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.

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%.

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.

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.

Cloud condensation nuclei activity and hygroscopicity of fresh and aged cooking organic aerosol

NASA Astrophysics Data System (ADS)

Li, Yanwei; Tasoglou, Antonios; Liangou, Aikaterini; Cain, Kerrigan P.; Jahn, Leif; Gu, Peishi; Kostenidou, Evangelia; Pandis, Spyros N.

2018-03-01

Cooking organic aerosol (COA) is potentially a significant fraction of organic particulate matter in urban areas. COA chemical aging experiments, using aerosol produced by grilling hamburgers, took place in a smog chamber in the presence of UV light or excess ozone. The water solubility distributions, cloud condensation nuclei (CCN) activity, and corresponding hygroscopicity of fresh and aged COA were measured. The average mobility equivalent activation diameter of the fresh particles at 0.4% supersaturation ranged from 87 to 126 nm and decreased for aged particles, ranging from 65 to 88 nm. Most of the fresh COA had water solubility less than 0.1 g L-1, even though the corresponding particles were quite CCN active. After aging, the COA fraction with water solubility greater than 0.1 g L-1 increased more than 2 times. Using the extended Köhler theory for multiple partially soluble components in order to predict the measured activation diameters, the COA solubility distribution alone could not explain the CCN activity. Surface tensions less than 30 dyn cm-1 were required to explain the measured activation diameters. In addition, COA particles appear to not be spherical, which can introduce uncertainties into the corresponding calculations.

Long-term observations of aerosol and cloud condensation nuclei concentrations in Barbados

NASA Astrophysics Data System (ADS)

Pöhlker, Mira L.; Klimach, Thomas; Krüger, Ovid O.; Hrabe de Angelis, Isabella; Ditas, Florian; Praß, Maria; Holanda, Bruna; Su, Hang; Weber, Bettina; Pöhlker, Christopher; Farrell, David A.; Stevens, Bjorn; Prospero, Joseph M.; Andreae, Meinrat O.; Pöschl, Ulrich

2017-04-01

Long-term observation of atmospheric aerosol and cloud condensation nuclei (CCN) concentrations has been conducted at the Ragged Point site in Barbados since August 2016. Ragged Point is a well-established station to monitor the transatlantic transport of Saharan dust outbreaks [1]. In the absence of dust plumes, it represents an ideal site to analyze the maritime boundary layer aerosol that is transported with the trade winds over the Atlantic towards Barbados [2,3]. Broad aerosol size distribution (10 nm to 10 µm) as well as size-resolved CCN measurements at 10 different supersaturations from 0.05 % to 0.84 % have been conducted. The continuous online analyses are supplemented by intensive sampling periods to probe specific aerosol properties with various offline techniques (i.e., microscopy and spectroscopy). Aerosol key properties from our measurements are compared with the continuous and in depth observation of cloud properties at Deebles Point, which is in close neighborhood to the Ragged Point site [2]. Moreover, our activities have been synchronized with the HALO-NARVAL-2 aircraft campaign in August 2016 that added further detailed information on shallow cumulus clouds, which are characteristic for the Atlantic trade winds and represent a crucial factor in the Earth climate system. Our measurements have the following two focal points: (i) We aim to obtain a detailed CCN climatology for the alternation of maritime and dust-impacted episodes at this unique coastal location. This study will complement our recent in-depth analysis for the long-term CCN variability at a remote rain forest location [4]. (ii) Furthermore, we aim to collect detailed information on the role of different aerosol populations on the properties of the climatically important shallow cumulus clouds. References: [1] Prospero, J. M., Collard, F. X., Molinie, J., Jeannot, A. (2014), Global Biogeochemical Cycles, 28, 757-773. [2] Stevens, B., et al. (2016), Bulletin of the American

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.;

Aerosol properties and their influences on surface cloud condensation nuclei during CAP-MBL and MC3E

NASA Astrophysics Data System (ADS)

Logan, T.; Dong, X.; Xi, B.

2016-12-01

Aerosol particles are of particular importance because of their influences on cloud development and precipitation processes over land and ocean. Aerosol physical and chemical properties and their ability to activate as cloud condensation nuclei (CCN) as well as influence CCN number concentration (NCCN) during the 2011 Midlatitude Continental Convective Clouds Experiment (MC3E) over the Southern Great Plains (SGP) region and the 2009-2010 Clouds, Aerosol, and Precipitation in the Marine Boundary Layer (CAP-MBL) over the Azores are presented in this study. Both regions periodically observe increases in NCCN when sulfate pollution and biomass burning smoke are present but over ocean, mineral dust diminishes NCCN. During clean conditions over the ocean, sea salt is the main contributor to CCN production, and strong (weak) surface winds and turbulent conditions can enhance (diminish) NCCN. Over the SGP, there were moderate to high correlations (R > 0.5) between increased magnitudes of aerosol loading (ssp), NCCN, chemical species, and PWV suggesting a shared common transport mechanism via the Gulf of Mexico further indicating the strong dependence on air mass type (e.g., marine vs. continental). Further investigations will greatly help to understand the seasonal influences of air masses on aerosol, NCCN, and cloud properties.

Plume-exit modeling to determine cloud condensation nuclei activity of aerosols from residential biofuel combustion

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mena, Francisco; Bond, Tami C.; Riemer, Nicole

Residential biofuel combustion is an important source of aerosols and gases in the atmosphere. The change in cloud characteristics due to biofuel burning aerosols is uncertain, in part, due to the uncertainty in the added number of cloud condensation nuclei (CCN) from biofuel burning. We provide estimates of the CCN activity of biofuel burning aerosols by explicitly modeling plume dynamics (coagulation, condensation, chemical reactions, and dilution) in a young biofuel burning plume from emission until plume exit, defined here as the condition when the plume reaches ambient temperature and specific humidity through entrainment. We found that aerosol-scale dynamics affect CCNmore » activity only during the first few seconds of evolution, after which the CCN efficiency reaches a constant value. Homogenizing factors in a plume are co-emission of semi-volatile organic compounds (SVOCs) or emission at small particle sizes; SVOC co-emission can be the main factor determining plume-exit CCN for hydrophobic or small particles. Coagulation limits emission of CCN to about 10 16 per kilogram of fuel. Depending on emission factor, particle size, and composition, some of these particles may not activate at low supersaturation ( s sat). Hygroscopic Aitken-mode particles can contribute to CCN through self-coagulation but have a small effect on the CCN activity of accumulation-mode particles, regardless of composition differences. Simple models (monodisperse coagulation and average hygroscopicity) can be used to estimate plume-exit CCN within about 20 % if particles are unimodal and have homogeneous composition, or when particles are emitted in the Aitken mode even if they are not homogeneous. On the other hand, if externally mixed particles are emitted in the accumulation mode without SVOCs, an average hygroscopicity overestimates emitted CCN by up to a factor of 2. This work has identified conditions under which particle populations become more homogeneous during plume

Plume-exit modeling to determine cloud condensation nuclei activity of aerosols from residential biofuel combustion

NASA Astrophysics Data System (ADS)

Mena, Francisco; Bond, Tami C.; Riemer, Nicole

2017-08-01

Residential biofuel combustion is an important source of aerosols and gases in the atmosphere. The change in cloud characteristics due to biofuel burning aerosols is uncertain, in part, due to the uncertainty in the added number of cloud condensation nuclei (CCN) from biofuel burning. We provide estimates of the CCN activity of biofuel burning aerosols by explicitly modeling plume dynamics (coagulation, condensation, chemical reactions, and dilution) in a young biofuel burning plume from emission until plume exit, defined here as the condition when the plume reaches ambient temperature and specific humidity through entrainment. We found that aerosol-scale dynamics affect CCN activity only during the first few seconds of evolution, after which the CCN efficiency reaches a constant value. Homogenizing factors in a plume are co-emission of semi-volatile organic compounds (SVOCs) or emission at small particle sizes; SVOC co-emission can be the main factor determining plume-exit CCN for hydrophobic or small particles. Coagulation limits emission of CCN to about 1016 per kilogram of fuel. Depending on emission factor, particle size, and composition, some of these particles may not activate at low supersaturation (ssat). Hygroscopic Aitken-mode particles can contribute to CCN through self-coagulation but have a small effect on the CCN activity of accumulation-mode particles, regardless of composition differences. Simple models (monodisperse coagulation and average hygroscopicity) can be used to estimate plume-exit CCN within about 20 % if particles are unimodal and have homogeneous composition, or when particles are emitted in the Aitken mode even if they are not homogeneous. On the other hand, if externally mixed particles are emitted in the accumulation mode without SVOCs, an average hygroscopicity overestimates emitted CCN by up to a factor of 2. This work has identified conditions under which particle populations become more homogeneous during plume processes. This

Plume-exit modeling to determine cloud condensation nuclei activity of aerosols from residential biofuel combustion

DOE PAGES

Mena, Francisco; Bond, Tami C.; Riemer, Nicole

2017-08-07

Residential biofuel combustion is an important source of aerosols and gases in the atmosphere. The change in cloud characteristics due to biofuel burning aerosols is uncertain, in part, due to the uncertainty in the added number of cloud condensation nuclei (CCN) from biofuel burning. We provide estimates of the CCN activity of biofuel burning aerosols by explicitly modeling plume dynamics (coagulation, condensation, chemical reactions, and dilution) in a young biofuel burning plume from emission until plume exit, defined here as the condition when the plume reaches ambient temperature and specific humidity through entrainment. We found that aerosol-scale dynamics affect CCNmore » activity only during the first few seconds of evolution, after which the CCN efficiency reaches a constant value. Homogenizing factors in a plume are co-emission of semi-volatile organic compounds (SVOCs) or emission at small particle sizes; SVOC co-emission can be the main factor determining plume-exit CCN for hydrophobic or small particles. Coagulation limits emission of CCN to about 10 16 per kilogram of fuel. Depending on emission factor, particle size, and composition, some of these particles may not activate at low supersaturation ( s sat). Hygroscopic Aitken-mode particles can contribute to CCN through self-coagulation but have a small effect on the CCN activity of accumulation-mode particles, regardless of composition differences. Simple models (monodisperse coagulation and average hygroscopicity) can be used to estimate plume-exit CCN within about 20 % if particles are unimodal and have homogeneous composition, or when particles are emitted in the Aitken mode even if they are not homogeneous. On the other hand, if externally mixed particles are emitted in the accumulation mode without SVOCs, an average hygroscopicity overestimates emitted CCN by up to a factor of 2. This work has identified conditions under which particle populations become more homogeneous during plume

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.

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.

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.

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ching, Ping Pui; Zaveri, Rahul A.; Easter, Richard C.

2016-05-27

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

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.

Rainforest Aerosols as Biogenic Nuclei of Clouds and Precipitation in the Amazon

NASA Astrophysics Data System (ADS)

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.

2010-09-01

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.

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.

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.

Organic condensation: A vital link connecting aerosol formation to climate forcing (Invited)

NASA Astrophysics Data System (ADS)

Riipinen, I.; Pierce, J. R.; Yli-Juuti, T.; Nieminen, T.; Häkkinen, S.; Ehn, M.; Junninen, H.; Lehtipalo, K.; Petdjd, T. T.; Slowik, J. G.; Chang, R. Y.; Shantz, N. C.; Abbatt, J.; Leaitch, W. R.; Kerminen, V.; Worsnop, D. R.; Pandis, S. N.; Donahue, N. M.; Kulmala, M. T.

2010-12-01

Aerosol-cloud interactions represent the largest uncertainty in calculations of Earth’s radiative forcing. Number concentrations of atmospheric aerosol particles are in the core of this uncertainty, as they govern the numbers of cloud condensation nuclei (CCN) and influence the albedo and lifetime of clouds. Aerosols also impair air quality through their adverse effects on atmospheric visibility and human health. The ultrafine fraction (<100 nm) of atmospheric aerosol particles often dominates the total aerosol numbers, and nucleation of atmospheric vapours is one of the most important sources of these particles. To have climatic relevance, however, the freshly-nucleated particles need to grow in size, and consequently their climatic importance remains to be quantified (see Fig. 1). We combine observations from two continental sites (Egbert, Canada and Hyytiälä, Finland) to show that condensation of organic vapours is a crucial factor governing the lifetimes and climatic importance of the smallest atmospheric particles. We demonstrate that state-of-the-science organic gas-particle partitioning models fail to reproduce the observations; we propose a new modelling approach that is consistent with the measurements. Finally, we demonstrate the large sensitivity of climatic forcing of atmospheric aerosols to these interactions between organic vapours and the smallest atmospheric nanoparticles - highlighting the need for representing this process in global climate models. Figure 1. Organic emissions and the dynamic processes governing the climatic importance of ultrafine aerosol. Condensable vapours are produced upon oxidation of volatile organic compounds (VOCs) and can 1) nucleate to form new small particles; 2) grow freshly formed particles to larger sizes and increase their probability to serve as CCN; 3) condense on the background aerosol (> 100 nm) and enhance the loss of ultrafine particles. Primary organic aerosol (POA) contributes to the large end of the

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.

Investigation of cloud condensation nuclei properties and droplet growth kinetics of the water-soluble aerosol fraction in Mexico City

NASA Astrophysics Data System (ADS)

Padró, Luz T.; Tkacik, Daniel; Lathem, Terry; Hennigan, Chris J.; Sullivan, Amy P.; Weber, Rodney J.; Huey, L. Greg; Nenes, Athanasios

2010-05-01

We present hygroscopic and cloud condensation nuclei (CCN) relevant properties of the water-soluble fraction of Mexico City aerosol collected upon filters during the 2006 Megacity Initiative: Local and Global Research Observations (MILAGRO) campaign. Application of κ-Köhler theory to the observed CCN activity gave a fairly constant hygroscopicity parameter (κ = 0.28 ± 0.06) regardless of location and organic fraction. Köhler theory analysis was used to understand this invariance by separating the molar volume and surfactant contributions to the CCN activity. Organics were found to depress surface tension (10-15%) from that of pure water. Daytime samples exhibited lower molar mass (˜200 amu) and surface tension depression than nighttime samples (˜400 amu); this is consistent with fresh hygroscopic secondary organic aerosol (SOA) condensing onto particles during peak photochemical hours, subsequently aging during nighttime periods of high relative humidity. Changes in surface tension partially compensate for shifts in average molar volume to give the constant hygroscopicity observed, which implies the amount (volume fraction) of soluble material in the parent aerosol is the key composition parameter required for CCN predictions. This finding, if applicable elsewhere, may explain why CCN predictions are often found to be insensitive to assumptions of chemical composition and provides a very simple way to parameterize organic hygroscopicity in atmospheric models (i.e., κorg = 0.28ɛWSOC). Special care should be given, however, to surface tension depression from organic surfactants, as its nonlinear dependence with organic fraction may introduce biases in observed (and predicted) hygroscopicity. Finally, threshold droplet growth analysis suggests the water-soluble organics do not affect activation kinetics.

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

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.

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.

Laboratory study of the effect of oxalic acid on the cloud condensation nuclei activity of mineral dust aerosol

NASA Astrophysics Data System (ADS)

Gierlus, Kelly M.; Laskina, Olga; Abernathy, Tricia L.; Grassian, Vicki H.

2012-01-01

Dicarboxylic acids, which make up a significant portion of the atmospheric organic aerosol, are emitted directly through biomass burning as well as produced through the oxidation of volatile organic compounds. Oxalic acid, the most abundant of the dicarboxylic acids, has been shown by recent field studies to be present in mineral dust aerosol particles. The presence of these internally mixed organic compounds can alter the water absorption and cloud condensation nuclei (CCN) abilities of mineral particles in the Earth's atmosphere. The University of Iowa's Multi-Analysis Aerosol Reactor System ( MAARS) was used to measure the CCN activity of internally mixed particles that were generated from a mixture of either calcite or polystyrene latex spheres (PSLs) in an aqueous solution of oxalic acid. Although PSL is not a mineral dust component, it is used here as a non-reactive, insoluble particle. CCN measurements indicate that the internally mixed oxalate/calcite particles showed nearly identical CCN activity compared to the original calcite particles whereas oxalic acid/PSL internally mixed particles showed much greater CCN activity compared to PSL particles alone. This difference is due to the reaction of calcite with oxalic acid, which produces a relatively insoluble calcium oxalate coating on the particle surface and not a soluble coating as it does on the PSL particle. Our results suggest that atmospheric processing of mineral dust aerosol through heterogeneous processes will likely depend on the mineralogy and the specific chemistry involved. Increase in the CCN activity by incorporation of oxalic acid are only expected for unreactive insoluble dust particles that form a soluble coating.

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.

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

NASA Astrophysics Data System (ADS)

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

2017-03-01

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

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

NASA Astrophysics Data System (ADS)

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

2017-01-01

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

Effect of metal complex formation on the potential of organic aerosols as cloud condensation nuclei

NASA Astrophysics Data System (ADS)

Furukawa, T.; Takahashi, Y.

2010-12-01

Secondary organic aerosols (SOA) play a key role on the solar radiation balance in troposphere, since SOA can act as cloud condensation nuclei (CCN) due to its high hygroscopic nature. Oxalic acid is one of the most dominant components of SOA, which has cooling effects of the earth by acting as CCN. However, it is uncertain whether the oxalic acid can exist as free oxalic acid or metal-oxalate complexes in aerosols, even if there is a largedifference in their solubilities into water. Consequently, XAFS measurement was conducted to demonstrate the presence of metal-oxalate complexes. Size fractionated aerosol samples were collected in Tsukuba (located at northeast about 60 km from Tokyo) using a low-volume Andersen-type air sampler. The sampler had eight stages and a back-up filter. The sampling was conducted during winter and summer in 2002. Calcium oxalate was observed in finer particles in each period from Ca K-edge XANES, and its fractions among total Ca were approximately 20%. Similarly,, Zn oxalate was also detected in finer particles from Zn K-edge XANES and EXAFS. The [Zn-oxalate] / [Zn]total ratio in each period clearly increased with the decrease in the particle diameter. This result revealed that Zn-oxalate was formed in the aqueous phase at particle surfaces or in cloud processing. In other words, Zn-oxalate was abundant at the particle surface, resulting from the increase in the [surface]/[bulk] ratio with decreasing particle size. Based on (i) total concentrations of oxalate, Ca, and Zn determined by ion-chromatography and ICP-AES analyses and (ii) Ca- and Zn- oxalate fractions obtained by XAFS, we determined the fraction of metal-oxalate complexes among total oxalate in aerosols. In winter, Ca- and Zn- oxalate fractions reached about 60% of total oxalate in the ranges of 1.1-2.1 μm and 0.65-1.1 μm, while the value was about 60-80% in the same particle size range in summer. On the other hand, Ca- and Zn- oxalates are highly insoluble, showing that

Atmospheric nuclei in the Pacific midtroposphere: Their nature, concentration, and evolution

NASA Technical Reports Server (NTRS)

Clarke, Antony D.

1993-01-01

An extensive flight series was carried out during May-June 1990 in the remote North and South Pacific free tropospheric aboard the NASA DC-8. Condensation nuclei counters and optical particle counters provided information on aerosol particles with diameters between 0.003 and 7.0 micrometers. Vertical profiles revealed aerosol layers to be a common feature of the free troposphere. Regions with highest aerosol mass tended to have the highest concentrations of surface-derived nuclei but the lowest concentrations of total nuclei. Regions with lowest aerosol mass tended to have the highest concentrations of the smaller 'ultrafine' condensation nuclei with diameters below 0.02 mircometers. Horizontal transects totaling over 35,000 km at about 9 to 10-km altitude exhibited variability of approximately 3 orders of magnitude in both aerosol mass and number concentrations over spatial scales ranging from 1 to 1000 km. At these altitudes an approximate inverse relationship between ultrafine concentrations and the surface area of the larger aerosol was evident. Regions having lowest aerosol mass were characterized by aerosol thermal volatility, indicative of a predominately sulfuric acid composition, and by very high concentrations of ultrafine nuclei, indicative of recent homogeneous nucleation. These conditions were frequently observed but were conspicuously evident above cloud over the intertropical convergence zone. The clean, free troposphere appears to be a significant source region for new tropospheric nuclei. A simplified model of the lifetime, coagulation, and cycling of these nuclei suggests that they constitute a source of cloud condensation nuclei in the lower troposphere.

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

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

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

PubMed Central

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

2017-01-01

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

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

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.

Cloud Condensation Nuclei in Cumulus Humilis - Selected Case Study During the CHAPS Campaign

NASA Astrophysics Data System (ADS)

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

2009-12-01

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 pact scavenging. The 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 on cloud top and cloud base as well as with 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 determined 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 was switched between the isokinetic inlet and the CVI to allow characterization of interstitial particles out 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 temperature were measured. This work will focus on studying 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 SEM/TEM coupled with EDX. We will specifically look into differences in particle properties such as chemical composition and morphology between activated and interstitial ones. The second analysis will link in situ measurements with the snap shots observations by TRAC. For instance, by looking into the characteristic m/z obtained by AMS vs. CO or isoprene, one can gain

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.

AN EXPERIMENTAL STUDY ON ARTIFICIAL CONDENSATION NUCLEI,

DTIC Science & Technology

NH4Cl, CaCl2, P205, NH4NO3, (NH4)2SO4, etc.) and suspensoids such as camphor , silicon minerals, kaolin, lamp black, and calcium lime (CaO). The...findings reveal that the above mentioned soluble nuclei and camphor powder are active artificial hygroscopic condensation nuclei and that lamp black

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.

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.

Cloud Condensation Nuclei Measurements During the First Year of the ORACLES Study

NASA Astrophysics Data System (ADS)

Kacarab, M.; Howell, S. G.; Wood, R.; Redemann, J.; Nenes, A.

2016-12-01

Aerosols have significant impacts on air quality and climate. Their ability to scatter and absorb radiation and to act as cloud condensation nuclei (CCN) plays a very important role in the global climate. Biomass burning organic aerosol (BBOA) can drastically elevate the concentration of CCN in clouds, but the response in droplet number may be strongly suppressed (or even reversed) owing to low supersaturations that may develop from the strong competition of water vapor (Bougiatioti et al. 2016). Understanding and constraining the magnitude of droplet response to biomass burning plumes is an important component of the aerosol-cloud interaction problem. The southeastern Atlantic (SEA) cloud deck provides a unique opportunity to study these cloud-BBOA interactions for marine stratocumulus, as it is overlain by a large, optically thick biomass burning aerosol plume from Southern Africa during the burning season. The interaction between these biomass burning aerosols and the SEA cloud deck is being investigated in the NASA ObseRvations of Aerosols above Clouds and their intEractionS (ORACLES) study. The CCN activity of aerosol around the SEA cloud deck and associated biomass burning plume was evaluated during the first year of the ORACLES study with direct measurements of CCN concentration, aerosol size distribution and composition onboard the NASA P-3 aircraft during August and September of 2016. Here we present analysis of the observed CCN activity of the BBOA aerosol in and around the SEA cloud deck and its relationship to aerosol size, chemical composition, and plume mixing and aging. We also evaluate the predicted and observed droplet number sensitivity to the aerosol fluctuations and quantify, using the data, the drivers of droplet number variability (vertical velocity or aerosol properties) as a function of biomass burning plume characteristics.

Condensation Kinetics of Water on Amorphous Aerosol Particles.

