is an essential prerequisite for the formation of precipitation at mid-latitudes. Ice formation at temperatures warmer than -35°C is only possible via heterogeneous ice nucleation, but up to now the exact pathways of heterogeneous ice formation are not sufficiently well understood. The research unit INUIT (Ice NUcleation research unIT), funded by the Deutsche Forschungsgemeinschaft (DFG FOR 1525) has been established in 2012 with the objective to investigate heterogeneous ice nucleation by combination of laboratory studies, model calculation and field experiments. The main field campaign of the INUIT project (INUIT-JFJ) was conducted at the High Alpine Research Station Jungfraujoch (Swiss Alps, 3580 m asl) during January and February 2013, in collaboration with several international partners in the framework of CLACE2013. The instrumentation included a large set of aerosol chemical and physical analysis instruments (particle counters, particle sizers, particle mass spectrometers, cloud condensation nuclei counters, ice nucleus counters etc.), that were operated inside the Sphinx laboratory and sampled in mixed phase clouds through two ice selective inlets (Ice-CVI, ISI) as well as through a total aerosol inlet that was used for out-of-cloud aerosol measurements. Besides the on-line measurements, also samples for off-line analysis (ESEM, STXM) have been taken in and out of clouds. Furthermore, several cloud microphysics instruments were operated outside the Sphinx laboratory. First results indicate that a large fraction of ice residues sampled from mixed phase clouds contain organic material, but also mineral dust. Soot and lead were not found to be enriched in ice residues. The concentration of heterogeneous ice nuclei was found to be variable (ranging between < 1 and > 100 per liter) and to be strongly dependent on the operating conditions of the respective IN counter. The number size distribution of ice residues

  2. Criteria for significance of simultaneous presence of both condensible vapors and aerosol particles on mass transfer (deposition) rates

    NASA Technical Reports Server (NTRS)

    Gokoglu, S. A.

    1987-01-01

    The simultaneous presence of aerosol particles and condensible vapors in a saturated boundary layer which may affect deposition rates to subcooled surfaces because of vapor-particle interactions is discussed. Scavenging of condensible vapors by aerosol particles may lead to increased particle size and decreased vapor mass fraction, which alters both vapor and particle deposition rates. Particles, if sufficiently concentrated, may also coagulate. Criteria are provided to assess the significance of such phenomena when particles are already present in the mainstream and are not created inside the boundary layer via homogeneous nucleation. It is determined that there is direct proportionality with: (1) the mass concentration of both condensible vapors and aerosol particles; and (2) the square of the boundary layer thickness to particle diameter ratio (delta d sub p) square. Inverse proportionality was found for mainstream to surface temperature difference if thermophoresis dominates particle transport. It is concluded that the square of the boundary layer thickness to particle diameter ratio is the most critical factor to consider in deciding when to neglect vapor-particle interactions.

  3. Criteria for significance of simultaneous presence of both condensible vapors and aerosol particles on mass transfer (deposition) rates

    NASA Technical Reports Server (NTRS)

    Gokoglu, S. A.

    1986-01-01

    The simultaneous presence of aerosol particles and condensible vapors in a saturated boundary layer which may affect deposition rates to subcooled surfaces because of vapor-particle interactions is discussed. Scavenging of condensible vapors by aerosol particles may lead to increased particle size and decreased vapor mass fraction, which alters both vapor and particle deposition rates. Particles, if sufficiently concentrated, may also coagulate. Criteria are provided to assess the significance of such phenomena when particles are already present in the mainstream and are not created inside the boundary layer via homogeneous nucleation. It is determined that there is direct proportionality with: (1) the mass concentration of both condensible vapors and aerosol particles; and (2) the square of the boundary layer thickness to particle diameter ratio (delta d sub p) square. Inverse proportionality was found for mainstream to surface temperature difference if thermophoresis dominates particle transport. It is concluded that the square of the boundary layer thickness to particle diameter ratio is the most critical factor to consider in deciding when to neglect vapor-particle interactions.

  4. 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.

  5. The effect of residence time on the dynamics of a condensating aerosol in a Hiemenz-type stagnation flow

    NASA Astrophysics Data System (ADS)

    Alshaarawi, Amjad; Zhou, Kun; Scribano, Gianfranco; Attili, Antonio; Bisetti, Fabrizio; Clean Combustion Research Center Team

    2013-11-01

    The effect of residence time on the formation and growth of a condensating aerosol is simulated in a Hiemenz-type stagnation flow setup, for which a unique and well-defined time scale characterizes the velocity field. In this configuration, a hot stream saturated with dibutyle phthalate (DBP) vapor mixes with a cold dry stream. A mixing layer forms at the stagnation plane triggering supersaturation and droplets are generated by homogeneous nucleation. Aerosol dynamics are simulated using the Quadrature Method of Moments (QMOM). Two regimes related to the flow residence time are observed, i.e., a nucleation regime and a condensation regime. The nucleation regime, at short residence times, is characterized by the consumption of DBP vapor into droplets having a negligible effect on the vapor phase. In this regime, both the number density and volume fraction of droplets increase with residence time. In the condensation regime, at long residence times, vapor condensation consumes the vapor phase considerably. For longer residence times, more vapor is consumed, resulting in lower number densities due to the lower nucleation rates, whereas the volume fraction saturates.

  6. Aerosol and nucleation research in support of NASA cloud physics experiments in space. [ice nuclei generator for the atmospheric cloud physics laboratory on Spacelab

    NASA Technical Reports Server (NTRS)

    Vali, G.; Rogers, D.; Gordon, G.; Saunders, C. P. R.; Reischel, M.; Black, R.

    1978-01-01

    Tasks performed in the development of an ice nucleus generator which, within the facility concept of the ACPL, would provide a test aerosol suitable for a large number and variety of potential experiments are described. The impact of Atmospheric Cloud Physics Laboratory scientific functional requirements on ice nuclei generation and characterization subsystems was established. Potential aerosol generating systems were evaluated with special emphasis on reliability, repeatability and general suitability for application in Spacelab. Possible contamination problems associated with aerosol generation techniques were examined. The ice nucleating abilities of candidate test aerosols were examined and the possible impact of impurities on the nucleating abilities of those aerosols were assessed as well as the relative merits of various methods of aerosol size and number density measurements.

  7. Evidence for the predominance of mid-tropopheric aerosols as subtropical anvil nuclei

    SciTech Connect

    Fridland, A; Ackermann, A; Jensen, E; Stevens, D

    2004-04-26

    NASA's recent CRYSTAL-FACE field experiment focused on anvil cirrus clouds, an important but poorly understood element of our climate system. Data obtained include the first comprehensive measurements of aerosols and cloud particles throughout the atmospheric column during the evolution of multiple deep convective storm systems. Coupling these new measurements with detailed cloud simulations that resolve the size distributions of aerosols and cloud particles, we find several lines of evidence that most anvil crystals form on mid-tropospheric rather than boundary layer aerosols. This result defies conventional wisdom and indicates that distant pollution sources may impact anvil clouds more than local sources.

  8. RACORO aerosol data processing

    SciTech Connect

    Elisabeth Andrews

    2011-10-31

    The RACORO aerosol data (cloud condensation nuclei (CCN), condensation nuclei (CN) and aerosol size distributions) need further processing to be useful for model evaluation (e.g., GCM droplet nucleation parameterizations) and other investigations. These tasks include: (1) Identification and flagging of 'splash' contaminated Twin Otter aerosol data. (2) Calculation of actual supersaturation (SS) values in the two CCN columns flown on the Twin Otter. (3) Interpolation of CCN spectra from SGP and Twin Otter to 0.2% SS. (4) Process data for spatial variability studies. (5) Provide calculated light scattering from measured aerosol size distributions. Below we first briefly describe the measurements and then describe the results of several data processing tasks that which have been completed, paving the way for the scientific analyses for which the campaign was designed. The end result of this research will be several aerosol data sets which can be used to achieve some of the goals of the RACORO mission including the enhanced understanding of cloud-aerosol interactions and improved cloud simulations in climate models.

  9. Cloud condensation nuclei (CCN) and HR-ToF-AMS measurements at a coastal site in Hong Kong: size-resolved CCN activity and closure analysis

    NASA Astrophysics Data System (ADS)

    Meng, J. W.; Yeung, M. C.; Li, Y. J.; Lee, B. Y. L.; Chan, C. K.

    2014-04-01

    The cloud condensation nuclei (CCN) properties of atmospheric aerosols were measured on 1-30 May 2011 at a coastal site in Hong Kong. Size-resolved CCN activation curves, the ratio of number concentration of CCN (NCCN) to aerosol concentration (NCN) as a function of particle size, were obtained at supersaturation (SS) = 0.15%, 0.35%, 0.50%, and 0.70% using a DMT CCN counter (CCNc) and a TSI scanning mobility particle sizer (SMPS). The mean bulk size-integrated NCCN ranged from ∼500 cm-3 at SS = 0.15% to ∼2100 cm-3 at SS = 0.70%, and the mean bulk NCCN / NCN ratio ranged from 0.16 at SS = 0.15% to 0.65 at SS = 0.70%. The average critical mobility diameters (D50) at SS = 0.15%, 0.35%, 0.50%, and 0.70% were 116 nm, 67 nm, 56 nm, and 46 nm, respectively. The corresponding average hygroscopic parameters (κCCN) were 0.39, 0.36, 0.31, and 0.28. The decrease in κCCN can be attributed to the increase in organic to inorganic volume ratio as particle size decreases, as measured by an Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). The κCCN correlates reasonably well with κAMS based on size-resolved AMS measurements: κAMS = κorg × forg + κinorg × finorg, where forg and finorg are the organic and inorganic volume fractions, respectively, κorg = 0.1 and κinorg = 0.6, with a R2 of 0.51. In closure analysis, NCCN was estimated by integrating the measured size-resolved NCN for particles larger than D50 derived from κ assuming internal mixing state. Estimates using κAMS from size-resolved AMS measurements show that the measured and predicted NCCN were generally within 10% of each other at all four SS. The deviation increased to 26% when κAMS was calculated from bulk PM1 AMS measurements of particles because PM1 was dominated by particles of 200 nm to 500 nm in diameter, which had a larger inorganic fraction than those of D50 (particle diameter < 200 nm). A constant κ = 0.33 (the average value of size-resolved κAMS over the

  10. 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.

  11. Aerosol and monsoon climate interactions over Asia: AEROSOL AND MONSOON CLIMATE INTERACTIONS

    SciTech Connect

    Li, Zhanqing; Lau, W. K. -M.; Ramanathan, V.; Wu, G.; Ding, Y.; Manoj, M. G.; Liu, J.; Qian, Y.; Li, J.; Zhou, T.; Fan, J.; Rosenfeld, D.; Ming, Y.; Wang, Y.; Huang, J.; Wang, B.; Xu, X.; Lee, S. -S.; Cribb, M.; Zhang, F.; Yang, X.; Zhao, C.; Takemura, T.; Wang, K.; Xia, X.; Yin, Y.; Zhang, H.; Guo, J.; Zhai, P. M.; Sugimoto, N.; Babu, S. S.; Brasseur, G. P.

    2016-11-15

    Asian monsoons and aerosols have been studied extensively which are intertwined in influencing the climate of Asia. This paper provides a comprehensive review of ample studies on Asian aerosol, monsoon and their interactions. The region is the primary source of aerosol emissions of varies species, influenced by distinct weather and climatic regimes. On continental scale, aerosols reduce surface insolation and weaken the land-ocean thermal contrast, thus inhibiting the development of monsoons. Locally, aerosol radiative effects alter the thermodynamic stability and convective potential of the lower atmosphere leading to reduced temperatures, increased atmospheric stability, and weakened wind and atmospheric circulation. The atmospheric thermodynamic state may also be altered by the aerosol serving as cloud condensation nuclei or ice nuclei. Many mechanisms have been put forth regarding how aerosols modulate the amplitude, frequency, intensity, and phase of numerous monsoon climate variables. A wide range of theoretical, observational, and modeling findings on the Asian monsoon, aerosols, and their interactions are synthesized. A new paradigm is proposed on investigating aerosol-monsoon interactions, in which natural aerosols such as desert dust, black carbon from biomass burning, and biogenic aerosols from vegetation are considered integral components of an intrinsic aerosol-monsoon climate system, subject to external forcings of global warming, anthropogenic aerosols, and land use and change. Future research on aerosol-monsoon interactions calls for an integrated approach and international collaborations based on long-term sustained observations, process measurements, and improved models, as well as using observations to constrain model simulations and projections.

  12. Classifying organic materials by oxygen-to-carbon elemental ratio to predict the activation regime of cloud condensation nuclei (CCN)

    NASA Astrophysics Data System (ADS)

    Kuwata, M.; Shao, W.; Lebouteiller, R.; Martin, S. T.

    2012-12-01

    The governing highly soluble, slightly soluble, or insoluble activation regime of organic compounds as cloud condensation nuclei (CCN) was examined as a function of oxygen-to-carbon elemental ratio (O : C). New data were collected for adipic, pimelic, suberic, azelaic and pinonic acids. Secondary organic materials (SOMs) produced by α-pinene ozonolysis and isoprene photo-oxidation were also included in the analysis. The saturation concentrations C of the organic compounds in aqueous solutions served as the key parameter for delineating regimes of CCN activation, and the values of C were tightly correlated to the O : C ratios. The highly soluble, slightly soluble, and insoluble regimes of CCN activation were found to correspond to ranges of [O : C] > 0.6, 0.2 < [O : C] < 0.6, and [O : C] < 0.2, respectively. These classifications were evaluated against CCN activation data of isoprene-derived SOM (O : C = 0.69-0.72) and α-pinene-derived SOM (O : C = 0.38-0.48). Isoprene-derived SOM had highly soluble activation behavior, consistent with its high O : C ratio. For α-pinene-derived SOM, although CCN activation can be modeled as a highly soluble mechanism, this behavior was not predicted by the O : C ratio, for which a slightly soluble mechanism was anticipated. Complexity in chemical composition, resulting in continuous water uptake and the absence of a deliquescence transition that can thermodynamically limit CCN activation, might explain the differences of α-pinene-derived SOM compared to the behavior of pure organic compounds. The present results suggest that atmospheric particles dominated by hydrocarbon-like organic components do not activate (i.e. insoluble regime) whereas those dominated by oxygenated organic components activate (i.e. highly soluble regime).

  13. Classifying organic materials by oxygen-to-carbon elemental ratio to predict the activation regime of Cloud Condensation Nuclei (CCN)

    NASA Astrophysics Data System (ADS)

    Kuwata, M.; Shao, W.; Lebouteiller, R.; Martin, S. T.

    2013-05-01

    The governing highly soluble, slightly soluble, or insoluble activation regime of organic compounds as cloud condensation nuclei (CCN) was examined as a function of oxygen-to-carbon elemental ratio (O : C). New data were collected for adipic, pimelic, suberic, azelaic, and pinonic acids. Secondary organic materials (SOMs) produced by α-pinene ozonolysis and isoprene photo-oxidation were also included in the analysis. The saturation concentrations C of the organic compounds in aqueous solutions served as the key parameter for delineating regimes of CCN activation, and the values of C were tightly correlated to the O : C ratios. The highly soluble, slightly soluble, and insoluble regimes of CCN activation were found to correspond to ranges of [O : C] > 0.6, 0.2 < [O : C] < 0.6, and [O : C] < 0.2, respectively. These classifications were evaluated against CCN activation data of isoprene-derived SOM (O : C = 0.69-0.72) and α-pinene-derived SOM (O : C = 0.38-0.48). Isoprene-derived SOM had highly soluble activation behavior, consistent with its high O : C ratio. For α-pinene-derived SOM, although CCN activation can be modeled as a highly soluble mechanism, this behavior was not predicted by the O : C ratio, for which a slightly soluble mechanism was anticipated. Complexity in chemical composition, resulting in continuous water uptake and the absence of a deliquescence transition that can thermodynamically limit CCN activation, might explain the difference in the behavior of α-pinene-derived SOM compared to that of pure organic compounds. The present results suggest that atmospheric particles dominated by hydrocarbon-like organic components do not activate (i.e., insoluble regime) whereas those dominated by oxygenated organic components activate (i.e., highly soluble regime) for typical atmospheric cloud life cycles.

  14. Properties of cloud condensation nuclei (CCN) in the trade wind marine boundary layer of the western North Atlantic

    NASA Astrophysics Data System (ADS)

    Kristensen, Thomas B.; Müller, Thomas; Kandler, Konrad; Benker, Nathalie; Hartmann, Markus; Prospero, Joseph M.; Wiedensohler, Alfred; Stratmann, Frank

    2016-03-01

    Cloud optical properties in the trade winds over the eastern Caribbean Sea have been shown to be sensitive to cloud condensation nuclei (CCN) concentrations. The objective of the current study was to investigate the CCN properties in the marine boundary layer (MBL) in the tropical western North Atlantic, in order to assess the respective roles of inorganic sulfate, organic species, long-range transported mineral dust and sea-salt particles. Measurements were carried out in June-July 2013, on the east coast of Barbados, and included CCN number concentrations, particle number size distributions and offline analysis of sampled particulate matter (PM) and sampled accumulation mode particles for an investigation of composition and mixing state with transmission electron microscopy (TEM) in combination with energy-dispersive X-ray spectroscopy (EDX). During most of the campaign, significant mass concentrations of long-range transported mineral dust was present in the PM, and influence from local island sources can be ruled out. The CCN and particle number concentrations were similar to what can be expected in pristine marine environments. The hygroscopicity parameter κ was inferred, and values in the range 0.2-0.5 were found during most of the campaign, with similar values for the Aitken and the accumulation mode. The accumulation mode particles studied with TEM were dominated by non-refractory material, and concentrations of mineral dust, sea salt and soot were too small to influence the CCN properties. It is highly likely that the CCN were dominated by a mixture of sulfate species and organic compounds.

  15. Evidence for the predominance of mid-tropospheric aerosols as subtropical anvil cloud nuclei.

    PubMed

    Fridlind, Ann M; Ackerman, Andrew S; Jensen, Eric J; Heymsfield, Andrew J; Poellot, Michael R; Stevens, David E; Wang, Donghai; Miloshevich, Larry M; Baumgardner, Darrel; Lawson, R Paul; Wilson, James C; Flagan, Richard C; Seinfeld, John H; Jonsson, Haflidi H; VanReken, Timothy M; Varutbangkul, Varuntida; Rissman, Tracey A

    2004-04-30

    NASA's recent Cirrus Regional Study of Tropical Anvils and Cirrus Layers-Florida Area Cirrus Experiment focused on anvil cirrus clouds, an important but poorly understood element of our climate system. The data obtained included the first comprehensive measurements of aerosols and cloud particles throughout the atmospheric column during the evolution of multiple deep convective storm systems. Coupling these new measurements with detailed cloud simulations that resolve the size distributions of aerosols and cloud particles, we found several lines of evidence indicating that most anvil crystals form on mid-tropospheric rather than boundary-layer aerosols. This result defies conventional wisdom and suggests that distant pollution sources may have a greater effect on anvil clouds than do local sources.

  16. Aerosol Observing System (AOS) Handbook

    SciTech Connect

    Jefferson, A

    2011-01-17

    The Aerosol Observing System (AOS) is a suite of in situ surface measurements of aerosol optical and cloud-forming properties. The instruments measure aerosol properties that influence the earth’s radiative balance. The primary optical measurements are those of the aerosol scattering and absorption coefficients as a function of particle size and radiation wavelength and cloud condensation nuclei (CCN) measurements as a function of percent supersaturation. Additional measurements include those of the particle number concentration and scattering hygroscopic growth. Aerosol optical measurements are useful for calculating parameters used in radiative forcing calculations such as the aerosol single-scattering albedo, asymmetry parameter, mass scattering efficiency, and hygroscopic growth. CCN measurements are important in cloud microphysical models to predict droplet formation.

  17. Constraining condensed-phase formation kinetics of secondary organic aerosol components from isoprene epoxydiols

    NASA Astrophysics Data System (ADS)

    Riedel, T. P.; Lin, Y.-H.; Zhang, Z.; Chu, K.; Thornton, J. A.; Vizuete, W.; Gold, A.; Surratt, J. D.

    2016-02-01

    Isomeric epoxydiols from isoprene photooxidation (IEPOX) have been shown to produce substantial amounts of secondary organic aerosol (SOA) mass and are therefore considered a major isoprene-derived SOA precursor. Heterogeneous reactions of IEPOX on atmospheric aerosols form various aerosol-phase components or "tracers" that contribute to the SOA mass burden. A limited number of the reaction rate constants for these acid-catalyzed aqueous-phase tracer formation reactions have been constrained through bulk laboratory measurements. We have designed a chemical box model with multiple experimental constraints to explicitly simulate gas- and aqueous-phase reactions during chamber experiments of SOA growth from IEPOX uptake onto acidic sulfate aerosol. The model is constrained by measurements of the IEPOX reactive uptake coefficient, IEPOX and aerosol chamber wall losses, chamber-measured aerosol mass and surface area concentrations, aerosol thermodynamic model calculations, and offline filter-based measurements of SOA tracers. By requiring the model output to match the SOA growth and offline filter measurements collected during the chamber experiments, we derive estimates of the tracer formation reaction rate constants that have not yet been measured or estimated for bulk solutions.

  18. Attribution of the United States “warming hole”: Aerosol indirect effect andprecipitable water vapor

    EPA Science Inventory

    Aerosols can influence the climate indirectly by acting as cloud condensation nuclei and /or ice nuclei, thereby modifying cloud optical properties. Observations show a striking cooling trend in summertime daily maximum temperature (Tmax) in the central and...

  19. Cloud Condensation Nuclei and Chemical Composition of size-resolved particles in a Brazilian megacity: Effect of NPF event, biomass burning and sea salt from remote regions on the CCN properties

    NASA Astrophysics Data System (ADS)

    Souto-Oliveira, Carlos; de Fátima Andrade, Maria; Kumar, Prashant; Lopes, Fabio; Babinski, Marly; Landulfo, Eduado; Vara-Vela, Angel

    2016-04-01

    Atmospheric aerosol particles are an important source of cloud condensation nuclei (CCN). Their microphysics and chemical composition can directly affect development of clouds and precipitation process1,2. Only a few studies in Latin American have reported the impact of urban aerosol on the formation of CCN and their contribution to global climate change3. In this study, we simultaneously measured size distributed particle number concentration (PNC), CCN, black carbon (BC) and elemental concentrations (EC) in aerosol samples from São Paulo city. The PNC was measured by DMPS (model 3936) operated with a DMA (model 3080) and CPC (TSI, model 3010). The CCN was measuredby a single-column continuous-flow stream-wise thermal gradient CCN chamber (DMT CCNC-100). The BC and EC were determined in polycarbonate filter collected by Cascade Impactor (MOUDI-MSP), using a smoke stain reflectometer and an ED-XRF (EDX 700; Shimadzu), respectively. During the study period, which was August to September 2014, four events of new particle formation (NPF), characterizing secondary process of aerosol formation were noted. The total PNC varied between 1106 and 29168 cm-3, while CCN presented concentrations of 206 to 12761 cm-3for SS=1.0%. The PNC showed different concentrations during diurnal and nocturnal periods with average of 16392±7811 cm-3 and 6874±3444cm-3, respectively. The activated ratio (CCN/CN) presented diurnal and nocturnal values of 0.19±0.10 and 0.41±0.18, while apparent activation diameter (Dact,a) was estimated to be 110±29 and 71±28 nm (SS=0.6%), respectively. Combining EC and BC results with air mass trajectory analysis (Lidar aerosol profiles and Hysplit air trajectories), apportionment events were identified for sea salt and biomass burning from coastal and continental regions, respectively. The nocturnal AR and Dact,apresented values of 0.46±0.11 and 49±15 nm (SS=0.6%) for sea salt events as opposed to 0.33±0.14 and 64±30 nm (SS=0.6%) during biomass

  20. A satellite view of aerosols in the climate system

    NASA Technical Reports Server (NTRS)

    Kaufman, Yoram J.; Tanre, Didier; Boucher, Olivier

    2002-01-01

    Anthropogenic aerosols are intricately linked to the climate system and to the hydrologic cycle. The net effect of aerosols is to cool the climate system by reflecting sunlight. Depending on their composition, aerosols can also absorb sunlight in the atmosphere, further cooling the surface but warming the atmosphere in the process. These effects of aerosols on the temperature profile, along with the role of aerosols as cloud condensation nuclei, impact the hydrologic cycle, through changes in cloud cover, cloud properties and precipitation. Unravelling these feedbacks is particularly difficult because aerosols take a multitude of shapes and forms, ranging from desert dust to urban pollution, and because aerosol concentrations vary strongly over time and space. To accurately study aerosol distribution and composition therefore requires continuous observations from satellites, networks of ground-based instruments and dedicated field experiments. Increases in aerosol concentration and changes in their composition, driven by industrialization and an expanding population, may adversely affect the Earth's climate and water supply.

  1. A satellite view of aerosols in the climate system.

    PubMed

    Kaufman, Yoram J; Tanré, Didier; Boucher, Olivier

    2002-09-12

    Anthropogenic aerosols are intricately linked to the climate system and to the hydrologic cycle. The net effect of aerosols is to cool the climate system by reflecting sunlight. Depending on their composition, aerosols can also absorb sunlight in the atmosphere, further cooling the surface but warming the atmosphere in the process. These effects of aerosols on the temperature profile, along with the role of aerosols as cloud condensation nuclei, impact the hydrologic cycle, through changes in cloud cover, cloud properties and precipitation. Unravelling these feedbacks is particularly difficult because aerosols take a multitude of shapes and forms, ranging from desert dust to urban pollution, and because aerosol concentrations vary strongly over time and space. To accurately study aerosol distribution and composition therefore requires continuous observations from satellites, networks of ground-based instruments and dedicated field experiments. Increases in aerosol concentration and changes in their composition, driven by industrialization and an expanding population, may adversely affect the Earth's climate and water supply.

  2. 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.

  3. Direct Quantification of Ice Nucleation Active Bacteria in Aerosols and Precipitation: Their Potential Contribution as Ice Nuclei

    NASA Astrophysics Data System (ADS)

    Hill, T. C.; DeMott, P. J.; Garcia, E.; Moffett, B. F.; Prenni, A. J.; Kreidenweis, S. M.; Franc, G. D.

    2013-12-01

    Ice nucleation active (INA) bacteria are a potentially prodigious source of highly active (≥-12°C) atmospheric ice nuclei, especially from agricultural land. However, we know little about the conditions that promote their release (eg, daily or seasonal cycles, precipitation, harvesting or post-harvest decay of litter) or their typical contribution to the pool of boundary layer ice nucleating particles (INP). To initiate these investigations we developed a quantitative Polymerase Chain Reaction (qPCR) test of the ina gene, the gene that codes for the ice nucleating protein, to directly count INA bacteria in environmental samples. The qPCR test amplifies most forms of the gene and is highly sensitive, able to detect perhaps a single gene copy (ie, a single bacterium) in DNA extracted from precipitation. Direct measurement of the INA bacteria is essential because environmental populations will be a mixture of living, viable-but-not culturable, moribund and dead cells, all of which may retain ice nucleating proteins. Using the qPCR test on leaf washings of plants from three farms in Wyoming, Colorado and Nebraska we found INA bacteria to be abundant on crops, especially on cereals. Mid-summer populations on wheat and barley were ~108/g fresh weigh of foliage. Broadleaf crops, such as corn, alfalfa, sugar beet and potato supported 105-107/g. Unexpectedly, however, in the absence of a significant physical disturbance, such as harvesting, we were unable to detect the ina gene in aerosols sampled above the crops. Likewise, in fresh snow samples taken over two winters, ina genes from a range of INA bacteria were detected in about half the samples but at abundances that equated to INA bacterial numbers that accounted for only a minor proportion of INP active at -10°C. By contrast, in a hail sample from a summer thunderstorm we found 0.3 INA bacteria per INP at -10°C and ~0.5 per hail stone. Although the role of the INA bacteria as warm-temperature INP in these samples

  4. Impacts of alternative fuels in aviation on microphysical aerosol properties and predicted ice nuclei concentration at aircraft cruise altitude

    NASA Astrophysics Data System (ADS)

    Weinzierl, B.; D'Ascoli, E.; Sauer, D. N.; Kim, J.; Scheibe, M.; Schlager, H.; Moore, R.; Anderson, B. E.; Ullrich, R.; Mohler, O.; Hoose, C.

    2015-12-01

    In the past decades air traffic has been substantially growing affecting air quality and climate. According to the International Civil Aviation Authority (ICAO), in the next few years world passenger and freight traffic is expected to increase annually by 6-7% and 4-5%, respectively. One possibility to reduce aviation impacts on the atmosphere and climate might be the replacement of fossil fuels by alternative fuels. However, so far the effects of alternative fuels on particle emissions from aircraft engines and their ability to form contrails remain uncertain. To study the effects of alternative fuels on particle emissions and the formation of contrails, the Alternative Fuel Effects on Contrails and Cruise Emissions (ACCESS) field experiment was conducted in California. In May 2014, the DLR Falcon 20 and the NASA HU-25 jet aircraft were instrumented with an extended aerosol and trace gas payload probing different types of fuels including JP-8 and JP-8 blended with HEFA (Hydroprocessed Esters and Fatty Acids) while the NASA DC8 aircraft acted as the source aircraft for ACCESS-2. Emission measurements were taken in the DC8 exhaust plumes at aircraft cruise level between 9-12 km altitude and at distances between 50 m and 20 km behind the DC8 engines. Here, we will present results from the ACCESS-2 aerosol measurements which show a 30-60% reduction of the non-volatile (mainly black carbon) particle number concentration in the aircraft exhaust for the HEFA-blend compared to conventional JP-8 fuel. Size-resolved particle emission indices show the largest reductions for larger particle sizes suggesting that the HEFA blend contains fewer and smaller black carbon particles. We will combine the airborne measurements with a parameterization of deposition nucleation developed during a number of ice nucleation experiments at the AIDA chamber in Karlsruhe and discuss the impact of alternative fuels on the abundance of potential ice nuclei at cruise conditions.

  5. High concentrations of biological aerosol particles and ice nuclei during and after rain

    NASA Astrophysics Data System (ADS)

    Huffman, J. A.; Pöhlker, C.; Prenni, A. J.; DeMott, P. J.; Mason, R. H.; Robinson, N. H.; Fröhlich-Nowoisky, J.; Tobo, Y.; Després, V. R.; Garcia, E.; Gochis, D. J.; Harris, E.; Müller-Germann, I.; Ruzene, C.; Schmer, B.; Sinha, B.; Day, D. A.; Andreae, M. O.; Jimenez, J. L.; Gallagher, M.; Kreidenweis, S. M.; Bertram, A. K.; Pöschl, U.

    2013-01-01

    Bioaerosols are relevant for public health and may play an important role in the climate system, but their atmospheric abundance, properties and sources are not well understood. Here we show that the concentration of airborne biological particles in a forest ecosystem increases dramatically during rain and that bioparticles are closely correlated with atmospheric ice nuclei (IN). The greatest increase of bioparticles and IN occurred in the size range of 2-6 μm, which is characteristic for bacterial aggregates and fungal spores. By DNA analysis we found high diversities of airborne bacteria and fungi, including human and plant pathogens (mildew, smut and rust fungi, molds, Enterobacteraceae, Pseudomonadaceae). In addition to known bacterial and fungal IN (Pseudomonas sp., Fusarium sporotrichioides), we discovered two species of IN-active fungi that were not previously known as biological ice nucleators (Isaria farinosa and Acremonium implicatum). Our findings suggest that atmospheric bioaerosols, IN and rainfall are more tightly coupled than previously assumed.

  6. High concentrations of biological aerosol particles and ice nuclei during and after rain

    NASA Astrophysics Data System (ADS)

    Huffman, J. Alex; Pöhlker, Christopher; Prenni, Anthony; DeMott, Paul; Mason, Ryan; Robinson, Niall; Fröhlich-Nowoisky, Janine; Tobo, Yutaka; Després, Viviane; Garcia, Elvin; Gochis, David; Sinha, Bärbel; Day, Douglas; Andreae, Meinrat; Jimenez, Jose; Gallagher, Martin; Kreidenweis, Sonia; Bertram, Allan; Pöschl, Ulrich

    2013-04-01

    Bioaerosols are relevant for public health and may play an important role in the climate system, but their atmospheric abundance, properties and sources are not well understood. Here we show that the concentration of airborne biological particles in a forest ecosystem increases dramatically during rain and that bioparticles are closely correlated with atmospheric ice nuclei (IN). The greatest increase of bioparticles and IN occurred in the size range of 2-6 µm, which is characteristic for bacterial aggregates and fungal spores. By DNA analysis we found high diversities of airborne bacteria and fungi, including human and plant pathogens (mildew, smut and rust fungi, molds, Enterobacteraceae, Pseudomonadaceae). In addition to known bacterial and fungal IN (Pseudomonas sp., Fusarium sporotrichioides), we discovered two species of IN-active fungi that were not previously known as biological ice nucleators (Isaria farinosa and Acremonium implicatum). Our findings suggest that atmospheric bioaerosols, IN and rainfall are more tightly coupled than previously assumed.

