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Sample records for aerosol condensation nuclei

  1. Primary Biological Aerosol as Cloud Condensation Nuclei

    NASA Astrophysics Data System (ADS)

    Pope, Francis; Griffiths, Paul; Herzog, Michael; Kalberer, Markus

    2013-04-01

    Primary biological aerosols (PBAs) represent a significant fraction of the total atmospheric aerosol mass burden. The low number density of PBA precludes a significant direct effect on the radiative budget of the Earth. However, the large particle size of PBA should allow them to have a significant indirect radiative effect on cloud processes if they are wettable. In particular, PBA may preferentially activate as cloud condensation nuclei (CCN) when compared to the smaller background aerosol. This effect will be most pronounced under pristine conditions where the background aerosol concentrations are small and of low hygroscopicity. Recent measurements of high PBA concentration within the Amazon (Huffman et al. 2012) suggest that this region may be particularly important for PBA-cloud interactions, and hence a potential feedback between the atmosphere and biosphere could be established (Pöschl et al. 2010). This study investigates the ability of primary biological aerosol (PBA) to influence cloud formation and precipitation dynamics. In particular, pollen grains and fungal spores have been studied using a combined laboratory and modelling approach. The laboratory studies assessed the hygroscopicity, wettability and activation of the particles. The model output data suggests that under certain atmospheric conditions the activation of PBA can significantly interfere with the activation of the fine aerosol mode thus changing cloud dynamics. This work expands upon our previously published results on pollen activation (Pope 2010, Griffiths et al. 2012). References Huffman et al. (2012) 12, 11997. doi:10.5194/acp-12-11997-2012 Pöschl et al. (2010) Science. 329(5998), 1513. doi:10.1126/science.1191056 Pope (2010) Environ. Res. Lett. 5, 004015. doi:10.1088/1748-9326/5/4/044015 Griffiths et al. (2012) Atmos. Sci. Lett. 13(4), 289. doi:10.1002/asl.397

  2. Organic Aerosols as Cloud Condensation Nuclei

    NASA Astrophysics Data System (ADS)

    Hudson, J. G.

    2002-05-01

    The large organic component of the atmospheric aerosol contributes to both natural and anthropogenic cloud condensation nuclei (CCN). Moreover, some organic substances may reduce droplet surface tension (Facchini et al. 1999), while others may be partially soluble (Laaksonen et al. 1998), and others may inhibit water condensation. The interaction of organics with water need to be understood in order to better understand the indirect aerosol effect. Therefore, laboratory CCN spectral measurements of organic aerosols are presented. These are measurements of the critical supersaturation (Sc), the supersaturation needed to produce an activated cloud droplet, as a function of the size of the organic particles. Substances include sodium lauryl (dodecyl) sulfate, oxalic, adipic, pinonic, hexadecanedioic, glutaric, stearic, succinic, phthalic, and benzoic acids. These size-Sc relationships are compared with theoretical and measured size-Sc relationships of common inorganic compounds (e.g., NaCl, KI, ammonium and calcium sulfate). Unlike most inorganics some organics display variations in solubility per unit mass as a function of particle size. Those showing relatively greater solubility at smaller sizes may be attributable to surface tension reduction, which is greater for less water dilution, as is the case for smaller particles, which are less diluted at the critical sizes. This was the case for sodium dodecyl sulfate, which does reduce surface tension. Relatively greater solubility for larger particles may be caused by greater dissolution at the higher dilutions that occur with larger particles; this is partial solubility. Measurements are also presented of internal mixtures of various organic and inorganic substances. These measurements were done with two CCN spectrometers (Hudson 1989) operating simultaneously. These two instruments usually displayed similar results in spite of the fact that they have different flow rates and supersaturation profiles. The degree of

  3. Global cloud condensation nuclei influenced by carbonaceous combustion aerosol

    NASA Astrophysics Data System (ADS)

    Spracklen, D. V.; Carslaw, K. S.; Pöschl, U.; Rap, A.; Forster, P. M.

    2011-03-01

    Black carbon in carbonaceous combustion aerosol warms the climate by absorbing solar radiation, meaning reductions in black carbon emissions are often perceived as an attractive global warming mitigation option. However, carbonaceous combustion aerosol can also act as cloud condensation nuclei (particles upon which cloud drops form) so they also cool the climate by increasing cloud albedo. The net radiative effect of carbonaceous combustion aerosol is uncertain because their contribution to cloud drops has not been evaluated on the global scale. By combining extensive observations of cloud condensation nuclei concentrations and a global aerosol model, we show that carbonaceous combustion aerosol accounts for more than half of global cloud condensation nuclei. The evaluated model predicts that wildfire and pollution (fossil fuel and biofuel) carbonaceous combustion aerosol causes a global mean aerosol indirect effect of -0.34 W m-2 due to changes in cloud albedo, with pollution sources alone causing a global mean aerosol indirect effect of -0.23 W m-2. The small size of carbonaceous combustion particles from pollution sources means that whilst they account for only one-third of the emitted mass from these sources they cause two-thirds of the cloud albedo indirect effect that is due to carbonaceous combustion aerosol. This cooling effect must be accounted for to ensure that black carbon emissions controls that reduce the high number concentrations of small pollution particles have the desired net effect on climate.

  4. 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.

  5. 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.

  6. Global cloud condensation nuclei influenced by carbonaceous combustion aerosol

    NASA Astrophysics Data System (ADS)

    Spracklen, D. V.; Carslaw, K. S.; Pöschl, U.; Rap, A.; Forster, P. M.

    2011-09-01

    Black carbon in carbonaceous combustion aerosol warms the climate by absorbing solar radiation, meaning reductions in black carbon emissions are often perceived as an attractive global warming mitigation option. However, carbonaceous combustion aerosol can also act as cloud condensation nuclei (CCN) so they also cool the climate by increasing cloud albedo. The net radiative effect of carbonaceous combustion aerosol is uncertain because their contribution to CCN has not been evaluated on the global scale. By combining extensive observations of CCN concentrations with the GLOMAP global aerosol model, we find that the model is biased low (normalised mean bias = -77 %) unless carbonaceous combustion aerosol act as CCN. We show that carbonaceous combustion aerosol accounts for more than half (52-64 %) of global CCN with the range due to uncertainty in the emitted size distribution of carbonaceous combustion particles. The model predicts that wildfire and pollution (fossil fuel and biofuel) carbonaceous combustion aerosol causes a global mean cloud albedo aerosol indirect effect of -0.34 W m-2, with stronger cooling if we assume smaller particle emission size. We calculate that carbonaceous combustion aerosol from pollution sources cause a global mean aerosol indirect effect of -0.23 W m-2. The small size of carbonaceous combustion particles from fossil fuel sources means that whilst pollution sources account for only one-third of the emitted mass they cause two-thirds of the cloud albedo aerosol indirect effect that is due to carbonaceous combustion aerosol. This cooling effect must be accounted for, along with other cloud effects not studied here, to ensure that black carbon emissions controls that reduce the high number concentrations of fossil fuel particles have the desired net effect on climate.

  7. Cloud condensation nuclei closure study on summer arctic aerosol

    NASA Astrophysics Data System (ADS)

    Martin, M.; Chang, R. Y.-W.; Sierau, B.; Sjogren, S.; Swietlicki, E.; Abbatt, J. P. D.; Leck, C.; Lohmann, U.

    2011-11-01

    We present an aerosol - cloud condensation nuclei (CCN) closure study on summer high Arctic aerosol based on measurements that were carried out in 2008 during the Arctic Summer Cloud Ocean Study (ASCOS) on board the Swedish ice breaker Oden. The data presented here were collected during a three-week time period in the pack ice (>85° N) when the icebreaker Oden was moored to an ice floe and drifted passively during the most biological active period into autumn freeze up conditions. CCN number concentrations were obtained using two CCN counters measuring at different supersaturations. The directly measured CCN number concentration was then compared with a CCN number concentration calculated using both bulk aerosol mass composition data from an aerosol mass spectrometer (AMS) and aerosol number size distributions obtained from a differential mobility particle sizer, assuming κ-Köhler theory, surface tension of water and an internally mixed aerosol. The last assumption was supported by measurements made with a hygroscopic tandem differential mobility analyzer (HTDMA) for particles >70 nm. For the two highest measured supersaturations, 0.73 and 0.41%, closure could not be achieved with the investigated settings concerning hygroscopicity and density. The calculated CCN number concentration was always higher than the measured one for those two supersaturations. This might be caused by a relative larger insoluble organic mass fraction of the smaller particles that activate at these supersaturations, which are thus less good CCN than the larger particles. On average, 36% of the mass measured with the AMS was organic mass. At 0.20, 0.15 and 0.10% supersaturation, closure could be achieved with different combinations of hygroscopic parameters and densities within the uncertainty range of the fit. The best agreement of the calculated CCN number concentration with the observed one was achieved when the organic fraction of the aerosol was treated as nearly water insoluble

  8. 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.

  9. 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.

  10. 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.

  11. Cloud condensation nuclei activity of aliphatic amine secondary aerosol

    Technology Transfer Automated Retrieval System (TEKTRAN)

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

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

    NASA Technical Reports Server (NTRS)

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

    2007-01-01

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

  13. 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

    2016-01-01

    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

  14. 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.

  15. 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

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

    NASA Astrophysics Data System (ADS)

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

    2011-10-01

    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.

  17. Atmospheric organic and bio-aerosols as cloud condensation nuclei (CCN): A review

    NASA Astrophysics Data System (ADS)

    Sun, Jiming; Ariya, Parisa A.

    Organic substances have been recognized as active cloud condensation and ice formation nuclei for several decades. In some regions of the world, these organic compounds (OC) consist predominantly of suspended matter mass, which can have local (e.g. toxicity, health hazards) and global (e.g. climate change) impacts. However, due to the complexity of their chemical nature, the significance of organic molecules in driving physical and chemical atmospheric processes is still very uncertain and poorly understood. The aim of this review paper is to assess the current state of knowledge regarding the role of organic aerosols (including bioaerosols) as cloud condensation nuclei (CCN), as well as to compare the existing theoretical and experimental data. It seems that classical Kohler theory does not adequately describe the hygroscopic behaviour of predominantly identified organic CCN such as pure dicarboxylic acid particles. Factors such as surface tension, impurities, volatility, morphology, contact angle, deliquescence, and the oxidation process should be considered in the theoretical prediction of the CCN ability of OC and the interpretation of experimental results. Major identified constituents of organic CCN, their main sources and their CCN properties will be herein reviewed. We will also discuss areas of uncertainty and expose key issues deserving of future research.

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

    PubMed

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

    2011-10-01

    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.

  20. Aerosol and cloud condensation nuclei formation at Mt. Kleiner Feldberg, Germany

    NASA Astrophysics Data System (ADS)

    Kohl, R.; Bonn, B.; Bourtsoukidis, S.; Wex, H.; Stratmann, F.; Bingemer, H.; Haunold, W.; Jacobi, S.

    2012-04-01

    New particle formation in number and mass is a quite ubiquous phenomenon in the atmospheric boundary layer. However, different locations provide different mechanisms for the initial particle production steps. Investigating the formation aims usually in explaining two aspects, the initial formation process and the contribution to cloud condensation nuclei production. In this study we focus on the latter. Once these particles are formed they grow further on until they reach cloud effective sizes. This is the size, where those particles can affect local climate via the indirect aerosol effect. This study deals with the processes mentioned at Mt. Kleiner Feldberg (810 m a.s.l.) about 50 km northwest of Frankfurt activation diameters. We have been determined using a CCN-counter (DMT, Boulder, U.S.) [Roberts and Nenes, 2005] and a SMPS (TSI 3936) with a long DMA (TSI 3081) and a UCPC (TSI 3025A). Particles were assumed to be equal in chemical composition since the vast majority of particles were smaller than 300 nm in diameter, i.e. secondary of nature. Therefore, measured CCN concentrations were intercompared with section wise integrated particle number concentrations starting at the largest size towards the smaller ones. The best match of integrated and CCN concentration was assumed to be the activation diameter (Dp,active). With this set-up the activation diameters were determined for five supersaturations (0.1, 0.2 0.3, 0.4 and 0.6%) during a two weeks period. This resulted in the expected detcrease in activation size with increasing supersaturation from about 130±10 nm at 0.1% to 70±5 nm at 0.6% supersaturation. The empirically fitted kappa-value [Petters and Kreidenweis, 2007] was obtained as 0.16±0.03 indicating aerosols of lower water-solubility. Second, measurements of ice nuclei [Klein et al., 2010] were conducted once per day during the same time period, which indicate that IN concentrations, were about one per mill of the CCN. Interestingly the cross

  1. 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%.

  2. 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.

  3. Inferring ammonium and sulfate aerosol concentrations using laser particle counters and condensation nuclei counters at summit, Greenland

    SciTech Connect

    Kuhns, H.; Davidson, C.; Bergin, M.

    1995-12-31

    Atmospheric measurements have been conducted in central Greenland over the last 10 years in connection with ice core research. While the primary objective of this research is to facilitate the quantitative interpretation of ice cores, interesting findings are being made in the field of Arctic air chemistry. In recent years, aerosol filters were run simultaneously with laser particle counters (LPC`s) and condensation nuclei counters (CNC`s). The LPC`s used in the this study count particles with diameters greater than 0.5 {mu}m, while the CNC`s count particles larger than approximately 0.01 {mu}m. Results from summertime aerosol sampling at Summit, Greenland are presented from the 1994 field season. Excellent agreement is observed between LPC data and particulate ammonium and sulfate. The correlation between ammonium and LPC data is r=0.88. Of all of the ionic species measured on the filters, the CNC results are in best agreement with MSA. The correlation for CNC and MSA is r=0.58. The relationship between the real-time particle sensor data and the aerosol chemistry has significant implications. The link between MSA and CNC supports the theory that marine biological activity enhances the production of cloud condensation nuclei. Also, this technique shows promise for remote sensing applications since once calibrated, the real time particle count data could be used to infer high temporal resolution aerosol chemistry.

  4. Impact of new particle formation on the concentrations of aerosol number and cloud condensation nuclei around Beijing

    SciTech Connect

    Matsui, H.; Koike, Makoto; Kondo, Yutaka; Takegawa, Nobuyuki; Wiedensohler, A.; Fast, Jerome D.; Zaveri, Rahul A.

    2011-10-13

    New particle formation (NPF) is one of the most important processes in controlling the concentrations of aerosol number (condensation nuclei, CN) and cloud condensation nuclei (CCN) in the atmosphere. In this study, we introduced a new aerosol model representation with 20 size bins between 1 nm and 10 {mu}m and activation-type and kinetic nucleation parameterizations into the WRF-chem model (called NPF-explicit WRF-chem). Model calculations were conducted in the Beijing region in China for the periods during the CARE-Beijing 2006 campaign conducted in August and September 2006. Model calculations successfully reproduced the timing of NPF and no-NPF days in the measurements (21 of 26 days). Model calculations also reproduced the subsequent rapid growth of new particles with a time scale of half a day. These results suggest that once a reasonable nucleation rate at a diameter of 1 nm is given, explicit calculations of condensation and coagulation processes can reproduce the clear contrast between NPF and no-NPF days as well as further growth up to several tens nanometers. With this reasonable representation of the NPF process, we show that NPF contributed 20-30% of CN concentrations (> 10 nm in diameter) in and around Beijing on average. We also show that NPF increases CCN concentrations at higher supersaturations (S > 0.2%), while it decreases them at lower supersaturations (S < 0.1%). This is likely because NPF suppresses the increases in both the size and hygroscopicity of pre-existing particles through the competition of condensable gases between new particles and pre-existing particles. Sensitivity calculations show that a reduction of primary aerosol emissions, such as black carbon (BC), would not necessarily decrease CCN concentrations because of an increase in NPF. Sensitivity calculations also suggest that the reduction ratio of primary aerosol and SO2 emissions will be key in enhancing or damping the BC mitigation effect.

  5. 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

  6. North American and Asian aerosols over the eastern Pacific Ocean and their role in regulating cloud condensation nuclei

    NASA Astrophysics Data System (ADS)

    Roberts, G.; Mauger, G.; Hadley, O.; Ramanathan, V.

    2006-07-01

    Measurements of aerosol and cloud properties in the Eastern Pacific Ocean were taken during an airborne experiment on the University of Wyoming's King Air during April 2004 as part of the Cloud Indirect Forcing Experiment (CIFEX). We observed a wide variety of aerosols, including those of long-range transport from Asia, clean marine boundary layer, and North American emissions. These aerosols, classified by their size distribution and history, were found in stratified layers between 500 to 7500 m above sea level and thicknesses from 100 to 3000 m. A comparison of the aerosol size distributions to measurements of cloud condensation nuclei (CCN) provides insight to the CCN activity of the different aerosol types. The overall ratio of measured to predicted CCN concentration (NCCN) is 0.56 ± 0.41 with a relationship of NCCN,measured = NCCN,predicted0.846±0.002 for 23 research flights and 1884 comparisons. Such a relationship does not accurately describe a CCN closure; however, it is consistent with our measurements that high CCN concentrations are more influenced by anthropogenic sources, which are less CCN active. While other CCN closures have obtained results closer to the expected 1:1 relationship, the different aerosol types (and presumably differences in aerosol chemistry) are responsible for the discrepancy. The measured NCCN at 0.3% supersaturation (Sc) ranged from 20 cm-3 (pristine) to 350 cm-3 (anthropogenic) with an average of 106 ± 54 cm-3 over the experiment. The inferred supersaturation in the clouds sampled during this experiment is ˜0.3%. CCN concentrations of cloud-processed aerosol were well predicted using an ammonium sulfate approximation for Sc ≤ 0.4%. Predicted NCCN for other aerosol types (i.e., Asian and North American aerosols) were high compared to measured values indicating a less CCN active aerosol. This study highlights the importance of chemical effects on CCN measurements and introduces a CCN activation index as a method of

  7. Relations Between Cloud Condensation Nuclei And Aerosol Optical Properties Relevant to Remote Sensing: Airborne Measurements in Biomass Burning, Pollution and Dust Aerosol Over North America

    NASA Astrophysics Data System (ADS)

    Shinozuka, Y.; Clarke, A.; Howell, S.; Kapustin, V.; McNaughton, C.; Zhou, J.; Decarlo, P.; Jimenez, J.; Roberts, G.; Tomlinson, J.; Collins, D.

    2008-12-01

    Remote sensing of the concentration of cloud condensation nuclei (CCN) would help investigate the indirect effect of tropospheric aerosols on clouds and climate. In order to assess its feasibility, this paper evaluates the spectral-based retrieval technique for aerosol number and seeks one for aerosol solubility, using in-situ aircraft measurements of aerosol size distribution, chemical composition, hygroscopicity, CCN activity and optical properties. Our statistical analysis reveals that the CCN concentration over Mexico can be optically determined to a relative error of <20%, smaller than that for the mainland US and the surrounding oceans (~a factor of 2). Mexico's advantage is four-fold. Firstly, many particles originating from the lightly regulated industrial combustion and biomass burning are large enough to significantly affect light extinction, elevating the correlation between extinction and CCN number in absence of substantial dust. Secondly, the generally low ambient humidity near the major aerosol sources limits the error in the estimated response of particle extinction to humidity changes. Thirdly, because many CCN contain black carbon, light absorption also provides a measure of the CCN concentration. Fourthly, the organic fraction of volatile mass of submicron particles (OMF) is anti-correlated with the wavelength dependence of extinction due to preferential anion uptake by coarse dust, which provides a potential tool for remote-sensing OMF and the particle solubility.

  8. 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

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

    NASA Astrophysics Data System (ADS)

    Petters, Sarah Suda; Petters, Markus Dirk

    2016-02-01

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

  10. Separating Cloud Forming Nuclei from Interstitial Aerosol

    SciTech Connect

    Kulkarni, Gourihar R.

    2012-09-12

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

  11. Contribution of carbonaceous material to cloud condensation nuclei concentrations in European background (Mt. Sonnblick) and urban (Vienna) aerosols

    NASA Astrophysics Data System (ADS)

    Hitzenberger, R.; Berner, A.; Giebl, H.; Kromp, R.; Larson, S. M.; Rouc, A.; Koch, A.; Marischka, S.; Puxbaum, H.

    During four intensive measurement campaigns (two on Mt. Sonnblick, European background aerosol, and two in Vienna, urban aerosol), cloud condensation nuclei (CCN) were measured at supersaturations of 0.5%. Impactor measurements of the mass size distribution in the size range 0.1-10 μm were performed and later analyzed for Cl -, NO -3, SO 2-4, Na +, NH +4, K +, Ca 2+ and Mg 2+ by ion chromatography, for total carbon (TC) using a combustion method, and for black carbon (BC) by an optical method (integrating sphere). Organic carbon (OC) was defined as the difference between TC (minus carbonate carbon) and BC. At all sites, the mass fraction of BC in the submicron aerosol was comparable (4-5%). CCN concentrations on Mt. Sonnblick were found to be 10-30% of those measured in Vienna, although high Mt. Sonnblick concentrations were comparable to low Vienna concentrations (around 800 cm -3). The contribution of organic material was estimated from the mass concentrations of the chemical species sampled on the impactor stage with the lowest cut point (0.1-0.215 μm aerodynamic equivalent diameter). On Mt. Sonnblick, TC material contributed 11% to the total mass in fall 1995, and 67% in summer 1996, while the OC fraction was 6 and 61%. The combined electrolytes and mineral material contributed 18 and 16% in fall and summer. During the Vienna spring campaign, the contributions of OC and electrolytes to the total mass concentration in this size range were 48 and 36%, respectively.

  12. 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.

  13. 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.

  14. 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

  15. 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

  16. 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.

  17. Characteristics of dimethylsulfide, ozone, aerosols, and cloud condensation nuclei in air masses over the northwestern Pacific Ocean

    NASA Astrophysics Data System (ADS)

    Nagao, Ippei; Matsumoto, Kiyoshi; Tanaka, Hiroshi

    1999-05-01

    Long-term measurements of several trace gases and aerosols were carried out from December 1994 to October 1996 at Ogasawara Hahajima Island over the northwestern Pacific Ocean. The continental impact on the concentrations of sulfur compounds, ozone (O3), and cloud condensation nuclei (CCN) was estimated on the basis of the classification of air mass into seven types by isentropic trajectory analysis. From May to October, the air mass originating from the central North Pacific Ocean is predominant and regarded as the clean marine air for the concentrations of sulfur compounds and CCN. From the results of the molar ratio of methane sulfonic acid to non-sea-salt sulfate (NSS) and the positive correlation between dimethylsulfide (DMS) and CCN in this air mass it can be concluded that DMS largely contributes to the production of NSS and CCN. On the other hand, continental and anthropogenic substances are preferably transported to the northwestern Pacific Ocean by the predominant continental air mass from November to March. The enhancement of concentrations by the outflow from the Asian continent are estimated by a factor of 2.8 for O3, 3.9 for SO2, 3.5 for CCN activated at 0.5% supersaturation (0.5% CCN), 4.7 for 1.0% CCN, and 5.5 for NSS. Moreover, the CCN supersaturation spectra are also affected by the continental substances resulting in factor 2 of enhancement of cloud droplet number concentration. The diurnal variations of DMS and O3 for each air mass show a pattern of daytime minimum and nighttime maximum, which are typically found in remote ocean, even though those amplitudes are different for each air mass. Consequently, it can be concluded that the influence of nitric oxides (NOx) for the daytime O3 production and nitrate (NO3) radical for the nighttime oxidation of DMS are small even in the continental air mass.

  18. 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.

  19. Cloud condensation nuclei near marine stratus

    NASA Technical Reports Server (NTRS)

    Hudson, James G.; Frisbie, Paul R.

    1991-01-01

    Extensive airborne measurements of cloud condensation nucleus (CCN) spectra and concentrations of total particles, or condensation nuclei (CN), below, in, and above the stratus cloud decks off the southern California coast point to important aerosol-cloud interactions. Consistently low CCN concentrations below cloud appear to be due to cloud scavenging processes which include Brownian coagulation, nucleation, coalescence, and drizzle. The higher CCN and CN concentrations above cloud are associated with ambient ozone concentrations which suggest a link with continental, probably anthropogenic, sources, even at distances of 500 km from the California coast.

  20. A statistical description of the evolution of cloud condensation nuclei activity during the heterogeneous oxidation of squalane and bis(2-ethylhexyl) sebacate aerosol by hydroxyl radicals.

    PubMed

    Harmon, Christopher W; Ruehl, Christopher R; Cappa, Christopher D; Wilson, Kevin R

    2013-06-28

    The heterogeneous reaction of hydroxyl radicals with chemically reduced organic aerosol comprised of either squalane or bis(2-ethylhexyl) sebacate are used as model systems to examine how cloud condensation nuclei (CCN) activity evolves with photochemical oxidation. Over the course of the reaction, the critical super-saturation evolves both by the formation of new oxygen functional groups and by changes in aerosol size through the formation of gas phase reaction products. A statistical model of the heterogeneous reaction reveals that it is the formation, volatilization, solubility, and surface activity of many generations of oxidation products that together control the average changes in aerosol hygroscopicity. The experimental observations and model demonstrate the importance of considering the underlying population or subpopulation of species within a particle and how they each uniquely contribute to the average hygroscopicity of a multi-component aerosol. To accurately predict changes in CCN activity upon oxidation requires a reduction in the surface tension of the activating droplet by a subpopulation of squalane reaction products. These results provide additional evidence that surface tension-concentration parameterizations based on macroscopic data should be modified for microscopic droplets.

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

    NASA Astrophysics Data System (ADS)

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

    2014-07-01

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

  2. 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.

  3. 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.

  4. 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.

  5. Cloud Condensation Nuclei in FIRE III

    NASA Technical Reports Server (NTRS)

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

    2002-01-01

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

  6. Pluvial Inhibition by Urban Cloud Condensation Nuclei

    NASA Astrophysics Data System (ADS)

    Hudson, J. G.; Yum, S. S.

    2002-05-01

    Cloud microphysics and sub-cloud aerosol measurements in urban and cleaner air masses showed the effects of anthropogenic air pollution. Cloud condensation nuclei (CCN) measurements in three different parts of the world displayed typical urban/clean air mass differences in concentrations. Near-simultaneous cloud droplet measurements (diameter < 50 micrometers) showed the higher concentrations and smaller sizes expected for higher CCN concentrations. The commensurate lower concentrations of large cloud droplets (30-50 micrometers) in urban air indicated that the higher CCN concentrations were responsible for the order(s) of magnitude lower drizzle drop (diameter > 50 micrometers) concentrations in the urban-influenced clouds. The similarity of the clean and urban- influenced cloud droplet spectra near cloud base suggested no differences in giant nuclei concentrations that have been suggested to be responsible for greater precipitation in cleaner clouds. This suppression of warm rain by higher CCN concentrations occurred hundreds of km from the urban sources. Similar effects were found for three different cloud types in these three field projects: 1) stratocumulus clouds in the eastern Atlantic (ASTEX); 2) small cumulus clouds in eastern Florida (SCMS); and small trade wind cumuli in the Indian Ocean (INDOEX). Comparisons of CCN and cloud droplet concentrations in the three projects showed a more-or-less linear relationship between CCN and cloud droplet concentrations. Comparisons of CCN and cloud droplet spectra showed that supersaturations were lower in the urban-influenced clouds due to greater competition for condensed water. This means that a smaller percentage of the higher urban CCN concentrations actually produced cloud droplets. However, the supersaturation suppression was smaller because droplet sizes were so reduced that many urban cloud droplets escaped detection. This underestimation of cloud droplet concentrations suggested a greater suppression of

  7. 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.

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

    NASA Astrophysics Data System (ADS)

    Stier, Philip

    2015-04-01

    Aerosol-cloud interactions are considered a key uncertainty in our understanding of climate change. Knowledge of the global abundance of aerosols suitable to act as cloud condensation nuclei 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. 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, important for studies of aerosol-cloud interactions. The findings suggest that multi-spectral vertically resolved remote sensing techniques, such as satellite-based high spectral resolution lidars, have a large potential for global monitoring of cloud condensation nuclei.

  9. 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.

  10. 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.

  11. 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.

  12. 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.

  13. 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.

  14. 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).

  15. 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.

  16. 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.

  17. Cloud condensation nuclei in Western Colorado: Observations and model predictions

    NASA Astrophysics Data System (ADS)

    Ward, Daniel Stewart

    Variations in the warm cloud-active portion of atmospheric aerosols, or cloud condensation nuclei (CCN), have been shown to impact cloud droplet number concentration and subsequently cloud and precipitation processes. This issue carries special significance in western Colorado where a significant portion of the region's water resources is supplied by precipitation from winter season, orographic clouds, which are particularly sensitive to variations in CCN. Temporal and spatial variations in CCN in western Colorado were investigated using a combination of observations and a new method for modeling CCN. As part of the Inhibition of Snowfall by Pollution Aerosols (ISPA-III) field campaign, total particle and CCN number concentration were measured for a 24-day period in Mesa Verde National Park, climatologically upwind of the San Juan Mountains. These data were combined with CCN observations from Storm Peak Lab (SPL) in northwestern Colorado and from the King Air platform, flying north to south along the Western Slope. Altogether, the sampled aerosols were characteristic of a rural continental environment and the cloud-active portion varied slowly in time, and little in space. Estimates of the is hygroscopicity parameter indicated consistently low aerosol hygroscopicity typical of organic aerosol species. The modeling approach included the addition of prognostic CCN to the Regional Atmospheric Modeling System (RAMS). The RAMS droplet activation scheme was altered using parcel model simulations to include variations in aerosol hygroscopicity, represented by K. Analysis of the parcel model output and a supplemental sensitivity study showed that model CCN will be sensitive to changes in aerosol hygroscopicity, but only for conditions of low supersaturation or small particle sizes. Aerosol number, size distribution median radius, and hygroscopicity (represented by the K parameter) in RAMS were constrained by nudging to forecasts of these quantities from the Weather

  18. 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.

  19. 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.

  20. 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.

  1. 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

  2. Cloud Condensation Nuclei in Fire-3

    NASA Technical Reports Server (NTRS)

    2000-01-01

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

  3. Concentrations of condensation nuclei in the vicinity of jetstream maxima

    NASA Technical Reports Server (NTRS)

    Cadle, R. D.; Shapiro, M. A.; Langer, G.

    1979-01-01

    Ozone and condensation nuclei were measured on March 29, 1977 (and March 30, GMT) from a Sabreliner in a frontal zone south of Denver, Colo. The ozone served as a tracer for stratospheric air and the condensation nuclei as a tracer for tropospheric air. Both the Langer condensation nucleus counter and the Rich-100 counter can be used to measure condensation nucleus concentrations in the vicinity of the tropopause. However, the former counter is more sensitive to low concentrations. The nuclei measured were found to be almost entirely larger than 0.005 micron in radius, consisting of thousands of molecules. The mesostructure of the ozone and condensation nucleus concentrations agreed well with a double structure of the frontal zone that became apparent from a detailed analysis of radiosonde data.

  4. Effect of secondary organic aerosol amount and condensational behavior on global aerosol size distributions

    NASA Astrophysics Data System (ADS)

    D'Andrea, S. D.; Häkkinen, S. A. K.; Westervelt, D. M.; Kuang, C.; Spracklen, D. V.; Riipinen, I.; Pierce, J. R.