PubMed

Rothfuss, Nicholas E; Marsh, Aleksandra; Rovelli, Grazia; Petters, Markus D; Reid, Jonathan P

2018-06-25

Responding to changes in the surrounding environment, aerosol particles can grow by water condensation changing rapidly in composition and changing dramatically in viscosity. The timescale for growth is important to establish for particles undergoing hydration processes in the atmosphere or during inhalation. Using an electrodynamic balance, we report direct measurements at -7.5, 0, and 20 °C of timescales for hygroscopic condensational growth on a range of model hygroscopic aerosol systems. These extend from viscous aerosol particles containing a single saccharide solute (sucrose, glucose, raffinose, or trehalose) and a starting viscosity equivalent to a glass of ∼10 12 Pa·s, to nonviscous (∼10 -2 Pa·s) tetraethylene glycol particles. The condensation timescales observed in this work indicate that water condensation occurs rapidly at all temperatures examined (<10 s) and for particles of all initial viscosities spanning 10 -2 to 10 12 Pa·s. Only a marginal delay (<1 order of magnitude) is observed for particles starting as a glass.

Can Condensing Organic Aerosols Lead to Less Cloud Particles?

NASA Astrophysics Data System (ADS)

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

2017-12-01

We examined the impact of condensing organic aerosols on activated cloud number concentration in a new aerosol microphysics box model, MATRIX-VBS. The model includes the volatility-basis set (VBS) framework in an aerosol microphysical scheme MATRIX (Multiconfiguration Aerosol TRacker of mIXing state) that resolves aerosol mass and number concentrations and aerosol mixing state. Preliminary results show that by including the condensation of organic aerosols, the new model (MATRIX-VBS) has less activated particles compared to the original model (MATRIX), which treats organic aerosols as non-volatile. Parameters such as aerosol chemical composition, mass and number concentrations, and particle sizes which affect activated cloud number concentration are thoroughly evaluated via a suite of Monte-Carlo simulations. The Monte-Carlo simulations also provide information on which climate-relevant parameters play a critical role in the aerosol evolution in the atmosphere. This study also helps simplifying the newly developed box model which will soon be implemented in the global model GISS ModelE as a module.

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.

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

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.

RACORO aerosol data processing

DOE Office of Scientific and Technical Information (OSTI.GOV)

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 measurementsmore » 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.« less

An uncertainty analysis for satellite-based estimates of cloud condensation nuclei number concentrations

NASA Astrophysics Data System (ADS)

Shinozuka, Y.; Clarke, A. D.; Nenes, A.; Jefferson, A.; Wood, R.; McNaughton, C. S.; Ström, J.; Tunved, P.; Redemann, J.; Thornhill, K. L., II; Moore, R.; Lathem, T. L.; Lin, J.; Yoon, Y. J.

2017-12-01

Aerosol-cloud interactions (ACI) are the largest source of uncertainty in estimates of anthropogenic radiative forcing responsible for the on-going climate change. ACI for warm clouds depend on the number concentration of cloud condensation nuclei (CCN), not on aerosol optical properties. Yet, aerosol optical depth (AOD) and its variants weighted by the spectral dependence over visible and near infrared wavelengths are commonly substituted for CCN in ACI studies. The substitution is motivated by the wide availability in space and time of satellite retrievals, an advantage over the sparse CCN measurements. If satellite-based CCN estimates are to continue to complement purely model-based ones, what CCN-AOD relationship should we assume and how large is the associated uncertainty? Our 2015 paper examines airborne and ground-based observations of aerosols to address these questions, focusing on the relationship between CCN and light extinction, σ, of dried particles averaged over one-kilometer horizontal distance. That paper discusses the way the CCN-AOD relationship is influenced not only by the CCN-σ relationship but also by the humidity response of light extinction, the vertical profile, the horizontal-temporal variability and the AOD measurement error. In this presentation, we apply these findings to passive satellite data to analyze the uncertainty in satellite-based CCN estimates.

Global variability of cloud condensation nuclei concentrations

NASA Astrophysics Data System (ADS)

Makkonen, Risto; Krüger, Olaf

2017-04-01

Atmospheric aerosols can influence cloud optical and dynamical processes by acting as cloud condensation nuclei (CCN). Globally, these indirect aerosol effects are significant to the radiative budget as well as a source of high uncertainty in anthropogenic radiative forcing. While historically many global climate models have fixed CCN concentrations to a certain level, most state-of-the-art models calculate aerosol-cloud interactions with sophisticated methodologies based on interactively simulated aerosol size distributions. However, due to scarcity of atmospheric observations simulated global CCN concentrations remain poorly constrained. Here we assess global CCN variability with a climate model, and attribute potential trends during 2000-2010 to changes in emissions and meteorological fields. Here we have used ECHAM5.5-HAM2 with model M7 microphysical aerosol model. The model has been upgraded with a secondary organic aerosol (SOA) scheme including ELVOCs. Dust and sea salt emissions are calculated online, based on wind speed and hydrology. Each experiment is 11 years, analysed after a 6-month spin-up period. The MODIS CCN product (Terra platform) is used to evaluate model performance throughout 2000-2010. While optical remote observation of CCN column includes several deficiencies, the products serves as a proxy for changes during the simulation period. In our analysis we utilize the observed and simulated vertical column integrated CCN concentration, and limit our analysis only over marine regions. Simulated annual CCN column densities reach 2ṡ108 cm-2 near strong source regions in central Africa, Arabian Sea, Bay of Bengal and China sea. The spatial concentration gradient in CCN(0.2%) is steep, and column densities drop to <50% a few hundred kilometers away from the coasts. While the spatial distribution of CCN at 0.2% supersaturation is closer to that of MODIS proxy, as opposed to 1.0% supersaturation, the overall column integrated CCN are too low. Still

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.

Cloud condensation nuclei activity of aliphatic amine secondary aerosol

USDA-ARS?s Scientific Manuscript database

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 ...

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

Ice nuclei emissions from biomass burning

Treesearch

Markus D. Petters; Matthew T. Parsons; Anthony J. Prenni; Paul J. DeMott; Sonia M. Kreidenweis; Christian M. Carrico; Amy P. Sullivan; Gavin R. McMeeking; Ezra Levin; Cyle E. Wold; Jeffrey L. Collett; Hans Moosmuller

2009-01-01

Biomass burning is a significant source of carbonaceous aerosol in many regions of the world. When present, biomass burning particles may affect the microphysical properties of clouds through their ability to function as cloud condensation nuclei or ice nuclei. We report on measurements of the ice nucleation ability of biomass burning particles performed on laboratory-...

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

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

PubMed Central

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

2013-01-01

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 [CnH(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. PMID:23674675

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.

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.

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

2002-06-06

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.

Partially soluble organics as cloud condensation nuclei: Role of trace soluble and surface active species

NASA Astrophysics Data System (ADS)

Broekhuizen, K.; Kumar, P. Pradeep; Abbatt, J. P. D.

2004-01-01

The ability of partially soluble organic species to act as cloud condensation nuclei (CCN) has been studied. A Köhler model incorporating solute solubility and droplet surface tension describes the behavior of solid adipic and succinic acid particles, whereas solid azelaic acid activates much more efficiently that predicted. In addition, it was shown that trace levels of either sulfate or surface active species have a dramatic effect on the activation of adipic acid, a moderately soluble organic, as predicted by the full Köhler model. For internally mixed particles in the atmosphere, these effects will greatly enhance the role of organic aerosols as CCN.

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

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pöhlker, Mira L.; Pöhlker, Christopher; Ditas, Florian

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

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

DOE PAGES

Pöhlker, Mira L.; Pöhlker, Christopher; Ditas, Florian; ...

2016-12-20

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

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.

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cziczo, D.

2016-03-01

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

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

PubMed

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

2012-07-17

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

Aerosol partitioning between the interstitial and the condensed phase in mixed-phase clouds

NASA Astrophysics Data System (ADS)

Verheggen, Bart; Cozic, Julie; Weingartner, Ernest; Bower, Keith; Mertes, Stephan; Connolly, Paul; Gallagher, Martin; Flynn, Michael; Choularton, Tom; Baltensperger, Urs

2007-12-01

The partitioning of aerosol particles between the cloud and the interstitial phase (i.e., unactivated aerosol) has been investigated during several Cloud and Aerosol Characterization Experiments (CLACE-3, CLACE-3? and CLACE-4) conducted in winter and summer 2004 and winter 2005 at the high alpine research station Jungfraujoch (3580 m altitude, Switzerland). Ambient air was sampled using different inlets in order to determine the activated fraction of aerosol particles, FN, defined as the fraction of the total aerosol number concentration (with particle diameter dp > 100 nm) that has been incorporated into cloud particles. The liquid and ice water content of mixed-phase clouds were characterized by analyzing multiple cloud probes. The dependence of the activated fraction on several environmental factors is discussed on the basis of more than 900 h of in-cloud observations and parameterizations for key variables are given. FN is found to increase with increasing liquid water content and to decrease with increasing particle number concentration in liquid clouds. FN also decreases with increasing cloud ice mass fraction and with decreasing temperature from 0 to -25°C. The Wegener-Bergeron-Findeisen process probably contributed to this trend, since the presence of ice crystals causes liquid droplets to evaporate, thus releasing the formerly activated particles back into the interstitial phase. Ice nucleation could also have prevented additional cloud condensation nuclei from activating. The observed activation behavior has significant implications for our understanding of the indirect effect of aerosols on climate.

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.

Long-term observations of cloud condensation nuclei in the Amazon rain forest

NASA Astrophysics Data System (ADS)

Pöhlker, Mira L.; Pöhlker, Christopher; Ditas, Florian; Klimach, Thomas; Hrabe de Angelis, Isabella; Brito, Joel; Carbone, Samara; Cheng, Yafang; Martin, Scot T.; Moran-Zuloaga, Daniel; Rose, Diana; Saturno, Jorge; Su, Hang; Thalman, Ryan; Walter, David; Wang, Jian; Barbosa, Henrique; Artaxo, Paulo; Andreae, Meinrat O.; Pöschl, Ulrich

2017-04-01

Size-resolved long-term measurements of atmospheric aerosol and cloud condensation nuclei (CCN) concentrations and hygroscopicity were conducted at the remote Amazon Tall Tower Observatory (ATTO) in the central Amazon Basin over a full seasonal cycle (Mar 2014 - Feb 2015). The measurements provide a climatology of CCN properties characteristic of a remote central Amazonian rain forest site [1,2]. The CCN measurements were continuously cycled through 10 levels of supersaturation (S = 0.11 to 1.10 %) and span the aerosol particle size range from 20 to 245 nm. The particle hygroscopicity exhibits a pronounced size dependence with lower values for the Aitken mode (κAit = 0.14 ± 0.03), higher values for the accumulation mode (κAcc = 0.22 ± 0.05), and an overall mean value of κmean = 0.17 ± 0.06, consistent with high fractions of organic aerosol. The hygroscopicity parameter, κ, exhibits remarkably little temporal variability: no pronounced diurnal cycles, only weak seasonal trends, and few short-term variations during long-range transport events. In contrast, the CCN number concentrations exhibit a pronounced seasonal cycle, tracking the pollution-related seasonality in total aerosol concentration. We find that the variability in the CCN concentrations in the central Amazon is mostly driven by aerosol particle number concentration and size distribution, while variations in aerosol hygroscopicity and chemical composition matter only during a few episodes. For modelling purposes, we compare different approaches of predicting CCN number concentration and present a novel parameterization, which allows accurate CCN predictions based on a small set of input data. In addition, we analyzed the CCN short-term variability in relation to air mass changes as well as aerosol emission and transformation processes. The CCN short term variability is presented for selected case studies, which analyze particularly interesting and characteristic events/conditions in the Amazon

Characterisation of aerosol combustible mixtures generated using condensation process

NASA Astrophysics Data System (ADS)

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

2012-06-01

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

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

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.

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

NASA Technical Reports Server (NTRS)

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

1988-01-01

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

Substantial Seasonal Contribution of Observed Biogenic Sulfate Particles to Cloud Condensation Nuclei.

PubMed

Sanchez, Kevin J; Chen, Chia-Li; Russell, Lynn M; Betha, Raghu; Liu, Jun; Price, Derek J; Massoli, Paola; Ziemba, Luke D; Crosbie, Ewan C; Moore, Richard H; Müller, Markus; Schiller, Sven A; Wisthaler, Armin; Lee, Alex K Y; Quinn, Patricia K; Bates, Timothy S; Porter, Jack; Bell, Thomas G; Saltzman, Eric S; Vaillancourt, Robert D; Behrenfeld, Mike J

2018-02-19

Biogenic sources contribute to cloud condensation nuclei (CCN) in the clean marine atmosphere, but few measurements exist to constrain climate model simulations of their importance. The chemical composition of individual atmospheric aerosol particles showed two types of sulfate-containing particles in clean marine air masses in addition to mass-based Estimated Salt particles. Both types of sulfate particles lack combustion tracers and correlate, for some conditions, to atmospheric or seawater dimethyl sulfide (DMS) concentrations, which means their source was largely biogenic. The first type is identified as New Sulfate because their large sulfate mass fraction (63% sulfate) and association with entrainment conditions means they could have formed by nucleation in the free troposphere. The second type is Added Sulfate particles (38% sulfate), because they are preexisting particles onto which additional sulfate condensed. New Sulfate particles accounted for 31% (7 cm -3 ) and 33% (36 cm -3 ) CCN at 0.1% supersaturation in late-autumn and late-spring, respectively, whereas sea spray provided 55% (13 cm -3 ) in late-autumn but only 4% (4 cm -3 ) in late-spring. Our results show a clear seasonal difference in the marine CCN budget, which illustrates how important phytoplankton-produced DMS emissions are for CCN in the North Atlantic.

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.

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.

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.

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.

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

NASA Astrophysics Data System (ADS)

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

2012-08-01

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

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rosenfeld, Daniel; Zheng, Youtong; Hashimshoni, Eyal

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

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

DOE PAGES

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

2016-03-04

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

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.

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.

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.

Aerosol effects on cloud water amounts were successfully simulated by a global cloud-system resolving model.

PubMed

Sato, Yousuke; Goto, Daisuke; Michibata, Takuro; Suzuki, Kentaroh; Takemura, Toshihiko; Tomita, Hirofumi; Nakajima, Teruyuki

2018-03-07

Aerosols affect climate by modifying cloud properties through their role as cloud condensation nuclei or ice nuclei, called aerosol-cloud interactions. In most global climate models (GCMs), the aerosol-cloud interactions are represented by empirical parameterisations, in which the mass of cloud liquid water (LWP) is assumed to increase monotonically with increasing aerosol loading. Recent satellite observations, however, have yielded contradictory results: LWP can decrease with increasing aerosol loading. This difference implies that GCMs overestimate the aerosol effect, but the reasons for the difference are not obvious. Here, we reproduce satellite-observed LWP responses using a global simulation with explicit representations of cloud microphysics, instead of the parameterisations. Our analyses reveal that the decrease in LWP originates from the response of evaporation and condensation processes to aerosol perturbations, which are not represented in GCMs. The explicit representation of cloud microphysics in global scale modelling reduces the uncertainty of climate prediction.

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gogoi, Mukunda M.; Babu, S. Suresh; Jayachandran, V.

2015-03-27

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

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.

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

NASA Astrophysics Data System (ADS)

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

2011-04-01

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

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

NASA Astrophysics Data System (ADS)

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

2010-12-01

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

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.

Cloud condensation nuclei in pristine tropical rainforest air of Amazonia: size-resolved measurements and modeling of atmospheric aerosol composition and CCN activity

NASA Astrophysics Data System (ADS)

Gunthe, S. S.; King, S. M.; Rose, D.; Chen, Q.; Roldin, P.; Farmer, D. K.; Jimenez, J. L.; Artaxo, P.; Andreae, M. O.; Martin, S. T.; Pöschl, U.

2009-10-01

Atmospheric aerosol particles serving as cloud condensation nuclei (CCN) are key elements of the hydrological cycle and climate. We have measured and characterized CCN at water vapor supersaturations in the range of S=0.10-0.82% in pristine tropical rainforest air during the AMAZE-08 campaign in central Amazonia. The effective hygroscopicity parameters describing the influence of chemical composition on the CCN activity of aerosol particles varied in the range of κ≍0.1-0.4 (0.16±0.06 arithmetic mean and standard deviation). The overall median value of κ≍0.15 was by a factor of two lower than the values typically observed for continental aerosols in other regions of the world. Aitken mode particles were less hygroscopic than accumulation mode particles (κ≍0.1 at D≍50 nm; κ≍0.2 at D≍200 nm), which is in agreement with earlier hygroscopicity tandem differential mobility analyzer (H-TDMA) studies. The CCN measurement results are consistent with aerosol mass spectrometry (AMS) data, showing that the organic mass fraction (forg) was on average as high as ~90% in the Aitken mode (D≤100 nm) and decreased with increasing particle diameter in the accumulation mode (~80% at D≍200 nm). The κ values exhibited a negative linear correlation with forg (R2=0.81), and extrapolation yielded the following effective hygroscopicity parameters for organic and inorganic particle components: κorg≍0.1 which can be regarded as the effective hygroscopicity of biogenic secondary organic aerosol (SOA) and κinorg≍0.6 which is characteristic for ammonium sulfate and related salts. Both the size dependence and the temporal variability of effective particle hygroscopicity could be parameterized as a function of AMS-based organic and inorganic mass fractions (κp=κorg×forg +κinorg×finorg). The CCN number concentrations predicted with κp were in fair agreement with the measurement results (~20% average deviation). The median CCN number concentrations at S=0

Cloud condensation nuclei in pristine tropical rainforest air of Amazonia: size-resolved measurements and modeling of atmospheric aerosol composition and CCN activity

NASA Astrophysics Data System (ADS)

Gunthe, S. S.; King, S. M.; Rose, D.; Chen, Q.; Roldin, P.; Farmer, D. K.; Jimenez, J. L.; Artaxo, P.; Andreae, M. O.; Martin, S. T.; Pöschl, U.

2009-02-01

Atmospheric aerosol particles serving as cloud condensation nuclei (CCN) are key elements of the hydrological cycle and climate. We have measured and characterized CCN at water vapor supersaturations in the range of S=0.10-0.82% in pristine tropical rainforest air during the AMAZE-08 campaign in central Amazonia. The effective hygroscopicity parameters describing the influence of chemical composition on the CCN activity of aerosol particles varied in the range of κ=0.05-0.45. The overall median value of κ≍0.15 was only half of the value typically observed for continental aerosols in other regions of the world. Aitken mode particles were less hygroscopic than accumulation mode particles (κ≍0.1 at D≍50 nm; κ≍0.2 at D≍200 nm). The CCN measurement results were fully consistent with aerosol mass spectrometry (AMS) data, which showed that the organic mass fraction (Xm,org) was on average as high as ~90% in the Aitken mode (D≤100 nm) and decreased with increasing particle diameter in the accumulation mode (~80% at D≍200 nm). The κ values exhibited a close linear correlation with Xm,org and extrapolation yielded the following effective hygroscopicity parameters for organic and inorganic particle components: κorg≍0.1 which is consistent with laboratory measurements of secondary organic aerosols and κinorg≍0.6 which is characteristic for ammonium sulfate and related salts. Both the size-dependence and the temporal variability of effective particle hygroscopicity could be parameterized as a function of AMS-based organic and inorganic mass fractions (κp=0.1 Xm,org+0.6 Xm,inorg), and the CCN number concentrations predicted with κp were in fair agreement with the measurement results. The median CCN number concentrations at S=0.1-0.82% ranged from NCCN,0.10≍30 cm-3 to NCCN,0.82≍150 cm-3, the median concentration of aerosol particles larger than 30 nm was NCN,30≍180 cm-3, and the corresponding integral CCN efficiencies were in the range of NCCN,0

Organic cloud condensation nuclei: the effect of phase, surface tension, trace soluble species, and oxidative processing on particle activation.

NASA Astrophysics Data System (ADS)

Broekhuizen, K. E.; Thornberry, T.; Abbatt, J. P.

2003-12-01

The ability of organic aerosols to act as cloud condensation nuclei (CCN) will be discussed. A variety of laboratory experiments will be presented which address several key questions concerning organic particle activation. Does the particle phase impact activation? How does surface tension play a role and can a trace amount of a surface active species impact activation? Does a trace amount of a highly soluble species impact the activation of organic particles of moderate to low solubility? Can the activation properties of organic aerosols be enhanced through oxidative processing? To systematically address these issues, the CCN activity of various diacids such as oxalic, malonic, succinic, adipic and azelaic acid have been studied, as well as the addition of trace amounts of nonanoic acid and ammonium sulfate to examine the roles of surface active and soluble species, respectively. The first examination of the role of oxidative processing on CCN activity has involved investigating the effect of ozone oxidation on the activity of oleic acid particles.

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.

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

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 (T_max) in the central and...

Amazon boundary layer aerosol concentration sustained by vertical transport during rainfall

DOE PAGES

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

2016-10-24

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

Amazon boundary layer aerosol concentration sustained by vertical transport during rainfall

NASA Astrophysics Data System (ADS)

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

2016-11-01

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

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

PubMed

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

2016-11-17

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

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.

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.

Cloud condensation nuclei droplet growth kinetics of ultrafine particles during anthropogenic nucleation events

NASA Astrophysics Data System (ADS)

Shantz, N. C.; Pierce, J. R.; Chang, R. Y.-W.; Vlasenko, A.; Riipinen, I.; Sjostedt, S.; Slowik, J. G.; Wiebe, A.; Liggio, J.; Abbatt, J. P. D.; Leaitch, W. R.

2012-02-01

Evolution of the cloud condensation nucleus (CCN) activity of 36 ± 4 nm diameter anthropogenic aerosol particles at a water supersaturation of 1.0 ± 0.1% is examined for particle nucleation and growth. During the early stages of one event, relatively few of the anthropogenic particles at 36 nm were CCN active and their growth rates by water condensation were delayed relative to ammonium sulphate particles. As the event progressed, the particle size distribution evolved to larger sizes and the relative numbers of particles at 36 nm that were CCN active increased until all the 36 nm particles were activating at the end of the event. Based on the chemistry of larger particles and the results from an aerosol chemical microphysics box model, the increase in CCN activity of the particles was most likely the result of the condensation of sulphate in this case. Despite the increased CCN activity, a delay was observed in the initial growth of these particles into cloud droplets, which persisted even when the aerosol was most CCN active later in the afternoon. Simulations show that the delay in water uptake is explained by a reduction of the mass accommodation coefficient assuming that the composition of the 36 nm particles is the same as the measured composition of the 60-100 nm particles.

Marine Aerosols and Clouds.

PubMed

Brooks, Sarah D; Thornton, Daniel C O

2018-01-03

The role of marine bioaerosols in cloud formation and climate is currently so uncertain that even the sign of the climate forcing is unclear. Marine aerosols form through direct emissions and through the conversion of gas-phase emissions to aerosols in the atmosphere. The composition and size of aerosols determine how effective they are in catalyzing the formation of water droplets and ice crystals in clouds by acting as cloud condensation nuclei and ice nucleating particles, respectively. Marine organic aerosols may be sourced both from recent regional phytoplankton blooms that add labile organic matter to the surface ocean and from long-term global processes, such as the upwelling of old refractory dissolved organic matter from the deep ocean. Understanding the formation of marine aerosols and their propensity to catalyze cloud formation processes are challenges that must be addressed given the major uncertainties associated with aerosols in climate models.

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

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 Kohler 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. Furthermore, 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

New particle formation and growth in biomass burning plumes: An important source of cloud condensation nuclei

NASA Astrophysics Data System (ADS)

Hennigan, Christopher J.; Westervelt, Daniel M.; Riipinen, Ilona; Engelhart, Gabriella J.; Lee, Taehyoung; Collett, Jeffrey L., Jr.; Pandis, Spyros N.; Adams, Peter J.; Robinson, Allen L.