  7. Some results of an experimental study of the atmospheric aerosol in Tomsk: A combined approach

    SciTech Connect

    Zuev, V.V.

    1996-04-01

    As widely accepted, aerosols strongly contribute to the formation of the earth`s radiation balance through the absorption and scattering of solar radiation. In addition, aerosols, being active condensation nuclei, also have a role in the cloud formation process. In this paper, results are presented of aerosol studies undertaken at the field measurement sites of the Institute of Atmospheric Optics in Tomsk and the Tomsk region.

  8. Aldol Condensation Products and Polyacetals in Organic Films Formed from Reactions of Propanal in Sulfuric Acid at Upper Troposphere/Lower Stratosphere (UT/LS) Aerosol Acidities

    NASA Astrophysics Data System (ADS)

    Bui, J. V. H.; Perez-Montano, S.; Li, E. S. W.; Nelson, T. E.; Ha, K. T.; Leong, L.; Iraci, L. T.; Van Wyngarden, A. L.

    2015-12-01

    Aerosols in the upper troposphere and lower stratosphere (UT/LS) consist mostly of concentrated sulfuric acid (40-80 wt. %) which is highly reflective towards UV and visible radiation. However, airborne measurements have shown that these particles may also contain a significant amount of organic material. Experiments combining organics (propanal, glyoxal and/or methylglyoxal) with sulfuric acid at concentrations typical of UT/LS aerosols produced highly colored surface films (and solutions) that have the potential to impact chemical, optical and/or cloud-forming properties of aerosols. In order to assess the potential for such films to impact aerosol chemistry or climate properties, experiments were performed to identify the chemical processes responsible for film formation. Surface films were analyzed via Attenuated Total Reflectance-FTIR and Nuclear Magnetic Resonance spectroscopies and are shown to consist primarily of aldol condensation products and cyclic and linear polyacetals, the latter of which are likely responsible for separation from the aqueous phase.

  9. High concentrations of biological aerosol particles and ice nuclei during and after rain

    NASA Astrophysics Data System (ADS)

    Huffman, J. A.; Prenni, A. J.; DeMott, P. J.; Pöhlker, C.; Mason, R. H.; Robinson, N. H.; Fröhlich-Nowoisky, J.; Tobo, Y.; Després, V. R.; Garcia, E.; Gochis, D. J.; Harris, E.; Müller-Germann, I.; Ruzene, C.; Schmer, B.; Sinha, B.; Day, D. A.; Andreae, M. O.; Jimenez, J. L.; Gallagher, M.; Kreidenweis, S. M.; Bertram, A. K.; Pöschl, U.

    2013-07-01

    Bioaerosols are relevant for public health and may play an important role in the climate system, but their atmospheric abundance, properties, and sources are not well understood. Here we show that the concentration of airborne biological particles in a North American forest ecosystem increases significantly during rain and that bioparticles are closely correlated with atmospheric ice nuclei (IN). The greatest increase of bioparticles and IN occurred in the size range of 2-6 μm, which is characteristic for bacterial aggregates and fungal spores. By DNA analysis we found high diversities of airborne bacteria and fungi, including groups containing human and plant pathogens (mildew, smut and rust fungi, molds, Enterobacteriaceae, Pseudomonadaceae). In addition to detecting known bacterial and fungal IN (Pseudomonas sp., Fusarium sporotrichioides), we discovered two species of IN-active fungi that were not previously known as biological ice nucleators (Isaria farinosa and Acremonium implicatum). Our findings suggest that atmospheric bioaerosols, IN, and rainfall are more tightly coupled than previously assumed.

  10. Biological aerosol particles and ice nuclei during rain, and other insights (Invited)

    NASA Astrophysics Data System (ADS)

    Huffman, J. A.; Prenni, A. J.; DeMott, P. J.; Pöhlker, C.; Mason, R.; Robinson, N.; Fröhlich-Nowoisky, J.; Tobo, Y.; Després, V.; Gochis, D. J.; Harris, E. J.; Sinha, B.; Day, D. A.; Andreae, M. O.; Jimenez, J. L.; Gallagher, M. W.; Kreidenweis, S. M.; Bertram, A. K.; Poeschl, U.

    2013-12-01

    Bioaerosols are relevant for public health and may play an important role in the climate system, but their atmospheric abundance, properties, and sources are not well understood. Here we show that the concentration of airborne biological particles in a North American forest ecosystem increases significantly during rain and that bioparticles are closely correlated with atmospheric ice nuclei (IN). The greatest increase of bioparticles and IN occurred in the size range of 2-6 μm, which is characteristic for bacterial aggregates and fungal spores. By DNA analysis we found high diversities of airborne bacteria and fungi, including groups containing human and plant pathogens (mildew, smut and rust fungi, molds, Enterobacteraceae, Pseudomonadaceae). In addition to detecting known bacterial and fungal IN (Pseudomonas sp., Fusarium sporotrichioides), we discovered two species of IN-active fungi that were not previously known as biological ice nucleators (Isaria farinosa and Acremonium implicatum). Our findings suggest that atmospheric bioaerosols, IN, and rainfall are more tightly coupled than previously assumed.

  11. Stress induced by premature chromatin condensation triggers chromosome shattering and chromothripsis at DNA sites still replicating in micronuclei or multinucleate cells when primary nuclei enter mitosis.

    PubMed

    Terzoudi, Georgia I; Karakosta, Maria; Pantelias, Antonio; Hatzi, Vasiliki I; Karachristou, Ioanna; Pantelias, Gabriel

    2015-11-01

    Combination of next-generation DNA sequencing, single nucleotide polymorphism array analyses and bioinformatics has revealed the striking phenomenon of chromothripsis, described as complex genomic rearrangements acquired in a single catastrophic event affecting one or a few chromosomes. Via an unproven mechanism, it is postulated that mechanical stress causes chromosome shattering into small lengths of DNA, which are then randomly reassembled by DNA repair machinery. Chromothripsis is currently examined as an alternative mechanism of oncogenesis, in contrast to the present paradigm that considers a stepwise development of cancer. While evidence for the mechanism(s) underlying chromosome shattering during cancer development remains elusive, a number of hypotheses have been proposed to explain chromothripsis, including ionizing radiation, DNA replication stress, breakage-fusion-bridge cycles, micronuclei formation and premature chromosome compaction. In the present work, we provide experimental evidence on the mechanistic basis of chromothripsis and on how chromosomes can get locally shattered in a single catastrophic event. Considering the dynamic nature of chromatin nucleoprotein complex, capable of rapid unfolding, disassembling, assembling and refolding, we first show that chromatin condensation at repairing or replicating DNA sites induces the mechanical stress needed for chromosome shattering to ensue. Premature chromosome condensation is then used to visualize the dynamic nature of interphase chromatin and demonstrate that such mechanical stress and chromosome shattering can also occur in chromosomes within micronuclei or asynchronous multinucleate cells when primary nuclei enter mitosis. Following an aberrant mitosis, chromosomes could find themselves in the wrong place at the wrong time so that they may undergo massive DNA breakage and rearrangement in a single catastrophic event. Specifically, our results support the hypothesis that premature chromosome

  12. Comparison between two Aitken counters and with cloud condensation nuclei counters at the 1980 International CCN Workshop

    NASA Technical Reports Server (NTRS)

    Rogers, C. F.; Mckenzie, R. L.

    1981-01-01

    The Pollak and the TSI 3020 counters agreed to within about 10% at concentrations below 1000 cu cm, whereas above that concentration, substantial systematic differences were observed. When the test aerosol was monodisperse and the CCN counters were operated at supersaturations that should nucleate all the aerosol, the Pollak counter read about 6% to 20% lower than the CCN counter in the concentration range from 250/cu cm to 1800/cu cm. The TSI 3020 read about 20% lower than the CCN counter at concentrations less than 1000/cu cm, and a factor of about two higher at concentrations above 1000/cu cm.

  13. Aerosols

    Atmospheric Science Data Center

    2013-04-17

    ... article title:  Aerosols over Central and Eastern Europe     View Larger Image ... last weeks of March 2003, widespread aerosol pollution over Europe was detected by several satellite-borne instruments. The Multi-angle ...

  14. Multiday production of condensing organic aerosol mass in urban and forest outflow

    DOE PAGES

    Lee-Taylor, J.; Hodzic, A.; Madronich, S.; ...

    2015-01-16

    Secondary organic aerosol (SOA) production in air masses containing either anthropogenic or biogenic (terpene-dominated) emissions is investigated using the explicit gas-phase chemical mechanism generator GECKO-A. Simulations show several-fold increases in SOA mass continuing for multiple days in the urban outflow, even as the initial air parcel is diluted into the regional atmosphere. The SOA mass increase in the forest outflow is more modest (~50%) and of shorter duration (1–2 days). The multiday production in the urban outflow stems from continuing oxidation of gas-phase precursors which persist in equilibrium with the particle phase, and can be attributed to multigenerational reaction productsmore » of both aromatics and alkanes, especially those with relatively low carbon numbers (C4–15). In particular we find large contributions from substituted maleic anhydrides and multi-substituted peroxide-bicyclic alkenes. The results show that the predicted production is a robust feature of our model even under changing atmospheric conditions and different vapor pressure schemes, and contradict the notion that SOA undergoes little mass production beyond a short initial formation period. The results imply that anthropogenic aerosol precursors could influence the chemical and radiative characteristics of the atmosphere over an extremely wide region, and that SOA measurements near precursor sources may routinely underestimate this influence.« less

  15. Multiday production of condensing organic aerosol mass in urban and forest outflow

    DOE PAGES

    Lee-Taylor, J.; Hodzic, A.; Madronich, S.; ...

    2014-07-03

    Secondary organic aerosol (SOA) production in air masses containing either anthropogenic or biogenic (terpene-dominated) emissions is investigated using the explicit gas-phase chemical mechanism generator GECKO-A. Simulations show several-fold increases in SOA mass continuing for several days in the urban outflow, even as the initial air parcel is diluted into the regional atmosphere. The SOA mass increase in the forest outflow is more modest (∼50%) and of shorter duration (1–2 days). The production in the urban outflow stems from continuing oxidation of gas-phase precursors which persist in equilibrium with the particle phase, and can be attributed to multigenerational reaction products ofmore » both aromatics and alkanes. In particular we find large contributions from substituted maleic anhydrides and multi-substituted peroxide-bicyclic alkenes. The results show that the predicted production is a robust feature of our model even under changing atmospheric conditions, and contradict the notion that SOA undergoes little mass production beyond a short initial formation period. The results imply that anthropogenic aerosol precursors could influence the chemical and radiative characteristics of the atmosphere over an extremely wide region, and that SOA measurements near precursor sources may routinely underestimate this influence.« less

  16. Multiday production of condensing organic aerosol mass in urban and forest outflow

    NASA Astrophysics Data System (ADS)

    Lee-Taylor, J.; Hodzic, A.; Madronich, S.; Aumont, B.; Camredon, M.; Valorso, R.

    2014-07-01

    Secondary organic aerosol (SOA) production in air masses containing either anthropogenic or biogenic (terpene-dominated) emissions is investigated using the explicit gas-phase chemical mechanism generator GECKO-A. Simulations show several-fold increases in SOA mass continuing for several days in the urban outflow, even as the initial air parcel is diluted into the regional atmosphere. The SOA mass increase in the forest outflow is more modest (∼50%) and of shorter duration (1-2 days). The production in the urban outflow stems from continuing oxidation of gas-phase precursors which persist in equilibrium with the particle phase, and can be attributed to multigenerational reaction products of both aromatics and alkanes. In particular we find large contributions from substituted maleic anhydrides and multi-substituted peroxide-bicyclic alkenes. The results show that the predicted production is a robust feature of our model even under changing atmospheric conditions, and contradict the notion that SOA undergoes little mass production beyond a short initial formation period. The results imply that anthropogenic aerosol precursors could influence the chemical and radiative characteristics of the atmosphere over an extremely wide region, and that SOA measurements near precursor sources may routinely underestimate this influence.

  17. Multiday production of condensing organic aerosol mass in urban and forest outflow

    NASA Astrophysics Data System (ADS)

    Lee-Taylor, J.; Hodzic, A.; Madronich, S.; Aumont, B.; Camredon, M.; Valorso, R.

    2015-01-01

    Secondary organic aerosol (SOA) production in air masses containing either anthropogenic or biogenic (terpene-dominated) emissions is investigated using the explicit gas-phase chemical mechanism generator GECKO-A. Simulations show several-fold increases in SOA mass continuing for multiple days in the urban outflow, even as the initial air parcel is diluted into the regional atmosphere. The SOA mass increase in the forest outflow is more modest (~50%) and of shorter duration (1-2 days). The multiday production in the urban outflow stems from continuing oxidation of gas-phase precursors which persist in equilibrium with the particle phase, and can be attributed to multigenerational reaction products of both aromatics and alkanes, especially those with relatively low carbon numbers (C4-15). In particular we find large contributions from substituted maleic anhydrides and multi-substituted peroxide-bicyclic alkenes. The results show that the predicted production is a robust feature of our model even under changing atmospheric conditions and different vapor pressure schemes, and contradict the notion that SOA undergoes little mass production beyond a short initial formation period. The results imply that anthropogenic aerosol precursors could influence the chemical and radiative characteristics of the atmosphere over an extremely wide region, and that SOA measurements near precursor sources may routinely underestimate this influence.

  18. 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

  19. 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

  20. On the prolonged lifetime of the El Chichon sulfuric acid aerosol cloud

    NASA Technical Reports Server (NTRS)

    Hofmann, D. J.; Rosen, J. M.

    1987-01-01

    The observed decay of the aerosol mixing ratio following the eruption of El Chichon appears to have been 20-30 percent slower than that following the eruption of Fuego in 1974, even though the sulfuric acid droplets were observed to grow to considerably larger sizes after El Chichon. This suggests the possible presence of a condensation nuclei and sulfuric acid vapor source and continued growth phenomena occurring well after the El Chichon eruption. It is proposed that the source of these nuclei and the associated vapor may be derived from annual evaporation and condensation of aerosol in the high polar regions during stratospheric warming events, with subsequent spreading to lower latitudes.

  1. Measurements of condensation nuclei above the jet stream - Evidence for cross jet transport by waves and new particle formation at high altitudes

    NASA Technical Reports Server (NTRS)

    Wilson, J. C.; Lai, W. T.; Smith, S. D.

    1991-01-01

    Condensation nuclei were used as a tracer in midlatitude NASA Stratosphere-Troposphere Exchange Project (STEP) experiments in April and May 1984 in order to study transport in the stratosphere. The very large scale, mean CN distribution was distorted by waves which had the effect of transporting air with anticyclonic properties several degrees to the cyclonic side of the jet and created a strongly layered structure in the CN distribution. Unfiltered CN data revealed short-wavelength oscillations in the CN distribution at the interface between the transported anticyclonic air parcel and the adjacent cyclonic air mass. These oscillations were also seen in the ozone data and increase the potential for mixing along that interface. If the mixing does occur, a wave mechanism for cross-jet transport has been observed.

  2. 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.

  3. 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.

  4. A modeling study of the response of tropical deep convection to the increase of cloud condensation nuclei concentration: 1. Dynamics and microphysics

    NASA Astrophysics Data System (ADS)

    Wang, Chien

    2005-11-01

    The responses of cloud physical processes of a developing tropical deep convection to the increase of CCN concentration have been studied using a three-dimensional cloud-resolving model. Three sets of model simulations, each consisting of 30 runs initialized using a set of 30 different CCN profiles with maximum concentrations ranging from 50 to 6000/cm3, have been carried out. The finding of this study that cloud droplet number concentration increases while cloud droplet size decreases with aerosol concentration is similar to the previous results mainly revealed in studies of stratiform clouds. However, the responses to increasing aerosol concentration of many other cloud properties illustrated in this study, particularly precipitation, are very different from those found or suggested in studies of stratiform clouds. Increasing CCN concentration causes a stronger convection, added mass of condensed water, and enhanced microphysical conversions, all leading to the increase in precipitation as well as the expansion of the cloud coverage. Interestingly, when initial CCN concentration exceeds a certain level, many of the above effects become insignificant, suggesting a relationship between some cloud properties and the logarithm of CCN concentration and further implying that a more substantial aerosol effect on deep convection could be seen over a clean rather than polluted region. Overall speaking, increasing CCN concentration does not significantly affect the precipitation efficiency. The increase with CCN concentration of upward flux of water vapor entering the cloud thus leads to an enhancement in moistening the free troposphere brought by the modeled cloud, besides adding more precipitation to the ground.

  5. Carbonaceous aerosols influencing atmospheric radiation: Black and organic carbon

    SciTech Connect

    Penner, J.E.

    1994-09-01

    Carbonaceous particles in the atmosphere may both scatter and absorb solar radiation. The fraction associated with the absorbing component is generally referred to as black carbon (BC) and is mainly produced from incomplete combustion processes. The fraction associated with condensed organic compounds is generally referred to as organic carbon (OC) or organic matter and is mainly scattering. Absorption of solar radiation by carbonaceous aerosols may heat the atmosphere, thereby altering the vertical temperature profile, while scattering of solar radiation may lead to a net cooling of the atmosphere/ocean system. Carbonaceous aerosols may also enhance the concentrations of cloud condensation nuclei. This paper summarizes observed concentrations of aerosols in remote continental and marine locations and provides estimates for the fine particle (D < 2.5 {mu}m) source rates of both OC and BC. The source rates for anthropogenic organic aerosols may be as large as the source rates for anthropogenic sulfate aerosols, suggesting a similar magnitude of direct forcing of climate. The role of BC in decreasing the amount of reflected solar radiation by OC and sulfates is discussed. The total estimated forcing depends on the source estimates for organic and black carbon aerosols which are highly uncertain. The role of organic aerosols acting as cloud condensation nuclei (CCN) is also described.

  6. Size-resolved and integral measurements of cloud condensation nuclei (CCN) at the high-alpine site Jungfraujoch

    NASA Astrophysics Data System (ADS)

    Rose, D.; Gunthe, S. S.; Jurányi, Z.; Gysel, M.; Frank, G. P.; Schneider, J.; Curtius, J.; Pöschl, U.

    2013-12-01

    As part of the CLACE-6 campaign we performed size-resolved CCN measurements for a~supersaturation range of S = 0.079 % to 0.66% at the high-alpine research station Jungfraujoch, Switzerland, in March~2007. The derived effective hygroscopicity parameter κ describing the influence of particle composition on CCN activity was on average 0.23-0.30 for Aitken (50-100 nm) and 0.32-0.43 for accumulation mode particles (100-200 nm). The campaign average value of κ = 0.3 is similar to the average value of κ for other continental locations. When air masses came from southeasterly directions crossing the Po Valley in Italy, particles were much more hygroscopic (κ ≈ 0.42) due to large sulfate mass fractions. The κ values obtained at S = 0.079 % exhibited a good negative correlation with the organic mass fractions derived from PM1 aerosol mass spectrometer (AMS) measurements. Applying a simple mixing rule the organic and inorganic mass fractions observed by the AMS could be used to reproduce the temporal fluctuations of the hygroscopicity of accumulation mode particles quite well. We show how during a cloud event the aerosol particles were activated as cloud droplets and then removed from the air by precipitation leaving behind only a small amount of accumulation mode particles consisting mainly of weakly CCN-active particles, most likely externally mixed unprocessed soot particles. During the campaign we had the opportunity to directly compare two DMT CCN counters for a certain time. The total CCN concentration (NCCN,tot) obtained by the two instruments at equal supersaturations agreed well for both possible operating modes: detecting NCCN,tot directly by sampling the polydisperse aerosol with the CCNC, or indirectly by combining size-resolved measurements of the activated fraction with parallel measurements of the particle size distribution (e.g., by SMPS). However, some supersaturation setpoints differed between the two CCNCs by as much as 20% after applying the

  7. A STUDY OF THE ABILITY OF SECONDARY ORGANIC AEROSOL TO ACT AS CLOUD CONDENSATION NUCLEI. (R823514)

    EPA Science Inventory

    The perspectives, information and conclusions conveyed in research project abstracts, progress reports, final reports, journal abstracts and journal publications convey the viewpoints of the principal investigator and may not represent the views and policies of ORD and EPA. Concl...

  8. 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

  9. Spectroscopic studies of non-volatile residue formed by photochemistry of solid C4N2: A model of condensed aerosol formation on Titan

    NASA Astrophysics Data System (ADS)

    Couturier-Tamburelli, Isabelle; Gudipati, Murthy S.; Lignell, Antti; Jacovi, Ronen; Piétri, Nathalie

    2014-05-01

    Following our recent communication (Gudipati, M.S. et al. [2013]. Nat. Commun. 4, 1648. http://dx.doi.org/10.1038/ncomms2649) on the discovery of condensed-phase non-volatile polymeric material with similar spectral features as tholins, we present here a comprehensive spectroscopic study of photochemical formation of polymeric material from condensed dicyanoacetylene (C4N2) ice films. C4N2 is chosen as starting material for the laboratory simulations because of the detection of this and similar molecules (nitriles and cyanoacetylenes) in Titan’s atmosphere. UV-Vis and infrared spectra obtained during long-wavelength (>300 nm) photon irradiation and subsequent warming of the ice films are used to analyze changes in C4N2 ice, evolution of tholins, and derive photopolymerization mechanisms. Our data analysis revealed that many processes occur during the photolysis of condensed Titan’s aerosol analogs, including isomerization and polymerization leading to the formation of long-chain as well as aromatic cyclic polymer molecules. In the light of tremendous new data from the Cassini mission on the seasonal variations in Titan’s atmosphere, our laboratory study and its results provide fresh insight into the formation and evolution of aerosols and haze in Titan’s atmosphere.

  10. The condensation of the corona for the correlation between the hard X-ray photon index Γ and the reflection scaling factor ℜ in active galactic nuclei

    NASA Astrophysics Data System (ADS)

    Qiao, Erlin; Liu, B. F.

    2017-01-01

    Observationally, it is found that there is a strong correlation between the hard X-ray photon index Γ and the Compton reflection scaling factor ℜ in active galactic nuclei. In this paper, we propose that the Γ - ℜ correlation can be explained within the framework of the condensation of the hot corona onto the cold accretion disc around a supermassive black hole. In the model, it is presumed that, initially, a vertically extended hot gas (corona) is supplied to the central supermassive black hole by capturing the interstellar medium and stellar wind. In this scenario, when the initial mass accretion rate dot{M}/ dot{M}_Edd gtrsim 0.01, at a critical radius rd, part of the hot gas begins to condense onto the equatorial disc plane of the black hole, forming an inner cold accretion disc. Then the matter is accreted in the form of the disc-corona structure extending down to the innermost stable circular orbits of the black hole. The size of the inner disc is determined by the initial mass accretion rate. With the increase of the initial mass accretion rate, the size of the inner disc increases, which results in both the increase of the Compton reflection scaling factor ℜ and the increase of the hard X-ray photon index Γ. By comparing with a sample of Seyfert galaxies with well-fitted X-ray spectra, it is found that our model can roughly explain the observations. Finally, we discuss the possibility to apply our model to high mass X-ray binaries, which are believed to be fueled by the hot wind from the companion star.

  11. 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.

  12. Aerosol microphysical processes and properties in Canadian boreal forest fire plumes measured during BORTAS

    NASA Astrophysics Data System (ADS)

    Sakamoto, Kimiko; Allen, James; Coe, Hugh; Taylor, Jonathan; Duck, Thomas; Pierce, Jeffrey

    2013-04-01

    Biomass burning emissions contribute significantly to aerosol concentrations and clound condensation nuclei in many regions of the atmosphere. Plume-aerosol characteristics vary according to age, fuel type, and region. These differences are poorly represented in regional and global aerosol models, and they contribute to large uncertainties in predicted size distributions in biomass-burning-dominated regions. The Quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites (BORTAS) measurement campaign was designed to invesigate boreal biomass burning emissions over Atlantic Canada during July-August of 2011. Aged (2-3 days) biomass burning aerosols originating from western Ontario were measured by an SMPS and AMS on board the British Atmospheric Research Aircraft. We identify the presence of plumes using CO concentrations and acetonitrile enhancement ratios. In-plume aerosol size distributions were collected for six aged plume profiles. The size distributions show an accumulation-mode median diameter of ~240 nm. However, there are persistant nucleation and Aitken modes present in the profiles, even 2-3 days from the source. Without continuous nucleation and condensation (likely SOA production), these small modes would be lost by coagulation in less than 1 day. We use an aerosol microphysics plume model to estimate the mean nucleation and condensation rates necessary to maintain the small aerosols, and calculate how these processes enhance the total number of particles and cloud condensation nuclei in the aged plume.

  13. A large source of low-volatility secondary organic aerosol.

    PubMed

    Ehn, Mikael; Thornton, Joel A; Kleist, Einhard; Sipilä, Mikko; Junninen, Heikki; Pullinen, Iida; Springer, Monika; Rubach, Florian; Tillmann, Ralf; Lee, Ben; Lopez-Hilfiker, Felipe; Andres, Stefanie; Acir, Ismail-Hakki; Rissanen, Matti; Jokinen, Tuija; Schobesberger, Siegfried; Kangasluoma, Juha; Kontkanen, Jenni; Nieminen, Tuomo; Kurtén, Theo; Nielsen, Lasse B; Jørgensen, Solvejg; Kjaergaard, Henrik G; Canagaratna, Manjula; Maso, Miikka Dal; Berndt, Torsten; Petäjä, Tuukka; Wahner, Andreas; Kerminen, Veli-Matti; Kulmala, Markku; Worsnop, Douglas R; Wildt, Jürgen; Mentel, Thomas F

    2014-02-27

    Forests emit large quantities of volatile organic compounds (VOCs) to the atmosphere. Their condensable oxidation products can form secondary organic aerosol, a significant and ubiquitous component of atmospheric aerosol, which is known to affect the Earth's radiation balance by scattering solar radiation and by acting as cloud condensation nuclei. The quantitative assessment of such climate effects remains hampered by a number of factors, including an incomplete understanding of how biogenic VOCs contribute to the formation of atmospheric secondary organic aerosol. The growth of newly formed particles from sizes of less than three nanometres up to the sizes of cloud condensation nuclei (about one hundred nanometres) in many continental ecosystems requires abundant, essentially non-volatile organic vapours, but the sources and compositions of such vapours remain unknown. Here we investigate the oxidation of VOCs, in particular the terpene α-pinene, under atmospherically relevant conditions in chamber experiments. We find that a direct pathway leads from several biogenic VOCs, such as monoterpenes, to the formation of large amounts of extremely low-volatility vapours. These vapours form at significant mass yield in the gas phase and condense irreversibly onto aerosol surfaces to produce secondary organic aerosol, helping to explain the discrepancy between the observed atmospheric burden of secondary organic aerosol and that reported by many model studies. We further demonstrate how these low-volatility vapours can enhance, or even dominate, the formation and growth of aerosol particles over forested regions, providing a missing link between biogenic VOCs and their conversion to aerosol particles. Our findings could help to improve assessments of biosphere-aerosol-climate feedback mechanisms, and the air quality and climate effects of biogenic emissions generally.

  14. Effects of meteoric debris on stratospheric aerosols and gases

    NASA Technical Reports Server (NTRS)

    Turco, R. P.; Toon, O. B.; Whitten, R. C.; Hamill, P.

    1981-01-01

    Characterizations of meteoric dust height and size distributions are obtained using Hunten's calculations of meteor ablation and recondensation rates. The contribution of meteor residues to aerosol composition, the role of meteoric dust as condensation nuclei, and the effects of meteor debris on aerosol size distributions are quantified, and particle surface areas are estimated. The potential importance of heterogeneous chemistry for stratospheric trace gases is discussed. The interaction between H2SO4 vapor and meteor metal vapors is investigated. It is concluded that meteoric particles may dominate the natural stratospheric aerosols at small (less than .01 micron radius) and large (greater than 1 micron radius) sizes under normal conditions.

  15. Calculations of condensation and chemistry in an aircraft contrail

    NASA Technical Reports Server (NTRS)

    Miake-Lye, Richard C.; Brown, R. C.; Anderson, M. R.; Kolb, C. E.

    1994-01-01

    The flow field, chemistry, and condensation nucleation behind a transport airplane are calculated in two regimes using two separate reacting flow codes: first the axisymmetric plume, then the three dimensional vortex wake. The included chemical kinetics equations follow the evolution of the NO(y) and SO(x) chemical families. In the plume regime, the chemistry is coupled with the binary homogeneous formation of sulfate condensation nuclei, where the calculated nucleation rates predict that copious quantities of H2SO4/H2O nuclei are produced in subnanometer sizes. These sulfate aerosols could play a major role in the subsequent condensation of water vapor and the formation of contrails under favorable atmospheric conditions.

  16. Direct observation of metal nanoparticles as heterogeneous nuclei for the condensation of supersaturated organic vapors: Nucleation of size-selected aluminum nanoparticles in acetonitrile and n-hexane vapors

    NASA Astrophysics Data System (ADS)

    Abdelsayed, Victor; Samy El-Shall, M.

    2014-08-01

    This work reports the direct observation and separation of size-selected aluminum nanoparticles acting as heterogeneous nuclei for the condensation of supersaturated vapors of both polar and nonpolar molecules. In the experiment, we study the condensation of supersaturated acetonitrile and n-hexane vapors on charged and neutral Al nanoparticles by activation of the metal nanoparticles to act as heterogeneous nuclei for the condensation of the organic vapor. Aluminum seed nanoparticles with diameters of 1 and 2 nm are capable of acting as heterogeneous nuclei for the condensation of supersaturated acetonitrile and hexane vapors. The comparison between the Kelvin and Fletcher diameters indicates that for the heterogeneous nucleation of both acetonitrile and hexane vapors, particles are activated at significantly smaller sizes than predicted by the Kelvin equation. The activation of the Al nanoparticles occurs at nearly 40% and 65% of the onset of homogeneous nucleation of acetonitrile and hexane supersaturated vapors, respectively. The lower activation of the charged Al nanoparticles in acetonitrile vapor is due to the charge-dipole interaction which results in rapid condensation of the highly polar acetonitrile molecules on the charged Al nanoparticles. The charge-dipole interaction decreases with increasing the size of the Al nanoparticles and therefore at low supersaturations, most of the heterogeneous nucleation events are occurring on neutral nanoparticles. No sign effect has been observed for the condensation of the organic vapors on the positively and negatively charged Al nanoparticles. The present approach of generating metal nanoparticles by pulsed laser vaporization within a supersaturated organic vapor allows for efficient separation between nucleation and growth of the metal nanoparticles and, consequently controls the average particle size, particle density, and particle size distribution within the liquid droplets of the condensing vapor. Strong

  17. Direct observation of metal nanoparticles as heterogeneous nuclei for the condensation of supersaturated organic vapors: Nucleation of size-selected aluminum nanoparticles in acetonitrile and n-hexane vapors

    SciTech Connect

    Abdelsayed, Victor; Samy El-Shall, M.

    2014-08-07

    This work reports the direct observation and separation of size-selected aluminum nanoparticles acting as heterogeneous nuclei for the condensation of supersaturated vapors of both polar and nonpolar molecules. In the experiment, we study the condensation of supersaturated acetonitrile and n-hexane vapors on charged and neutral Al nanoparticles by activation of the metal nanoparticles to act as heterogeneous nuclei for the condensation of the organic vapor. Aluminum seed nanoparticles with diameters of 1 and 2 nm are capable of acting as heterogeneous nuclei for the condensation of supersaturated acetonitrile and hexane vapors. The comparison between the Kelvin and Fletcher diameters indicates that for the heterogeneous nucleation of both acetonitrile and hexane vapors, particles are activated at significantly smaller sizes than predicted by the Kelvin equation. The activation of the Al nanoparticles occurs at nearly 40% and 65% of the onset of homogeneous nucleation of acetonitrile and hexane supersaturated vapors, respectively. The lower activation of the charged Al nanoparticles in acetonitrile vapor is due to the charge-dipole interaction which results in rapid condensation of the highly polar acetonitrile molecules on the charged Al nanoparticles. The charge-dipole interaction decreases with increasing the size of the Al nanoparticles and therefore at low supersaturations, most of the heterogeneous nucleation events are occurring on neutral nanoparticles. No sign effect has been observed for the condensation of the organic vapors on the positively and negatively charged Al nanoparticles. The present approach of generating metal nanoparticles by pulsed laser vaporization within a supersaturated organic vapor allows for efficient separation between nucleation and growth of the metal nanoparticles and, consequently controls the average particle size, particle density, and particle size distribution within the liquid droplets of the condensing vapor. Strong

  18. Direct observation of metal nanoparticles as heterogeneous nuclei for the condensation of supersaturated organic vapors: nucleation of size-selected aluminum nanoparticles in acetonitrile and n-hexane vapors.