    2013-05-01

    Recent research has shown that secondary organic aerosols (SOA) are major contributors to ultrafine particle growth to climatically relevant sizes, increasing global cloud condensation nuclei (CCN) concentrations within the continental boundary layer. Many models treat SOA solely as semivolatile, which leads to condensation of SOA proportional to the aerosol mass distribution; however, recent closure studies with field measurements show that a significant fraction of SOA condenses proportional to the aerosol surface area, which suggests a very low volatility. Additionally, while many global models contain only biogenic sources of SOA (with emissions generally 10-30 Tg yr-1), recent studies have shown a need for an additional source of SOA around 100 Tg yr-1 correlated with anthropogenic carbon monoxide (CO) emissions is required to match measurements. Here, we explore the significance of these two findings using the GEOS-Chem-TOMAS global aerosol microphysics model. The percent change in the number of particles of size Dp > 40 nm (N40) within the continental boundary layer between the surface-area-and massdistribution condensation schemes, both with the base biogenic SOA only, yielded a global increase of 8% but exceeds 100% in biogenically active regions. The percent change in N40 within the continental boundary layer between the base simulation (19 Tg yr-1) and the additional SOA (100 Tg yr-1) both using the surface area condensation scheme (very low volatility) yielded a global increase of 14%, and a global decrease in the number of particles of size Dp > 10 nm (N10) of 32%. These model simulations were compared to measured data from Hyytiälä, Finland and other global locations and confirmed a decrease in the model-measurement bias. Thus, treating SOA as very low volatile as well as including additional SOA correlated with anthropogenic CO emissions causes a significant global increase in the number of climatically relevant sized particles, and therefore we

  5. 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

  6. 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.

  7. 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

  8. Isovector pairing and quartet condensation in N=Z nuclei

    SciTech Connect

    Sandulescu, N.; Negrea, D.; Dukelsky, J.; Johnson, C. W.

    2012-11-20

    We introduce and study a quartet condensate model (QCM) to treat the isovector pairing correlations in N=Z nuclei, by conserving the particle number and the total spin and isospin in the ground state of such nuclei. For the calculations we choose different isovector pairing forces acting on spherical and axially deformed single particle states. The results show that the QCM model describes very well the isovector pairing correlations for nuclear systems with N=Z.

  9. 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.

  10. Observations of condensation nuclei in the 1987 airborne Antarctic ozone experiment

    NASA Technical Reports Server (NTRS)

    Wilson, J. C.; Smith, S. D.; Ferry, G. V.; Loewenstein, M.

    1988-01-01

    The condensation nucleus counter (CNC) flown of the NASA ER-2 in the Airborne Antarctic Ozone Experiment provides a measurement of the number mixing ratio of particles which can be grown by exposure to supersaturated n-butyl alcohol vapor to diameters of a few microns. Such particles are referred to as condensation nuclei (CN). The ER-2 CNC was calibrated with aerosols of known size and concentration and was found to provide an accurate measure of the number concentration of particles larger than about 0.02 micron. Since the number distribution of stratospheric aerosols is usually dominated by particles less than a few tenths of micron in diameter, the upper cutoff of the ER-2 CNC has not been determined experimentally. However, theory suggests that the sampling and counting efficiency should remain near one for particles as large as 1 micron in diameter. Thus, the CN mixing ratio is usually a good measure of the mixing ratio of submicron particles.

  11. Bose condensation of nuclei in heavy ion collisions.

    PubMed

    Tripathi, R K; Townsend, L W

    1994-07-01

    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.

  12. 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.

  13. 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.

  14. Rainforest aerosols as biogenic nuclei of clouds and precipitation in the Amazon.

    PubMed

    Pöschl, U; Martin, S T; Sinha, B; Chen, Q; Gunthe, S S; Huffman, J A; Borrmann, S; Farmer, D K; Garland, R M; Helas, G; Jimenez, J L; King, S M; Manzi, A; Mikhailov, E; Pauliquevis, T; Petters, M D; Prenni, A J; Roldin, P; Rose, D; Schneider, J; Su, H; Zorn, S R; Artaxo, P; Andreae, M O

    2010-09-17

    The Amazon is one of the few continental regions where atmospheric aerosol particles and their effects on climate are not dominated by anthropogenic sources. During the wet season, the ambient conditions approach those of the pristine pre-industrial era. We show that the fine submicrometer particles accounting for most cloud condensation nuclei are predominantly composed of secondary organic material formed by oxidation of gaseous biogenic precursors. Supermicrometer particles, which are relevant as ice nuclei, consist mostly of primary biological material directly released from rainforest biota. The Amazon Basin appears to be a biogeochemical reactor, in which the biosphere and atmospheric photochemistry produce nuclei for clouds and precipitation sustaining the hydrological cycle. The prevailing regime of aerosol-cloud interactions in this natural environment is distinctly different from polluted regions.

  15. 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.

  16. 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.

  17. Analysis of feedbacks between nucleation rate, survival probability and cloud condensation nuclei formation

    NASA Astrophysics Data System (ADS)

    Westervelt, D. M.; Pierce, J. R.; Adams, P. J.

    2014-06-01

    Aerosol nucleation is an important source of particle number in the atmosphere. However, in order to become cloud condensation nuclei (CCN), freshly nucleated particles must undergo significant condensational growth while avoiding coagulational scavenging. In an effort to quantify the contribution of nucleation to CCN, this work uses the GEOS-Chem-TOMAS global aerosol model to calculate changes in CCN concentrations against a broad range of nucleation rates and mechanisms. We then quantify the factors that control CCN formation from nucleation, including daily nucleation rates, growth rates, coagulation sinks, condensation sinks, survival probabilities, and CCN formation rates, in order to examine feedbacks that may limit growth of nucleated particles to CCN. Nucleation rate parameterizations tested in GEOS-Chem-TOMAS include ternary nucleation (with multiple tuning factors), activation nucleation (with two pre-factors), binary nucleation, and ion-mediated nucleation. We find that nucleation makes a significant contribution to boundary layer CCN(0.2%), but this contribution is only modestly sensitive to the choice of nucleation scheme, ranging from 49 to 78% increase in concentrations over a control simulation with no nucleation. Moreover, a two order-of-magnitude increase in the globally averaged nucleation rate (via changes to tuning factors) results in small changes (less than 10%) to global CCN(0.2%) concentrations. To explain this, we present a simple theory showing that survival probability has an exponentially decreasing dependence on the square of the condensation sink. This functional form stems from a negative correlation between condensation sink and growth rate and a positive correlation between condensation sink and coagulational scavenging. Conceptually, with a fixed condensable vapor budget (sulfuric acid and organics), any increase in CCN concentrations due to higher nucleation rates necessarily entails an increased aerosol surface area in the

  18. 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.

  19. 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

  20. 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.

  1. 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

  2. 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.

  3. The cloud condensation nuclei and ice nuclei effects on tropical anvil characteristics and water vapor of the tropical tropopause layer

    SciTech Connect

    Fan, Jiwen; Comstock, Jennifer M.; Ovchinnikov, Mikhail

    2010-11-10

    Cloud anvils from deep convective clouds are of great importance to the radiative energy budget and the aerosol impact on them is the least understood. Few studies examined the effects of both cloud condensation nuclei (CCN) and ice nuclei (IN) on anvil properties and water vapor content (WVC) in the Tropical Tropopause Layer (TTL). Using a 3-dimensional cloud-resolving model with size-resolved cloud microphysics, we focus on the CCN and IN effects on cloud anvil properties and WVC in the TTL. We find that cloud microphysical changes induced by CCN/IN play a very important role in determining cloud anvil area and WVC in the TTL, whether convection is enhanced or suppressed. Also, CCN effects on anvil microphysical properties, anvil size and lifetime are much more evident relative to IN. IN has little effect on convection, but can increase ice number and mass concentrations significantly under humid conditions. CCN in the PBL is found to have greater effects on convective strength and mid-tropospheric CCN has negligible effects on convection and cloud properties. Convective transport may only moisten the main convective outflow region but the cloud anvil size determines the WVC in the TTL domain. This study shows an important role of CCN in the lower-troposphere in modifying convection, the upper-level cloud properties. It also shows the effects of IN and the PBL CCN on the upper-level clouds depends on the humidity, resolving some contradictory results in past studies. 2

  4. Cold and transition season cloud condensation nuclei measurements in western Colorado

    NASA Astrophysics Data System (ADS)

    Ward, D. S.; Cotton, W. R.

    2011-05-01

    Recent studies have shown that orographic precipitation and the water resources that depend on it in the Colorado Rocky Mountains are sensitive to the variability of the region's aerosols, whether emitted locally or from distant sources. However, observations of cloud droplet nucleating aerosols in western Colorado, climatologically upwind of the Colorado Rocky Mountains, have been limited to a few studies at a single, northern site. To address this knowledge gap, atmospheric aerosols were sampled at a ground site in southwestern Colorado and in low-level north to south transects of the Colorado Western Slope as part of the Inhibition of Snowfall by Pollution Aerosols (ISPA-III) field campaign. Total particle and cloud condensation nuclei (CCN) number concentrations were measured for a 24-day period in Mesa Verde National Park, in September and October 2009. Regression analysis showed a positive relationship between mid-troposphere atmospheric pressure to the west of the site and the total particle count at the ground site, but no similar statistically significant relationship was found for the observed CCN. These data were supplemented with particle and CCN number concentration, as well as particle size distribution measurements collected aboard the King Air platform during December 2009. A CCN closure attempt was performed and suggested that the sampled aerosol may have had a low hygroscopicity that changed little with the large-scale wind direction. Together, the sampled aerosols from these field programs were characteristic of a rural continental environment with CCN number concentrations that varied slowly in time, and little in space along the Western Slope.

  5. Cold and transition season cloud condensation nuclei measurements in western Colorado

    NASA Astrophysics Data System (ADS)

    Ward, D. S.; Cotton, W. R.

    2010-11-01

    Recent research has shown that orographic precipitation and the water resources that depend on it in the Colorado Rocky Mountains are sensitive to the variability of the region's aerosols, whether emitted locally or from distant sources. However, observations of cloud-active aerosols in western Colorado, climatologically upwind of the Colorado Rocky Mountains, have been limited to a few studies at a single, northern site. To address this knowledge gap, atmospheric aerosols were sampled at a ground site in southwestern Colorado and in low-level north to south transects of the Colorado Western Slope as part of the Inhibition of Snowfall by Pollution Aerosols (ISPA-III) field campaign. Total particle and cloud condensation nuclei (CCN) number concentration were measured for a 24-day period in Mesa Verde National Park, climatologically upwind of the San Juan Mountains, in Sept. and Oct. 2009. Regression analysis showed a positive relationship between mid-troposphere atmospheric pressure to the west of the site and the total particle count at the ground site, but no similar statistically significant relationship for the observed CCN. These data were supplemented with particle and CCN number concentration, as well as particle size distribution measurements aboard the KingAir platform during December 2009. A CCN closure attempt was performed using the size distribution information and suggested that the sampled aerosol in general had low hygroscopicity that changed slightly with the large-scale wind direction. Together, the sampled aerosols from these field programs were characteristic of a rural continental environment with a cloud active portion that varied slowly in time, and little in space along the Western Slope.

  6. Effect of primary organic sea spray emissions on cloud condensation nuclei concentrations

    NASA Astrophysics Data System (ADS)

    Westervelt, D. M.; Moore, R. H.; Nenes, A.; Adams, P. J.

    2012-01-01

    This work estimates the primary marine organic aerosol global emission source and its impact on cloud condensation nuclei (CCN) concentrations by implementing an organic sea spray source function into a series of global aerosol simulations. The source function assumes that a fraction of the sea spray emissions, depending on the local chlorophyll concentration, is organic matter in place of sea salt. Effect on CCN concentrations (at 0.2% supersaturation) is modeled using the Two-Moment Aerosol Sectional (TOMAS) microphysics algorithm coupled to the GISS II-prime general circulation model. The presence of organics affects CCN activity in competing ways: by reducing the amount of solute available in the particle and decreasing surface tension of CCN. To model surfactant effects, surface tension depression data from seawater samples taken near the Georgia coast were applied as a function of carbon concentrations. A global marine organic aerosol emission rate of 17.7 Tg C yr-1 is estimated from the simulations. Marine organics exert a localized influence on CCN(0.2%) concentrations, decreasing regional concentrations by no more than 5% and by less than 0.5% over most of the globe, assuming direct replacement of sea salt aerosol with organic aerosol. The decrease in CCN concentrations results from the fact that the decrease in particle solute concentration outweighs the organic surfactant effects. The low sensitivity of CCN(0.2%) to the marine organic emissions is likely due to the small compositional changes: the mass fraction of OA in accumulation mode aerosol increases by only ~15% in a biologically active region of the Southern Ocean. To test the sensitivity to uncertainty in the sea spray emissions process, we relax the assumption that sea spray aerosol number and mass remain fixed and instead can add to sea spray emissions rather than replace existing sea salt. In these simulations, we find that marine organic aerosol can increase CCN by up to 50% in the Southern

  7. 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.

  8. 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.

  9. New particle formation events as a source for cloud condensation nuclei in an urban environment

    NASA Astrophysics Data System (ADS)

    Wonaschütz, Anna; Burkart, Julia; Wagner, Robert; Reischl, Georg; Steiner, Gerhard; Hitzenberger, Regina

    2014-05-01

    Nucleation and growth events have been observed in many remote, urban and rural environments. The new particles can contribute significantly to cloud condensation nuclei concentrations, after growing into the appropriate size range (Kerminen et al., 2012). Several studies have attempted to quantify this contribution (e.g. Asmi et al., 2011, Matsui et al., 2013), but only a limited number of them to date have used simultaneous measurements of CCN concentrations and particle size distributions for this purpose (e.g. Levin et al., 2012). In this study, a data set from an urban background station, consisting of 22 months of size distribution and 12 months of CCN concentration measurements (Burkart et al., 2011, Burkart et al., 2012) with 10 months of overlapping measurements is combined to explore the variability of CCN concentrations, their possible causes, and the contribution of nucleation and growth events to CCN concentrations. Consistent with observations in many other locations, nucleation and growth events occur on 30% of all days in spring and summer, on 11% of days in fall and on 4% of days in winter. This suggests a potentially large source of CCN from nucleation and growth events, particularly in the warm season. We acknowledge funding from FWF (Austrian Science Fund) P19515-N20 References: Asmi E., Kivekas, N., Kerminen, V. M., Komppula, M., Hyvarinen, A. P., Hatakka, J., Viisanen, Y., and Lihavainen, H.: Secondary new particle formation in Northern Finland Pallas site between the years 2000 and 2010, Atmos. Chem. Phys., 11, 12959-12972, doi: 10.5194/acp-11-12959-2011, 2011 Burkart J., Steiner, G., Reischl, G., and Hitzenberger, R.: Long-term study of cloud condensation nuclei (CCN) acticvation of the atmospheric aerosol in Vienna, Atmos. Environ., 45, 5751-5759, doi: 10.1016/j.atmosenv.2011.07.022, 2011. Burkart J., Hitzenberger, R., Reischl, G., Bauer, H., Leder, K., and Puxbaum, H.: Activation of "synthetic ambient" aerosols - relation to chemical

  10. 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.

  11. On the effect of dust particles on global cloud condensation nuclei and cloud droplet number

    NASA Astrophysics Data System (ADS)

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

    2011-12-01

    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.

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

    NASA Technical Reports Server (NTRS)

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

    2011-01-01

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

  13. Effect of primary organic sea spray emissions on cloud condensation nuclei concentrations

    NASA Astrophysics Data System (ADS)

    Westervelt, D. M.; Moore, R. H.; Nenes, A.; Adams, P. J.

    2011-02-01

    This work quantifies the primary marine organic aerosol global emission source and its impact on cloud condensation nuclei (CCN) concentrations by implementing an organic sea spray source function into a series of global aerosol simulations. The source function assumes that a fraction of the sea spray emissions, depending on the local chlorophyll concentration, is organic matter in place of NaCl. Effect on CCN concentrations (at 0.2% supersaturation) is modeled using the Two-Moment Aerosol Sectional (TOMAS) microphysics algorithm coupled to the GISS II-prime general circulation model. The presence of organics affects CCN activity in competing ways: by reducing the amount of solute available in the particle and decreasing surface tension of CCN. To model surfactant effects, surface tension depression data from seawater samples taken near the Georgia coast were applied as a function of carbon concentrations. A global marine organic aerosol emission rate of 17.7 Tg C yr-1 is estimated from the simulations. Marine organics exert a localized influence on CCN(0.2%) concentrations, decreasing regional concentrations by no more than 5% and by less than 0.5% over most of the globe. The decrease in CCN concentrations results from the fact that the decrease in particle solute concentration outweighs the organic surfactant effects. The low sensitivity of CCN(0.2%) to the marine organic emissions is likely due to the small compositional changes: the mass fraction of OA in accumulation mode aerosol increases by only 15% in a biologically active region of the Southern Ocean.

  14. 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.

  15. Closure Between Measured and Predicted Cloud Condensation Nuclei Concentration at Kanpur, Indo-Gangetic Basin

    NASA Astrophysics Data System (ADS)

    Bhattu, D.; Tripathi, S. N.

    2013-12-01

    Aerosols play a significant role in the Earth climate system directly by absorbing and scattering sunlight, and indirectly by acting as cloud condensation nuclei (CCN), ultimately affecting the cloud microphysical and radiative properties. To reduce the uncertainty involved in global radiative forcing assessment, there is a need to quantify the effect of chemical composition and mixing state on the hygroscopic growth of aerosols to understand their CCN activity. The role of soluble inorganics as a single component system in droplet activation is well understood, while the properties of organics and their mixtures need further studies. To understand the CCN activity of the ambient aerosols, relative contribution of the major factors like, aerosol size distribution, size resolved chemical composition and mixing state needs to be understood. Past studies have tested the performance of CCN closure study depending on how well the chemical composition, mainly organics, and mixing state of aerosols is treated. It has been found that the comparison between modelled and measured CCN concentration improves as the distance from the source region increases because the particles become more internally mixed and less size dependent. Measurements were conducted for 21 days in November, 2012 at the Indian Institute of Technology Kanpur (80 20'E, 26 26'N), India. Round the clock sampling of aerosol size distribution, chemical composition and cloud condensation nuclei (CCN) at various supersaturations (0.2-1%) was done to understand the diurnal variability of CCN properties of aerosols. The main goal of this study is to perform CCN closure study by focusing into the effect of organics and their hygroscopicity on CCN activity. Kohler theory is used to predict the CCN concentration at five different SS from the size distribution obtained from Scanning Mobility Particle Sizer (SMPS) and chemical composition (bulk and size resolved) from Aerodyne HR-ToF-AMS assuming different mixing

  16. 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.

  17. 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.

  18. 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.

  19. 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.

  20. 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

  1. 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

  2. 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.

  3. 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

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

    NASA Astrophysics Data System (ADS)

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

    2016-05-01

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

  5. 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.

  6. 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.

  7. 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. PMID:26944081

  8. 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.

  9. 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

  10. Condensation-nuclei (Aitken Particle) measurement system used in NASA global atmospheric sampling program

    NASA Technical Reports Server (NTRS)

    Nyland, T. W.

    1979-01-01

    The condensation-nuclei (Aitken particle) measuring system used in the NASA Global Atmospheric Sampling Program is described. Included in the paper is a description of the condensation-nuclei monitor sensor, the pressurization system, and the Pollack-counter calibration system used to support the CN measurement. The monitor has a measurement range to 1000 CN/cm cubed and a noise level equivalent to 5 CN/cm cubed at flight altitudes between 6 and 13 km.

  11. 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.

  12. The influence of marine monoterpene emissions on cloud condensation nuclei concentrations over the Southern Hemisphere oceans

    NASA Astrophysics Data System (ADS)

    Walker, Hannah; Arnold, Steve; Spracklen, Dominick; Rap, Alexandru; Scott, Catherine; Hackenberg, Sina; Carpenter, Lucy

    2016-04-01

    Changes in the concentration of cloud condensation nuclei (CCN) can affect Earth's climate by altering cloud properties such as lifetime, spatial extent, and brightness. Cloud properties are most sensitive to changes in CCN at the low concentrations typical of the remote marine environment. Underestimation of remote marine water-soluble organic carbon aerosol suggests that a source of secondary organic aerosol is missing from current model mechanisms. Oxidation products of oceanic reactive carbon are a candidate for this missing source, and have the potential to contribute to new particle formation and particle growth. Marine phytoplankton are known to produce monoterpenes (C10H16) and elevated monoterpene concentrations have been observed in regions of enhanced biological activity. A top-down estimate places the global oceanic monoterpene source in the region of 30 TgC a-1 but it remains very uncertain. In this study we use a global model of aerosol processes (GLOMAP) to investigate the potential impacts of oceanic monoterpenes on CCN concentrations over remote ocean regions. Satellite observations of chlorophyll-a inform the spatial distribution of oceanic monoterpene emission in the model. Using comparisons with new observations of atmospheric monoterpene concentrations from cruises in the North and South Atlantic oceans, we determine the optimum emission for marine monoterpenes. GLOMAP is implemented within the global chemistry-transport model TOMCAT and includes a detailed aerosol microphysics scheme, simulating size- and composition-resolved aerosol. Oxidation products of monoterpenes contribute to new particle formation. Oxidation products of both monoterpenes and isoprene contribute to particle growth. We find that oceanic monoterpene emission rates of 1-35 Tg a-1 (approximately 0.7-24 % of the estimated terrestrial source) lead to average annual global increases in CCN (particles having a dry diameter greater than 50 nm) of 1.6-31 % at the surface. The

  13. 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.; Kristensen, K.; Ylisirniö, A.; Virtanen, A.; Petäjä, T.; Glasius, M.; Prisle, N. L.

    2014-12-01

    Atmospheric aerosols have the ability to act as cloud condensation nuclei (CCN), initiating the formation of clouds and hereby influencing the climate system. The ability of aerosols to act as CCN is believed to depend on particle size and chemical composition. Organosulfates (OS), e.g sulfate esters, have been observed as constituents of secondary organic aerosols in numerous atmospheric environments, even as far as the Arctic, where OS have been found to comprise 7-15% of total organic matter and 9-11% of submicron organic matter in two independent studies. However, the properties of particulate OS have not yet been investigated. Here limonene derived OS were synthesized and the hygroscopic properties of these OS and their mixtures with ammonium sulfate (AS) were examined through a series of laboratory experiments. Laboratory generated particles of limonene-derived OS and AS were analysed using a unique set-up splitting the particle flow between a Hygroscopicity Tandem Differential Mobility Analyzer and a Cloud Condensation Nuclei counter, enabling simultaneous measurements of hygroscopic growth and CCN activation. Limonene-derived OS were chosen as study components, since monoterpenes (including limonene) have been identified as important precursors of OS in field samples as well as in smog chamber experiments. AS was used as a representative of the inorganic fraction in atmospheric aerosols. The preliminary results show that limonene-derived OS exhibit weak hygroscopic growth as well as CCN activation potential, however, not as strong as AS. For the organic-inorganic mixtures, it was observed that AS dominated the hygroscopic properties over the limonene-derived OS and became dictating for the measured values of hygroscopic growth and CCN activation, when the mass fraction of AS reached 20% or above. The results will be discussed further and supplementary measurements of OS surface tension and water activity will be presented.

  14. The Remarkable Condensational Growth of Cloud Droplets Grown on Giant Sea-salt Aerosol Particles

    NASA Astrophysics Data System (ADS)

    Jensen, J. B.; Nugent, A. D.

    2015-12-01

    Condensational growth of cloud drops is often assumed to be a well-understood process, using the drop growth equation: After activation of cloud condensation nuclei into cloud drops at cloud base, model studies often assume that drops quickly become dilute and consist of pure water. As a consequence, adiabatic ascent predicts that the growth rate of these drops is inversely proportional to their radius, and consequently that the drop spectrum will narrow with altitude. Here we demonstrate that drop growth on giant sea-salt aerosol particles (GCCN, dry radius > 0.5 μm) behaves very differently. For typical marine stratocumulus updrafts (0.4 m s-1), and for dry radius > 2 μm, these drops typically remain concentrated solution drops, and their condensational growth is so fast that they accelerate away from the main drop peak, and thus very rapidly attain precipitation drop sizes through condensation only. We show how many studies, that have attempted to include the effects of GCCN by initiating large pure water drops at cloud base, may have seriously underestimated the effects of GCCN on warm rain formation. We also speculate on possible solutions to this issue.

  15. 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

  16. 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.

  17. Approximate formulas for the mean dry size and the size-class fractions of cloud condensation nuclei as a function of supersaturation

    SciTech Connect

    Rivera-Carpio, C.A.; Novakov, T.

    1995-12-31

    Approximate formulas are presented for the mean dry size and the submicron and Aitken-size fractions of cloud condensation nuclei (CCN) as function of supersaturation. The expressions allow to estimate these CCN size-related characteristics, at the supersaturation levels reached during cloud formation, from aerosol size distribution and activation parametric data. The proposed formulas are derived based on approximations inferred from the very good agreement observed between measured and predicted slopes of CCN supersaturation activation spectra. Their application to the problem of assessing the physico-chemical characteristics of CCN-active aerosol particles in marine and continental air masses is illustrated.

  18. 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.

  19. 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.

  20. 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.

  1. Measured and modelled cloud condensation nuclei concentration at the high alpine site Jungfraujoch

    NASA Astrophysics Data System (ADS)

    Jurányi, Z.; Gysel, M.; Weingartner, E.; Decarlo, P. F.; Kammermann, L.; Baltensperger, U.

    2010-04-01

    Atmospheric aerosol particles are able to act as cloud condensation nuclei (CCN) and are therefore important for the climate and the hydrological cycle, but their properties are not fully understood. Total CCN number concentrations at 10 different supersaturations in the range of SS = 0.12-1.18% were measured in May 2008 at the remote high alpine research station, Jungfraujoch, Switzerland (3580 m asl.). In this paper, we present a closure study between measured and predicted CCN number concentrations. CCN predictions were done using number size distribution (scanning particle mobility sizer, SMPS) and bulk chemical composition data (aerosol mass spectrometer, AMS, and multi-angle absorption photometer, MAAP) in a simplified Köhler theory. The predicted and the measured CCN concentrations agree very well and are highly correlated. A sensitivity study showed that the temporal variability of the chemical composition at the Jungfraujoch can be neglected for a reliable CCN prediction, whereas it is important to know the mean chemical composition. The exact bias introduced by using a too low or too high hygroscopicity parameter for CCN prediction was further quantified and shown to be substantial for the lowest supersaturation. Despite the high average organic mass fraction (45%) during the measurement campaign, there was no indication that the surface tension was substantially reduced at the point of CCN activation. A comparison between hygroscopicity tandem differential mobility analyzer (HTDMA), AMS/MAAP, and CCN derived κ values showed that HTDMA measurements can be used as a chemical composition proxy for CCN predictions if no suitable chemical composition data are available.

  2. Measured and modelled cloud condensation nuclei number concentration at the high alpine site Jungfraujoch

    NASA Astrophysics Data System (ADS)

    Jurányi, Z.; Gysel, M.; Weingartner, E.; Decarlo, P. F.; Kammermann, L.; Baltensperger, U.

    2010-08-01

    Atmospheric aerosol particles are able to act as cloud condensation nuclei (CCN) and are therefore important for the climate and the hydrological cycle, but their properties are not fully understood. Total CCN number concentrations at 10 different supersaturations in the range of SS=0.12-1.18% were measured in May 2008 at the remote high alpine research station, Jungfraujoch, Switzerland (3580 m a.s.l.). In this paper, we present a closure study between measured and predicted CCN number concentrations. CCN predictions were done using dry number size distribution (scanning particle mobility sizer, SMPS) and bulk chemical composition data (aerosol mass spectrometer, AMS, and multi-angle absorption photometer, MAAP) in a simplified Köhler theory. The predicted and the measured CCN number concentrations agree very well and are highly correlated. A sensitivity study showed that the temporal variability of the chemical composition at the Jungfraujoch can be neglected for a reliable CCN prediction, whereas it is important to know the mean chemical composition. The exact bias introduced by using a too low or too high hygroscopicity parameter for CCN prediction was further quantified and shown to be substantial for the lowest supersaturation. Despite the high average organic mass fraction (~45%) in the fine mode, there was no indication that the surface tension was substantially reduced at the point of CCN activation. A comparison between hygroscopicity tandem differential mobility analyzer (HTDMA), AMS/MAAP, and CCN derived κ values showed that HTDMA measurements can be used to determine particle hygroscopicity required for CCN predictions if no suitable chemical composition data are available.

  3. Use of In Situ Data to Test a Raman Lidar-Based Cloud Condensation Nuclei Remote Sensing Method

    SciTech Connect

    Ghan, Steven J.; Collins, Donald R.

    2004-02-01

    A method of retrieving vertical profiles of cloud condensation nuclei (CCN) concentration from surface measurements is proposed. Surface measurements of the CCN concentration are scaled by the ratio of the backscatter (or extinction) vertical profile to the backscatter (or extinction) at or near the surface. The backscatter (or extinction) profile is measured by Raman lidar, and is corrected to dry conditions using the vertical profile of relative humidity (also measured by Raman lidar) and surface measurements of the dependence of backscatter (or extinction) on relative humidity. The method assumes the surface aerosol size distribution and composition are representative of the vertical column. Aircraft measurements of aerosol size distribution are used to test the dependence of the retrieval on the uniformity of aerosol size distribution. The retrieval is found to be robust for supersaturations less than 0.02%, but breaks down at higher supersaturations if the vertical profile of aerosol size distribution differs markedly from the distribution at the surface. Such conditions can be detected from the extinction/backscatter ratio.

  4. 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.

  5. Impact on Modeled Cloud Characteristics Due to Simplified Treatment of Uniform Cloud Condensation Nuclei During NEAQS 2004

    SciTech Connect

    Gustafson, William I.; Chapman, Elaine G.; Ghan, Steven J.; Easter, Richard C.; Fast, Jerome D.

    2007-10-12

    Subgrid-scale cloud condensation nuclei (CCN) heterogeneity is not represented in global climate models (GCM) and potentially contributes systematic errors to simulated cloud effects. High-resolution mesoscale model simulations were performed to investigate the impact of assuming a uniform CCN distribution on cloud properties and surface radiation over a region the size of a GCM grid column. Results indicate that a prescribed CCN distribution allowing for vertical and temporal fluctuations does substantially better in simulating cloud properties and radiative effects than does a prescribed uniform and constant CCN distribution. Spatially and temporally averaged net effects on downwelling shortwave radiation are between -3 and -11 W m-2 for the fluctuating and uniform distributions, respectively, versus a control simulation with fully interactive aerosols. Both prescribed CCN distributions produce optically thicker clouds more often than the control, with the mean cloud optical depth increasing by over 25% when using the uniform and constant CCN distribution.

  6. 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<...

  7. Correlations of small cumuli droplet and drizzle drop concentrations with cloud condensation nuclei concentrations

    NASA Astrophysics Data System (ADS)

    Hudson, James G.; Noble, Stephen; Jha, Vandana; Mishra, Subhashree

    2009-03-01

    Aircraft field measurements of cloud condensation nuclei (CCN) and cloud microphysics in maritime air masses showed ubiquitous influence of CCN. Flight averages of CCN concentrations and cloud droplet and drizzle drop concentrations were examined for as many as 17 flights during the Rain in Cumulus over the Ocean (RICO) project. CCN concentrations at only one supersaturation (S) of 1% measured at 100-m altitude were compared with cloud droplet and drizzle drop concentrations at six altitude bands between 600 and 3000 m. High positive correlations (R) between these CCN concentrations and the small size threshold of the cumulative cloud droplet concentrations (i.e., total activated cloud droplets) were found at all altitudes. These high R values also persisted for cloud parcels with a wide span of liquid water contents (LWCs), most of which were far below adiabatic (unmixed) values. For all but the lowest LWC parcels, R was essentially constant. There was an even more consistent negative R between CCN and large cloud droplet and drizzle drop concentrations. There was a sharp transition from positive to negative R over a small size range. The size at which this R transition occurred increased with altitude and LWC as overall droplet sizes increased with altitude or LWC. Entrainment seemed to show an opposite effect on R, but this was only apparent at the highest altitudes where entrainment was greatest and only for the smallest droplet sizes. These results indicate that the effect of CCN concentrations on cloud microphysics was pervasive with altitude, LWC, cloud droplet, and drizzle drop concentrations. This indicates greater impact of the indirect aerosol effect (IAE) in both of its manifestations, first IAE cloud radiation and second IAE precipitation.