2012-05-01

Experiments were performed in an environmental chamber to characterize the effects of photo-chemical aging on biomass burning emissions. Photo-oxidation of dilute exhaust from combustion of 12 different North American fuels induced significant new particle formation that increased the particle number concentration by a factor of four (median value). The production of secondary organic aerosol caused these new particles to grow rapidly, significantly enhancing cloud condensation nuclei (CCN) concentrations. Using inputs derived from these new data, global model simulations predict that nucleation in photo-chemically aging fire plumes produces dramatically higher CCN concentrations over widespread areas of the southern hemisphere during the dry, burning season (Sept.-Oct.), improving model predictions of surface CCN concentrations. The annual indirect forcing from CCN resulting from nucleation and growth in biomass burning plumes is predicted to be -0.2 W m-2, demonstrating that this effect has a significant impact on climate that has not been previously considered.

Aerosol Production and Growth in the Upper Troposphere over the Amazon Forest Observed during ACRIDICON-CHUVA

NASA Astrophysics Data System (ADS)

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

2016-12-01

Observations during ACRIDICON-CHUVA showed high aerosol concentrations in the upper troposphere (UT) over the Amazon Basin, with aerosol number concentrations after normalization to STP often exceeding those in the boundary layer (BL) by one or two orders of magnitude. The measurements were made during 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. The campaign 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. Aerosol enhancements were consistently observed on all flights, using 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 depleted in aerosol particles, whereas dramatically enhanced small (<90 nm diameter) aerosol number concentrations were found in UT regions that had experienced outflow from deep convection in the preceding 24-48 hours. We also found elevated concentrations of larger (>90 nm) particles in the UT, which consisted mostly of organic matter and nitrate and were very effective CCN. Our findings suggest that aerosol production takes place in the UT from volatile material brought up by deep convection, which is converted to condensable species in the UT. 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

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.

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.

Control of particle size by coagulation of novel condensation aerosols in reservoir chambers.

PubMed

Hong, John N; Hindle, Michael; Byron, Peter R

2002-01-01

The coagulation growth behavior of capillary aerosol generator (CAG) condensation aerosols was investigated in a series of reservoir chambers. Aerosols consisted of a condensed system of 0.7% w/w benzil (model drug) in propylene glycol (vehicle). These were generated into 250-, 500-, 1,000-, and 2,000-mL reservoirs in both flowing air-stream and static air experiments. Changes in drug and total aerosol particle size were measured by a MOUDI cascade impactor. In both series of experiments the CAG aerosols grew in size. Growth in flowing air-stream experiments was attributed to the amount of accumulation aerosols experienced in reservoirs during sampling and increased with increasing reservoir volume. Mean (SD) MMAD's for the total mass distribution measured for the 250- and 2,000-mL reservoirs were 0.70 (0.02) and 0.87 (0.03) microm, respectively. For the benzil mass distribution, they were 0.64 (0.02) and 0.87 (0.06) microm, respectively. Growth in static air experiments was dependent on the volume aerosol boluses were restricted to and increased with decreasing reservoir volume. Mean (SD) initial MMAD's for the benzil mass distribution for the 250- and 2,000-mL reservoirs were 1.44 (0.03) and 1.24 (0.08) microm, respectively. Holding aerosols for up to 60 sec further increased their size. Mean (SD) MMAD's for benzil after holding for 60 sec in these reservoirs were 2.28 (0.04) and 1.67 (0.09) microm, respectively. The coagulation behavior and therefore particle size of CAG aerosols may be modified and controlled by reservoir chambers for drug targeting within the respiratory tract.

Characterization of distinct Arctic aerosol accumulation modes and their sources

NASA Astrophysics Data System (ADS)

Lange, R.; Dall'Osto, M.; Skov, H.; Nøjgaard, J. K.; Nielsen, I. E.; Beddows, D. C. S.; Simo, R.; Harrison, R. M.; Massling, A.

2018-06-01

In this work we use cluster analysis of long term particle size distribution data to expand an array of different shorter term atmospheric measurements, thereby gaining insights into longer term patterns and properties of Arctic aerosol. Measurements of aerosol number size distributions (9-915 nm) were conducted at Villum Research Station (VRS), Station Nord in North Greenland during a 5 year record (2012-2016). Alongside this, measurements of aerosol composition, meteorological parameters, gaseous compounds and cloud condensation nuclei (CCN) activity were performed during different shorter occasions. K-means clustering analysis of particle number size distributions on daily basis identified several clusters. Clusters of accumulation mode aerosols (main size modes > 100 nm) accounted for 56% of the total aerosol during the sampling period (89-91% during February-April, 1-3% during June-August). By association to chemical composition, cloud condensation nuclei properties, and meteorological variables, three typical accumulation mode aerosol clusters were identified: Haze (32% of the time), Bimodal (14%) and Aged (6%). In brief: (1) Haze accumulation mode aerosol shows a single mode at 150 nm, peaking in February-April, with highest loadings of sulfate and black carbon concentrations. (2) Accumulation mode Bimodal aerosol shows two modes, at 38 nm and 150 nm, peaking in June-August, with the highest ratio of organics to sulfate concentrations. (3) Aged accumulation mode aerosol shows a single mode at 213 nm, peaking in September-October and is associated with cloudy and humid weather conditions during autumn. The three aerosol clusters were considered alongside CCN concentrations. We suggest that organic compounds, that are likely marine biogenic in nature, greatly influence the Bimodal cluster and contribute significantly to its CCN activity. This stresses the importance of better characterizing the marine ecosystem and the aerosol-mediated climate effects in the

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<...

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

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

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.

Aerosols and their Impact on Radiation, Clouds, Precipitation & Severe Weather Events

DOE Office of Scientific and Technical Information (OSTI.GOV)

Li, Zhanqing; Rosenfeld, Daniel; Fan, Jiwen

Aerosols, the tiny particles suspended in the atmosphere, have been in the forefront of environmental and climate change sciences as the primary atmospheric pollutant and external force affecting Earth’s weather and climate. There are two dominant mechanisms by which aerosols affect weather and climate: aerosol-radiation interactions (ARI) and aerosol-cloud interactions (ACI). ARI arises from aerosol scattering and absorption, which alters the radiation budgets of the atmosphere and surface, while ACI is rooted to the fact that aerosols serve as cloud condensation nuclei and ice nuclei. Both ARI and ACI are coupled with atmospheric dynamics to produce a chain of complexmore » interactions with a large range of meteorological variables that influence both weather and climate. Elaborated here are the impacts of aerosols on the radiation budget, clouds (microphysics, structure, and lifetime), precipitation, and severe weather events (lightning, thunderstorms, hail, and tornados). Depending on environmental variables and aerosol properties, the effects can be both positive and negative, posing the largest uncertainties in the external forcing of the climate system. This has considerably hindered our ability in projecting future climate changes and in doing accurate numerical weather predictions.« less

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.

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zelenyuk, Alla; Imre, D.; Earle, Michael

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 70more » 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.« less

Repulsive four-body interactions of α particles and quasistable nuclear α -particle condensates in heavy self-conjugate nuclei

NASA Astrophysics Data System (ADS)

Bai, Dong; Ren, Zhongzhou

2018-05-01

We study the effects of repulsive four-body interactions of α particles on nuclear α -particle condensates in heavy self-conjugate nuclei using a semianalytic approach, and find that the repulsive four-body interactions could decrease the critical number of α particles, beyond which quasistable α -particle condensate states can no longer exist, even if these four-body interactions make only tiny contributions to the total energy of the Hoyle-like state of 16O. Explicitly, we study eight benchmark parameter sets, and find that the critical number Ncr decreases by |Δ Ncr|˜1 -4 from Ncr˜11 with vanishing four-body interactions. We also discuss the effects of four-body interactions on energies and radii of α -particle condensates. Our study can be useful for future experiments to study α -particle condensates in heavy self-conjugate nuclei. Also, the experimental determination of Ncr will eventually help establish a better understanding on the α -particle interactions, especially the four-body interactions.

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

NASA Astrophysics Data System (ADS)

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

2011-08-01

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

Implementing marine organic aerosols into the GEOS-Chem model

DOE PAGES

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

2015-03-17

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

Implementing Marine Organic Aerosols Into the GEOS-Chem Model

NASA Technical Reports Server (NTRS)

Johnson, Matthew S.

2015-01-01

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

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.

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.

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.

Global Distribution of Solid Ammonium Sulfate Aerosols and their Climate Impact Acting as Ice Nuclei

NASA Astrophysics Data System (ADS)

Zhou, C.; Penner, J.

2017-12-01

Laboratory experiments show that liquid ammonium sulfate particles effloresce when RHw is below 34% to become solid and dissolve when RHw is above 79%. Solid ammonium sulfate aerosols can act as heterogeneous ice nuclei particles (INPs) to form ice particles in deposition mode when the relative humidity over ice is above 120%. In this study we used the coupled IMPACT/CAM5 model to track the efflorescence and deliquescence processes of ammonium sulfate. Results show that about 20% of the total simulated pure sulfate aerosol mass is in the solid state and is mainly distributed in the northern hemisphere (NH) from 50 hPa to 200 hPa. When these solid ammonium sulfate aerosols are allowed to act as ice nuclei particles, they act to increase the ice water path in the NH and reduce ice water path in the tropics. The addition of these particles leads to a positive net radiative effect at the TOA ranging from 0.5-0.9 W/m2 depending on the amounts of other ice nuclei particles (e.g., dust, soot) used in the ice nucleation process. The short-term climate feedback shows that the ITCZ shifts northwards and precipitation increases in the NH. There is also an average warming of 0.05-0.1 K near the surface (at 2 meter) in the NH which is most obvious in the Arctic region.

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.

Initial Stage of Aerosol Formation from Oversaturated Vapors

NASA Astrophysics Data System (ADS)

Lushnikov, A. A.; Zagainov, V. A.; Lyubovtseva, Yu. S.

2018-03-01

The formation of aerosol particles from oversaturated vapor was considered assuming that the stable nuclei of the new phase contain two (dimers) or three (trimers) condensing vapor molecules. Exact expressions were derived and analyzed for the partition functions of the dimer and trimer suspended in a carrier gas for the rectangular well and repulsive core intermolecular potentials. The equilibrium properties of these clusters and the nucleation rate of aerosol particles were discussed. The bound states of clusters were introduced using a limitation on their total energy: molecular clusters with a negative total energy were considered to exclude configurations with noninteracting fragments.

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.

Understanding the Impact of Model Surfactants on Cloud Condensation Nuclei Activity of Sea Spray Aerosols

NASA Astrophysics Data System (ADS)

Forestieri, S.; Cappa, C. D.; Ruehl, C. R.; Bertram, T. H.; Staudt, S.; Kuborn, T.

2017-12-01

Aerosol impacts on cloud properties, also known as indirect effects, remain a major source of uncertainty in modeling global radiative forcing. Reducing this uncertainty necessitates better understanding of how aerosol chemical composition impacts the cloud-forming ability of aerosols. The presence of surfactants in aerosols can decrease the surface tension of activating droplets relative to water and lead to more efficient activation. The importance of this effect has been debated, but recent surface tension measurements of microscopic droplets indicate that surface tension is substantially depressed relative to water for lab-generated particles consisting of salt and a single organic species and for complex mixtures of organic matter. However, little work has been done on understanding how chemical complexity (i.e. interaction between different surfactant species) impacts surface tension for particles containing mixtures of surfactants. In this work, we quantified the surface tension of lab-generated aerosols containing surfactants that are commonly found in nascent sea spray aerosol (SSA) at humidities close to activation using a continuous flow stream-wise thermal gradient chamber (CFSTGC). Surface tension was quantified for particles containing single surfactant species and mixtures of these surfactants to investigate the role of chemical complexity on surface tension and molecular packing at the air-water interface. For all surfactants tested in this study, substantial surface tension depression (20-40 mN/m) relative to water was observed for particles containing large fractions of organic matter at humidities just below activation. However, the presence of these surfactants only weakly depressed surface tension at activation. Kinetic limitations were observed for particles coated with just palmitic acid, since palmitic acid molecules inhibit water uptake through their ability to pack tightly at the surface. However, these kinetic limitations disappeared when

Strong impacts on aerosol indirect effects from historical oxidant changes

NASA Astrophysics Data System (ADS)

Hafsahl Karset, Inger Helene; Koren Berntsen, Terje; Storelvmo, Trude; Alterskjær, Kari; Grini, Alf; Olivié, Dirk; Kirkevåg, Alf; Seland, Øyvind; Iversen, Trond; Schulz, Michael

2018-06-01

Uncertainties in effective radiative forcings through aerosol-cloud interactions (ERFaci, also called aerosol indirect effects) contribute strongly to the uncertainty in the total preindustrial-to-present-day anthropogenic forcing. Some forcing estimates of the total aerosol indirect effect are so negative that they even offset the greenhouse gas forcing. This study highlights the role of oxidants in modeling of preindustrial-to-present-day aerosol indirect effects. We argue that the aerosol precursor gases should be exposed to oxidants of its era to get a more correct representation of secondary aerosol formation. Our model simulations show that the total aerosol indirect effect changes from -1.32 to -1.07 W m-2 when the precursor gases in the preindustrial simulation are exposed to preindustrial instead of present-day oxidants. This happens because of a brightening of the clouds in the preindustrial simulation, mainly due to large changes in the nitrate radical (NO3). The weaker oxidative power of the preindustrial atmosphere extends the lifetime of the precursor gases, enabling them to be transported higher up in the atmosphere and towards more remote areas where the susceptibility of the cloud albedo to aerosol changes is high. The oxidation changes also shift the importance of different chemical reactions and produce more condensate, thus increasing the size of the aerosols and making it easier for them to activate as cloud condensation nuclei.

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.

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

Description and evaluation of GLOMAP-mode: a modal global aerosol microphysics model for the UKCA composition-climate model

NASA Astrophysics Data System (ADS)

Mann, G. W.; Carslaw, K. S.; Spracklen, D. V.; Ridley, D. A.; Manktelow, P. T.; Chipperfield, M. P.; Pickering, S. J.; Johnson, C. E.

2010-10-01

A new version of the Global Model of Aerosol Processes (GLOMAP) is described, which uses a two-moment pseudo-modal aerosol dynamics approach rather than the original two-moment bin scheme. GLOMAP-mode simulates the multi-component global aerosol, resolving sulfate, sea-salt, dust, black carbon (BC) and particulate organic matter (POM), the latter including primary and biogenic secondary POM. Aerosol processes are simulated in a size-resolved manner including primary emissions, secondary particle formation by binary homogeneous nucleation of sulfuric acid and water, particle growth by coagulation, condensation and cloud-processing and removal by dry deposition, in-cloud and below-cloud scavenging. A series of benchmark observational datasets are assembled against which the skill of the model is assessed in terms of normalised mean bias (b) and correlation coefficient (R). Overall, the model performs well against the datasets in simulating concentrations of aerosol precursor gases, chemically speciated particle mass, condensation nuclei (CN) and cloud condensation nuclei (CCN). Surface sulfate, sea-salt and dust mass concentrations are all captured well, while BC and POM are biased low (but correlate well). Surface CN concentrations compare reasonably well in free troposphere and marine sites, but are underestimated at continental and coastal sites related to underestimation of either primary particle emissions or new particle formation. The model compares well against a compilation of CCN observations covering a range of environments and against vertical profiles of size-resolved particle concentrations over Europe. The simulated global burden, lifetime and wet removal of each of the simulated aerosol components is also examined and each lies close to multi-model medians from the AEROCOM model intercomparison exercise.

Description and evaluation of GLOMAP-mode: a modal global aerosol microphysics model for the UKCA composition-climate model

NASA Astrophysics Data System (ADS)

Mann, G. W.; Carslaw, K. S.; Spracklen, D. V.; Ridley, D. A.; Manktelow, P. T.; Chipperfield, M. P.; Pickering, S. J.; Johnson, C. E.

2010-05-01

A new version of the Global Model of Aerosol Processes (GLOMAP) is described, which uses a two-moment modal aerosol scheme rather than the original two-moment bin scheme. GLOMAP-mode simulates the multi-component global aerosol, resolving sulphate, sea-salt, dust, black carbon (BC) and particulate organic matter (POM), the latter including primary and biogenic secondary POM. Aerosol processes are simulated in a size-resolved manner including primary emissions, secondary particle formation by binary homogeneous nucleation of sulphuric acid and water, particle growth by coagulation, condensation and cloud-processing and removal by dry deposition, in-cloud and below-cloud scavenging. A series of benchmark observational datasets are assembled against which the skill of the model is assessed in terms of normalised mean bias (b) and correlation coefficient (R). Overall, the model performs well against the datasets in simulating concentrations of aerosol precursor gases, chemically speciated particle mass, condensation nuclei (CN) and cloud condensation nuclei (CCN). Surface sulphate, sea-salt and dust mass concentrations are all captured well, while BC and POM are biased low (but correlate well). Surface CN concentrations compare reasonably well in free troposphere and marine sites, but are underestimated at continental and coastal sites related to underestimation of either primary particle emissions or new particle formation. The model compares well against a compilation of CCN observations covering a range of environments and against vertical profiles of size-resolved particle concentrations over Europe. The simulated global burden, lifetime and wet removal of each of the simulated aerosol components is also examined and each lies close to multi-model medians from the AEROCOM model intercomparison exercise.

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

Organic condensation - a vital link connecting aerosol formation to climate forcing

NASA Astrophysics Data System (ADS)

Riipinen, I.; Pierce, J. R.; Yli-Juuti, T.; Nieminen, T.; Häkkinen, S.; Ehn, M.; Junninen, H.; Lehtipalo, K.; Petäjä, T.; Slowik, J.; Chang, R.; Shantz, N. C.; Abbatt, J.; Leaitch, W. R.; Kerminen, V.-M.; Worsnop, D. R.; Pandis, S. N.; Donahue, N. M.; Kulmala, M.

2011-01-01

Atmospheric aerosol particles influence global climate as well as impair air quality through their effects on atmospheric visibility and human health. Ultrafine (<100 nm) particles often dominate aerosol numbers, and nucleation of atmospheric vapors is an important source of these particles. To have climatic relevance, however, the freshly-nucleated particles need to grow in size. We combine observations from two continental sites (Egbert, Canada and Hyytiälä, Finland) to show that condensation of organic vapors is a crucial factor governing the lifetimes and climatic importance of the smallest atmospheric particles. We demonstrate that state-of-the-science organic gas-particle partitioning models fail to reproduce the observations, and propose a modeling approach that is consistent with the measurements. We demonstrate the large sensitivity of climatic forcing of atmospheric aerosols to these interactions between organic vapors and the smallest atmospheric nanoparticles - highlighting the need for representing this process in global climate models.

Aerosol characteristics and particle production in the upper troposphere over the Amazon Basin

NASA Astrophysics Data System (ADS)

Andreae, Meinrat O.; Afchine, Armin; Albrecht, Rachel; Amorim Holanda, Bruna; Artaxo, Paulo; Barbosa, Henrique M. J.; Borrmann, Stephan; Cecchini, Micael A.; Costa, Anja; Dollner, Maximilian; Fütterer, Daniel; Järvinen, Emma; Jurkat, Tina; Klimach, Thomas; Konemann, Tobias; Knote, Christoph; Krämer, Martina; Krisna, Trismono; Machado, Luiz A. T.; Mertes, Stephan; Minikin, Andreas; Pöhlker, Christopher; Pöhlker, Mira L.; Pöschl, Ulrich; Rosenfeld, Daniel; Sauer, Daniel; Schlager, Hans; Schnaiter, Martin; Schneider, Johannes; Schulz, Christiane; Spanu, Antonio; Sperling, Vinicius B.; Voigt, Christiane; Walser, Adrian; Wang, Jian; Weinzierl, Bernadett; Wendisch, Manfred; Ziereis, Helmut

2018-01-01

Airborne observations over the Amazon Basin showed high aerosol particle concentrations in the upper troposphere (UT) between 8 and 15 km altitude, with number densities (normalized to standard temperature and pressure) often exceeding those in the planetary boundary layer (PBL) by 1 or 2 orders of magnitude. The measurements were made during the German-Brazilian cooperative aircraft campaign ACRIDICON-CHUVA, where ACRIDICON stands for Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems and CHUVA is the acronym for Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the GPM (global precipitation measurement), on the German High Altitude and Long Range Research Aircraft (HALO). The campaign took place in September-October 2014, with the objective of studying tropical deep convective clouds over the Amazon rainforest and their interactions with atmospheric trace gases, aerosol particles, and atmospheric radiation. Aerosol enhancements were observed consistently on all flights during which the UT was probed, using several aerosol metrics, including condensation nuclei (CN) and cloud condensation nuclei (CCN) number concentrations and chemical species mass concentrations. The UT particles differed sharply in their chemical composition and size distribution from those in the PBL, ruling out convective transport of combustion-derived particles from the boundary layer (BL) as a source. The air in the immediate outflow of deep convective clouds was depleted of aerosol particles, whereas strongly enhanced number concentrations of small particles (< 90 nm diameter) were found in UT regions that had experienced outflow from deep convection in the preceding 5-72 h. We also found elevated concentrations of larger (> 90 nm) particles in the UT, which consisted mostly of organic matter and nitrate and were very effective CCN. Our findings suggest a

Aerosol characteristics and particle production in the upper troposphere over the Amazon Basin

DOE PAGES

Andreae, Meinrat O.; Afchine, Armin; Albrecht, Rachel; ...

2018-01-25

Airborne observations over the Amazon Basin showed high aerosol particle concentrations in the upper troposphere (UT) between 8 and 15 km altitude, with number densities (normalized to standard temperature and pressure) often exceeding those in the planetary boundary layer (PBL) by 1 or 2 orders of magnitude. The measurements were made during the German–Brazilian cooperative aircraft campaign ACRIDICON–CHUVA, where ACRIDICON stands for Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems and CHUVA is the acronym for Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the GPM (globalmore » precipitation measurement), on the German High Altitude and Long Range Research Aircraft (HALO). The campaign took place in September–October 2014, with the objective of studying tropical deep convective clouds over the Amazon rainforest and their interactions with atmospheric trace gases, aerosol particles, and atmospheric radiation. Aerosol enhancements were observed consistently on all flights during which the UT was probed, using several aerosol metrics, including condensation nuclei (CN) and cloud condensation nuclei (CCN) number concentrations and chemical species mass concentrations. The UT particles differed sharply in their chemical composition and size distribution from those in the PBL, ruling out convective transport of combustion-derived particles from the boundary layer (BL) as a source. The air in the immediate outflow of deep convective clouds was depleted of aerosol particles, whereas strongly enhanced number concentrations of small particles (< 90 nm diameter) were found in UT regions that had experienced outflow from deep convection in the preceding 5–72 h. We also found elevated concentrations of larger (> 90 nm) particles in the UT, which consisted mostly of organic matter and nitrate and were very effective CCN. Our findings suggest a conceptual

Aerosol characteristics and particle production in the upper troposphere over the Amazon Basin

DOE Office of Scientific and Technical Information (OSTI.GOV)

Andreae, Meinrat O.; Afchine, Armin; Albrecht, Rachel

Airborne observations over the Amazon Basin showed high aerosol particle concentrations in the upper troposphere (UT) between 8 and 15 km altitude, with number densities (normalized to standard temperature and pressure) often exceeding those in the planetary boundary layer (PBL) by 1 or 2 orders of magnitude. The measurements were made during the German–Brazilian cooperative aircraft campaign ACRIDICON–CHUVA, where ACRIDICON stands for Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems and CHUVA is the acronym for Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the GPM (globalmore » precipitation measurement), on the German High Altitude and Long Range Research Aircraft (HALO). The campaign took place in September–October 2014, with the objective of studying tropical deep convective clouds over the Amazon rainforest and their interactions with atmospheric trace gases, aerosol particles, and atmospheric radiation. Aerosol enhancements were observed consistently on all flights during which the UT was probed, using several aerosol metrics, including condensation nuclei (CN) and cloud condensation nuclei (CCN) number concentrations and chemical species mass concentrations. The UT particles differed sharply in their chemical composition and size distribution from those in the PBL, ruling out convective transport of combustion-derived particles from the boundary layer (BL) as a source. The air in the immediate outflow of deep convective clouds was depleted of aerosol particles, whereas strongly enhanced number concentrations of small particles (< 90 nm diameter) were found in UT regions that had experienced outflow from deep convection in the preceding 5–72 h. We also found elevated concentrations of larger (> 90 nm) particles in the UT, which consisted mostly of organic matter and nitrate and were very effective CCN. Our findings suggest a conceptual

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

NASA Astrophysics Data System (ADS)

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

2011-04-01

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

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

NASA Technical Reports Server (NTRS)

Gokoglu, S. A.