    PubMed

    Abdelsayed, Victor; El-Shall, M Samy

    2014-08-07

    This work reports the direct observation and separation of size-selected aluminum nanoparticles acting as heterogeneous nuclei for the condensation of supersaturated vapors of both polar and nonpolar molecules. In the experiment, we study the condensation of supersaturated acetonitrile and n-hexane vapors on charged and neutral Al nanoparticles by activation of the metal nanoparticles to act as heterogeneous nuclei for the condensation of the organic vapor. Aluminum seed nanoparticles with diameters of 1 and 2 nm are capable of acting as heterogeneous nuclei for the condensation of supersaturated acetonitrile and hexane vapors. The comparison between the Kelvin and Fletcher diameters indicates that for the heterogeneous nucleation of both acetonitrile and hexane vapors, particles are activated at significantly smaller sizes than predicted by the Kelvin equation. The activation of the Al nanoparticles occurs at nearly 40% and 65% of the onset of homogeneous nucleation of acetonitrile and hexane supersaturated vapors, respectively. The lower activation of the charged Al nanoparticles in acetonitrile vapor is due to the charge-dipole interaction which results in rapid condensation of the highly polar acetonitrile molecules on the charged Al nanoparticles. The charge-dipole interaction decreases with increasing the size of the Al nanoparticles and therefore at low supersaturations, most of the heterogeneous nucleation events are occurring on neutral nanoparticles. No sign effect has been observed for the condensation of the organic vapors on the positively and negatively charged Al nanoparticles. The present approach of generating metal nanoparticles by pulsed laser vaporization within a supersaturated organic vapor allows for efficient separation between nucleation and growth of the metal nanoparticles and, consequently controls the average particle size, particle density, and particle size distribution within the liquid droplets of the condensing vapor. Strong

  19. 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.

  20. A Simple Model of Global Aerosol Indirect Effects

    SciTech Connect

    Ghan, Steven J.; Smith, Steven J.; Wang, Minghuai; Zhang, Kai; Pringle, K. J.; Carslaw, K. S.; Pierce, Jeffrey; Bauer, Susanne E.; Adams, P. J.

    2013-06-28

    Most estimates of the global mean indirect effect of anthropogenic aerosol on the Earth’s energy balance are from simulations by global models of the aerosol lifecycle coupled with global models of clouds and the hydrologic cycle. Extremely simple models have been developed for integrated assessment models, but lack the flexibility to distinguish between primary and secondary sources of aerosol. Here a simple but more physically-based model expresses the aerosol indirect effect using analytic representations of droplet nucleation, cloud and aerosol vertical structure, and horizontal variability in cloud water and aerosol concentration. Although the simple model is able to produce estimates of aerosol indirect effects that are comparable to those from some global aerosol models using the same global mean aerosol properties, the estimates are found to be sensitive to several uncertain parameters, including the preindustrial cloud condensation nuclei concentration, primary and secondary anthropogenic emissions, the size of the primary particles, the fraction of the secondary anthropogenic emissions that accumulates on the coarse mode, the fraction of the secondary mass that forms new particles, and the sensitivity of liquid water path to droplet number concentration. Aerosol indirect effects are surprisingly linear in emissions. This simple model provides a much stronger physical basis for representing aerosol indirect effects than previous representations in integrated assessment models designed to quickly explore the parameter space of emissions-climate interactions. The model also produces estimates that depend on parameter values in ways that are consistent with results from detailed global aerosol-climate simulation models.

  1. The MODIS Aerosol Algorithm, Products and Validation

    NASA Technical Reports Server (NTRS)

    Remer, L. A.; Kaufman, Y. J.; Tanre, D.; Mattoo, S.; Chu, D. A.; Martins, J. V.; Li, R.-R.; Ichoku, C.; Levy, R. C.; Kleidman, R. G.

    2003-01-01

    The MODerate resolution Imaging Spectroradiometer (MODIS) aboard both NASA's Terra and Aqua satellites is making near global daily observations of the earth in a wide spectral range. These measurements are used to derive spectral aerosol optical thickness and aerosol size parameters over both land and ocean. The aerosol products available over land include aerosol optical thickness at three visible wavelengths, a measure of the fraction of aerosol optical thickness attributed to the fine mode and several derived parameters including reflected spectral solar flux at top of atmosphere. Over ocean, the aerosol optical thickness is provided in seven wavelengths from 0.47 microns to 2.13 microns. In addition, quantitative aerosol size information includes effective radius of the aerosol and quantitative fraction of optical thickness attributed to the fine mode. Spectral aerosol flux, mass concentration and number of cloud condensation nuclei round out the list of available aerosol products over the ocean. The spectral optical thickness and effective radius of the aerosol over the ocean are validated by comparison with two years of AERONET data gleaned from 133 AERONET stations. 8000 MODIS aerosol retrievals colocated with AERONET measurements confirm that one-standard deviation of MODIS optical thickness retrievals fall within the predicted uncertainty of delta tauapproximately equal to plus or minus 0.03 plus or minus 0.05 tau over ocean and delta tay equal to plus or minus 0.05 plus or minus 0.15 tau over land. 271 MODIS aerosol retrievals co-located with AERONET inversions at island and coastal sites suggest that one-standard deviation of MODIS effective radius retrievals falls within delta r_eff approximately equal to 0.11 microns. The accuracy of the MODIS retrievals suggests that the product can be used to help narrow the uncertainties associated with aerosol radiative forcing of global climate.

  2. 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

  3. Aerosol and monsoon climate interactions over Asia

    NASA Astrophysics Data System (ADS)

    Li, Zhanqing; Lau, W. K.-M.; Ramanathan, V.; Wu, G.; Ding, Y.; Manoj, M. G.; Liu, J.; Qian, Y.; Li, J.; Zhou, T.; Fan, J.; Rosenfeld, D.; Ming, Y.; Wang, Y.; Huang, J.; Wang, B.; Xu, X.; Lee, S.-S.; Cribb, M.; Zhang, F.; Yang, X.; Zhao, C.; Takemura, T.; Wang, K.; Xia, X.; Yin, Y.; Zhang, H.; Guo, J.; Zhai, P. M.; Sugimoto, N.; Babu, S. S.; Brasseur, G. P.

    2016-12-01

    The increasing severity of droughts/floods and worsening air quality from increasing aerosols in Asia monsoon regions are the two gravest threats facing over 60% of the world population living in Asian monsoon regions. These dual threats have fueled a large body of research in the last decade on the roles of aerosols in impacting Asian monsoon weather and climate. This paper provides a comprehensive review of studies on Asian aerosols, monsoons, and their interactions. The Asian monsoon region is a primary source of emissions of diverse species of aerosols from both anthropogenic and natural origins. The distributions of aerosol loading are strongly influenced by distinct weather and climatic regimes, which are, in turn, modulated by aerosol effects. On a continental scale, aerosols reduce surface insolation and weaken the land-ocean thermal contrast, thus inhibiting the development of monsoons. Locally, aerosol radiative effects alter the thermodynamic stability and convective potential of the lower atmosphere leading to reduced temperatures, increased atmospheric stability, and weakened wind and atmospheric circulations. The atmospheric thermodynamic state, which determines the formation of clouds, convection, and precipitation, may also be altered by aerosols serving as cloud condensation nuclei or ice nuclei. Absorbing aerosols such as black carbon and desert dust in Asian monsoon regions may also induce dynamical feedback processes, leading to a strengthening of the early monsoon and affecting the subsequent evolution of the monsoon. Many mechanisms have been put forth regarding how aerosols modulate the amplitude, frequency, intensity, and phase of different monsoon climate variables. A wide range of theoretical, observational, and modeling findings on the Asian monsoon, aerosols, and their interactions are synthesized. A new paradigm is proposed on investigating aerosol-monsoon interactions, in which natural aerosols such as desert dust, black carbon from

  4. Aircraft measurements made during the spring maximum of ozone over Hawaii: Peroxides, CO, O3, NOy, condensation nuclei, selected hydrocarbons, halocarbons, and alkyl nitrates between 0.5 and 9 km altitude

    NASA Astrophysics Data System (ADS)

    Ridley, B. A.; Atlas, E. L.; Walega, J. G.; Kok, G. L.; Staffelbach, T. A.; Greenberg, J. P.; Grahek, F. E.; Hess, P. G.; Montzka, D. D.

    1997-08-01

    Between April 22 and May 11, 1992, ten flights of the University of Wyoming King Air were made during the maximum in tropospheric ozone over the central North Pacific Ocean in conjunction with the spring intensive of the second Mauna Loa Observatory Photochemistry Experiment. During the first week of flights, an episode of remarkably large total reactive nitrogen, NOy (˜2 ppbv) persisted in the 5-9 km altitude region for 3-4 days. Backtrajectory calculations combined with the trace gas and aerosol measurements confirm that its source was due primarily to export from northern latitude continental surface regions. The total amount of odd nitrogen transported over Hawaii during this event was estimated to be 1-2% of the annual emissions from subsonic aircraft or from stratospheric input. Throughout the measurement program layers of elevated O3, NOy, condensation nuclei (CN), and other species were frequently found between the onset of the marine boundary layer temperature inversion and 4-5 km altitude. Structure and strong gradients within these layers contribute to the daily variations seen at the 3.4 km elevation of the Mauna Loa Observatory during the nighttime downslope flow. The dryness of these low-altitude layers and the calculated air mass trajectories indicate that export from northern latitudes occurred mainly with subsidence to the Hawaii region rather than from transit just above the boundary layer inversion. There was no evidence of recent stratospheric input to the altitude region sampled below 9 km. However, the observations cannot distinguish whether O3 input from the stratosphere occurred earlier in the air mass histories at higher latitudes. Fine vertical scale anticorrelations between CN and O3 or NOy were also often observed particularly in the last week of the program when NOy mixing ratios were more typical of the remote troposphere. These features are attributed to new particle formation near the tops of cloud convection episodes and they

  5. Atmospheric particles acting as Ice Forming Nuclei in different size ranges

    NASA Astrophysics Data System (ADS)

    Santachiara, G.; Di Matteo, L.; Prodi, F.; Belosi, F.

    2010-05-01

    The work presents the results of an experimental campaign performed at a rural site (S. Pietro Capofiume, near Bologna July 2007) concerning measurements of ice nuclei in different size classes of aerosol: PM1, PM2.5, PM10 and total suspended particles (TSP). Simultaneous measurements of particle number concentrations were also performed. Aerosol in the PM1 fraction contributes about 50% of the measured ice nuclei number concentration, and in the PM10 fraction contributes about 70-90%. Consequently, the dominant fraction of aerosol that can be activated as ice nuclei involves particles with aerodynamic diameter less than 10 μm. A positive correlation is observed between higher supersaturation with respect to ice and water ( Sice and Sw, respectively) values, and ice nuclei number concentration. The variations of Sw from 2 to 10% and Sice from 20 to 32% ( Tair = - 15 °C) determine an approximately threefold increase (from 110 to 337 m - 3 ) in the ice nuclei average number concentration. There is no correlation between ice nuclei measured in the different size ranges, either with the particle number concentration measured with the counter spectrometer ( d > 0.3 μm) or with the condensation nuclei counter.

  6. Incorporation of advanced aerosol activation treatments into CESM/CAM5: model evaluation and impacts on aerosol indirect effects

    NASA Astrophysics Data System (ADS)

    Gantt, B.; He, J.; Zhang, X.; Zhang, Y.; Nenes, A.

    2014-07-01

    One of the greatest sources of uncertainty in the science of anthropogenic climate change is from aerosol-cloud interactions. The activation of aerosols into cloud droplets is a direct microphysical linkage between aerosols and clouds; parameterizations of this process link aerosol with cloud condensation nuclei (CCN) and the resulting indirect effects. Small differences between parameterizations can have a large impact on the spatiotemporal distributions of activated aerosols and the resulting cloud properties. In this work, we incorporate a series of aerosol activation schemes into the Community Atmosphere Model version 5.1.1 within the Community Earth System Model version 1.0.5 (CESM/CAM5) which include factors such as insoluble aerosol adsorption and giant cloud condensation nuclei (CCN) activation kinetics to understand their individual impacts on global-scale cloud droplet number concentration (CDNC). Compared to the existing activation scheme in CESM/CAM5, this series of activation schemes increase the computation time by ~10% but leads to predicted CDNC in better agreement with satellite-derived/in situ values in many regions with high CDNC but in worse agreement for some regions with low CDNC. Large percentage changes in predicted CDNC occur over desert and oceanic regions, owing to the enhanced activation of dust from insoluble aerosol adsorption and reduced activation of sea spray aerosol after accounting for giant CCN activation kinetics. Comparison of CESM/CAM5 predictions against satellite-derived cloud optical thickness and liquid water path shows that the updated activation schemes generally improve the low biases. Globally, the incorporation of all updated schemes leads to an average increase in column CDNC of 150% and an increase (more negative) in shortwave cloud forcing of 12%. With the improvement of model-predicted CDNCs and better agreement with most satellite-derived cloud properties in many regions, the inclusion of these aerosol activation

  7. Aerosol measurements at the south pole during 1987. Data report

    SciTech Connect

    Bodhaine, B.A.; Harris, J.M.

    1992-11-01

    The Climate Monitoring and Diagnostics Laboratory (CMDL) of the National Oceanic and Atmospheric Administration (NOAA) operates an atmospheric monitoring observatory at Amundsen-Scott Station, South Pole. The aerosol measurement program consists of the continuous measurement of condensation nuclei (CN) concentration and aerosol scattering extinction coefficient. During 1987, a special aerosol experiment was conducted that included filter samples for subsequent analysis by the proton induced x-ray emission technique, diffusion battery measurements for size information in the sub-0.1 micrometer size range, and aerosol absorption measurements using an aethalometer. Surface and upper air meteorological data were also available. The purpose of the report is to present all of the aerosol data obtained during 1987.

  8. How Important Is Organic Aerosol Hygroscopicity to Aerosol Indirect Forcing?

    SciTech Connect

    Liu, Xiaohong; Wang, Jian

    2010-12-07

    Organics are among the most abundant aerosol components in the atmosphere. However, there are still large uncertainties with emissions of primary organic aerosol (POA) and volatile organic compounds (VOCs) (precursor gases of secondary organic aerosol, SOA), formation and yield of SOA, and chemical and physical properties (e.g., hygroscopicity) of POA and SOA. All these may have significant impacts on aerosol direct and indirect forcing estimated from global models. In this study a modal aerosol module (MAM) in the NCAR Community Atmospheric Model (CAM) is used to examine sensitivities of aerosol indirect forcing to hygroscopicity (“κ” value) of POA and SOA. Our model simulation indicates that in the present-day condition changing “κ” value of POA from 0 to 0.1 increases the number concentration of cloud condensational nuclei (CCN) at supersaturation S=0.1% by 40-60% over the POA source regions, while changing “κ” value of SOA by ±50% (from 0.14 to 0.07 and 0.21) changes the CCN within 30%. Changes in the in-cloud droplet number concentrations (CDNC) are within 20% in most locations on the globe with the above changes in “κ” value of POA and SOA. Global annual mean anthropogenic aerosol indirect forcing (AIF) between present-day (PD) and pre-industrial (PI) conditions change by 0.4 W m-2 with the control run of -1.3 W m-2. AIF reduces with the increase hygroscopicity of organic aerosol, indicating the important role of natural organic aerosol in buffering the relative change of CDNC from PI to PD.

  9. Development, evaluation and comparison of two independent sampling and analytical methods for ortho-phthalaldehyde vapors and condensation aerosols in air† ‡

    PubMed Central

    2015-01-01

    Two independent sampling and analytical methods for ortho-phthalaldehyde (OPA) in air have been developed, evaluated and compared (1) a reagent-coated solid sorbent HPLC-UV method and (2) an impinger-fluorescence method. In the first method, air sampling is conducted at 1.0 L min−1 with a sampler containing 350 mg of silica gel coated with 1 mg of acidified 2,4-dinitrophenylhydrazine (DNPH). After sampling, excess DNPH in ethyl acetate is added to the sampler prior to storage for 68 hours. The OPA-DNPH derivative is eluted with 4.0 mL of dimethyl sulfoxide (DMSO) for measurement by HPLC with a UV detector set at 3S5 nm. The estimated detection limit is 0.016 µg per sample or 0.067 µg m−3 (0.012 ppb) for a 240 L air sample. Recoveries of vapor spikes at levels of 1.2 to 6.2 µg were 96 to 101%. Recoveries of spikes as mixtures of vapor and condensation aerosols were 97 to 100%. In the second method, air sampling is conducted at 1.0 L mm−1 with a midget impinger containing 10 mL of DMSO solution containing N-acetyl-l-cysteine and ethylenediamine. The fluorescence reading is taken 80 min after the completion of air sampling. Since the time of taking the fluorescence reading is critical, the reading is taken with a portable fluorometer. The estimated detection limit is 0.024 µg per sample or 0.1 µg m−3 (0.018 ppb) for a 240 L air sample. Recoveries of OPA vapor spikes at levels of 1.4 to 5.0 µg per sample were 97 to 105%. Recoveries of spikes as mixtures of vapors and condensation aerosols were 95 to 99%. The collection efficiency for a mixture of vapor and condensation aerosol was 99.4%. The two methods were compared side-by-side in a generation system constructed for producing controlled atmospheres of OPA vapor in air. Average air concentrations of OPA vapor found by both methods agreed within ±10%. PMID:26346658

  10. 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.

  11. Impact of the modal aerosol scheme GLOMAP-mode on aerosol forcing in the Hadley Centre Global Environmental Model

    NASA Astrophysics Data System (ADS)

    Bellouin, N.; Mann, G. W.; Woodhouse, M. T.; Johnson, C.; Carslaw, K. S.; Dalvi, M.

    2013-03-01

    The Hadley Centre Global Environmental Model (HadGEM) includes two aerosol schemes: the Coupled Large-scale Aerosol Simulator for Studies in Climate (CLASSIC), and the new Global Model of Aerosol Processes (GLOMAP-mode). GLOMAP-mode is a modal aerosol microphysics scheme that simulates not only aerosol mass but also aerosol number, represents internally-mixed particles, and includes aerosol microphysical processes such as nucleation. In this study, both schemes provide hindcast simulations of natural and anthropogenic aerosol species for the period 2000-2006. HadGEM simulations of the aerosol optical depth using GLOMAP-mode compare better than CLASSIC against a data-assimilated aerosol re-analysis and aerosol ground-based observations. Because of differences in wet deposition rates, GLOMAP-mode sulphate aerosol residence time is two days longer than CLASSIC sulphate aerosols, whereas black carbon residence time is much shorter. As a result, CLASSIC underestimates aerosol optical depths in continental regions of the Northern Hemisphere and likely overestimates absorption in remote regions. Aerosol direct and first indirect radiative forcings are computed from simulations of aerosols with emissions for the year 1850 and 2000. In 1850, GLOMAP-mode predicts lower aerosol optical depths and higher cloud droplet number concentrations than CLASSIC. Consequently, simulated clouds are much less susceptible to natural and anthropogenic aerosol changes when the microphysical scheme is used. In particular, the response of cloud condensation nuclei to an increase in dimethyl sulphide emissions becomes a factor of four smaller. The combined effect of different 1850 baselines, residence times, and abilities to affect cloud droplet number, leads to substantial differences in the aerosol forcings simulated by the two schemes. GLOMAP-mode finds a present-day direct aerosol forcing of -0.49 W m-2 on a global average, 72% stronger than the corresponding forcing from CLASSIC. This

  12. Natural and anthropogenic aerosols in the Eastern Mediterranean and Middle East: possible impacts.

    PubMed

    Kallos, G; Solomos, S; Kushta, J; Mitsakou, C; Spyrou, C; Bartsotas, N; Kalogeri, C

    2014-08-01

    The physical and chemical properties of airborne particles have significant implications on the microphysical cloud processes. Maritime clouds have different properties than polluted ones and the final amounts and types of precipitation are different. Mixed phase aerosols that contain soluble matter are efficient cloud condensation nuclei (CCN) and enhance the liquid condensate spectrum in warm and mixed phase clouds. Insoluble particles such as mineral dust and black carbon are also important because of their ability to act as efficient ice nuclei (IN) through heterogeneous ice nucleation mechanisms. The relative contribution of aerosol concentrations, size distributions and chemical compositions on cloud structure and precipitation is discussed in the framework of RAMS/ICLAMS model. Analysis of model results and comparison with measurements reveals the complexity of the above links. Taking into account anthropogenic emissions and all available aerosol-cloud interactions the model precipitation bias was reduced by 50% for a storm simulation over eastern Mediterranean.

  13. Aerosol formation and distribution in the Arctic during AGASP-II, March-April 1986

    NASA Technical Reports Server (NTRS)

    Schnell, Russell C.; Kahl, Jonathan D.; Herbert, Gary A.; Bodhaine, B. A.; Bridgman, Howard A.

    1988-01-01

    The Arctic Gas and Aerosol Sampling Program has undertaken the determination of the distribution, transport, chemistry, aerosol physics, and radiative effects of the 'Arctic haze' air-pollution phenomenon. Attention has been given the April 2-3, 1986 haze zone, with large condensation nuclei, SO2, and soot-carbon concentrations, which appeared near the Barrow Baseline Station. The composite trajectory of the haze zone has been determined, as has its probable source region. After travelling 10,000 km, the haze still had SO2, aerosol black carbon, and condensation nuclei concentrations in excess of those measured off the East Coast of the U.S. in January of the same year.

  14. Effects of cloud condensation nuclei and ice nucleating particles on precipitation processes and supercooled liquid in mixed-phase orographic clouds

    DOE PAGES

    Fan, Jiwen; Leung, L. Ruby; Rosenfeld, Daniel; ...

    2017-01-23

    How orographic mixed-phase clouds respond to the change in cloud condensation nuclei (CCN) and ice nucleating particles (INPs) are highly uncertain. The main snow production mechanism in warm and cold mixed-phase orographic clouds (referred to as WMOCs and CMOCs, respectively, distinguished here as those having cloud tops warmer and colder than −20 °C) could be very different. We quantify the CCN and INP impacts on supercooled water content, cloud phases, and precipitation for a WMOC case and a CMOC case, with sensitivity tests using the same CCN and INP concentrations between the WMOC and CMOC cases. It was found that depositionmore » plays a more important role than riming for forming snow in the CMOC case, while the role of riming is dominant in the WMOC case. As expected, adding CCN suppresses precipitation, especially in WMOCs and low INPs. However, this reverses strongly for CCN of 1000 cm−3 and larger. We found a new mechanism through which CCN can invigorate mixed-phase clouds over the Sierra Nevada and drastically intensify snow precipitation when CCN concentrations are high (1000 cm−3 or higher). In this situation, more widespread shallow clouds with a greater amount of cloud water form in the Central Valley and foothills west of the mountain range. The increased latent heat release associated with the formation of these clouds strengthens the local transport of moisture to the windward slope, invigorating mixed-phase clouds over the mountains, and thereby producing higher amounts of snow precipitation. Under all CCN conditions, increasing the INPs leads to decreased riming and mixed-phase fraction in the CMOC as a result of liquid-limited conditions, but has the opposite effects in the WMOC as a result of ice-limited conditions. However, precipitation in both cases is increased by increasing INPs due to an increase in deposition for the CMOC but enhanced riming and deposition in the WMOC. Increasing the INPs dramatically reduces

  15. Effects of cloud condensation nuclei and ice nucleating particles on precipitation processes and supercooled liquid in mixed-phase orographic clouds

    SciTech Connect

    Fan, Jiwen; Leung, L. Ruby; Rosenfeld, Daniel; DeMott, Paul J.

    2017-01-01

    How orographic mixed-phase clouds respond to the change in cloud condensation nuclei (CCN) and ice nucleating particles (INPs) are highly uncertain. The main snow production mechanism in warm and cold mixed-phase orographic clouds (referred to as WMOCs and CMOCs, respectively, distinguished here as those having cloud tops warmer and colder than -20°C) could be very different. We quantify the CCN and INP impacts on supercooled water content, cloud phases, and precipitation for a WMOC case and a CMOC case, with sensitivity tests using the same CCN and INP concentrations between the WMOC and CMOC cases. It was found that deposition plays a more important role than riming for forming snow in the CMOC case, while the role of riming is dominant in the WMOC case. As expected, adding CCN suppresses precipitation, especially in WMOCs and low INPs. However, this reverses strongly for CCN of 1000 cm-3 and larger. We found a new mechanism through which CCN can invigorate mixed-phase clouds over the Sierra Nevada and drastically intensify snow precipitation when CCN concentrations are high (1000 cm-3 or higher). In this situation, more widespread shallow clouds with a greater amount of cloud water form in the Central Valley and foothills west of the mountain range. The increased latent heat release associated with the formation of these clouds strengthens the local transport of moisture to the windward slope, invigorating mixed-phase clouds over the mountains, and thereby producing higher amounts of snow precipitation. Under all CCN conditions, increasing the INPs leads to decreased riming and mixed-phase fraction in the CMOC as a result of liquid-limited conditions, but has the opposite effects in the WMOC as a result of ice-limited conditions. However, precipitation in both cases is increased by increasing INPs due to an increase in deposition for the CMOC but enhanced riming and deposition in the WMOC. Increasing the INPs dramatically reduces

  16. A comparative study of cloud condensation nuclei measured between non-heating and heating periods at a suburb site of Qingdao in the North China

    NASA Astrophysics Data System (ADS)

    Li, Kai; Zhu, Yujiao; Gao, Huiwang; Yao, Xiaohong

    2015-07-01

    In this paper, we studied concentrations of cloud condensation nuclei (CCN) and CCN activity measured at a suburb site of Qingdao in the North China during a non-heating period from 19 May to 3 June 2013 and a heating period from 6 November to 6 December 2013. Concentrations of CCN during the non-heating period were 3.1 ± 1.9 (mean ± standard deviation), 4.9 ± 3.4, 5.6 ± 3.9, 6.1 ± 4.3 and 6.5 ± 4.6 in unit of ×103 cm-3 at supersaturation (SS) of 0.2%, 0.4%, 0.6%, 0.8% and 1.0%, respectively. The corresponding CCN activities of atmospheric particles were 0.28 ± 0.17, 0.43 ± 0.24, 0.48 ± 0.26, 0.52 ± 0.27 and 0.54 ± 0.28, respectively. Concentrations of CCN during the heating period were 3.1 ± 1.3, 6.4 ± 2.3, 8.5 ± 2.9, 9.6 ± 3.5 and 10 ± 3.9 in unit of ×103 cm-3 at SS of 0.2%, 0.4%, 0.6%, 0.8% and 1.0%, respectively. The corresponding CCN activities were 0.11 ± 0.06, 0.24 ± 0.11, 0.31 ± 0.14, 0.35 ± 0.15 and 0.37 ± 0.15, respectively. At SS ≥ 0.4%, concentrations of CCN were significantly larger during the heating period than during the non-heating period with 95% confidence because of larger particle number concentrations associated. However, CCN activities were significantly lower during the heating period than during the non-heating period at each SS. The lower CCN activities during the heating period were analyzed in terms of origins, median mobility diameter and possible chemical composition of atmospheric particles. However, when new particle formation events during the heating and the non-heating periods were considered alone, CCN activities of grown new particles at the same size range sometimes appeared to be constant regardless of the heating or non-heating periods.

  17. Cloud condensation nuclei (CCN) activity and oxygen-to-carbon elemental ratios following thermodenuder treatment of organic particles grown by α-pinene ozonolysis.

    PubMed

    Kuwata, Mikinori; Chen, Qi; Martin, Scot T

    2011-08-28

    The effects of thermodenuder treatment on the cloud condensation nuclei (CCN) activity and elemental composition of organic particles grown by α-pinene ozonolysis were investigated. The secondary organic material (SOM) was produced in a continuous-flow chamber, with steady-state organic particle mass concentrations M(org) ranging from 1.4 to 37 μg m(-3). Particles exiting in the outflow were heated to temperatures T of up to 100 °C in a thermodenuder. The oxygen-to-carbon (O:C) and hydrogen-to-carbon (H:C) ratios were measured by on-line mass spectrometry. The observed elemental ratios were fit by a linear function, given by (H:C) = -0.8 (O:C) +1.8 for 0.38 < O:C < 0.50. This fit included the dependence on both M(org) and T, meaning that the single variable of post-thermodenuder M(org) was sufficient as an accurate predictor for O:C(M(org)(T)) and H:C(M(org)(T)). This result suggests that equilibrium partitioning theory largely governed the initial volatilization in the thermodenuder. By comparison, the CCN activity had a different dependence on thermodenuder treatment. At 25 °C, the CCN activity was independent of M(org), having an effective hygroscopicity parameter κ(org) of 0.103 ± 0.002. At 100 °C, however, κ(org) varied from 0.105 for M(org) = 1.4 μg m(-3) to 0.079 for M(org) = 37 μg m(-3), indicating that for high mass concentration the CCN activity decreased with heat treatment. The interpretation is that the oligomer fraction of the SOM increased at elevated T, both because of particle-phase reactions that produced oligomers under those conditions and because of the relative enrichment of lower-volatility oligomers in the SOM accompanying the evaporation of higher-volatility monomers from the SOM. Oligomers have high effective molecular weights and thereby significantly influence CCN activity. The production rates of different types of oligomers depend on the types and concentrations of functional groups present in the SOM, which in turn are

  18. Effects of cloud condensation nuclei and ice nucleating particles on precipitation processes and supercooled liquid in mixed-phase orographic clouds

    NASA Astrophysics Data System (ADS)

    Fan, Jiwen; Leung, L. Ruby; Rosenfeld, Daniel; DeMott, Paul J.

    2017-01-01

    How orographic mixed-phase clouds respond to the change in cloud condensation nuclei (CCN) and ice nucleating particles (INPs) are highly uncertain. The main snow production mechanism in warm and cold mixed-phase orographic clouds (referred to as WMOCs and CMOCs, respectively, distinguished here as those having cloud tops warmer and colder than -20 °C) could be very different. We quantify the CCN and INP impacts on supercooled water content, cloud phases, and precipitation for a WMOC case and a CMOC case, with sensitivity tests using the same CCN and INP concentrations between the WMOC and CMOC cases. It was found that deposition plays a more important role than riming for forming snow in the CMOC case, while the role of riming is dominant in the WMOC case. As expected, adding CCN suppresses precipitation, especially in WMOCs and low INPs. However, this reverses strongly for CCN of 1000 cm-3 and larger. We found a new mechanism through which CCN can invigorate mixed-phase clouds over the Sierra Nevada and drastically intensify snow precipitation when CCN concentrations are high (1000 cm-3 or higher). In this situation, more widespread shallow clouds with a greater amount of cloud water form in the Central Valley and foothills west of the mountain range. The increased latent heat release associated with the formation of these clouds strengthens the local transport of moisture to the windward slope, invigorating mixed-phase clouds over the mountains, and thereby producing higher amounts of snow precipitation. Under all CCN conditions, increasing the INPs leads to decreased riming and mixed-phase fraction in the CMOC as a result of liquid-limited conditions, but has the opposite effects in the WMOC as a result of ice-limited conditions. However, precipitation in both cases is increased by increasing INPs due to an increase in deposition for the CMOC but enhanced riming and deposition in the WMOC. Increasing the INPs dramatically reduces supercooled water content and

  19. Biogenic Potassium Salt Particles as Seeds for Secondary Organic Aerosol in the Amazon

    NASA Astrophysics Data System (ADS)

    Pöhlker, Christopher; Wiedemann, Kenia T.; Sinha, Bärbel; Shiraiwa, Manabu; Gunthe, Sachin S.; Smith, Mackenzie; Su, Hang; Artaxo, Paulo; Chen, Qi; Cheng, Yafang; Elbert, Wolfgang; Gilles, Mary K.; Kilcoyne, Arthur L. D.; Moffet, Ryan C.; Weigand, Markus; Martin, Scot T.; Pöschl, Ulrich; Andreae, Meinrat O.

    2012-08-01

    The fine particles serving as cloud condensation nuclei in pristine Amazonian rainforest air consist mostly of secondary organic aerosol. Their origin is enigmatic, however, because new particle formation in the atmosphere is not observed. Here, we show that the growth of organic aerosol particles can be initiated by potassium-salt-rich particles emitted by biota in the rainforest. These particles act as seeds for the condensation of low- or semi-volatile organic compounds from the atmospheric gas phase or multiphase oxidation of isoprene and terpenes. Our findings suggest that the primary emission of biogenic salt particles directly influences the number concentration of cloud condensation nuclei and affects the microphysics of cloud formation and precipitation over the rainforest.

  20. Estimating Black Carbon Aging Time-Scales with a Particle-Resolved Aerosol Model

    SciTech Connect

    Riemer, Nicole; West, Matt; Zaveri, Rahul A.; Easter, Richard C.

    2010-01-13

    Understanding the aging process of aerosol particles is important for assessing their chemical reactivity, cloud condensation nuclei activity, radiative properties and health impacts. In this study we investigate the aging of black carbon containing particles in an idealized urban plume using a new approach, the particleresolved aerosol model PartMC-MOSAIC. We present a method to estimate aging time-scales using an aging criterion based on cloud condensation nuclei activation. The results show a separation into a daytime regime where condensation dominates and a nighttime regime where coagulation dominates. For the chosen urban plume scenario, depending on the supersaturation threshold, the values for the aging timescales vary between 0.06 hours and 10 hours during the day, and between 6 hours and 20 hours during the night.

  1. Final Technical Report for "Ice nuclei relation to aerosol properties: Data analysis and model parameterization for IN in mixed-phase clouds" (DOE/SC00002354)

    SciTech Connect

    Anthony Prenni; Kreidenweis, Sonia M.