  8. 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.

  9. Generation and characterization of condensation aerosols of benzo(a)pyrene

    SciTech Connect

    Tu, K.W.; Kanapilly, G.M.; Mitchell, C.E.

    1981-03-01

    Condensation aerosols of benzo(a)pyrene (BaP) with particle sizes ranging from 0.1 to 2 ..mu..m (aerodynamic diameter) were produced and studied. These aerosols were generated in a glove box by direct vaporization of BaP and homogeneous condensation of the vapor. The aerosol concentration ranged from 50 to 700 ..mu..g/l with aerosol production rates up to 15 mg BaP per minute. The effects of vaporization temperature and flow rate of diluting air on the particle size distribution and aerosol output were studied. The BaP aerosol was produced with relatively constant mass concentration and particle size distribution for more than 5 h. The aerosol was physicochemically and thermally stable. Data on the in vitro dissolution of BaP particles in aqueous solvents and in different dissolution systems suggested that the organic BaP particle does not dissolve in simple aqueous solvents.

  10. 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.

  11. In-Situ Characterization of Cloud Condensation Nuclei, Interstitial, and background Particles using Single Particle Mass Spectrometer, SPLAT II

    SciTech Connect

    Zelenyuk, Alla; Imre, D.; Earle, Michael; Easter, Richard C.; Korolev, Alexei; Leaitch, W. R.; Liu, Peter; Macdonald, A. M.; Ovchinnikov, Mikhail; Strapp, Walter

    2010-10-01

    Aerosol indirect effect remains the most uncertain aspect of climate change modeling because proper test requires knowledge of individual particles sizes and compositions with high spatial and temporal resolution. We present the first deployment of a single particle mass spectrometer (SPLAT II) that is operated in a dual data acquisition mode to measure all the required individual particle properties with sufficient temporal resolution to definitively resolve the aerosol-cloud interaction in this exemplary case. We measured particle number concentrations, asphericity, and individual particle size, composition, and density with better than 60 seconds resolution. SPLAT II measured particle number concentrations between 70 particles cm-3and 300 particles cm-3, an average particle density of 1.4 g cm-3. Found that most particles are composed of oxygenated organics, many of which are mixed with sulfates. Biomass burn particles some with sulfates were prevalent, particularly at higher altitudes, and processed sea-salt was observed over the ocean. Analysis of cloud residuals shows that with time cloud droplets acquire sulfate by the reaction of peroxide with SO2. Based on the particle mass spectra and densities we find that the compositions of cloud condensation nuclei are similar to those of background aerosol but, contain on average ~7% more sulfate, and do not include dust and metallic particles. A comparison between the size distributions of background, activated, and interstitial particles shows that while nearly none of the activated particles is smaller than 115 nm, more than 80% of interstitial particles are smaller than 115 nm. We conclude that for this cloud the most important difference between CCN and background aerosol is particle size although having more sulfate also helps.

  12. Are sesquiterpenes a good source of secondary organic cloud condensation nuclei (CCN)? Revisiting β-caryophyllene CCN

    NASA Astrophysics Data System (ADS)

    Tang, X.; Cocker, D. R., III; Asa-Awuku, A.

    2012-09-01

    Secondary organic aerosol (SOA) was formed in an environmental reaction chamber from the ozonolysis of β-caryophyllene (β-C) at low concentrations (5 ppb or 20 ppb). Experimental parameters were varied to characterize the effects of hydroxyl radicals, light and the presence of lower molecular weight terpene precursor (isoprene) for β-C SOA formation and cloud condensation nuclei (CCN) characteristics. Changes in β-C SOA chemicophysical properties (e.g., density, volatility, oxidation state) were explored with online techniques to improve our predictive understanding of β-C CCN activity. In the absence of OH scavenger, light intensity had negligible impacts on SOA oxidation state and CCN activity. In contrast, when OH reaction was effectively suppressed (> 11 ppm scavenger), SOA showed a much lower CCN activity and slightly less oxygenated state consistent with previously reported values. Though there is significant oxidized material present (O / C > 0.25), no linear correlation existed between the mass ratio ion fragment 44 in the bulk organic mass (f44) and O / C for the β-C-O3 system. No direct correlations were observed with other aerosol bulk ion fragment fraction (fx) and κ as well. A mixture of β-C and lower molecular weight terpenes (isoprene) consumed more ozone and formed SOA with distinct characteristics dependent on isoprene amounts. The addition of isoprene also improved the CCN predictive capabilities with bulk aerosol chemical information. The β-C SOA CCN activity reported here is much higher than previous studies (κ < 0.1) that use higher precursor concentration in smaller environmental chambers; similar results were only achieved with significant use of OH scavenger. Results show that aerosol formed from a mixture of low and high molecular weight terpene ozonolysis can be hygroscopic and can contribute to the global biogenic SOA CCN budget.

  13. Isoscalar-isovector proton-neutron pairing and quartet condensation in N =Z nuclei

    NASA Astrophysics Data System (ADS)

    Sambataro, M.; Sandulescu, N.

    2016-05-01

    We show that the correlations generated in the ground state of N =Z nuclei by the isovector and isoscalar pairing forces can be treated with high precision as a condensate of alpha-like quartets. To treat these correlations, the quartet condensation model (QCM) is extended to the treatment of spherically symmetric isovector (T =1 ,J =0 ) and isoscalar (T =0 ,J =1 ) pairing forces. Within the QCM, we discuss the competition between T =1 and T =0 pairing correlations in the case of a two-level model and for N =Z nuclei with nucleons moving in the open shells above 16O,40Ca, and 100Sn. We show that, in N =Z systems, isovector and isoscalar proton-neutron pairing correlations always coexist.

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

    PubMed Central

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

    2012-01-01

    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 ≫103 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 > 1013 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. PMID:22753520

  15. 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

  16. 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.

  17. 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.

  18. Fluorimetric measurements and chromatin condensation patterns of nuclei from 3T3 cells throughout G1.

    PubMed

    Moser, G C; Fallon, R J; Meiss, H K

    1981-02-01

    Using two cytological methods based on nuclear morphology, quinacrine dihydrochloride (QDH) staining and premature chromosome condensation (PCC), it has been possible to identify cell cycle positions within G1 of growing and arrested 3T3 cells. The fluorescent intensity of QDH-stained interphase cells appears to decrease as the cells pass from mitosis to S phase. Likewise, the length and thickness of prematurely condensed chromatids can be related to the cells; position within the G1 period. Data are presented that deal with three interrelated topics: 1) We determined by fluorometric measurements of nuclei from 3T3 cells that the visual observation of the decrease in QDH fluorescence during G1 reflects an actual decrease in total fluorescence and not a dispersion of the fluorescent chromatin in a larger nuclear area. 2) We correlated the results obtained by QDH staining with those of PCC on the same cell samples blocked in G1 by different conditions. Serum-starved and contact-inhibited cell nuclei had the highest intensity, hydroxyurea-treated ones had the lowest intensity, while that of isoleucine-deprived cells was in between. The same relative order of G1 positions was obtained based on PCC morphology. Thus, both methods monitor the state of chromatin condensation and can be used to identify cell cycle position within G1. 3) We showed with both methods that the states of chromatin resulting from the various G1 blocking conditions differ from each other.

  19. Thermodynamics of water condensation on a primary marine aerosol coated by surfactant organic molecules.

    PubMed

    Djikaev, Yuri S; Ruckenstein, Eli

    2014-10-23

    A large subset of primary marine aerosols can be initially (immediately upon formation) treated using an "inverted micelle" model. We study the thermodynamics of heterogeneous water condensation on such a marine aerosol. Its hydrophobic organic coating can be processed by chemical reactions with atmospheric species; this enables the marine aerosol to serve as a nucleating center for water condensation. The most probable pathway of such "aging" involves atmospheric hydroxyl radicals that abstract hydrogen atoms from organic molecules coating the aerosol (first step), the resulting radicals being quickly oxidized by ubiquitous atmospheric oxygen molecules to produce surface-bound peroxyl radicals (second step). Taking these two reactions into account, we derive an expression for the free energy of formation of an aqueous droplet on a marine aerosol. The model is illustrated by numerical calculations. The results suggest that the formation of aqueous droplets on marine aerosols is most likely to occur via Köhler activation rather than via nucleation. The model allows one to determine the threshold parameters necessary for the Köhler activation of such aerosols. Numerical results also corroborate previous suggestions that one can omit some chemical species of aerosols (and other details of their chemical composition) in investigating aerosol effects on climate.

  20. 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. PMID:16772683

  1. 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.

  2. 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.

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

    NASA Astrophysics Data System (ADS)

    Wilson, James Charles

    1994-11-01

    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.

  4. 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.

  5. 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

  6. 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.

  7. Enhanced persistence of fog under illumination for carbon nanotube fog condensation nuclei

    NASA Astrophysics Data System (ADS)

    Banerjee, Saumyabrata; Tripathi, Sachchida N.; Das, Utpal; Ranjan, Raju; Jadhav, Nilesh; Singh, Vivek P.; Jariwala, Chinmay; Sonkar, Sumit; Sarkar, Sabyasachi

    2012-07-01

    Black carbon (BC) emissions have increased over South Asia and more persistent winter fogs are common during last decade. However, a physical mechanism connecting these two is still unknown. A significant fraction of BC is known to be in the form of carbon-nanotube (CNT). We have investigated the effects of two different sets of fog condensation nuclei, viz., inorganic salts (sodium chloride and ammonium sulphate) and BC (graphite and CNT) on the dissipation of chamber generated fog under dark and halogen lamp illuminated conditions at a controlled temperature, relative humidity, and fog condensation nuclei distribution. We found that, for inorganic salts, fog dissipates at a faster rate under illumination than in dark conditions showing similar trends for both sodium chloride and ammonium chloride. On the contrary, fog is found to be more persistent, for illuminated conditions, in the case of BC. Moreover, fog persistence is found to be more than twice for CNT compared to graphite in illuminated conditions. CNT is known to be an extremely effective absorber of light which leads to microscopic heating and subsequent evaporation which inhibits droplet growth. Small droplets have large residence time leading to longer fog persistence. This hitherto unknown mechanism may be responsible for persistent fog in India during last decade.

  8. Observations of cloud condensation nuclei in Mt. Huang: instrumentation and early observations

    NASA Astrophysics Data System (ADS)

    Chen, Kui; Yin, Yan; Chen, Chen; Yang, Weifeng; Deng, Wei; Hu, Zhenghua; Wu, Fangfang

    2009-07-01

    A new commercial instrument for measuring Cloud Condensation Nuclei (CCN), the Droplet Measurement Technologies Cylindrical Continuous-Flow Streamwise Thermal Gradient CCN Chamber (CFSTGC), installed on Mount Huang meteorological station (30°19'N, 118°14'E, 1840m above sea level) from 16 April to 28 July 2008. This instrument can measure CCN concentrations at supersaturations from 0.1% to 2% (potentially up to 6%), as well as a 1 Hz sampling rate that is sufficient for ground-based or airborne platform operation. The instrument records data continuously at 1-second intervals 24 hours a day. For the 98-day, continuous study the average CCN concentration was found to range between a few hundred and a few thousand nuclei per cm3 at supersaturations between 0.3 and 1%. Diurnal variations were observed, as well as other possible influences, such as wind speed, wind direction and mixing depth. At a constant supersaturation of 0.5% the CCN concentration is typically on the order of 361 to 2297 nuclei per cm3. A description of the instrumentation and early observations are presented and discussed.

  9. A numerical determination of the evolution of cloud drop spectra due to condensation on natural aerosol particles

    NASA Technical Reports Server (NTRS)

    Lee, I. Y.; Haenel, G.; Pruppacher, H. R.

    1980-01-01

    The time variation in size of aerosol particles growing by condensation is studied numerically by means of an air parcel model which allows entrainment of air and aerosol particles. Particles of four types of aerosols typically occurring in atmospheric air masses were considered. The present model circumvents any assumption about the size distribution and chemical composition of the aerosol particles by basing the aerosol particle growth on actually observed size distributions and on observed amounts of water taken up under equilibrium by a deposit of the aerosol particles. Characteristic differences in the drop size distribution, liquid water content and supersaturation were found for the clouds which evolved from the four aerosol types considered.

  10. 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.

  11. 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.

  12. 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

  13. LIMA (v1.0): a 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.

    2015-09-01

    The paper describes the 2-moment microphysical scheme LIMA (Liquid Ice Multiple Aerosols), which relies on the prognostic evolution of a three-dimensional (3-D) aerosol population, and the careful description of the nucleating properties that enable cloud droplets and pristine ice crystals to form. LIMA uses the aerosol nucleating properties to form cloud droplets and pristine ice crystals. 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 temperature. 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 formation of hydrometeors is standard. 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

  14. 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

  15. 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

  16. 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.

  17. 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

  18. 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.

  19. 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.

  20. 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.; Knopf, D. A.

    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

  1. 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.; 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 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, chemical

  2. 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

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

    NASA Astrophysics Data System (ADS)

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

    2015-09-01

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

  4. 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.

  5. 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.

  6. 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

  7. 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.

  8. Quantifying wet scavenging processes in aircraft observations of nitric acid and cloud condensation nuclei

    NASA Astrophysics Data System (ADS)

    Garrett, T. J.; Avey, L.; Palmer, P. I.; Stohl, A.; Neuman, J. A.; Brock, C. A.; Ryerson, T. B.; Holloway, J. S.

    2006-12-01

    Wet scavenging is an important sink term for many atmospheric constituents. However, production of precipitation in clouds is poorly understood, and pollutant removal through wet scavenging is difficult to separate from removal through dry scavenging, atmospheric mixing, or chemical transformations. Here we use airborne data from the International Consortium for Atmospheric Research on Transport and Transformation project to show that measured ratios of soluble and insoluble trace gases provide a useful indicator for quantifying wet scavenging. Specifically, nitric acid (HNO3), produced as a by-product of combustion, is highly soluble and removed efficiently from clouds by rain. Regional carbon monoxide (CO), which is also an indicator of anthropogenic activity, is insoluble and has a lifetime against oxidation of about a month. We find that relative concentrations of HNO3 to regional CO observed in clear air are negatively correlated with precipitation production rates in nearby cloudy air (r2 = 0.85). Also, we show that relative concentrations of HNO3 and CO can be used to quantify cloud condensation nucleus (CCN) scavenging by precipitating clouds. This is because CCN and HNO3 molecules are both fully soluble in cloud water and hence can be treated as analogous species insofar as wet scavenging is concerned. While approximate, the practical advantage of this approach to scavenging studies is that it requires only measurement in clear air and no a priori knowledge of the cloud or aerosol properties involved.

  9. 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

  10. Efficient formation of stratospheric aerosol for climate engineering by emission of condensible vapor from aircraft

    NASA Astrophysics Data System (ADS)

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

    2010-09-01

    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.

  11. 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.

  12. 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

  13. 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

  14. Interactions of Water with Mineral Dust Aerosol: Water Adsorption, Hygroscopicity, Cloud Condensation, and Ice Nucleation.

    PubMed

    Tang, Mingjin; Cziczo, Daniel J; Grassian, Vicki H

    2016-04-13

    Mineral dust aerosol is one of the major types of aerosol present in the troposphere. The molecular level interactions of water vapor with mineral dust are of global significance. Hygroscopicity, light scattering and absorption, heterogneous reactivity and the ability to form clouds are all related to water-dust interactions. In this review article, experimental techniques to probe water interactions with dust and theoretical frameworks to understand these interactions are discussed. A comprehensive overview of laboratory studies of water adsorption, hygroscopicity, cloud condensation, and ice nucleation of fresh and atmspherically aged mineral dust particles is provided. Finally, we relate laboratory studies and theoretical simulations that provide fundemental insights into these processes on the molecular level with field measurements that illustrate the atmospheric significance of these processes. Overall, the details of water interactions with mineral dust are covered from multiple perspectives in this review article. PMID:27015126

  15. Interactions of Water with Mineral Dust Aerosol: Water Adsorption, Hygroscopicity, Cloud Condensation, and Ice Nucleation.

    PubMed

    Tang, Mingjin; Cziczo, Daniel J; Grassian, Vicki H

    2016-04-13

    Mineral dust aerosol is one of the major types of aerosol present in the troposphere. The molecular level interactions of water vapor with mineral dust are of global significance. Hygroscopicity, light scattering and absorption, heterogneous reactivity and the ability to form clouds are all related to water-dust interactions. In this review article, experimental techniques to probe water interactions with dust and theoretical frameworks to understand these interactions are discussed. A comprehensive overview of laboratory studies of water adsorption, hygroscopicity, cloud condensation, and ice nucleation of fresh and atmspherically aged mineral dust particles is provided. Finally, we relate laboratory studies and theoretical simulations that provide fundemental insights into these processes on the molecular level with field measurements that illustrate the atmospheric significance of these processes. Overall, the details of water interactions with mineral dust are covered from multiple perspectives in this review article.

  16. 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.

  17. The effects of marine primary biogenic organic aerosols as heterogeneous ice nuclei in mixed-phase clouds

    NASA Astrophysics Data System (ADS)

    Yun, Y.; Penner, J. E.

    2012-12-01

    There have been reports in the literature about marine primary biogenic organic aerosols (marine POA) acting as ice nuclei. These marine POA can be transported to the atmosphere through the bursting of air bubbles by breaking waves. In this study, we add marine POA as heterogeneous ice nuclei in mixed-phase clouds in a coupled general circulation model and aerosol transport model (CAM-IMPACT). The emission of the marine POA is determined by the sea salt emissions and a sea spray organic fraction function. The wet and dry deposition scheme in the CAM-IMPACT model will be extended to treat marine POA. The ice nucleation ability of the marine POA will be determined according to the in situ observation of the surface ice nuclei ratio, as well as the simulated surface concentration of marine POA and other aerosols. Several sensitivity tests will be performed on the sea salt emission flux, the sea spray organic fraction function, as well as the freezing efficiency of marine POA. The simulated ice water amount will be compared to satellite observations. This study attempts to evaluate the effect of marine biological organics as ice nuclei on a global scale.

  18. Influence of oceanic dimethyl sulfide emissions on cloud condensation nuclei concentrations and seasonality over the remote Southern Hemisphere oceans: A global model study

    NASA Astrophysics Data System (ADS)

    Korhonen, Hannele; Carslaw, Kenneth S.; Spracklen, Dominick V.; Mann, Graham W.; Woodhouse, Matthew T.

    2008-08-01

    We use a global chemical transport model with size-resolved aerosol microphysics to investigate the sources of cloud condensation nuclei (CCN) in the Southern Hemisphere remote marine boundary layer (MBL). Long-term observations of CCN number at Cape Grim (40°41'S, 144°41'E) show a clear seasonal cycle with a 2-3 times higher concentration in summer than in winter, which has been attributed to seasonal changes in the dimethyl sulfide (DMS) ocean-to-atmosphere flux. We find that this cycle at Cape Grim and also throughout the 30°-45°S latitude band is caused mostly by changes in the regional-scale DMS ocean water concentration. In this latitude band, DMS emissions increase the simulated CCN concentrations from November to April, with a maximum effect of 46% in January (calculated at 0.23% supersaturation). Farther south, the impact of DMS on CCN is apparent only from December to February and increases the CCN concentration at most by 18% at 45°-60°S and by 40% at 60°-75°S. These model-derived contributions of DMS to Southern Ocean summertime CCN are smaller than the 80% derived from correlations between satellite-observed chlorophyll and column CCN, which we explain in terms of nonlinear behavior of CCN from the free troposphere (FT). We show that the main microphysical pathway of DMS influence on CCN number is nucleation of DMS-derived H2SO4 in the FT and subsequent growth of formed particles by condensation and coagulation during entrainment into the MBL. Our simulations suggest that >90% of the increase in MBL CCN when DMS is added to the model is formed in this way. The growth of ultrafine sea spray particles to CCN sizes due to condensation of DMS-derived H2SO4 in the MBL affects the simulated CCN concentrations by less than 6%. Overall, entrainment of nucleated sulfate aerosol into the MBL from the FT accounts for 43-65% of the summer zonal mean CCN concentrations but only 7-20% of the winter CCN over the Southern Hemisphere oceans.

  19. Condensation nuclei measurement in the stratosphere for the NASA ACE program. Final report, 1 February 1980-31 January 1987

    SciTech Connect

    Wilson, J.C.

    1994-11-01

    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.

  20. 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

  1. 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.

  2. 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.

  3. Airborne measurement of tropospheric ice nuclei aerosols using the Portable Ice Nucleation Chamber (PINC)

    NASA Astrophysics Data System (ADS)

    Chou, C.; Stetzer, O.; Sierau, B.; Lohmann, U.

    2009-04-01

    Ice clouds and mixed phase clouds have different microphysical and radiative properties that need to be assessed in order to understand their impact on the climate. Indeed, on one hand ice crystals found in the ice phase have the ability to scatter incoming solar radiation and absorb terrestrial radiation. On the other hand, about 70% of the tropical precipitation forms via the ice-phase, this means an impact on the hydrological cycle. Investigation of the ability of an aerosol to act as Ice Nuclei (IN) requires knowledge of the thermodynamics conditions, i.e. relative humidity and temperature at which this aerosol form ice crystal. The PerformPINC project was a research campaign within the Education & Training program of the EUropean Fleet for Airborne Research (EUFAR). The project objectives were to measure the number concentration of IN in free and upper troposphere using the Portable Ice Nucleation Chamber (PINC) recently developed by the Institute for Atmospheric Climate Sciences at the ETH Zürich, and thus as a primary objective, testing the technical performance of the instrument during in-situ airborne measurements at different conditions within the chamber. The PINC is the portable version of the Zurich Ice Nucleation Chamber (ZINC) (Stetzer et al., 2008) and is meant for in-situ measurements. Both ZINC and PINC follow the same principle as the Continuous Flow Diffusion Chamber of the Colorado University (Rogers, 1988) that has proven to be of good performance in previous airborne in-situ campaigns (DeMott et al., 2003a). Unlike the CFDC, the PINC has a flat design composed of a main chamber, and an evaporation part. The cooling system of the PINC is also different and consists for the warm side of two BD120 compressors mounted in parallel. For the cold side, it is four BD120 compressors in parallel mounted to another BD120 compressor in serial, thus allowing us to reach lower temperature than the warm side. Aerosols are collected through an inlet where

  4. Airborne measurement of tropospheric ice nuclei aerosols using the Portable Ice Nucleation Chamber (PINC)

    NASA Astrophysics Data System (ADS)

    Chou, C.; Stetzer, O.; Sierau, B.; Lohmann, U.

    2009-04-01

    Ice clouds and mixed phase clouds have different microphysical and radiative properties that need to be assessed in order to understand their impact on the climate. Indeed, on one hand ice crystals found in the ice phase have the ability to scatter incoming solar radiation and absorb terrestrial radiation. On the other hand, about 70% of the tropical precipitation forms via the ice-phase, this means an impact on the hydrological cycle. Investigation of the ability of an aerosol to act as Ice Nuclei (IN) requires knowledge of the thermodynamics conditions, i.e. relative humidity and temperature at which this aerosol form ice crystal. The PerformPINC project was a research campaign within the Education & Training program of the EUropean Fleet for Airborne Research (EUFAR). The project objectives were to measure the number concentration of IN in free and upper troposphere using the Portable Ice Nucleation Chamber (PINC) recently developed by the Institute for Atmospheric Climate Sciences at the ETH Zürich, and thus as a primary objective, testing the technical performance of the instrument during in-situ airborne measurements at different conditions within the chamber. The PINC is the portable version of the Zurich Ice Nucleation Chamber (ZINC) (Stetzer et al., 2008) and is meant for in-situ measurements. Both ZINC and PINC follow the same principle as the Continuous Flow Diffusion Chamber of the Colorado University (Rogers, 1988) that has proven to be of good performance in previous airborne in-situ campaigns (DeMott et al., 2003a). Unlike the CFDC, the PINC has a flat design composed of a main chamber, and an evaporation part. The cooling system of the PINC is also different and consists for the warm side of two BD120 compressors mounted in parallel. For the cold side, it is four BD120 compressors in parallel mounted to another BD120 compressor in serial, thus allowing us to reach lower temperature than the warm side. Aerosols are collected through an inlet where

  5. The impact of time-averaged volcanic sulphur emissions on the global cloud condensation nuclei budget in the pre-industrial era

    NASA Astrophysics Data System (ADS)

    Schmidt, Anja; Carslaw, Kenneth; Mann, Graham; Merikanto, Joonas

    2010-05-01

    Volcanoes are a strong source of sulphur dioxide (SO2) with time-averaged emission inventories (e.g. Andres and Kasgnoc, 1998) indicating that volcanoes account for around 40% of the total annual SO2 flux in the pre-industrial atmosphere. We use a global aerosol microphysics model (GLOMAP-mode) to quantify the contribution of time-averaged volcanic sulphur emissions (from both continuous passive degassing and explosive volcanoes) on the global cloud condensation nuclei (CCN) budget. GLOMAP-mode is capable of simulating microphysical processes, such as binary homogeneous nucleation, hygroscopic growth, coagulation, condensation, cloud processing (oxidation of dissolved SO2 to SO4 in cloud droplets), as well as dry and wet deposition. For this study we use a sulphur chemistry scheme which includes 7 species (DMS, DMSO, MSA, SO2, H2SO4, COS, CS2). The runs were conducted using four internally mixed aerosol components, sulphate (SO4), sea salt, black carbon (BC) and organic carbon (OC). We simulated the impact of volcanic degassing in a pre-industrial setting (i.e. using 1750 BC and OC emissions in the absence of any anthropogenic emissions) using the volcanic emission inventory by Dentener et al. (2006). This volcanic inventory is based on datasets by Andres and Kasgnoc (1998) and Halmer et al. (2002) and accounts for an annual flux of ~13 Tg(S) of volcanic SO2. Our simulations suggest that volcanic degassing contributes on average ~50 CCN (>35nm in radius) per cubic centimetre to the annual zonal mean CCN concentrations in the tropical boundary layer. The simulations also reveal complex changes in annual zonal mean total particle concentrations (CN). CN concentrations are more than double in large parts of the tropical boundary layer when comparing the unperturbed run (i.e. without volcanic degassing) to the run featuring time-averaged volcanic degassing. However, the simulations also reveal that the additional SO2 and its subsequent conversion to sulphate aerosol

  6. 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

  7. Martian dust particles as condensation nuclei - A preliminary assessment of mineralogical factors

    NASA Technical Reports Server (NTRS)

    Gooding, J. L.

    1986-01-01

    Experiments were performed to determine the factors influencing ice nucleation detected in Viking Lander data from the Mars surface. The study focused on the relationship between mineral properties and condensate formation under Mars conditions. Pulverized particles of the primary phases of basaltic rocks and their alteration products, expandable clay minerals and a nonexpandable clay mineral, and petrologically well-characterized regolith materials ranging from 10-60 microns in size, were studied. The powders were individually or in combinations mixed with water in a flowing CO2 atmosphere while calorimetry data was taken on the ice nucleation threshold. The ice-forming characteristics of the mixes were found to be a function of the crystallographic disregistry, chemical bonding, and active-site properties of the individual minerals. The crystalline materials were better nucleators of condensates than were the cryptocrystalline mineral specimens, while nonexpandable clay materials, particularly zeolite, were the more effective nucleators among the weathering product materials.

  8. 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.

  9. 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.

  10. 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.

  11. 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.

  12. 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.

  13. Aerosol and cloud droplet number concentrations observed in marine stratocumulus

    SciTech Connect

    Vong, R.J.; Covert, D.S.

    1995-12-01

    The relationship between measurements of cloud droplet number concentration and cloud condensation nuclei (CCN) concentration, as inferred from aerosol size spectra, was investigated at a {open_quote}clean air{close_quote}, marine site (Cheeka Peak) located near the coast of the Olympic Peninsula in Washington State. Preliminary results demonstrated that cloud droplet number increased and droplet diameter decreased as aerosol number concentration (CCN) increased. These results support predictions of a climate cooling due to any future increases in marine aerosol concentrations.

  14. 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

  15. Impact of clouds and precipitation on atmospheric aerosol

    NASA Astrophysics Data System (ADS)

    Andronache, Constantin

    2015-04-01

    Aerosols have a significant impact on the dynamics and microphysics of continental mixed-phase convective clouds. High aerosol concentrations provide enhanced cloud condensation nuclei that can lead to the invigoration of convection and increase of surface rainfall. Such effects are dependent on environmental conditions and aerosol properties. Clouds are not only affected by aerosol, they also alter aerosol properties by various processes. Cloud processing of aerosol includes: convective redistribution, modification in the number and size of aerosol particles, chemical processing, new particle formation around clouds, and aerosol removal by rainfall to the surface. Among these processes, the wet removal during intense rain events, in polluted continental regions, can lead to spikes in acidic deposition into environment. In this study, we address the effects of clouds and precipitation on the aerosol distribution in cases of convective precipitation events in eastern US. We examine the effects of clouds and precipitation on various aerosol species, as well as their temporal and spatial variability.

  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. 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.

  18. Turbulent mixing condensation nucleus counter

    NASA Astrophysics Data System (ADS)

    Mavliev, Rashid

    The construction and operating principles of the Turbulent Mixing Condensation Nucleus Counter (TM CNC) are described. Estimations based on the semiempirical theory of turbulent jets and the classical theory of nucleation and growth show the possibility of detecting particles as small as 2.5 nm without the interference of homogeneous nucleation. This conclusion was confirmed experimentally during the International Workshop on Intercomparison of Condensation Nuclei and Aerosol Particle Counters (Vienna, Austria). Number concentration, measured by the Turbulent Mixing CNC and other participating instruments, is found to be essentially equal.

  19. Aerosol Enhancements in the Upper Troposphere Over The Amazon Forest: Do Amazonian Clouds Produce Aerosols?

    NASA Astrophysics Data System (ADS)

    Andreae, M. O.; Afchine, A.; Albrecht, R. I.; Artaxo, P.; Borrmann, S.; Cecchini, M. A.; Costa, A.; Dollner, M.; Fütterer, D.; Järvinen, E.; Klimach, T.; Konemann, T.; Kraemer, M.; Krüger, M. L.; Machado, L.; Mertes, S.; Pöhlker, C.; Poeschl, U.; Sauer, D. N.; Schnaiter, M.; Schneider, J.; Schulz, C.; Spanu, A.; Walser, A.; Weinzierl, B.; Wendisch, M.