1987-01-01

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

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.

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.

A new method for calculating number concentrations of cloud condensation nuclei based on measurements of a three-wavelength humidified nephelometer system

NASA Astrophysics Data System (ADS)

Tao, Jiangchuan; Zhao, Chunsheng; Kuang, Ye; Zhao, Gang; Shen, Chuanyang; Yu, Yingli; Bian, Yuxuan; Xu, Wanyun

2018-02-01

The number concentration of cloud condensation nuclei (CCN) plays a fundamental role in cloud physics. Instrumentations of direct measurements of CCN number concentration (NCCN) based on chamber technology are complex and costly; thus a simple way for measuring NCCN is needed. In this study, a new method for NCCN calculation based on measurements of a three-wavelength humidified nephelometer system is proposed. A three-wavelength humidified nephelometer system can measure the aerosol light-scattering coefficient (σsp) at three wavelengths and the light-scattering enhancement factor (fRH). The Ångström exponent (Å) inferred from σsp at three wavelengths provides information on mean predominate aerosol size, and hygroscopicity parameter (κ) can be calculated from the combination of fRH and Å. Given this, a lookup table that includes σsp, κ and Å is established to predict NCCN. Due to the precondition for the application, this new method is not suitable for externally mixed particles, large particles (e.g., dust and sea salt) or fresh aerosol particles. This method is validated with direct measurements of NCCN using a CCN counter on the North China Plain. Results show that relative deviations between calculated NCCN and measured NCCN are within 30 % and confirm the robustness of this method. This method enables simplerNCCN measurements because the humidified nephelometer system is easily operated and stable. Compared with the method using a CCN counter, another advantage of this newly proposed method is that it can obtain NCCN at lower supersaturations in the ambient atmosphere.

Calibration Uncertainties in the Droplet Measurement Technologies Cloud Condensation Nuclei Counter

NASA Astrophysics Data System (ADS)

Hibert, Kurt James

Cloud condensation nuclei (CCN) serve as the nucleation sites for the condensation of water vapor in Earth's atmosphere and are important for their effect on climate and weather. The influence of CCN on cloud radiative properties (aerosol indirect effect) is the most uncertain of quantified radiative forcing changes that have occurred since pre-industrial times. CCN influence the weather because intrinsic and extrinsic aerosol properties affect cloud formation and precipitation development. To quantify these effects, it is necessary to accurately measure CCN, which requires accurate calibrations using a consistent methodology. Furthermore, the calibration uncertainties are required to compare measurements from different field projects. CCN uncertainties also aid the integration of CCN measurements with atmospheric models. The commercially available Droplet Measurement Technologies (DMT) CCN Counter is used by many research groups, so it is important to quantify its calibration uncertainty. Uncertainties in the calibration of the DMT CCN counter exist in the flow rate and supersaturation values. The concentration depends on the accuracy of the flow rate calibration, which does not have a large (4.3 %) uncertainty. The supersaturation depends on chamber pressure, temperature, and flow rate. The supersaturation calibration is a complex process since the chamber's supersaturation must be inferred from a temperature difference measurement. Additionally, calibration errors can result from the Kohler theory assumptions, fitting methods utilized, the influence of multiply-charged particles, and calibration points used. In order to determine the calibration uncertainties and the pressure dependence of the supersaturation calibration, three calibrations are done at each pressure level: 700, 840, and 980 hPa. Typically 700 hPa is the pressure used for aircraft measurements in the boundary layer, 840 hPa is the calibration pressure at DMT in Boulder, CO, and 980 hPa is the

An interfacial mechanism for cloud droplet formation on organic aerosols

DOE PAGES

Ruehl, C. R.; Davies, J. F.; Wilson, K. R.

2016-03-25

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 depressionmore » 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.« less

An interfacial mechanism for cloud droplet formation on organic aerosols

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ruehl, C. R.; Davies, J. F.; Wilson, K. R.

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 depressionmore » 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.« less

From aerosol-limited to invigoration of warm convective clouds.

PubMed

Koren, Ilan; Dagan, Guy; Altaratz, Orit

2014-06-06

Among all cloud-aerosol interactions, the invigoration effect is the most elusive. Most of the studies that do suggest this effect link it to deep convective clouds with a warm base and cold top. Here, we provide evidence from observations and numerical modeling of a dramatic aerosol effect on warm clouds. We propose that convective-cloud invigoration by aerosols can be viewed as an extension of the concept of aerosol-limited clouds, where cloud development is limited by the availability of cloud-condensation nuclei. A transition from pristine to slightly polluted atmosphere yields estimated negative forcing of ~15 watts per square meter (cooling), suggesting that a substantial part of this anthropogenic forcing over the oceans occurred at the beginning of the industrial era, when the marine atmosphere experienced such transformation. Copyright © 2014, American Association for the Advancement of Science.

OH-initiated Aging of Biomass Burning Aerosol during FIREX

NASA Astrophysics Data System (ADS)

Lim, C. Y.; Hagan, D. H.; Cappa, C. D.; Kroll, J. H.; Coggon, M.; Koss, A.; Sekimoto, K.; De Gouw, J. A.; Warneke, C.

2017-12-01

Biomass burning emissions represent a major source of fine particulate matter to the atmosphere, and this source will likely become increasingly important in the future due to changes in the Earth's climate. Understanding the effects that increased fire emissions have on both air quality and climate requires understanding the composition of the particles emitted, since chemical and physical composition directly impact important particle properties such as absorptivity, toxicity, and cloud condensation nuclei activity. However, the composition of biomass burning particles in the atmosphere is dynamic, as the particles are subject to the condensation of low-volatility vapors and reaction with oxidants such as the hydroxyl radical (OH) during transport. Here we present a series of laboratory chamber experiments on the OH-initiated aging of biomass burning aerosol performed at the Fire Sciences Laboratory in Missoula, MT as part of the Fire Influences on Regional and Global Environments Experiment (FIREX) campaign. We describe the evolution of biomass burning aerosol produced from a variety of fuels operating the chamber in both particle-only and gas + particle mode, focusing on changes to the organic composition. In particle-only mode, gas-phase biomass burning emissions are removed before oxidation to focus on heterogeneous oxidation, while gas + particle mode includes both heterogeneous oxidation and condensation of oxidized volatile organic compounds onto the particles (secondary organic aerosol formation). Variability in fuels and burning conditions lead to differences in aerosol loading and secondary aerosol production, but in all cases aging results in a significant and rapid increases in the carbon oxidation state of the particles.

Organic Condensation and Particle Growth to CCN Sizes in the Summertime Marine Arctic Is Driven by Materials More Semivolatile Than at Continental Sites

NASA Astrophysics Data System (ADS)

Burkart, Julia; Hodshire, Anna L.; Mungall, Emma L.; Pierce, Jeffrey R.; Collins, Douglas B.; Ladino, Luis A.; Lee, Alex K. Y.; Irish, Victoria; Wentzell, Jeremy J. B.; Liggio, John; Papakyriakou, Tim; Murphy, Jennifer; Abbatt, Jonathan

2017-10-01

Ship-based aerosol measurements in the summertime Arctic indicate elevated concentrations of ultrafine particles with occasional growth to cloud condensation nuclei (CCN) sizes. Focusing on one episode with two continuously growing modes, growth occurs faster for a large, preexisting mode (dp ≈ 90 nm) than for a smaller nucleation mode (dp ≈ 20 nm). We use microphysical modeling to show that growth is largely via organic condensation. Unlike results for midlatitude forested regions, most of these condensing species behave as semivolatile organics, as lower volatility organics would lead to faster growth of the smaller mode. The magnitude of the CCN hygroscopicity parameter for the growing particles, 0.1, is also consistent with organic species constituting a large fraction of the particle composition. Mixing ratios of common aerosol growth precursors, such as isoprene and sulfur dioxide, are not elevated during the episode, indicating that an unidentified aerosol growth precursor is present in this high-latitude marine environment.

Experimental investigation of aerosol composition and growth rates

NASA Astrophysics Data System (ADS)

Wimmer, Daniela; Winkler, Paul; Kulmala, Markku; Petäjä, Tuukka

2017-04-01

Atmospheric aerosol particles have relevant influence on human lives. Human health is affected, as by breathing in the aerosol particles, they deposit in the lungs causing various health problems. Also they interfere indirectly and directly with sunlight, which affects the climate on Earth. Primary aerosol particles originate for example from anthropogenic sources, such as Diesel cars or natural sources such as dessert dust. Secondary aerosol particles are formed via condensation of low volatile gas phase compounds. First, small clusters consisting of a few gas molecules only are formed, which can then grow to bigger aerosol particles. These then form seeds for cloud droplets. The chemical composition of the cloud particles determines whether the cloud absorbs or scatters sunlight more. Intensive experimental and theoretical work has been put into understanding the details of the initial processes leading to the natural formation of these secondary aerosol particles. According to modelling studies, aerosol particles formed via the nucleation process are responsible for about 50% of the global cloud condensation nuclei concentration. With currently used methods, the chemical composition of small molecular clusters (up to 2nm in diameter) can be resolved. Also standard methods to determine aerosol particle composition at sizes >10 nm are available. Within this project, the aerosol particle composition in the 2-4 nm size range will be investigated experimentally. The setup will consist of a combination of an electrical method that allows determine the electrical mobility of the particles which then can be converted to a diameter. By letting the charged particles travel through a changing electrical field, they travel at different speeds according to their mobility. That allows to particles with certain mobilities, which then can be converted to a diameter. After the size selection, the particles are counted by means of optical detection. Condensation particle counters

Constraining the instantaneous aerosol influence on cloud albedo.

PubMed

Gryspeerdt, Edward; Quaas, Johannes; Ferrachat, Sylvaine; Gettelman, Andrew; Ghan, Steven; Lohmann, Ulrike; Morrison, Hugh; Neubauer, David; Partridge, Daniel G; Stier, Philip; Takemura, Toshihiko; Wang, Hailong; Wang, Minghuai; Zhang, Kai

2017-05-09

Much of the uncertainty in estimates of the anthropogenic forcing of climate change comes from uncertainties in the instantaneous effect of aerosols on cloud albedo, known as the Twomey effect or the radiative forcing from aerosol-cloud interactions (RFaci), a component of the total or effective radiative forcing. Because aerosols serving as cloud condensation nuclei can have a strong influence on the cloud droplet number concentration ( N d ), previous studies have used the sensitivity of the N d to aerosol properties as a constraint on the strength of the RFaci. However, recent studies have suggested that relationships between aerosol and cloud properties in the present-day climate may not be suitable for determining the sensitivity of the N d to anthropogenic aerosol perturbations. Using an ensemble of global aerosol-climate models, this study demonstrates how joint histograms between N d and aerosol properties can account for many of the issues raised by previous studies. It shows that if the anthropogenic contribution to the aerosol is known, the RFaci can be diagnosed to within 20% of its actual value. The accuracy of different aerosol proxies for diagnosing the RFaci is investigated, confirming that using the aerosol optical depth significantly underestimates the strength of the aerosol-cloud interactions in satellite data.

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/).

An interfacial mechanism for cloud droplet formation on organic aerosols.

PubMed

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

2016-03-25

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. Copyright © 2016, American Association for the Advancement of Science.

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.

Observational Study and Parameterization of Aerosol-fog Interactions

NASA Astrophysics Data System (ADS)

Duan, J.; Guo, X.; Liu, Y.; Fang, C.; Su, Z.; Chen, Y.

2014-12-01

Studies have shown that human activities such as increased aerosols affect fog occurrence and properties significantly, and accurate numerical fog forecasting depends on, to a large extent, parameterization of fog microphysics and aerosol-fog interactions. Furthermore, fogs can be considered as clouds near the ground, and enjoy an advantage of permitting comprehensive long-term in-situ measurements that clouds do not. Knowledge learned from studying aerosol-fog interactions will provide useful insights into aerosol-cloud interactions. To serve the twofold objectives of understanding and improving parameterizations of aerosol-fog interactions and aerosol-cloud interactions, this study examines the data collected from fogs, with a focus but not limited to the data collected in Beijing, China. Data examined include aerosol particle size distributions measured by a Passive Cavity Aerosol Spectrometer Probe (PCASP-100X), fog droplet size distributions measured by a Fog Monitor (FM-120), Cloud Condensation Nuclei (CCN), liquid water path measured by radiometers and visibility sensors, along with meteorological variables measured by a Tethered Balloon Sounding System (XLS-Ⅱ) and Automatic Weather Station (AWS). The results will be compared with low-level clouds for similarities and differences between fogs and clouds.

Experimental Characterization and Hygroscopicity Determination of Secondary Aerosol from D5 Cyclic Siloxane Oxidation

NASA Astrophysics Data System (ADS)

Stanier, C. O.; Janechek, N. J.; Bryngelson, N.; Marek, R. F.; Lersch, T.; Bunker, K.; Casuccio, G.; Brune, W. H.; Hornbuckle, K. C.

2017-12-01

Cyclic volatile methyl siloxanes are anthropogenic chemicals present in personal care products such as antiperspirants and lotions. These are volatile chemicals that are readily released into the atmosphere by product use. Due to their emission and relatively slow kinetics of their major transformation pathway, reaction with hydroxyl radicals (OH), these compounds are present in high concentrations in indoor environments and widespread in outdoor environments. Cyclic siloxane reaction with OH can lead to secondary organic aerosols, and due to the widespread prevalence of the parent compounds, may be an important source of ambient aerosols. Atmospheric aerosols have important influences to the climate by affecting the radiative balance and by serving as cloud condensation nuclei (CCN) which influence clouds. While the parent compounds have been well-studied, the oxidation products have received much less attention, with almost no ambient measurements or experimental physical property data. We report physical properties of aerosols generated by reacting the cyclic siloxane D5 with OH using a Potential Aerosol Mass (PAM) photochemical chamber. The particles were characterized by SMPS, imaging and elemental analysis using both Transmission Electron Microscopy and Scanning Transmission Electron Microscopy equipped with Energy Dispersive X-ray Spectroscopy systems (TEM-EDS and STEM-EDS), volatility measurements using Volatility Tandem Differential Mobility Analyzer (V-TDMA), and hygroscopicity measurements to determine CCN potential using a Droplet Measurement Technologies Cloud Condensation Nuclei Counter (DMT-CCN). Aerosol yield sensitivity to D5 and OH concentrations, residence time, and seed aerosols were analyzed. TEM-EDS and STEM-EDS analysis show spherical particle morphology with elemental composition consistent with aerosols derived from cyclic siloxane sources. Measured aerosol yields were 20-50% with typical aerosol concentrations 300,000 particles cm-3, up to

How much does sea spray aerosol organic matter impact clouds and radiation? Sensitivity studies in the Community Atmosphere Model

NASA Astrophysics Data System (ADS)

Burrows, S. M.; Liu, X.; Elliott, S.; Easter, R. C.; Singh, B.; Rasch, P. J.

2015-12-01

Submicron marine aerosol particles are frequently observed to contain substantial fractions of organic material, hypothesized to enter the atmosphere as part of the primary sea spray aerosol formed through bubble bursting. This organic matter in sea spray aerosol may affect cloud condensation nuclei and ice nuclei concentrations in the atmosphere, particularly in remote marine regions. Members of our team have developed a new, mechanistic representation of the enrichment of sea spray aerosol with organic matter, the OCEANFILMS parameterization (Burrows et al., 2014). This new representation uses fields from an ocean biogeochemistry model to predict properties of the emitted aerosol. We have recently implemented the OCEANFILMS representation of sea spray aerosol composition into the Community Atmosphere Model (CAM), and performed sensitivity experiments and comparisons with alternate formulations. Early results from these sensitivity simulations will be shown, including impacts on aerosols, clouds, and radiation. References: Burrows, S. M., Ogunro, O., Frossard, A. A., Russell, L. M., Rasch, P. J., and Elliott, S. M.: A physically based framework for modeling the organic fractionation of sea spray aerosol from bubble film Langmuir equilibria, Atmos. Chem. Phys., 14, 13601-13629, doi:10.5194/acp-14-13601-2014, 2014.

Aerosol and monsoon climate interactions over Asia

NASA Astrophysics Data System (ADS)

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

2016-12-01

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

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

Herich, Hanna; Tritscher, Torsten; Wiacek, Aldona

2009-11-01

Airborne mineral dust particles serve as cloud condensation nuclei (CCN), thereby influencing the formation and properties of warm clouds. It is therefore of particular interest how dust aerosols with different mineralogy behave when exposed to high relative humidity (RH) or supersaturation with respect to liquid water similar to atmospheric conditions. In this study the sub-saturated hygroscopic growth and the supersaturated cloud condensation nucleus activity of pure clays and real desert dust aerosols was 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 wellmore » as three desert dust samples (Saharan dust (SD), Chinese dust (CD) and Arizona test dust (ATD)) were used. Aerosols were generated both with a wet and a dry disperser and the water uptake was parameterized via the hygroscopicity parameter, κ. The hygroscopicity of dry generated dust aerosols was found to be negligible when compared to processed atmospheric aerosols, with CCNC derived κ values between 0.00 and 0.02. The latter value can be idealized as a particle consisting of 96.7% (by volume) insoluble material and ~3.3% ammonium sulfate. Pure clay aerosols were found to be generally less hygroscopic than real desert dust particles. All illite and montmorillonite samples had κ~0.003, kaolinites were least hygroscopic and had κ=0.001. SD (κ=0.023) was found to be the most hygroscopic dry-generated desert dust followed by CD (κ=0.007) and ATD (κ=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 while immersed in an aqueous medium during atomization, thus indicating that specification of the generation method is critically important when presenting such data. Any atmospheric

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

Campaign datasets for Two-Column Aerosol Project (TCAP)

DOE Data Explorer

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

2013-12-30

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

Constraining the instantaneous aerosol influence on cloud albedo

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gryspeerdt, Edward; Quaas, Johannes; Ferrachat, Sylvaine

Much of the uncertainty in estimates of the anthropogenic forcing of climate change comes from uncertainties in the instantaneous effect of aerosols on cloud albedo, known as the Twomey effect or the radiative forcing from aerosol–cloud interactions (RFaci), a component of the total or effective radiative forcing. Because aerosols serving as cloud condensation nuclei can have a strong influence on the cloud droplet number concentration ( N d), previous studies have used the sensitivity of the N d to aerosol properties as a constraint on the strength of the RFaci. However, recent studies have suggested that relationships between aerosol andmore » cloud properties in the present-day climate may not be suitable for determining the sensitivity of the N d to anthropogenic aerosol perturbations. Using an ensemble of global aerosol–climate models, this study demonstrates how joint histograms between N d and aerosol properties can account for many of the issues raised by previous studies. It shows that if the anthropogenic contribution to the aerosol is known, the RFaci can be diagnosed to within 20% of its actual value. Furthermore, the accuracy of different aerosol proxies for diagnosing the RFaci is investigated, confirming that using the aerosol optical depth significantly underestimates the strength of the aerosol–cloud interactions in satellite data.« less

Constraining the instantaneous aerosol influence on cloud albedo

DOE PAGES

Gryspeerdt, Edward; Quaas, Johannes; Ferrachat, Sylvaine; ...

2017-04-26

Much of the uncertainty in estimates of the anthropogenic forcing of climate change comes from uncertainties in the instantaneous effect of aerosols on cloud albedo, known as the Twomey effect or the radiative forcing from aerosol–cloud interactions (RFaci), a component of the total or effective radiative forcing. Because aerosols serving as cloud condensation nuclei can have a strong influence on the cloud droplet number concentration ( N d), previous studies have used the sensitivity of the N d to aerosol properties as a constraint on the strength of the RFaci. However, recent studies have suggested that relationships between aerosol andmore » cloud properties in the present-day climate may not be suitable for determining the sensitivity of the N d to anthropogenic aerosol perturbations. Using an ensemble of global aerosol–climate models, this study demonstrates how joint histograms between N d and aerosol properties can account for many of the issues raised by previous studies. It shows that if the anthropogenic contribution to the aerosol is known, the RFaci can be diagnosed to within 20% of its actual value. Furthermore, the accuracy of different aerosol proxies for diagnosing the RFaci is investigated, confirming that using the aerosol optical depth significantly underestimates the strength of the aerosol–cloud interactions in satellite data.« less

Constraining the instantaneous aerosol influence on cloud albedo

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gryspeerdt, Edward; Quaas, Johannes; Ferrachat, Sylvaine

2017-04-26

Much of the uncertainty in estimates of the anthropogenic forcing of climate change comes from uncertainties in the instantaneous effect of aerosols on cloud albedo, known as the Twomey effect or the radiative forcing from aerosol–cloud interactions (RFaci), a component of the total or effective radiative forcing. Because aerosols serving as cloud condensation nuclei can have a strong influence on the cloud droplet number concentration (Nd), previous studies have used the sensitivity of the Nd to aerosol properties as a constraint on the strength of the RFaci. However, recent studies have suggested that relationships between aerosol and cloud properties inmore » the present-day climate may not be suitable for determining the sensitivity of the Nd to anthropogenic aerosol perturbations. Using an ensemble of global aerosol–climate models, this study demonstrates how joint histograms between Nd and aerosol properties can account for many of the issues raised by previous studies. It shows that if the anthropogenic contribution to the aerosol is known, the RFaci can be diagnosed to within 20% of its actual value. The accuracy of different aerosol proxies for diagnosing the RFaci is investigated, confirming that using the aerosol optical depth significantly underestimates the strength of the aerosol–cloud interactions in satellite data.« less

Assessing the Dynamics of Organic Aerosols over the North Atlantic Ocean

PubMed Central

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

2017-01-01

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

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

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

Semi-continuous measurement and characteristics of water-soluble organic carbon and ions of PM2.5 aerosol with PILS-TOC-IC in Baengnyeong Island

NASA Astrophysics Data System (ADS)

Kang, S.; Kim, K.; Park, G.; Ban, J.; Park, D.; Bae, M. S.; Shin, H. J.; Lee, M.; Seo, Y.; Choi, J.; Jung, D.; Seo, S.; Lee, T.; Kim, D. S.

2016-12-01

Aerosols have an important effect from scattering and absorbing the solar energy and indirectly by acting as cloud condensation nuclei and also some of the effects of aerosols are reduction in visibility, deterioration of human health, and deposition of pollutants to ecosystems. In various experimental results were showed that organic compounds have an important fraction from 10 to 70% of the total aerosol mass. Organic carbon contains water-soluble organic carbon (WSOC) and water insoluble organic carbon. WSOC are involved in the most unknown liquid-phase chemistry of wet aerosol and clouds. It is also worked as cloud condensation nuclei (CCN). Formation of secondary organic aerosol by chemical reaction of hydrocarbon compounds is a source of main pollution of WSOC compounds. Study of pollution source of WSOC is important method for creation process of secondary organic aerosol that completely has not studied.Analysis of WSOC is important and need to real-time measurement system for definition of chemical cause and sources. In this study, Particle-into-liquid sampler (PILS) coupled with total organic carbon (TOC) analyser and ion chromatography (PILS-TOC-IC), was used for semi-continuous measurement of WSOC and ionic compounds of PM2.5 during April-June 2016 at Baengnyeong Island Atmospheric Research Center, operated by the Korea National Institute of Environmental Research (NIER). PILS-TOC-IC can provide chemical information about real-time changes from ions composition and concentrations of WSOC and ionic compounds.