    2012-09-28

    Clouds play an important role in weather and climate. In addition to their key role in the hydrologic cycle, clouds scatter incoming solar radiation and trap infrared radiation from the surface and lower atmosphere. Despite their importance, feedbacks involving clouds remain as one of the largest sources of uncertainty in climate models. To better simulate cloud processes requires better characterization of cloud microphysical processes, which can affect the spatial extent, optical depth and lifetime of clouds. To this end, we developed a new parameterization to be used in numerical models that describes the variation of ice nuclei (IN) number concentrations active to form ice crystals in mixed-phase (water droplets and ice crystals co-existing) cloud conditions as these depend on existing aerosol properties and temperature. The parameterization is based on data collected using the Colorado State University continuous flow diffusion chamber in aircraft and ground-based campaigns over a 14-year period, including data from the DOE-supported Mixed-Phase Arctic Cloud Experiment. The resulting relationship is shown to more accurately represent the variability of ice nuclei distributions in the atmosphere compared to currently used parameterizations based on temperature alone. When implemented in one global climate model, the new parameterization predicted more realistic annually averaged cloud water and ice distributions, and cloud radiative properties, especially for sensitive higher latitude mixed-phase cloud regions. As a test of the new global IN scheme, it was compared to independent data collected during the 2008 DOE-sponsored Indirect and Semi-Direct Aerosol Campaign (ISDAC). Good agreement with this new data set suggests the broad applicability of the new scheme for describing general (non-chemically specific) aerosol influences on IN number concentrations feeding mixed-phase Arctic stratus clouds. Finally, the parameterization was implemented into a regional

  2. Aerosol particles and the formation of advection fog

    NASA Technical Reports Server (NTRS)

    Hung, R. J.; Liaw, G. S.; Vaughan, O. H., Jr.

    1979-01-01

    A study of numerical simulation of the effects of concentration, particle size, mass of nuclei, and chemical composition on the dynamics of warm fog formation, particularly the formation of advection fog, is presented. This formation is associated with the aerosol particle characteristics, and both macrophysical and microphysical processes are considered. In the macrophysical model, the evolution of wind components, water vapor content, liquid water content, and potential temperature under the influences of vertical turbulent diffusion, turbulent momentum, and turbulent energy transfers are taken into account. In the microphysical model, the supersaturation effect is incorporated with the surface tension and hygroscopic material solution. It is shown that the aerosol particles with the higher number density, larger size nuclei, the heavier nuclei mass, and the higher ratio of the Van't Hoff factor to the molecular weight favor the formation of the lower visibility advection fogs with stronger vertical energy transfer during the nucleation and condensation time period.

  3. Impact of the modal aerosol scheme GLOMAP-mode on aerosol forcing in the Hadley Centre Global Environmental Model

    NASA Astrophysics Data System (ADS)

    Bellouin, N.; Mann, G. W.; Woodhouse, M. T.; Johnson, C.; Carslaw, K. S.; Dalvi, M.

    2012-08-01

    The Hadley Centre Global Environmental Model (HadGEM) includes two aerosol schemes: the Coupled Large-scale Aerosol Simulator for Studies in Climate (CLASSIC), and the new Global Model of Aerosol Processes (GLOMAP-mode). GLOMAP-mode is a modal aerosol microphysics scheme that simulates not only aerosol mass but also aerosol number, represents internally-mixed particles, and includes aerosol microphysical processes such as nucleation. In this study, both schemes provide hindcast simulations of natural and anthropogenic aerosol species for the period 2000-2006. HadGEM simulations using GLOMAP-mode compare better than CLASSIC against a data-assimilated aerosol re-analysis and aerosol ground-based observations. GLOMAP-mode sulphate aerosol residence time is two days longer than CLASSIC sulphate aerosols, whereas black carbon residence time is much shorter. As a result, CLASSIC underestimates aerosol optical depths in continental regions of the Northern Hemisphere and likely overestimates absorption in remote regions. Aerosol direct and first indirect radiative forcings are computed from simulations of aerosols with emissions for the year 1850 and 2000. In 1850, GLOMAP-mode predicts lower aerosol optical depths and higher cloud droplet number concentrations than CLASSIC. Consequently, simulated clouds are much less susceptible to natural and anthropogenic aerosol changes when the microphysical scheme is used. In particular, the response of cloud condensation nuclei to an increase in dimethyl sulphide emissions becomes a factor of four smaller. The combined effect of different 1850 baselines, residence times, and cloud susceptibilities, leads to substantial differences in the aerosol forcings simulated by the two schemes. GLOMAP-mode finds a present-day direct aerosol forcing of -0.49 W m-2 on a global average, 72% stronger than the corresponding forcing from CLASSIC. This difference is compensated by changes in first indirect aerosol forcing: the forcing of -1.17 W m-2

  4. The NASA-AMES Research Center Stratospheric Aerosol Model. 1. Physical Processes and Computational Analogs

    NASA Technical Reports Server (NTRS)

    Turco, R. P.; Hamill, P.; Toon, O. B.; Whitten, R. C.; Kiang, C. S.

    1979-01-01

    A time-dependent one-dimensional model of the stratospheric sulfate aerosol layer is presented. In constructing the model, a wide range of basic physical and chemical processes are incorporated in order to avoid predetermining or biasing the model predictions. The simulation, which extends from the surface to an altitude of 58 km, includes the troposphere as a source of gases and condensation nuclei and as a sink for aerosol droplets. The size distribution of aerosol particles is resolved into 25 categories with particle radii increasing geometrically from 0.01 to 2.56 microns such that particle volume doubles between categories.

  5. 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.

  6. Advection fog formation and aerosols produced by combustion-originated air pollution

    NASA Technical Reports Server (NTRS)

    Hung, R. J.; Liaw, G. S.; Vaughan, O. H., Jr.

    1980-01-01

    The way in which pollutants produced by the photochemical reaction of NO(X) and SO(X) affect the quality of the human environment through such phenomena as the formation of advection fog is considered. These pollutants provide the major source of condensation nuclei for the formation of fog in highways, airports and seaports. Results based on the monodisperse, multicomponent aerosol model show that: (1) condensation nuclei can grow and form a dense fog without the air having attained supersaturation; (2) the mass concentration range for NO(X) is one-third that of SO(X); and (3) the greater the mass concentration, the particle concentration, and the radius of condensation nuclei, the denser the fog that is formed.

  7. THIRD YEAR REPORT: Sea-Salt Aerosol in Hawaii and the Influence of Large Organized Structures (LOS) or Rolls on Fluxes and Visibility

    DTIC Science & Technology

    2009-09-30

    measurements under accelerating wind conditions in the “natural wind tunnels” between Hawaiian Islands. These experiments revealed the typical...chemistry to measured cloud condensation nuclei (CCN, T. Nenes ). Our HR-ToF-AMS is key to understanding the nature of that organic aerosol and related

  8. Climate effects of anthropogenic aerosols over East Asia based on modeling study

    NASA Astrophysics Data System (ADS)

    Mukai, Makiko

    The increasing emission of anthropogenic aerosols causes serious air pollution episodes and various effects on the climate by the aerosols interacting with the radiation budget by directly absorbing and scattering the solar radiation, and by them indirectly modifying the optical properties and lifetimes of clouds. In East Asia anthropogenic aerosol concentrations are rapidly increasing. It is therefore necessary to evaluate the sensitivity of anthropogenic aerosols upon the radiative forcing in this region. For this purpose we utilize an atmospheric general circulation model (AGCM) with an aerosol transport and radiation model and an ocean mixed-layer model. The model in this study was a three-dimensional aerosol transport-radiation model (SPRINTARS), driven by the AGCM developed by CCSR (Center for Climate System Research), NIES (National Institute for Environmental Studies), and FRCGC (Frontier Research Center for Global Change). This model incorporates sulfate, carbonaceous, sea salt, and mineral dust aerosols, the first three of which are assumed to acts as cloud condensation nuclei that generate cloud droplets whose number increases with the number of nuclei. We assumed sulfate and carbonaceous aerosol from fuel burning for anthropogenic aerosol. And the model simulations of equilibrium experiments were performed to investigate the impact of anthropogenic aerosols based on present-day emission data and the preindustrial-era emission data. Our simulation results showed that copious anthropogenic aerosol loading causes significant decrease in the surface downward shortwave radiation flux (SDSWRF), which indicates that a direct effect of aerosols has the greatest influence on the surface radiation. It is found from our model simulations that low-level clouds increase but convective clouds decrease due to reduced convective activity caused by surface cooling when anthropogenic aerosol increases. It was also found that the contributions of aerosols to the radiation

  9. Implementing marine organic aerosols into the GEOS-Chem model

    NASA Astrophysics Data System (ADS)

    Gantt, B.; Johnson, M. S.; Crippa, M.; Prévôt, A. S. H.; Meskhidze, N.

    2014-09-01

    Marine organic aerosols (MOA) have been shown to play an important role in tropospheric chemistry by impacting surface mass, cloud condensation nuclei, and ice nuclei concentrations over remote marine and coastal regions. In this work, an online marine primary organic aerosol emission parameterization, designed to be used for both global and regional models, was implemented into the GEOS-Chem model. The implemented emission scheme improved the large underprediction of organic aerosol concentrations in clean marine regions (normalized mean bias decreases from -79% when using the default settings to -12% when marine organic aerosols are added). Model predictions were also in good agreement (correlation coefficient of 0.62 and normalized mean bias of -36%) with hourly surface concentrations of MOA observed during the summertime at an inland site near Paris, France. Our study shows that MOA have weaker coastal-to-inland concentration gradients than sea-salt aerosols, leading to several inland European cities having > 10% of their surface submicron organic aerosol mass concentration with a marine source. The addition of MOA tracers to GEOS-Chem enabled us to identify the regions with large contributions of freshly-emitted or aged aerosol having distinct physicochemical properties, potentially indicating optimal locations for future field studies.

  10. Implementing marine organic aerosols into the GEOS-Chem model

    NASA Astrophysics Data System (ADS)

    Gantt, B.; Johnson, M. S.; Crippa, M.; Prévôt, A. S. H.; Meskhidze, N.

    2015-03-01

    Marine-sourced organic aerosols (MOAs) have been shown to play an important role in tropospheric chemistry by impacting surface mass, cloud condensation nuclei, and ice nuclei concentrations over remote marine and coastal regions. In this work, an online marine primary organic aerosol emission parameterization, designed to be used for both global and regional models, was implemented into the GEOS-Chem (Global Earth Observing System Chemistry) model. The implemented emission scheme improved the large underprediction of organic aerosol concentrations in clean marine regions (normalized mean bias decreases from -79% when using the default settings to -12% when marine organic aerosols are added). Model predictions were also in good agreement (correlation coefficient of 0.62 and normalized mean bias of -36%) with hourly surface concentrations of MOAs observed during the summertime at an inland site near Paris, France. Our study shows that MOAs have weaker coastal-to-inland concentration gradients than sea-salt aerosols, leading to several inland European cities having >10% of their surface submicron organic aerosol mass concentration with a marine source. The addition of MOA tracers to GEOS-Chem enabled us to identify the regions with large contributions of freshly emitted or aged aerosol having distinct physicochemical properties, potentially indicating optimal locations for future field studies.

  11. Implementing marine organic aerosols into the GEOS-Chem model

    DOE PAGES

    Gantt, B.; Johnson, M. S.; Crippa, M.; ...

    2015-03-17

    Marine-sourced organic aerosols (MOAs) have been shown to play an important role in tropospheric chemistry by impacting surface mass, cloud condensation nuclei, and ice nuclei concentrations over remote marine and coastal regions. In this work, an online marine primary organic aerosol emission parameterization, designed to be used for both global and regional models, was implemented into the GEOS-Chem (Global Earth Observing System Chemistry) model. The implemented emission scheme improved the large underprediction of organic aerosol concentrations in clean marine regions (normalized mean bias decreases from -79% when using the default settings to -12% when marine organic aerosols are added). Modelmore » predictions were also in good agreement (correlation coefficient of 0.62 and normalized mean bias of -36%) with hourly surface concentrations of MOAs observed during the summertime at an inland site near Paris, France. Our study shows that MOAs have weaker coastal-to-inland concentration gradients than sea-salt aerosols, leading to several inland European cities having >10% of their surface submicron organic aerosol mass concentration with a marine source. The addition of MOA tracers to GEOS-Chem enabled us to identify the regions with large contributions of freshly emitted or aged aerosol having distinct physicochemical properties, potentially indicating optimal locations for future field studies.« less

  12. Implementing Marine Organic Aerosols Into the GEOS-Chem Model

    NASA Technical Reports Server (NTRS)

    Johnson, Matthew S.

    2015-01-01

    Marine-sourced organic aerosols (MOA) have been shown to play an important role in tropospheric chemistry by impacting surface mass, cloud condensation nuclei, and ice nuclei concentrations over remote marine and coastal regions. In this work, an online marine primary organic aerosol emission parameterization, designed to be used for both global and regional models, was implemented into the GEOS-Chem model. The implemented emission scheme improved the large under-prediction of organic aerosol concentrations in clean marine regions (normalized mean bias decreases from -79% when using the default settings to -12% when marine organic aerosols are added). Model predictions were also in good agreement (correlation coefficient of 0.62 and normalized mean bias of -36%) with hourly surface concentrations of MOA observed during the summertime at an inland site near Paris, France. Our study shows that MOA have weaker coastal-to-inland concentration gradients than sea-salt aerosols, leading to several inland European cities having > 10% of their surface submicron organic aerosol mass concentration with a marine source. The addition of MOA tracers to GEOS-Chem enabled us to identify the regions with large contributions of freshly-emitted or aged aerosol having distinct physicochemical properties, potentially indicating optimal locations for future field studies.

  13. CCN activity of aliphatic amine secondary aerosol

    NASA Astrophysics Data System (ADS)

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

    2014-01-01

    Aliphatic amines can form secondary aerosol via oxidation with atmospheric radicals (e.g. hydroxyl radical and nitrate radical). The particle composition can contain both secondary organic aerosol (SOA) and inorganic salts. The fraction 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. TMA + N2O5 form semi-volatile organics in low RH conditions that have κ ~ 0.20, indicative of slightly soluble organic material. As RH increases, several 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. Higher CCN activity (κ > 0.3) was also observed for humid BA+N2O5 aerosols compared with dry aerosol (κ ~ 0.2), as a result of the formation of inorganic salts such as NH4NO3 and butylamine nitrate (C4H11N · HNO3). Compared with TMA, BA+N2O5 reactions produce more volatile aerosols. The BA+N2O5 aerosol products under humid experiments were found to be very sensitive to the temperature within the stream-wise continuous flow thermal gradient CCN counter. The CCN counter, when set above a 21 °C temperature difference, evaporates BA+N2O5 aerosol formed at RH ≥ 30%; κ ranges from 0.4 to 0.7 and is dependent on the instrument supersaturation (ss) settings. The aerosol behaves non-ideally, hence simple ZSR rules cannot be applied to the CCN results from the primary aliphatic amine system. Overall, aliphatic amine aerosol systems κ ranges from 0.2 < κ < 0.7. This work indicates that

  14. 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.

  15. Aerosol activation properties and CCN closure during TCAP

    NASA Astrophysics Data System (ADS)

    Mei, F.; Tomlinson, J. M.; Shilling, J. E.; Wilson, J. M.; Zelenyuk, A.; Chand, D.; Comstock, J. M.; Hubbe, J.; Berg, L. K.; Schmid, B.

    2013-12-01

    The indirect effects of atmospheric aerosols currently remain the most uncertain components in forcing of climate change over the industrial period (IPCC, 2007). This large uncertainty is partially due to our incomplete understanding of the ability of particles to form cloud droplets under atmospherically relevant supersaturation. In addition, there is a large uncertainty in the aerosol optical depth (AOD) simulated by climate models near the North American coast and a wide variety in the types of clouds are observed over this region. The goal of the US Department of Energy Two Column Aerosol Project (TCAP) is to understand the processes responsible for producing and maintaining aerosol distributions and associated radiative and cloud forcing off the coast of North America. During the TCAP study, aerosol total number concentration, cloud condensation nuclei (CCN) spectra and aerosol chemical composition were in-situ measured from the DOE Gulfstream 1 (G-1) research aircraft during two Intensive Operations Periods (IOPs), one conducted in July 2012 and the other in February 2013. An overall aerosol size distribution was achieved by merging the observations from several instruments, including Ultra High Sensitivity Aerosol Spectrometer - Airborne (UHSAS-A, DMT), Passive Cavity Aerosol Spectrometer Probe (PCASP-200, DMT), and Cloud Aerosol Spectrometer (CAS, DMT). Aerosol chemical composition was characterized using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS, Aerodyne Inc.) and single particle mass spectrometer, mini-SPLAT. Based on the aerosol size distribution, CCN number concentration (characterized by a DMT dual column CCN counter with a range from 0.1% to 0.4%), and chemical composition, a CCN closure was obtained. The sensitivity of CCN closure to organic hygroscopicity was investigated. The differences in aerosol/CCN properties between two columns, and between two phases, will be discussed.

  16. 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.

  17. 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.

  18. Optical properties and CCN activity of aerosols in a high-altitude Himalayan environment: Results from RAWEX-GVAX

    NASA Astrophysics Data System (ADS)

    Gogoi, Mukunda M.; Babu, S. Suresh; Jayachandran, V.; Moorthy, K. Krishna; Satheesh, S. K.; Naja, Manish; Kotamarthi, V. R.

    2015-03-01

    The seasonality and mutual dependence of aerosol optical properties and cloud condensation nuclei (CCN) activity under varying meteorological conditions at the high-altitude Nainital site (~2 km) in the Indo-Gangetic Plains were examined using nearly year-round measurements (June 2011 to March 2012) at the Atmospheric Radiation Measurement mobile facility as part of the Regional Aerosol Warming Experiment-Ganges Valley Aerosol Experiment of the Indian Space Research Organization and the U.S. Department of Energy. The results from collocated measurements provided enhanced aerosol scattering and absorption coefficients, CCN concentrations, and total condensation nuclei concentrations during the dry autumn and winter months. The CCN concentration (at a supersaturation of 0.46) was higher during the periods of high aerosol absorption (single scattering albedo (SSA) < 0.80) than during the periods of high aerosol scattering (SSA > 0.85), indicating that the aerosol composition seasonally changes and influences the CCN activity. The monthly mean CCN activation ratio (at a supersaturation of 0.46) was highest (>0.7) in late autumn (November); this finding is attributed to the contribution of biomass-burning aerosols to CCN formation at high supersaturation conditions.

  19. Impact of Mixing State on Anthropogenic Aerosol Radiative Forcing and Associated Climate Response

    NASA Astrophysics Data System (ADS)

    Avramov, A.; Shin, H. J.; Wang, C.

    2014-12-01

    Atmospheric aerosols affect Earth's radiation balance directly by scattering and absorbing solar radiation and, indirectly, by changing the microphysical structure, lifetime and spatial extent of clouds. The aerosol mixing state to a large extent determines not only their optical properties (direct effect) but also their ability to serve as cloud condensation nuclei or ice nuclei (indirect effect). Results from previous research have highlighted the importance of the aerosol mixing assumptions in radiative forcing estimates in model simulations. Here we take a step further to analyze the differences in associated climate responses, using a multimodal, size- and mixing-dependent aerosol model (MARC) incorporated within the Community Earth System Model (CESM). The new model allows for a detailed representation of aerosol-radiation and aerosol-cloud interactions by including an improved treatment of aerosol mixing state and composition. First, we estimate and compare the magnitudes of direct and indirect forcing of anthropogenic aerosols under different mixing assumptions. We then carry out several century-long fully-coupled climate simulations designed to isolate the climate responses to direct and indirect forcings under the same aerosol mixing assumptions. In our analysis, we specifically focus on the following three climate response components: 1) cloud distribution and coverage; 2) precipitation amount and distribution; and 3) changes in circulation patterns.

  20. 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.

  1. An OpenFOAM®-based tool for computational modeling of aerosol nucleation and transport

    NASA Astrophysics Data System (ADS)

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

    2013-05-01

    In the process of single-species homogeneous vapor condensation into aerosol, surface is created between liquid and vapor. The energy of formation of such surface limits the condensation of vapor from a supersaturated state. Nucleation, the mechanism of generation of embryo sites, or nuclei, on which vapor is able to condense, is an important process. Developing an understanding of this process is important, as it may lead to a considerable contribution to many engineering problems, as well as atmospheric and environmental science. In this work, we present an OpenFOAM®-based numerical simulation tool, which is capable of predicting aerosol formation using a two-moment representation of the aerosol and classical nucleation theory. We aim at developing a flexible utility, which enables researchers interested in various aerosol production-related applications to quickly study concepts like aerosol nucleation, condensation, diffusion and transport. We compare our numerical approach with the results of physical experiments, each using a laminar flow diffusion chamber (Ref. [1, 2, 3]) with different species and/or carrier gasses. A good agreement between experimental and numerical results for the aerosol droplet number density is shown.

  2. Potential impact of dust aerosols on the pre-Helene (2006) mesoscale convective vortex

    NASA Astrophysics Data System (ADS)

    Zhang, H.; Sokolik, I. N.; Curry, J. A.

    2011-12-01

    The potential impact of dust aerosols on the early development of Hurricane Helene (2006) was examined using the Weather Research and Forecasting (WRF) and WRF-Chem model. The goal of this study is to examine the extent to which dust aerosols can influence the intensity, track, and structure of a developing TC through the microphysical and radiation processes. Remote sensing observations from Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO), CloudSat, Moderate Resolution Imaging Spectroradiometer (MODIS), and Tropical Rainfall Measuring Mission (TRMM) were utilized to examine the distributions and characteristics of dust particles, hydrometeors, cloud top temperature, latent heat release and precipitation, as well as to constrain and evaluate the model simulations. The WRF simulations were conducted by implementing an ice nucleation parameterization accounting for the deliquescent heterogeneous freezing (DHF) mode. The DHF mode refers to the freezing process for internally mixed aerosols with soluble and insoluble species that can serve as both cloud condensation nuclei (CCN) and ice nuclei (IN), such as dust. Simulations showed the tendency of DHF mode to promote ice formation at lower altitudes in strong updraft cores, increase the local latent heat release, and produce more low clouds and less high clouds. Further more, a series of WRF-Chem simulations were conducted, which includes aerosol emission scheme, a radiative transfer scheme accounting for aerosol optical properties, and a dual moment microphysics scheme that will account for environmental aerosols as nuclei. Differences between the results from WRF and WRF-Chem simulations were examined.

  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. Unexpectedly high ultrafine aerosol concentrations above East Antarctic sea ice

    NASA Astrophysics Data System (ADS)

    Humphries, R. S.; Klekociuk, A. R.; Schofield, R.; Keywood, M.; Ward, J.; Wilson, S. R.

    2016-02-01

    Better characterisation of aerosol processes in pristine, natural environments, such as Antarctica, have recently been shown to lead to the largest reduction in uncertainties in our understanding of radiative forcing. Our understanding of aerosols in the Antarctic region is currently based on measurements that are often limited to boundary layer air masses at spatially sparse coastal and continental research stations, with only a handful of studies in the vast sea-ice region. In this paper, the first observational study of sub-micron aerosols in the East Antarctic sea ice region is presented. Measurements were conducted aboard the icebreaker Aurora Australis in spring 2012 and found that boundary layer condensation nuclei (CN3) concentrations exhibited a five-fold increase moving across the polar front, with mean polar cell concentrations of 1130 cm-3 - higher than any observed elsewhere in the Antarctic and Southern Ocean region. The absence of evidence for aerosol growth suggested that nucleation was unlikely to be local. Air parcel trajectories indicated significant influence from the free troposphere above the Antarctic continent, implicating this as the likely nucleation region for surface aerosol, a similar conclusion to previous Antarctic aerosol studies. The highest aerosol concentrations were found to correlate with low-pressure systems, suggesting that the passage of cyclones provided an accelerated pathway, delivering air masses quickly from the free troposphere to the surface. After descent from the Antarctic free troposphere, trajectories suggest that sea-ice boundary layer air masses travelled equatorward into the low-albedo Southern Ocean region, transporting with them emissions and these aerosol nuclei which, after growth, may potentially impact on the region's radiative balance. The high aerosol concentrations and their transport pathways described here, could help reduce the discrepancy currently present between simulations and observations of

  5. Linker DNA destabilizes condensed chromatin.

    PubMed

    Green, G R; Ferlita, R R; Walkenhorst, W F; Poccia, D L

    2001-01-01

    The contribution of the linker region to maintenance of condensed chromatin was examined in two model systems, namely sea urchin sperm nuclei and chicken red blood cell nuclei. Linkerless nuclei, prepared by extensive digestion with micrococcal nuclease, were compared with Native nuclei using several assays, including microscopic appearance, nuclear turbidity, salt stability, and trypsin resistance. Chromatin in the Linkerless nuclei was highly condensed, resembling pyknotic chromatin in apoptotic cells. Linkerless nuclei were more stable in low ionic strength buffers and more resistant to trypsin than Native nuclei. Analysis of histones from the trypsinized nuclei by polyacrylamide gel electrophoresis showed that specific histone H1, H2B, and H3 tail regions stabilized linker DNA in condensed nuclei. Thermal denaturation of soluble chromatin preparations from differentially trypsinized sperm nuclei demonstrated that the N-terminal regions of histones Sp H1, Sp H2B, and H3 bind tightly to linker DNA, causing it to denature at a high temperature. We conclude that linker DNA exerts a disruptive force on condensed chromatin structure which is counteracted by binding of specific histone tail regions to the linker DNA. The inherent instability of the linker region may be significant in all eukaryotic chromatins and may promote gene activation in living cells.

  6. 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.

  7. Physical and chemical characterization of marine atmospheric aerosols over the North and South Pacific Oceans using single particle mass spectrometry

    NASA Astrophysics Data System (ADS)

    Furutani, H.; Jung, J.; Miura, K.; Uematsu, M.

    2010-12-01

    Physical and chemical properties of marine atmospheric aerosols were characterized and compared over the North and South Pacific Ocean during two trans-Pacific cruises (from Japan to Chile and Australia to Japan) during the period of January-June 2009, which cover broad region of Pacific Ocean from 40°N to 55°S and 140°E to 70°W. The measured parameters of aerosol properties were single particle size-resolved chemical composition (D = 100 ~ 1500 nm), cloud condensation nuclei (CCN) and condensation nuclei (CN) concentrations, size distribution from 10 nm to 5 μm, total aerosol nitrate and sulfate concentrations, and filter-based chemical composition. Trace gas concentrations of O3 and CO were also measured to aid air parcel categorization during the cruises. Reflecting larger anthropogenic emission in the Northern Hemisphere, pronounced concentration gradient between the North and South Pacific Ocean was observed for aerosol nitrate, CO, and O3. Aerosol sulfate also showed a similar concentration drop in the equatorial region, relatively higher sulfate concentration was observed in 30°S-40°S and 55°S regions, which was associated with increased aerosol methanesulfonic acid (MSA) concentration but little increase in local marine chlorophyll concentration, suggesting contribution of long-range transported marine biogenic sulfur from the high primary production area over the South Pacific high latitude region. Aerosol chemical classification by single particle chemical analysis revealed that certain aerosol types, such as biomass burning, elemental carbon, and elemental/organic carbon mixed type, were mainly observed in the North Pacific region, while several specific organic aerosol types with abundant aged organic and disulfur composition were identified in the South Pacific region. Further comparison of aerosol properties, aerosol sources, and atmospheric aerosol processing in the North and South Pacific Oceans will be discussed.

  8. A Simple Model of Global Aerosol Indirect Effects

    NASA Technical Reports Server (NTRS)

    Ghan, Steven J.; Smith, Steven J.; Wang, Minghuai; Zhang, Kai; Pringle, Kirsty; Carslaw, Kenneth; Pierce, Jeffrey; Bauer, Susanne; Adams, Peter

    2013-01-01

    Most estimates of the global mean indirect effect of anthropogenic aerosol on the Earth's energy balance are from simulations by global models of the aerosol lifecycle coupled with global models of clouds and the hydrologic cycle. Extremely simple models have been developed for integrated assessment models, but lack the flexibility to distinguish between primary and secondary sources of aerosol. Here a simple but more physically based model expresses the aerosol indirect effect (AIE) using analytic representations of cloud and aerosol distributions and processes. Although the simple model is able to produce estimates of AIEs that are comparable to those from some global aerosol models using the same global mean aerosol properties, the estimates by the simple model are sensitive to preindustrial cloud condensation nuclei concentration, preindustrial accumulation mode radius, width of the accumulation mode, size of primary particles, cloud thickness, primary and secondary anthropogenic emissions, the fraction of the secondary anthropogenic emissions that accumulates on the coarse mode, the fraction of the secondary mass that forms new particles, and the sensitivity of liquid water path to droplet number concentration. Estimates of present-day AIEs as low as 5 W/sq m and as high as 0.3 W/sq m are obtained for plausible sets of parameter values. Estimates are surprisingly linear in emissions. The estimates depend on parameter values in ways that are consistent with results from detailed global aerosol-climate simulation models, which adds to understanding of the dependence on AIE uncertainty on uncertainty in parameter values.

  9. Amazon boundary layer aerosol concentration sustained by vertical transport during rainfall.

    PubMed

    Wang, Jian; Krejci, Radovan; Giangrande, Scott; Kuang, Chongai; Barbosa, Henrique M J; Brito, Joel; Carbone, Samara; Chi, Xuguang; Comstock, Jennifer; Ditas, Florian; Lavric, Jost; Manninen, Hanna E; Mei, Fan; Moran-Zuloaga, Daniel; Pöhlker, Christopher; Pöhlker, Mira L; Saturno, Jorge; Schmid, Beat; Souza, Rodrigo A F; Springston, Stephen R; Tomlinson, Jason M; Toto, Tami; Walter, David; Wimmer, Daniela; Smith, James N; Kulmala, Markku; Machado, Luiz A T; Artaxo, Paulo; Andreae, Meinrat O; Petäjä, Tuukka; Martin, Scot T

    2016-11-17

    The nucleation of atmospheric vapours is an important source of new aerosol particles that can subsequently grow to form cloud condensation nuclei in the atmosphere. Most field studies of atmospheric aerosols over continents are influenced by atmospheric vapours of anthropogenic origin (for example, ref. 2) and, in consequence, aerosol processes in pristine, terrestrial environments remain poorly understood. The Amazon rainforest is one of the few continental regions where aerosol particles and their precursors can be studied under near-natural conditions, but the origin of small aerosol particles that grow into cloud condensation nuclei in the Amazon boundary layer remains unclear. Here we present aircraft- and ground-based measurements under clean conditions during the wet season in the central Amazon basin. We find that high concentrations of small aerosol particles (with diameters of less than 50 nanometres) in the lower free troposphere are transported from the free troposphere into the boundary layer during precipitation events by strong convective downdrafts and weaker downward motions in the trailing stratiform region. This rapid vertical transport can help to maintain the population of particles in the pristine Amazon boundary layer, and may therefore influence cloud properties and climate under natural conditions.

  10. Amazon boundary layer aerosol concentration sustained by vertical transport during rainfall

    NASA Astrophysics Data System (ADS)

    Wang, Jian; Krejci, Radovan; Giangrande, Scott; Kuang, Chongai; Barbosa, Henrique M. J.; Brito, Joel; Carbone, Samara; Chi, Xuguang; Comstock, Jennifer; Ditas, Florian; Lavric, Jost; Manninen, Hanna E.; Mei, Fan; Moran-Zuloaga, Daniel; Pöhlker, Christopher; Pöhlker, Mira L.; Saturno, Jorge; Schmid, Beat; Souza, Rodrigo A. F.; Springston, Stephen R.; Tomlinson, Jason M.; Toto, Tami; Walter, David; Wimmer, Daniela; Smith, James N.; Kulmala, Markku; Machado, Luiz A. T.; Artaxo, Paulo; Andreae, Meinrat O.; Petäjä, Tuukka; Martin, Scot T.

    2016-11-01

    The nucleation of atmospheric vapours is an important source of new aerosol particles that can subsequently grow to form cloud condensation nuclei in the atmosphere. Most field studies of atmospheric aerosols over continents are influenced by atmospheric vapours of anthropogenic origin (for example, ref. 2) and, in consequence, aerosol processes in pristine, terrestrial environments remain poorly understood. The Amazon rainforest is one of the few continental regions where aerosol particles and their precursors can be studied under near-natural conditions, but the origin of small aerosol particles that grow into cloud condensation nuclei in the Amazon boundary layer remains unclear. Here we present aircraft- and ground-based measurements under clean conditions during the wet season in the central Amazon basin. We find that high concentrations of small aerosol particles (with diameters of less than 50 nanometres) in the lower free troposphere are transported from the free troposphere into the boundary layer during precipitation events by strong convective downdrafts and weaker downward motions in the trailing stratiform region. This rapid vertical transport can help to maintain the population of particles in the pristine Amazon boundary layer, and may therefore influence cloud properties and climate under natural conditions.