    2015-12-01

    The German-Brazilian cooperative aircraft campaign ACRIDICON-CHUVA (Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems) on the German research aircraft HALO took place over the Amazon Basin in September/October 2014, with the objective of studying tropical deep convective clouds over the Amazon rainforest and their interactions with trace gases, aerosol particles, and atmospheric radiation. The aircraft was equipped with about 30 remote sensing and in-situ instruments for meteorological, trace gas, aerosol, cloud, precipitation, and solar radiation measurements. Fourteen research flights were conducted during this campaign. Observations during ACRIDICON-CHUVA showed high aerosol concentrations in the upper troposphere (UT) over the Amazon Basin, with concentrations after normalization to standard conditions often exceeding those in the boundary layer (BL). This behavior was consistent between several aerosol metrics, including condensation nuclei (CN), cloud condensation nuclei (CCN), and chemical species mass concentrations. These UT aerosols were different in their composition and size distribution from the aerosol in the BL, making convective transport of particles unlikely as a source. The regions in the immediate outflow of deep convective clouds were found to be depleted in aerosol particles, whereas enhanced aerosol number and mass concentrations were found in UT regions that had experienced outflow from deep convection in the preceding 24-48 hours. This suggests that aerosol production takes place in the UT based on volatile and condensable material brought up by deep convection. Subsequently, downward mixing and transport of upper tropospheric aerosol may be a source of particles to the BL, where they increase in size by the condensation of biogenic volatile organic carbon (BVOC) oxidation products. This may be an important source of aerosol particles in the Amazonian BL, where aerosol nucleation and new

  20. Volatility dependence of Henry's law constants of condensable organics: Application to estimate depositional loss of secondary organic aerosols

    NASA Astrophysics Data System (ADS)

    Hodzic, A.; Aumont, B.; Knote, C.; Lee-Taylor, J.; Madronich, S.; Tyndall, G.

    2014-07-01

    The water solubility of oxidation intermediates of volatile organic compounds that can condense to form secondary organic aerosol (SOA) is largely unconstrained in current chemistry-climate models. We apply the Generator of Explicit Chemistry and Kinetics of Organics in the Atmosphere to calculate Henry's law constants for these intermediate species. Results show a strong negative correlation between Henry's law constants and saturation vapor pressures. Details depend on precursor species, extent of photochemical processing, and NOx levels. Henry's law constants as a function of volatility are made available over a wide range of vapor pressures for use in 3-D models. In an application using the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) over the U.S. in summer, we find that dry (and wet) deposition of condensable organic vapors leads to major reductions in SOA, decreasing surface concentrations by ~50% (10%) for biogenic and ~40% (6%) for short chain anthropogenic precursors under the considered volatility conditions.

  1. 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...

  2. 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.

  3. 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.

  4. 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.

  5. 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.

    2015-10-01

    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.

  6. 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.

  7. 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

  8. 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

  9. Anthropogenic Aerosols and Tropical Precipitation

    NASA Astrophysics Data System (ADS)

    Wang, C.; Kim, D.; Ekman, A. M. L.; Barth, M. C.; Rasch, P. J.

    2009-04-01

    Anthropogenic aerosols can affect the radiative balance of the Earth-atmosphere system and precipitation by acting as cloud condensation nuclei (CCN) or ice nuclei (IN) and thus modifying the optical and microphysical properties as well as lifetimes of clouds. Recent studies have also suggested that the direct radiative effect of anthropogenic aerosols, particularly absorbing aerosols, can perturb the large-scale circulation and cause a significant change in both quantity and distribution of critical tropical precipitation systems ranging from Pacific and Indian to Atlantic Oceans. This effect of aerosols on precipitation often appears in places away from aerosol-concentrated regions and current results suggest that the precipitation changes caused by it could be much more substantial than that by the microphysics-based aerosol effect. To understand the detailed mechanisms and strengths of such a "remote impact" and the climate response/feedback to anthropogenic aerosols in general, an interactive aerosol-climate model has been developed based on the Community Climate System Model (CCSM) of NCAR. Its aerosol module describes size, chemical composition, and mixing states of various sulfate and carbonaceous aerosols. Several model processes are derived based on 3D cloud-resolving model simulations. We have conducted a set of long integrations using the model driven by radiative effects of different combinations of various carbonaceous and sulfate aerosols and their mixtures. The responses of tropical precipitation systems to the forcing of these aerosols are analyzed using both model and observational data. Detailed analyses on the aerosol-precipitation causal relations of two systems: i.e., the Indian summer monsoon and Pacific ITCZ will be specifically presented.

  10. 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

  11. 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.

  12. 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.

  13. 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.

  14. Dissipation of marine stratiform clouds and collapse of the marine boundary layer due to the depletion of cloud condensation nuclei by clouds.

    PubMed

    Ackerman, A S; Toon, O B; Hobbs, P V

    1993-10-01

    When the production of cloud condensation nuclei in the stratocumulus-topped marine boundary layer is low enough, droplet collisions can reduce concentrations of cloud droplet numbers to extremely low values. At low droplet concentrations a cloud layer can become so optically thin that cloud-top radiative cooling cannot drive vertical mixing. Under these conditions, model simulations indicate that the stratocumulus-topped marine boundary layer collapses to a shallow fog layer. Through this mechanism, marine stratiform clouds may limit their own lifetimes.

  15. 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.

  16. 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.

  17. 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.

  18. Cloud condensation nucleus (CCN) behavior of organic aerosol particles generated by atomization of water and methanol solutions

    NASA Astrophysics Data System (ADS)

    Rissman, T. A.; Varutbangkul, V.; Surratt, J. D.; Topping, D. O.; McFiggans, G.; Flagan, R. C.; Seinfeld, J. H.

    2006-12-01

    Cloud condensation nucleus (CCN) experiments were carried out for malonic acid, succinic acid, oxalacetic acid, DL-malic acid, glutaric acid, DL-glutamic acid monohydrate, and adipic acid, using both water and methanol as atomization solvents, at three operating supersaturations (0.11% 0.21%, and 0.32%) in the Caltech three-column CCN instrument (CCNC3). Predictions of CCN behavior for five of these compounds were made using the Aerosol Diameter Dependent Equilibrium Model (ADDEM). The experiments presented here expose important considerations associated with the laboratory measurement of the CCN behavior of organic compounds. Choice of atomization solvent results in significant differences in CCN activation for some of the compounds studied, which could result from residual solvent, particle morphology differences, and chemical reactions between the particle and gas phases. Also, significant changes in aerosol size distribution occurred after classification in a differential mobility analyzer (DMA) for malonic acid and glutaric acid. Filter analysis of adipic acid atomized from methanol solution indicates that gas-particle phase reactions may have taken place after atomization and before the methanol was removed from the sample gas stream. Careful consideration of these experimental issues is necessary for successful design and interpretation of laboratory CCN measurements.

  19. Cloud condensation nucleus (CCN) behavior of organic aerosol particles generated by atomization of water and methanol solutions

    NASA Astrophysics Data System (ADS)

    Rissman, T. A.; Varutbangkul, V.; Surratt, J. D.; Topping, D. O.; McFiggans, G.; Flagan, R. C.; Seinfeld, J. H.

    2007-06-01

    Cloud condensation nucleus (CCN) experiments were carried out for malonic acid, succinic acid, oxalacetic acid, DL-malic acid, glutaric acid, DL-glutamic acid monohydrate, and adipic acid, using both water and methanol as atomization solvents, at three operating supersaturations (0.11%, 0.21%, and 0.32%) in the Caltech three-column CCN instrument (CCNC3). Predictions of CCN behavior for five of these compounds were made using the Aerosol Diameter Dependent Equilibrium Model (ADDEM). The experiments presented here expose important considerations associated with the laboratory measurement of the CCN behavior of organic compounds. Choice of atomization solvent results in significant differences in CCN activation for some of the compounds studied, which could result from residual solvent, particle morphology differences, and chemical reactions between the particle and gas phases. Also, significant changes in aerosol size distribution occurred after classification in a differential mobility analyzer (DMA) for malonic acid and glutaric acid, preventing confident interpretation of experimental data for these two compounds. Filter analysis of adipic acid atomized from methanol solution indicates that gas-particle phase reactions may have taken place after atomization and before methanol was removed from the sample gas stream. Careful consideration of these experimental issues is necessary for successful design and interpretation of laboratory CCN measurements.

  20. 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.

  1. 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

  2. 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

  3. The dynamics of 57Fe nuclei in Fe(II)-DNA and [Fe(II)(1-methyl-2-mercaptoimidazole)2]-DNA condensates.

    PubMed

    Silvestri, Arturo; Ruisi, Giuseppe; Girasolo, Maria Assunta

    2002-11-25

    Alcoholic solutions of FeCl(2) and Fe(II)(Hmmi)(2)Cl(2) (Hmmi=1-methyl-2-mercaptoimidazole) induce calf thymus DNA condensation from aqueous solutions buffered at pH 7.4. A 1:1 Fe(II)-(DNA monomer) stoichiometry is assumed. The (57)Fe Mössbauer hyperfine parameters suggest an octahedral coordination environment, severely distorted, in both Fe(II)-(DNA monomer) and [Fe(II)(Hmmi)(2)]-(DNA monomer) condensates. The dynamic properties of iron nuclei in freeze-dried samples were investigated by means of variable temperature (57)Fe Mössbauer spectroscopy. Mean square displacements, (T), were calculated, such as the effective vibrating mass and the Mössbauer lattice temperature of the solids. increases linearly with the temperature in the whole temperature range explored; the absolute values are typical for lattice or solid-state vibrations. Very similar values for the effective vibrating masses were extracted, suggesting comparable covalency of the bonding interaction between the metal atom and its ligands, while the Mössbauer lattice temperatures show a softening of the lattice for [Fe(II)(Hmmi)(2)]-(DNA monomer) with respect to Fe(II)-(DNA monomer) condensate.

  4. 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.

  5. The NASA-Ames Research Center stratospheric aerosol model. 2. Sensitivity studies and comparison with observatories

    NASA Technical Reports Server (NTRS)

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

    1979-01-01

    Sensitivity tests were performed on a one-dimensional, physical-chemical model of the unperturbed stratospheric aerosols, and model calculations were compared with observations. The tests and comparisons suggest that coagulation controls the particle number mixing ratio, although the number of condensation nuclei at the tropopause and the diffusion coefficient at high altitudes are also important. The sulfur gas source strength and the aerosol residence time are much more important than the supply of condensation nuclei in establishing mass and large particle concentrations. The particle size is also controlled mainly by gas supply and residence time. In situ observations of the aerosols and laboratory measurements of aerosols, parameters that can provide further information about the physics and chemistry of the stratosphere and the aerosols found there are provided.

  6. Airborne measurements of cloud condensation nuclei using a new continuous-flow streamwise thermal-gradient CCN chamber

    NASA Astrophysics Data System (ADS)

    Roberts, G. C.; Nenes, A.; Vanreken, T.; Rissman, T.; Conant, W. C.; Varutbangkul, V.; Jonsson, H. H.; Flagan, R. C.; Seinfeld, J. H.; Ramanathan, V.

    2003-04-01

    A light-weight continuous-flow thermal gradient diffusion chamber was developed for autonomous operation in airborne studies employing a novel technique of generating a supersaturation along the streamwise axis of the instrument. A vertical cylindrical column, whose surfaces are wetted and exposed to an increasing temperature gradient along the vertical axis, constitutes the chamber volume. This design exploits the differences in diffusion between water vapor and heat to maintain a uniform supersaturation along the streamwise axis of the chamber, which maximizes the growth rate of activated droplets; thereby enhancing the performance of the instrument. The current CCN instrument provides measurements of CCN between 0.13% and 3% supersaturation at a sampling rate sufficient for airborne operation. We have successfully tested the instrument on airborne experiments during the Cirrus Regional Study of Tropical Anvils and Cirrus Layers - Florida Area Cirrus Experiment (CRYSTAL-FACE) in July 2002. The results from the CRYSTAL-FACE campaign have yielded a remarkably good aerosol/CCN closure at 0.2 and 0.8% supersaturation. CCN concentrations were measured with a sampling resolution of 1Hz at a fixed supersaturation and compared to dry aerosol size distributions on one-minute intervals. An aerosol-cloud microphysical closure was also performed using the observed updraft velocity and below-cloud aerosol properties in a detailed adiabatic cloud activation model. The model accurately predicts the cloud drop concentration 100 m above cloud base in warm tropical cumulus.

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

    DOE PAGES

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

    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

  8. 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.

  9. 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.

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

    DOE PAGES

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

    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

  11. Photochemistry of Model Organic Aerosol Systems

    NASA Astrophysics Data System (ADS)

    Mang, S. A.; Bateman, A. P.; Dailo, M.; Do, T.; Nizkorodov, S. A.; Pan, X.; Underwood, J. S.; Walser, M. L.

    2007-05-01

    Up to 90 percent of urban aerosol particles have been shown to contain organic molecules. Reactions of these particles with atmospheric oxidants and/or sunlight result in large changes in their composition, toxicity, and ability to act as cloud condensation nuclei. For this reason, chemistry of model organic aerosol particles initiated by oxidation and direct photolysis is of great interest to atmospheric, climate, and health scientists. Most studies in this area have focused on identifying the products of oxidation of the organic aerosols, while the products of direct photolysis of the resulting molecules remaining in the aerosol particle have been left mostly unexplored. We have explored direct photolytic processes occurring in selected organic aerosol systems using infrared cavity ringdown spectroscopy to identify small gas phase products of photolysis, and mass-spectrometric and photometric techniques to study the condensed phase products. The first model system was secondary organic aerosol formed from the oxidation of several monoterpenes by ozone in the presence and absence of NOx, under different humidities. The second system modeled after oxidatively aged primary organic aerosol particles was a thin film of either alkanes or saturated fatty acids oxidized in several different ways, with the oxidation initiated by ozone, chlorine atom, or OH. In every case, the general conclusion was that the photochemical processing of model organic aerosols is significant. Such direct photolysis processes are believed to age organic aerosol particles on time scales that are short compared to the particles' atmospheric lifetimes.

  12. Marine aerosol formation from biogenic iodine emissions.

    PubMed

    O'Dowd, Colin D; Jimenez, Jose L; Bahreini, Roya; Flagan, Richard C; Seinfeld, John H; Hämeri, Kaarle; Pirjola, Liisa; Kulmala, Markku; Jennings, S Gerard; Hoffmann, Thorsten

    2002-06-01

    The formation of marine aerosols and cloud condensation nuclei--from which marine clouds originate--depends ultimately on the availability of new, nanometre-scale particles in the marine boundary layer. Because marine aerosols and clouds scatter incoming radiation and contribute a cooling effect to the Earth's radiation budget, new particle production is important in climate regulation. It has been suggested that sulphuric acid derived from the oxidation of dimethyl sulphide is responsible for the production of marine aerosols and cloud condensation nuclei. It was accordingly proposed that algae producing dimethyl sulphide play a role in climate regulation, but this has been difficult to prove and, consequently, the processes controlling marine particle formation remains largely undetermined. Here, using smog chamber experiments under coastal atmospheric conditions, we demonstrate that new particles can form from condensable iodine-containing vapours, which are the photolysis products of biogenic iodocarbons emitted from marine algae. Moreover, we illustrate, using aerosol formation models, that concentrations of condensable iodine-containing vapours over the open ocean are sufficient to influence marine particle formation. We suggest therefore that marine iodocarbon emissions have a potentially significant effect on global radiative forcing.

  13. Marine aerosol formation from biogenic iodine emissions.

    PubMed

    O'Dowd, Colin D; Jimenez, Jose L; Bahreini, Roya; Flagan, Richard C; Seinfeld, John H; Hämeri, Kaarle; Pirjola, Liisa; Kulmala, Markku; Jennings, S Gerard; Hoffmann, Thorsten

    2002-06-01

    The formation of marine aerosols and cloud condensation nuclei--from which marine clouds originate--depends ultimately on the availability of new, nanometre-scale particles in the marine boundary layer. Because marine aerosols and clouds scatter incoming radiation and contribute a cooling effect to the Earth's radiation budget, new particle production is important in climate regulation. It has been suggested that sulphuric acid derived from the oxidation of dimethyl sulphide is responsible for the production of marine aerosols and cloud condensation nuclei. It was accordingly proposed that algae producing dimethyl sulphide play a role in climate regulation, but this has been difficult to prove and, consequently, the processes controlling marine particle formation remains largely undetermined. Here, using smog chamber experiments under coastal atmospheric conditions, we demonstrate that new particles can form from condensable iodine-containing vapours, which are the photolysis products of biogenic iodocarbons emitted from marine algae. Moreover, we illustrate, using aerosol formation models, that concentrations of condensable iodine-containing vapours over the open ocean are sufficient to influence marine particle formation. We suggest therefore that marine iodocarbon emissions have a potentially significant effect on global radiative forcing. PMID:12050661

  14. CCN activation of ambient and "synthetic ambient" urban aerosol

    NASA Astrophysics Data System (ADS)

    Burkart, Julia; Reischl, Georg; Steiner, Gerhard; Bauer, Heidi; Leder, Klaus; Kistler, Magda; Puxbaum, Hans; Hitzenberger, R.

    2013-05-01

    In this study, the Cloud Condensation Nuclei (CCN) activation properties of the urban aerosol in Vienna, Austria, were investigated in a long term (11 month) field study. Filter samples of the aerosol below 100 nm were taken in parallel to these measurements, and later used to generate "synthetic ambient" aerosols. Activation parameters of this "synthetic ambient" aerosol were also obtained. Hygroscopicity parameters κ [1] were calculated both for the urban and the "synthetic ambient" aerosol and also from the chemical composition. Average κ for the "synthetic ambient" aerosol ranged from 0.20 to 0.30 with an average value of 0.24, while the κ from the chemical composition of this "synthetic ambient" aerosol was significantly higher (average 0.43). The full results of the study are given elsewhere [2,3].

  15. 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.

  16. 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.

  17. 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...

  18. 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

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

    NASA Astrophysics Data System (ADS)

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

    2014-12-01

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

  20. Understanding the Processes Controlling Aerosol-Cloud Interactions in the Arctic Marine Boundary Layer

    NASA Astrophysics Data System (ADS)

    Browse, J.; Carslaw, K. S.; Pringle, K.; Mann, G.; Reddington, C.; Brooks, I. M.; Mulcahy, J.; Young, G.; Allan, J. D.; Liu, D.; Trembath, J.; Dean, A.; Yoshioka, M.

    2015-12-01

    Here we use multiple configurations of the UKCA chemistry and aerosol scheme in a global climate model, capable of simulating cloud condensation nuclei (CCN) and cloud droplet number, to understand the processes controlling aerosol-cloud interactions in the marine Arctic boundary layer. Evaluation against an unprecedented number of aerosol and cloud observations made available through the Global Aerosol Synthesis and Science Project (GASSP), International Arctic Systems for Observing the Atmosphere (IASOA) and the 2013 ACCACIA campaign, suggest that Arctic summertime CCN is well represented in the model. Sensitivity studies indicate that DMS derived nucleation events are the primary source of Arctic summertime aerosol increasing mean (median) surface CCN concentrations north of 70N from 21(14) cm-3 to 46(33) cm-3. However, evaluation against observed aerosol size distributions suggests that UKCA overestimates nucleation mode (~10nm) particle concentrations either due to overestimation of boundary layer nucleation rates or underestimation of the Arctic marine boundary layer condensation sink.

  1. Flood or drought: how do aerosols affect precipitation?

    PubMed

    Rosenfeld, Daniel; Lohmann, Ulrike; Raga, Graciela B; O'Dowd, Colin D; Kulmala, Markku; Fuzzi, Sandro; Reissell, Anni; Andreae, Meinrat O

    2008-09-01

    Aerosols serve as cloud condensation nuclei (CCN) and thus have a substantial effect on cloud properties and the initiation of precipitation. Large concentrations of human-made aerosols have been reported to both decrease and increase rainfall as a result of their radiative and CCN activities. At one extreme, pristine tropical clouds with low CCN concentrations rain out too quickly to mature into long-lived clouds. On the other hand, heavily polluted clouds evaporate much of their water before precipitation can occur, if they can form at all given the reduced surface heating resulting from the aerosol haze layer. We propose a conceptual model that explains this apparent dichotomy.

  2. 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.

  3. 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. PMID:24572423

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

    NASA Astrophysics Data System (ADS)

    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.

    2014-02-01

    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.

  5. 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.

  6. 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.

  7. 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.

  8. Is formation of NH4NO3 a critical factor for the growth of > 10 nm new particles to cloud condensation nuclei size in marine boundary layer?

    NASA Astrophysics Data System (ADS)

    Liu, X.; Zhu, Y.; Gao, H.; Zhang, T.; Yao, X.

    2013-12-01

    In the last three decades, huge efforts have been taken to improve understanding of the relationship between ambient nucleation of new particles and its impact on the climate in marine boundary layer (MBL), e.g., CLAW hypothesis and studies related. However, only >40-50 nm new particles could be activated as cloud condensation nuclei (CCN) under typical range of water supersatuations occurring in MBL. The knowledge gap still existed, i.e., which chemicals are critical factors in growing nucleated particles to CCN size in MBL. In this study, we found that nucleated particles in MBL cannot grow over 40 nm in absence of strong formation of NH4NO3. However, the strong formation of NH4NO3 together with organics can grow nucleated particles close to or over 50 nm in MBL. These indicate that the strong formation of NH4NO3 is a critical factor to grow nucleated particles to CCN size in MBL. However, the strong formation of NH4NO3 occurred only in polluted air mass in MBL. Thus, ambient nucleation of new particles in clear and remote MBL is probably not a source of CCN due to lack of a strong formation of NH4NO3 and the nucleation may have no impact on the climate.

  9. 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

  10. 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

    2014-08-01

    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

  11. Are anthropogenic aerosols affecting rainfall?

    NASA Astrophysics Data System (ADS)

    Junkermann, Wolfgang; Hacker, Jorg

    2013-04-01

    Modification of cloud microphysics by anthropogenic aerosols is well known since several decades. Whether the underlying processes leads to changes in precipitation is by far less confirmed. Several different factors affect the production of rain in a way that a causality between increasing aerosol load in the atmosphere and a change of annual rainfall is very difficult to confirm. What would be expected as an effect of additional cloud condensation nuclei is a shift in the spatial and temporal rainfall distribution towards a lower number of days with low rain intensity and more frequent or more vigorous single events. In fact such a shift has been observed in several locations worldwide and has been suggested to be caused by increasing aerosol load, however, without further specification of the nature and number of the aerosols involved. Measurements of aerosols which might be important for cloud properties are extremely sparse and no long term monitoring data sets are available up to now. The problem of missing long term aerosol data that could be compared to available long term meteorological data sets can possibly be resolved in certain areas where well characterized large anthropogenic aerosol sources were installed in otherwise pristine areas without significant changes in land use over several decades. We investigated aerosol sources and current aerosol number, size and spatial distributions with airborne measurements in the planetary boundary layer over two regions in Australia that are reported to suffer from extensive drought despite the fact that local to regional scale water vapor in the atmosphere is slowly and constantly increasing. Such an increase of the total water in the planetary boundary layer would imply also an increase in annual precipitation as observed in many other locations elsewhere. The observed decline of rainfall in these areas thus requires a local to regional scale physical process modifying cloud properties in a way that rain

  12. 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

  13. Complex organic matter in Titan's atmospheric aerosols from in situ pyrolysis and analysis.

    PubMed

    Israël, G; Szopa, C; Raulin, F; Cabane, M; Niemann, H B; Atreya, S K; Bauer, S J; Brun, J-F; Chassefière, E; Coll, P; Condé, E; Coscia, D; Hauchecorne, A; Millian, P; Nguyen, M-J; Owen, T; Riedler, W; Samuelson, R E; Siguier, J-M; Steller, M; Sternberg, R; Vidal-Madjar, C

    2005-12-01

    Aerosols in Titan's atmosphere play an important role in determining its thermal structure. They also serve as sinks for organic vapours and can act as condensation nuclei for the formation of clouds, where the condensation efficiency will depend on the chemical composition of the aerosols. So far, however, no direct information has been available on the chemical composition of these particles. Here we report an in situ chemical analysis of Titan's aerosols by pyrolysis at 600 degrees C. Ammonia (NH3) and hydrogen cyanide (HCN) have been identified as the main pyrolysis products. This clearly shows that the aerosol particles include a solid organic refractory core. NH3 and HCN are gaseous chemical fingerprints of the complex organics that constitute this core, and their presence demonstrates that carbon and nitrogen are in the aerosols.

  14. Complex organic matter in Titan's atmospheric aerosols from in situ pyrolysis and analysis.

    PubMed

    Israël, G; Szopa, C; Raulin, F; Cabane, M; Niemann, H B; Atreya, S K; Bauer, S J; Brun, J-F; Chassefière, E; Coll, P; Condé, E; Coscia, D; Hauchecorne, A; Millian, P; Nguyen, M-J; Owen, T; Riedler, W; Samuelson, R E; Siguier, J-M; Steller, M; Sternberg, R; Vidal-Madjar, C

    2005-12-01

    Aerosols in Titan's atmosphere play an important role in determining its thermal structure. They also serve as sinks for organic vapours and can act as condensation nuclei for the formation of clouds, where the condensation efficiency will depend on the chemical composition of the aerosols. So far, however, no direct information has been available on the chemical composition of these particles. Here we report an in situ chemical analysis of Titan's aerosols by pyrolysis at 600 degrees C. Ammonia (NH3) and hydrogen cyanide (HCN) have been identified as the main pyrolysis products. This clearly shows that the aerosol particles include a solid organic refractory core. NH3 and HCN are gaseous chemical fingerprints of the complex organics that constitute this core, and their presence demonstrates that carbon and nitrogen are in the aerosols. PMID:16319825

  15. 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.

  16. The impact of natural aerosols on Indian summer monsoon

    NASA Astrophysics Data System (ADS)

    Vinoj, V.; Wang, H.; Yoon, J.; Rasch, P.

    2011-12-01

    Atmospheric aerosols emitted from a variety of natural and anthropogenic sources impact the earth's radiation and water budget. Most of the studies in the recent past have been focusing on anthropogenic aerosols and their impact. However, natural aerosols like sea-salt and dust form the bulk of the aerosol mass loading in the atmosphere. For example, oceans cover about 70% of the earth's surface area and are a major source of sea-salt aerosols in the atmosphere. Sea-salt emission is the single largest contributor to natural aerosols and accounts for nearly half of the global aerosol optical depth. Dust emission, the counterpart over land, also contributes substantially to natural atmospheric aerosols. In addition to their direct effect on solar radiation, these aerosols also actively participate in cloud formation by acting as cloud condensation and ice nuclei and have indirect effects on clouds. Both sea-salt and dust particles are primarily formed by the action of winds that largely determine seasonal/annual variations in their source strength and atmospheric loading. Over the Indian Ocean region, especially the Arabian Sea is characterized by high winds during the monsoon that generate a large amount of sea-salt aerosols. Also these high winds mobilize large amount of dust aerosols in the northern Arabian Sea depending on wind direction. These natural aerosols together with anthropogenic emissions impact Indian monsoon precipitation. We use satellite observation of precipitation and column aerosol loading along with a global climate model (Community Atmosphere Model version 5, CAM5) to show that the variability of natural aerosols (i.e., sea-salt and dust) play an important role in modulating the Indian monsoon precipitation and the response of the monsoon system to anthropogenic aerosols. The effect of dust and sea-salt on precipitation is found to be opposite to each other. Our study suggests that the observed spatial and temporal trends in precipitation

  17. 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. PMID:24630589

  18. 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.

  19. 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.

  20. The role of Saharan dust in determining the first aerosol indirect effect

    NASA Astrophysics Data System (ADS)

    Shao, H.; Liu, G.

    2007-12-01

    Anthropogenic aerosols acting as cloud condensation nuclei affect Earth's radiative balance indirectly by changing cloud radiative properties. This so-called first aerosol indirect effect (AIE) has a potentially large but poorly quantified cooling effect. In modeling the aerosol indirect forcing, because the aerosol-cloud interaction is not resolved in global climate models (GCMs), cloud droplet number concentration is typically parameterized using an empirical relationship that directly relates droplet number concentration to aerosol number concentration based on the measurements between polluted and clean clouds. It is realized that the first AIE obtained in this way can be contaminated by the coherent variation in the pertinent variables such as cloud liquid water and the degree of entrainment mixing. However, the influence from changes in aerosol properties themselves has not received a deserved attention. Using satellite observations over eastern subtropical oceans, we show that over the north-eastern Atlantic the aerosols properties are distinct from the other regions due to the dust particles originating from Sahara desert. These dust particles may significantly reduce the efficiency of aerosols to act as cloud condensation nuclei. As a result, the locally observed first AIE from this region can be significantly deviated from global mean, even resulting in positive values. Because of the large areal fraction of this region, ignoring the influence from the northern Africa dust particles will underestimate the globally averaged first AIE approximately by half.

  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. 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

  3. [Investigation of Aerosol Mixed State and CCN Activity in Nanjing].

    PubMed

    Zhu, Lin; Ma, Yan; Zheng, Jun; Li, Shi-zheng; Wang, Li-peng

    2016-04-15

    During 11-18 September 2014, the size-resolved aerosol Cloud Condensation Nuclei (CCN) activity and mixing state were measured using Cloud Condensation Nuclei Counter (CCNC), Aerosol Particle Mass (APM) and Scanning Mobility Particle Sizer (SMPS). The results showed that aerosols mainly existed as an internal mixture. For 76, 111, 138 and 181 nm particles, black carbon (BC) accounted for 5.4%, 10%, l0.7% and 6.7% of the particle mass, but as high as 51%, 57%, 70% and 59% of the particle number concentrations, respectively, suggesting that BC was a type of important condensation nuclei in the atmosphere and made significant contributions to particle numbers. The occasionally observed external mixtures were mainly present in 111 and 138 nm particles. The critical supersaturation was 0.25%, 0.13%, 0.06% and 0.015% for 76, 111, 138 and 181 nm particles, respectively. Precipitation and haze had significant effects on the particle CCN activity. The hygroscopicity parameter K was 0.37, 0.29 and 0.39 in rainy, clear and hazy days, respectively. Particle density and CCN activity were impacted by chemical compositions. Compared with clear days, higher contents of inorganic salts and lower contents of organics were found on hazy days, accompanied by lower particle density and higher CCN activity. PMID:27548938

  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. 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

  6. 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

  7. 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.

  8. Balloonborne ozone and aerosol measurements in the antarctic ozone hole

    SciTech Connect

    Hofmann, D.J.; Harder, J.W.; Rolf, S.R.; Rosen, J.M. )

    1987-01-01

    The National Ozone Expedition (NOZE) was mounted in 1986 using winter fly-in flights to McMurdo Station in August, which is approximately the time the ozone reduction begins. The University of Wyoming Atmospheric Physics group participated in this expedition through balloonborne measurements of the vertical distribution of ozone and aerosol particles. Between 24 August and 6 November, 33 ozone soundings, 6 aerosol sounding, and 3 condensation nuclei soundings were conducted using polyethylene balloons which were able to penetrate the cold (< {minus}80C) antarctic stratosphere. The authors summarize these results here.

  9. Global aerosol effects on convective clouds

    NASA Astrophysics Data System (ADS)

    Wagner, Till; Stier, Philip

    2013-04-01

    Atmospheric aerosols affect cloud properties, and thereby the radiation balance of the planet and the water cycle. The influence of aerosols on clouds is dominated by increase of cloud droplet and ice crystal numbers (CDNC/ICNC) due to enhanced aerosols acting as cloud condensation and ice nuclei. In deep convective clouds this increase in CDNC/ICNC is hypothesised to increase precipitation because of cloud invigoration through enhanced freezing and associated increased latent heat release caused by delayed warm rain formation. Satellite studies robustly show an increase of cloud top height (CTH) and precipitation with increasing aerosol optical depth (AOD, as proxy for aerosol amount). To represent aerosol effects and study their influence on convective clouds in the global climate aerosol model ECHAM-HAM, we substitute the standard convection parameterisation, which uses one mean convective cloud for each grid column, with the convective cloud field model (CCFM), which simulates a spectrum of convective clouds, each with distinct values of radius, mixing ratios, vertical velocity, height and en/detrainment. Aerosol activation and droplet nucleation in convective updrafts at cloud base is the primary driver for microphysical aerosol effects. To produce realistic estimates for vertical velocity at cloud base we use an entraining dry parcel sub cloud model which is triggered by perturbations of sensible and latent heat at the surface. Aerosol activation at cloud base is modelled with a mechanistic, Köhler theory based, scheme, which couples the aerosols to the convective microphysics. Comparison of relationships between CTH and AOD, and precipitation and AOD produced by this novel model and satellite based estimates show general agreement. Through model experiments and analysis of the model cloud processes we are able to investigate the main drivers for the relationship between CTH / precipitation and AOD.