An Aerosol Condensation Model for Sulfur Trioxide

DOE Office of Scientific and Technical Information (OSTI.GOV)

Grant, K E

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,more » 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

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.

Traffic is a major source of atmospheric nanocluster aerosol

PubMed Central

Kuuluvainen, Heino; Karjalainen, Panu; Keskinen, Jorma; Hillamo, Risto; Niemi, Jarkko V.; Pirjola, Liisa; Timonen, Hilkka J.; Saarikoski, Sanna; Saukko, Erkka; Järvinen, Anssi; Silvennoinen, Henna; Rostedt, Antti; Olin, Miska; Yli-Ojanperä, Jaakko; Nousiainen, Pekka; Kousa, Anu; Dal Maso, Miikka

2017-01-01

In densely populated areas, traffic is a significant source of atmospheric aerosol particles. Owing to their small size and complicated chemical and physical characteristics, atmospheric particles resulting from traffic emissions pose a significant risk to human health and also contribute to anthropogenic forcing of climate. Previous research has established that vehicles directly emit primary aerosol particles and also contribute to secondary aerosol particle formation by emitting aerosol precursors. Here, we extend the urban atmospheric aerosol characterization to cover nanocluster aerosol (NCA) particles and show that a major fraction of particles emitted by road transportation are in a previously unmeasured size range of 1.3–3.0 nm. For instance, in a semiurban roadside environment, the NCA represented 20–54% of the total particle concentration in ambient air. The observed NCA concentrations varied significantly depending on the traffic rate and wind direction. The emission factors of NCA for traffic were 2.4·1015 (kgfuel)−1 in a roadside environment, 2.6·1015 (kgfuel)−1 in a street canyon, and 2.9·1015 (kgfuel)−1 in an on-road study throughout Europe. Interestingly, these emissions were not associated with all vehicles. In engine laboratory experiments, the emission factor of exhaust NCA varied from a relatively low value of 1.6·1012 (kgfuel)−1 to a high value of 4.3·1015 (kgfuel)−1. These NCA emissions directly affect particle concentrations and human exposure to nanosized aerosol in urban areas, and potentially may act as nanosized condensation nuclei for the condensation of atmospheric low-volatile organic compounds. PMID:28674021

Traffic is a major source of atmospheric nanocluster aerosol.

PubMed

Rönkkö, Topi; Kuuluvainen, Heino; Karjalainen, Panu; Keskinen, Jorma; Hillamo, Risto; Niemi, Jarkko V; Pirjola, Liisa; Timonen, Hilkka J; Saarikoski, Sanna; Saukko, Erkka; Järvinen, Anssi; Silvennoinen, Henna; Rostedt, Antti; Olin, Miska; Yli-Ojanperä, Jaakko; Nousiainen, Pekka; Kousa, Anu; Dal Maso, Miikka

2017-07-18

In densely populated areas, traffic is a significant source of atmospheric aerosol particles. Owing to their small size and complicated chemical and physical characteristics, atmospheric particles resulting from traffic emissions pose a significant risk to human health and also contribute to anthropogenic forcing of climate. Previous research has established that vehicles directly emit primary aerosol particles and also contribute to secondary aerosol particle formation by emitting aerosol precursors. Here, we extend the urban atmospheric aerosol characterization to cover nanocluster aerosol (NCA) particles and show that a major fraction of particles emitted by road transportation are in a previously unmeasured size range of 1.3-3.0 nm. For instance, in a semiurban roadside environment, the NCA represented 20-54% of the total particle concentration in ambient air. The observed NCA concentrations varied significantly depending on the traffic rate and wind direction. The emission factors of NCA for traffic were 2.4·10 15 (kg fuel ) -1 in a roadside environment, 2.6·10 15 (kg fuel ) -1 in a street canyon, and 2.9·10 15 (kg fuel ) -1 in an on-road study throughout Europe. Interestingly, these emissions were not associated with all vehicles. In engine laboratory experiments, the emission factor of exhaust NCA varied from a relatively low value of 1.6·10 12 (kg fuel ) -1 to a high value of 4.3·10 15 (kg fuel ) -1 These NCA emissions directly affect particle concentrations and human exposure to nanosized aerosol in urban areas, and potentially may act as nanosized condensation nuclei for the condensation of atmospheric low-volatile organic compounds.

Aerosols and Aerosol-related haze forecasting in China Meteorological Adminstration

NASA Astrophysics Data System (ADS)

Zhou, Chunhong; Zhang, Xiaoye; Gong, Sunling; Liu, Hongli; Xue, Min

2017-04-01

CMA Unified Atmospheric Chemistry Environmental Forecasting System (CUACE) is a unified numerical chemical weather forecasting system with BC, OC, Sulfate, Nitrate, Ammonia, Dust and Sea-Salt aerosols and their sources, gas to particle processes, SOA, microphysics and transformation. With an open interface, CUACE has been online coupled to mesoscale model MM5 and the new NWP system GRAPES (Global/Regional Assimilation and Prediction Enhanced System)min CMA. With Chinese Emissions from Cao and Zhang(2012 and 2013), a forecasting system called CUACE/Haze-fog has been running in real time in CMA and issue 5-days PM10, O3 and Visibility forecasts. A comprehensive ACI scheme has also been developed in CUACE Calculated by a sectional aerosol activation scheme based on the information of size and mass from CUACE and the thermal-dynamic and humid states from the weather model at each time step, the cloud condensation nuclei (CCN) is fed online interactively into a two-moment cloud scheme (WDM6) and a convective parameterization to drive the cloud physics and precipitation formation processes. The results show that interactive aerosols with the WDM6 in CUACE obviously improve the clouds properties and the precipitation, showing 24% to 48% enhancements of TS scoring for 6-h precipitation .

Implementation of aerosol-cloud interactions in the regional atmosphere-aerosol model COSMO-MUSCAT(5.0) and evaluation using satellite data

NASA Astrophysics Data System (ADS)

Dipu, Sudhakar; Quaas, Johannes; Wolke, Ralf; Stoll, Jens; Mühlbauer, Andreas; Sourdeval, Odran; Salzmann, Marc; Heinold, Bernd; Tegen, Ina

2017-06-01

The regional atmospheric model Consortium for Small-scale Modeling (COSMO) coupled to the Multi-Scale Chemistry Aerosol Transport model (MUSCAT) is extended in this work to represent aerosol-cloud interactions. Previously, only one-way interactions (scavenging of aerosol and in-cloud chemistry) and aerosol-radiation interactions were included in this model. The new version allows for a microphysical aerosol effect on clouds. For this, we use the optional two-moment cloud microphysical scheme in COSMO and the online-computed aerosol information for cloud condensation nuclei concentrations (Cccn), replacing the constant Cccn profile. In the radiation scheme, we have implemented a droplet-size-dependent cloud optical depth, allowing now for aerosol-cloud-radiation interactions. To evaluate the models with satellite data, the Cloud Feedback Model Intercomparison Project Observation Simulator Package (COSP) has been implemented. A case study has been carried out to understand the effects of the modifications, where the modified modeling system is applied over the European domain with a horizontal resolution of 0.25° × 0.25°. To reduce the complexity in aerosol-cloud interactions, only warm-phase clouds are considered. We found that the online-coupled aerosol introduces significant changes for some cloud microphysical properties. The cloud effective radius shows an increase of 9.5 %, and the cloud droplet number concentration is reduced by 21.5 %.

A study of aerosol indirect effects and feedbacks on convective precipitation

NASA Astrophysics Data System (ADS)

Da Silva, Nicolas; Mailler, Sylvain; Drobinski, Philippe

2017-04-01

Atmospheric aerosols from natural and anthropogenic origin are present in the troposphere of the Mediterranean basin and continental Europe, occasionnally reaching very high concentrations in air masses with a strong content of aerosols related to mineral dust emissions, wildfires, or anthropogenic contamination [1]. On the other hand precipitations in the Mediterranean basin need to be understood precisely since drought and extreme precipitation events are a part of Mediterranean climate which can strongly affect the people and the economic activity in the Mediterranean basin [2]. The present study is a contribution to the investigations on the effects of aerosols on precipitation in the Mediterranean basin and continental Europe. For that purpose, we used the Weather Research and Forecasting Model (WRF) parameterized with the Thompson aerosol-aware microphysics schemes, performing two sensitivity simulations forced with two different aerosol climatologies during six months covering an entire summer season on a domain, covering the Mediterranean basin and continental Europe at 50 km resolution. Aerosols may affect atmospheric dynamics through their direct and semidirect radiative effects as well as through their indirect effects (through the changes of cloud microphysics). While it is difficult to disentangle these differents effects in reality, numerical modelling with the WRF model make it possible to isolate indirect effects by modifying them without affecting the direct or semidirect effects of aerosols in an attempt to examine the effect of aerosols on precipitations through microphysical effects only. Our first results have shown two opposite responses depending whether the precipitation are convective or large-scale. Since convective precipitations seem to be clearly inhibited by increased concentrations of cloud-condensation nuclei, we attempted to understand which processes and feedbacks are involved in this reduction of parameterized convective

Analysis and interpretation of lidar observations of the stratospheric aerosol

NASA Technical Reports Server (NTRS)

Hamill, P.; Swissler, T. J.; Osborn, M.; Mccormick, M. P.

1980-01-01

Data obtained with a 48 in. telescope lidar system are compared with results obtained using a one-dimensional stratospheric aerosol model to analyze various microphysical processes influencing the formation of this aerosol. Special attention is given to the following problems: (1) how lidar data can help determine the composition of the aerosol particles and (2) how the layer corresponds to temperature profile variations. The lidar record during the period 1974 to 1979 shows a considerable decrease of the peak value of the backscatter ratio. Seasonal variations in the aerosol layer and a gradual decrease in stratospheric loading are observed. The aerosol model simulates a background stratospheric aerosol layer, and it predicts stratospheric aerosol concentrations and compositions. Numerical experiments are carried out by using the model and by comparing the theoretical results with the experimentally obtained lidar record. Comparisons show that the backscatter profile is consistent with the composition when the particles are sulfuric acid and water; it is not consistent with an ammonium sulfate composition. It is shown that the backscatter ratio is not sensitive to the composition or stratospheric loading of condensation nuclei such as meteoritic debris.

Combustion Aerosol over Marine Stratus: Long Range Transport, Subsidence and Aerosol-Cloud Interactions over the South East Pacific

NASA Astrophysics Data System (ADS)

Clarke, A. D.; Snider, J.; Freitag, S.; Feingold, G.; Campos, T. L.; Breckhovskikh, V.; Kazil, J.

2011-12-01

The worlds largest stratus deck over the South East Pacific (SEP) was a study target for the VOCALS (http://www.eol.ucar.edu/projects/vocals/) experiment in October 2008. Aerosol-cloud interactions were one major goal of several ship and aircraft studies including results from 14 flights of the NCAR C-130 aircraft reported here. Each flight covered about a 1000 km range with multiple profiles and legs below, in and above the Sc deck. Strong aerosol sources along the coast of Chile were expected and found to influence cloud condensation nuclei (CCN) in coastal clouds. However; "rivers" of elevated CO, black carbon (BC) associated with combustion aerosol effective as CCN at <0.3%S were also common in subsiding FT air overlying the extensive Sc deck for over 1000km offshore. This subsidence, linked to the Hadley circulation, brought in aerosol from sources over the western Pacific as well as South America. Observed entrainment of this aerosol appeared linked to cloud related turbulence. When present, this combustion aerosol increased available CCN and decreased effective radius compared to clouds in "clean" MBL air advected from the South Pacific. We hypothesize that this entrainment can help buffer MBL clouds over the SEP against depletion of CCN by drizzle. This may delay transition of closed cell to open cell convection, potentially leading to increased lifetimes of Sc clouds that entrain such aerosol.

Cloud droplet activation through oxidation of organic aerosol influenced by temperature and particle phase state: CLOUD ACTIVATION BY AGED ORGANIC AEROSOL

DOE PAGES

Slade, Jonathan H.; Shiraiwa, Manabu; Arangio, Andrea; ...

2017-02-04

Chemical aging of organic aerosol (OA) through multiphase oxidation reactions can alter their cloud condensation nuclei (CCN) activity and hygroscopicity. However, the oxidation kinetics and OA reactivity depend strongly on the particle phase state, potentially influencing the hydrophobic-to-hydrophilic conversion rate of carbonaceous aerosol. Here, amorphous Suwannee River fulvic acid (SRFA) aerosol particles, a surrogate humic-like substance (HULIS) that contributes substantially to global OA mass, are oxidized by OH radicals at different temperatures and phase states. When oxidized at low temperature in a glassy solid state, the hygroscopicity of SRFA particles increased by almost a factor of two, whereas oxidation ofmore » liquid-like SRFA particles at higher temperatures did not affect CCN activity. Low-temperature oxidation appears to promote the formation of highly-oxygenated particle-bound fragmentation products with lower molar mass and greater CCN activity, underscoring the importance of chemical aging in the free troposphere and its influence on the CCN activity of OA.« less

Development of a global aerosol model using a two-dimensional sectional method: 1. Model design

NASA Astrophysics Data System (ADS)

Matsui, H.

2017-08-01

This study develops an aerosol module, the Aerosol Two-dimensional bin module for foRmation and Aging Simulation version 2 (ATRAS2), and implements the module into a global climate model, Community Atmosphere Model. The ATRAS2 module uses a two-dimensional (2-D) sectional representation with 12 size bins for particles from 1 nm to 10 μm in dry diameter and 8 black carbon (BC) mixing state bins. The module can explicitly calculate the enhancement of absorption and cloud condensation nuclei activity of BC-containing particles by aging processes. The ATRAS2 module is an extension of a 2-D sectional aerosol module ATRAS used in our previous studies within a framework of a regional three-dimensional model. Compared with ATRAS, the computational cost of the aerosol module is reduced by more than a factor of 10 by simplifying the treatment of aerosol processes and 2-D sectional representation, while maintaining good accuracy of aerosol parameters in the simulations. Aerosol processes are simplified for condensation of sulfate, ammonium, and nitrate, organic aerosol formation, coagulation, and new particle formation processes, and box model simulations show that these simplifications do not substantially change the predicted aerosol number and mass concentrations and their mixing states. The 2-D sectional representation is simplified (the number of advected species is reduced) primarily by the treatment of chemical compositions using two interactive bin representations. The simplifications do not change the accuracy of global aerosol simulations. In part 2, comparisons with measurements and the results focused on aerosol processes such as BC aging processes are shown.

Aerosol Chemical Composition and its Effects on Cloud-Aerosol Interactions during the 2007 CHAPS Experiment

NASA Astrophysics Data System (ADS)

Lee, Y.; Alexander, L.; Newburn, M.; Jayne, J.; Hubbe, J.; Springston, S.; Senum, G.; Andrews, B.; Ogren, J.; Kleinman, L.; Daum, P.; Berg, L.; Berkowitz, C.

2007-12-01

Chemical composition of submicron aerosol particles was determined using an Aerodyne Time-of-Flight Aerosol Mass Spectrometer (AMS) outfitted on the DOE G-1 aircraft during the Cumulus Humilis Aerosol Processing Study (CHAPS) conducted in Oklahoma City area in June 2007. The primary objective of CHAPS was to investigate the effects of urban emissions on cloud aerosol interactions as a function of processing of the emissions. Aerosol composition was typically determined at three different altitudes: below, in, and above cloud, in both upwind and downwind regions of the urban area. Aerosols were sampled from an isokinetic inlet with an upper size cut-off of ~1.5 micrometer. During cloud passages, the AMS also sampled particles that were dried from cloud droplets collected using a counter-flow virtual impactor (CVI) sampler. The aerosol mass concentrations were typically below 10 microgram per cubic meter, and were dominated by organics and sulfate. Ammonium was often less than required for complete neutralization of sulfate. Aerosol nitrate levels were very low. We noted that nitrate levels were significantly enhanced in cloud droplets compared to aerosols, most likely resulting from dissolution of gaseous nitric acid. Organic to sulfate ratios appeared to be lower in cloud droplets than in aerosols, suggesting cloud condensation nuclei properties of aerosol particles might be affected by loading and nature of the organic components in aerosols. In-cloud formation of sulfate was considered unimportant because of the very low SO2 concentration in the region. A detailed examination of the sources of the aerosol organic components (based on hydrocarbons determined using a proton transfer reaction mass spectrometer) and their effects on cloud formation as a function of atmospheric processing (based on the degree of oxidation of the organic components) will be presented.

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

PubMed

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

2008-05-15

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

Lidar characterizations of atmospheric aerosols and clouds

NASA Astrophysics Data System (ADS)

Ferrare, R. A.; Hostetler, C. A.; Hair, J. W.; Burton, S. P.

2017-12-01

Knowledge of the vertical profile, composition, concentration, and size distribution of aerosols is required to quantify the impacts of aerosols on human health, global and regional climate, clouds and precipitation. In particular, radiative forcing due to anthropogenic aerosols is the most uncertain part of anthropogenic radiative forcing, with aerosol-cloud interactions (ACI) as the largest source of uncertainty in current estimates of global radiative forcing. Improving aerosol transport model predictions of the vertical profile of aerosol optical and microphysical characteristics is crucial for improving assessments of aerosol radiative forcing. Understanding how aerosols and clouds interact is essential for investigating the aerosol indirect effect and ACI. Through its ability to provide vertical profiles of aerosol and cloud distributions as well as important information regarding the optical and physical properties of aerosols and clouds, lidar is a crucial tool for addressing these science questions. This presentation describes how surface, airborne, and satellite lidar measurements have been used to address these questions, and in particular how High Spectral Resolution Lidar (HSRL) measurements provide profiles of aerosol properties (backscatter, extinction, depolarization, concentration, size) important for characterizing radiative forcing. By providing a direct measurement of aerosol extinction, HSRL provides more accurate aerosol measurement profiles and more accurate constraints for models than standard retrievals from elastic backscatter lidar, which loses accuracy and precision at lower altitudes due to attenuation from overlying layers. Information regarding particle size and abundance from advanced lidar retrievals provides better proxies for cloud-condensation-nuclei (CCN), which are required for assessing aerosol-cloud interactions. When combined with data from other sensors, advanced lidar measurements can provide information on aerosol and

Study of the chemical composition of atmospheric aerosol particles in Hungary: a review

NASA Astrophysics Data System (ADS)

Mészáros, E.

The methods used in Hungarian laboratories to study the chemical composition of atmospheric aerosol particles over the last 30 years are reviewed. Individual particles were identified by topochemical techniques and morphological identification with an electron microscope. Bulk analyses were also carried out by applying wet chemical methods, and more recently by the PIXE procedure. The results gained are summarized in connection with the general development of atmospheric aerosol science during the last decades. These studies demonstrated that cloud condensation nuclei are water soluble Aitken sized particles which are composed of sulfates. Neutralized and acidic sulfate particles constitute the main class of fine aerosol particles under continental and oceanic background conditions. Coarse particles contain mostly sodium, silicon and aluminium. The formation and origin of particles in different size ranges are also discussed.

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

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

PubMed Central

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

2008-01-01

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 ≈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. PMID:18645179

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

NASA Astrophysics Data System (ADS)

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

2014-12-01

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

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.

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

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

NASA Astrophysics Data System (ADS)

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

2015-08-01

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

The time dependent growth of H2O-H2SO4 aerosols by heteromolecular condensation

NASA Technical Reports Server (NTRS)

Hamill, P.

1975-01-01

A theory for the time-dependent growth of solution droplets by heteromolecular condensation is presented. The theory is applied to the growth of H2O-H2SO4 aerosols for relative humidities less than 100 per cent. Growth curves (droplet radius as a function of time) for different values of relative humidity are evaluated.

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.

Contribution of bioaerosols to the global organic aerosol budget

NASA Astrophysics Data System (ADS)

Janssen, R.; Heald, C. L.

2017-12-01

Bioaerosols are ubiquitous in the atmosphere and may contribute significantly to cloud condensation and ice nuclei populations, and consequently to formation of clouds and precipitation. However, quantifying the contribution of bioaerosols to the global organic aerosol budget is a challenge, since bioaerosol sources are poorly constrained on the global scale. Previous global estimates of global primary biological aerosol particle (PBAP) emissions, including bacteria, fungal spores and pollen, range from 78-296 Tg/year. Over the past several years, size-resolved measurements of fluorescent biological aerosol particles have been made in tropical, temperate and boreal ecosystems. Besides, single particle mass spectroscopy has been used to quantify bioaerosol concentrations at various locations in the US. We use these observations to develop and evaluate a bioaerosol emission scheme that describes both the biological production of bioaerosols and the meteorological drivers of the emission of these particles into the atmosphere. Then, we implement this scheme in the GEOS-Chem global chemical transport model to estimate the emission, burden and lifetime of bioaerosols. Finally, we evaluate the contribution of bioaerosols to the total organic aerosol budget, which further consists of primary and secondary organic aerosol.

Simulating the effect of photochemical aging on the oxidation state and hygroscopicity of organic aerosol

NASA Astrophysics Data System (ADS)

Tsimpidi, A.; Karydis, V.; Pandis, S. N.; Lelieveld, J.

2016-12-01

Hygroscopicity is an important property of aerosols which describes their propensity to absorb water vapor. The hygroscopicity of organic aerosol (OA) can change during its atmospheric aging affecting the total aerosol hygroscopicity. A more hygroscopic particle will grow more rapidly under humid conditions, scatter incident sunlight more efficiently; and it will more likely form cloud droplets. Both phenomena strongly influence the radiative forcing of climate through the direct and indirect effects of aerosols. Therefore, taking into account the hygrscopicity changes of OA during its atmospheric aging is of prime importance to accurately estimate the aerosol climatic impact. Here, we use a computationally efficient module for the description of OA composition and evolution in the atmosphere (ORACLE) (Tsimpidi et al., 2014) in the frame of the global chemistry climate model EMAC to simulate the global distribution of the OA oxidation state and hygroscopicity. To track the evolution of the OA oxidation state during its atmospheric aging, ORACLE is modified to include the description of the OA oxygen content change when mass from any OA surrogate species reacts with the OH radical. Subsequently, it is assumed that the cloud condensation nuclei (CCN) activity of OA, expressed in the form of the hygroscopicity parameter κ, will increase with increasing oxygen content (expressed by the oxygen per carbon ratio, O:C) and will range from κ = 0 (for O:C ≤ 0.2) to κ = 0.35 (for O:C = 1). The exact relationship between O:C and κ is determined based on aerosol mass spectrometer (AMS) and continuous flow CCN (CCNC) measurements of SOA (Lambe et al., 2011). Following a straightforward mixing rule, the hygroscopicity and oxygen content of total OA is calculated based on the hygroscopicities of the individual OA compounds and their degree of oxidation. A global dataset of O:C measurements is used to validate the model results. ReferencesLambe, A. T., et al. : Laboratory

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.

Evolution of the stratospheric aerosol in the northern hemisphere following the June 1991 volcanic eruption of Mount Pinatubo: Role of tropospheric-stratospheric exchange and transport

NASA Astrophysics Data System (ADS)

Jónsson, Hafliòi H.; Wilson, James C.; Brock, Charles A.; Dye, J. E.; Ferry, G. V.; Chan, K. R.