  11. Amazon boundary layer aerosol concentration sustained by vertical transport during rainfall

    SciTech Connect

    Wang, Jian; Krejci, Radovan; Giangrande, Scott; Kuang, Chongai; Barbosa, Henrique M. J.; Brito, Joel; Carbone, Samara; Chi, Xuguang; Comstock, Jennifer; Ditas, Florian; Lavric, Jost; Manninen, Hanna E.; Mei, Fan; Moran-Zuloaga, Daniel; Pöhlker, Christopher; Pöhlker, Mira L.; Saturno, Jorge; Schmid, Beat; Souza, Rodrigo A. F.; Springston, Stephen R.; Tomlinson, Jason M.; Toto, Tami; Walter, David; Wimmer, Daniela; Smith, James N.; Kulmala, Markku; Machado, Luiz A. T.; Artaxo, Paulo; Andreae, Meinrat O.; Petäjä, Tuukka; Martin, Scot T.

    2016-10-24

    The nucleation of atmospheric vapours is an important source of new aerosol particles that can subsequently grow to form cloud condensation nuclei in the atmosphere. Most field studies of atmospheric aerosols over continents are influenced by atmospheric vapours of anthropogenic origin and, in consequence, aerosol processes in pristine, terrestrial environments remain poorly understood. The Amazon rainforest is one of the few continental regions where aerosol particles and their precursors can be studied under near-natural conditions, but the origin of small aerosol particles that grow into cloud condensation nuclei in the Amazon boundary layer remains unclear. Here we present aircraft- and ground-based measurements under clean conditions during the wet season in the central Amazon basin. We find that high concentrations of small aerosol particles (with diameters of less than 50 nanometres) in the lower free troposphere are transported from the free troposphere into the boundary layer during precipitation events by strong convective downdrafts and weaker downward motions in the trailing stratiform region. Lastly, this rapid vertical transport can help to maintain the population of particles in the pristine Amazon boundary layer, and may therefore influence cloud properties and climate under natural conditions.

  12. Amazon boundary layer aerosol concentration sustained by vertical transport during rainfall

    DOE PAGES

    Wang, Jian; Krejci, Radovan; Giangrande, Scott; ...

    2016-10-24

    The nucleation of atmospheric vapours is an important source of new aerosol particles that can subsequently grow to form cloud condensation nuclei in the atmosphere. Most field studies of atmospheric aerosols over continents are influenced by atmospheric vapours of anthropogenic origin and, in consequence, aerosol processes in pristine, terrestrial environments remain poorly understood. The Amazon rainforest is one of the few continental regions where aerosol particles and their precursors can be studied under near-natural conditions, but the origin of small aerosol particles that grow into cloud condensation nuclei in the Amazon boundary layer remains unclear. Here we present aircraft- andmore » ground-based measurements under clean conditions during the wet season in the central Amazon basin. We find that high concentrations of small aerosol particles (with diameters of less than 50 nanometres) in the lower free troposphere are transported from the free troposphere into the boundary layer during precipitation events by strong convective downdrafts and weaker downward motions in the trailing stratiform region. Lastly, this rapid vertical transport can help to maintain the population of particles in the pristine Amazon boundary layer, and may therefore influence cloud properties and climate under natural conditions.« less

  13. Comparison of Aerosol Classification Results from Airborne High Spectral Resolution Lidar (HSRL) Measurements and the Calipso Vertical Feature Mask

    NASA Technical Reports Server (NTRS)

    Burton, S. P.; Ferrare, R. A.; Hostetler, C. A.; Hair, J. W.; Rogers, R. R.; Obland, M. D.; Butler, C. F.; Cook, A. L.; Harper, D. B.; Froyd, K. D.; Omar, A.

    2012-01-01

    Knowledge of the vertical profile, composition, concentration, and size of aerosols is required for assessing the direct impact of aerosols on radiation, the indirect effects of aerosols on clouds and precipitation, and attributing these effects to natural and anthropogenic aerosols. Because anthropogenic aerosols are predominantly submicrometer, fine mode fraction (FMF) retrievals from satellite have been used as a tool for deriving anthropogenic aerosols. Although column and profile satellite retrievals of FMF have been performed over the ocean, such retrievals have not yet been been done over land. Consequently, uncertainty in satellite estimates of the anthropogenic component of the aerosol direct radiative forcing is greatest over land, due in large part to uncertainties in the FMF. Satellite measurements have been used to detect and evaluate aerosol impacts on clouds; however, such efforts have been hampered by the difficulty in retrieving vertically-resolved cloud condensation nuclei (CCN) concentration, which is the most direct parameter linking aerosol and clouds. Recent studies have shown correlations between average satellite derived column aerosol optical thickness (AOT) and in situ measured CCN. However, these same studies, as well as others that use detailed airborne in situ measurements have noted that vertical variability of the aerosol distribution, impacts of relative humidity, and the presence of coarse mode aerosols such as dust introduce large uncertainties in such relations.

  14. An Overview of Observations of Interstitial Aerosol during ICE-T

    NASA Astrophysics Data System (ADS)

    Dhaniyala, S.; Craig, L.; Moharreri, A.; Brown, M.; Lathem, T.; Nenes, A.; Rogers, D. C.

    2011-12-01

    Aerosols play a significant role in global climate through their direct and indirect interaction with longwave and shortwave radiation. Of particular importance is the indirect contribution of aerosols to the radiative forcing budget through the formation and evolution of cloud systems. Accurate global climate modeling requires an effective treatment of the indirect effect with simple aerosol-cloud parametric models. Validation of such models requires data from a wide range of cloud systems. Aerosol-cloud model validation efforts have relied mostly on the measurement of activated particles, largely because of a lack of data on the non-activated or interstitial particle populations. Knowledge of interstitial particles in cloud systems enables, not just an improved validation of existing aerosol-cloud models, but also a more complete understanding of the aerosol processing in clouds and the possible role of aerosol in ice nucleation. During the recent ICE-T campaign, comprehensive interstitial 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. Central to the sampling of interstitial aerosol was the deployment of a new aerosol sampler that provides shatter-free sampling of aerosol particles in ice clouds and significantly reduced shattering in warm clouds (relative to other aircraft aerosol inlets). This inlet samples aerosol particles smaller than ~2 microns. The condensation nuclei (CN) measurements were made with a TSI 3010 condensation particle counter (CPC), while particle size distributions were measured using DMT's ultra-high sensitivity aerosol spectrometer (UHSAS) instrument and a new fast mobility spectrometer. The fast mobility spectrometer consists of a new high-flow dual channel differential mobility

  15. Global measurements of gaseous and aerosol trace species in the upper troposphere and lower stratosphere from daily flights of 747 airliners

    NASA Technical Reports Server (NTRS)

    Perkins, P. J.

    1976-01-01

    Extensive measurements include ozone, carbon monoxide, water vapor, and aerosol and condensation nuclei number density. Less extensive measurements include chlorofluoromethanes, sulfates and nitrates. Certain meteorological and flight information are also recorded at the time of these measurements. World routes range in latitude from about 60 deg N near North America to about 40 deg S over Australia and 23 deg S over South America. Typical data show significant changes in ozone, carbon monoxide, and water vapor when crossing the tropopause either during changes in altitude or at cruise altitude. These gases as well as light scattering particles and condensation nuclei exhibit considerable variability along a flight route.

  16. Observations of Aerosol Conditions Associated with Precipitation Events in the Remote Sierra Nevada Foothills

    NASA Astrophysics Data System (ADS)

    Collins, D. B.; Kingsmill, D.; Roberts, G. C.; Noblitt, S.; Prather, K. A.

    2011-12-01

    Recent investigations of atmospheric aerosols have suggested their importance in affecting clouds and precipitation patterns, especially in regions where anthropogenic contributions to aerosol loadings are large. Aerosols entrained into precipitating clouds have been shown to either enhance or suppress precipitation based on the characteristics of the cloud condensation nuclei (CCN) or ice nuclei (IN) introduced. Due to the inherent chemical dependence of CCN activity, the chemical composition of aerosols introduced into precipitating clouds will determine their effect on precipitation. This presentation will utilize ground-based chemical and physical measurements of aerosols and precipitation from multiple winter seasons gathered at Sugar Pine Dam (Foresthill, CA) as part of the CalWater experiment. The coupled behavior of landfalling frontal systems, regional terrain-parallel flow along the windward slopes of the Sierra Nevada (i.e., the Sierra Barrier Jet), and observed aerosol conditions in the Sierra Nevada foothills will be demonstrated and related issues explored. Temporally correlated changes in aerosol chemical composition with approaching winter storms may provide key insights into the evolution of the Sierra Barrier Jet, a dynamic feature that can have a major influence on orographically-forced precipitation in this region, and could provide clues to the coupling of Central Valley pollution with winter-time orographic precipitation episodes (or lack thereof). Gaining an overall understanding of the frequency and magnitude of the entrainment of Central Valley pollutants on winter storm systems will ultimately provide an estimate of how much aerosols affect precipitation in California.

  17. Characterization of the Changes in Hygroscopicity of Ambient Organic Aerosol due to Oxidation by Gas Phase OH

    NASA Astrophysics Data System (ADS)

    Wong, J. P.; McWhinney, R. D.; Slowik, J. G.; Abbatt, J.

    2011-12-01

    Despite the ubiquitous nature of organic aerosols and their importance in climate forcing, the influence of chemical processes on their ability to act as cloud condensation nuclei (CCN) in the atmosphere remains uncertain. Changes to the hygroscopicity of ambient organic aerosol due to OH oxidation were explored at a remote forested (Whistler, British Columbia) and an urban (Toronto, Ontario) site. Organic aerosol was exposed to controlled levels of OH radicals in a portable flow tube reactor, the Toronto Photo-Oxidation Tube (TPOT). An Aerodyne Aerosol Mass Spectrometer (AMS) monitored the changes in the chemical composition due to OH-initiated oxidation. The CCN activity of size-selected particles was measured with a DMT Cloud Condensation Nuclei Counter (CCNc) to determine the hygroscopicity parameter, κ. Preliminary results suggest that gas phase OH oxidation increases the degree of oxygenation of organic aerosol, leading to increases in hygroscopicity. These results yield insights into the mechanism by which oxidation affects the hygroscopicity of ambient aerosol of various sources, and to constrain the main aging process that leads to the observation of increasing hygroscopicity with increasing oxidation of organic aerosol.

  18. The role of organic condensation on ultrafine particle growth during nucleation events

    NASA Astrophysics Data System (ADS)

    Patoulias, D.; Fountoukis, C.; Riipinen, I.; Pandis, S. N.

    2015-06-01

    A new aerosol dynamics model (DMANx) has been developed that simulates aerosol size/composition distribution and includes the condensation of organic vapors on nanoparticles through the implementation of the recently developed volatility basis set framework. Simulations were performed for Hyytiälä (Finland) and Finokalia (Greece), two locations with different organic sources where detailed measurements were available to constrain the new model. We investigate the effect of condensation of organics and chemical aging reactions of secondary organic aerosol (SOA) precursors on ultrafine particle growth and particle number concentration during a typical springtime nucleation event in both locations. This work highlights the importance of the pathways of oxidation of biogenic volatile organic compounds and the production of extremely low volatility organics. At Hyytiälä, organic condensation dominates the growth process of new particles. The low-volatility SOA contributes to particle growth during the early growth stage, but after a few hours most of the growth is due to semi-volatile SOA. At Finokalia, simulations show that organics have a complementary role in new particle growth, contributing 45% to the total mass of new particles. Condensation of organics increases the number concentration of particles that can act as CCN (cloud condensation nuclei) (N100) by 13% at Finokalia and 25% at Hyytiälä during a typical spring day with nucleation. The sensitivity of our results to the surface tension used is discussed.

  19. 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

  20. Fine Mode Aerosol over the United Arab Emirates

    NASA Astrophysics Data System (ADS)

    Ross, K. E.; Piketh, S. J.; Reid, J. S.; Reid, E. A.

    2005-12-01

    The aerosol loading of the atmosphere over the Arabian Gulf region is extremely diverse and is composed not only of dust, but also of pollution that is derived largely from oil-related activities. Fine mode pollution particles are most efficient at scattering incoming solar radiation and have the potential to act as cloud condensation nuclei (CCN), and may therefore have implications for climate change. The smaller aerosols may also pose a health hazard if present in high concentrations. The United Arab Emirates Unified Aerosol Experiment (UAE2) was designed to investigate aerosol and meteorological characteristics over the region using ground-based, aircraft and satellite measurements, and was conducted in August and September 2004. Aerosol chemical composition has been obtained from filters that were collected at the site of the Mobile Atmospheric Aerosol and Radiation Characterization Observatory (MAARCO) on the coast of the UAE between Abu Dhabi and Dubai. Filter samples were also collected on an airborne platform in order to assess how aerosol chemical composition varies across the region and throughout the depth of the boundary layer. Results of the analysis of the PM2.5 coastal samples show that ammonium sulphate is the most prevalent constituent of the fine mode aerosol in the region (>50% of the mass), followed by organic matter, alumino-silicates, calcium carbonate and black carbon. Source apportionment indicates that most of the fine aerosol mass is derived from fossil fuel combustion, while mineral dust and local vehicle emissions also contribute to the fine aerosol loading. The organic carbon-to-total carbon ratio of the aerosol is 0.65, which is typical of fossil fuel combustion. The dominance of sulphates means that the fine mode aerosol in the region is probably responsible for a negative radiative forcing, and that the polluting emissions significantly elevate the concentration of CCN.

  1. The effect of dry and wet deposition of condensable vapors on secondary organic aerosols concentrations over the continental US

    NASA Astrophysics Data System (ADS)

    Knote, C.; Hodzic, A.; Jimenez, J. L.

    2014-05-01

    The effect of dry and wet deposition of semi-volatile organic compounds (SVOC) in the gas-phase on the concentrations of secondary organic aerosol (SOA) is reassessed using recently derived water solubility information. The water solubility of SVOCs was implemented as a function of their volatility distribution within the regional chemistry transport model WRF-Chem, and simulations were carried out over the continental United States for the year 2010. Results show that including dry and wet removal of gas-phase SVOCs reduces annual average surface concentrations of anthropogenic and biogenic SOA by 48% and 63% respectively over the continental US Dry deposition of gas-phase SVOCs is found to be more effective than wet deposition in reducing SOA concentrations (-40% vs. -8% for anthropogenics, -52% vs. -11% for biogenics). Reductions for biogenic SOA are found to be higher due to the higher water solubility of biogenic SVOCs. The majority of the total mass of SVOC + SOA is actually deposited via the gas-phase (61% for anthropogenics, 76% for biogenics). A number of sensitivity studies shows that this is a robust feature of the modeling system. Other models that do not consider dry and wet removal of gas-phase SVOCs would hence overestimate SOA concentrations by roughly 50%. Assumptions about the water solubility of SVOCs made in some current modeling systems (H* = 105 M atm-1; H* = H* (HNO3)) still lead to an overestimation of 25% / 10% compared to our best estimate. A saturation effect is observed for Henry's law constants above 108 M atm-1, suggesting an upper bound of reductions in surface level SOA concentrations by 60% through removal of gas-phase SVOCs. Considering reactivity of gas-phase SVOCs in the dry deposition scheme was found to be negligible. Further sensitivity studies where we reduce the volatility of organic matter show that consideration of gas-phase SVOC removal still reduces average SOA concentrations by 31% on average. We consider this a lower

  2. The effect of dry and wet deposition of condensable vapors on secondary organic aerosols concentrations over the continental US

    NASA Astrophysics Data System (ADS)

    Knote, C.; Hodzic, A.; Jimenez, J. L.

    2015-01-01

    The effect of dry and wet deposition of semi-volatile organic compounds (SVOCs) in the gas phase on the concentrations of secondary organic aerosol (SOA) is reassessed using recently derived water solubility information. The water solubility of SVOCs was implemented as a function of their volatility distribution within the WRF-Chem regional chemistry transport model, and simulations were carried out over the continental United States for the year 2010. Results show that including dry and wet removal of gas-phase SVOCs reduces annual average surface concentrations of anthropogenic and biogenic SOA by 48 and 63% respectively over the continental US. Dry deposition of gas-phase SVOCs is found to be more effective than wet deposition in reducing SOA concentrations (-40 vs. -8% for anthropogenics, and -52 vs. -11% for biogenics). Reductions for biogenic SOA are found to be higher due to the higher water solubility of biogenic SVOCs. The majority of the total mass of SVOC + SOA is actually deposited via the gas phase (61% for anthropogenics and 76% for biogenics). Results are sensitive to assumptions made in the dry deposition scheme, but gas-phase deposition of SVOCs remains crucial even under conservative estimates. Considering reactivity of gas-phase SVOCs in the dry deposition scheme was found to be negligible. Further sensitivity studies where we reduce the volatility of organic matter show that consideration of gas-phase SVOC removal still reduces average SOA concentrations by 31% on average. We consider this a lower bound for the effect of gas-phase SVOC removal on SOA concentrations. A saturation effect is observed for Henry's law constants above 108 M atm-1, suggesting an upper bound of reductions in surface level SOA concentrations by 60% through removal of gas-phase SVOCs. Other models that do not consider dry and wet removal of gas-phase SVOCs would hence overestimate SOA concentrations by roughly 50%. Assumptions about the water solubility of SVOCs made in

  3. The effect of dry and wet deposition of condensable vapors on secondary organic aerosols concentrations over the continental US

    DOE PAGES

    Knote, C.; Hodzic, A.; Jimenez, J. L.

    2015-01-06

    The effect of dry and wet deposition of semi-volatile organic compounds (SVOCs) in the gas phase on the concentrations of secondary organic aerosol (SOA) is reassessed using recently derived water solubility information. The water solubility of SVOCs was implemented as a function of their volatility distribution within the WRF-Chem regional chemistry transport model, and simulations were carried out over the continental United States for the year 2010. Results show that including dry and wet removal of gas-phase SVOCs reduces annual average surface concentrations of anthropogenic and biogenic SOA by 48 and 63% respectively over the continental US. Dry deposition ofmore » gas-phase SVOCs is found to be more effective than wet deposition in reducing SOA concentrations (−40 vs. −8% for anthropogenics, and −52 vs. −11% for biogenics). Reductions for biogenic SOA are found to be higher due to the higher water solubility of biogenic SVOCs. The majority of the total mass of SVOC + SOA is actually deposited via the gas phase (61% for anthropogenics and 76% for biogenics). Results are sensitive to assumptions made in the dry deposition scheme, but gas-phase deposition of SVOCs remains crucial even under conservative estimates. Considering reactivity of gas-phase SVOCs in the dry deposition scheme was found to be negligible. Further sensitivity studies where we reduce the volatility of organic matter show that consideration of gas-phase SVOC removal still reduces average SOA concentrations by 31% on average. We consider this a lower bound for the effect of gas-phase SVOC removal on SOA concentrations. A saturation effect is observed for Henry's law constants above 108 M atm−1, suggesting an upper bound of reductions in surface level SOA concentrations by 60% through removal of gas-phase SVOCs. Other models that do not consider dry and wet removal of gas-phase SVOCs would hence overestimate SOA concentrations by roughly 50%. Assumptions about the water solubility

  4. 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

  5. In Situ Aerosol Properties Measured over the California Central Valley and the Sierra Nevada Mountain Range

    NASA Astrophysics Data System (ADS)

    Tomlinson, J. M.; Comstock, J. M.; Hubbe, J.; Kluzek, C.; Schmid, B.; Jonsson, H.; Woods, R.

    2011-12-01

    Anthropogenic aerosols are hypothesized to influence the formation of clouds and precipitation amounts within the Sierra Nevada Mountains. This could have a profound effect on the California water supply. To study this phenomena, an Ultra High Sensitivity Aerosol Spectrometer (UHSAS), Passive Cavity Aerosol Spectrometer (PCASP), and Cloud Aerosol Spectrometer (CAS) were operated aboard the Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Aerial Facility (AAF) Gulfstream-1 aircraft from February 2 to March 6, 2011 during the CalWater field campaign. The combined aerosol size distribution from the three instruments characterizes the size-resolved concentration of the submicron and supermicron aerosol over the California Central Valley and Sierra Nevada Mountain Range. The measured aerosol size distributions from CalWater are compared with the size distributions measured during the DOE Carbonaceous Aerosol and Radiative Effects Study (CARES) in June 2010 to determine the changes in the aerosol size distributions during different seasons, atmospheric river events, and long-range transport events from Asia. These changes are used to estimate the resulting aerosol effect on cloud condensation nuclei concentrations and the potential impact on cloud formation and precipitation.

  6. 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.

  7. Unexpectedly high ultrafine aerosol concentrations above East Antarctic sea-ice

    NASA Astrophysics Data System (ADS)

    Humphries, R. S.; Klekociuk, A. R.; Schofield, R.; Keywood, M.; Ward, J.; Wilson, S. R.

    2015-10-01

    The effect of aerosols on clouds and their radiative properties is one of the largest uncertainties in our understanding of radiative forcing. A recent study has concluded that better characterisation of pristine, natural aerosol processes leads to the largest reduction in these uncertainties. Antarctica, being far from anthropogenic activities, is an ideal location for the study of natural aerosol processes. Aerosol measurements in Antarctica are often limited to boundary layer air-masses at spatially sparse coastal and continental research stations, with only a handful of studies in the sea ice region. In this paper, the first observational study of sub-micron aerosols in the East Antarctic sea ice region is presented. Measurements were conducted aboard the ice-breaker Aurora Australis in spring 2012 and found that boundary layer condensation nuclei (CN3) concentrations exhibited a five-fold increase moving across the Polar Front, with mean Polar Cell concentrations of 1130 cm-3 - higher than any observed elsewhere in the Antarctic and Southern Ocean region. The absence of evidence for aerosol growth suggested that nucleation was unlikely to be local. Air parcel trajectories indicated significant influence from the free troposphere above the Antarctic continent, implicating this as the likely nucleation region for surface aerosol, a similar conclusion to previous Antarctic aerosol studies. The highest aerosol concentrations were found to correlate with low pressure systems, suggesting that the passage of cyclones provided an accelerated pathway, delivering air-masses quickly from the free-troposphere to the surface. After descent from the Antarctic free troposphere, trajectories suggest that sea ice boundary layer air-masses travelled equator-ward into the low albedo Southern Ocean region, transporting with them emissions and these aerosol nuclei where, after growth, may potentially impact on the region's radiative balance. The high aerosol concentrations and

  8. A Sensitivity Study of Aerosol Effects on an Idealized Supercell Storm

    NASA Astrophysics Data System (ADS)

    Takeishi, A.; Storelvmo, T.

    2013-12-01

    One of the largest uncertainties in future climate projections lies in the climatic effects of aerosols. It has been shown that the cooling effect of aerosols could partially offset the current global warming induced by increased greenhouse gas concentration. Among the effects of aerosols, the interaction between aerosols and deep convective clouds is especially difficult to quantify, due to the complex interaction and limited measurements available. Although the radiative effect of deep convective clouds on climate is small, they could affect the local, regional, and global climate by altering precipitation and the large-scale circulations. Thus, it is of importance to understand how deep convection changes its development and evolution with aerosol loading. This study aims to understand the effects of varying aerosol number concentrations on deep convective clouds, using the Weather Research and Forecasting (WRF) model. A quarter-circular shear supercell is simulated with three different microphysics schemes in an idealized setting, while mimicking the changes in aerosol concentration by changing either cloud droplet concentration or activated cloud condensation nuclei concentration. We find that the simulated amount of precipitation has quite different sensitivities to aerosol concentration, depending on the microphysics scheme used; one of the simulations shows a drastic decrease in precipitation with increased aerosol loading, whereas simulations with the other two schemes show relatively low sensitivities to aerosol concentration. This fact highlights uncertainties in the complex microphysical interactions in convective clouds. In addition, changes in ice nuclei concentration are mimicked by changing the ice nucleation rate in each scheme. Sensitivity to this variation is also dependent on the microphysics scheme used. Furthermore, radiation is added in the simulations so that both radiative and microphysical effects of aerosol on the supercell storm are

  9. Acid-catalyzed condensed-phase reactions of limonene and terpineol and their impacts on gas-to-particle partitioning in the formation of organic aerosols.

    PubMed

    Li, Yong Jie; Cheong, Gema Y L; Lau, Arthur P S; Chan, Chak K

    2010-07-15

    We investigated the condensed-phase reactions of biogenic VOCs with C double bond C bonds (limonene, C(10)H(16), and terpineol, C(10)H(18)O) catalyzed by sulfuric acid by both bulk solution (BS) experiments and gas-particle (GP) experiments using a flow cell reactor. Product analysis by gas chromatography-mass spectrometry (GC-MS) showed that cationic polymerization led to dimeric and trimeric product formation under conditions of relative humidity (RH) <20% (in the GP experiments) and a sulfuric acid concentration of 57.8 wt % (in the BS experiments), while hydration occurred under conditions of RH > 20% (in the GP experiments) and sulfuric acid concentrations of 46.3 wt % or lower (in the BS experiments). Apparent partitioning coefficients (K(p,rxn)) were estimated from the GP experiments by including the reaction products. Only under extremely low RH conditions (RH < 5%) did the values of K(p,rxn) ( approximately 5 x 10(-6) m(3)/microg for limonene and approximately 2 x 10(-5) m(3)/microg for terpineol) substantially exceed the physical partitioning coefficients (K(p) = 6.5 x 10(-8) m(3)/microg for limonene and =2.3 x 10(-6) m(3)/microg for terpineol) derived from the absorptive partitioning theory. At RH higher than 5%, the apparent partitioning coefficients (K(p,rxn)) of both limonene and terpineol were in the same order of magnitude as the K(p) values derived from the absorptive partitioning theory. Compared with other conditions including VOC concentration and degree of neutralization (by ammonium) of acidic particles, RH is a critical parameter that influences both the reaction mechanisms and the uptake ability (K(p,rxn) values) of these processes. The finding suggests that RH needs to be considered when taking the effects of acid-catalyzed reactions into account in estimating organic aerosol formation from C double bond C containing VOCs.

  10. 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

  11. 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

  12. Atmospheric science: marine aerosols and iodine emissions.

    PubMed

    McFiggans, Gordon

    2005-02-10

    O'Dowd et al. describe the formation of marine aerosols from biogenic iodine and the growth of these aerosols into cloud-condensation nuclei (CCN). Based on chamber and modelling results, the authors suggest that biogenic organic iodine compounds emitted from macroalgae may be responsible for coastal particle bursts and that production of these compounds in the open ocean could increase CCN there too. It has since been shown that coastal particles are more likely to be produced from the photooxidation of molecular iodine. Moreover, I contend that open-ocean particle production and cloud enhancement do not result from emissions of organic iodine at atmospheric levels. For iodine particles to affect cloud properties over the remote ocean, an additional source of iodine is necessary as organic precursors cannot be responsible.

  13. ModelE2-TOMAS development and evaluation using aerosol optical depths, mass and number concentrations

    NASA Astrophysics Data System (ADS)

    Lee, Y. H.; Adams, P. J.; Shindell, D. T.

    2014-09-01

    The TwO-Moment Aerosol Sectional microphysics model (TOMAS) has been integrated into the state-of-the-art general circulation model, GISS ModelE2. TOMAS has the flexibility to select a size resolution as well as the lower size cutoff. A computationally efficient version of TOMAS is used here, which has 15 size bins covering 3 nm to 10 μm aerosol dry diameter. For each bin, it simulates the total aerosol number concentration and mass concentrations of sulphate, pure elementary carbon (hydrophobic), mixed elemental carbon (hydrophilic), hydrophobic organic matter, hydrophilic organic matter, sea salt, mineral dust, ammonium, and aerosol-associated water. This paper provides a detailed description of the ModelE2-TOMAS model and evaluates the model against various observations including aerosol precursor gas concentrations, aerosol mass and number concentrations, and aerosol optical depths. Additionally, global budgets in ModelE2-TOMAS are compared with those of other global aerosol models, and the TOMAS model is compared to the default aerosol model in ModelE2, which is a bulk aerosol model. Overall, the ModelE2-TOMAS predictions are within the range of other global aerosol model predictions, and the model has a reasonable agreement with observations of sulphur species and other aerosol components as well as aerosol optical depth. However, ModelE2-TOMAS (as well as the bulk aerosol model) cannot capture the observed vertical distribution of sulphur dioxide over the Pacific Ocean possibly due to overly strong convective transport. The TOMAS model successfully captures observed aerosol number concentrations and cloud condensation nuclei concentrations. Anthropogenic aerosol burdens in the bulk aerosol model running in the same host model as TOMAS (ModelE2) differ by a few percent to a factor of 2 regionally, mainly due to differences in aerosol processes including deposition, cloud processing, and emission parameterizations. Larger differences are found for naturally

  14. Climate Change and Aerosol Feedbacks

    NASA Astrophysics Data System (ADS)

    Norman, Ann-Lise

    2008-05-01

    Climate instability is expected as mixing ratios of greenhouse gases in the Earth's atmosphere increase. The current trend in rising temperature can be related to anthropogenic greenhouse gas emissions. However, this trend may change as feedback mechanisms amplify; one of the least-understood aspects of climate change. Formation of cloud condensation nuclei from rising sulfate concentrations in the atmosphere may counteract the current warming trend. A key point is where the sulfate, and cloud condensation nuclei are formed. Is cloud formation widespread or localized near sulfate emission sources? A major source of atmospheric sulfate is dimethylsulfide, a compound related to biotic turnover in the surface ocean that constitutes a widespread natural source of aerosols over the remote ocean. A second major source contributing a significant proportion of atmospheric sulfate in the northern hemisphere is produced over continents from industrial activities and fossil fuel combustion. Distinguishing the source of sulfate in well-mixed air is important so that relationships with cloud formation, sea-ice in polar regions, and albedo can be explored. This distinction in sulfate sources can be achieved using isotope apportionment techniques. Recent measurements show an increase in biogenic sulfate coincident with rising temperatures in the Arctic and large amounts sulfur from DMS oxidation over the Atlantic, potentially indicating a widespread biotic feedback to warming over northern oceans.

  15. Development of the RAQM2 aerosol chemical transport model and predictions of the Northeast Asian aerosol mass, size, chemistry, and mixing type

    NASA Astrophysics Data System (ADS)

    Kajino, M.; Inomata, Y.; Sato, K.; Ueda, H.; Han, Z.; An, J.; Katata, G.; Deushi, M.; Maki, T.; Oshima, N.; Kurokawa, J.; Ohara, T.; Takami, A.; Hatakeyama, S.

    2012-12-01

    A new aerosol chemical transport model, the Regional Air Quality Model 2 (RAQM2), was developed to simulate the Asian air quality. We implemented a simple version of a triple-moment modal aerosol dynamics model (MADMS) and achieved a completely dynamic (non-equilibrium) solution of a gas-to-particle mass transfer over a wide range of aerosol diameters from 1 nm to super-μm. To consider a variety of atmospheric aerosol properties, a category approach was utilized in which the aerosols were distributed into four categories: particles in the Aitken mode (ATK), soot-free particles in the accumulation mode (ACM), soot aggregates (AGR), and particles in the coarse mode (COR). The aerosol size distribution in each category is characterized by a single mode. The condensation, evaporation, and Brownian coagulations for each mode were solved dynamically. A regional-scale simulation (Δx = 60 km) was performed for the entire year of 2006 covering the Northeast Asian region. The modeled PM1/bulk ratios of the chemical components were consistent with observations, indicating that the simulated aerosol mixing types were consistent with those in nature. The non-sea-salt SO42- mixed with ATK + ACM was the largest at Hedo in summer, whereas the SOSO42- was substantially mixed with AGR in the cold seasons. Ninety-eight percent of the modeled NO3- was mixed with sea salt at Hedo, whereas 53.7% of the NO3- was mixed with sea salt at Gosan, which is located upwind toward the Asian continent. The condensation of HNO3 onto sea salt particles during transport over the ocean accounts for the difference in the NO3- mixing type at the two sites. Because the aerosol mixing type alters the optical properties and cloud condensation nuclei activity, its accurate prediction and evaluation are indispensable for aerosol-cloud-radiation interaction studies.

  16. Characteristics of regional aerosols: Southern Arizona and eastern Pacific Ocean

    NASA Astrophysics Data System (ADS)

    Prabhakar, Gouri

    concentration of giant cloud condensation nuclei (Dp > 2 microm) in ship plumes relative to the unperturbed background regions over the ocean.

  17. Impact of Asia Dust Aerosols on Regional Environment and Climate

    NASA Astrophysics Data System (ADS)

    Huang, J.

    2015-12-01

    East Asia is a major dust source in the world and has great impacts on regional climate in Asia, where the large arid and semi-arid regions are. In this study, the typical transport paths of East Asia dust, which affect regional and global climates, are demonstrated and numerous effects of dust aerosols on clouds and precipitation primarily over East Asian arid and semi-arid regions are discussed. Compared with the dust aerosols of Saharan, those of East Asian are more absorptive of solar radiation, and can influence the cloud properties not only by acting as cloud condensation nuclei and ice nuclei but also through changing the relative humidity and stability of the atmosphere (via semi-direct effect). Converting visible light to thermal energy, dust aerosols can burn clouds to produce a warming effect on climate, which is opposite to the first and second indirect effects of aerosols. Over Asia arid and semi-arid regions, the positive feedback in the aerosol-cloud-precipitation interaction may aggravate drought in its inner land. Impact of Asia dust on regional environment, especially on haze weather, are also presented in this talk.