  10. 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.

  11. 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

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

    DOE PAGES

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

    2014-09-09

    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 goodmore » 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.« less

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

    DOE PAGES

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

    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

  14. 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.

  15. 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.

  16. 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

  17. 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.

  18. A Physically-Based Estimate of Radiative Forcing by Anthropogenic Sulfate Aerosol

    SciTech Connect

    Ghan, Steven J. ); Easter, Richard C. ); Chapman, Elaine G. ); Abdul-Razzak, Hayder; Zhang, Yang ); Leung, Ruby ); Laulainen, Nels S. ); Saylor, Rick D. ); Zaveri, Rahul A. )

    2001-04-01

    Estimates of direct and indirect radiative forcing by anthropogenic sulfate aerosols from an integrated global aerosol and climate modeling system are presented. A detailed global tropospheric chemistry and aerosol model that predicts concentrations of oxidants as well as aerosols and aerosol precursors, is coupled to a general circulation model that predicts both cloud water mass and cloud droplet number. Both number and mass of several externally-mixed aerosol size modes are predicted, with internal mixing assumed for the different aerosol components within each mode. Predicted aerosol species include sulfate, organic and black carbon, soil dust, and sea salt. The models use physically-based treatments of aerosol radiative properties (including dependence on relative humidity) and aerosol activation as cloud condensation nuclei. Parallel simulations with and without anthropogenic sulfate aerosol are performed for a global domain. The global and annual mean direct and indirect radiative forcing due to anthropogenic sulfate are estimated to be -0.3 to -0.5 and -1.5 to -3.0 W m-2, respectively. The radiative forcing is sensitive to the model's horizontal resolution, the use of predicted vs. analyzed relative humidity, the prediction vs. diagnosis of aerosol number and droplet number, and the parameterization of droplet collision/coalescence. About half of the indirect radiative forcing is due to changes in droplet radius and half to increased cloud liquid water.

  19. Aerosols in clean and smoky air at Bozeman, Montana

    NASA Astrophysics Data System (ADS)

    Shaw, J. A.; Thomas, M.; Lathem, T. L.; Shaw, G. E.; Nenes, A.; Pust, N.; Repasky, K. S.

    2010-12-01

    The northern Rocky Mountain region of the United States is a natural laboratory for studying aerosols in a relatively uncontaminated environment punctuated by episodes of wildfire smoke. In autumn 2009, we conducted a field experiment at Montana State University in Bozeman, Montana to characterize the boundary layer aerosols as they transition from smoky periods to relatively clean background air. Physical and chemical properties of the aerosols were conducted, including high time resolution of Cloud Condensation Nuclei and inter comparison with AERONET data during times of deep atmospheric mixing. The key results of this experiment are: 1) the air in this northern Rocky Mountain location is surprisingly pristine with frequent aerosol size distributions devoid of a an accumulation mode; 2) periods of night-time growth of Aitken-mode aerosols were observed; 3) a persistent diurnal variation occurred, with upslope daytime winds bringing aerosols exhibiting moderate anthropogenic influence , and down slope nighttime winds bringing aerosols with weak accumulation mode; 4) the smoke aerosol was weakly soluble; and 5) satisfactory agreement was found between the inverted estimate of the fine mode aerosol from AERONET solar radiometry with that measured in situ.

  20. Initial steps of aerosol growth

    NASA Astrophysics Data System (ADS)

    Kulmala, M.; Laakso, L.; Lehtinen, K. E. J.; Riipinen, I.; Dal Maso, M.; Anttila, T.; Kerminen, V.-M.; Hõrrak, U.; Vana, M.; Tammet, H.

    2004-12-01

    The formation and growth of atmospheric aerosols depend on several steps, namely nucleation, initial steps of growth and subsequent - mainly condensational - growth. This work focuses on the initial steps of growth, meaning the growth right after nucleation, where the interplay of curvature effects and thermodynamics has a significant role on the growth kinetics. More specifically, we investigate how ion clusters and aerosol particles grow from 1.5 nm to 20 nm (diameter) in atmospheric conditions using experimental data obtained by air ion and aerosol spectrometers. The measurements have been performed at a boreal forest site in Finland. The observed trend that the growth rate seems to increase as a function of size can be used to investigate possible growth mechanisms. Such a growth rate is consistent with a recently suggested nano-Köhler mechanism, in which growth is activated at a certain size with respect to condensation of organic vapors. The results also imply that charge-enhanced growth associated with ion-mediated nucleation plays only a minor role in the initial steps of growth, since it would imply a clear decrease of the growth rate with size. Finally, further evidence was obtained on the earlier suggestion that atmospheric nucleation and the subsequent growth of fresh nuclei are likely to be uncoupled phenomena via different participating vapors.

  1. Initial steps of aerosol growth

    NASA Astrophysics Data System (ADS)

    Kulmala, O.; Laakso, L.; Lehtinen, K. E. J.; Riipinen, I.; Dal Maso, M.; Anttila, T.; Kerminen, V.-M.; Hõrrak, U.; Vana, M.; Tammet, H.

    2004-09-01

    The formation and growth of atmospheric aerosols depend on several steps, namely nucleation, initial steps of growth and subsequent - mainly condensational - growth. This work focuses on the initial steps of growth, meaning the growth right after nucleation, where the interplay of curvature effects and thermodynamics has a significant role on the growth kinetics. More specifically, we investigate how ion clusters and aerosol particles grow from 1.5 nm to 20 nm in atmospheric conditions using experimental data obtained by air ion and aerosol spectrometers. The measurements have been performed at a boreal forest site in Finland. The observed trend that the growth rate seems to increase as a function of size can be used to investigate possible growth mechanisms. Such a growth rate is consistent with a recently suggested nano-Köhler mechanism, in which growth is activated at a certain size with respect to condensation of organic vapors. The results also imply that charge-enhance growth associated with ion-mediated nucleation plays only a minor role in the initial steps of growth, since it would imply a clear decrease of the growth rate with size. Finally, further evidence was obtained on the earlier suggestion that atmospheric nucleation and the subsequent growth of fresh nuclei are likely to be uncoupled phenomena via different participating vapors.

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

    PubMed

    Koren, Ilan; Dagan, Guy; Altaratz, Orit

    2014-06-01

    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.

  3. An interfacial mechanism for cloud droplet formation on organic aerosols

    NASA Astrophysics Data System (ADS)

    Ruehl, Christopher R.; Davies, James F.; Wilson, Kevin R.

    2016-03-01

    Accurate predictions of aerosol/cloud interactions require simple, physically accurate parameterizations of the cloud condensation nuclei (CCN) activity of aerosols. Current models assume that organic aerosol species contribute to CCN activity by lowering water activity. We measured droplet diameters at the point of CCN activation for particles composed of dicarboxylic acids or secondary organic aerosol and ammonium sulfate. Droplet activation diameters were 40 to 60% larger than predicted if the organic was assumed to be dissolved within the bulk droplet, suggesting that a new mechanism is needed to explain cloud droplet formation. A compressed film model explains how surface tension depression by interfacial organic molecules can alter the relationship between water vapor supersaturation and droplet size (i.e., the Köhler curve), leading to the larger diameters observed at activation.

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

    PubMed

    Koren, Ilan; Dagan, Guy; Altaratz, Orit

    2014-06-01

    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. PMID:24904161

  5. The effect of the number of condensed phases modeled on aerosol behavior during an induced steam generator tube rupture sequence

    SciTech Connect

    Bixler, N.E.; Schaperow, J.H.

    1998-06-01

    VICTORIA is a mechanistic computer code designed to analyze fission product behavior within a nuclear reactor coolant system (RCS) during a severe accident. It provides detailed predictions of the release of radioactive and nonradioactive materials from the reactor core and transport and deposition of these materials within the RCS. A recently completed independent peer review of VICTORIA, while confirming the overall adequacy of the code, recommended a number of modeling improvements. One of these recommendations, to model three rather than a single condensed phase, is the focus of the work reported here. The recommendation has been implemented as an option so that either a single or three condensed phases can be treated. Both options have been employed in the study of fission product behavior during an induced steam generator tube rupture sequence. Differences in deposition patterns and mechanisms predicted using these two options are discussed.

  6. Holistic aerosol evaluation using synthesized aerosol aircraft measurements

    NASA Astrophysics Data System (ADS)

    Watson-Parris, Duncan; Reddington, Carly; Schutgens, Nick; Stier, Philip; Carslaw, Ken; Liu, Dantong; Allan, James; Coe, Hugh

    2016-04-01

    Despite ongoing efforts there are still large uncertainties in aerosol concentrations and loadings across many commonly used GCMs. This in turn leads to large uncertainties in the contributions of the direct and indirect aerosol forcing on climate. However, constraining these fields using earth observation data, although providing global coverage, is problematic for many reasons, including the large uncertainties in retrieving aerosol loadings. Additionally, the inability to retrieve aerosols in or around cloudy scenes leads to further sampling biases (Gryspeerdt 2015). Many in-situ studies have used regional datasets to attempt to evaluate the model uncertainties, but these are unable to provide an assessment of the models ability to represent aerosols properties on a global scale. Within the Global Aerosol Synthesis and Science Project (GASSP) we have assembled the largest collection of quality controlled, in-situ aircraft observations ever synthesized to a consistent format. This provides a global set of in-situ measurements of Cloud Condensation Nuclei (CCN) and Black Carbon (BC), amongst others. In particular, the large number of vertical profiles provided by this aircraft data allows us to investigate the vertical structure of aerosols across a wide range of regions and environments. These vertical distributions are particularly valuable when investigating the dominant processes above or below clouds where remote sensing data is not available. Here we present initial process-based assessments of the BC lifetimes and vertical distributions of CCN in the HadGEM-UKCA and ECHAM-HAM models using this data. We use point-by-point based comparisons to avoid the sampling issues associated with comparing spatio-temporal aggregations.

  7. Aerosols-Cloud-Microphysics Interactions in Tropical Cyclone Earl

    NASA Astrophysics Data System (ADS)

    Luna-Cruz, Yaitza

    Aerosols-cloud-microphysical processes are largely unknown in their influence on tropical cyclone evolution and intensification; aerosols possess the largest uncertainty. For example: What is the link between aerosols and cloud microphysics quantities? How efficient are the aerosols (i.e. dust from the Saharan Air Layer -SAL) as cloud condensation nuclei (CCN) and ice nuclei (IN)? Does aerosols affect the vertical velocity, precipitation rates, cloud structure and lifetime? What are the dominant factors and in which sectors of the tropical cyclone? To address some of the questions in-situ microphysics measurements from the NASA DC-8 aircraft were obtained during the Genesis and Rapid Intensification Processes (GRIP) 2010 field campaign. A total of four named storms (Earl, Gaston, Karl and Mathew) were sampled. Earl presented the excellent opportunity to study aerosols-cloud-microphysics interactions because Saharan dust was present and it underwent rapid intensification. This thesis seeks to explore hurricane Earl to develop a better understanding of the relationship between the SAL aerosols and cloud microphysics evolution. To assist in the interpretation of the microphysics observations, high resolution numerical simulations of hurricane Earl were performed using the Weather Research and Forecasting (WRF-ARW) model with the new Aerosol-Aware bulk microphysics scheme. This new version of Thompson scheme includes explicit activation of cloud condensation nuclei (CCN) from a major CCN source (i.e. sulfates and sea salt) and explicit ice nucleation (IN) from mineral dust. Three simulations are performed: (1) the Control case with the old Thompson scheme and initial conditions from GFS model, (2) the Aerosol-Aware first baseline case with GOCART aerosol module as an input conditions, and (3) the Aerosol-Aware increase case in which the GOCART aerosols concentrations were increased significantly. Overall, results of model simulations along with aircraft observations

  8. 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.

  9. 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

  10. Evaluating the potential impact of marine organic aerosols on climate assessments

    NASA Astrophysics Data System (ADS)

    Meskhidze, N.; Gantt, B.; Xu, J.

    2011-12-01

    Natural aerosols influence clouds and the hydrological cycle by their ability to act as cloud condensation nuclei (CCN). Because the anthropogenic contribution to climate forcing represents the difference between the total forcing and that from natural aerosols, understanding background aerosols is necessary to evaluate the influences of anthropogenic aerosols on cloud reflectivity and persistence (so-called indirect radiative forcing) and on precipitation. The effects of marine organic aerosols on microphysical properties of shallow clouds are explored using the NCAR Community Atmosphere Model (CAM5.0), coupled with the PNNL Modal Aerosol Model. Organic enrichment of sea spray is estimated using newly developed wind speed dependent size-resolved source function, while production of secondary organic aerosol of marine origin is inferred from the ocean emissions of biogenic trace gases. Model-predicted abundance of CCN in remote marine atmosphere is compared to satellite and in-situ data. Simulations show that over biologically productive ocean waters organic aerosols of marine origin can contribute up to 20% increase in CCN (at a supersaturation of 0.2%) number concentrations. Corresponding changes associated with cloud properties (liquid water path and droplet number) can reduce global annual mean indirect radiative forcing of anthropogenic aerosol by 0.1 Wm-2 or 8%. This study suggests that neglecting the effects of marine organic aerosol in climate models could result in overprediction of aerosol indirect effect.

  11. Aerosol Microphysical and Macrophysical Effects on Deep Convective Clouds

    NASA Astrophysics Data System (ADS)

    Yuan, T.; Li, Z.; Wilcox, E. M.; Oreopoulos, L.; Remer, L. A.; Yu, H.; Platnick, S. E.; Posselt, D. J.; Zhang, Z.; Martins, J. V.

    2014-12-01

    We illustrate a conceptual model of hydrometeor vertical development inside a convective cloud and its utility in studying of aerosol-DCC interactions. Both case studies and ensemble means are used to investigate aerosol-DCC interactions. We identify a few scenarios where possible signal of aerosol effect on DCC may be extracted. The results show a consistent and physically sound picture of aerosols affecting DCC microphysics as well as macrophysical properties. Specifically, pollutions and smokes are shown to consistently decrease ice particle size. On the contrary, dust particles close to source regions are shown to make cloud ice particle size more maritime like. We postulate that dust may achieve this by acting as either heterogeneous ice nuclei or giant cloud condensation nuclei. This contrast between smoke or pollution and dust also exists for their effects on cloud glaciation temperature. Smoke and pollution aerosols are shown to decrease glaciation temperature while dust particles do the opposite. Possible Implications of our results for studying aerosol indirect forcing, cirrus cloud properties, troposphere-stratosphere water vapor exchange and cloud latent heating are discussed.

  12. 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.

  13. 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.

  14. 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.

  15. Experimentally measured morphology of biomass burning aerosol and its impacts on CCN ability

    NASA Astrophysics Data System (ADS)

    Giordano, M.; Espinoza, C.; Asa-Awuku, A.

    2014-05-01

    This study examines the morphological properties of freshly emitted and atmospherically aged aerosols from biomass burning. The impacts of particle morphology assumptions on hygroscopic predictions are examined. Chamber experiments were conducted at the UC-Riverside Center for Environmental Research and Technology (CE-CERT) Atmospheric Processes Lab using two biomass fuel sources, manzanita and chamise. Morphological data was obtained through the use of an aerosol particle mass analyzer (APM), scanning mobility particle sizer (SMPS) system and transmission electron microscopy (TEM). Data from these instruments was used to calculate both a dynamic shape factor and a fractal-like dimension for the biomass burning emissions. This data was then used with κ-Köhler theory to adjust the calculated hygroscopicity for experimentally determined morphological characteristics of the aerosol. Laboratory measurement of biomass burning aerosol from two chaparral fuels show that particles are non-spherical with dynamic shape factors greater than 1.15 for aerosol sizes relevant to cloud condensation nuclei (CCN) activation. Accounting for particle morphology can shift the hygroscopicity parameter κ by 0.15 or more. To our knowledge, this work provides the first laboratory chamber measurements of morphological characteristics for biomass burning cloud condensation nuclei and provides experimental particle shape evidence to support the variation in reported hygroscopicities of the complex aerosol.

  16. Experimentally measured morphology of biomass burning aerosol and its impacts on CCN ability

    NASA Astrophysics Data System (ADS)

    Giordano, M.; Espinoza, C.; Asa-Awuku, A.

    2015-02-01

    This study examines the morphological properties of freshly emitted and atmospherically aged aerosols from biomass burning. The impacts of particle morphology assumptions on hygroscopic predictions are examined. Chamber experiments were conducted at the University of California, Riverside, Center for Environmental Research and Technology (CE-CERT) atmospheric processes lab using two biomass fuel sources: manzanita and chamise. Morphological data was obtained through the use of an aerosol particle mass analyzer (APM), scanning mobility particle sizer (SMPS) system and transmission electron microscope (TEM). Data from these instruments was used to calculate both a dynamic shape factor and a fractal-like dimension for the biomass burning emissions. This data was then used with κ-Köhler theory to adjust the calculated hygroscopicity for experimentally determined morphological characteristics of the aerosol. Laboratory measurement of biomass burning aerosol from two chaparral fuels show that particles are nonspherical with dynamic shape factors greater than 1.15 for aerosol sizes relevant to cloud condensation nuclei (CCN) activation. Accounting for particle morphology can shift the hygroscopicity parameter by 0.15 or more. To our knowledge, this work provides the first laboratory chamber measurements of morphological characteristics for biomass burning cloud condensation nuclei and provides experimental particle shape evidence to support the variation in reported hygroscopicities of the complex aerosol.

  17. 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.

  18. 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.

  19. 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.

  20. Biogenic Contributions to Summertime Arctic Aerosol: Observations of Aerosol Composition from the Netcare 2014 Aircraft Campaign

    NASA Astrophysics Data System (ADS)

    Willis, M. D.; Burkart, J.; Koellner, F.; Schneider, J.; Bozem, H.; Hoor, P. M.; Brauner, R.; Herber, A. B.; Leaitch, W. R.; Abbatt, J.

    2014-12-01

    The Arctic is a complex and poorly studied aerosol environment, impacted by strong anthropogenic contributions during winter months and by regional sources in cleaner summer months. In order to gain a predictive understanding of the changing climate in this region, it is necessary to understand the balance between these two aerosol sources to clarify how aerosol might be altered by or contribute to climate change. We present results of vertically resolved, submicron aerosol composition from an Aerodyne high-resolution aerosol mass spectrometer (AMS) during the NETCARE 2014 Polar6 aircraft campaign. The campaign was based in the high Arctic, at Resolute, NU (74°N), allowing measurements from 60 to 2900 meters over ice, open water and near the ice-edge. Concurrent measurements aboard the Polar6 included ultrafine and accumulation mode particle number and size, cloud condensation nuclei concentrations, trace gas concentrations and single particle composition. Aerosol vertical profiles measured by the AMS can be broadly characterized into two regimes corresponding to different meteorological conditions: the first with very low aerosol loading (<0.1 μg/m3) at low altitudes compared to that aloft and high numbers of nucleation mode particles, and the second with higher concentrations at lower levels. This second regime was associated with low concentrations of nucleation mode particles, and higher observable levels of methane sulphonic acid (MSA) from AMS measurements at low altitudes. MSA, produced during the oxidation of dimethyl sulphide, is a marker for the contribution of ocean-derived biogenic sulphur to particulate sulphur and could be identified and quantified using the high-resolution AMS. MSA to sulphate ratios were observed to increase towards lower altitudes, suggesting a contribution to aerosol loading from the ocean. In addition, we present measurements of aerosol neutralization and the characteristics of organic aerosol that relate to the growth of

  1. Characterizing interactions between aerosols and cloud droplets in marine boundary layer clouds

    NASA Astrophysics Data System (ADS)

    Andersen, Hendrik; Cermak, Jan

    2016-04-01

    This contribution presents a method to characterize the nonlinearities of interactions between aerosols and cloud droplets in marine boundary layer clouds based on global MODIS observations. Clouds play a crucial role in the climate system as their radiative properties and precipitation patterns significantly impact the Earth's energy balance. Cloud properties are determined by environmental conditions, as cloud formation requires the availability of water vapour ("precipitable water") and condensation nuclei in sufficiently saturated conditions. The ways in which aerosols as condensation nuclei in particular influence the optical, micro- and macrophysical properties of clouds are one of the largest remaining uncertainties in climate-change research. In particular, cloud droplet size is believed to be impacted, and thereby cloud reflectivity, lifetime, and precipitation susceptibility. However, the connection between aerosols and cloud droplets is nonlinear, due to various factors and processes. The impact of aerosols on cloud properties is thought to be strongest with low aerosol loadings, whereas it saturates with high aerosol loadings. To gain understanding of the processes that govern low cloud water properties in order to increase accuracy of climate models and predictions of future changes in the climate system is thus of great importance. In this study, global Terra MODIS L3 data sets are used to characterize the nonlinearities of the interactions between aerosols and cloud droplets in marine boundary layer clouds. MODIS observations are binned in classes of aerosol loading to identify at what loading aerosol impact on cloud droplets is the strongest and at which loading it saturates. Results are connected to ERA-Interim and MACC data sets to identify connections of detected patterns to meteorology and aerosol species.

  2. 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.

  3. 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

  4. Halogenation processes of secondary organic aerosol and implications on halogen release mechanisms

    NASA Astrophysics Data System (ADS)

    Ofner, J.; Balzer, N.; Buxmann, J.; Grothe, H.; Schmitt-Kopplin, P.; Platt, U.; Zetzsch, C.

    2012-01-01

    Reactive halogen species (RHS), such as X·, X2 and HOX containing X = chlorine and/or bromine, are released by various sources like photo-activated sea-salt aerosol or from salt pans, and salt lakes. Despite many studies of RHS reactions, the potential of RHS reacting with secondary organic aerosol (SOA) and organic aerosol derived from biomass-burning (BBOA) has been neglected. Such reactions can constitute sources of gaseous organohalogen compounds or halogenated organic matter in the tropospheric boundary layer and can influence physicochemical properties of atmospheric aerosols. Model SOA from α-pinene, catechol, and guaiacol was used to study heterogeneous interactions with RHS. Particles were exposed to molecular chlorine and bromine in an aerosol smog-chamber in the presence of UV/VIS irradiation and to RHS released from simulated natural halogen sources like salt pans. Subsequently the aerosol was characterized in detail using a variety of physicochemical and spectroscopic methods. Fundamental features were correlated with heterogeneous halogenation, which result in new functional groups, changed UV/VIS absorption, or aerosol size distribution. However, the halogen release mechanisms were also found to be affected by the presence of organic aerosol. Those interaction processes, changing chemical and physical properties of the aerosol are likely to influence e.g. the ability of the aerosol to act as cloud condensation nuclei, its potential to adsorb other gases with low-volatility, or its contribution to radiative forcing and ultimately the Earth's radiation balance.

  5. 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

  6. 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

  7. 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.

  8. Aerosol measurements at the South Pole

    NASA Astrophysics Data System (ADS)

    Bodhaine, Barry A.; Deluisi, John J.; Harris, Joyce M.; Houmere, Pamela; Bauman, Sene

    1986-09-01

    Some results are given regarding the aerosol measurement program conducted by the NOAA at their atmospheric monitoring observatory at Amundsen-Scott Station, South Pole. The program consists of the continuous measurement of condensation nuclei (CN) concentration and aerosol scattering extinction coefficient. A time series of sodium, chlorine, and sulfur concentrations shows that the sulfur and CN records are similar and that the sodium, chlorine, and extinction coefficient records are similar. Large episodes of sodium are measured at the ground in the austral winter and are apparently caused by large-scale warming and weakening of the surface temperature inversion. The CN data show an annual cycle with a maximum exceeding 100 per cubic centimeter in the austral summer and a minimum of about 10 per cubic centimeter in the winter. The extinction coefficient data show an anual cycle markedly different from that of CN with a maximum in late winter, a secondary maximum in summer, and a minimum in May.

  9. 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. PMID:15703706

  10. The Role of Aerosols on Precipitation Processes

    NASA Technical Reports Server (NTRS)

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

    2006-01-01

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

  11. 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.

    2014-05-26

    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-phasemore » 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

  12. 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

  13. 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

  14. 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

  15. Water adsorption around oxalic acid aggregates: a molecular dynamics simulation of water nucleation on organic aerosols.

    PubMed

    Darvas, Maria; Picaud, Sylvain; Jedlovszky, Pál

    2011-11-28

    The phase behaviour of binary oxalic acid-water mixtures has been investigated by means of computer simulation techniques. Such mixtures play an important role in atmospheric processes, since the hydrogen bonding ability of oxalic acid molecules allows them to form aerosol particles. Water can in turn be readily adsorbed on the surface of such aerosol particles, which results in the formation of small ice grains. These grains are thus considered to be acting as cloud condensation nuclei, giving rise to the formation of ice clouds.

  16. 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.

  17. simplified aerosol representations in global modeling

    NASA Astrophysics Data System (ADS)

    Kinne, Stefan; Peters, Karsten; Stevens, Bjorn; Rast, Sebastian; Schutgens, Nick; Stier, Philip

    2015-04-01

    The detailed treatment of aerosol in global modeling is complex and time-consuming. Thus simplified approaches are investigated, which prescribe 4D (space and time) distributions of aerosol optical properties and of aerosol microphysical properties. Aerosol optical properties are required to assess aerosol direct radiative effects and aerosol microphysical properties (in terms of their ability as aerosol nuclei to modify cloud droplet concentrations) are needed to address the indirect aerosol impact on cloud properties. Following the simplifying concept of the monthly gridded (1x1 lat/lon) aerosol climatology (MAC), new approaches are presented and evaluated against more detailed methods, including comparisons to detailed simulations with complex aerosol component modules.

  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. Latitudinal and altitudinal variation of size distribution of stratospheric aerosols inferred from SAGE aerosol extinction coefficient measurements at two wavelengths

    NASA Technical Reports Server (NTRS)

    Yue, G. K.; Deepak, A.

    1984-01-01

    A method of retrieving aerosol size distribution from the measured extinction of solar radiation at wavelengths of 0.45 microns and 1.0 microns has recently been proposed. This method is utilized to obtain latitudinal and altitudinal variations of size distributions of stratospheric aerosols from the Stratospheric Aerosol and Gas Experiment data for March 1979. Small particles are found in the lower stratosphere of the tropical region, and large particles are found at higher altitudes and latitudes in both hemispheres. Results of this study are consistent with the suggestion that the upper troposphere in tropical regions is a source of condensation nuclei in the stratosphere, and they become mature as they move to higher altitudes and latitude.

  1. 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.

  2. 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.

  3. Study of the CCN formation as a function of aerosol components

    NASA Astrophysics Data System (ADS)

    Fanourgakis, George S.; Myriokefalitakis, Stelios; Kanakidou, Maria

    2016-04-01

    Understanding the role of aerosols in Earth's climate through direct and indirect effects has attracted a lot of attention over the last years. Due to the chemical complexity of aerosols along with the variety of the primary emissions sources and the conversions from gas to particle in atmosphere, accurate predictions for the aerosols impact on a regional and global scale still remains a challenging problem. In this study, we examine the relative contribution of directly emitted particles in the atmosphere (primary particles) and particles formed from gas-to-particle conversion (secondary particles) to the global aerosols and to the cloud condensation nuclei (CCN) formation. The Chemistry Transport Model v4.0 (TM4-ECPL) coupled with an extended version of the aerosol micro-physics model M7, which describes microphysical processes (nucleation, coagulation, condensation of gas-phase species) for sulfate, black carbon, organic carbon sea salt, dust and various secondary organic aerosols, is here used. A systematic analysis on the CCN production as a function of the aerosol chemical composition is performed. The sensitivity of the results to physical parameters that affect the CCN formation and cannot be accurately determined, such as hygroscopicity, is investigated based on a detailed sensitivity analysis. This work has been supported by the European FP7 collaborative project BACCHUS (Impact of Biogenic versus Anthropogenic emissions on Clouds and Climate: towards a Holistic UnderStanding).

  4. 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

  5. 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.

    2013-12-01

    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 link between aerosols and clouds; parameterizations of this process realistically 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, giant cloud condensation nuclei (CCN) activation kinetics, and entrainment to understand their individual impacts on global scale cloud droplet number concentrations (CDNCs). Compared to the existing simple activation scheme in CESM/CAM5, this series of schemes predict CDNCs that are typically in better agreement with satellite-derived and observed values. The largest changes in predicted CDNCs occur over desert and oceanic regions, owing to the enhanced activation of dust from insoluble aerosol adsorption and reductions in cloud supersaturation from the intense absorption of water vapor in regions of strong giant CCN emissions (e.g., sea-salt). Comparison of CESM/CAM5 against satellite-derived cloud optical thickness and liquid water path shows that the updated activation schemes improve the low biases in their predictions. Globally, the incorporation of all updated schemes leads to an average increase in column CDNCs of 155%, an increase in shortwave cloud forcing of 13%, and a decrease in surface shortwave radiation of 4%. In terms of meteorological impacts, these updated aerosol activation schemes result in a slight decrease in near-surface temperature of 0.9 °C and precipitation of 0.04 mm day-1

  6. 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.

  7. Remote sensing of cirrus clouds and aerosols by a sun photometer in Tunisia

    NASA Astrophysics Data System (ADS)

    Chtioui, H.; Mansour, F. B.; Elouragini, S.; Flamant, P. H.

    2006-04-01

    Some ground based measurements of solar radiation by using a sun photometer, have been conducted in Tunisia during the period of November 2000-February 2002. Five key measurement sites were selected: Three Sites (Tunis, Sousse, Gabes) are located on the Mediterranean coast and Two sites (Gafsa, Tozeur) on the boarder of Sahara. Over a total of 149 measurement days, 21 days are identified as clear sky, 114 days as Cirrus clouds and 14 days as aerosols. Aerosols and Cirrus clouds Optical Thickness (AOT) are derived from photometric measurements at 532 nm wavelength. Spatial and temporal variabilities of AOT are presented and discussed in this paper. Cirrus clouds were frequently observed at Gafsa and Tozeur where saharan aerosol events are expected to be more frequent than cirrus clouds. The mediterranean sea and saharan aerosols are suspected to have the main role in cirrus clouds formation, by providing water vapor and high concentrations of cloud condensation and ice forming nuclei.

  8. 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.

  9. 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

  10. Comparison of Observed and Modeled Regional Scale Aerosol Characteristics for ACE-ASIA and TRACE-P

    NASA Astrophysics Data System (ADS)

    Kapustin, V.; Clarke, A.; Carmichael, G.; Tang, Y.; McNaughton, C.