1996-01-01

Since the eruption of Mount Pinatubo in June, 1991, measurements of particle size and concentration have intermittently been carried out from an ER-2 aircraft at altitudes of up to 21 km at midlatitudes and high latitudes in the northern hemisphere. They show the evolution and purge of the volcanic aerosol to be due to an interaction of aerosol mechanics with tropospheric-stratospheric exchange processes, transport, and mixing. During the first 5 months after the eruption the volcanic plume spread to higher latitudes in laminae and filaments, producing steep spatial gradients in the properties of the stratospheric aerosol. At the same time the concentration of newly formed particles in the plume rapidly decreased toward background values as a result of coagulation while particle size and aerosol surface area continued to increase. By December 1991, the particle number mixing ratios and aerosol surface area mixing ratios had become spatially uniform over a wide range of latitudes above 18 km. The surface area mixing ratios peaked in this region of the stratosphere at ˜35 times their background values in the winter of 1992. The corresponding condensed mass mixing ratio enhancement was by a factor of ˜200. After the winter of 1992, a gradual removal of the volcanic mass began and initially was dominated by sedimentation above 18 km. The aerosol surface area mixing ratio thus decreased by an order of magnitude over 2.5 years, and the aerosol volume, or condensed mass, mixing ratio decayed by an order of magnitude over approximately 1.7 years. Below 18 km, the purging of the Pinatubo aerosol at mid-latitudes appeared sporadic and disorderly and was strongly influenced by episodal rapid quasi-isentropic transport and dilution by tropical air of tropospheric origin having high condensation nuclei mixing ratios but low mixing ratios of aerosol surface area or condensed mass compared to the volcanic aerosol.

Atmo-metabolomics: a new measurement approach for investigating aerosol composition and ecosystem functioning.

NASA Astrophysics Data System (ADS)

Rivas-Ubach, A.; Liu, Y.; Sardans, J.; Tfaily, M. M.; Kim, Y. M.; Bourrianne, E.; Paša-Tolić, L.; Penuelas, J.; Guenther, A. B.

2016-12-01

Aerosols play crucial roles in the processes controlling the composition of the atmosphere and the functioning of ecosystems. Gaining a deeper understanding of the chemical composition of aerosols is one of the major challenges for atmospheric and climate scientists and is beginning to be recognized as important for ecological research. Better comprehension of aerosol chemistry can potentially provide valuable information on atmospheric processes such as oxidation of organics and the production of cloud condensation nuclei as well as provide an approximation of the general status of an ecosystem through the measurement of certain stress biomarkers. In this study, we describe an efficient aerosol sampling method, the metabolite extraction and the analytical procedures for the chemical characterization of aerosols, namely, the atmo-metabolome. We used mass spectrometry (MS) coupled to liquid chromatography (LC-MS), gas chromatography (GC-MS) and Fourier transform ion cyclotron resonance (FT-ICR-MS) to characterize the atmo-metabolome of two marked seasons; spring and summer. Our sampling and extraction methods demonstrated to be suitable for aerosol chemical characterization with any of the analytical platforms used in this study. The atmo-metabolome between spring and summer showed overall statistically differences. We identified several metabolites that can be attributed to pollen and other plant-related aerosols. Spring aerosols exhibit higher concentrations of metabolites linked to higher plant activity while summer samples had higher concentrations of metabolites that may reflect certain oxidative stresses in primary producers. Moreover, the elemental composition of aerosols showed clear different between seasons. Summer aerosols were generally higher in molecular weight and with higher O/C ratios, indicating higher oxidation levels and condensation of compounds relative to spring. Our method represents an advanced approach for characterizing the composition of

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

Aerosol and CCN in southwest Saudi Arabia

NASA Astrophysics Data System (ADS)

Collins, Don; Li, Runjun; Axisa, Duncan; Kucera, Paul; Burger, Roelof

2010-05-01

As part of an ongoing study of the microphysical and dynamical controls on precipitation in southwest Saudi Arabia, a number of surface and aircraft-based instruments were used in summer / fall 2009 to measure the size distribution, hygroscopic properties, and cloud droplet nucleation efficiency of the local aerosol. Submicron size distributions were measured using differential mobility analyzers both on the ground and on board the aircraft, while an aerodynamic particle sizer and a forward scattering spectrometer probe were used to measure the supermicron size distributions on the ground and from on board the aircraft, respectively. Identical continuous flow cloud condensation nuclei counters were used to measure CCN spectra at the surface and aloft and a humidified tandem differential mobility analyzer was operated on the ground to measure size-resolved hygroscopicity. The aerosol in this arid environment is characterized by a persistent accumulation mode having hygroscopic and CCN efficiency properties consistent with a sulfate-rich aged aerosol. The particles in that background aerosol are generally sufficiently large and hygroscopic to activate at those supersaturations expected in the convective clouds responsible for most of the regional precipitation, which consequently acts as a lower bound on the resulting cloud droplet concentrations. Though the concentration, size distribution, and properties of the submicron aerosol generally changed very slowly over periods of several hours, abrupt ~doubling in concentration almost always accompanied the arrival of the sea breeze front that began along the Red Sea. Interestingly, the hygroscopicity and the shape of the size distribution differed little in the pre- and post-sea breeze air masses. The dust-dominated coarse mode typically contributed significantly more to the aerosol mass concentration than did the submicron mode and likely controlled the ice nuclei concentration, though no direct measurements were made

Radiative forcing of the desert aerosol at Ouarzazate (Morocco)

NASA Astrophysics Data System (ADS)

Tahiri, Abdelouahid; Diouri, Mohamed

2018-05-01

The atmospheric aerosol contributes to the definition of the climate with direct effect, the diffusion and absorption of solar and terrestrial radiations, and indirect, the cloud formation process where aerosols behave as condensation nuclei and alter the optical properties. Satellites and ground-based networks (solar photometers) allow the terrestrial aerosol observation and the determination of impact. Desert aerosol considered among the main types of tropospheric aerosols whose optical property uncertainties are still quite important. The analysis concerns the optical parameters recorded in 2015 at Ouarzazate solar photometric station (AERONET/PHOTONS network, http://aeronet.gsfc.nasa.gov/) close to Saharan zone. The daily average aerosol optical depthτaer at 0.5μm, are relatively high in summer and less degree in spring (from 0.01 to 1.82). Daily average of the Angstrom coefficients α vary between 0.01 and 1.55. The daily average of aerosol radiative forcing at the surface range between -150W/m2 and -10 W/m2 with peaks recorded in summer, characterized locally by large loads of desert aerosol in agreement with the advections of the Southeast of Morocco. Those recorded at the Top of the atmosphere show a variation from -74 W/m2 to +24 W/m2

Ice nuclei measurements at a high altitude remote station in the Northern Apennines

NASA Astrophysics Data System (ADS)

Schrod, Jann; Bingemer, Heinz; Haunold, Werner; Curtius, Joachim; Decesari, Stefano; Marinoni, Angela; Rinaldi, Matteo; Bonasoni, Paolo; Cristofanelli, Paolo

2013-04-01

During a field campaign of the PEGASOS (Pan-European Gas-AeroSOls-climate interactions Study, http://pegasos.iceht.forth.gr/) project in June 2012 we have made daily ice nucleus measurements on top of the Monte Cimone (44.18° N, 10.70° E, 2165 m asl) in the Northern Apennines at the "O. Vittori" Climate Observatory. Samples were taken at this GAW-WMO Global Station in a six hour rhythm (4 a.m., 10 a.m., 4 p.m. and 10 p.m.) and at increased frequency during specific events (e.g. dust transport episodes). Ice nuclei were measured by an offline technique. Aerosol particles of 40 liters of air were collected by electrostatic precipitation on a silicon substrate. Subsequently the ice nuclei were analyzed in the vacuum diffusion chamber FRIDGE [Klein et al. 2010] (FRankfurt Ice Nuclei Deposition FreezinG Experiment) by exposing the particles to supersaturation with respect to ice (106 % to 119 %) at -8 ° C, -13 ° C and -18 ° C. In our setup ice nuclei are activated in deposition and condensation freezing modes. A camera detects and counts ice crystals grown on ice nuclei. Every ice crystal counted is assumed to represent at least one ice nucleus. The mean IN concentration at Mt. Cimone was 60 IN per liter (at -18 ° C and 119% relative humility over ice), significantly higher than a longstanding mean at Mt. Kleiner Feldberg (30 IN/l), Germany for June. A mean active site density (IN per surface area of large aerosol particles) of 2.3 * 109 m-2 was calculated. The origin of the air masses sampled was established based on backward trajectories. With more than 100 IN/l on average (at -18° C and 119% relative humility over ice) the samples originating from North Africa were highest, and activated fractions were 4 to 20 times higher than for other transport sectors. An intensive event of dust transport was recorded by several instruments in the middle of June. At its peak in the morning of the 21st of June large aerosol surface and mass concentrations were observed by

Investigation of Atmospheric Aerosol properties by Atomic Force Microscopy

NASA Astrophysics Data System (ADS)

Sevalia, Barry; Joseph, Kelli; Gasseller, Morewell

The effects of aerosols on the atmosphere, climate, and public health are among the central topics in current environmental research. Aerosol particles scatter and absorb solar and terrestrial radiation, they are involved in the formation of clouds and precipitation as cloud condensation and ice nuclei, and they affect the abundance and distribution of atmospheric trace gases by chemical reactions and other multiphase processes. Moreover, airborne particles play an important role in the spreading of biological organisms, reproductive materials, and pathogens and they can cause or enhance respiratory, cardiovascular, infectious, and allergic diseases. In this study we use two distinct methods to characterize atmospheric aerosol particles. With the AFM, we use analytical and interpretative techniques to deduce fundamental physical properties of the aerosol particles such as particle sizes and morphology. The microscopy techniques are then compared and complemented with optical techniques that employ hand held sun photometers to measure aerosol optical thickness (AOT) of the atmosphere. The chemical nature of the aerosols is investigated by exposing the samples to a stream of ozone gas and then reimage them. Using this approach, we are only able to classify particles as organic, gr Maryam Foroozesh, Ph.D. Chair, Division of Mathematical and Physical Sciences Head, Department of Chemistry.

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

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

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

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

Multiphase OH and O 3 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 O 3 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 particlesmore » exposed to OH and O 3 is evaluated by determining the hygroscopicity parameter, κ, as a function of particle type, mixing state, and OH and O 3 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 O 3 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 of single and multicomponent biomass burning aerosol surrogate particles by OH: implications for cloud condensation nucleus activity

DOE PAGES

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

2015-09-14

Multiphase OH and O 3 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 O 3 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 particlesmore » exposed to OH and O 3 is evaluated by determining the hygroscopicity parameter, κ, as a function of particle type, mixing state, and OH and O 3 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 O 3 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 of single and multicomponent biomass burning aerosol surrogate-particles by OH: Implications for cloud condensation nucleus activity

DOE PAGES

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

2015-03-06

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

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

NASA Technical Reports Server (NTRS)

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

1997-01-01

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

Aerosol-Cloud Interactions during Tropical Deep Convection: Evidence for the Importance of Free Tropospheric Aerosols

NASA Technical Reports Server (NTRS)

Ackerman, A.; Jensen, E.; Stevens, D.; Wang, D.; Heymsfield, A.; Miloshevich, L.; Twohy, C.; Poellot, M.; VanReken, T.; Fridland, Ann

2003-01-01

NASA's 2002 CRYSTAL-FACE field experiment focused on the formation and evolution of tropical cirrus cloud systems in southern Florida. Multiple aircraft extensively sampled cumulonimbus dynamical and microphysical properties, as well as characterizing ambient aerosol populations both inside and outside the full depth of the convective column. On July 18, unique measurements were taken when a powerful updraft was traversed directly by aircraft, providing a window into the primary source region of cumulonimbus anvil crystals. Observations of the updraft, entered at approximately l0 km altitude and -34 C, indicated more than 200 cloud particles per mL at vertical velocities exceeding 20 m/s and the presence of significant condensation nuclei and liquid water within the core. In this work, aerosol and cloud phase observations are integrated by simulating the updraft conditions using a large-eddy resolving model with 3 explicit multiphase microphysics, including treatment of size-resolved aerosol fields, aerosol activation and freezing, and evaporation of cloud particles back to the aerosol phase. Simulations were initialized with observed thermodynamic and aerosol size distributions profiles and convection was driven by surface fluxes assimilated from the ARPS forecast model. Model results are consistent with the conclusions that most crystals are homogeneously frozen droplets and that entrained free tropospheric aerosols may contribute a significant fraction of the crystals. Thus most anvil crystals appear to be formed aloft in updraft cores, well above cloud base. These conclusions are supported by observations of hydrometeor size distribution made while traversing the dore, as well as aerosol and cloud particle size distributions generally observed by aircraft below 4km and crystal properties generally observed by aircraft above 12km.

The physico-chemical evolution of atmospheric aerosols and the gas-particle partitioning of inorganic aerosol during KORUS-AQ

NASA Astrophysics Data System (ADS)

Lee, T.; Park, T.; Lee, J. B.; Lim, Y. J.; Ahn, J.; Park, J. S.; Soo, C. J.; Desyaterik, Y.; Collett, J. L., Jr.

2017-12-01

Aerosols influence climate change directly by scattering and absorption and indirectly by acting as cloud condensation nuclei and some of the effects of aerosols are reduction in visibility, deterioration of human health, and deposition of pollutants to ecosystems. Urban area is large source of aerosols and aerosol precursors. Aerosol sources are both local and from long-range transport. Long-range transport processed aerosol are often dominant sources of aerosol pollution in Korea. To improve our knowledge of aerosol chemistry, Korea and U.S-Air Quality (KORUS-AQ) of Aircraft-based aerosol measurement took place in and around Seoul, Korea during May and June 2016. KORUS-AQ campaigns were conducted to study the chemical characterization and processes of pollutants in the Seoul Metropolitan area to regional scales of Korean peninsula. Aerodyne High Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed on aircraft platforms on-board DC-8 (NASA) aircraft. We characterized aerosol chemical properties and mass concentrations of sulfate, nitrate, ammonium and organics in polluted air plumes and investigate the spatial and vertical distribution of the species. The results of studies show that organics is predominant in Aerosol and a significant fraction of the organics is oxygenated organic aerosol (OOA) at the high altitude. Both Nitrate and sulfate can partition between the gas and particle phases. The ratios for HNO3/(N(V) (=gaseous HNO3 + particulate Nitrate) and SO2/(SO2+Sulfate) were found to exhibit quite different distributions between the particles and gas phase for the locations during KORUS-AQ campaign, representing potential for formation of additional particulate nitrate and sulfate. The results of those studies can provide highly resolved temporal and spatial air pollutant, which are valuable for air quality model input parameters for aerosol behaviour.

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.

Cloud forming potential of oligomers relevant to secondary organic aerosols

NASA Astrophysics Data System (ADS)

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

2014-09-01

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

Uncertainty in aerosol hygroscopicity resulting from semi-volatile organic compounds

NASA Astrophysics Data System (ADS)

Goulden, Olivia; Crooks, Matthew; Connolly, Paul

2018-01-01

We present a novel method of exploring the effect of uncertainties in aerosol properties on cloud droplet number using existing cloud droplet activation parameterisations. Aerosol properties of a single involatile particle mode are randomly sampled within an uncertainty range and resulting maximum supersaturations and critical diameters calculated using the cloud droplet activation scheme. Hygroscopicity parameters are subsequently derived and the values of the mean and uncertainty are found to be comparable to experimental observations. A recently proposed cloud droplet activation scheme that includes the effects of co-condensation of semi-volatile organic compounds (SVOCs) onto a single lognormal mode of involatile particles is also considered. In addition to the uncertainties associated with the involatile particles, concentrations, volatility distributions and chemical composition of the SVOCs are randomly sampled and hygroscopicity parameters are derived using the cloud droplet activation scheme. The inclusion of SVOCs is found to have a significant effect on the hygroscopicity and contributes a large uncertainty. For non-volatile particles that are effective cloud condensation nuclei, the co-condensation of SVOCs reduces their actual hygroscopicity by approximately 25 %. A new concept of an effective hygroscopicity parameter is introduced that can computationally efficiently simulate the effect of SVOCs on cloud droplet number concentration without direct modelling of the organic compounds. These effective hygroscopicities can be as much as a factor of 2 higher than those of the non-volatile particles onto which the volatile organic compounds condense.

Sea Spray Aerosol Production over the North Atlantic

NASA Astrophysics Data System (ADS)

Bates, T. S.; Quinn, P.

2017-12-01

Breaking waves on the ocean surface generate air bubbles that scavenge organic matter from the surrounding seawater. When injected into the atmosphere, these bubbles burst, yielding sea spray aerosol (SSA), a mixture of organic and inorganic compounds with the organic matter enriched relative to seawater. SSA mass is well documented as the dominant component of aerosol light scattering over the remote oceans. The importance of SSA number to marine boundary layer cloud condensation nuclei (CCN) is much less certain. During the Western Atlantic Climate Study cruises (WACS-1 - August 2012 and WACS-2 - May-June 2014) and the North Atlantic Aerosols and Marine Ecosystem Study cruises (NAAMES-1 - November 2015, NAAMES-2 - May 2016, and NAAMES-3 - September 2017), we generated and measured freshly emitted SSA using the Sea Sweep SSA generator. During the 2017 cruise we also generated SSA with a Marine Aerosol Reference Tank (MART). Using the data generated on these 5 cruises and a large database of remote marine boundary layer aerosol measurements we will address three questions during this presentation: 1 - Do phytoplankton ecosystems affect the organic enrichment of freshly emitted SSA?, 2 - Do plankton ecosystems affect the number production flux of SSA?, and 3 - Is SSA a significant source of atmospheric CCN?

Aerosol microphysical and radiative effects on continental cloud ensembles

NASA Astrophysics Data System (ADS)

Wang, Yuan; Vogel, Jonathan M.; Lin, Yun; Pan, Bowen; Hu, Jiaxi; Liu, Yangang; Dong, Xiquan; Jiang, Jonathan H.; Yung, Yuk L.; Zhang, Renyi

2018-02-01

Aerosol-cloud-radiation interactions represent one of the largest uncertainties in the current climate assessment. Much of the complexity arises from the non-monotonic responses of clouds, precipitation and radiative fluxes to aerosol perturbations under various meteorological conditions. In this study, an aerosol-aware WRF model is used to investigate the microphysical and radiative effects of aerosols in three weather systems during the March 2000 Cloud Intensive Observational Period campaign at the US Southern Great Plains. Three simulated cloud ensembles include a low-pressure deep convective cloud system, a collection of less-precipitating stratus and shallow cumulus, and a cold frontal passage. The WRF simulations are evaluated by several ground-based measurements. The microphysical properties of cloud hydrometeors, such as their mass and number concentrations, generally show monotonic trends as a function of cloud condensation nuclei concentrations. Aerosol radiative effects do not influence the trends of cloud microphysics, except for the stratus and shallow cumulus cases where aerosol semi-direct effects are identified. The precipitation changes by aerosols vary with the cloud types and their evolving stages, with a prominent aerosol invigoration effect and associated enhanced precipitation from the convective sources. The simulated aerosol direct effect suppresses precipitation in all three cases but does not overturn the aerosol indirect effect. Cloud fraction exhibits much smaller sensitivity (typically less than 2%) to aerosol perturbations, and the responses vary with aerosol concentrations and cloud regimes. The surface shortwave radiation shows a monotonic decrease by increasing aerosols, while the magnitude of the decrease depends on the cloud type.

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.

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.

Vertical distributions of fluorescent aerosol over the Eastern U.S.

NASA Astrophysics Data System (ADS)

Perring, A. E.; Robinson, E. S.; Schwarz, J. P.; Gao, R. S.

2016-12-01

The prevalence of bioaerosol in the atmosphere is relevant to atmospheric chemistry, microbial ecology and climate. These particles can act as effective cloud condensation nuclei (CCN) and ice nuclei (IN), representing a potential feedback between vegetation and precipitation. As bioaerosol frequently account for a substantial fraction of coarse mode aerosol in the boundary layer, they may have significant impacts on mixed-phase and/or cirrus cloud formation and climate. Very few measurements are available, however, to constrain loadings of bioaerosol in the free troposphere. Here we present vertical profiles of fluorescent aerosol concentration as a proxy for bioaerosol. The data were obtained over the eastern U.S. during the summer of 2016 using a Wide Band Integrated Bioaerosol Sensor (WIBS) installed aboard a NOAA Twin Otter research aircraft. The airspeed and inlet configuration were chosen to permit efficient sampling of aerosol with diameters of up to 10 μm. Vertical profiles extend from 1000 to 17,500 feet AGL, spanning a temperature range relevant to ice formation. 100 hours of data cover a latitude range from 30N to 46N and target a variety of potential bioaerosol source regions including forests, croplands, the Gulf of Mexico, and Lake Michigan. Observed vertical profiles are compared to expected loadings based on current model parameterizations and implications are discussed.

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

PubMed

Abdelsayed, Victor; El-Shall, M Samy

2014-08-07

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

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

Abdelsayed, Victor; Samy El-Shall, M., E-mail: mselshal@vcu.edu

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 indicatesmore » 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

Twenty years of balloon-borne tropospheric aerosol measurements at Laramie, Wyoming

NASA Technical Reports Server (NTRS)

Hofmann, David J.

1993-01-01

The paper examines the tropospheric aerosol record obtained over the period 1971 to 1990, during which high-altitude balloons with optical particle counters were launched at Laramie, Wyoming, in a long-term study of the stratospheric sulfate aerosol layer. All aerosol particle size ranges display pronounced seasonal variations, with the condensation nuclei concentration and the optically active component showing a summer maximum throughout the troposphere. Mass estimates, assuming spherical sulfate particles, indicate an average column mass between altitudes of 2.5 and 10 km of about 4 and 16 mg/sq m in winter and summer, respectively. Calculated optical depths vary between 0.01 and 0.04 from winter to summer; the estimated mass scattering cross section is about 3 sq m/g throughout the troposphere. There is evidence for a decreasing trend of 1.6-1.8 percent/yr in the optically active tropospheric aerosol over the past 20 yr, which may be related to a similar reduction in SO2 emission in the U.S. over this period.

A dichotomy in primary marine organic aerosol-cloud-climate system

NASA Astrophysics Data System (ADS)

Ceburnis, D.; Ovadnevaite, J.; Martucci, G.; Bialek, J.; Monahan, C.; Rinaldi, M.; Facchini, C.; Berresheim, H.; Worsnop, D. R.; O'Dowd, C.

2011-12-01

D. Ceburnis1, J. Ovadnevaite1, G. Martucci1, J. Bialek1, C. Monahan1, M. Rinaldi2, M. C. Facchini2, H. Berresheim1, D. R. Worsnop3,4 and C. D. O'Dowd1 1School of Physics & Centre for Climate and Air Pollution Studies, National University of Ireland Galway, University Road, Galway, Ireland 2Institute of Atmospheric Sciences and Climate, National Research Council, Bologna, 20129, Italy. 3 Aerodyne Research, Inc., 45 Manning Road, Billerica, MA 01821-3976, USA 4 Physics Department, University of Helsinki, P.O. Box 64, 00014, Helsinki, Finland Organic matter has been observed to significantly contribute to particulate matter in every environment including pristine remote oceans. A significant if not dominant contribution of insoluble organic matter to marine aerosol has been proved to be of biogenic origin1,2. High time resolution measurements of marine organic matter have demonstrated a dynamic system with regular organic matter plume events occurring during summer3 as well as frequent open ocean particle formation events4. High-time resolution measurements of primary marine organic sea-spray physico-chemical properties reveal an apparent dichotomous behavior in terms of water uptake: specifically sea-spray aerosol enriched in organic matter possesses a low hygroscopic Growth Factor (GF~1.25) while simultaneously having a cloud condensation nucleus/condensation nuclei (CCN/CN) activation efficiency of between 83% at 0.25% supersaturation and 100% at 0.75%5. Simultaneous retrieval of Cloud Droplet Number Concentration (CDNC) during primary organic aerosol plumes reveal CDNC concentrations of 350 cm-3 in newly formed marine stratocumulus cloud for boundary layer organic mass concentrations of 3-4 ug m-36. It is suggested that marine hydrogels are responsible for this dichotomous behavior which has profound impacts to aerosol-cloud-climate system along with a better understood process analysis of aerosol formation by sea-spray7. A hydrophobic character of organic matter

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.