  18. 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.

  19. The Two-Column Aerosol Project (TCAP) Science Plan

    SciTech Connect

    Berkowitz, CM; Berg, LK; Cziczo, DJ; Flynn, CJ; Kassianov, EI; Fast, JD; Rasch, PJ; Shilling, JE; Zaveri, RA; Zelenyuk, A; Ferrare, RA; Hostetler, CA; Cairns, B; Russell, PB; Ervens, B

    2011-07-27

    The Two-Column Aerosol Project (TCAP) field campaign will provide a detailed set of observations with which to (1) perform radiative and cloud condensation nuclei (CCN) closure studies, (2) evaluate a new retrieval algorithm for aerosol optical depth (AOD) in the presence of clouds using passive remote sensing, (3) extend a previously developed technique to investigate aerosol indirect effects, and (4) evaluate the performance of a detailed regional-scale model and a more parameterized global-scale model in simulating particle activation and AOD associated with the aging of anthropogenic aerosols. To meet these science objectives, the Atmospheric Radiation Measurement (ARM) Climate Research Facility will deploy the ARM Mobile Facility (AMF) and the Mobile Aerosol Observing System (MAOS) on Cape Cod, Massachusetts, for a 12-month period starting in the summer of 2012 in order to quantify aerosol properties, radiation, and cloud characteristics at a location subject to both clear and cloudy conditions, and clean and polluted conditions. These observations will be supplemented by two aircraft intensive observation periods (IOPs), one in the summer and a second in the winter. Each IOP will deploy one, and possibly two, aircraft depending on available resources. The first aircraft will be equipped with a suite of in situ instrumentation to provide measurements of aerosol optical properties, particle composition and direct-beam irradiance. The second aircraft will fly directly over the first and use a multi-wavelength high spectral resolution lidar (HSRL) and scanning polarimeter to provide continuous optical and cloud properties in the column below.

  20. 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.

  1. The Atmospheric Radiation Measurement Program May 2003 Intensive Operations Period Examining Aerosol Properties and Radiative Influences: Preface to Special Section

    NASA Technical Reports Server (NTRS)

    Ferrare, Richard; Feingold, Graham; Ghan, Steven; Ogren, John; Schmid, Beat; Schwartz, Stephen E.; Sheridan, Pat

    2006-01-01

    Atmospheric aerosols influence climate by scattering and absorbing radiation in clear air (direct effects) and by serving as cloud condensation nuclei, modifying the microphysical properties of clouds, influencing radiation and precipitation development (indirect effects). Much of present uncertainty in forcing of climate change is due to uncertainty in the relations between aerosol microphysical and optical properties and their radiative influences (direct effects) and between microphysical properties and their ability to serve as cloud condensation nuclei at given supersaturations (indirect effects). This paper introduces a special section that reports on a field campaign conducted at the Department of Energy Atmospheric Radiation Measurement site in North Central Oklahoma in May, 2003, examining these relations using in situ airborne measurements and surface-, airborne-, and space-based remote sensing.

  2. 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.

  3. Modeling aerosols and their interactions with shallow cumuli during the 2007 CHAPS field study

    SciTech Connect

    Shrivastava, ManishKumar B.; Berg, Larry K.; Fast, Jerome D.; Easter, Richard C.; Laskin, Alexander; Chapman, Elaine G.; Gustafson, William I.; Liu, Ying; Berkowitz, Carl M.

    2013-02-07

    The Weather Research and Forecasting model coupled with chemistry (WRF-Chem) is used to simulate relationships between aerosols and clouds in the vicinity of Oklahoma City during the June 2007 Cumulus Humilis Aerosol Processing Study (CHAPS). The regional scale simulation completed using 2 km horizontal grid spacing evaluates four important relationships between aerosols and shallow cumulus clouds observed during CHAPS. First, the model reproduces the trends of higher nitrate volume fractions in cloud droplet residuals compared to interstitial non-activated aerosols, as measured using the Aerosol Mass Spectrometer. Comparing simulations with cloud chemistry turned on and off, we show that nitric acid vapor uptake by cloud droplets explains the higher nitrate content of cloud droplet residuals. Second, as documented using an offline code, both aerosol water and other inorganics (OIN), which are related to dust and crustal emissions, significantly affect predicted aerosol optical properties. Reducing the OIN content of wet aerosols by 50% significantly improves agreement of model predictions with measurements of aerosol optical properties. Third, the simulated hygroscopicity of aerosols is too high as compared to their hygroscopicity derived from cloud condensation nuclei and particle size distribution measurements, indicating uncertainties associated with simulating size-dependent chemical composition and treatment of aerosol mixing state within the model. Fourth, the model reasonably represents the observations of the first aerosol indirect effect where pollutants in the vicinity of Oklahoma City increase cloud droplet number concentrations and decrease the droplet effective radius. While previous studies have often focused on cloud-aerosol interactions in stratiform and deep convective clouds, this study highlights the ability of regional-scale models to represent some of the important aspects of cloud-aerosol interactions associated with fields of short

  4. 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.

  5. 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.

  6. Simultaneous Retrieval of Multiple Aerosol Parameters Using a Multi-Angular Approach

    NASA Technical Reports Server (NTRS)

    Kuo, K. S.; Weger, R. C.; Welch, R. M.

    1997-01-01

    Atmospheric aerosol particles, both natural and anthropogenic, are important to the earth's radiative balance through their direct and indirect effects. They scatter the incoming solar radiation (direct effect) and modify the shortwave reflective properties of clouds by acting as cloud condensation nuclei (indirect effect). Although it has been suggested that aerosols exert a net cooling influence on climate, this effect has received less attention than the radiative forcing due to clouds and greenhouse gases. In order to understand the role that aerosols play in a changing climate, detailed and accurate observations are a prerequisite. The retrieval of aerosol optical properties by satellite remote sensing has proven to be a difficult task. The difficulty results mainly from the tenuous nature and variable composition of aerosols. To date, with single-angle satellite observations, we can only retrieve reliably against dark backgrounds, such as over oceans and dense vegetation. Even then, assumptions must be made concerning the chemical composition of aerosols. The best hope we have for aerosol retrievals over bright backgrounds are observations from multiple angles, such as those provided by the MISR and POLDER instruments. In this investigation we examine the feasibility of simultaneous retrieval of multiple aerosol optical parameters using reflectances from a typical set of twelve angles observed by the French POLDER instrument. The retrieved aerosol optical parameters consist of asymmetry factor, single scattering albedo, surface albedo, and optical thickness.

  7. PHYSICAL STUDIES OF ISOLATED EUCARYOTIC NUCLEI

    PubMed Central

    Olins, Donald E.; Olins, Ada L.

    1972-01-01

    The degree of chromatin condensation in isolated rat liver nuclei and chicken erythrocyte nuclei was studied by phase-contrast microscopy as a function of solvent pH, K+ and Mg++ concentrations Data were represented as "phase" maps, and standard solvent conditions selected that reproducibly yield granular, slightly granular, and homogeneous nuclei Nuclei in these various states were examined by ultraviolet absorption and circular dichroism (CD) spectroscopy, low-angle X-ray diffraction, electron microscopy, and binding capacity for ethidium bromide Homogeneous nuclei exhibited absorption and CD spectra resembling those of isolated nucleohistone. Suspensions of granular nuclei showed marked turbidity and absorption flattening, and a characteristic blue-shift of a crossover wavelength in the CD spectra. In all solvent conditions studied, except pH < 2 3, low-angle X-ray reflections characteristic of the native, presumably superhelical, nucleohistone were observed from pellets of intact nuclei. Threads (100–200 A diameter) were present in the condensed and dispersed phases of nuclei fixed under the standard solvent conditions, and examined in the electron microscope after thin sectioning and staining Nuclei at neutral pH, with different degrees of chromatin condensation, exhibited similar binding capacities for ethidium bromide. These data suggest a model that views chromatin condensation as a close packing of superhelical nucleohistone threads but still permits condensed chromatin to respond rapidly to alterations in solvent environment. PMID:4554987

  8. Reducing uncertainty of aerosol indirect effects using a joint satellite-reanalysis approach

    NASA Astrophysics Data System (ADS)

    Block, Karoline; Quaas, Johannes

    2015-04-01

    Aerosols are known to have a significant impact on cloud microphysics, acting as cloud condensation nuclei (CCN) and thereby altering cloud properties. Global estimates of indirect aerosol effects purely from satellites are very uncertain and often give insignificant results. To improve observationally based estimates we use a joint multi-component approach combining cloud retrievals from the A-Train satellite instruments and aerosol information from the MACC-II reanalysis. We show the ability of this approach to compute CCN and validate the results with insitu measurements. Furthermore we discuss the impact of these findings for computing cloud droplet numbers and cloud albedo to fill the gap in the chain leading to an accurate estimate of the first aerosol indirect radiative forcing.

  9. 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

  10. A51F-0123: Model Analysis of Tropospheric Aerosol Variability and Sources over the North Atlantic During NAAMES 2015-2016

    NASA Technical Reports Server (NTRS)

    Liu, Hongyu; Moore, Richard; Hostetler, Chris A.; Ferrare, Richard Anthony; Fairlie, Thomas Duncan; Hu, Youngxiang; Chen, Gao; Hair, Johnathan W.; Johnson, Matthew S.

    2016-01-01

    The North Atlantic Aerosols and Marine Ecosystems Study (NAAMES) is a five-year Earth-Venture Suborbital-2 Mission to characterize the plankton ecosystems and their influences on remote marine aerosols, boundary layer clouds, and their implications for climate in the North Atlantic. While marine-sourced aerosols have been shown to make important contributions to surface aerosol loading, cloud condensation nuclei and ice nuclei concentrations over remote marine and coastal regions, it is still a challenge to differentiate the marine biogenic aerosol signal from the strong influence of continental pollution outflow. We examine here the spatiotemporal variability and quantify the sources of tropospheric aerosols over the North Atlantic during the first two phases (November 2015 and May-June 2016) of NAAMES using a state-of-the-art chemical transport model (GEOS-Chem). The model is driven by the Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2) from the NASA Global Modeling and Assimilation Office (GMAO). It includes sulfate-nitrate-ammonium aerosol thermodynamics coupled to ozone-NOx-hydrocarbon-aerosol chemistry, mineral dust, sea salt, elemental and organic carbon aerosols, and especially a recently implemented parameterization for the marine primary organic aerosol emission. The simulated aerosols over the North Atlantic are evaluated with available satellite (e.g., MODIS) observations of aerosol optical depths (AOD), and aircraft and ship aerosol measurements. We diagnose transport pathways for continental pollution outflow over the North Atlantic using carbon monoxide, an excellent tracer for anthropogenic pollution transport. We also conduct model perturbation experiments to quantify the relative contributions of terrestrial and oceanic sources to the aerosol loading, AOD, and their variability over the North Atlantic.

  11. Transport characteristics of aerosol from urban point sources

    NASA Astrophysics Data System (ADS)

    Kunkel, Daniel; Lawrence, Mark G.; Kerkweg, Astrid; Tost, Holger; Jöckel, Patrick; Borrmann, Stephan

    2010-05-01

    Urban aerosols are an important source of regional and global air pollution. The local buildup, long-range transport, and dry and wet deposition of aerosols depend strongly on the aerosol size distribution and on the regional meteorological characteristics. We examine the characteristics of urban aerosol dispersion based on simulations of monodisperse passive aerosol tracers with sizes of 0.1, 1.0, 2.5, and 10.0 μm, performed with the global chemistry circulation model EMAC (ECHAM5-MESSy-Atmospheric-Chemistry). 39 point sources were selected for the analysis, originating from major population centers (MPCs) around the world. All tracers, one for each source and size, have the same total, constant emission flux, and undergo dry and wet aerosol deposition. Sensitivity simulations are performed in which either there is no activation of the aerosol as cloud condensation nuclei (CCN), or all aerosol is activated as CCN. Using the same constant emission rate for each MPC allows us to compare how different large point sources pollute the atmosphere and the surface on different horizontal scales. The transport and deposition of the aerosol tracers from each MPC are quantitatively compared by the application of metrics. The analysis focuses on: the efficiency of short- and long-range horizontal transport; the fraction of tracer transported to the upper troposphere; and the fractions which are dry or wet deposited. Smaller particles with longer lifetimes (two to 14 days) are more effective at polluting remote locations (horizontal and vertical) and are deposited mostly by scavenging, while larger particles, with shorter lifetimes (several hours to a couple of days) more effectively pollute the environment nearby their source, and are most strongly removed by dry deposition from the atmosphere. By means of considering the same emission for each city, the presentation provides a detailed view of how aerosol tracers disperse and deposit on different spatial scales, depending

  12. Enhanced Volatile Organic Compounds emissions and organic aerosol mass increase the oligomer content of atmospheric aerosols.

    PubMed

    Kourtchev, Ivan; Giorio, Chiara; Manninen, Antti; Wilson, Eoin; Mahon, Brendan; Aalto, Juho; Kajos, Maija; Venables, Dean; Ruuskanen, Taina; Levula, Janne; Loponen, Matti; Connors, Sarah; Harris, Neil; Zhao, Defeng; Kiendler-Scharr, Astrid; Mentel, Thomas; Rudich, Yinon; Hallquist, Mattias; Doussin, Jean-Francois; Maenhaut, Willy; Bäck, Jaana; Petäjä, Tuukka; Wenger, John; Kulmala, Markku; Kalberer, Markus

    2016-10-13

    Secondary organic aerosol (SOA) accounts for a dominant fraction of the submicron atmospheric particle mass, but knowledge of the formation, composition and climate effects of SOA is incomplete and limits our understanding of overall aerosol effects in the atmosphere. Organic oligomers were discovered as dominant components in SOA over a decade ago in laboratory experiments and have since been proposed to play a dominant role in many aerosol processes. However, it remains unclear whether oligomers are relevant under ambient atmospheric conditions because they are often not clearly observed in field samples. Here we resolve this long-standing discrepancy by showing that elevated SOA mass is one of the key drivers of oligomer formation in the ambient atmosphere and laboratory experiments. We show for the first time that a specific organic compound class in aerosols, oligomers, is strongly correlated with cloud condensation nuclei (CCN) activities of SOA particles. These findings might have important implications for future climate scenarios where increased temperatures cause higher biogenic volatile organic compound (VOC) emissions, which in turn lead to higher SOA mass formation and significant changes in SOA composition. Such processes would need to be considered in climate models for a realistic representation of future aerosol-climate-biosphere feedbacks.

  13. Enhanced Volatile Organic Compounds emissions and organic aerosol mass increase the oligomer content of atmospheric aerosols

    NASA Astrophysics Data System (ADS)

    Kourtchev, Ivan; Giorio, Chiara; Manninen, Antti; Wilson, Eoin; Mahon, Brendan; Aalto, Juho; Kajos, Maija; Venables, Dean; Ruuskanen, Taina; Levula, Janne; Loponen, Matti; Connors, Sarah; Harris, Neil; Zhao, Defeng; Kiendler-Scharr, Astrid; Mentel, Thomas; Rudich, Yinon; Hallquist, Mattias; Doussin, Jean-Francois; Maenhaut, Willy; Bäck, Jaana; Petäjä, Tuukka; Wenger, John; Kulmala, Markku; Kalberer, Markus

    2016-10-01

    Secondary organic aerosol (SOA) accounts for a dominant fraction of the submicron atmospheric particle mass, but knowledge of the formation, composition and climate effects of SOA is incomplete and limits our understanding of overall aerosol effects in the atmosphere. Organic oligomers were discovered as dominant components in SOA over a decade ago in laboratory experiments and have since been proposed to play a dominant role in many aerosol processes. However, it remains unclear whether oligomers are relevant under ambient atmospheric conditions because they are often not clearly observed in field samples. Here we resolve this long-standing discrepancy by showing that elevated SOA mass is one of the key drivers of oligomer formation in the ambient atmosphere and laboratory experiments. We show for the first time that a specific organic compound class in aerosols, oligomers, is strongly correlated with cloud condensation nuclei (CCN) activities of SOA particles. These findings might have important implications for future climate scenarios where increased temperatures cause higher biogenic volatile organic compound (VOC) emissions, which in turn lead to higher SOA mass formation and significant changes in SOA composition. Such processes would need to be considered in climate models for a realistic representation of future aerosol-climate-biosphere feedbacks.

  14. Enhanced Volatile Organic Compounds emissions and organic aerosol mass increase the oligomer content of atmospheric aerosols

    PubMed Central

    Kourtchev, Ivan; Giorio, Chiara; Manninen, Antti; Wilson, Eoin; Mahon, Brendan; Aalto, Juho; Kajos, Maija; Venables, Dean; Ruuskanen, Taina; Levula, Janne; Loponen, Matti; Connors, Sarah; Harris, Neil; Zhao, Defeng; Kiendler-Scharr, Astrid; Mentel, Thomas; Rudich, Yinon; Hallquist, Mattias; Doussin, Jean-Francois; Maenhaut, Willy; Bäck, Jaana; Petäjä, Tuukka; Wenger, John; Kulmala, Markku; Kalberer, Markus

    2016-01-01

    Secondary organic aerosol (SOA) accounts for a dominant fraction of the submicron atmospheric particle mass, but knowledge of the formation, composition and climate effects of SOA is incomplete and limits our understanding of overall aerosol effects in the atmosphere. Organic oligomers were discovered as dominant components in SOA over a decade ago in laboratory experiments and have since been proposed to play a dominant role in many aerosol processes. However, it remains unclear whether oligomers are relevant under ambient atmospheric conditions because they are often not clearly observed in field samples. Here we resolve this long-standing discrepancy by showing that elevated SOA mass is one of the key drivers of oligomer formation in the ambient atmosphere and laboratory experiments. We show for the first time that a specific organic compound class in aerosols, oligomers, is strongly correlated with cloud condensation nuclei (CCN) activities of SOA particles. These findings might have important implications for future climate scenarios where increased temperatures cause higher biogenic volatile organic compound (VOC) emissions, which in turn lead to higher SOA mass formation and significant changes in SOA composition. Such processes would need to be considered in climate models for a realistic representation of future aerosol-climate-biosphere feedbacks. PMID:27733773

  15. 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

  16. Evaluation of the global aerosol microphysical ModelE2-TOMAS model against satellite and ground-based observations

    NASA Astrophysics Data System (ADS)

    Lee, Y. H.; Adams, P. J.; Shindell, D. T.

    2015-03-01

    The TwO-Moment Aerosol Sectional (TOMAS) microphysics model has been integrated into the state-of-the-art general circulation model, GISS ModelE2. This paper provides a detailed description of the ModelE2-TOMAS model and evaluates the model against various observations including aerosol precursor gas concentrations, aerosol mass and number concentrations, and aerosol optical depths. Additionally, global budgets in ModelE2-TOMAS are compared with those of other global aerosol models, and the ModelE2-TOMAS model is compared to the default aerosol model in ModelE2, which is a one-moment aerosol (OMA) model (i.e. no aerosol microphysics). Overall, the ModelE2-TOMAS predictions are within the range of other global aerosol model predictions, and the model has a reasonable agreement (mostly within a factor of 2) with observations of sulfur species and other aerosol components as well as aerosol optical depth. However, ModelE2-TOMAS (as well as ModelE2-OMA) cannot capture the observed vertical distribution of sulfur dioxide over the Pacific Ocean, possibly due to overly strong convective transport and overpredicted precipitation. The ModelE2-TOMAS model simulates observed aerosol number concentrations and cloud condensation nuclei concentrations roughly within a factor of 2. Anthropogenic aerosol burdens in ModelE2-OMA differ from ModelE2-TOMAS by a few percent to a factor of 2 regionally, mainly due to differences in aerosol processes including deposition, cloud processing, and emission parameterizations. We observed larger differences for naturally emitted aerosols such as sea salt and mineral dust, as those emission rates are quite different due to different upper size cutoff assumptions.

  17. Science Overview Document Indirect and Semi-Direct Aerosol Campaign (ISDAC) April 2008

    SciTech Connect

    SJ Ghan; B Schmid; JM Hubbe; CJ Flynn; A Laskin; AA Zelenyuk; DJ Czizco; CN Long; G McFarquhar; J Verlinde; J Harrington; JW Strapp; P Liu; A Korolev; A McDonald; M Wolde; A Fridlind; T Garrett; G Mace; G Kok; S Brooks; D Collins; D Lubin; P Lawson; M Dubey; C Mazzoleni; M Shupe; S Xie; DD Turner; Q Min; EJ Mlawer; D Mitchell

    2007-11-01

    The ARM Climate Research Facility’s (ACRF) Aerial Vehicle Program (AVP) will deploy an intensive cloud and aerosol observing system to the ARM North Slope of Alaska (NSA) locale for a five week Indirect and Semi-Direct Aerosol Campaign (ISDAC) during period 29 March through 30 April 2008. The deployment period is within the International Polar Year, thus contributing to and benefiting from the many ancillary observing systems collecting data synergistically. We will deploy the Canadian National Research Council Convair 580 aircraft to measure temperature, humidity, total particle number, aerosol size distribution, single particle composition, concentrations of cloud condensation nuclei and ice nuclei, optical scattering and absorption, updraft velocity, cloud liquid water and ice contents, cloud droplet and crystal size distributions, cloud particle shape, and cloud extinction. In addition to these aircraft measurements, ISDAC will deploy two instruments at the ARM site in Barrow: a spectroradiometer to retrieve cloud optical depth and effective radius, and a tandem differential mobility analyzer to measure the aerosol size distribution and hygroscopicity. By using many of the same instruments used during Mixed-Phase Arctic Cloud Experiment (M-PACE), conducted in October 2004, we will be able to contrast the arctic aerosol and cloud properties during the fall and spring transitions. The aerosol measurements can be used in cloud models driven by objectively analyzed boundary conditions to test whether the cloud models can simulate the aerosol influence on the clouds. The influence of aerosol and boundary conditions on the simulated clouds can be separated by running the cloud models with all four combinations of M-PACE and ISDAC aerosol and boundary conditions: M-PACE aerosol and boundary conditions, M-PACE aerosol and ISDAC boundary conditions, ISDAC aerosol and M-PACE boundary conditions, and ISDAC aerosol and boundary conditions. ISDAC and M-PACE boundary

  18. Novel Measurements of Aerosol Particle Interfaces Using Biphasic Microfluidics

    NASA Astrophysics Data System (ADS)

    Metcalf, A. R.; Dutcher, C. S.

    2014-12-01

    Secondary organic aerosol (SOA) particles are nearly ubiquitous in the atmosphere and yet there remains large uncertainties in their formation processes and ambient properties. These particles are complex microenvironments, which can contain multiple interfaces due to internal aqueous-organic phase partitioning and to the external liquid-vapor surface. These aerosol interfaces can profoundly affect the fate of condensable organic compounds emitted into the atmosphere by altering the way in which organic vapors interact with the ambient aerosol. Aerosol interfaces affect particle internal structure, species uptake, equilibrium partitioning, activation to cloud condensation or ice nuclei, and optical properties. For example, organic thin films can shield the core of the aerosol from the ambient environment, which may disrupt equilibrium partitioning and mass transfer. To improve our ability to accurately predict the fate of SOA in the atmosphere, we must improve our knowledge of aerosol interfaces and their interactions with the ambient environment. Few technologies exist to accurately probe aerosol interfaces at atmospherically-relevant conditions. In this talk, a novel method using biphasic microscale flows will be introduced for generating, trapping, and perturbing complex interfaces at atmospherically relevant conditions. These microfluidic experiments utilize high-speed imaging to monitor interfacial phenomena at the microscale and are performed with phase contrast and fluorescence microscopy on a temperature-controlled inverted microscope stage. From these experiments, interfacial thermodynamic properties such as surface tension, rheological properties such as interfacial moduli, and kinetic properties such as mass transfer coefficients can be measured or inferred. Chemical compositions of the liquid phases studied here span a range of viscosities and include electrolyte and water soluble organic acid species often observed in the atmosphere, such as mixtures

  19. Development of infrared photothermal deflection spectroscopy (mirage effect) for analysis of condensed-phase aerosols collected in a micro-orifice uniform deposit impactor.

    PubMed

    Dada, Oluwatosin O; Bialkowski, Stephen E

    2008-12-01

    The potential of mid-infrared photothermal deflection spectrometry for aerosol analysis is demonstrated. Ammonium nitrate aerosols are deposited on a flat substrate using a micro-orifice uniform deposit impactor (MOUDI). Photothermal spectroscopy with optical beam deflection (mirage effect) is used to detect deposited aerosols. Photothermal deflection from aerosols is measured by using pulsed infrared laser light to heat up aerosols collected on the substrate. The deflection signal is obtained by measuring the position of a spot from a beam of light as it passes near the heated surface. The results indicate non-rotating impaction as the preferred MOUDI impaction method. Energy-dependent photothermal measurement shows a linear relationship between signal and laser intensity, and no loss of signal with time is observed. The detection limit from the signal-mass curve is 7.31 ng. For 30 minutes collection time and 30 L/min flow rate of the impactor, the limit of detection in terms of aerosol mass concentration is 0.65 microg m(-3).

  20. Simultaneous Retrieval of Multiple Aerosol Parameters Using a Multi-Angular Approach

    NASA Technical Reports Server (NTRS)

    Kuo, K.-S.; Weger, R. C.; Welch, R. M.

    1997-01-01

    Atmospheric aerosol particles, both natural and anthropogenic, are important to the earth's radiative balance through their direct and indirect effects. They scatter the incoming solar radiation (direct effect) and modify the shortwave reflective properties of clouds by acting as cloud condensation nuclei (indirect effect). Although it has been suggested that aerosols exert a net cooling influence on climate, this effect has received less attention than the radiative forcing due to clouds and greenhouse gases. In order to understand the role that aerosols play in a changing climate, detailed and accurate observations are a prerequisite. The retrieval of aerosol optical properties by satellite remote sensing has proven to be a difficult task. The difficulty results mainly from the tenuous nature and variable composition of aerosols. To date, with single-angle satellite observations, we can only retrieve reliably against dark backgrounds, such as over oceans and dense vegetation. Even then, assumptions must be made concerning the chemical composition of aerosols. In this investigation we examine the feasibility of simultaneous retrieval of multiple aerosol optical parameters using reflectances from a typical set of twelve angles observed by the French POLDER instrument. The retrieved aerosol optical parameters consist of asymmetry factor, single scattering albedo, surface albedo, and optical thickness.

  1. Reconciling Organic Aerosol Volatility, Hygroscopicity, and Oxidation State During the Colorado DISCOVER-AQ Deployment

    NASA Astrophysics Data System (ADS)

    Hite, J. R.; Moore, R.; Martin, R.; Thornhill, K. L., II; Winstead, E.; Anderson, B. E.; Nenes, A.

    2014-12-01

    The organic fraction of submicron aerosol can profoundly impact radiative forcing on climate directly, through enhancement of extinction, or indirectly through modulation of cloud formation. Semi-volatile constituents of organic ambient aerosol are of particular interest as their partitioning between the vapor and aerosol phases is not well constrained by current atmospheric models and appears to play an important role in the formation of cloud condensation nuclei (CCN) as suggested by recent research. An experimental setup consisting of a DMT CCN counter and SMPS downstream of a custom-built thermodenuder assembly was deployed during the summer 2014 DISCOVER-AQ field campaign to retrieve simultaneous, size-resolved volatility and hygroscopicity - through the use of scanning mobility CCN analysis (SMCA). Housed in the NASA Langley mobile laboratory, a suite of complimentary measurements were made available onboard including submicron aerosol composition and oxidation state provided by an HR-ToF-AMS, and aerosol optical properties provided by a range of other instruments including an SP2. Air masses sampled from locations across the Central Colorado region include influences from regional aerosol nucleation/growth events, long-range transport of Canadian biomass burning aerosols, cattle feedlot emissions and influences of the Denver urban plume - amidst a backdrop of widespread oil and gas exploration. The analysis focuses on the reconciliation of the retrieved aerosol volatility distributions and corresponding hygroscopicity and oxidation state observations, including the use of AMS factor analysis.

  2. Aerosol transport along the Andes from Amazonia to the remote Pacific Ocean: A multiyear CALIOP assessment

    NASA Astrophysics Data System (ADS)

    Bourgeois, Quentin; Ekman, Annica; Krejci, Radovan

    2015-04-01

    The free troposphere over South America and the Pacific Ocean is a particularly interesting region to study due to the prevailing easterly wind direction, forcing air over Amazonia towards the Pacific Ocean but encountering a natural barrier - the Andes - in between which might play a significant role. In addition, the strong contrast between the wet, relatively clean season and the dry, relatively polluted season as well as the difference between day and night meteorological conditions may influence the vertical distribution of aerosols in the free troposphere. Six years (2007-2012) of CALIOP observations at both day and night were used to investigate the vertical distribution, transport and removal processes of aerosols over South America and the Pacific Ocean. The multiyear assessment shows that aerosols, mainly biomass burning particles emitted during the dry season in Amazonia, may be lifted along the Andes. During their lifting, aerosols remain in the boundary layer which makes them subject to scavenging and deposition processes. The removal aerosol extinction rate was quantified. After reaching the top of the Andes, free tropospheric aerosols are likely pushed by the large-scale subsidence towards the marine boundary layer (MBL) during their transport over the Pacific Ocean. CALIOP observations may indicate that aerosols are transported over thousands of kilometers in the free troposphere over the Pacific Ocean. During their long range transport, aerosols could be entrained into the MBL and may further act as cloud condensation nuclei, and influence climate and the radiative budget of the Earth.

  3. Characterization of Halyomorpha halys (brown marmorated stink bug) biogenic volatile organic compound emissions and their role in secondary organic aerosol formation.

    PubMed

    Solomon, Danielle; Dutcher, Dabrina; Raymond, Timothy

    2013-11-01

    The formation of aerosols is a key component in understanding cloud formation in the context of radiative forcings and global climate modeling. Biogenic volatile organic compounds (BVOCs) are a significant source of aerosols, yet there is still much to be learned about their structures, sources, and interactions. The aims of this project were to identify the BVOCs found in the defense chemicals of the brown marmorated stink bug Halymorpha halys and quantify them using gas chromatography-mass spectrometry (GC/MS) and test whether oxidation of these compounds by ozone-promoted aerosol and cloud seed formation. The bugs were tested under two conditions: agitation by asphyxiation and direct glandular exposure. Tridecane, 2(5H)-furanone 5-ethyl, and (E)-2-decenal were identified as the three most abundant compounds. H. halys were also tested in the agitated condition in a smog chamber. It was found that in the presence of 100-180 ppm ozone, secondary aerosols do form. A scanning mobility particle sizer (SMPS) and a cloud condensation nuclei counter (CCNC) were used to characterize the secondary aerosols that formed. This reaction resulted in 0.23 microg/ bug of particulate mass. It was also found that these secondary organic aerosol particles could act as cloud condensation nuclei. At a supersaturation of 1%, we found a kappa value of 0.09. Once regional populations of these stink bugs stablilize and the populations estimates can be made, the additional impacts of their contribution to regional air quality can be calculated.

  4. 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/).

  5. Mushrooms as Rainmakers: How Spores Act as Nuclei for Raindrops

    PubMed Central

    2015-01-01

    Millions of tons of fungal spores are dispersed in the atmosphere every year. These living cells, along with plant spores and pollen grains, may act as nuclei for condensation of water in clouds. Basidiospores released by mushrooms form a significant proportion of these aerosols, particularly above tropical forests. Mushroom spores are discharged from gills by the rapid displacement of a droplet of fluid on the cell surface. This droplet is formed by the condensation of water on the spore surface stimulated by the secretion of mannitol and other hygroscopic sugars. This fluid is carried with the spore during discharge, but evaporates once the spore is airborne. Using environmental electron microscopy, we have demonstrated that droplets reform on spores in humid air. The kinetics of this process suggest that basidiospores are especially effective as nuclei for the formation of large water drops in clouds. Through this mechanism, mushroom spores may promote rainfall in ecosystems that support large populations of ectomycorrhizal and saprotrophic basidiomycetes. Our research heightens interest in the global significance of the fungi and raises additional concerns about the sustainability of forests that depend on heavy precipitation. PMID:26509436

  6. Size-resolved aerosol composition and its link to hygroscopicity at a forested site in Colorado

    NASA Astrophysics Data System (ADS)

    Levin, E. J. T.; Prenni, A. J.; Palm, B. B.; Day, D. A.; Campuzano-Jost, P.; Winkler, P. M.; Kreidenweis, S. M.; DeMott, P. J.; Jimenez, J. L.; Smith, J. N.