    2002-12-01

    During spring of 2001 we measured aerosol physical, chemical and optical properties for Asian aerosol with our similar instrument sets [University of Hawaii] from two aircraft - the NASA P3-B (TRACE-P) and NSF C-130 (ACE-ASIA). Observed aerosol characteristics included aerosol number concentration, measured with Ultrafine Condensation Nuclei counter (UCN) and CN counters; size distributions, obtained from a radial differential mobility analyzer (RDMA), a laser optical particle counter (OPC), aerodynamic particle sizer (APS) and wing mounted probes; aerosol light scattering and absorption obtained from nephelometers and a Particle Soot Absorption Photometers (PSAP). On the C-130 a dry and humidified nephelometer was operated to measure humidity dependence of aerosol light scattering, f(RH). Size distributions and number concentrations were measured with thermal aerosol volatilization to infer particles volatility and refractory properties linked to dust and soot aerosol components. Here we compare these observations to results from the University of Iowa CFORS/STEM model of related aerosol characteristics during these measurement periods. This model includes a wide variety of aerosol chemical and optical properties - black and organic carbon (BC and OC), dust, sulfate concentrations and calculated aerosol optical depth. This comparison is based not only on case studies bur also on regional scale air mass characterization. To facilitate this comparison a set of scatter "signature" plots of measured aerosol parameters like f(RH) vs. fractional submicron aerosol surface area or submicron refractory volume vs. total aerosol absorption is used. This approach generates clusters of data characteristics for different air masses. The model shows a high degree of consistency in identifying the main features of biomass burning, urban/industrial pollution, and dust events. This combination of measured and modeled aerosol parameters is shown to be valuable in quantifying the

  11. Reducing the uncertainty in background marine aerosol radiative properties using CAM5 model results and CALIPSO-retrievals

    NASA Astrophysics Data System (ADS)

    Meskhidze, N.; Gantt, B.; Dawson, K.; Johnson, M. S.; Gasso, S.

    2012-12-01

    Abundance of natural aerosols in the atmosphere strongly affects global aerosol optical depth (AOD) and influences clouds and the hydrological cycle through its ability to act as cloud condensation nuclei (CCN). Because the anthropogenic contribution to climate forcing represents the difference between the total forcing and that from natural aerosols, understanding background aerosols is necessary to evaluate the influences of anthropogenic aerosols on cloud reflectivity and persistence (so-called indirect radiative forcing). The effects of marine aerosols are explored using remotely sensed data obtained by Cloud-aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) and the NCAR Community Atmosphere Model (CAM5.0), coupled with the PNNL Modal Aerosol Model. CALIPSO-provided high resolution vertical profile information about different aerosol subtypes (defined as clean continental, marine, desert dust, polluted continental, polluted dust, and biomass burning), particulate depolarization ratio (or particle non-sphericity), reported aerosol color ratio (the ratio of aerosol backscatter at the two wavelengths) and lidar ratios over different parts of the oceans are compared to model-simulations to help evaluate the contribution of biogenic aerosol to CCN budget in the marine boundary layer. Model-simulations show that over biologically productive ocean waters primary organic aerosols of marine origin can contribute up to a 20% increase in CCN (at a supersaturation of 0.2%) number concentrations. Corresponding changes associated with cloud properties (liquid water path and droplet number) can decrease global annual mean indirect radiative forcing of anthropogenic aerosol (less cooling) by ~0.1 Wm-2 (7%). This study suggests ignoring the complex chemical composition and size distribution of sea spray particles could result in considerable uncertainties in predicted anthropogenic aerosol indirect effect.

  12. Aerosol dynamics in ship tracks

    NASA Astrophysics Data System (ADS)

    Russell, Lynn M.; Seinfeld, John H.; Flagan, Richard C.; Ferek, Ronald J.; Hegg, Dean A.; Hobbs, Peter V.; Wobrock, Wolfram; Flossmann, Andrea I.; O'Dowd, Colin D.; Nielsen, Kurt E.; Durkee, Phillip A.

    1999-01-01

    Ship tracks are a natural laboratory to isolate the effect of anthropogenic aerosol emissions on cloud properties. The Monterey Area Ship Tracks (MAST) experiment in the Pacific Ocean west of Monterey, California, in June 1994, provides an unprecedented data set for evaluating our understanding of the formation and persistence of the anomalous cloud features that characterize ship tracks. The data set includes conditions in which the marine boundary layer is both clean and continentally influenced. Two case studies during the MAST experiment are examined with a detailed aerosol microphysical model that considers an external mixture of independent particle populations. The model allows tracking individual particles through condensational and coagulational growth to identify the source of cloud condensation nuclei (CCN). In addition, a cloud microphysics model was employed to study specific effects of precipitation. Predictions and observations reveal important differences between clean (particle concentrations below 150 cm-3) and continentally influenced (particle concentrations above 400 cm-3) background conditions: in the continentally influenced conditions there is a smaller change in the cloud effective radius, drop number and liquid water content in the ship track relative to the background than in the clean marine case. Predictions of changes in cloud droplet number concentrations and effective radii are consistent with observations although there is significant uncertainty in the absolute concentrations due to a lack of measurements of the plume dilution. Gas-to-particle conversion of sulfur species produced by the combustion of ship fuel is predicted to be important in supplying soluble aerosol mass to combustion-generated particles, so as to render them available as CCN. Studies of the impact of these changes on the cloud's potential to precipitate concluded that more complex dynamical processes must be represented to allow sufficiently long drop

  13. 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

  14. Water uptake of clay and desert dust aerosol particles at sub- and supersaturated water vapor conditions.

    PubMed

    Herich, Hanna; Tritscher, Torsten; Wiacek, Aldona; Gysel, Martin; Weingartner, Ernest; Lohmann, Ulrike; Baltensperger, Urs; Cziczo, Daniel J

    2009-09-28

    Airborne mineral dust particles serve as cloud condensation nuclei (CCN), thereby influencing the formation and properties of warm clouds. It is therefore of atmospheric interest how dust aerosols with different mineralogy behave when exposed to high relative humidity (RH) or supersaturation (SS) with respect to liquid water. In this study the subsaturated hygroscopic growth and the supersaturated cloud condensation nucleus activity of pure clays and real desert dust aerosols were determined using a hygroscopicity tandem differential mobility analyzer (HTDMA) and a cloud condensation nuclei counter (CCNC), respectively. Five different illite, montmorillonite and kaolinite clay samples as well as three desert dust samples (Saharan dust (SD), Chinese dust (CD) and Arizona test dust (ATD)) were investigated. Aerosols were generated both with a wet and a dry disperser. The water uptake was parameterized via the hygroscopicity parameter kappa. The hygroscopicity of dry generated dust aerosols was found to be negligible when compared to processed atmospheric aerosols, with CCNC derived kappa values between 0.00 and 0.02 (the latter corresponds to a particle consisting of 96.7% by volume insoluble material and approximately 3.3% ammonium sulfate). Pure clay aerosols were generally found to be less hygroscopic than natural desert dust particles. The illite and montmorillonite samples had kappa approximately 0.003. The kaolinite samples were less hygroscopic and had kappa=0.001. SD (kappa=0.023) was found to be the most hygroscopic dry-generated desert dust followed by CD (kappa=0.007) and ATD (kappa=0.003). Wet-generated dust showed an increased water uptake when compared to dry-generated samples. This is considered to be an artifact introduced by redistribution of soluble material between the particles. Thus, the generation method is critically important when presenting such data. These results indicate any atmospheric processing of a fresh mineral dust particle which

  15. Water uptake of clay and desert dust aerosol particles at sub- and supersaturated water vapor conditions.

    PubMed

    Herich, Hanna; Tritscher, Torsten; Wiacek, Aldona; Gysel, Martin; Weingartner, Ernest; Lohmann, Ulrike; Baltensperger, Urs; Cziczo, Daniel J

    2009-09-28

    Airborne mineral dust particles serve as cloud condensation nuclei (CCN), thereby influencing the formation and properties of warm clouds. It is therefore of atmospheric interest how dust aerosols with different mineralogy behave when exposed to high relative humidity (RH) or supersaturation (SS) with respect to liquid water. In this study the subsaturated hygroscopic growth and the supersaturated cloud condensation nucleus activity of pure clays and real desert dust aerosols were determined using a hygroscopicity tandem differential mobility analyzer (HTDMA) and a cloud condensation nuclei counter (CCNC), respectively. Five different illite, montmorillonite and kaolinite clay samples as well as three desert dust samples (Saharan dust (SD), Chinese dust (CD) and Arizona test dust (ATD)) were investigated. Aerosols were generated both with a wet and a dry disperser. The water uptake was parameterized via the hygroscopicity parameter kappa. The hygroscopicity of dry generated dust aerosols was found to be negligible when compared to processed atmospheric aerosols, with CCNC derived kappa values between 0.00 and 0.02 (the latter corresponds to a particle consisting of 96.7% by volume insoluble material and approximately 3.3% ammonium sulfate). Pure clay aerosols were generally found to be less hygroscopic than natural desert dust particles. The illite and montmorillonite samples had kappa approximately 0.003. The kaolinite samples were less hygroscopic and had kappa=0.001. SD (kappa=0.023) was found to be the most hygroscopic dry-generated desert dust followed by CD (kappa=0.007) and ATD (kappa=0.003). Wet-generated dust showed an increased water uptake when compared to dry-generated samples. This is considered to be an artifact introduced by redistribution of soluble material between the particles. Thus, the generation method is critically important when presenting such data. These results indicate any atmospheric processing of a fresh mineral dust particle which

  16. Aerosol First Indirect Effects on Non-Precipitating Low-Level Liquid Cloud Properties as Simulated by CAM5 at ARM Sites

    SciTech Connect

    Zhao, Chuanfeng; Klein, Stephen A.; Xie, Shaocheng; Liu, Xiaohong; Boyle, James; Zhang, Yuying

    2012-04-28

    We quantitatively examine the aerosol first indirect effects (FIE) for non-precipitating low-level single-layer liquid phase clouds simulated by the Community Atmospheric Model version 5 (CAM5) running in the weather forecast mode at three DOE Atmospheric Radiation Measurement (ARM) sites. The FIE is quantified in terms of a relative change in cloud droplet effective radius for a relative change in aerosol accumulation mode number concentration under conditions of fixed liquid water content (LWC). CAM5 simulates aerosol-cloud interactions reasonably well for this specific cloud type, and the simulated FIE is consistent with the long-term observations at the examined locations. The FIE in CAM5 generally decreases with LWC at coastal ARM sites, and is larger by using cloud condensation nuclei rather than aerosol accumulation mode number concentration as the choice of aerosol amount. However, it has no significant variations with location and has no systematic strong seasonal variations at examined ARM sites.

  17. 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

  18. Atmospheric aerosols local-regional discrimination for a semi-urban area in India

    NASA Astrophysics Data System (ADS)

    Hooda, R. K.; Hyvärinen, A.-P.; Vestenius, M.; Gilardoni, S.; Sharma, V. P.; Vignati, E.; Kulmala, M.; Lihavainen, H.

    2016-02-01

    In the European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI), measurements were carried out with a sequential filter-based aerosol sampler and on-line instruments for aerosol composition and behaviour at Gual Pahari, close to New Delhi. In fine mode (PM2.5), the secondary organic carbon (SOC) to total organic carbon ratio was 46%. This indicated that condensation of SOC on fine size particles could occur rapidly which may be related to the growth of aerosols and the potential to the size of cloud condensation nuclei in the region. Source region discrimination was improved significantly through coupling conditional probability functions with receptor modelling, and validation through volume size distribution. The air masses from industrial and dense populated regions show a mix of local as well as regional emissions to fine mode aerosols. The back-trajectory analysis captured the long-range transport of sea-salt aerosols enriched with mineral dust. The surface wind directions identified the influence of local emission activities.

  19. 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.

  20. Simulating Aerosol-cloud-radiation Feedbacks Over East Asia Using WRF-Chem

    NASA Astrophysics Data System (ADS)

    Wang, J.; Allen, D. J.; Pickering, K. E.; Li, Z.

    2013-12-01

    Aerosols play an important role in climate change through their impact on the radiative balance and hydrological cycle of the atmosphere. Recently much effort has been put into studying the radiative forcing of aerosols in East Asia. In this study, we apply the regional chemistry and transport model, WRF-Chem, to study aerosol radiative forcing over eastern Asia. Four model simulations have been conducted to ascertain the direct and indirect (cloud albedo and cloud lifetime) effects of aerosols on radiation and precipitation. The time period of interest is from Feb 22, 2005 to March 31, 2005 when there were extensive measurements of radiation, trace gases, and aerosol properties available from EAST-AIRE (East Asian Study of Tropospheric Aerosols: An International Regional Experiment ). Measurements from EAST-AIRE site Xianghe, MODIS, CERES, and AERONET are used to assess the performance of the base simulation. The base run shows good agreement with observations, although the model underestimates the aerosol loading in East Asia, especially over highly polluted regions. We compare the base run with the sensitivity runs and investigate the difference in short wave radiation at the surface and the top of atmosphere, cloud properties (cloud fraction, cloud condensation nuclei, effective radius, and liquid water path), and precipitation patterns. Preliminary results indicate that short wave radiation at the surface is reduced by 28 W m-2 at Xianghe site due to the aerosol direct effect.

  1. 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.

  2. Aerosol-cloud associations over Gangetic Basin during a typical monsoon depression event using WRF-Chem simulation

    NASA Astrophysics Data System (ADS)

    Sarangi, Chandan; Tripathi, S. N.; Tripathi, Shivam; Barth, Mary C.

    2015-10-01

    To study aerosol-cloud interactions over the Gangetic Basin of India, the Weather Research and Forecasting model coupled with chemistry (WRF-Chem) has been applied to a typical monsoon depression event prevalent between the 23 and 29 August 2009. This event was sampled during the Cloud Aerosol Interaction and Precipitation Enhancement EXperiment (CAIPEEX) aircraft campaign, providing measurements of aerosol and cloud microphysical properties from two sorties. Comparison of the simulated meteorological, thermodynamical, and aerosol fields against satellite and in situ aircraft measurements illustrated that the westward propagation of the monsoon depression and the cloud, aerosol, and rainfall spatial distribution was simulated reasonably well using anthropogenic emission rates from Monitoring Atmospheric Composition and Climate project along with cityZEN projects (MACCity)+Intercontinental Chemical Transport Experiment Phase B anthropogenic emission rates. However,the magnitude of aerosol optical depth was underestimated by up to 50%. A simulation with aerosol emissions increased by a factor of 6 over the CAIPEEX campaign domain increased the simulated aerosol concentrations to values close to the observations, mainly within boundary layer. Comparison of the low-aerosol simulation and high-aerosol simulation for the two sorties illustrated that more anthropogenic aerosols increased the cloud condensing nuclei (CCN) and cloud droplet mass concentrations. The number of simulated cloud droplets increased while the cloud droplet effective radii decreased, highlighting the importance of CCN-cloud feedbacks over this region. The increase in simulated anthropogenic aerosols (including absorbing aerosols) also increased the temperature of air parcels below clouds and thus the convective available potential energy (CAPE). The increase in CAPE intensified the updraft and invigorated the cloud, inducing formation of deeper clouds with more ice-phase hydrometeors for both cases

  3. 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/).

  4. Field and Laboratory Studies of Atmospheric Organic Aerosol

    NASA Astrophysics Data System (ADS)

    Coggon, Matthew Mitchell

    This thesis is the culmination of field and laboratory studies aimed at assessing processes that affect the composition and distribution of atmospheric organic aerosol. An emphasis is placed on measurements conducted using compact and high-resolution Aerodyne Aerosol Mass Spectrometers (AMS). The first three chapters summarize results from aircraft campaigns designed to evaluate anthropogenic and biogenic impacts on marine aerosol and clouds off the coast of California. Subsequent chapters describe laboratory studies intended to evaluate gas and particle-phase mechanisms of organic aerosol oxidation. The 2013 Nucleation in California Experiment (NiCE) was a campaign designed to study environments impacted by nucleated and/or freshly formed aerosol particles. Terrestrial biogenic aerosol with > 85% organic mass was observed to reside in the free troposphere above marine stratocumulus. This biogenic organic aerosol (BOA) originated from the Northwestern United States and was transported to the marine atmosphere during periodic cloud-clearing events. Spectra recorded by a cloud condensation nuclei counter demonstrated that BOA is CCN active. BOA enhancements at latitudes north of San Francisco, CA coincided with enhanced cloud water concentrations of organic species such as acetate and formate. Airborne measurements conducted during the 2011 Eastern Pacific Emitted Aerosol Cloud Experiment (E-PEACE) were aimed at evaluating the contribution of ship emissions to the properties of marine aerosol and clouds off the coast of central California. In one study, analysis of organic aerosol mass spectra during periods of enhanced shipping activity yielded unique tracers indicative of cloud-processed ship emissions (m/z 42 and 99). The variation of their organic fraction (f42 and f 99) was found to coincide with periods of heavy (f 42 > 0.15; f99 > 0.04), moderate (0.05 < f42 < 0.15; 0.01 < f99 < 0.04), and negligible (f42 < 0.05; f99 < 0.01) ship influence. Application of

  5. 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

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

    PubMed

    Hassett, Maribeth O; Fischer, Mark W F; Money, Nicholas P

    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

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

    PubMed

    Hassett, Maribeth O; Fischer, Mark W F; Money, Nicholas P

    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.

  8. 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

  9. Greater Influence of Aerosol on Cloud Microphysics

    NASA Astrophysics Data System (ADS)

    Jha, V.; Hudson, J. G.; Noble, S.

    2009-12-01

    CCN and cloud microphysics measurements are presented from four projects: RICO, PASE,ICE-L and POST. Correlations coefficients (R) between 1% supersaturation CCN concentrations and total cloud droplet concentrations were 0.80 in all four projects and for the combined data. R between CCN and larger cloud droplet concentrations progressively decreased with increasing sizes (Fig. 1A). At ~20 µm R was maximum negative and then reversed to smaller negative and even positive at larger drop sizes. R is positive for CCN with total cloud droplets because droplets are proportional to the concentrations of nuclei that they condensed upon, CCN. The negative R for CCN with larger droplets is due to competition among droplets for condensate. Competition for condensate is greater when CCN concentrations are higher and this limits droplet sizes, more so for higher concentrations. Negative R ensues because this reduces droplet concentrations above specific sizes to a greater extent for higher CCN concentrations. The greatest negative R thus occurs at the size range where droplet concentrations are the largest, the mode of the droplet size distributions. In Fig. 1 this is just beyond the average mode. At larger sizes droplet concentrations are lower (Fig. 1B) and thus there is less competition for condensate. The more numerous small sized droplets do not have enough surface area to affect the growth of the larger less numerous droplets. Thus at larger sizes with reduced competition, droplet concentrations are again proportional to the concentrations of the nuclei that they condensed upon. Often particle concentrations at various sizes are proportional. When this is the case there will be a positive R for CCN at 1% with such larger droplet concentrations such as PASE in Fig. 1A. Thus there are two directly conflicting influences on R; the usual positive R between CCN and droplets and the negative R due to competition for condensate. Thus lower R between CCN and droplet

  10. Balloonborne meaurements of Pinatubo aerosol during 1991 and 1992 at 41[degrees] N: Verticle profiles, size distribution, and volatility

    SciTech Connect

    Deshler, T.; Johnson, B.J.; Rozier, W.R.

    1993-07-23

    The authors report balloon borne measurements of the aerosol loading above Laramie, Wyoming from June, 1991, following the eruption of the Mt Pinatubo volcano. Estimates place the stratospheric loading at 20 to 30 Mtons of SO[sub 2] from this eruption. The authors measure the densities of condensation nuclei, with r > 0.01[mu]m, and of optical aerosols, with r > 0.15[mu]m. Following an initial peaking, the mass loading, and total scattering surface areas were observed to peak roughly 180 days after the eruption. In most of 1992 the aerosol observations remained fairly homogeneous and constant. Volatility measurements indicated the aerosol was mainly a mixture of water and sulfuric acid.

  11. Aerosol Interactions with Extensive Stratus Cloud During VOCALS

    NASA Astrophysics Data System (ADS)

    Clarke, A. D.; McNaughton, C. S.; Freitag, S.; Howell, S.; Kapustin, V.; Snider, J.; Campos, T. L.; Leon, D.; Shank, L.; Wood, R.

    2009-12-01

    The 2008 VOCALS experiment over the Pacific and off the north coast of Chile provided numerous opportunities to examine aerosol-stratus interactions over 1000km flight legs and processes associated with their breakup into pockets of open cells (POC’s). Our HiGEAR (Hawaii Group for Environmental Aerosol Research) measurements on the NCAR C-130 aircraft included the aerosol size-distribution, size-resolved volatile and non-volatile components, ionic and organic chemistry (AMS), black carbon (BC, as measured by Single Particle Soot Photometer - SP2) and associated optical properties. We are exploring these observations in conjunction with meteorological data, trace gas data (eg. O3, CO) and cloud condensation nuclei (CCN) to resolve features related to the source, removal and evolution of aerosol active as CCN. Stratus clouds decks along the coast were heavily impacted by anthropogenic combustion sources along the coast. Offshore in the marine boundary layer (MBL) below cloud these influences diminished and transitioned to clean central Pacific aerosol west of about 75W. Periods with smallest aerosol sizes tended to show subsidence around the South Pacific high pressure system while larger sizes had spent more time in the MBL. However, at various altitudes in the free troposphere (FT) above cloud, relatively low concentrations of biomass burning (BB) aerosol occurred in patches and “rivers” of flow. These BB aerosol were often near cloud top or within a day of subsiding to cloud top for estimated rates of about 0.4 cm/s. The BB aerosol was generally associated with elevated CO, organic, non-volatile aerosol, and BC. POC’s were lowest in CO compared to both adjacent cloudy air and FT air, indicating less prior influence from combustion aerosol than cloudy regions. POC regions manifested dramatic aerosol reduction through precipitation and drizzle resulting in low concentrations with diameters often less than about 40nm. Offshore, drizzling cloudy regions

  12. Stratospheric sulfate aerosol in and near the Northern Hemisphere polar vortex - The morphology of the sulfate layer, multimodal size distributions, and the effect of denitrification

    NASA Technical Reports Server (NTRS)

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

    1992-01-01

    Measurements were made of stratospheric sulfate aerosols using a passive cavity aerosol spectrometer and a condensation nucleus counter on a NASA ER-2 aircraft in the Airborne Arctic Stratospheric Experiment of 1989. The problems of representative and accurate sampling and particle evaporation were explicitly addressed in the design of the inlets and reduction of the data. The measurements suggest that the sulfate aerosol is bimodal in the polar vortex above the mass mixing ratio maximum in the sulfate layer. It appears that a nuclei mode of small, newly formed particles exists in this region. A stronger case is made for a nuclei mode in the upper few kilometers of the troposphere and in the lower few kilometers of the stratosphere. This mode is probably a global phenomenon occurring in all seasons. Comparison of denitrified and nondenitrified air suggests that denitrification removes some of the larger sulfate particles.

  13. 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

  14. 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

  15. 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

  16. Opacity of monodisperse sulfuric acid aerosols

    NASA Astrophysics Data System (ADS)

    Pilat, Michael J.; Wilder, James M.

    The plume opacity and droplet diameters of a monodisperse sulfuric acid aerosol were calculated as a function of the initial H 2SO 4 concentration, initial H 2O concentration and final gas temperature after cooling from an original stack gas temperature of 300°C. Calculation assumptions include heterogeneous heteromolecular condensation of H 2SO 4 and H 2O onto monodisperse nuclei of 0.05 μm dia., three aerosol particle nuclei concentrations of 10 6, 10 7 and 10 8 cm -3 (at 300°C and 760 mm Hg); and a stack or plume diameter of 6 m. The calculated results show that for the conditions considered and with the stack temperatures in excess of 125°C, initial H 2SO 4 stack gas concentrations of 10ppm or less will result in calculated opacities of less than 20 % for a plume diameter of 6 m. The results show that the calculated opacity is significantly affected by the initial H 2SO 4 and initial H 2O concentrations and the final gas temperature. The increases in the calculated opacities upon cooling of the stack gases are similar in general to the increases in the measured opacities between instack and outstack reported by Nader and Conner (1978) for an oil-fired boiler.

  17. 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

  18. Evolution of the Physicochemical and Activation Properties of Aerosols within Smoke Plumes during the Biomass Burning Observation Project (BBOP)

    NASA Astrophysics Data System (ADS)

    Tomlinson, J. M.; Mei, F.; Wang, J.; Comstock, J. M.; Hubbe, J. M.; Pekour, M. S.; Shilling, J. E.; Fortner, E.; Chand, D.; Sedlacek, A. J., III; Kleinman, L. I.; Senum, G.; Schmid, B.

    2014-12-01

    Biomass burning from wildfires and controlled agricultural burns are known to be a major source of fine particles and organic aerosols at northern temperate latitudes during the summer months. However, the evolution of the physicochemical properties of the aerosol during transport and the potential impact of this evolution on cloud condensation nuclei (CCN) activity has rarely been studied for these events. During the DOE-sponsored Biomass Burning Observation Project (BBOP) conducted in the summer and fall of 2013, over 30 research flights sampled biomass burning plumes from wildfires in the Northwestern United States and agricultural burns in the Mid-South region of the United States. A large suite of instruments aboard the DOE G-1 (Gulfstream-1) measured the chemical, physical, and optical properties of biomass burning aerosol with an emphasis on black carbon. A Fast Integrated Mobility Spectrometer (FIMS), Ultra High Sensitivity Aerosol Spectrometer - Airborne (UHSAS-A), and Passive Cavity Aerosol Spectrometer (PCASP) were used to measure the aerosol size distribution from 15 - 3,000 nm at 1-Hz. A dual column CCN counter measured the CCN number concentration at supersaturations of 0.25% and 0.50% at a time resolution of 1-Hz and the aerosol chemical composition was measured using a soot particle aerosol mass spectrometer (SP-AMS, Aerodyne, Inc). The SP-AMS was operated in two modes: (i) as a traditional high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS, Aerodyne Inc.), which measured chemical composition of non-refractory aerosols and (ii) as the SP-AMS which measured chemical composition of the refractory black carbon-containing (rBC) particle coating and rBC aerosol mass. Utilizing the aforementioned measurements, a CCN closure study is used to investigate the emitted aerosol hygroscopicity, the evolution of the physicochemical properties of the aerosol, and the potential impacts on cloud microphysics from the different fuel sources.

  19. Atmospheric electricity and aerosol-cloud interactions in earth's atmosphere

    NASA Astrophysics Data System (ADS)

    Manninen, Hanna E.; Tammet, Hannes; Mäkelä, Antti; Haapalainen, Jussi; Mirme, Sander; Nieminen, Tuomo; Franchin, Alessandro; Petäjä, Tuukka; Kulmala, Markku; Hõrrak, Urmas

    2013-05-01

    Firstly, atmospheric ions play an important role in the fair weather electricity in Earth's atmosphere. Small ions, or charged molecular clusters, carry electric currents in the atmosphere. These small ions are continuously present, and their lifetime in lower atmosphere is about one minute. It's essential to find out a connection between the production rate of cluster ions, ion-ion recombination, and ion-aerosol attachment, and their ambient concentrations, in order to understand electrical properties of air. Secondly, atmospheric ions are important for Earth's climate, due to their potential role in secondary aerosol formation, which can lead to increased number of cloud condensation nuclei (CCN), which in turn can change the cloud properties. Our aim is to quantify the connections between these two important roles of air ions based on field observations.

  20. 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.

  1. Parameterization of the Cloud Nucleating Activity of Fresh, Aged, and Internally-Mixed Organic Aerosols

    NASA Astrophysics Data System (ADS)

    Kreidenweis, S.; Petters, M.; Demott, P.; Prenni, A.; Ziemann, P.

    2006-12-01

    Carbonaceous particle types affect global climate, visibility, and human health, but their primary and secondary sources, sinks, and tropospheric lifetimes are highly uncertain. The size and hygroscopicity of particles, and in particular their activity as cloud condensation nuclei (CCN), plays a large role in determining their atmospheric impacts and lifetimes. However, hygroscopicity is difficult to parameterize for many organic species for which no thermodynamic data exist, and for complex, multicomponent aerosols of undefined composition. We propose a simple method to describe the relationship between dry particle diameter and CCN activity using a single hygroscopicity parameter, κ. We derive values of κ from fitting of experimental CCN-activity data from the literature and from recent experiments, including oxidation-aged organic particles and secondary organic aerosols. Values of κ are between 0.5 and 2 for highly-CCN- active salts such as sodium chloride, between 0.01 and 0.5 for slightly to very hygroscopic organic aerosols such as those produced in biomass burning and as secondary organic aerosols, and 0 for nonhygroscopic components. The hygroscopicity of internal mixtures can be calculated as a volume fraction weighted average of the hygroscopicity parameters of the individual species comprising the mixture. Aging of aerosol, understood as changes in hygroscopicity due to condensation of hydrophilic species, coagulation of aerosol populations, or heterogeneous chemical reactions, are described conveniently by changes in κ. Our studies show that oxidative aging that proceeds by addition of functional groups to the CHx carbon backbone leads to only small changes in κ, and thus the process alone is inefficient at rendering small, initially- hydrophobic primary organic particles capable of being scavenged by cloud-drop nucleation. Other processes, such as coagulation and condensation, control the rate of hydrophobic-to-hydrophilic conversion of primary

  2. Anthropogenic influence on the distribution of tropospheric sulphate aerosol

    NASA Astrophysics Data System (ADS)

    Langner, J.; Rodhe, H.; Crutzen, P. J.; Zimmermann, P.

    1992-10-01

    HUMAN activities have increased global emissions of sulphur gases by about a factor of three during the past century, leading to increased sulphate aerosol concentrations, mainly in the Northern Hemisphere. Sulphate aerosols can affect the climate directly, by increasing the backscattering of solar radiation in cloud-free air, and indirectly, by providing additional cloud condensation nuclei1-4. Here we use a global transport-chemistry model to estimate the changes in the distribution of tropospheric sulphate aerosol and deposition of non-seasalt sulphur that have occurred since pre-industrial times. The increase in sulphate aerosol concentration is small over the Southern Hemisphere oceans, but reaches a factor of 100 over northern Europe in winter. Our calculations indicate, however, that at most 6% of the anthropogenic sulphur emissions is available for the formation of new aerosol particles. This is because about one-half of the sulphur dioxide is deposited on the Earth's surface, and most of the remainder is oxidized in cloud droplets so that the sulphate becomes associated with pre-existing particles. Even so, the rate of formation of new sulphate particles may have doubled since pre-industrial times.

  3. 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.

  4. 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.

  5. Water nucleation properties of chaparral fire aerosol particles

    SciTech Connect

    Hudson, J.G.; Rogers, C.F.; Hallett, J.

    1989-05-01

    In December, 1986, planned and prescribed forest management burns took place at Lodi Canyon, on the north side of the Los Angeles Basin, California. These fires involved a mixture of species of small trees and shrubs, including scrub oak, chamise, and mountain mahogany, known collectively as ''chaparral'' in the Western US. Over a period of about two weeks, about 200 hectares of chaparral were consumed. This prescribed burn presented an opportunity for three days of airborne measurements of aerosol properties including total particle or condensation nuclei (CN) concentrations and cloud condensation nuclei (CCN) concentrations. This study is in coordination with other efforts conducted simultaneously; here the emphasis will be on the airborne CN and CCN measurements and on related studies conducted on a laboratory scale. In this study, we distinguish between CCN and the total aerosol particle population as gauged by the CN count. CCN and CN concentrations and CCN/CN ratios will be presented for the airborne measurements and for laboratory measurements employing a similar fuel. Ancillary ion chromatography (IC) and scanning electron microscopy (SEM) information will also be presented for the laboratory-scale chaparral burn. 11 refs., 4 figs., 4 tabs.

  6. 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.

  7. 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

    2014-01-01

    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 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. PMID:25373416

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

    NASA Astrophysics Data System (ADS)

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

    2014-11-01

    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.

  9. 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

  10. [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.