Global observations of aerosol-cloud-precipitation-climate interactions

NASA Astrophysics Data System (ADS)

Rosenfeld, Daniel; Andreae, Meinrat O.; Asmi, Ari; Chin, Mian; de 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.

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

NASA Technical Reports Server (NTRS)

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

1997-01-01

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

A cloud-resolving model study of aerosol-cloud correlation in a pristine maritime environment

NASA Astrophysics Data System (ADS)

Nishant, Nidhi; Sherwood, Steven C.

2017-06-01

In convective clouds, satellite-observed deepening or increased amount of clouds with increasing aerosol concentration has been reported and is sometimes interpreted as aerosol-induced invigoration of the clouds. However, such correlations can be affected by meteorological factors that affect both aerosol and clouds, as well as observational issues. In this study, we examine the behavior in a 660 × 660 km2 region of the South Pacific during June 2007, previously found by Koren et al. (2014) to show strong correlation between cloud fraction, cloud top pressure, and aerosols, using a cloud-resolving model with meteorological boundary conditions specified from a reanalysis. The model assumes constant aerosol loading, yet reproduces vigorous clouds at times of high real-world aerosol concentrations. Days with high- and low-aerosol loading exhibit deep-convective and shallow clouds, respectively, in both observations and the simulation. Synoptic analysis shows that vigorous clouds occur at times of strong surface troughs, which are associated with high winds and advection of boundary layer air from the Southern Ocean where sea-salt aerosol is abundant, thus accounting for the high correlation. Our model results show that aerosol-cloud relationships can be explained by coexisting but independent wind-aerosol and wind-cloud relationships and that no cloud condensation nuclei effect is required.

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

NASA Technical Reports Server (NTRS)

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

2016-01-01

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

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

PubMed Central

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

2016-01-01

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

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jiang, Yiquan; Liu, Xiaohong; Yang, Xiuqun

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 increasemore » 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.« less

Aerosol-Cloud Interactions and Cloud Microphysical Properties in the Asir Region of Saudi Arabia

NASA Astrophysics Data System (ADS)

Kucera, P. A.; Axisa, D.; Burger, R. P.; Li, R.; Collins, D. R.; Freney, E. J.; Buseck, P. R.

2009-12-01

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, located adjacent to the Red Sea in the southwest region of Saudi Arabia. Ground measurements of aerosol size distributions, hygroscopic growth factors, CCN concentrations as well as aircraft measurements of cloud hydrometeor size distributions were observed in the Asir region in August 2009. The presentation will include a summary of the analysis and results with a focus on aerosol-cloud interactions and cloud microphysical properties observed during the convective season in the Asir region.

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.

Impacts of the mixing state and chemical composition on the cloud condensation nuclei (CCN) activity in Beijing during winter, 2016

NASA Astrophysics Data System (ADS)

Ren, J.; Zhang, F.

2017-12-01

Abstract.Understanding aerosol chemical composition and mixing state on CCN activity in polluted urban area is crucial to determine NCCN accurately and thus to quantify aerosol indirect effects. Aerosol hrgroscopicity, size-resolved cloud condensation nuclei (CCN) concentration and chemical composition are measured under polluted and background conditions in Beijing based on the Air Pollution and Human Health (APHH) field campaign in winter 2016. The CCN number concentration (NCCN) is predicted by using κ-Köhler theory from the PNSD and five simplified of the mixing state and chemical composition. The assumption of EIS (sulfate, nitrate and SOA internally mixed, and POA and BC externally mixed with size-resolved chemical composition) shows the best closure to predict NCCN with the ratio of predicted to measured NCCN of 0.96-1.12 both in POL and BG conditions. Under BG conditions, IB (internal mixture with bulk chemical composition) scheme achieves the best CCN closure during any periods of a day. In polluted days, EIS and IS (internal mixture with size-resolved chemical composition) scheme may achieve better closure than IB scheme due to the heterogeneity in particles composition across different size. ES (external mixture with size-resolved chemical composition) and EB (external mixture with bulk chemical composition) scheme markedly underestimate the NCCN with the ratio of predicted to measured NCCN of 0.6-0.8. In addition, we note that assumptions of size-resolved composition (IS or ES) show very limited promotes by comparing with the assumptions of bulk composition (IB or EB), furthermore, the prediction becomes worse by using size-resolved assumption in clean days. The predicted NCCN during eve-rush periods shows the most sensitivity to the five different assumptions, with ratios of the predicted and measured NCCN ranging from 0.5 to 1.4, reflecting great impacts from evening traffic and cooking sources. The result from the sensitivity examination of predict

Background aerosol over the Himalayas and Tibetan Plateau: observed characteristics of aerosol mass loading

NASA Astrophysics Data System (ADS)

Liu, Bin; Cong, Zhiyuan; Wang, Yuesi; Xin, Jinyuan; Wan, Xin; Pan, Yuepeng; Liu, Zirui; Wang, Yonghong; Zhang, Guoshuai; Wang, Zhongyan; Wang, Yongjie; Kang, Shichang

2017-01-01

barren to forest, in inverse relation to the PM2.5 ratios. The seasonality of aerosol mass parameters was land-cover dependent. Over forest and grassland areas, TSP mass, PM2.5 mass, MISR-AOD and fine-mode AOD were higher in spring and summer, followed by relatively lower values in autumn and winter. At the barren site (the QOMS station), there were inconsistent seasonal patterns between surface TSP mass (PM2.5 mass) and atmospheric column AOD (fine-mode AOD). Our findings implicate that HTP aerosol masses (especially their regional characteristics and fine-particle emissions) need to be treated sensitively in relation to assessments of their climatic effect and potential role as cloud condensation nuclei and ice nuclei.

CCN activity of thermodenuded aerosol particles downwind of the Sacramento area urban plume

NASA Astrophysics Data System (ADS)

Hiranuma, N.; Cziczo, D. J.; Nelson, D.; Zhang, Q.; Setyan, A.; Song, C.; Shrivastava, M.; Shilling, J. E.

2010-12-01

This study focuses on the characterization of cloud condensation nuclei (CCN) properties of aerosol particles measured during the Carbonaceous Aerosols and Radiative Effects Study (CARES) near Sacramento, CA in June 2010. Supersaturation-dependant CCN activity (0.07 - 0.5% supersaturation) was measured with DMT CCN counters at two locations; one near the city center (T0) and the other in Cool, CA, a small town located ~40 kilometers downwind of the urban plume in the Sierra Nevada foothills (T1). The T1 CCN counter was operated behind a thermodenuder to study volatility-dependant CCN activity of the urban aerosol plume as it was transported into the biogenically influenced foothills. Preliminary analysis indicated that activated fraction was inversely proportional to the thermodenuder temperature, suggesting that the more-volatile fraction of the aerosol might have played an important role in the CCN activity of the aerosol. The relationship between the chemical composition and CCN activity of the aerosol will be discussed. The physical and chemical transformations of particles aged in the foothills as well as the diurnal profiles of CCN both at T0 and T1 will also be discussed for the transport event of 15 June 2010.

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

Characterization of a large biogenic secondary organic aerosol event from eastern Canadian forests

NASA Astrophysics Data System (ADS)

Slowik, J. G.; Stroud, C.; Bottenheim, J. W.; Brickell, P. C.; Chang, R. Y.-W.; Liggio, J.; Makar, P. A.; Martin, R. V.; Moran, M. D.; Shantz, N. C.; Sjostedt, S. J.; van Donkelaar, A.; Vlasenko, A.; Wiebe, H. A.; Xia, A. G.; Zhang, J.; Leaitch, W. R.; Abbatt, J. P. D.

2010-03-01

Measurements of aerosol composition, volatile organic compounds, and CO are used to determine biogenic secondary organic aerosol (SOA) concentrations at a rural site 70 km north of Toronto. These biogenic SOA levels are many times higher than past observations and occur during a period of increasing temperatures and outflow from Northern Ontario and Quebec forests in early summer. A regional chemical transport model approximately predicts the event timing and accurately predicts the aerosol loading, identifying the precursors as monoterpene emissions from the coniferous forest. The agreement between the measured and modeled biogenic aerosol concentrations contrasts with model underpredictions for polluted regions. Correlations of the oxygenated organic aerosol mass with tracers such as CO support a secondary aerosol source and distinguish biogenic, pollution, and biomass burning periods during the field campaign. Using the Master Chemical Mechanism, it is shown that the levels of CO observed during the biogenic event are consistent with a photochemical source arising from monoterpene oxidation. The biogenic aerosol mass correlates with satellite measurements of regional aerosol optical depth, indicating that the event extends across the eastern Canadian forest. This regional event correlates with increased temperatures, indicating that temperature-dependent forest emissions can significantly affect climate through enhanced direct optical scattering and higher cloud condensation nuclei numbers.

Aerosol Activation Properties within and above Mixing Layer in the North China Plain

NASA Astrophysics Data System (ADS)

Deng, Z.; Ran, L.

2013-12-01

Aerosol particles, serving as cloud condensation nuclei (CCN), may modify the properties of clouds and have an impact on climate. The vertical distribution of aerosols and their activation properties is critical to quantify the effect of aerosols on clouds. An intensive field campaign, Vertical Observations of trace Gases and Aerosols in the North China Plain (VOGA-NCP 2013), was conducted in the North China Plain during the late July and early August 2013 to measure the vertical profiles of atmospheric components in this polluted region and estimate their effects on atmospheric environment and climate. Aerosols were measured with in-situ instruments and Lidar. Particularly, the aerosols were collected at 1000 m height with a 1 m3 bag sampler attached to a tethered balloon, and subsequently measured with combined scanning mobility particle sizer (SMPS) and CCN counter. Comparisons of size-resolved activation ratios at ground level and 1000 m height showed that aerosols in upper atmosphere were not only less concentrated, but also less CCN-active than those at the surface. The difference in aerosol properties between upper atmosphere and the ground indicates that the analysis of impacts of aerosols on cloud might be misleading in heavily polluted region based on the relationship of cloud properties and surface aerosols or column without considering the vertical distribution of aerosol activation abilities.

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

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

2016-05-27

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

Spatial Variability of CCN Sized Aerosol Particles

NASA Astrophysics Data System (ADS)

Asmi, A.; Väänänen, R.

2014-12-01

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

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

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.

Sensitivity of Aerosol Mass and Microphysics to Treatments of Condensational Growth of Secondary Organic Compounds in a Regional Model

NASA Astrophysics Data System (ADS)

Topping, D. O.; Lowe, D.; McFiggans, G.; Zaveri, R. A.

2016-12-01

Gas to particle partitioning of atmospheric compounds occurs through disequilibrium mass transfer rather than through instantaneous equilibrium. However, it is common to treat only the inorganic compounds as partitioning dynamically whilst organic compounds, represented by the Volatility Basis Set (VBS), are partitioned instantaneously. In this study we implement a more realistic dynamic partitioning of organic compounds in a regional framework and assess impact on aerosol mass and microphysics. It is also common to assume condensed phase water is only associated with inorganic components. We thus also assess sensitivity to assuming all organics are hygroscopic according to their prescribed molecular weight.For this study we use WRF-Chem v3.4.1, focusing on anthropogenic dominated North-Western Europe. Gas-phase chemistry is represented using CBM-Z whilst aerosol dynamics are simulated using the 8-section MOSAIC scheme, including a 9-bin volatility basis set (VBS) treatment of organic aerosol. Results indicate that predicted mass loadings can vary significantly. Without gas phase ageing of higher volatility compounds, dynamic partitioning always results in lower mass loadings downwind of emission sources. The inclusion of condensed phase water in both partitioning models increases the predicted PM mass, resulting from a larger contribution from higher volatility organics, if present. If gas phase ageing of VBS compounds is allowed to occur in a dynamic model, this can often lead to higher predicted mass loadings, contrary to expected behaviour from a simple non-reactive gas phase box model. As descriptions of aerosol phase processes improve within regional models, the baseline descriptions of partitioning should retain the ability to treat dynamic partitioning of organic compounds. Using our simulations, we discuss whether derived sensitivities to aerosol processes in existing models may be inherently biased.This work was supported by the Nature Environment

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

NASA Astrophysics Data System (ADS)

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

2013-12-01

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

A technique for the measurement of organic aerosol hygroscopicity, oxidation level, and volatility distributions

NASA Astrophysics Data System (ADS)

Cain, Kerrigan P.; Pandis, Spyros N.

2017-12-01

Hygroscopicity, oxidation level, and volatility are three crucial properties of organic pollutants. This study assesses the feasibility of a novel measurement and analysis technique to determine these properties and establish their relationship. The proposed experimental setup utilizes a cloud condensation nuclei (CCN) counter to quantify hygroscopic activity, an aerosol mass spectrometer to measure the oxidation level, and a thermodenuder to evaluate the volatility. The setup was first tested with secondary organic aerosol (SOA) formed from the ozonolysis of α-pinene. The results of the first experiments indicated that, for this system, the less volatile SOA contained species that had on average lower O : C ratios and hygroscopicities. In this SOA system, both low- and high-volatility components can have comparable oxidation levels and hygroscopicities. The method developed here can be used to provide valuable insights about the relationships among organic aerosol hygroscopicity, oxidation level, and volatility.

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

NASA Astrophysics Data System (ADS)

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

2016-11-01

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

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.

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.

Redistribution of ice nuclei between cloud and rain droplets: Parameterization and application to deep convective clouds: ICE NUCLEI IN RAIN DROPLETS

DOE PAGES

Paukert, M.; Hoose, C.; Simmel, M.

2017-02-21

In model studies of aerosol-dependent immersion freezing in clouds, a common assumption is that each ice nucleating aerosol particle corresponds to exactly one cloud droplet. Conversely, the immersion freezing of larger drops—“rain”—is usually represented by a liquid volume-dependent approach, making the parameterizations of rain freezing independent of specific aerosol types and concentrations. This may lead to inconsistencies when aerosol effects on clouds and precipitation shall be investigated, since raindrops consist of the cloud droplets—and corresponding aerosol particles—that have been involved in drop-drop-collisions. We introduce an extension to a two-moment microphysical scheme in order to account explicitly for particle accumulation inmore » raindrops by tracking the rates of selfcollection, autoconversion, and accretion. This also provides a direct link between ice nuclei and the primary formation of large precipitating ice particles. A new parameterization scheme of drop freezing is presented to consider multiple ice nuclei within one drop and effective drop cooling rates. In our test cases of deep convective clouds, we find that at altitudes which are most relevant for immersion freezing, the majority of potential ice nuclei have been converted from cloud droplets into raindrops. Compared to the standard treatment of freezing in our model, the less efficient mineral dust-based freezing results in higher rainwater contents in the convective core, affecting both rain and hail precipitation. The aerosol-dependent treatment of rain freezing can reverse the signs of simulated precipitation sensitivities to ice nuclei perturbations.« less

Redistribution of ice nuclei between cloud and rain droplets: Parameterization and application to deep convective clouds: ICE NUCLEI IN RAIN DROPLETS

DOE Office of Scientific and Technical Information (OSTI.GOV)

Paukert, M.; Hoose, C.; Simmel, M.

In model studies of aerosol-dependent immersion freezing in clouds, a common assumption is that each ice nucleating aerosol particle corresponds to exactly one cloud droplet. Conversely, the immersion freezing of larger drops—“rain”—is usually represented by a liquid volume-dependent approach, making the parameterizations of rain freezing independent of specific aerosol types and concentrations. This may lead to inconsistencies when aerosol effects on clouds and precipitation shall be investigated, since raindrops consist of the cloud droplets—and corresponding aerosol particles—that have been involved in drop-drop-collisions. We introduce an extension to a two-moment microphysical scheme in order to account explicitly for particle accumulation inmore » raindrops by tracking the rates of selfcollection, autoconversion, and accretion. This also provides a direct link between ice nuclei and the primary formation of large precipitating ice particles. A new parameterization scheme of drop freezing is presented to consider multiple ice nuclei within one drop and effective drop cooling rates. In our test cases of deep convective clouds, we find that at altitudes which are most relevant for immersion freezing, the majority of potential ice nuclei have been converted from cloud droplets into raindrops. Compared to the standard treatment of freezing in our model, the less efficient mineral dust-based freezing results in higher rainwater contents in the convective core, affecting both rain and hail precipitation. The aerosol-dependent treatment of rain freezing can reverse the signs of simulated precipitation sensitivities to ice nuclei perturbations.« less

Density-induced suppression of the {alpha}-particle condensate in nuclear matter and the structure of {alpha}-cluster states in nuclei

DOE Office of Scientific and Technical Information (OSTI.GOV)

Funaki, Y.; Horiuchi, H.; International Institute for Advanced Studies, Kizugawa 619-0225

2008-06-15

At low densities, with decreasing temperatures, in symmetric nuclear matter {alpha} particles are formed, which eventually give raise to a quantum condensate with four-nucleon {alpha}-like correlations (quartetting). Starting with a model of {alpha} matter, where undistorted {alpha} particles interact via an effective interaction such as the Ali-Bodmer potential, the suppression of the condensate fraction at zero temperature with increasing density is considered. Using a Jastrow-Feenberg approach, it is found that the condensate fraction vanishes near saturation density. Additionally, the modification of the internal state of the {alpha} particle due to medium effects will further reduce the condensate. In finite systems,more » an enhancement of the S-state wave function of the center-of-mass orbital of {alpha}-particle motion is considered as the correspondence to the condensate. Wave functions have been constructed for self-conjugate 4n nuclei that describe the condensate state but are fully antisymmetrized on the nucleonic level. These condensate-like cluster wave functions have been successfully applied to describe properties of low-density states near the n{alpha} threshold. Comparison with orthogonality condition model calculations in {sup 12}C and {sup 16}O shows strong enhancement of the occupation of the S-state center-of-mass orbital of the {alpha} particles. This enhancement is decreasing if the baryon density increases, similar to the density-induced suppression of the condensate fraction in {alpha} matter. The ground states of {sup 12}C and {sup 16}O show no enhancement at all, thus a quartetting condensate cannot be formed at saturation densities.« less

Global sensing of gaseous and aerosol trace species using automated instrumentation on 747 airliners

NASA Technical Reports Server (NTRS)

Perkins, P. J.; Papathakos, L. C.

1978-01-01

The Global Atmospheric Sampling Program (GASP) is collecting and analyzing data on gaseous and aerosol trace contaminants in the upper troposphere and lower stratosphere. Measurements are obtained from automated systems installed on four 747 airliners flying global air routes. Improved instruments and analysis techniques are providing an expanding data base for trace species including ozone, carbon monoxide, water vapor, condensation nuclei, and mass concentration of sulfates and nitrates. Simultaneous measurements of several trace species obtained frequently can be used to identify the source of the air mass as being typically tropospheric or stratospheric.

Hygroscopicity of dicarbonyl-amine secondary organic aerosol products investigated with HTDMA

NASA Astrophysics Data System (ADS)

Hawkins, L. N.; de Haan, D. O.

2010-12-01

Recent studies have shown the importance of amine-dicarbonyl chemistry as a secondary organic aerosol (SOA) formation pathway, producing imines, imidazoles, and N-containing oligomers. Preliminary work in our group has suggested that some of these products may be surface active. Therefore, the presence of these products may result in important changes to submicron particle hygroscopicity that affect aerosol scattering and cloud condensation nuclei (CCN) activity, especially in regions with significant amine-containing particles. To investigate their hygroscopicity, we have designed a hygroscopicity tandem differential mobility analyzer (HTDMA) system around a 300 L Teflon chamber that allows for longer humidification times needed for some organic aerosol components that are only slightly hygroscopic. This modification provides a range of residence times from 2.5 minutes up to 1 hour, unlike previously published systems that vary from 2-30 seconds. Using the modified hygroscopicity tandem differential mobility analyzer (HTDMA), we have measured the hygroscopic growth factor (HGF) of SOA formed from reactions of glyoxal (and methylglyoxal) with methylamine, ammonium sulfate, and several amino acids. Changes to inorganic aerosol HGF in response to the presence of SOA products are also investigated.

Influence of inland aerosol loading on the monsoon over Indian subcontinent

NASA Astrophysics Data System (ADS)

Satyanarayana, M.; Krishnakumar, V.; Mahadevan Pillai, V. P.; Radhakrishnan, S. R.; Raghunath, K.

2008-12-01

The monsoon water cycle is the lifeline to over 60% of the world's population. The study on the behavioral change of Indian monsoon due to aerosol loading will help for the better understanding of Indian Monsoon. Aerosol system influences the atmosphere in two ways; it affects directly the radiation budget and indirectly provides condensation nuclei required for the clouds. The precipitation of the clouds in the monsoon season depends on the microphysical properties of the clouds. The effect of aerosol on cirrus clouds is being looked into through this work as an effort to study the role of aerosol on Indian Monsoon. The microphysical properties of high altitude clouds were obtained from the ground based lidar experiments at a low latitude station in the Indian subcontinent. Measurements during the Indian monsoon period from the inland station National Atmospheric Research Laboratory (NARL) Gadanki (13.5_ N, 79.2_ E), Tirupati, India were used for the investigation. The depolarization characteristics of the cirrus clouds were measured and the correlation between the depolarization and the precipitation characteristics were studied. The results obtained over a period of one year from January 1998 to December 1998 were presented.

Aerosol Microphysical and Radiative Effects on Continental Cloud Ensembles

DOE PAGES

Wang, Yuan; Vogel, Jonathan M.; Lin, Yun; ...

2018-01-10

Aerosol-cloud-radiation interactions represent one of the largest uncertainties in the current climate assessment. Much of the complexity arises from the non-monotonic responses of clouds, precipitation and radiative fluxes to aerosol perturbations under various meteorological conditions. Here, an aerosol-aware Weather Research and Forecasting (WRF) model is used to investigate the microphysical and radiative effects of aerosols in three weather systems during the March 2000 Cloud Intensive Observational Period campaign at the Southern Great Plains site of the US Atmospheric Radiation Measurement Program. Three cloud ensembles with different meteorological conditions are simulated, including a low-pressure deep convective cloud system, a series ofmore » lessprecipitating stratus and shallow cumulus, and a cold frontal passage. The WRF simulations are evaluated by the available observations of cloud fraction, liquid water path, precipitation, and surface temperature. The microphysical properties of cloud hydrometeors, such as their mass and number concentrations, generally show monotonic trends as a function of cloud condensation nuclei concentrations. Aerosol radiative effects do not interfere the trends of cloud microphysics, except for the stratus and shallow cumulus cases where aerosol semi-direct effects are identified. The precipitation changes by aerosols vary with the cloud types and their evolving stages, with more prominent aerosol invigoration effect and associated enhanced precipitation from the convective sources. Furthermore, the simulated aerosol direct effect suppresses precipitation in all three cases but does not overturn the direction of precipitation changes by the aerosol indirect effect. Cloud fraction exhibits much smaller sensitivity (typically less than 2%) to aerosol perturbations than the cloud microphysics, and the responses vary with aerosol concentrations and cloud regimes. The surface shortwave radiation shows a monotonic decrease by

Aerosol Microphysical and Radiative Effects on Continental Cloud Ensembles

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Yuan; Vogel, Jonathan M.; Lin, Yun

Aerosol-cloud-radiation interactions represent one of the largest uncertainties in the current climate assessment. Much of the complexity arises from the non-monotonic responses of clouds, precipitation and radiative fluxes to aerosol perturbations under various meteorological conditions. Here, an aerosol-aware Weather Research and Forecasting (WRF) model is used to investigate the microphysical and radiative effects of aerosols in three weather systems during the March 2000 Cloud Intensive Observational Period campaign at the Southern Great Plains site of the US Atmospheric Radiation Measurement Program. Three cloud ensembles with different meteorological conditions are simulated, including a low-pressure deep convective cloud system, a series ofmore » lessprecipitating stratus and shallow cumulus, and a cold frontal passage. The WRF simulations are evaluated by the available observations of cloud fraction, liquid water path, precipitation, and surface temperature. The microphysical properties of cloud hydrometeors, such as their mass and number concentrations, generally show monotonic trends as a function of cloud condensation nuclei concentrations. Aerosol radiative effects do not interfere the trends of cloud microphysics, except for the stratus and shallow cumulus cases where aerosol semi-direct effects are identified. The precipitation changes by aerosols vary with the cloud types and their evolving stages, with more prominent aerosol invigoration effect and associated enhanced precipitation from the convective sources. Furthermore, the simulated aerosol direct effect suppresses precipitation in all three cases but does not overturn the direction of precipitation changes by the aerosol indirect effect. Cloud fraction exhibits much smaller sensitivity (typically less than 2%) to aerosol perturbations than the cloud microphysics, and the responses vary with aerosol concentrations and cloud regimes. The surface shortwave radiation shows a monotonic decrease by

Quantification of chromatin condensation level by image processing.