    2014-03-01

    Aerosol hygroscopicity describes the ability of a particle to take up water and form a cloud droplet. Modeling studies have shown sensitivity of precipitation-producing cloud systems to the availability of aerosol particles capable of serving as cloud condensation nuclei (CCN), and hygroscopicity is a key parameter controlling the number of available CCN. Continental aerosol is typically assumed to have a representative hygroscopicity parameter, κ, of 0.3; however, in remote locations this value can be lower due to relatively large mass fractions of organic components. To further our understanding of aerosol properties in remote areas, we measured size-resolved aerosol chemical composition and hygroscopicity in a forested, mountainous site in Colorado during the six-week BEACHON-RoMBAS (Bio-hydro-atmosphere interactions of Energy, Aerosols, Carbon, H2O, Organics and Nitrogen-Rocky Mountain Biogenic Aerosol Study) campaign. This campaign followed a year-long measurement period at this site, and results from the intensive campaign shed light on the previously reported seasonal cycle in aerosol hygroscopicity. New particle formation events were observed routinely at this site and nucleation mode composition measurements indicated that the newly formed particles were predominantly organic. These events likely contribute to the dominance of organic species at smaller sizes, where aerosol organic mass fractions were between 70 and 90%. Corresponding aerosol hygroscopicity was observed to be in the range κ = 0.15-0.22, with hygroscopicity increasing with particle size. Aerosol chemical composition measured by an aerosol mass spectrometer and calculated from hygroscopicity measurements agreed very well during the intensive study, with an assumed value of κorg = 0.13 resulting in the best agreement.

  7. Aircraft- and ground-based assessment of the CCN-AOD relationship and implications on model analysis of ACI and underlying aerosol processes

    NASA Astrophysics Data System (ADS)

    Shinozuka, Y.; Clarke, A. D.; Nenes, A.; Lathem, T. L.; Redemann, J.; Jefferson, A.; Wood, R.

    2014-12-01

    Contrary to common assumptions in satellite-based modeling of aerosol-cloud interactions, ∂logCCN/∂logAOD is less than unity, i.e., the number concentration of cloud condensation nuclei (CCN) less than doubles as aerosol optical depth (AOD) doubles. This can be explained by omnipresent aerosol processes. Condensation, coagulation and cloud processing, for example, generally make particles scatter more light while hardly increasing their number. This paper reports on the relationship in local air masses between CCN concentration, aerosol size distribution and light extinction observed from aircraft and the ground at diverse locations. The CCN-to-local-extinction relationship, when averaged over ~1 km distance and sorted by the wavelength dependence of extinction, varies approximately by a factor of 2, reflecting the variability in aerosol intensive properties. This, together with retrieval uncertainties and the variability in aerosol spatio-temporal distribution and hygroscopic growth, challenges satellite-based CCN estimates. However, the large differences in estimated CCN may correspond to a considerably lower uncertainty in cloud drop number concentration (CDNC), given the sublinear response of CDNC to CCN. Overall, our findings from airborne and ground-based observations call for model-based reexamination of aerosol-cloud interactions and underlying aerosol processes.

  8. Laboratory Experiments and Instrument Intercomparison Studies of Carbonaceous Aerosol Particles

    SciTech Connect

    Davidovits, Paul

    2015-10-20

    Aerosols containing black carbon (and some specific types of organic particulate matter) directly absorb incoming light, heating the atmosphere. In addition, all aerosol particles backscatter solar light, leading to a net-cooling effect. Indirect effects involve hydrophilic aerosols, which serve as cloud condensation nuclei (CCN) that affect cloud cover and cloud stability, impacting both atmospheric radiation balance and precipitation patterns. At night, all clouds produce local warming, but overall clouds exert a net-cooling effect on the Earth. The effect of aerosol radiative forcing on climate may be as large as that of the greenhouse gases, but predominantly opposite in sign and much more uncertain. The uncertainties in the representation of aerosol interactions in climate models makes it problematic to use model projections to guide energy policy. The objective of our program is to reduce the uncertainties in the aerosol radiative forcing in the two areas highlighted in the ASR Science and Program Plan. That is, (1) addressing the direct effect by correlating particle chemistry and morphology with particle optical properties (i.e. absorption, scattering, extinction), and (2) addressing the indirect effect by correlating particle hygroscopicity and CCN activity with particle size, chemistry, and morphology. In this connection we are systematically studying particle formation, oxidation, and the effects of particle coating. The work is specifically focused on carbonaceous particles where the uncertainties in the climate relevant properties are the highest. The ongoing work consists of laboratory experiments and related instrument inter-comparison studies both coordinated with field and modeling studies, with the aim of providing reliable data to represent aerosol processes in climate models. The work is performed in the aerosol laboratory at Boston College. At the center of our laboratory setup are two main sources for the production of aerosol particles: (a

  9. 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

  10. Spatial Variability of CCN Sized Aerosol Particles

    NASA Astrophysics Data System (ADS)

    Asmi, A.; Väänänen, R.

    2014-12-01

    The computational limitations restrict the grid size used in GCM models, and for many cloud types they are too large when compared to the scale of the cloud formation processes. Several parameterizations for e.g. convective cloud formation exist, but information on spatial subgrid variation of the cloud condensation nuclei (CCNs) sized aerosol concentration is not known. We quantify this variation as a function of the spatial scale by using datasets from airborne aerosol measurement campaigns around the world including EUCAARI LONGREX, ATAR, INCA, INDOEX, CLAIRE, PEGASOS and several regional airborne campaigns in Finland. The typical shapes of the distributions are analyzed. When possible, we use information obtained by CCN counters. In some other cases, we use particle size distribution measured by for example SMPS to get approximated CCN concentration. Other instruments used include optical particle counters or condensational particle counters. When using the GCM models, the CCN concentration used for each the grid-box is often considered to be either flat, or as an arithmetic mean of the concentration inside the grid-box. However, the aircraft data shows that the concentration values are often lognormal distributed. This, combined with the subgrid variations in the land use and atmospheric properties, might cause that the aerosol-cloud interactions calculated by using mean values to vary significantly from the true effects both temporary and spatially. This, in turn, can cause non-linear bias into the GCMs. We calculate the CCN aerosol concentration distribution as a function of different spatial scales. The measurements allow us to study the variation of these distributions within from hundreds of meters up to hundreds of kilometers. This is used to quantify the potential error when mean values are used in GCMs.

  11. 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

  12. Aerosol and CCN properties at Princess Elisabeth station, East Antarctica: seasonality, new particle formation events and properties around precipitation events

    NASA Astrophysics Data System (ADS)

    Mangold, Alexander; Laffineur, Quentin; De Backer, Hugo; Herenz, Paul; Wex, Heike; Gossart, Alexandra; Souverijns, Niels; Gorodetskaya, Irina; Van Lipzig, Nicole

    2016-04-01

    Since 2010, several complementary ground-based instruments for measuring the aerosol composition of the Antarctic atmosphere have been operated at the Belgian Antarctic research station Princess Elisabeth, in Dronning Maud Land, East Antarctica (71.95° S, 23.35° E, 1390 m asl.). In addition, three ground-based remote sensing instruments for cloud and precipitation observations have been installed for continuous operation, including a ceilometer (cloud base height, type, vertical extent), a 24 Ghz micro-rain radar (vertical profiles of radar effective reflectivity and Doppler velocity), and a pyrometer (cloud base temperature). The station is inhabited from November to end of February and operates under remote control during the other months. In this contribution, the general aerosol and cloud condensation nuclei (CCN) properties will be described with a special focus on new particle formation events and around precipitation events. New particle formation events are important for the atmospheric aerosol budget and they also show that aerosols are not only transported to Antarctica but are also produced there, also inland. Aerosols are essential for cloud formation and therefore also for precipitation, which is the only source for mass gain of the Antarctic ice sheet. Measured aerosol properties comprise size distribution, total number, total mass concentration, mass concentration of light-absorbing aerosol and absorption coefficient and total scattering coefficient. In addition, a CCN counter has been operated during austral summers 2013/14, 2014/15 and 2015/16. The baseline total number concentration N-total was around some hundreds of particles/cm3. During new particle formation events N-total increased to some thousands of particles/cm3. Simultaneous measurements of N-total, size distribution and CCN number revealed that mostly the number of particles smaller than 100 nm increased and that the concentration of cloud condensation nuclei increased only very

  13. Seasonal variability in aerosol, CCN and their relationship observed at a high altitude site in Western Ghats

    NASA Astrophysics Data System (ADS)

    Leena, P. P.; Pandithurai, G.; Anilkumar, V.; Murugavel, P.; Sonbawne, S. M.; Dani, K. K.

    2016-04-01

    Atmospheric aerosols which serve as cloud condensation nuclei (CCN) are key elements of the hydrological cycle and climate. In the present work, aerosol-CCN variability and their relationship have been studied for the first time at Mahabaleshwar, a high altitude (1348 m AMSL) site in Western Ghats, using one year (June 2012-May 2013) of observations. Present study has been done in two sections in which first temporal variability (diurnal and seasonal) of aerosol and CCN has been analyzed. Later CCN to aerosol ratio and other microphysical properties have been investigated along with detail discussion on possible sources of aerosol. First part, i.e., diurnal variation in aerosol and CCN concentration has shown relatively higher values during early morning hours in monsoon season whereas in winter and pre-monsoon it was higher in the evening hours. Seasonal mean variation in aerosol and CCN (SS above 0.6 %) has shown higher (less) in monsoon (winter) season. Temporal variation reveals dominance of fine-mode aerosol during monsoon season over the study region. In the second part temporal variation of activation ratio, k value (exponent of CCN super-saturation spectra) and geometric mean aerosol diameter have been analyzed. Variation of activation ratio showed the ratio is higher in monsoon especially for SS 0.6-1 %. The analysis also showed high k value during monsoon season as compared to other seasons (pre-monsoon and winter) which may be due to dominance of hygroscopic aerosols in the maritime air masses from Arabian Sea and biogenic aerosol emissions from the wet forest. Analyzed mean aerosol diameter is much smaller during monsoon season with less variability compared to other seasons. Overall analysis showed that aerosol and CCN concentration was higher over this high altitude site despite of dominant sink processes such as cloud scavenging and washout mechanisms indicating local emissions and biogenic Volatile Organic Compounds (BVOC) emissions from wet forest

  14. Simulating the Evolution of Soot Mixing State with a Particle-Resolved Aerosol Model

    SciTech Connect

    Riemer, Nicole; West, Matt; Zaveri, Rahul A.; Easter, Richard C.

    2009-05-05

    The mixing state of soot particles in the atmosphere is of crucial importance for assessing their climatic impact, since it governs their chemical reactivity, cloud condensation nuclei activity and radiative properties. To improve the mixing state representation in models, we present a new approach, the stochastic particle-resolved model PartMC-MOSAIC, which explicitly resolves the composition of individual particles in a given population of different types of aerosol particles. This approach accurately tracks the evolution of the mixing state of particles due to emission, dilution, condensation and coagulation. To make this direct stochastic particle-based method practical, we implemented a new multiscale stochastic coagulation method. With this method we achieved optimal efficiency for applications when the coagulation kernel is highly non-uniform, as is the case for many realistic applications. PartMC-MOSAIC was applied to an idealized urban plume case representative of a large urban area to simulate the evolution of carbonaceous aerosols of different types due to coagulation and condensation. For this urban plume scenario we quantified the individual processes that contribute to the aging of the aerosol distribution, illustrating the capabilities of our modeling approach. The results showed for the first time the multidimensional structure of particle composition, which is usually lost in internally-mixed sectional or modal aerosol models.

  15. 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.

  16. Campaign datasets for Two-Column Aerosol Project (TCAP)

    DOE Data Explorer

    Berg,Larry; Mei,Fan; Cairns,Brian; Chand,Duli; Comstock,Jennifer; Cziczo,Daniel; Hostetler,Chris; Hubbe,John; Long,Chuck; Michalsky,Joseph; Pekour,Mikhail; Russell,Phil; Scott,Herman; Sedlacek,Arthur; Shilling,John; Springston,Stephen; Tomlinson,Jason; Watson,Thomas; Zelenyuk-Imre,Alla

    2013-12-30

    This campaign was designed to provide a detailed set of observations with which to 1) perform radiative and cloud condensation nuclei (CCN) closure studies, 2) evaluate a new retrieval algorithm for aerosol optical depth (AOD) in the presence of clouds using passive remote sensing 3) extend a previously developed technique to investigate aerosol indirect effects, and 4) evaluate the performance of a detailed regional-scale model and a more parameterized global-scale model in simulating particle activation and AOD associated with the aging of anthropogenic aerosols. To meet these science objectives, the ARM Mobile Facility (AMF) and the Mobile Aerosol Observing System (MAOS) was deployed on Cape Cod, Massachusetts for a 12-month period starting in the summer of 2012 in order to quantify aerosol properties, radiation and cloud characteristics at a location subject to both clear- and cloudy- conditions, and clean- and polluted-conditions. These observations were supplemented by two aircraft intensive observation periods (IOPS), one in the summer and a second in the winter. Each IOP required two aircraft.

  17. Evaluation of Aerosol Indirect Radiative Forcing in MIRAGE

    SciTech Connect

    Ghan, Steven J.; Easter, Richard C.; Hudson, J D.; Breon, Francois

    2001-04-01

    We evaluate aerosol indirect radiative forcing simulated by the Model for Integrated Research on Atmospheric Global Exchanges (MIRAGE). Although explicit measurements of aerosol indirect radiative forcing do not exist, measurements of many of the links between aerosols and indirect radiative forcing are available and can be used for evaluation. These links include the cloud condensation nuclei concentration, the ratio of droplet number to aerosol number, the droplet number concentration, the column droplet number, the column cloud water, the droplet effective radius, the cloud optical depth, the correlation between cloud albedo and droplet effective radius, and the cloud radiative forcing. The CCN concentration simulated by MIRAGE agrees with measurements for supersaturations larger than 0.1%, but not for smaller supersaturations. Simulated droplet number concentrations are too low in most, but not all, locations with available measurements, even when normalized by aerosol number. MIRA GE correctly simulates the higher droplet numbers and smaller droplet sizes over continents and in the Northern Hemisphere. Biases in column cloud water, cloud optical depth, and shortwave cloud radiative forcing are evident in the Intertropical Convergence Zone and in the subtropical oceans. MIRAGE correctly simulates a negative correlation between cloud albedo and droplet size over remote oceans for cloud optical depths greater than 15 and a positive correlation for cloud optical depths less than 15, but fails to simulate a negative correlation over land.

  18. Aerosol Activity and Hygroscopicity Combined with Lidar Data in the Urban Atmosphere of Athens, Greece in the Frame of the HYGRA_CD Campaign

    NASA Astrophysics Data System (ADS)

    Bougiatioti, Aikaterini; Papayannis, Alexandros; Vratolis, Stergios; Argyrouli, Athina; Mihalopoulos, Nikolaos; Tsagkaraki, Maria; Nenes, Athanasios; Eleftheriadis, Konstantinos

    2016-06-01

    Measurements of cloud condensation nuclei (CCN) concentrations between 0.2-1.0% supersaturation and aerosol size distribution were performed at an urban background site of Athens during HygrA-CD. The site is affected by local and long-range transported emissions as portrayed by the external mixing of the particles, as the larger ones appear to be more hygroscopic and more CCN-active than smaller ones. Activation fractions at all supersaturations exhibit a diurnal variability with minimum values around noon, which are considerably lower than unity. This reinforces the conclusion that the aerosol is mostly externally mixed between "fresher", less hygroscopic components with more aged, CCN active constituents.

  19. 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.

  20. Attribution of the United States "warming hole": aerosol indirect effect and precipitable water vapor.

    PubMed

    Yu, Shaocai; Alapaty, Kiran; Mathur, Rohit; Pleim, Jonathan; Zhang, Yuanhang; Nolte, Chris; Eder, Brian; Foley, Kristen; Nagashima, Tatsuya

    2014-11-06

    Aerosols can influence the climate indirectly by acting as cloud condensation nuclei and/or ice nuclei, thereby modifying cloud optical properties. In contrast to the widespread global warming, the central and south central United States display a noteworthy overall cooling trend during the 20(th) century, with an especially striking cooling trend in summertime daily maximum temperature (Tmax) (termed the U.S. "warming hole"). Here we used observations of temperature, shortwave cloud forcing (SWCF), longwave cloud forcing (LWCF), aerosol optical depth and precipitable water vapor as well as global coupled climate models to explore the attribution of the "warming hole". We find that the observed cooling trend in summer Tmax can be attributed mainly to SWCF due to aerosols with offset from the greenhouse effect of precipitable water vapor. A global coupled climate model reveals that the observed "warming hole" can be produced only when the aerosol fields are simulated with a reasonable degree of accuracy as this is necessary for accurate simulation of SWCF over the region. These results provide compelling evidence of the role of the aerosol indirect effect in cooling regional climate on the Earth. Our results reaffirm that LWCF can warm both winter Tmax and Tmin.

  1. Attribution of the United States “warming hole”: Aerosol indirect effect and precipitable water vapor

    PubMed Central

    Yu, Shaocai; Alapaty, Kiran; Mathur, Rohit; Pleim, Jonathan; Zhang, Yuanhang; Nolte, Chris; Eder, Brian; Foley, Kristen; Nagashima, Tatsuya

    2014-01-01

    Aerosols can influence the climate indirectly by acting as cloud condensation nuclei and/or ice nuclei, thereby modifying cloud optical properties. In contrast to the widespread global warming, the central and south central United States display a noteworthy overall cooling trend during the 20th century, with an especially striking cooling trend in summertime daily maximum temperature (Tmax) (termed the U.S. “warming hole”). Here we used observations of temperature, shortwave cloud forcing (SWCF), longwave cloud forcing (LWCF), aerosol optical depth and precipitable water vapor as well as global coupled climate models to explore the attribution of the “warming hole”. We find that the observed cooling trend in summer Tmax can be attributed mainly to SWCF due to aerosols with offset from the greenhouse effect of precipitable water vapor. A global coupled climate model reveals that the observed “warming hole” can be produced only when the aerosol fields are simulated with a reasonable degree of accuracy as this is necessary for accurate simulation of SWCF over the region. These results provide compelling evidence of the role of the aerosol indirect effect in cooling regional climate on the Earth. Our results reaffirm that LWCF can warm both winter Tmax and Tmin. PMID:25373416

  2. [Hygroscopic Properties of Aerosol Particles in North Suburb of Nanjing in Spring].

    PubMed

    Xu, Bin; Zhang, Ze-feng; Li, Yan-weil; Qin, Xin; Miao, Qing; Shen, Yan

    2015-06-01

    The hygroscopic properties of submicron aerosol particles have significant effects on spectral distribution, CCN activation, climate forcing, human health and so on. A Hygroscopic Tandem Differential Mobility Analyzer (HTDMA) was utilized to analyze the hygroscopic properties of aerosol particles in the northern suburb of Nanjing during 16 April to 21 May, 2014. At relative humidity (RH) of 90%, for particles with dry diameters 30-230 nm, the probability distribution of GF (GF-PDF) shows a distinct bimodal pattern, with a dominant more-hygroscopic group and a smaller less-hygroscopic group. A contrast analysis between day and night suggests that, aerosol particles during day time have a stronger hygroscopicity and a higher number fraction of more-hygroscopic group than that at night overall. Aerosol particles during night have a higher degree of externally mixed state. Backward trajectory analysis using HYSPLIT mode reveals that, the sampling site is mainly affected by three air masses. For aitken nuclei, northwest continental air masses experience a longer aging process and have a stronger hygroscopicity. For condensation nuclei, east air masses have a stronger hygroscopicity and have a higher number fraction of more-hygroscopic group. Aerosol particles in local air masses have a high number fraction of more-hygroscopic group in the whole diameter range.

  3. Assessing the Dynamics of Organic Aerosols over the North Atlantic Ocean

    PubMed Central

    Kasparian, Jérôme; Hassler, Christel; Ibelings, Bas; Berti, Nicolas; Bigorre, Sébastien; Djambazova, Violeta; Gascon-Diez, Elena; Giuliani, Grégory; Houlmann, Raphaël; Kiselev, Denis; de Laborie, Pierric; Le, Anh-Dao; Magouroux, Thibaud; Neri, Tristan; Palomino, Daniel; Pfändler, Stéfanie; Ray, Nicolas; Sousa, Gustavo; Staedler, Davide; Tettamanti, Federico; Wolf, Jean-Pierre; Beniston, Martin

    2017-01-01

    The influence of aerosols on climate is highly dependent on the particle size distribution, concentration, and composition. In particular, the latter influences their ability to act as cloud condensation nuclei, whereby they impact cloud coverage and precipitation. Here, we simultaneously measured the concentration of aerosols from sea spray over the North Atlantic on board the exhaust-free solar-powered vessel “PlanetSolar”, and the sea surface physico-chemical parameters. We identified organic-bearing particles based on individual particle fluorescence spectra. Organic-bearing aerosols display specific spatio-temporal distributions as compared to total aerosols. We propose an empirical parameterization of the organic-bearing particle concentration, with a dependence on water salinity and sea-surface temperature only. We also show that a very rich mixture of organic aerosols is emitted from the sea surface. Such data will certainly contribute to providing further insight into the influence of aerosols on cloud formation, and be used as input for the improved modeling of aerosols and their role in global climate processes. PMID:28361985

  4. Assessing the Dynamics of Organic Aerosols over the North Atlantic Ocean.

    PubMed

    Kasparian, Jérôme; Hassler, Christel; Ibelings, Bas; Berti, Nicolas; Bigorre, Sébastien; Djambazova, Violeta; Gascon-Diez, Elena; Giuliani, Grégory; Houlmann, Raphaël; Kiselev, Denis; de Laborie, Pierric; Le, Anh-Dao; Magouroux, Thibaud; Neri, Tristan; Palomino, Daniel; Pfändler, Stéfanie; Ray, Nicolas; Sousa, Gustavo; Staedler, Davide; Tettamanti, Federico; Wolf, Jean-Pierre; Beniston, Martin

    2017-03-31

    The influence of aerosols on climate is highly dependent on the particle size distribution, concentration, and composition. In particular, the latter influences their ability to act as cloud condensation nuclei, whereby they impact cloud coverage and precipitation. Here, we simultaneously measured the concentration of aerosols from sea spray over the North Atlantic on board the exhaust-free solar-powered vessel "PlanetSolar", and the sea surface physico-chemical parameters. We identified organic-bearing particles based on individual particle fluorescence spectra. Organic-bearing aerosols display specific spatio-temporal distributions as compared to total aerosols. We propose an empirical parameterization of the organic-bearing particle concentration, with a dependence on water salinity and sea-surface temperature only. We also show that a very rich mixture of organic aerosols is emitted from the sea surface. Such data will certainly contribute to providing further insight into the influence of aerosols on cloud formation, and be used as input for the improved modeling of aerosols and their role in global climate processes.

  5. Influence of Surface Seawater and Atmospheric Conditions on the Ccn Activity of Ocean-Derived Aerosol

    NASA Astrophysics Data System (ADS)

    Quinn, P.; Bates, T. S.; Russell, L. M.; Frossard, A. A.; Keene, W. C.; Kieber, D. J.; Hakala, J. P.

    2012-12-01

    Ocean-derived aerosols are produced from direct injection into the atmosphere (primary production) and gas-to-particle conversion in the atmosphere (secondary production). These different production mechanisms result in a broad range of particle sizes that has implications for the impact of ocean-derived aerosol on climate. The chemical composition of ocean-derived aerosols is a result of a complex mixture of inorganic sea salt and organic matter including polysaccharides, proteins, amino acids, microorganisms and their fragments, and secondary oxidation products. Both production mechanisms and biological processes in the surface ocean impact the ability of ocean-derived aerosol to act as cloud condensation nuclei (CCN). In addition, CCN activity can be impacted by atmospheric processing that modifies particle size and composition after the aerosol is emitted from the ocean. To understand relationships between production mechanism, surface ocean biology, and atmospheric processing, measurements were made of surface ocean chlorophyll and dissolved organic matter; nascent sea spray aerosol freshly emitted from the ocean surface; and ambient marine aerosol. These measurements were made along the coast of California and in the North Atlantic between the northeast US and Bermuda. These regions include both eutrophic and oligotraphic waters and, thus, provide for observations over a wide range of ocean conditions.

  6. 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.

  7. On the characteristics of aerosol indirect effect based on dynamic regimes in global climate models

    NASA Astrophysics Data System (ADS)

    Zhang, Shipeng; Wang, Minghuai; Ghan, Steven J.; Ding, Aijun; Wang, Hailong; Zhang, Kai; Neubauer, David; Lohmann, Ulrike; Ferrachat, Sylvaine; Takeamura, Toshihiko; Gettelman, Andrew; Morrison, Hugh; Lee, Yunha; Shindell, Drew T.; Partridge, Daniel G.; Stier, Philip; Kipling, Zak; Fu, Congbin

    2016-03-01

    Aerosol-cloud interactions continue to constitute a major source of uncertainty for the estimate of climate radiative forcing. The variation of aerosol indirect effects (AIE) in climate models is investigated across different dynamical regimes, determined by monthly mean 500 hPa vertical pressure velocity (ω500), lower-tropospheric stability (LTS) and large-scale surface precipitation rate derived from several global climate models (GCMs), with a focus on liquid water path (LWP) response to cloud condensation nuclei (CCN) concentrations. The LWP sensitivity to aerosol perturbation within dynamic regimes is found to exhibit a large spread among these GCMs. It is in regimes of strong large-scale ascent (ω500 < -25 hPa day-1) and low clouds (stratocumulus and trade wind cumulus) where the models differ most. Shortwave aerosol indirect forcing is also found to differ significantly among different regimes. Shortwave aerosol indirect forcing in ascending regimes is close to that in subsidence regimes, which indicates that regimes with strong large-scale ascent are as important as stratocumulus regimes in studying AIE. It is further shown that shortwave aerosol indirect forcing over regions with high monthly large-scale surface precipitation rate (> 0.1 mm day-1) contributes the most to the total aerosol indirect forcing (from 64 to nearly 100 %). Results show that the uncertainty in AIE is even larger within specific dynamical regimes compared to the uncertainty in its global mean values, pointing to the need to reduce the uncertainty in AIE in different dynamical regimes.

  8. On the characteristics of aerosol indirect effect based on dynamic regimes in global climate models

    SciTech Connect

    Zhang, S.; Wang, Minghuai; Ghan, Steven J.; Ding, A.; Wang, Hailong; Zhang, Kai; Neubauer, David; Lohmann, U.; Ferrachat, S.; Takeamura, Toshihiko; Gettelman, A.; Morrison, H.; Lee, Y. H.; Shindell, D. T.; Partridge, Daniel; Stier, P.; Kipling, Z.; Fu, Congbin

    2016-03-04

    Aerosol-cloud interactions continue to constitute a major source of uncertainty for the estimate of climate radiative forcing. The variation of aerosol indirect effects (AIE) in climate models is investigated across different dynamical regimes, determined by monthly mean 500 hPa vertical pressure velocity (ω500), lower-tropospheric stability (LTS) and large-scale surface precipitation rate derived from several global climate models (GCMs), with a focus on liquid water path (LWP) response to cloud condensation nuclei (CCN) concentrations. The LWP sensitivity to aerosol perturbation within dynamic regimes is found to exhibit a large spread among these GCMs. It is in regimes of strong large-scale ascend (ω500 < -25 hPa/d) and low clouds (stratocumulus and trade wind cumulus) where the models differ most. Shortwave aerosol indirect forcing is also found to differ significantly among different regimes. Shortwave aerosol indirect forcing in ascending regimes is as large as that in stratocumulus regimes, which indicates that regimes with strong large-scale ascend are as important as stratocumulus regimes in studying AIE. 42" It is further shown that shortwave aerosol indirect forcing over regions with high monthly large-scale surface precipitation rate (> 0.1 mm/d) contributes the most to the total aerosol indirect forcing (from 64% to nearly 100%). Results show that the uncertainty in AIE is even larger within specific dynamical regimes than that globally, pointing to the need to reduce the uncertainty in AIE in different dynamical regimes.

  9. Residence times of fine tropospheric aerosols as determined by {sup 210}Pb progeny.

    SciTech Connect

    Marley, N. A.; Gaffney, J. S.; Drayton, P. J.; Cunningham, M. M.; Mielcarek, C.; Ravelo, R.; Wagner, C.

    1999-10-05

    Fine tropospheric aerosols can play important roles in the radiative balance of the atmosphere. The fine aerosols can act directly to cool the atmosphere by scattering incoming solar radiation, as well as indirectly by serving as cloud condensation nuclei. Fine aerosols, particularly carbonaceous soots, can also warm the atmosphere by absorbing incoming solar radiation. In addition, aerosols smaller than 2.5 {micro}m have recently been implicated in the health effects of air pollution. Aerosol-active radioisotopes are ideal tracers for the study of atmospheric transport processes. The source terms of these radioisotopes are relatively well known, and they are removed from the atmosphere only by radioactive decay or by wet or dry deposition of the host aerosol. The progeny of the primordial radionuclide {sup 238}U are of particular importance to atmospheric studies. Uranium-238 is common throughout Earth's crust and decays to the inert gas {sup 222}Rn, which escapes into the atmosphere. Radon-222 decays by the series of alpha and beta emissions shown in Figure 1 to the long-lived {sup 210}Pb. Once formed, {sup 210}Pb becomes attached to aerosol particles with average attachment times of 40 s to 3 min.

  10. 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.

  11. Influence of the external mixing state of atmospheric aerosol on derived CCN number concentrations

    NASA Astrophysics Data System (ADS)

    Wex, H.; McFiggans, G.; Henning, S.; Stratmann, F.

    2010-05-01

    We derived the range of particle hygroscopicities ($\\kappa$) that occurs in the atmosphere, based on literature data of measured hygroscopic growth or based on chemical composition. The derived $\\kappa$-values show that the atmospheric aerosol often is an external mixture with respect to hygroscopicity. Mean $\\kappa$ were derived for urban, rural, and marine aerosols for the different hygroscopic modes. Using these $\\kappa$ and exemplary particle number size distributions for the different aerosols, the number concentration of cloud condensation nuclei (NCCN) was derived for two cases, (1) accounting for the less hygroscopic fraction of particles and (2) assuming all particles to have $\\kappa$ of the more hygroscopic mode. NCCN derived from measured particle hygroscopicity is overestimated for case (2). Overestimation of NCCN is largest for fresh continental aerosol and less pronounced for marine aerosol. With $\\kappa$ derived from bulk aerosol composition data, only the hygroscopicity of more soluble aerosol particles is captured. Bulk or even size-resolved composition data will be insufficient to predict NCCN under many conditions unless independent information about particle mixing state is available.

  12. 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.

  13. Development of an aerosol microphysical module: Aerosol Two-dimensional bin module for foRmation and Aging Simulation (ATRAS)

    SciTech Connect

    Matsui, H.; Koike, Makoto; Kondo, Yutaka; Fast, Jerome D.; Takigawa, M.

    2014-09-30

    Number concentrations, size distributions, and mixing states of aerosols are essential parameters for accurate estimation of aerosol direct and indirect effects. In this study, we developed an aerosol module, designated Aerosol Two-dimensional bin module for foRmation and Aging Simulation (ATRAS), that can represent these parameters explicitly by considering new particle formation (NPF), black carbon (BC) aging, and secondary organic aerosol (SOA) processes. A two-dimensional bin representation is used for particles with dry diameters from 40 nm to 10 µm to resolve both aerosol size (12 bins) and BC mixing state (10 bins) for a total of 120 bins. The particles with diameters from 1 to 40 nm are resolved using an additional 8 size bins to calculate NPF. The ATRAS module was implemented in the WRF-chem model and applied to examine the sensitivity of simulated mass, number, size distributions, and optical and radiative parameters of aerosols to NPF, BC aging and SOA processes over East Asia during the spring of 2009. BC absorption enhancement by coating materials was about 50% over East Asia during the spring, and the contribution of SOA processes to the absorption enhancement was estimated to be 10 – 20% over northern East Asia and 20 – 35% over southern East Asia. A clear north-south contrast was also found between the impacts of NPF and SOA processes on cloud condensation nuclei (CCN) concentrations: NPF increased CCN concentrations at higher supersaturations (smaller particles) over northern East Asia, whereas SOA increased CCN concentrations at lower supersaturations (larger particles) over southern East Asia. Application of ATRAS to East Asia also showed that the impact of each process on each optical and radiative parameter depended strongly on the process and the parameter in question. The module can be used in the future as a benchmark model to evaluate the accuracy of simpler aerosol models and examine interactions between NPF, BC aging, and SOA

  14. Development of an aerosol microphysical module: Aerosol Two-dimensional bin module for foRmation and Aging Simulation (ATRAS)

    NASA Astrophysics Data System (ADS)

    Matsui, H.; Koike, M.; Kondo, Y.; Fast, J. D.; Takigawa, M.

    2014-09-01

    Number concentrations, size distributions, and mixing states of aerosols are essential parameters for accurate estimations of aerosol direct and indirect effects. In this study, we develop an aerosol module, designated the Aerosol Two-dimensional bin module for foRmation and Aging Simulation (ATRAS), that can explicitly represent these parameters by considering new particle formation (NPF), black carbon (BC) aging, and secondary organic aerosol (SOA) processes. A two-dimensional bin representation is used for particles with dry diameters from 40 nm to 10 μm to resolve both aerosol sizes (12 bins) and BC mixing states (10 bins) for a total of 120 bins. The particles with diameters between 1 and 40 nm are resolved using additional eight size bins to calculate NPF. The ATRAS module is implemented in the WRF-Chem model and applied to examine the sensitivity of simulated mass, number, size distributions, and optical and radiative parameters of aerosols to NPF, BC aging, and SOA processes over East Asia during the spring of 2009. The BC absorption enhancement by coating materials is about 50% over East Asia during the spring, and the contribution of SOA processes to the absorption enhancement is estimated to be 10-20% over northern East Asia and 20-35% over southern East Asia. A clear north-south contrast is also found between the impacts of NPF and SOA processes on cloud condensation nuclei (CCN) concentrations: NPF increases CCN concentrations at higher supersaturations (smaller particles) over northern East Asia, whereas SOA increases CCN concentrations at lower supersaturations (larger particles) over southern East Asia. The application of ATRAS in East Asia also shows that the impact of each process on each optical and radiative parameter depends strongly on the process and the parameter in question. The module can be used in the future as a benchmark model to evaluate the accuracy of simpler aerosol models and examine interactions between NPF, BC aging, and SOA

  15. Development of an aerosol microphysical module: Aerosol Two-dimensional bin module for foRmation and Aging Simulation (ATRAS)

    NASA Astrophysics Data System (ADS)

    Matsui, H.; Koike, M.; Kondo, Y.; Fast, J. D.; Takigawa, M.