  11. Radical-initiated formation of organosulfates and surfactants in atmospheric aerosols

    NASA Astrophysics Data System (ADS)

    Nozière, Barbara; Ekström, Sanna; Alsberg, Tomas; Holmström, Sara

    2010-03-01

    Many atmospheric aerosols contain both organic compounds and inorganic material, such as sulfate salts. In this work, we show that these sulfates could trigger some chemical transformations of the organic compounds by producing sulfate radicals, SO4-, when exposed to UV light (280-320 nm). In particular, we show by mass spectrometry (LC/ESI-MSMS) that isoprene, methyl vinyl ketone, methacrolein, and α-pinene in irradiated sulfate solutions (ammonium and sodium sulfate) produce the same organosulfates as previously identified in aerosols, and even some that had remained unidentified until now. With a typical time constant of 9 h instead of 4600 days for esterifications, these radical reactions would be a plausible origin for the atmospheric organosulfates. These reactions also produced efficient surfactants, possibly resembling the long-chain organosulfates found in the experiments. Thus, photochemistry in mixed sulfate/organic aerosols could increase cloud condensation nuclei (CCN) numbers, which would be supported by previous atmospheric observations.

  12. 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.

  13. Hygroscopicity of Amine Secondary Aerosol - Mixtures of Organic and Inorganic Components

    NASA Astrophysics Data System (ADS)

    Tang, X.; Cocker, D. R.; Purvis-Roberts, K.; Asa-Awuku, A. A.

    2012-12-01

    Aliphatic amines are emitted from both biogenic and anthropogenic sources and contribute to the formation of secondary aerosol in reactions with atmospheric radicals. However, the cloud condensation nuclei (CCN) ability of amine aerosol has not been explored yet. Here, we study the hygroscopicity of aerosol formed from three aliphatic amines (trimethylamine, diethylamine and butylamine) in the UCR environmental chamber. Amines can react with NO3, a dominant night time oxidant in acid-base and/or oxidation reactions. The mass fraction of organic and inorganic components of formed aerosol was measured by Particle-into-Liquid Sampler coupled to dual ion chromatographs (PILS-ICs) and Scanning Mobility Particle Sizer (SMPS). CCN counter was used to measure the water-uptake ability of these particles. Significantly high hygroscopicity (κ>0.3) was observed for aerosols formed from diethylamine and butylamine with NO3 radicals, which comprised >40% inorganic salt. Compared with amines oxidized by hydroxyl radicals, the presence of aminium salts formed in acid-base reactions greatly improved CCN activity of NO3-initiated aerosol. The effect of water vapor on the formation of aminium salts and aerosol hygroscopicity was also studied. Our results will significantly impact the estimation and role of amines in atmospheric chemistry and global climate models.

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

    SciTech Connect

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

    2012-08-15

    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 (S{sub pop}), is a good measure of the liquid water path response to aerosol perturbation ({lambda}), as both Spop and {lambda} 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. S{sub pop} 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 (SWCF) 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 S{sub pop} and to examine S{sub pop} in high-resolution models.

  15. 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.

  16. The Composition of Droplet-Forming Aerosol as a Function of Supersaturation

    NASA Astrophysics Data System (ADS)

    Friedman, B.; Browne, E. C.; Ardon-Dryer, K.; Carrasquillo, A. J.; Daumit, K. E.; Boulanger, K.; Kroll, J. H.; Thornton, J. A.; Cziczo, D. J.

    2013-12-01

    Ambient aerosol measurements were conducted during February 2013 as part of the Department of Energy's Two Column Aerosol Project (TCAP). Located in North Truro, MA, the site provided access to a variety of air mass sources, including marine, continental, and aged urban outflow. A CCN closure study was conducted with measurements from a commercial Cloud Condensation Nuclei Counter (CCNC, Droplet Measurement Technologies) at a range of supersaturation conditions, as well as an Aerosol Mass Spectrometer (AMS, Aerodyne). Further measurements were conducted utilizing a Pumped Counterflow Virtual Impactor (PCVI) in order to separate the activated droplets, as a function of supersaturation, from un-activated aerosol at the output of the CCNC. Subsequent composition measurements of the droplet residuals were conducted with the AMS. High-resolution residual aerosol composition will be presented as a function of instrument supersaturation and air mass, and will be compared to the total ambient aerosol composition. Results indicate an enhancement of nitrate as well as compositional differences between the organic content of the un-activated aerosol and the droplet residuals. The advantages and disadvantages of the CCNC/PCVI/AMS instrumental setup will be discussed with a focus on how this new technique allows for an improvement in our understanding of warm cloud formation.

  17. 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

  18. 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.

  19. Physicochemical properties of aerosols over the northeast Atlantic: Evidence for wind-speed-related submicron sea-salt aerosol production

    SciTech Connect

    O'Dowd, C.D.; Smith, M.H. )

    1993-01-20

    Physicochemical characteristics of submicron aerosol particles over the Northeast Atlantic (63[degrees]N, 8[degrees]W) during October/November 1989 have been examined using a thermal analytical technique and are classified according 10 air mass origin. Aerosol associated with anthropogenically influenced air masses contained typically 80% sulphate particles by number, the remainder being soot carbon and sea salt. For Arctic air masses the contribution of sulphate to the total aerosol was reduced to around 65%, due to low concentrations relative 10 sea salt which is dependent on wind speed. In situations with clean maritime air and high wind speeds, sulphate aerosol accounted for less than 25% of the total accumulation mode particles, the remainder consisting predominantly of sea salt. Arctic air masses and clean maritime air during periods of high winds were consistently acidic with inferred molar ratios of NH[sub 4][sup +]/SO[sub 4][sup =] near 0.2. The continental and modified maritime aerosol encountered was found to have molar ratios of about 0.8. Soot carbon was present in all air masses to a similar degree (5-13%). In clean air masses, submicron sea salt aerosol concentrations showed a strong exponential increase with wind speed (correlation coefficients cc [ge] 0.8), down to a dry particle radius of 0.05 [mu]m. Under these clean air' conditions and high winds the sea salt aerosol dominated all particle sizes for r > 0.05 [mu]m and accounted for approximately 75% of the total concentration, suggesting that under these conditions, sea salt aerosol would comprise the primary source cloud condensation nuclei (CCN) in stratiform clouds. 30 refs., 8 figs., 4 tabs.

  20. The Role of Aerosol-Cloud-Radiation Interactions in Regional Air Quality - A NU-WRF Study Over the United States

    NASA Astrophysics Data System (ADS)

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

    2014-12-01

    Aerosol plays an integrated role in the Earth's weather and climate system. It alters the atmospheric heating profiles through absorbing and/or scattering solar radiation that leads to changes in temperature, wind, and humidity. It also serves as cloud condensation nuclei and ice nuclei to modify cloud properties and precipitation. The aerosol-induced changes in local/regional weather pattern and planetary boundary layer structure would subsequently impact atmospheric composition and air quality. Before the advent of the fully coupled air quality models, the feedbacks among aerosol, cloud, and radiation (ACR) are often ignored, and the impact of such feedbacks on air quality is less understood. The principle purpose of this work is to assess the impact of ACR interactions on U.S. regional air quality, focusing on ozone and PM2.5, using the NASA Unified WRF (NU-WRF) modeling system. NU-WRF builds on the community WRF model with integrations of several NASA components. Specifically it couples with the Goddard Chemistry Aerosol Radiation and Transport (GOCART) model to account for ACR effects explicitly. A series of three month long simulations spanning from spring to early summer, a season laden with both local and long-range transported aerosols, have been carried out to explore the effect of ACR interactions on U.S. air quality, in which the factor separation method has been applied in order to isolate the contribution from aerosol-radiation and aerosol-cloud effect.

  1. 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.

  2. Investigating marine stratocumulus with a fully coupled cloud-aerosol scheme in a WRF/Chem Large Eddy Simulation

    NASA Astrophysics Data System (ADS)

    Kazil, J.; Wang, H.; Feingold, G.

    2009-12-01

    Drizzle in stratocumulus clouds is triggered by low concentrations of cloud condensation nuclei (CCN), and concurrently acts as a sink of CCN. The progression of this cloud-aerosol feedback may result in a transition in marine boundary layer dynamics and cloud structure; Closed cell circulation, characterized by a solid stratocumulus layer, may transition into an open cellular mode featuring low cloud fraction. Aerosol sources may balance the loss of CCN from drizzle, and delay or prevent the emergence of open cell circulation. Such sources include particle emissions from the sea surface, entrainment of aerosol from the free troposphere into the cloud deck, advection from land sources, and aerosol nucleation. In order to investigate the role of aerosol sources and processes in the transition between these two states, we have coupled in detail aerosol processes, cloud microphysics, and gas and aqueous chemistry in the WRF/Chem model. We operate WRF/Chem in Large Eddy Simulation mode. Aerosol nucleation is described with a sulfuric acid/water scheme based on laboratory measurements of the nucleation process. Here we present first results on the role of aerosol nucleation for cloud properties and drizzle formation in pristine conditions of the South-East Pacific region, and in polluted conditions.

  3. In situ studies on volatile jet exhaust particle emissions: Impact of fuel sulfur content and environmental conditions on nuclei mode aerosols

    NASA Astrophysics Data System (ADS)

    Schröder, F.; Brock, C. A.; Baumann, R.; Petzold, A.; Busen, R.; Schulte, P.; Fiebig, M.

    2000-08-01

    In situ measurements of ultrafine aerosol particle emissions were performed at cruise altitudes behind the Deutsches Zentrum für Luft-und Raumfahrt ATTAS research jet (Rolls-Royce/Snecma M45H M501 engines) and a B737-300 aircraft (CFM International 56-3B1 engines). Measurements were made 0.15-20 s after emission as the source aircraft burned fuel with sulfur contents (FSC) of 2.6, 56, or 118mg kg-1. Particle size distributions of from 3- to 60-nm diameter were determined by using condensationnuclei-counters with varying lower size detection limits. Volatile particle concentrations in the aircraft plumes strongly increased as diameter decreased toward the sizes of large molecular clusters, illustrating that apparent particle emissions are extremely sensitive to the smallest particle size detectable by the instrument used. Environmental conditions and plume age alone could influence the number of detected ultrafine (volatile) aerosols within an order of magnitude, as well. The observed volatile particle emissions decreased nonlinearly as FSC decreased to 60mg kg-1, reaching minimum values of about 2×1017kg-1 and 2×1016kg-1 for particles >3nm and >5nm, respectively. Volatile particle emissions did not change significantly as FSCs were further reduced below 60mg kg-1. Volatile particle emissions did not differ significantly between the two studied engine types. In contrast, soot particle emissions from the modern CFM56-3B1 engines were 4-5 times less (4×1014kg-1) than from the older RR M45H M501 engines (1.8×1015kg-1). Contrail processing has been identified as an efficient sink/quenching parameter for ultrafine particles and reduces the remaining interstitial aerosol by factors of 2-10 depending on particle size. These and previously published data are consistent with volatile particle emissions of 2.4×1017kg-1 independent of environmental conditions, engine type and FSCs ranging between 2.6 and 2700mg kg-1. There are clear experimental indications that

  4. 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.

  5. 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

  6. Condensation in Titan's lower atmosphere

    NASA Astrophysics Data System (ADS)

    Lavvas, P.; Griffith, C. A.; Yelle, R. V.

    2011-10-01

    We present a self-consistent description of Titan's aerosols-clouds-gases system and compare our results with the optical properties retrieved from measurements made by the Descent Imager / Spectral Radiometer (DISR) experiment on the Huygens probe [4]. Our calculations include the condensation of methane, ethane and hydrogen cyanide on photochemical aerosols produced in the thermosphere. Our results suggest that the two distinct extinction layers observed by DISR below 80 km are produced by HCN and methane condensation, respectively, while for the Huygens' equatorial conditions simulated here, the contribution of ethane clouds to the total opacity is negligible

  7. Quantifying aerosol mixing state with entropy and diversity measures

    NASA Astrophysics Data System (ADS)

    Riemer, N.; West, M.

    2013-11-01

    This paper presents the first quantitative metric for aerosol population mixing state, defined as the distribution of per-particle chemical species composition. This new metric, the mixing state index χ, is an affine ratio of the average per-particle species diversity Dα and the bulk population species diversity Dγ, both of which are based on information-theoretic entropy measures. The mixing state index χ enables the first rigorous definition of the spectrum of mixing states from so-called external mixture to internal mixture, which is significant for aerosol climate impacts, including aerosol optical properties and cloud condensation nuclei activity. We illustrate the usefulness of this new mixing state framework with model results from the stochastic particle-resolved model PartMC-MOSAIC. These results demonstrate how the mixing state metrics evolve with time for several archetypal cases, each of which isolates a specific process such as coagulation, emission, or condensation. Further, we present an analysis of the mixing state evolution for a complex urban plume case, for which these processes occur simultaneously. We additionally derive theoretical properties of the mixing state index and present a family of generalized mixing state indexes that vary in the importance assigned to low-mass-fraction species.

  8. 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

  9. 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

  10. 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

  11. Halogenation processes of secondary organic aerosol and implications on halogen release mechanisms

    NASA Astrophysics Data System (ADS)

    Ofner, J.; Balzer, N.; Buxmann, J.; Grothe, H.; Schmitt-Kopplin, Ph.; Platt, U.; Zetzsch, C.

    2012-07-01

    Reactive halogen species (RHS), such as X·, X2 and HOX containing X = chlorine and/or bromine, are released by various sources like photo-activated sea-salt aerosol or from salt pans, and salt lakes. Despite many studies of RHS reactions, the potential of RHS reacting with secondary organic aerosol (SOA) and organic aerosol derived from biomass-burning (BBOA) has been neglected. Such reactions can constitute sources of gaseous organohalogen compounds or halogenated organic matter in the tropospheric boundary layer and can influence physicochemical properties of atmospheric aerosols. Model SOA from α-pinene, catechol, and guaiacol was used to study heterogeneous interactions with RHS. Particles were exposed to molecular chlorine and bromine in an aerosol smog-chamber in the presence of UV/VIS irradiation and to RHS, released from simulated natural halogen sources like salt pans. Subsequently, the aerosol was characterized in detail using a variety of physicochemical and spectroscopic methods. Fundamental features were correlated with heterogeneous halogenation, which results in new functional groups (FTIR spectroscopy), changes UV/VIS absorption, chemical composition (ultrahigh resolution mass spectroscopy (ICR-FT/MS)), or aerosol size distribution. However, the halogen release mechanisms were also found to be affected by the presence of organic aerosol. Those interaction processes, changing chemical and physical properties of the aerosol are likely to influence e.g. the ability of the aerosol to act as cloud condensation nuclei, its potential to adsorb other gases with low-volatility, or its contribution to radiative forcing and ultimately the Earth's radiation balance.

  12. 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.

  13. 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}.

  14. Aerosols at a mountaintop observatory in Arizona

    NASA Astrophysics Data System (ADS)

    Shaw, Glenn E.

    2007-04-01

    This paper discusses physics of aerosols measured at the summit of Mt. Lemmon, Arizona (2790 m), from February to May 2002, where "clean" air representative of the free troposphere sometimes occurs. We confirmed Marti's findings of a persistent daily variation in the number concentration of condensation nuclei (diameter > 10 nm), with a strong maximum occurring in the afternoon and minimum in the early morning. These particles show evidence of growth at rates of 10-23 nm per hour. The diurnal variation was present even on days when the planetary boundary layer remained below the mountain. From the rate of growth and Maxwellian diffusion theory, we deduce that precursor condensable species are present in daytime concentrations of 107-108 cm-3, and that these are produced at a rate of 105-106 cm-3 s-1. Increased convection caused by solar heating of the mountain often carries contaminated air to the summit. Yet only a small (factor of 1.5) diurnal pattern was found for accumulation mode (diameter ˜ 130 nm) particles on days where the convective boundary layer passed well above the station. We hypothesize that these long-lived (e.g., several days) aerosols are pumped into the free troposphere and remain behind at night in a residual layer. The free tropospheric aerosol size distribution measured at Mt. Lemmon was similar in shape but higher in magnitude (by around 50%) than at Jungfraujoch in the Swiss Alps (3580 m). There is much greater diurnal variation in Aitken-sized particles (daily factor of from 7 to 10) at Mt. Lemmon than observed at Jungfraujoch (factor of from 1.0 to 1.6), evidently arising from stronger photochemical rate of productions of precursor gases.

  15. 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. PMID:26794419

  16. 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.

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

    PubMed

    Penner, J E; Dickinson, R E; O'neill, C A

    1992-06-01

    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 of sulfate aerosols. Anthropogenic increases of smoke emission thus may have helped weaken the net greenhouse warming from anthropogenic trace gases.

  18. 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.

  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 anthropogenic aerosol climate impacts. One way aerosols impact climate is by scattering solar radiation, and how much light is scattered depends upon the size of aerosols. Aerosols grow larger via water uptake and thus scatter more light at elevated relative humidities. This growth depends on composition. SSA can become enriched in organics during phytoplankton blooms, becoming less salty and therefore less hygroscopic. Aerosol hygroscopicity of SSA sampled during an in-lab phytoplankton bloom were measured during the CAICE-IMPACTS 2014 study. SSA were generated via breaking waves in an enclosed 33 m wave channel filled with natural seawater. Aerosol hygroscopicity was characterized by measuring light extinction at 532 nm of dry aerosols and of aerosols humidified to 85% relative humidity using a Cavity Ringdown Spectrometer. These optical growth factors (humidified extinction/dry extinction) were converted to physical growth factors using Mie Theory calculations and aerosol size distributions measured with a scanning electrical mobility spectrometer (SEMS) and an aerodynamic particle sizer (APS). Growth factors for super- and sub-micron SSA were quantified separately through the use of a PM2.5 cyclone or PM1 impactor. The observed SSA growth factors will be linked to SSA and source water chemical composition determined by both offline and online analysis of samples. The SSA bulk growth factors will also be compared with concurrent measurements of the efficiency with which SSA act as cloud condensation nuclei. Observed SSA growth factors will also be compared to offline hygroscopic growth measurements.

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

    DOE PAGES

    Meskhidze, Nicholas; Nenes, Athanasios

    2010-01-01

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

  1. CCN, hygroscopicity, and activation kinetics of Los Angeles aerosol

    NASA Astrophysics Data System (ADS)

    Lin, J. J.; Lathem, T. L.; Nenes, A.; Suski, K.; Cahill, J. F.; Prather, K. A.; Craven, J. S.; Metcalf, A. R.; Jonsson, H. H.; Flagan, R. C.; Seinfeld, J. H.

    2010-12-01

    The CalNex field campaign was designed as a comprehensive regional air quality and climate assessment study with an emphasis on the interaction between air quality and climate change. The southern California region is an excellent location for the study of air quality and climate change due to the existence and interaction of biogenic, dust, and urban plumes. Research flights aboard the Center for Interdisciplinary Remotely-Piloted Aircraft Studies (CIRPAS) Twin Otter platform focused on the origin and evolution of the Los Angeles plume as it is advected across the basin and outflows into the Coachella valley and Mojave Desert. This study focuses on cloud condensation nuclei (CCN) measurements taken aboard the Twin Otter. A continuous flow streamwise thermal gradient chamber operating in scanning flow CCN analysis (SFCA) mode provided high resolution, in situ CCN spectra (0.4-0.8% supersaturation) once every 40 seconds. In conjuncture with other aerosol instrumentation aboard the Twin Otter, the data provide a comprehensive picture of the interaction of ambient aerosol with water vapor. The analysis presented then quantifies the relationship between aerosol size, chemical composition, mixing state, hygroscopicity, and activation kinetics of aerosol from the variety of sources sampled.

  2. Aerosol Variations in Boundary Atmospheres: Review and Prospect

    NASA Astrophysics Data System (ADS)

    Chen, Bin; Shi, Guangyu

    Atmospheric aerosols play important roles in climate and atmospheric chemistry: They scatter sunlight, provide condensation nuclei for cloud droplets, and participate in heterogeneous chemical reactions. To enable better understanding of the vertical physical, chemical and optical feathers of the aerosols in East Asia, using some atmospheric and aerosol measurement instruments on board a kind of tethered-balloon system, a series of measurements were operated in some typical areas of East Asia, including Dunhuang, which is located in the source origin district of Asian dust and Beijing, which is the representative of large inland city during the years of 2002-2011. Mineral compositions carried by the airborne particles were analyzed as well as the microbial components, meanwhile the Lidar data were compared to the direct measurements in order to get the correlation between the optical properties of the particles and their physical and chemical variations in the boundary atmosphere. Moreover, the simultaneous observations over the districts of China, Japan and Korea, and even Pakistan supported by an international cooperative project are highly expected, in order to know the changes of the chemical, physical and even optical and radiation properties of the atmospheric aerosols during their long-range transport.

  3. Aerosol detection efficiency in inductively coupled plasma mass spectrometry

    DOE PAGES

    Hubbard, Joshua A.; Zigmond, Joseph A.

    2016-03-02

    We used an electrostatic size classification technique to segregate particles of known composition prior to being injected into an inductively coupled plasma mass spectrometer (ICP-MS). Moreover, we counted size-segregated particles with a condensation nuclei counter as well as sampled with an ICP-MS. By injecting particles of known size, composition, and aerosol concentration into the ICP-MS, efficiencies of the order of magnitude aerosol detection were calculated, and the particle size dependencies for volatile and refractory species were quantified. Similar to laser ablation ICP-MS, aerosol detection efficiency was defined as the rate at which atoms were detected in the ICP-MS normalized bymore » the rate at which atoms were injected in the form of particles. This method adds valuable insight into the development of technologies like laser ablation ICP-MS where aerosol particles (of relatively unknown size and gas concentration) are generated during ablation and then transported into the plasma of an ICP-MS. In this study, we characterized aerosol detection efficiencies of volatile species gold and silver along with refractory species aluminum oxide, cerium oxide, and yttrium oxide. Aerosols were generated with electrical mobility diameters ranging from 100 to 1000 nm. In general, it was observed that refractory species had lower aerosol detection efficiencies than volatile species, and there were strong dependencies on particle size and plasma torch residence time. Volatile species showed a distinct transition point at which aerosol detection efficiency began decreasing with increasing particle size. This critical diameter indicated the largest particle size for which complete particle detection should be expected and agreed with theories published in other works. Aerosol detection efficiencies also displayed power law dependencies on particle size. Aerosol detection efficiencies ranged from 10-5 to 10-11. Free molecular heat and mass transfer theory was

  4. Aerosol detection efficiency in inductively coupled plasma mass spectrometry

    NASA Astrophysics Data System (ADS)

    Hubbard, Joshua A.; Zigmond, Joseph A.

    2016-05-01

    An electrostatic size classification technique was used to segregate particles of known composition prior to being injected into an inductively coupled plasma mass spectrometer (ICP-MS). Size-segregated particles were counted with a condensation nuclei counter as well as sampled with an ICP-MS. By injecting particles of known size, composition, and aerosol concentration into the ICP-MS, efficiencies of the order of magnitude aerosol detection were calculated, and the particle size dependencies for volatile and refractory species were quantified. Similar to laser ablation ICP-MS, aerosol detection efficiency was defined as the rate at which atoms were detected in the ICP-MS normalized by the rate at which atoms were injected in the form of particles. This method adds valuable insight into the development of technologies like laser ablation ICP-MS where aerosol particles (of relatively unknown size and gas concentration) are generated during ablation and then transported into the plasma of an ICP-MS. In this study, we characterized aerosol detection efficiencies of volatile species gold and silver along with refractory species aluminum oxide, cerium oxide, and yttrium oxide. Aerosols were generated with electrical mobility diameters ranging from 100 to 1000 nm. In general, it was observed that refractory species had lower aerosol detection efficiencies than volatile species, and there were strong dependencies on particle size and plasma torch residence time. Volatile species showed a distinct transition point at which aerosol detection efficiency began decreasing with increasing particle size. This critical diameter indicated the largest particle size for which complete particle detection should be expected and agreed with theories published in other works. Aerosol detection efficiencies also displayed power law dependencies on particle size. Aerosol detection efficiencies ranged from 10- 5 to 10- 11. Free molecular heat and mass transfer theory was applied, but

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

    NASA Astrophysics Data System (ADS)

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

    2015-04-01

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

  6. A Fast and Efficient Version of the TwO-Moment Aerosol Sectional (TOMAS) Global Aerosol Microphysics Model

    NASA Technical Reports Server (NTRS)

    Lee, Yunha; Adams, P. J.

    2012-01-01

    This study develops more computationally efficient versions of the TwO-Moment Aerosol Sectional (TOMAS) microphysics algorithms, collectively called Fast TOMAS. Several methods for speeding up the algorithm were attempted, but only reducing the number of size sections was adopted. Fast TOMAS models, coupled to the GISS GCM II-prime, require a new coagulation algorithm with less restrictive size resolution assumptions but only minor changes in other processes. Fast TOMAS models have been evaluated in a box model against analytical solutions of coagulation and condensation and in a 3-D model against the original TOMAS (TOMAS-30) model. Condensation and coagulation in the Fast TOMAS models agree well with the analytical solution but show slightly more bias than the TOMAS-30 box model. In the 3-D model, errors resulting from decreased size resolution in each process (i.e., emissions, cloud processing wet deposition, microphysics) are quantified in a series of model sensitivity simulations. Errors resulting from lower size resolution in condensation and coagulation, defined as the microphysics error, affect number and mass concentrations by only a few percent. The microphysics error in CN70CN100 (number concentrations of particles larger than 70100 nm diameter), proxies for cloud condensation nuclei, range from 5 to 5 in most regions. The largest errors are associated with decreasing the size resolution in the cloud processing wet deposition calculations, defined as cloud-processing error, and range from 20 to 15 in most regions for CN70CN100 concentrations. Overall, the Fast TOMAS models increase the computational speed by 2 to 3 times with only small numerical errors stemming from condensation and coagulation calculations when compared to TOMAS-30. The faster versions of the TOMAS model allow for the longer, multi-year simulations required to assess aerosol effects on cloud lifetime and precipitation.

  7. Cloud Nucleating Properties of Aerosols During TexAQS - GoMACCS 2006: Influence of Aerosol Sources, Composition, and Size

    NASA Astrophysics Data System (ADS)

    Quinn, P. K.; Bates, T. S.; Coffman, D. J.; Covert, D. S.; Onasch, T. B.; Alllan, J. D.; Worsnop, D.

    2006-12-01

    TexAQS - GoMACCS 2006 was conducted from July to September 2006 in the Gulf of Mexico and Houston Ship Channel to investigate sources and processing of gas and particulate phase species and to determine their impact on regional air quality and climate. As part of the experiment, the NOAA R.V. Ronald H. Brown transited from Charleston, S.C. to the study region. The ship was equipped with a full compliment of gas and aerosol instruments. To determine the cloud nucleating properties of aerosols, measurements were made of the aerosol number size distribution, aerosol chemical composition, and cloud condensation nuclei (CCN) concentration at five supersaturations. During the transit and over the course of the experiment, a wide range of aerosol sources and types was encountered. These included urban and industrial emissions from the S.E. U.S. as the ship left Charleston, a mixture of Saharan dust and marine aerosol during the transit around Florida and across the Gulf of Mexico, urban emissions from Houston, and emissions from the petrochemical industries, oil platforms, and marine vessels in the Gulf coast region. Highest activation ratios (ratio of CCN to total particle number concentration at 0.4 percent supersaturation) were measured in anthropogenic air masses when the aerosol was composed primarily of ammonium sulfate salts and in marine air masses with an aerosol composed of sulfate and sea salt. A strong gradient in activation ratio was measured as the ship moved from the Gulf of Mexico to the end of the Houston Ship Channel (values decreasing from about 0.8 to less than 0.1) and the aerosol changed from marine to industrial. The activation ratio under these different regimes in addition to downwind of marine vessels and oil platforms will be discussed in the context of the aerosol size distribution and chemical composition. The discussion of composition will include the organic mass fraction of the aerosol, the degree of oxidation of the organics, and the water

  8. High resolution simulations of aerosol microphysics in a global and regionally nested chemical transport model

    NASA Astrophysics Data System (ADS)

    Adams, P. J.; Marks, M.

    2015-12-01

    The aerosol indirect effect is the largest source of forcing uncertainty in current climate models. This effect arises from the influence of aerosols on the reflective properties and lifetimes of clouds, and its magnitude depends on how many particles can serve as cloud droplet formation sites. Assessing levels of this subset of particles (cloud condensation nuclei, or CCN) requires knowledge of aerosol levels and their global distribution, size distributions, and composition. A key tool necessary to advance our understanding of CCN is the use of global aerosol microphysical models, which simulate the processes that control aerosol size distributions: nucleation, condensation/evaporation, and coagulation. Previous studies have found important differences in CO (Chen, D. et al., 2009) and ozone (Jang, J., 1995) modeled at different spatial resolutions, and it is reasonable to believe that short-lived, spatially-variable aerosol species will be similarly - or more - susceptible to model resolution effects. The goal of this study is to determine how CCN levels and spatial distributions change as simulations are run at higher spatial resolution - specifically, to evaluate how sensitive the model is to grid size, and how this affects comparisons against observations. Higher resolution simulations are necessary supports for model/measurement synergy. Simulations were performed using the global chemical transport model GEOS-Chem (v9-02). The years 2008 and 2009 were simulated at 4ox5o and 2ox2.5o globally and at 0.5ox0.667o over Europe and North America. Results were evaluated against surface-based particle size distribution measurements from the European Supersites for Atmospheric Aerosol Research project. The fine-resolution model simulates more spatial and temporal variability in ultrafine levels, and better resolves topography. Results suggest that the coarse model predicts systematically lower ultrafine levels than does the fine-resolution model. Significant

  9. Cosmogenic nuclei

    NASA Technical Reports Server (NTRS)

    Raisbeck, G. M.

    1986-01-01

    Cosmogenic nuclei, nuclides formed by nuclear interactions of galactic and solar cosmic rays with extraterrestrial or terrestrial matter are discussed. Long lived radioactive cosmogenic isotopes are focused upon. Their uses in dating, as tracers of the interactions of cosmic rays with matter, and in obtaining information on the variation of primary cosmic ray flux in the past are discussed.

  10. An amorphous solid state of biogenic secondary organic aerosol particles.

    PubMed

    Virtanen, Annele; Joutsensaari, Jorma; Koop, Thomas; Kannosto, Jonna; Yli-Pirilä, Pasi; Leskinen, Jani; Mäkelä, Jyrki M; Holopainen, Jarmo K; Pöschl, Ulrich; Kulmala, Markku; Worsnop, Douglas R; Laaksonen, Ari

    2010-10-14

    Secondary organic aerosol (SOA) particles are formed in the atmosphere from condensable oxidation products of anthropogenic and biogenic volatile organic compounds (VOCs). On a global scale, biogenic VOCs account for about 90% of VOC emissions and of SOA formation (90 billion kilograms of carbon per year). SOA particles can scatter radiation and act as cloud condensation or ice nuclei, and thereby influence the Earth's radiation balance and climate. They consist of a myriad of different compounds with varying physicochemical properties, and little information is available on the phase state of SOA particles. Gas-particle partitioning models usually assume that SOA particles are liquid, but here we present experimental evidence that they can be solid under ambient conditions. We investigated biogenic SOA particles formed from oxidation products of VOCs in plant chamber experiments and in boreal forests within a few hours after atmospheric nucleation events. On the basis of observed particle bouncing in an aerosol impactor and of electron microscopy we conclude that biogenic SOA particles can adopt an amorphous solid-most probably glassy-state. This amorphous solid state should provoke a rethinking of SOA processes because it may influence the partitioning of semi-volatile compounds, reduce the rate of heterogeneous chemical reactions, affect the particles' ability to accommodate water and act as cloud condensation or ice nuclei, and change the atmospheric lifetime of the particles. Thus, the results of this study challenge traditional views of the kinetics and thermodynamics of SOA formation and transformation in the atmosphere and their implications for air quality and climate.