    2014-04-01

    Number concentrations, size distributions, and mixing states of aerosols are essential parameters for accurate estimation of aerosol direct and indirect effects. In this study, we develop an aerosol module, designated Aerosol Two-dimensional bin module for foRmation and Aging Simulation (ATRAS), that can represent these parameters explicitly by considering new particle formation (NPF), black carbon (BC) aging, and secondary organic aerosol (SOA) processes. A two-dimensional bin representation is used for particles with dry diameters from 40 nm to 10 μm to resolve both aerosol size (12 bins) and BC mixing state (10 bins) for a total of 120 bins. The particles with diameters from 1 to 40 nm are resolved using an additional 8 size bins to calculate NPF. The ATRAS module is implemented in the WRF-chem model and applied to examine the sensitivity of simulated mass, number, size distributions, and optical and radiative parameters of aerosols to NPF, BC aging and SOA processes over East Asia during the spring of 2009. BC absorption enhancement by coating materials is about 50% over East Asia during the spring, and the contribution of SOA processes to the absorption enhancement is estimated to be 10-20% over northern East Asia and 20-35% over southern East Asia. A clear north-south contrast is also found between the impacts of NPF and SOA processes on cloud condensation nuclei (CCN) concentrations: NPF increases CCN concentrations at higher supersaturations (smaller particles) over northern East Asia, whereas SOA increases CCN concentrations at lower supersaturations (larger particles) over southern East Asia. Application of ATRAS to East Asia also shows that the impact of each process on each optical and radiative parameter depends strongly on the process and the parameter in question. The module can be used in the future as a benchmark model to evaluate the accuracy of simpler aerosol models and examine interactions between NPF, BC aging, and SOA processes under

  16. Chemical composition and characteristics of ambient aerosols and rainwater residues during Indian summer monsoon: Insight from aerosol mass spectrometry

    NASA Astrophysics Data System (ADS)

    Chakraborty, Abhishek; Gupta, Tarun; Tripathi, Sachchida N.

    2016-07-01

    more efficiently as cloud condensation nuclei.

  17. Infrared spectroscopy of aerosols

    NASA Astrophysics Data System (ADS)

    Mentel, Th.; Sebald, H.

    2003-04-01

    In our large Aerosol Chamber at the FZ Jülich we apply HR FTIR absorption spectroscopy for the determination of trace gases. In the FTIR spectra we also observe broad absorptions of several 10 to a few 100 cm-1 widths that arise from species in the condensed aerosol phase: liquid H_2O, NO_3^-, SO_42-, HSO_4^-, or dicarboxylic acids. Moreover, the aerosol droplets caused extinctions over several 1000 cm-1 by IR scattering. This allows for in-situ observation of changes in the condensed aerosol phase e.g. on HNO_3 uptake, like the shift of the sulfate/bisulfate equilibrium or the growth by water condensation. The IR absorptions of the condensed aerosol phase provide useful extra information in process studies, if they can be quantified. Therefore the absorption cross section, respective, the absorption index which is the imaginary part of the complex refractive index is needed. We set up an aerosol flow tube in which IR spectroscopy on a 8 m light path and aerosol size distribution measurements in the range from 20 nm - 10 μm can be performed simultaneously. We measured sulfate aerosols at several relative humidities (dry, metastable, deliquescent). We will demonstrate an iterative procedure based on Mie calculations and Kramers Kronig transformation to retrieve the absorption index from the observed IR spectra and the corresponding size distribution (for dry ammonium sulfate). We will compare resulting absorption indices for aqueous sodium bisulfate aerosols at several relative humidties with thermodynamic model calculations for the Na^+/H^+/HSO_4^-/SO_42-/H_2O system.

  18. Weekly variability of precipitation induced by anthropogenic aerosols: A case study in Korea in summer 2004.

    SciTech Connect

    Bae, Soo Ya; Jeong, Jaein I.; Park, R.; Lim, Kyo-Sun; Hong, Song-You

    2016-01-06

    We examine the effect of anthropogenic aerosols on the weekly variability of precipitation in Korea in summer 2004 by using Weather Research and Forecasting (WRF) and Community Multiscale Air Quality (CMAQ) models. We con-duct two WRF simulations including a baseline simulation with empirically based cloud condensation nuclei (CCN) number concentrations and a sensitivity simulation with our implementation to account for the effect of aerosols on CCN number concentrations. The first simulation underestimates observed precipitation amounts, particularly in northeastern coastal areas of Korea, whereas the latter shows higher precipitation amounts that are in better agree-ment with the observations. In addition, the sensitivity model with the aerosol effects reproduces the observed weekly variability, particularly for precipitation frequency with a high R at 0.85, showing 20% increase of precipita-tion events during the weekend than those during weekdays. We find that the aerosol effect results in higher CCN number concentrations during the weekdays and a three-fold increase of the cloud water mixing ratio through en-hanced condensation. As a result, the amount of warm rain is generally suppressed because of the low auto-conversion process from cloud water to rain water under high aerosol conditions. The inefficient conversion, how-ever, leads to higher vertical development of clouds in the mid-atmosphere with stronger updrafts in the sensitivity model, which increases by 21% cold-phase hydrometeors including ice, snow, and graupel relative to the baseline model and ultimately results in higher precipitation amounts in summer.

  19. Weekly variability of precipitation induced by anthropogenic aerosols: A case study in Korea in summer 2004.

    PubMed

    Bae, Soo Ya; Jeong, Jaein I; Park, Rokjin J; Lim, Kyo-Sun Sunny; Hong, Song-You

    2016-01-15

    We examine the effect of anthropogenic aerosols on the weekly variability of precipitation in Korea in summer 2004 by using Weather Research and Forecasting (WRF) and Community Multiscale Air Quality (CMAQ) models. We conduct two WRF simulations including a baseline simulation with empirically based cloud condensation nuclei (CCN) number concentrations and a sensitivity simulation with our implementation to account for the effect of aerosols on CCN number concentrations. The first simulation underestimates observed precipitation amounts, particularly in northeastern coastal areas of Korea, whereas the latter shows higher precipitation amounts that are in better agreement with the observations. In addition, the sensitivity model with the aerosol effects reproduces the observed weekly variability, particularly for precipitation frequency with a high R at 0.85, showing 20% increase of precipitation events during the weekend than those during weekdays. We find that the aerosol effect results in higher CCN number concentrations during the weekdays and a three-fold increase of the cloud water mixing ratio through enhanced condensation. As a result, the amount of warm rain is generally suppressed because of the low auto-conversion process from cloud water to rain water under high aerosol conditions. The inefficient conversion, however, leads to higher vertical development of clouds in the mid-atmosphere with stronger updrafts in the sensitivity model, which increases by 21% cold-phase hydrometeors including ice, snow, and graupel relative to the baseline model and ultimately results in higher precipitation amounts in summer.

  20. Aircraft measurements of aerosol properties during GoAmazon - G1 and HALO inter-comparison

    NASA Astrophysics Data System (ADS)

    Mei, F.; Cecchini, M. A.; Wang, J.; Tomlinson, J. M.; Comstock, J. M.; Hubbe, J. M.; Pekour, M. S.; Machado, L.; Wendisch, M.; Longo, K.; Martin, S. T.; Schmid, B.; Weinzierl, B.; Krüger, M. L.; Zöger, M.

    2015-12-01

    Currently, the indirect effects of atmospheric aerosols remain the most uncertain components in forcing of climate change over the industrial period (IPCC, 2013). This large uncertainty is partially a result of our incomplete understanding of the ability of particles to form cloud droplets under atmospherically relevant supersaturations. One objective of the US Department of Energy (DOE) Green Ocean Amazon Project (GoAmazon2014/5) is to understand the influence of the emission from Manaus, a tropical megacity, on aerosol size, concentration, and chemical composition, and their impact on cloud condensation nuclei (CCN) spectrum. The GoAmazon2014/5 study was an international campaign with the collaboration efforts from US, Brazil and Germany. During the intensive operation period, in the dry season (Sep. 1st - Oct. 10th, 2014), aerosol concentration, size distributions, and CCN spectra, both under pristine conditions and inside the Manaus plume, were characterized in-situ from the DOE Gulfstream-1 (G-1) research aircraft and German HALO aircraft during 4 coordinated flights on Sep. 9th, Sep. 16th, Sep 21st and Oct. 1st, 2014. During those four flights, aerosol number concentrations and CCN concentrations at two supersaturations (0.25% and 0.5%) were measured by condensation particle counters (CPCs) and a DMT dual column CCN counter onboard both G-1 and HALO. Aerosol size distribution was also measured by a Fast Integrated Mobility Spectrometer (FIMS) aboard the G-1 and is compared with the size distribution from Ultra High Sensitivity Aerosol Spectrometer - Airborne (UHSAS-A, DMT), which were deployed both on the G-1 and the HALO. Good agreement between the aerosol properties measured from the two aircraft has been achieved. The vertical profiles of aerosol size distribution and CCN spectrum will be discussed.

  1. 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

  2. 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.

  3. Nanoscopic structure of DNA condensed for gene delivery.

    PubMed Central

    Dunlap, D D; Maggi, A; Soria, M R; Monaco, L

    1997-01-01

    Scanning force microscopy was used to examine DNA condensates prepared with varying stoichiometries of lipospermine or polyethylenimine in physiological solution. For the first time, individual DNA strands were clearly visualized in incomplete condensates without drying. Using lipospermine at sub-saturating concentrations, discrete nuclei of condensation were observed often surrounded by folded loops of DNA. Similar packing of DNA loops occurred for polyethylenimine-induced condensation. Increasing the amount of the condensing agent led to the progressive coalescence or aggregation of initial condensation nuclei through folding rather than winding the DNA. At over-saturating charge ratios of the cationic lipid or polymer to DNA, condensates had sizes smaller than or equal to those measured previously in electron micrographs. Polyethylenimine condensates were more compact than lipospermine condensates and both produced more homogeneously compacted plasmids when used in a 2-4-fold charge excess. The size and morphology of the condensates may affect their efficiency in transfection. PMID:9224610

  4. Physics of Unstable Nuclei

    NASA Astrophysics Data System (ADS)

    Khoa, Dao Tien; Egelhof, Peter; Gales, Sydney; Giai, Nguyen Van; Motobayashi, Tohru

    2008-04-01

    Studies at the RIKEN RI beam factory / T. Motobayashi -- Dilute nuclear states / M. Freer -- Studies of exotic systems using transfer reactions at GANIL / D. Beaumel et al. -- First results from the Magnex large-acceptance spectrometer / A. Cunsolo et al. -- The ICHOR project and spin-isospin physics with unstable beams / H. Sakai -- Structure and low-lying states of the [symbol]He exotic nucleus via direct reactions on proton / V. Lapoux et al. -- Shell gap below [symbol]Sn based on the excited states in [symbol]Cd and [symbol]In / M. Górska -- Heavy neutron-rich nuclei produced in the fragmentation of a [symbol]Pb beam / Zs. Podolyák et al. -- Breakup and incomplete fusion in reactions of weakly-bound nuclei / D.J. Hinde et al. -- Excited states of [symbol]B and [symbol]He and their cluster aspect / Y. Kanada-En'yo et al. -- Nuclear reactions with weakly-bound systems: the treatment of the continuum / C. H. Dasso, A. Vitturi -- Dynamic evolution of three-body decaying resonances / A. S. Jensen et al. -- Prerainbow oscillations in [symbol]He scattering from the Hoyle state of [symbol]C and alpha particle condensation / S. Ohkubo, Y. Hirabayashi -- Angular dispersion behavior in heavy ion elastic scattering / Q. Wang et al. -- Microscopic optical potential in relativistic approach / Z.Yu. Ma et al. -- Exotic nuclei studied in direct reactions at low momentum transfer - recent results and future perspectives at fair / P. Egelhof -- Isotopic temperatures and symmetry energy in spectator fragmentation / M. De Napoli et al. -- Multi-channel algebraic scattering theory and the structure of exotic compound nuclei / K. Amos et al. -- Results for the first feasibility study for the EXL project at the experimental storage ring at GSI / N. Kalantar-Nayestanaki et al. -- Coulomb excitation of ISOLDE neutron-rich beams along the Z = 28 chain / P. Van Duppen -- The gamma decay of the pygmy resonance far from stability and the GDR at finite temperature / G. Benzoni et al

  5. Simulation of the effects of aerosol on mixed-phase orographic clouds using the WRF model with a detailed bin microphysics scheme

    NASA Astrophysics Data System (ADS)

    Xiao, Hui; Yin, Yan; Jin, Lianji; Chen, Qian; Chen, Jinghua

    2015-08-01

    The Weather Research Forecast (WRF) mesoscale model coupled with a detailed bin microphysics scheme is used to investigate the impact of aerosol particles serving as cloud condensation nuclei and ice nuclei on orographic clouds and precipitation. A mixed-phase orographic cloud developed under two scenarios of aerosol (a typical continental background and a relatively polluted urban condition) and ice nuclei over an idealized mountain is simulated. The results show that, when the initial aerosol condition is changed from the relatively clean case to the polluted scenario, more droplets are activated, leading to a delay in precipitation, but the precipitation amount over the terrain is increased by about 10%. A detailed analysis of the microphysical processes indicates that ice-phase particles play an important role in cloud development, and their contribution to precipitation becomes more important with increasing aerosol particle concentrations. The growth of ice-phase particles through riming and Wegener-Bergeron-Findeisen regime is more effective under more polluted conditions, mainly due to the increased number of droplets with a diameter of 10-30 µm. Sensitivity tests also show that a tenfold increase in the concentration of ice crystals formed from ice nucleation leads to about 7% increase in precipitation, and the sensitivity of the precipitation to changes in the concentration and size distribution of aerosol particles is becoming less pronounced when the concentration of ice crystals is also increased.

  6. Where on Earth can we observe pristine aerosol?

    NASA Astrophysics Data System (ADS)

    Hamilton, Douglas; Carslaw, Ken; Spracklen, Dominick; Lee, Lindsay; Pringle, Kirsty; Reddington, Carly

    2014-05-01

    To understand how sensitive the climate is to greenhouse gas and aerosol emissions it is important to define the baseline from which the aerosol forcings are calculated [Carslaw et al., 2013]; but if no regions in the world are anthropogenically unaltered, where on Earth can we observe and learn about the behaviour of pristine environments? This question is relevant to both future modelling and long-term observational studies in climate science. Identification of such regions is also important if we are to fully understand climate response to natural aerosol changes [Spracklen and Rap, 2013]. Here we use a combination of model simulations and statistical emulation of the Global Model of Aerosol Processes (GLOMAP) to identify regions which are most pristine in today's atmosphere. The simulations are used to identify present day (PD) regions which have daily mean cloud condensation nuclei (CCN) concentration similar to pre-industrial (PI) levels. The emulation of an ensemble of perturbed parameter runs [Lee et al., 2013] for the PI and PD allows a full Monte Carlo variance-based sensitivity analysis of CCN to 28 different parameters, covering both natural and anthropogenic emissions and their processes, which affect the uncertainty in CCN concentrations. We use this information to assess which regions exhibit little change in the sensitivity the 28 parameters between the PI and PD. Potentially pristine environments are defined based on where both the CCN number concentration and its sensitivity to the 28 parameters have remained constant through the industrial period. Our results indicate that the low to mid-latitude maritime southern hemisphere is the most pristine region in the PD atmosphere, especially during the austral summer. Other pristine regions include Alaska and Yukon, the Melanesian islands and the Antarctic Peninsula. Simulated anthropogenic influence on CCN has high seasonality in the southern hemisphere but low seasonality in the northern hemisphere

  7. Hygroscopic Properties of Aircraft Engine Exhaust Aerosol Produced From Traditional and Alternative Fuels

    NASA Astrophysics Data System (ADS)

    Moore, R.; Ziemba, L. D.; Beyersdorf, A. J.; Thornhill, K. L.; Winstead, E. L.; Crumeyrolle, S.; Chen, G.; Anderson, B. E.

    2012-12-01

    Aircraft emissions of greenhouse gases and aerosols constitute an important component of anthropogenic climate forcing, of which aerosol-cloud interactions remain poorly understood. It is currently thought that the ability of these aerosols to alter upper tropospheric cirrus cloud properties may produce radiative forcings many times larger than the impact of linear contrails alone and which may partially offset the impact of greenhouse gas emissions from aviation (Burkhardt and Karcher, Nature, 2011). Consequently, it is important to characterize the ability of these engine-emitted aerosol to act as cloud condensation nuclei (CCN) and ice nuclei (IN) to form clouds. While a number of studies in the literature have examined aerosol-cloud interactions for laboratory-generated soot or from aircraft engines burning traditional fuels, limited attention has been given to how switching to alternative jet fuels impacts the ability of engine-emitted aerosols to form clouds. The key to understanding these changes is the aerosol hygroscopicity. To address this need, the second NASA Alternative Aviation Fuel Experiment (AAFEX-II) was conducted in 2011 to examine the aerosol emissions from the NASA DC-8 under a variety of different engine power and fuel type conditions. Five fuel types were considered including traditional JP-8 fuel, synthetic Fischer-Tropsh (FT) fuel , sulfur-doped FT fuel (FTS) , hydrotreated renewable jet (HRJ) fuel, and a 50:50 blend of JP-8 with HRJ. Emissions were sampled from the DC-8 on the airport jetway at a distance of 145 meters downwind of the engine by a comprehensive suite of aerosol instrumentation that provided information on the aerosol concentration, size distribution, soot mass, and CCN activity. Concurrent measurements of carbon dioxide were used to account for plume dilution so that characteristic emissions indices could be determined. It is found that both engine power and fuel type significantly influence the hygroscopic properties of

  8. Resuspension of Aerosol Particles from Evaporated Rain Drops to the Coarse Mode

    NASA Astrophysics Data System (ADS)

    Wang, H.; Easter, R. C.; Ganguly, D.; Singh, B.; Rasch, P. J.

    2015-12-01

    Precipitation scavenging (i.e., wet removal) has long been recognized as one of the major removal processes for tropospheric aerosol particles, and the dominant one for accumulation-mode size particles. When rain drops evaporate, the aerosol material contained in drops is resuspended, and this process has received much less attention. Unlike the resuspension from evaporated cloud droplets, the aerosol particles resuspended from evaporated rain drops have much larger sizes than most of the aerosol particles that acted as cloud condensation nuclei (CCN), became cloud borne, and then were collected by rain drops, because each rain drop generally collects thousands of cloud droplets. Here we present some aspects of this resuspension process obtained from modeling studies. First, we investigate some details of the process using a simple drop-size resolved model of raindrop evaporation in sub-saturated air below cloud base. Using these results, we then investigate different treatments of this process in a global aerosol and climate model that employs a modal aerosol representation. Compared to the model's original treatment of this process in which rain-borne aerosol is resuspended to the mode that it came from with its original size, the new treatment that resuspends to the coarse mode produces notable reductions in global CCN concentrations, as well as sulfate, black carbon, and organic aerosol mass, because the resuspended aerosol particles have much shorter lifetimes due to their larger sizes. Somewhat surprisingly, there are also notable reductions in coarse-mode sea salt and mineral dust burdens. These species are resuspended to the coarse mode in both the original and new treatments, but these resuspended particles are fewer in number and larger in size in the new treatment. This finding highlights some issues of the modal aerosol treatment for coarse mode particles.

  9. 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}.

  10. Hygroscopicity of Early Earth and Titan Laboratory Aerosol Analogs

    NASA Astrophysics Data System (ADS)

    Hasenkopf, C. A.; Beaver, M. R.; Freedman, M. A.; Toon, O. B.; Tolbert, M. A.

    2009-12-01

    We have explored the ability of organic hazes, known to exist in the atmosphere of Titan and postulated to have existed in the Archean Earth atmosphere, to act as cloud condensation nuclei (CCN). These laboratory aerosol analogs are generated via UV-photolysis of early Earth and Titan analog gas mixtures and are designed to mimic the present day atmospheric conditions on Titan and the early Earth atmosphere before the rise of oxygen. Water uptake is observed to occur on the early Earth and Titan aerosol analogs at relative humidities of 80% - 90% via optical growth measurements using cavity ring-down aerosol extinction spectroscopy. We find the optical growth of these aerosols is similar to known slightly-soluble organic acids, such as phthalic and pyromellitic acids. On average, the optical growth of the early Earth analog is slightly larger than the Titan analog. In order to translate our measurements obtained in a subsaturated regime into the CCN ability of these particles, we rely on the hygroscopicity parameter κ, developed by Petters & Kreidenweis (2007). We retrieve κ = 0.17±0.03 and 0.06±0.01 for the early Earth and Titan analogs, respectively. This early Earth analog hygroscopicity value indicates that the aerosol could activate at reasonable water vapor supersaturations. We use previous aerosol mass spectrometry results to correlate the chemical structure of the two types of analog with their hygroscopicity. The hygroscopicity of the early Earth aerosol analog, coupled with the apparent lack of other good CCN during the Archean, helps explain the role of the organic haze in the indirect effect of clouds on the early Earth and indicates that it may have had a significant impact on the hydrological cycle.

  11. Hygroscopic Characteristics of Alkylaminium Carboxylate Aerosols.

    PubMed

    Gomez-Hernandez, Mario; McKeown, Megan; Secrest, Jeremiah; Marrero-Ortiz, Wilmarie; Lavi, Avi; Rudich, Yinon; Collins, Don R; Zhang, Renyi

    2016-03-01

    The hygroscopic growth factor (HGF) and cloud condensation nuclei (CCN) activity for a series of alkylaminium carboxylate aerosols have been measured using a hygroscopicity tandem differential mobility analyzer coupled to a condensation particle counter and a CCN counter. The particles, consisting of the mixtures of mono- (acetic, propanoic, p-toluic, and cis-pinonic acid) and dicarboxylic (oxalic, succinic, malic, adipic, and azelaic acid) acid with alkylamine (mono-, di-, and trimethylamines), represent those commonly found under diverse environmental conditions. The hygroscopicity parameter (κ) of the alkylaminium carboxylate aerosols was derived from the HGF and CCN results and theoretically calculated. The HGF at 90% RH is in the range of 1.3 to 1.8 for alkylaminium monocarboxylates and 1.1 to 2.2 for alkylaminium dicarboxylates, dependent on the molecular functionality (i.e., the carboxylic or OH functional group in organic acids and methyl substitution in alkylamines). The κ value for all alkylaminium carboxylates is in the range of 0.06-1.37 derived from the HGF measurements at 90% RH, 0.05-0.49 derived from the CCN measurements, and 0.22-0.66 theoretically calculated. The measured hygroscopicity of the alkylaminium carboxylates increases with decreasing acid to base ratio. The deliquescence point is apparent for several of the alkylaminium dicarboxylates but not for the alkylaminium monocarboxylates. Our results reveal that alkylaminium carboxylate aerosols exhibit distinct hygroscopic and deliquescent characteristics that are dependent on their molecular functionality, hence regulating their impacts on human health, air quality, and direct and indirect radiative forcing on climate.

  12. Superdeformed nuclei

    SciTech Connect

    Janssens, R.V.F.; Khoo, Teng Lek.

    1991-01-01

    This paper reviews the most recent advances in the understanding of the physics of superdeformed nuclei from the point of view of the experimentalists. It covers among other subjects the following topics: (1) the discovery of a new region of superdeformed nuclei near A=190, (2) the surprising result of the occurrence of bands with identical transition energies in neighboring superdeformed nuclei near A=150 and A=190, (3) the importance of octupole degrees of freedom at large deformation and (4) the properties associated with the feeding and the decay of superdeformed bands. The text presented hereafter will appear as a contribution to the Annual Review of Nuclear and Particle Science, Volume 41. 88 refs., 11 figs.

  13. Effects of aerosol from biomass burning on the global radiation budget

    NASA Technical Reports Server (NTRS)

    Penner, Joyce E.; Dickinson, Robert E.; O'Neill, Christine A.

    1992-01-01

    An analysis is made of the likely contribution of smoke particles from biomass burning to the global radiation balance. These particles act to reflect solar radiation directly; they also can act as cloud condensation nuclei, increasing the reflectivity of clouds. Together these effects, although uncertain, may add up globally to a cooling effect as large as 2 watts per square meter, comparable to the estimated contribution to sulfate aerosols. Anthropogenic increases of smoke emission thus may have helped weaken the net greenhouse warming from anthropogenic trace gases.

  14. Complex Coupling of Air Quality and Climate-Relevant Aerosols in a Chemistry-Aerosol Microphysics Model

    NASA Astrophysics Data System (ADS)

    Yoshioka, M.; Carslaw, K. S.; Reddington, C.; Mann, G.

    2013-12-01

    Controlling emissions of aerosols and their precursors to improve air quality will impact the climate through direct and indirect radiative forcing. We have investigated the impacts of changes in a range of aerosol and gas-phase emission fluxes and changes in temperature on air quality and climate change metrics using a global aerosol microphysics and chemistry model, GLOMAP. We investigate how the responses of PM2.5 and cloud condensation nuclei (CCN) are coupled, and how attempts to improve air quality could have inadvertent effects on CCN, clouds and climate. The parameter perturbations considered are a 5°C increase in global temperature, increased or decreased precursor emissions of anthropogenic SO2, NH3, and NOx, and biogenic monoterpenes, and increased or decreased primary emissions of organic and black carbon aerosols from wildfire, fossil fuel, and biofuel. To quantify the interactions, we define a new sensitivity metric in terms of the response of CCN divided by the response of PM in different regions. .Our results show that the coupled chemistry and aerosol processes cause complex responses that will make any co-benefit policy decision problematic. In particular, we show that reducing SO2 emissions effectively reduces surface-level PM2.5 over continental regions in summer when background PM2.5 is high, with a relatively small reduction in marine CCN (and hence indirect radiative cooling over ocean), which is beneficial for near-term climate. Reducing NOx emissions does not improve summertime air quality very effectively but leads to a relatively high reduction of marine CCN. Reducing NH3 emissions has moderate effects on both PM2.5 and CCN. These three species are strongly coupled chemically and microphysically and the effects of changing emissions of one species on mass and size distributions of aerosols are very complex and spatially and temporally variable. For example, reducing SO2 emissions leads to reductions in sulphate and ammonium mass

  15. Assessment of CCN based on size-resolved hygroscopicity data: Results from urban aerosol measurements in Nagoya, Japan

    NASA Astrophysics Data System (ADS)

    Kawana, K.; Nakayama, T.; Mochida, M.

    2012-12-01

    To assess the number concentrations and the proportion of cloud condensation nuclei (CCN) and the CCN activation diameter (dact) of urban aerosols based on size-resolved hygroscopicity, the atmospheric observation was performed for 10 days at an urban site of Nagoya, Japan in September 2009. The hygroscopic growth factor (HGF) distributions of aerosol particles at 85% RH were measured using a hygroscopicity tandem differential mobility analyzer (HTDMA) system, which consists of two differential mobility analyzers (DMAs) and a condensation particle counter (CPC). The proportion of CCN in the aerosol particles exiting the first DMA of the HTDMA was measured using a CCN counter and a CPC. The number concentrations of CCN (NCCN), the ratio of NCCN to the number concentrations of condensation nuclei (NCN), and dact were predicted from the observed HTDMA data based on k-köhler theory, and they were compared with measured values. Here, measured NCCN is that obtained from the number-size distribution of aerosol particles and the size-resolved NCCN/NCN. The measured dact was obtained from a curve fit to a CCN efficiency spectrum. The dact was predicted using different two methods. Whereas one of the methods to predict dact is based on the mean hygroscopic growth factor (gmean) at each diameter, the other accounts for activation of aerosol particles at each HGF bin. The NCCN and NCCN/NCN were predicted using the latter method only. The predicted NCCN and the predicted NCCN/NCN were, respectively, on average 19% and 15% lower than the measured values. The predicted dact were on average 8% higher than the measured values by both of the methods.

  16. Ground Based Remote Sensing of the First Aerosol Indirect Effect: An Update

    NASA Astrophysics Data System (ADS)

    Previdi, M.; Feingold, G.; Veron, D. E.; Eberhard, W. L.

    2003-12-01

    The first aerosol indirect effect can be defined as an increase in the shortwave albedo of clouds due to higher concentrations of atmospheric aerosol, whereby the aerosol acts as cloud condensation nuclei to produce increased cloud droplet concentrations and smaller, more reflective droplets. The current work is one step toward achieving a more complete understanding of the indirect effect, which will consequently allow for a better determination of how changes in cloud induced by aerosol may affect the radiation budget and thus the climate. We utilize a series of continuous ground-based measurements from the Southern Great Plains (SGP) Atmospheric Radiation Measurement (ARM) program to investigate the indirect effect. Days that exhibit ice-free, single layered, nonprecipitating clouds are analyzed, with the indirect effect quantified as the relative change in cloud droplet effective radius for a relative change in aerosol extinction (under conditions of equivalent cloud liquid water path). Several cases from the first six years of our analysis (1998-2003) are described here, and probable reasons for the differences in the cloud response to aerosol among the cases are discussed.

  17. The role of sulfate aerosol in the formation of cloudiness over the sea

    NASA Astrophysics Data System (ADS)

    Aloyan, A. E.; Yermakov, A. N.; Arutyunyan, V. O.

    2016-07-01

    We estimate the impact of sulfate aerosols on cloudiness formation over the sea in the middle troposphere and the involvement of these particles in the formation of polar stratospheric clouds (PSCs) in the lower stratosphere. The first of these problems is solved using a combined model of moist convection and the formation of cloudiness and sulfate aerosols in the troposphere and lower stratosphere over the sea, incorporating natural emissions of sulfur-containing compounds. We have found that a significant source of condensation nuclei in the troposphere is the photochemical transformation of biogenic dimethyl sulfide (in addition to NaCl). The results of numerical experiments indicate that the absence of sulfate aerosols hinders the cloudiness formation over the sea in the middle and upper troposphere. The problem of sulfate aerosol involvement in the formation of supercooled ternary solutions (STSs) (PSC Type Ib) in the lower stratosphere is solved using a mathematical model of global transport of multicomponent gas pollutants and aerosols in the atmosphere. Using the combined model, numerical experiments were performed for the winter season in both hemispheres. Sulfate aerosols were found to really participate in the formation of STS particles. Without their participation, the formation of STS particles in the lower stratosphere would be hindered. We present the results of numerical calculations and discuss the distribution of concentrations of gaseous nitric and sulfuric acids, as well as mass concentrations of these components in STS particles.

  18. Climate-relevant physical properties of molecular constituents for isoprene-derived secondary organic aerosol material

    NASA Astrophysics Data System (ADS)

    Upshur, M. A.; Strick, B. F.; McNeill, V. F.; Thomson, R. J.; Geiger, F. M.

    2014-10-01

    Secondary organic aerosol (SOA) particles, formed from gas-phase biogenic volatile organic compounds (BVOCs), contribute large uncertainties to the radiative forcing that is associated with aerosols in the climate system. Reactive uptake of surface-active organic oxidation products of BVOCs at the gas-aerosol interface can potentially decrease the overall aerosol surface tension and therefore influence their propensity to act as cloud condensation nuclei (CCN). Here, we synthesize and measure some climate-relevant physical properties of SOA particle constituents consisting of the isoprene oxidation products α-, δ-, and cis- and trans-β-IEPOX (isoprene epoxide), as well as syn- and anti-2-methyltetraol. Following viscosity measurements, we use octanol-water partition coefficients to quantify the relative hydrophobicity of the oxidation products while dynamic surface tension measurements indicate that aqueous solutions of α- and trans-β-IEPOX exhibit significant surface tension depression. We hypothesize that the surface activity of these compounds may enhance aerosol CCN activity, and that trans-β-IEPOX may be highly relevant for surface chemistry of aerosol particles relative to other IEPOX isomers.

  19. Variations in hygroscopic growth of sub- and super-micron sea spray aerosols during a phytoplankton bloom

    NASA Astrophysics Data System (ADS)

    Forestieri, S.; Jayarathne, T. S.; Stone, E. A.; Laskina, O.; Grassian, V. H.; Lee, C.; Sultana, C. M.; Moore, K.; Cornwell, G.; Novak, G.; Bertram, T. H.; Prather, K. A.; Cappa, C. D.

    2014-12-01

    Marine sea spray aerosols (SSA) make up an important portion of natural aerosols (prior to anthropogenic influence) and are therefore important in establishing the baseline for