  11. An amorphous solid state of biogenic secondary organic aerosol particles.

    PubMed

    Virtanen, Annele; Joutsensaari, Jorma; Koop, Thomas; Kannosto, Jonna; Yli-Pirilä, Pasi; Leskinen, Jani; Mäkelä, Jyrki M; Holopainen, Jarmo K; Pöschl, Ulrich; Kulmala, Markku; Worsnop, Douglas R; Laaksonen, Ari

    2010-10-14

    Secondary organic aerosol (SOA) particles are formed in the atmosphere from condensable oxidation products of anthropogenic and biogenic volatile organic compounds (VOCs). On a global scale, biogenic VOCs account for about 90% of VOC emissions and of SOA formation (90 billion kilograms of carbon per year). SOA particles can scatter radiation and act as cloud condensation or ice nuclei, and thereby influence the Earth's radiation balance and climate. They consist of a myriad of different compounds with varying physicochemical properties, and little information is available on the phase state of SOA particles. Gas-particle partitioning models usually assume that SOA particles are liquid, but here we present experimental evidence that they can be solid under ambient conditions. We investigated biogenic SOA particles formed from oxidation products of VOCs in plant chamber experiments and in boreal forests within a few hours after atmospheric nucleation events. On the basis of observed particle bouncing in an aerosol impactor and of electron microscopy we conclude that biogenic SOA particles can adopt an amorphous solid-most probably glassy-state. This amorphous solid state should provoke a rethinking of SOA processes because it may influence the partitioning of semi-volatile compounds, reduce the rate of heterogeneous chemical reactions, affect the particles' ability to accommodate water and act as cloud condensation or ice nuclei, and change the atmospheric lifetime of the particles. Thus, the results of this study challenge traditional views of the kinetics and thermodynamics of SOA formation and transformation in the atmosphere and their implications for air quality and climate. PMID:20944744

  12. Variability in morphology, hygroscopicity, and optical properties of soot aerosols during atmospheric processing.

    PubMed

    Zhang, Renyi; Khalizov, Alexei F; Pagels, Joakim; Zhang, Dan; Xue, Huaxin; McMurry, Peter H

    2008-07-29

    The atmospheric effects of soot aerosols include interference with radiative transfer, visibility impairment, and alteration of cloud formation and are highly sensitive to the manner by which soot is internally mixed with other aerosol constituents. We present experimental studies to show that soot particles acquire a large mass fraction of sulfuric acid during atmospheric aging, considerably altering their properties. Soot particles exposed to subsaturated sulfuric acid vapor exhibit a marked change in morphology, characterized by a decreased mobility-based diameter but an increased fractal dimension and effective density. These particles experience large hygroscopic size and mass growth at subsaturated conditions (<90% relative humidity) and act efficiently as cloud-condensation nuclei. Coating with sulfuric acid and subsequent hygroscopic growth enhance the optical properties of soot aerosols, increasing scattering by approximately 10-fold and absorption by nearly 2-fold at 80% relative humidity relative to fresh particles. In addition, condensation of sulfuric acid is shown to occur at a similar rate on ambient aerosols of various types of a given mobility size, regardless of their chemical compositions and microphysical structures. Representing an important mechanism of atmospheric aging, internal mixing of soot with sulfuric acid has profound implications on visibility, human health, and direct and indirect climate forcing.

  13. Long Range Transport of Amazon Aerosol in the Free Troposphere: Influence of Amazon Combustion Aerosol on CCN in the Pacific Marine Boundary Layer

    NASA Astrophysics Data System (ADS)

    Howell, S. G.; Clarke, A. D.; Freitag, S.; Kapustin, V.; Hudson, J.; Campos, T.; Pollack, I. B.; Heizer, C. G.; Weinheimer, A. J.

    2008-12-01

    The Pacific Atmosphere Sulfur Experiment (PASE, Sept. 2007) on the NCAR C-130 aircraft was based in the Equatorial Pacific to explore the remote marine sulfur cycle. We investigated sources that control particle number and cloud condensation nuclei, CCN, in the clean marine boundary layer (MBL). Earlier studies here demonstrated particle number above the MBL was dominated by natural production of new volatile particles in cloud outflow. However, during PASE we also found coated refractory aerosol (non-volatile at 350C) aloft were linearly related to ozone concentrations and were effective CCN at 0.2% supersaturation. These aerosol had larger diameters than naturally produced volatile aerosol and trajectory analysis traced them back to deep convection in biomass burning haze over the Amazon basin over 10,000km away. These refractory soot and/or organic aerosol appear to be detrained from deep convective clouds after the near- source scavenging of larger sizes that dominate the smoke/haze aerosol mass. Following transport and once mixed into MBL they were found to account for as much as 30% of the CCN at the value of 0.2%S (a typical value for small trade-wind cumulus clouds). Hence, cloud-scavenged combustion derived aerosol, too small to be detectable optically in satellite plumes, appears to provide seed nuclei for CCN in the remote marine boundary layer. This acts over hemispheric scales for this region and presumably elsewhere. Hence; various mechanisms including convective scavenging, long range transport, particle production aloft, entrainment into the MBL, boundary layer nucleation and sea-salt production all need to be considered in modeling the MBL CCN population.

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

    NASA Astrophysics Data System (ADS)

    Kulmala, Markku

    2016-04-01

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

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

    NASA Technical Reports Server (NTRS)

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

    2008-01-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2011-12-01

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

  17. Global observations of aerosol-cloud-precipitation-climate interactions

    NASA Astrophysics Data System (ADS)

    Rosenfeld, Daniel; Andreae, Meinrat O.; Asmi, Ari; Chin, Mian; Leeuw, Gerrit; Donovan, David P.; Kahn, Ralph; Kinne, Stefan; Kivekäs, Niku; Kulmala, Markku; Lau, William; Schmidt, K. Sebastian; Suni, Tanja; Wagner, Thomas; Wild, Martin; Quaas, Johannes

    2014-12-01

    Cloud drop condensation nuclei (CCN) and ice nuclei (IN) particles determine to a large extent cloud microstructure and, consequently, cloud albedo and the dynamic response of clouds to aerosol-induced changes to precipitation. This can modify the reflected solar radiation and the thermal radiation emitted to space. Measurements of tropospheric CCN and IN over large areas have not been possible and can be only roughly approximated from satellite-sensor-based estimates of optical properties of aerosols. Our lack of ability to measure both CCN and cloud updrafts precludes disentangling the effects of meteorology from those of aerosols and represents the largest component in our uncertainty in anthropogenic climate forcing. Ways to improve the retrieval accuracy include multiangle and multipolarimetric passive measurements of the optical signal and multispectral lidar polarimetric measurements. Indirect methods include proxies of trace gases, as retrieved by hyperspectral sensors. Perhaps the most promising emerging direction is retrieving the CCN properties by simultaneously retrieving convective cloud drop number concentrations and updraft speeds, which amounts to using clouds as natural CCN chambers. These satellite observations have to be constrained by in situ observations of aerosol-cloud-precipitation-climate (ACPC) interactions, which in turn constrain a hierarchy of model simulations of ACPC. Since the essence of a general circulation model is an accurate quantification of the energy and mass fluxes in all forms between the surface, atmosphere and outer space, a route to progress is proposed here in the form of a series of box flux closure experiments in the various climate regimes. A roadmap is provided for quantifying the ACPC interactions and thereby reducing the uncertainty in anthropogenic climate forcing.

  18. Aerosol and CCN Concentrations under Extremely High DMS Levels over the North Atlantic Ocean

    NASA Astrophysics Data System (ADS)

    Deng, C.; Brooks, S. D.; Thornton, D. C.; Bell, T. G.; Saltzman, E. S.; De Bruyn, W. J.

    2013-12-01

    Despite numerous studies since the CLAW hypothesis was first suggested in 1987, the extent to which marine phytoplankton derived dimethyl sulfide (CH3SCH3, DMS) contributes to marine atmospheric aerosol populations and the ability of those aerosols to act as cloud condensation nuclei (CCN) remains unclear, especially over oceanic areas obviously influenced by continental sources. Here, we present data from a cruise aboard the R/V Knorr over the North Atlantic during June-July 2011which passed through areas of both high and low phytoplankton biomasses, as well as intermediate primary production bloom regions where extremely high DMS concentrations (over 1800 pptv) were observed. Continuous ambient measurements of aerosol concentration, cloud condensation nuclei (CCN) concentration, aerosol particle size distributions, and surface seawater and atmospheric dimethyl sulfide (DMS) concentrations were performed simultaneously during the three-week-cruise. Throughout the cruise, CCN concentrations were measured at a series of five supersaturation levels and used to derive the critical supersaturation required for aerosols to activate as CCN. Air masses have been classified into three different categories based on the 48-hr back trajectories, i.e., air mass influenced by continents, coasts and the open ocean. Aerosol concentrations have noticeably different patterns depending on the air mass paths. Continually high CCN and aerosol concentrations had been found to coincide with high DMS concentration over the open ocean, which may be explained by the nucleation and condensational growth in marine boundary layer (MBL) resulting from the oxidation products of DMS or primary aerosols from the sea surface. Calculation of DMS oxidation rates based on the variation of DMS in the lower atmosphere and sea-to-air flux measurement during the whole cruise verified that the influence of continental sources on marine atmosphere is significant during the majority of sample times

  19. Sources and transformations of atmospheric aerosol particles

    NASA Astrophysics Data System (ADS)

    Cross, Eben Spencer

    Aerosol particles are an important component of the Earth-Atmosphere system because of their influence on the radiation budget both directly (through absorption and scattering) and indirectly (through cloud condensation nuclei (CCN) activity). The magnitude of the raditaive forcing attributed to the direct and indirect aerosol effects is highly uncertain, leading to large uncertainties in projections of global climate change. Real-time measurements of aerosol properties are a critical step toward constraining the uncertainties in current global climate modeling and understanding the influence that anthropogenic activities have on the climate. The objective of the work presented in this thesis is to gain a more complete understanding of the atmospheric transformations of aerosol particles and how such transformations influence the direct and indirect radiative effects of the particles. The work focuses on real-time measurements of aerosol particles made with the Aerodyne Aerosol Mass Spectrometer (AMS) developed in collaboration with the Boston College research group. A key feature of the work described is the development of a light scattering module for the AMS. Here we present the first results obtained with the integrated light scattering - AMS system. The unique and powerful capabilities of this new instrument combination are demonstrated through laboratory experiments and field deployments. Results from two field studies are presented: (1) The Northeast Air Quality Study (NEAQS), in the summer of 2004, conducted at Chebogue Point, Nova Scotia and (2) The Megacity Initiative: Local and Global Research Observations (MILAGRO) field campaign conducted in and around Mexico City, Mexico in March of 2006. Both field studies were designed to study the transformations that occur within pollution plumes as they are transported throughout the atmosphere. During the NEAQS campaign, the pollution plume from the Northeastern United States was intercepted as it was

  20. Variability and Sources of Tropospheric Aerosols Over the North Atlantic in Fall: A Model Analysis in Support of the NASA NAAMES Earth-Venture Suborbital-2 Mission

    NASA Astrophysics Data System (ADS)

    Liu, H.; Moore, R.; Hostetler, C. A.; Ferrare, R. A.; Fairlie, T. D.; Hu, Y.; Chen, G.; Johnson, M. S.; Gantt, B.; Jaegle, L.

    2015-12-01

    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, with the first field deployment in November 2015. 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. As a pre-mission analysis, we examine here the spatiotemporal variability and quantify the sources of tropospheric aerosols over the North Atlantic during November 2008 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 (MERRA at 2°×2.5° horizontal resolution) from the NASA Global Modeling 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, 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 surface aerosol measurements. We diagnose transport pathways for continental pollution outflow over the North Atlantic using carbon monoxide, an excellent tracer for anthropogenic pollution transport. Simulations indicate that, along the NAAMES nominal ship and flight tracks (40°W, 40-57°N), episodic pollution transport associated with frontal passages occurs at both the surface and free troposphere, with periods of relatively unperturbed marine air as indicated by

  1. CONDENSATION CAN

    DOEpatents

    Booth, E.T. Jr.; Pontius, R.B.; Jacobsohn, B.A.; Slade, C.B.

    1962-03-01

    An apparatus is designed for condensing a vapor to a solid at relatively low back pressures. The apparatus comprises a closed condensing chamber, a vapor inlet tube extending to the central region of the chamber, a co-axial tubular shield surrounding the inlet tube, means for heating the inlet tube at a point outside the condensing chamber, and means for refrigeratirg the said chamber. (AEC)

  2. Springtime precipitation effects on the abundance of fluorescent biological aerosol particles and HULIS in Beijing

    NASA Astrophysics Data System (ADS)

    Yue, Siyao; Ren, Hong; Fan, Songyun; Sun, Yele; Wang, Zifa; Fu, Pingqing

    2016-07-01

    Bioaerosols and humic-like substances (HULIS) are important components of atmospheric aerosols, which can affect regional climate by acting as cloud condensation nuclei and some of which can damage human health. Up to date, release of bioaerosols and HULIS initiated by precipitation is still poorly understood. Here we present different release processes for bioaerosols, non-bioaerosols and HULIS during a precipitation event in Beijing, China. Large fungal-spore-like aerosols were emitted at the onset and later weak stage of precipitation, the number concentration of which increased by more than two folds, while the number concentration of bacteria-like particles doubled when the precipitation strengthened. Besides, a good correlation between protein-like substances that were measured simultaneously by on-line and off-line fluorescence techniques consolidated their applications to measure bioaerosols. Furthermore, our EEM results suggest that the relative contribution of water-soluble HULIS to microbial materials was enhanced gradually by the rain event.

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

    NASA Astrophysics Data System (ADS)

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

    2016-09-01

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

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

    NASA Technical Reports Server (NTRS)

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

    2005-01-01

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

  5. Supersaturation in the spontaneous formation of nuclei in water vapor

    NASA Technical Reports Server (NTRS)

    Sander, Adolf; Damkohler, Gerhard

    1953-01-01

    According to experience, a certain supersaturation is required for condensation of water vapor in the homogeneous phase; that is, for inception of the condensation, at a prescribed temperature, the water vapor partial pressure must lie above the saturation pressure. The condensation starts on so-called condensation nuclei. Solid or liquid suspended particles may serve as nuclei; these particles may either a priori be present in the gas phase (dust, soot), or may spontaneously be formed from the vapor molecules to be condensed themselves. Only the second case will be considered. Gas ions which facilitate the spontaneous formation of nuclei may be present or absent. The supersaturations necessary for spontaneous nucleus formation are in general considerable higher than those in the presence of suspended particles.

  6. Global Distribution and Sources of Volatile and Nonvolatile Aerosol In the Remote Troposphere

    NASA Technical Reports Server (NTRS)

    Singh, Hanwant B.; Avery, M.; Viezee, W.; Che, Y.; Tabazadeh, A.; Hamill, P.; Pueschel, R.; Hannan, J. R.; Anderson, B.; Fuelberg, H. E.; Hipskind, R. Stephen (Technical Monitor)

    2001-01-01

    Airborne measurements of aerosol (Condensation Nuclei, CN) and selected trace gases made in the areas of the North Atlantic Ocean during SONEX (October/November 1997), and the south tropical Pacific Ocean during PEM-Tropics A (September/October 1996) and PEM-Tropics B (March/April 1999) have been analyzed. Emphasis is on the interpretations of variations in the number densities of the fine (>17 nm) and ultrafine (>8 nm) CN in the upper troposphere (8-12 km). These data suggest that large number densities of highly volatile CN (10(exp 4)-10(exp 5)/cu cm) are present in the clean upper troposphere with highest values over the tropical1subtropical region. Through marine convection and long-distance horizontal transport, volatile CN originating from the tropical/subtropical regions can frequently impact the abundance of aerosol in the middle and upper troposphere at mid to high latitudes. Nonvolatile aerosol particles behave in a manner similar to tracers of combustion (CO) and photochemical pollution (PAN), implying a source from continental pollution of industrial or biomass burning origin. In the upper troposphere, we find that volatile and nonvolatile partials number densities are inversely correlated. An aerosol microphysical model is used to suggest that coagulation of fine volatile particles with fewer larger nonvolatile particles provides one possible mechanism for this relationship. It appears that nonvolatile particles, of principally anthropogenic origin,provide a highly efficient removal process for the fine volatile aerosol.

  7. Effect of Increasing Temperature on Carbonaceous Aerosol Direct Radiative Effect over Southeastern US

    NASA Astrophysics Data System (ADS)

    Mielonen, Tero; Kokkola, Harri; Hienola, Anca; Kühn, Thomas; Merikanto, Joonas; Korhonen, Hannele; Arola, Antti; Kolmonen, Pekka; Sogacheva, Larisa; de Leeuw, Gerrit

    2016-04-01

    Aerosols are an important regulator of the Earth's climate. They scatter and absorb incoming solar radiation and thus cool the climate by reducing the amount of energy reaching the atmospheric layers and the surface below (direct effect). A certain subset of the particles can also act as initial formation sites for cloud droplets and thereby modify the microphysics, dynamics, radiative properties and lifetime of clouds (indirect effects). The magnitude of aerosol radiative effects remains the single largest uncertainty in current estimates of anthropogenic radiative forcing. One of the key quantities needed for accurate estimates of anthropogenic radiative forcing is an accurate estimate of the radiative effects from natural unperturbed aerosol. The dominant source of natural aerosols over Earth's vast forested regions are biogenic volatile organic compounds (BVOC) which, following oxidation in the atmosphere, can condense onto aerosol particles to form secondary organic aerosol (SOA) and significantly modify the particles' properties. In accordance with the expected positive temperature dependence of BVOC emissions, several previous studies have shown that some aerosol properties, such as mass concentration and ability to act as cloud condensation nuclei (CCN), also correlate positively with temperature at many forested sites. There is conflicting evidence as to whether the aerosol direct effects have a temperature dependence due to increased BVOC emissions. The main objective of this study is to investigate the causes of the observed effect of increasing temperatures on the aerosol direct radiative effect, and to provide a quantitative estimate of this effect and of the resulting negative feedback in a warming climate. More specifically, we will investigate the causes of the positive correlation between aerosol optical depth (AOD) and land surface temperature (LST) over southeastern US where biogenic emissions are a significant source of atmospheric particles. In

  8. Associative study of Absorbing Aerosol Index (AAI) and precipitation in India during monsoon season (2005 to 2014)

    NASA Astrophysics Data System (ADS)

    Dubey, Shivali; Mehta, Manu; Singh, Ankit

    2016-05-01

    Based on their interaction with solar radiations, aerosols may be categorized as absorbing or scattering in nature. The absorbing aerosols are coarser and influence precipitation mainly due to microphysical effect (participating in the formation of Cloud Condensation Nuclei) and radiative forcing (by absorbing electromagnetic radiations). The prominent absorbing aerosols found in India are Black Carbon, soil dust, sand and mineral dust. Their size, distribution, and characteristics vary spatially and temporally. This paper aims at showing the spatio-temporal variation of Absorbing Aerosol Index (AAI) and precipitation over the four most polluted zones of Indian sub-continent (Indo-Gangetic plains 1, Indo-Gangetic plains 2, Central and Southern India) for monsoon season (June, July, August, September) during the last decade (2005 to 2014). Zonal averages AAI have been found to be exhibiting an increasing trend, hence region-wise correlations have been computed between AAI and precipitation during monsoon. Daily Absorption Aerosol Index (AAI) obtained from Aura OMI Aerosol Global Gridded Data Product-OMAEROe (V003) and monthly precipitation from TRMM 3B42-V7 gridded data have been used.

  9. Hierarchical condensation near phase equilibrium

    NASA Astrophysics Data System (ADS)

    Olemskoi, A. I.; Yushchenko, O. V.; Borisyuk, V. N.; Zhilenko, T. I.; Kosminska, Yu. O.; Perekrestov, V. I.

    2012-06-01

    A novel mechanism of new phase formation is studied both experimentally and theoretically in the example of quasi-equilibrium stationary condensation in an ion-plasma sputterer. Copper condensates are obtained to demonstrate that a specific network structure is formed as a result of self-assembly in the course of deposition. The fractal pattern related is inherent in the phenomena of diffusion limited aggregation. Condensate nuclei are shown to form statistical ensemble of hierarchically subordinated objects distributed in ultrametric space. The Langevin equation and the Fokker-Planck equation related are found to describe stationary distribution of thermodynamic potential variations at condensation. Time dependence of the formation probability of branching structures is found to clarify the experimental situation.

  10. Aerosol and Cloud Microphysical Properties in the Asir region of Saudi Arabia

    NASA Astrophysics Data System (ADS)

    Axisa, Duncan; Kucera, Paul; Burger, Roelof; Li, Runjun; Collins, Don; Freney, Evelyn; Posada, Rafael; Buseck, Peter

    2010-05-01

    In recent advertent and inadvertent weather modification studies, a considerable effort has been made to understand the impact of varying aerosol properties and concentration on cloud properties. Significant uncertainties exist with aerosol-cloud interactions for which complex microphysical processes link the aerosol and cloud properties. Under almost all environmental conditions, increased aerosol concentrations within polluted air masses will enhance cloud droplet concentration relative to that in unperturbed regions. The interaction between dust particles and clouds are significant, yet the conditions in which dust particles become cloud condensation nuclei (CCN) are uncertain. In order to quantify this aerosol effect on clouds and precipitation, a field campaign was launched in the Asir region of Saudi Arabia as part of a Precipitation Enhancement Feasibility Study. Ground measurements of aerosol size distributions, hygroscopic growth factor, CCN concentrations as well as aircraft measurements of cloud hydrometeor size distributions were done in the Asir region of Saudi Arabia in August 2009. Research aircraft operations focused primarily on conducting measurements in clouds that are targeted for cloud top-seeding, on their microphysical characterization, especially the preconditions necessary for precipitation; understanding the evolution of droplet coalescence, supercooled liquid water, cloud ice and precipitation hydrometeors is necessary if advances are to be made in the study of cloud modification by cloud seeding. Non-precipitating mixed-phase clouds less than 3km in diameter that developed on top of the stable inversion were characterized by flying at the convective cloud top just above the inversion. Aerosol measurements were also done during the climb to cloud base height. The presentation will include a summary of the analysis and results with a focus on the unique features of the Asir region in producing convective clouds, characterization of the

  11. Activation of "synthetic ambient" aerosols - Relation to chemical composition of particles <100 nm

    NASA Astrophysics Data System (ADS)

    Burkart, J.; Hitzenberger, R.; Reischl, G.; Bauer, H.; Leder, K.; Puxbaum, H.

    2012-07-01

    Cloud condensation nuclei (CCN) are an important fraction of atmospheric aerosols because of their role in cloud formation. Experimental studies focus either on direct field measurements of complex ambient aerosols or laboratory investigations on well defined aerosols produced from single substances or substance mixtures. In this study, we focussed on the ultrafine aerosol because in terms of number concentration, the majority of the CCN are expected to have sizes in this range. A field study was performed from July 2007 to October 2008 to investigate the activation behaviour of the atmospheric aerosol in Vienna (Burkart et al., 2011). Filter samples of the aerosol <0.1 μm aerodynamic equivalent diameter were collected, elutriated and used to generate "synthetic ambient" aerosol in a nebulizer. Chemical analyses of the ultrafine water soluble material were also performed. The CCN properties of the "synthetic ambient" aerosol were obtained using the University of Vienna CCN counter (Giebl et al., 2002; Dusek et al., 2006b) at a nominal supersaturation (SS) of 0.5%. Activation diameters dact ranged from 54.5 nm to 66 nm, were larger than dact of typical single inorganic salts and showed no seasonal pattern in contrast to the fraction of water soluble organic carbon (WSOC), which ranged from 44% in spring to 15% in winter. The average hygroscopicity parameter κ (Petters and Kreidenweis, 2007) obtained from the activation curves ranged from 0.20 to 0.30 (average 0.24), which was significantly lower than κchem calculated from the chemical composition (0.43 ± 0.07).

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

    SciTech Connect

    Fast, JD; Berg, LK

    2015-12-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

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

  14. Aerosol dynamics in the equatorial Pacific Marine boundary layer: Microphysics, diurnal cycles and entertainment

    SciTech Connect

    Clarke, A D; Litchy, M; Li, Z

    1996-04-01

    During July-August of 1994 the authors measured the size resolved physiochemical properties of aerosol particles at Christmas Island in the equatorial Pacific. In spite of rapid diurnal conversion of dimethylsulfide (DMS) to sulfur dioxide (SO{sub 2}) the authors found no evidence for new particle production in the marine boundary layer (MBL) and more than 95% of all particles were consistently larger than 0.02{mu}m diameter, indicating an aged aerosol number (size-distribution) was bimodal with peaks near 0.05{mu}m and 0.2{mu}m particle diameter (D{sub p}) and had a cloud-processed intermode minimum at about 0.09{mu}m that varied in phase with diurnal changes in ozone concentration. This suggests that the number distribution for condensation nuclei (CN) and cloud condensation (CCN) was maintained by a quasiequilibrium between entrainment (estimated to be 0.6{+-}0.2 cm s{sup {minus}1}) from sources aloft and processes in the MBL. This implies a replenishment timescale for nuclei of about 2 and 4 days for this region. The stability of the distribution and the 0.09{mu}m cloud processed minima suggests trade winds cumulus supersaturations near 0.35% and updrafts near 1 m s{sup {minus}1}. 17 refs., 4 fig., 1 tab.

  15. Ageing of aerosol and their radiative properties in the Mediterranean Basin

    NASA Astrophysics Data System (ADS)

    Roberts, Greg; Léon, Jean-François; Pont, Véronique; Mallet, Marc; Augustin, Patrick; Dulac, François; Junkermann, Wolfgang

    2014-05-01

    The VESSAER campaign (VErtical Structure and Sources of AERosols in the Mediterranean Region) identified different sources of aerosol in the Mediterranean Basin and assessed the regional impact of aerosol on cloud microphysical and radiative properties. The airborne aspect of VESSAER was conducted on an ultra-light aircraft in summer 2012. Ground-based activities included observations in the central and northern regions of Corsica, as well as aerosol LIDAR and sun photometer measurements on the eastern coast. The main scientific goals were to investigate local versus long-range sources of aerosol and cloud condensation nuclei (CCN) and their vertical structure in the lower troposphere, study evolution and ageing related to atmospheric processes, and determine aerosol direct radiative impacts over a larger spatial scale in the Mediterranean Basin. Even though Corsica is separated by from the European continent by ca. 100 km with no immediate sources of urban aerosol, the background concentrations in Corsica were similar to those in the continental European boundary layer. The background total aerosol concentrations within the boundary layer in Corsica are nearly 2000 cm-3. Nearly all of the particles in the boundary layer (> 90%) are CCN-active at 0.37% supersaturation as they had become hygroscopic during their transport. Ageing (with respect to CCN-activity) of European emissions occurred exclusively in the boundary layer and not in aerosol layers aloft. In contrast, aerosol hygroscopicity did not change as a function of transport time in elevated aerosol layers, suggesting that photochemical ageing of less hygroscopic material is relatively slow compared to ageing processes in the boundary layer. The vertical profiles clearly show the long-range transport of dust from the Saharan Desert and pollution from the European continent -- which were the two major sources of aerosol during the campaign. Two of the research flights coincided with CALIPSO overpasses, when

  16. Aerosols: Non-CO2 Non-Greenhouse Non-Gas Forcing

    NASA Astrophysics Data System (ADS)

    Schwartz, S. E.

    2005-05-01

    Tropospheric aerosols influence Earth's radiation budget and climate by scattering and absorbing solar radiation (direct effects) and by modifying the reflectivity and extent of clouds (indirect effects). While aerosol forcing is arguably less important from a policy perspective than greenhouse gas forcing because of the short residence times of these aerosols (about a week) compared to the lifetimes of the well mixed greenhouse gases (decades to centuries), knowledge of aerosol forcing over the industrial period is essential to empirical inference of Earth's climate sensitivity from temperature change over this period and to evaluation of the performance of climate model simulations over this period. Accuracy in global-average forcing by anthropogenic aerosols required for these purposes is estimated to be ~0.5 w m-2 [Schwartz, J. Air Waste Management Assoc. 54, 1351-1359 (2004)]. For an accumulation-mode (radius 50-1000 nm) scattering aerosol above a dark surface the forcing per optical depth (at 550 nm) during daylight hours for cloud-free sky is 50 to 100 W m-2. Such a forcing intensity implies, taking into account 50% nighttime and ~50% cloud cover, that global average optical depth of anthropogenic aerosol must be known to 0.02 - 0.04, an accuracy achievable by careful ground-based measurements, but which would be difficult to achieve globally because of high spatial and temporal variation. Top-of-atmosphere forcing for a given optical depth is sensitive also to single scattering albedo, size distribution (as manifested in asymmetry parameter, backscatter fraction, or Angstrom exponent) and surface reflectance; these sensitivities are examined here. It is necessary as well to determine the fraction of forcing that is due to anthropogenic aerosol. Similar considerations apply to aerosol indirect forcing, which depends to first approximation on the number concentration of cloud condensation nuclei as a function of applied supersaturation, which depends on the

  17. The thermodynamic and kinetic impacts of organics on marine aerosols

    NASA Astrophysics Data System (ADS)

    Crahan, Kathleen

    were also applied to a cloud parcel model to examine cloud condensation nuclei closure. The best agreement was found when the solution activity was calculated using Svenningsson's model estimates, suggesting the nonlinear impact of organics on solution activity is the most important impact of organics on the marine aerosol.

  18. Ice nuclei measurements from solid rocket motor effluents

    NASA Technical Reports Server (NTRS)

    Hindman, E. E., II

    1980-01-01

    The ice crystal forming nuclei (IN) measured in solid rocket motor (SRM) exhaust products is discussed in relation to space shuttle exhaust. Preliminary results from laboratory investigations and flight preparations for March 1978 Titan launch are discussed. The work necessary to provide adequate measurements of IN and cloud condensation nuclei (CCN) in the stabilized ground clouds from SRM's is studied.

  19. CCN frequency distributions and aerosol chemical composition from long-term observations at European ACTRIS supersites

    NASA Astrophysics Data System (ADS)

    Decesari, Stefano; Rinaldi, Matteo; Schmale, Julia Yvonne; Gysel, Martin; Fröhlich, Roman; Poulain, Laurent; Henning, Silvia; Stratmann, Frank; Facchini, Maria Cristina

    2016-04-01

    Cloud droplet number concentration is regulated by the availability of aerosol acting as cloud condensation nuclei (CCN). Predicting the air concentrations of CCN involves knowledge of all physical and chemical processes that contribute to shape the particle size distribution and determine aerosol hygroscopicity. The relevance of specific atmospheric processes (e.g., nucleation, coagulation, condensation of secondary organic and inorganic aerosol, etc.) is time- and site-dependent, therefore the availability of long-term, time-resolved aerosol observations at locations representative of diverse environments is strategic for the validation of state-of-the-art chemical transport models suited to predict CCN concentrations. We focused on long-term (year-long) datasets of CCN and of aerosol composition data including black carbon, and inorganic as well as organic compounds from the Aerosol Chemical Speciation Monitor (ACSM) at selected ACTRIS supersites (http://www.actris.eu/). We discuss here the joint frequency distribution of CCN levels and of aerosol chemical components concentrations for two stations: an alpine site (Jungfraujoch, CH) and a central European rural site (Melpitz, DE). The CCN frequency distributions at Jungfraujoch are broad and generally correlated with the distributions of the concentrations of aerosol chemical components (e.g., high CCN concentrations are most frequently found for high organic matter or black carbon concentrations, and vice versa), which can be explained as an effect of the strong seasonality in the