PubMed

Irianto, Jerome; Lee, David A; Knight, Martin M

2014-03-01

The level of chromatin condensation is related to the silencing/activation of chromosomal territories and therefore impacts on gene expression. Chromatin condensation changes during cell cycle, progression and differentiation, and is influenced by various physicochemical and epigenetic factors. This study describes a validated experimental technique to quantify chromatin condensation. A novel image processing procedure is developed using Sobel edge detection to quantify the level of chromatin condensation from nuclei images taken by confocal microscopy. The algorithm was developed in MATLAB and used to quantify different levels of chromatin condensation in chondrocyte nuclei achieved through alteration in osmotic pressure. The resulting chromatin condensation parameter (CCP) is in good agreement with independent multi-observer qualitative visual assessment. This image processing technique thereby provides a validated unbiased parameter for rapid and highly reproducible quantification of the level of chromatin condensation. Copyright © 2013 IPEM. Published by Elsevier Ltd. All rights reserved.

Spatio-temporal aerosol particle distributions in the UT/LMS measured by the IAGOS-CARIBIC Observatory

NASA Astrophysics Data System (ADS)

Assmann, Denise; Hermann, Markus; Weigelt, Andreas; Martinsson, Bengt; Brenninkmeijer, Carl; Rauthe-Schöch, Armin; van Velthoven, Peter; Bönisch, Harald; Zahn, Andreas

2017-04-01

Submicrometer aerosol particles in the upper troposphere and lowermost stratosphere (UT/LMS) influence the Earth`s radiation budget directly and, more important, indirectly, by acting as cloud condensation nuclei and by changing trace gas concentrations through heterogeneous chemical processes. Since 1997, regular in situ UT/LMS aerosol particle measurements have been conducted by the Leibniz Institute for Tropospheric Research, Leipzig, Germany and the University of Lund, Sweden, using the the CARIBIC (now IAGOS-CARIBIC) observatory (www.caribic-atmospheric.com) onboard a passenger aircraft. Submicrometer aerosol particle number concentrations and the aerosol particle size distribution are measured using three condensation particle counters and one optical particle size spectrometer. Moreover, particle elemental composition is determined using an aerosol impactor sampler and post-flight ion beam analysis (PIXE, PESA) of the samples in the laboratory. Based on this unique data set, including meteorological analysis, we present representative spatio-temporal distributions of particle number, surface, volume and elemental concentrations in an altitude of 8-12 km covering a large fraction of the northern hemisphere. We discuss the measured values in the different size regimes with respect to sources and sinks in different regions. Additionally, we calculated highly resolved latitudinal and longitudinal cross sections of the particle number size distribution, probability density functions and trends in particle number concentrations, but also in elemental composition, determined from our regular measurements over more than a decade. Moreover, we generated seasonal contour plots for particle number concentrations, the potential temperature, and the equivalent latitude. The results are interpreted with respect to aerosol microphysics and transport using CARIBIC trace gas data like ozone and water vapour. The influence of clouds in the troposphere and the different

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

SJ Ghan; B Schmid; JM Hubbe

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 icemore » 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

Ice nucleation properties of atmospheric aerosol particles collected during a field campaign in Cyprus

NASA Astrophysics Data System (ADS)

Yordanova, Petya; Maier, Stefanie; Lang-Yona, Naama; Tamm, Alexandra; Meusel, Hannah; Pöschl, Ulrich; Weber, Bettina; Fröhlich-Nowoisky, Janine

2017-04-01

Atmospheric aerosol particles, including desert and soil dust as well as marine aerosols, are well known to act as ice nuclei (IN) and thus have been investigated in numerous ice nucleation studies. Based on their cloud condensation nuclei potential and their impacts on radiative properties of clouds (via scattering and absorption of solar radiation), aerosol particles may significantly affect the cloud and precipitation development. Atmospheric aerosols of the Eastern Mediterranean have been described to be dominated by desert dust, but only little is known on their composition and ice nucleating properties. In this study we investigated the ice nucleating ability of total suspended particles (TSP), collected at the remote site Agia Marina Xyliatou on Cyprus during a field campaign in April 2016. Airborne TSP samples containing air masses of various types such as African (Saharan) and Arabian dust and European and Middle Eastern pollution were collected on glass fiber filters at 24 h intervals. Sampling was performed ˜5 m above ground level and ˜521 m above sea level. During the sampling period, two major dust storms (PM 10max 118 μg/m3 and 66 μg/m3) and a rain event (rainfall amount: 3.4 mm) were documented. Chemical and physical characterizations of the particles were analyzed experimentally through filtration, thermal, chemical and enzyme treatments. Immersion freezing experiments were performed at relatively high subzero temperatures (-1 to -15˚ C) using the mono ice nucleation array. Preliminary results indicate that highest IN particle numbers (INPs) occurred during the second dust storm event with lower particle concentrations. Treatments at 60˚ C lead to a gradual IN deactivation, indicating the presence of biological INPs, which were observed to be larger than 300 kDa. Additional results originating from this study will be shown. Acknowledgement: This work was funded by the DFG Ice Nuclei Research Unit (INUIT).

Sensitivity of Aerosol Mass and Microphysics to varying treatments of Condensational Growth of Secondary Organic Compounds in a regional model

NASA Astrophysics Data System (ADS)

Lowe, Douglas; Topping, David; McFiggans, Gordon

2017-04-01

Gas to particle partitioning of atmospheric compounds occurs through disequilibrium mass transfer rather than through instantaneous equilibrium. However, it is common to treat only the inorganic compounds as partitioning dynamically whilst organic compounds, represented by the Volatility Basis Set (VBS), are partitioned instantaneously. In this study we implement a more realistic dynamic partitioning of organic compounds in a regional framework and assess impact on aerosol mass and microphysics. It is also common to assume condensed phase water is only associated with inorganic components. We thus also assess sensitivity to assuming all organics are hygroscopic according to their prescribed molecular weight. For this study we use WRF-Chem v3.4.1, focusing on anthropogenic dominated North-Western Europe. Gas-phase chemistry is represented using CBM-Z whilst aerosol dynamics are simulated using the 8-section MOSAIC scheme, including a 9-bin VBS treatment of organic aerosol. Results indicate that predicted mass loadings can vary significantly. Without gas phase ageing of higher volatility compounds, dynamic partitioning always results in lower mass loadings downwind of emission sources. The inclusion of condensed phase water in both partitioning models increases the predicted PM mass, resulting from a larger contribution from higher volatility organics, if present. If gas phase ageing of VBS compounds is allowed to occur in a dynamic model, this can often lead to higher predicted mass loadings, contrary to expected behaviour from a simple non-reactive gas phase box model. As descriptions of aerosol phase processes improve within regional models, the baseline descriptions of partitioning should retain the ability to treat dynamic partitioning of organics compounds. Using our simulations, we discuss whether derived sensitivities to aerosol processes in existing models may be inherently biased. This work was supported by the Natural Environment Research Council within

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

NASA Astrophysics Data System (ADS)

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

2012-04-01

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

Chemical and physical properties of biomass burning aerosols and their CCN activity: A case study in Beijing, China.

PubMed

Wu, Zhijun; Zheng, Jing; Wang, Yu; Shang, Dongjie; Du, Zhoufei; Zhang, Yuanhang; Hu, Min

2017-02-01

Biomass burning emits large amounts of both trace gases and particles into the atmosphere. It plays a profound role in regional air quality and climate change. In the present study, an intensive campaign was carried out at an urban site in Beijing, China, in June 2014, which covered the winter wheat harvest season over the North China Plain (NCP). Meanwhile, two evident biomass-burning events were observed. A clear burst in ultrafine particles (below 100nm in diameter, PM 1 ) and subsequent particle growth took place during the events. With the growth of the ultrafine particles, the organic fraction of PM 1 increased significantly. The ratio of oxygen to carbon (O:C), which had an average value of 0.23±0.04, did not show an obvious enhancement, indicating that a significant chemical aging process of the biomass-burning aerosols was not observed during the course of events. This finding might have been due to the fact that the biomass-burning events occurred in the late afternoon and grew during the nighttime, which is associated with a low atmospheric oxidation capacity. On average, organics and black carbon (BC) were dominant in the biomass-burning aerosols, accounting for 60±10% and 18±3% of PM 1 . The high organic and BC fractions led to a significant suppression of particle hygroscopicity. Comparisons among hygroscopicity tandem differential mobility analyzer (HTDMA)-derived, cloud condensation nuclei counter (CCNc)-derived, and aerosol mass spectrometer-based hygroscopicity parameter (κ) values were consistent. The mean κ values of biomass-burning aerosols derived from both HTDMA and CCNc measurements were approximately 0.1, regardless of the particle size, indicating that the biomass-burning aerosols were less active. The burst in particle count during the biomass-burning events resulted in an increased number of cloud condensation nuclei (CCN) at supersaturation (SS)=0.2-0.8%. Copyright © 2016 Elsevier B.V. All rights reserved.

Role of air sampling in investigation of an outbreak of legionnaires' disease associated with exposure to aerosols from an evaporative condenser.

PubMed

Breiman, R F; Cozen, W; Fields, B S; Mastro, T D; Carr, S J; Spika, J S; Mascola, L

1990-06-01

Epidemiologic studies have suggested that legionnaires' disease can be transmitted to susceptible hosts by contaminated aerosolized water from cooling towers and evaporative condensers; however, epidemic strains of Legionella have not been isolated by air sampling at such sites during epidemiologic investigations. An outbreak of legionnaires' disease occurred at a retirement hotel; Legionella pneumophila serogroup 1 was isolated from an evaporative condenser and from potable water. A case-control study showed that the only significant exposure risk was in area A. L. pneumophila serogroup 1 was isolated during air sampling near the evaporative condenser exhaust site, the air conditioning intake vent, and an air vent in area A, but not in shower stalls. Monoclonal antibody subtype patterns of L. pneumophila serogroup 1 isolates from patients matched those from the evaporative condenser but not from shower water. Air sampling and monoclonal antibody subtyping results support epidemiologic evidence that the evaporative condenser was the source of this outbreak.

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

Numerical investigation of the coagulation mixing between dust and hygroscopic aerosol particles and its impacts

NASA Astrophysics Data System (ADS)

Tsai, I.-Chun; Chen, Jen-Ping; Lin, Yi-Chiu; Chung-Kuang Chou, Charles; Chen, Wei-Nai

2015-05-01

A statistical-numerical aerosol parameterization was incorporated into the Community Multiscale Air Quality modeling system to study the coagulation mixing process focusing on a dust storm event that occurred over East Asia. Simulation results show that the coagulation mixing process tends to decrease aerosol mass, surface area, and number concentrations over the dust source areas. Over the downwind oceanic areas, aerosol concentrations generally increased due to enhanced sedimentation as particles became larger upon coagulation. The mixture process can reduce the overall single-scattering albedo by up to 10% as a result of enhanced core with shell absorption by dust and reduction in the number of scattering particles. The enhanced dry deposition speed also altered the vertical distribution. In addition, the ability of aerosol particles to serve as cloud condensation nuclei (CCN) increased from around 107 m-3 to above 109 m-3 over downwind areas because a large amount of mineral dust particles became effective CCN with solute coating, except over the highly polluted areas where multiple collections of hygroscopic particles by dust in effect reduced CCN number. This CCN effect is much stronger for coagulation mixing than by the uptake of sulfuric acid gas on dust, although the nitric acid gas uptake was not investigated. The ability of dust particles to serve as ice nuclei may decrease or increase at low or high subzero temperatures, respectively, due to the switching from deposition nucleation to immersion freezing or haze freezing.

Collection of Viable Aerosolized Influenza Virus and Other Respiratory Viruses in a Student Health Care Center through Water-Based Condensation Growth

PubMed Central

Pan, Maohua; Bonny, Tania S.; Loeb, Julia; Jiang, Xiao; Eiguren-Fernandez, Arantzazu; Hering, Susanne; Fan, Z. Hugh; Wu, Chang-Yu

2017-01-01

ABSTRACT The dynamics and significance of aerosol transmission of respiratory viruses are still controversial, for the major reasons that virus aerosols are inefficiently collected by commonly used air samplers and that the collected viruses are inactivated by the collection method. Without knowledge of virus viability, infection risk analyses lack accuracy. This pilot study was performed to (i) determine whether infectious (viable) respiratory viruses in aerosols could be collected from air in a real world environment by the viable virus aerosol sampler (VIVAS), (ii) compare and contrast the efficacy of the standard bioaerosol sampler, the BioSampler, with that of the VIVAS for the collection of airborne viruses in a real world environment, and (iii) gain insights for the use of the VIVAS for respiratory virus sampling. The VIVAS operates via a water vapor condensation process to enlarge aerosolized virus particles to facilitate their capture. A variety of viable human respiratory viruses, including influenza A H1N1 and H3N2 viruses and influenza B viruses, were collected by the VIVAS located at least 2 m from seated patients, during a late-onset 2016 influenza virus outbreak. Whereas the BioSampler when operated following our optimized parameters also collected virus aerosols, it was nevertheless overall less successful based on a lower frequency of virus isolation in most cases. This side-by-side comparison highlights some limitations of past studies based on impingement-based sampling, which may have generated false-negative results due to either poor collection efficiency and/or virus inactivation due to the collection process. IMPORTANCE The significance of virus aerosols in the natural transmission of respiratory diseases has been a contentious issue, primarily because it is difficult to collect or sample virus aerosols using currently available air sampling devices. We tested a new air sampler based on water vapor condensation for efficient sampling of

Aerosol properties associated with air masses arriving into the North East Atlantic during the 2008 Mace Head EUCAARI intensive observing period: an overview

NASA Astrophysics Data System (ADS)

Dall'Osto, M.; Ceburnis, D.; Martucci, G.; Bialek, J.; Dupuy, R.; Jennings, S. G.; Berresheim, H.; Wenger, J.; Healy, R.; Facchini, M. C.; Rinaldi, M.; Giulianelli, L.; Finessi, E.; Worsnop, D.; Ehn, M.; Mikkilä, J.; Kulmala, M.; O'Dowd, C. D.

2010-09-01

As part of the EUCAARI Intensive Observing Period, a 4-week campaign to measure aerosol physical, chemical and optical properties, atmospheric structure, and cloud microphysics was conducted from mid-May to mid-June, 2008 at the Mace Head Atmospheric Research Station, located at the interface of Western Europe and the N. E. Atlantic and centered on the west Irish coastline. During the campaign, continental air masses comprising both young and aged continental plumes were encountered, along with polar, Arctic and tropical air masses. Polluted-continental aerosol concentrations were of the order of 3000 cm-3, while background marine air aerosol concentrations were between 400-600 cm-3. The highest marine air concentrations occurred in polar air masses in which a 15 nm nucleation mode, with concentration of 1100 cm-3, was observed and attributed to open ocean particle formation. Continental air submicron chemical composition (excluding refractory sea salt) was dominated by organic matter, closely followed by sulphate mass. Although the concentrations and size distribution spectral shape were almost identical for the young and aged continental cases, hygroscopic growth factors (GF) and cloud condensation nuclei (CCN) to total condensation nuclei (CN) concentration ratios were significantly less in the younger pollution plume, indicating a more oxidized organic component to the aged continental plume. The difference in chemical composition and hygroscopic growth factor appear to result in a 40-50% impact on aerosol scattering coefficients and Aerosol Optical Depth, despite almost identical aerosol microphysical properties in both cases, with the higher values been recorded for the more aged case. For the CCN/CN ratio, the highest ratios were seen in the more age plume. In marine air, sulphate mass dominated the sub-micron component, followed by water soluble organic carbon, which, in turn, was dominated by methanesulphonic acid (MSA). Sulphate concentrations were

Properties of Arctic Aerosol Particles and Residuals of Warm Clouds: Cloud Activation Efficiency and the Aerosol Indirect Effect

NASA Astrophysics Data System (ADS)

Zelenyuk, A.; Imre, D. G.; Leaitch, R.; Ovchinnikov, M.; Liu, P.; Macdonald, A.; Strapp, W.; Ghan, S. J.; Earle, M. E.

2012-12-01

Single particle mass spectrometer, SPLAT II, was used to characterize the size, composition, number concentration, density, and shape of individual Arctic spring aerosol. Background particles, particles above and below the cloud, cloud droplet residuals, and interstitial particles were characterized with goal to identify the properties that separate cloud condensation nuclei (CCN) from background aerosol particles. The analysis offers a comparison between warm clouds formed on clean and polluted days, with clean days having maximum particle concentrations (Na) lower than ~250 cm-3, as compared with polluted days, in which maximum concentration was tenfold higher. On clean days, particles were composed of organics, organics mixed with sulfates, biomass burning (BB), sea salt (SS), and few soot and dust particles. On polluted days, BB, organics associated with BB, and their mixtures with sulfate dominated particle compositions. Based on the measured compositions and size distributions of cloud droplet residuals, background aerosols, and interstitial particles, we conclude that these three particle types had virtually the same compositions, which means that cloud activation probabilities were surprisingly nearly composition independent. Moreover, these conclusions hold in cases in which less than 20% or more than 90% of background particles got activated. We concluded that for the warm clouds interrogated in this study particle size played a more important factor on aerosol CCN activity. Comparative analysis of all studied clouds reveals that aerosol activation efficiency strongly depends on the aerosol concentrations, such that at Na <200 cm-3, nearly all particles activate, and at higher concentrations the activation efficiency is lower. For example, when Na was greater than 1500 cm-3, less than ~30% of particles activated. The data suggest that as the number of nucleated droplets increases, condensation on existing droplets effectively competes with particle

Microphysical processes affecting stratospheric aerosol particles

NASA Technical Reports Server (NTRS)

Hamill, P.; Toon, O. B.; Kiang, C. S.

1977-01-01

Physical processes which affect stratospheric aerosol particles include nucleation, condensation, evaporation, coagulation and sedimentation. Quantitative studies of these mechanisms to determine if they can account for some of the observed properties of the aerosol are carried out. It is shown that the altitude range in which nucleation of sulfuric acid-water solution droplets can take place corresponds to that region of the stratosphere where the aerosol is generally found. Since heterogeneous nucleation is the dominant nucleation mechanism, the stratospheric solution droplets are mainly formed on particles which have been mixed up from the troposphere or injected into the stratosphere by volcanoes or meteorites. Particle growth by heteromolecular condensation can account for the observed increase in mixing ratio of large particles in the stratosphere. Coagulation is important in reducing the number of particles smaller than 0.05 micron radius. Growth by condensation, applied to the mixed nature of the particles, shows that available information is consistent with ammonium sulfate being formed by liquid phase chemical reactions in the aerosol particles. The upper altitude limit of the aerosol layer is probably due to the evaporation of sulfuric acid aerosol particles, while the lower limit is due to mixing across the tropopause.

Aerosol effects on clouds and precipitation over the eastern China

NASA Astrophysics Data System (ADS)

Wang, W. C.; Chen, G.; Song, Y.

2017-12-01

Anthropogenic aerosols (sulfates, nitrates and black carbons) can act as cloud condensation nuclei to regulate cloud droplet number and size, thereby changing cloud radiative properties and atmospheric short- and long-wave radiation. These together with aerosol direct radiative effects in turn alter the circulation with likely effects on the spatial distribution of cloud and precipitation. We conduct WRF model simulations over the eastern China to investigate the aerosol-cloud-climate interactions. In general, more aerosols yield more but smaller cloud droplets and larger cloud water content, whereas the changes of vertical distribution of cloud cover exhibit strong regional variations. For example, the low-cloud fraction and water content increase by more than 10% over the west part of the Yangtze-Huai River Valley (YHRV) and the southeast coastal region, but decrease over the east part of the YHRV, and high-cloud fraction decreases in South and North China but increases in the YHRV. The radiative forcing of aerosols and cloud changes are compared, with focus on the effects of changes of vertical distribution of cloud properties (microphysics and fraction). The precipitation changes are found to be closely associated with the circulation change, which favors more (and longer duration) rainfall over the YHRV but less (and shorter) rainfall over other regions. Details of the circulation change and its associations with clouds and precipitation will be presented.

Uptake of Alkylamines on Dicarboxylic Acids Relevant to Secondary Organic Aerosol Formation

NASA Astrophysics Data System (ADS)

Marrero-Ortiz, W.; Secrest, J.; Zhang, R.

2017-12-01

Aerosols play a critical role in climate directly by scattering and absorbing solar radiation, and indirectly by functioning as cloud condensation nuclei (CCN); both represent the largest uncertainties in climate predictions. New particle formation contributes significantly to CCN production; however, the mechanisms related to particle nucleation and growth processes are not well understood. Organic acids are atmospherically abundant, and their neutralization by low molecular weight amines may result in the formation of stable low volatility aminium salt products contributing to the growth of secondary organic aerosols and even the alteration of the aerosol properties. The acid-base neutralization of particle phase succinic acid and tartaric acid by low molecular weight aliphatic amines, i.e. methylamine, dimethylamine, and trimethylamine, has been investigated by employing a low-pressure fast flow reactor at 298K with an ion drift - chemical ionization mass spectrometer (ID-CIMS). The heterogeneous uptake is time dependent and influenced by organic acids functionality, alkylamines basicity, and steric effect. The implications of our results to atmospheric nanoparticle growth will be discussed.

Urban aerosol hygroscopicity and CCN activity measured during the MAPS-Seoul 2016 campaign

NASA Astrophysics Data System (ADS)

Kim, N.; Park, M.; Yum, S. S.; Kim, D. S.

2016-12-01

While submicron aerosols in atmosphere and their effects on air quality and climate are a rising issue in atmospheric sciences, scientific understanding of them is still limited due to the lack of comprehensive observations. In particular, studies for hygroscopic properties of aerosols, closely related to cloud condensation nuclei (CCN) activity, are essential to aerosol-cloud-interaction study as aerosols can act as CCN, which crucially influence cloud microphysical and radiative properties. Urban aerosol properties were measured at Olympic Park in Seoul, a typical megacity with various anthropogenic sources, during the Megacity Air Pollution Studies (MAPS-Seoul 2016) campaign (9 May- 12 June 2016) for understanding diverse aspects of air quality problem in Korea. Physical properties of aerosols, including aerosol and CCN number concentration, aerosol size distribution and growth factor were measured by CPC, CCNC, SMPS and H-TDMA, respectively. Simultaneously, size-resolved chemical component of aerosol and water-soluble aerosol mass concentration were measured by AMS and PILS-IC. These measurement data are used for comprehensive analysis. A main focus will be on the relationship between overall properties of aerosols and their CCN activity in urban area. Results from MAPS-Seoul 2015 will also be used as reference for comparison with measurements in 2016 campaign. For example, aerosol number concentrations peaked at 0800, 1500 and 2000 LT due to traffic at rush hours and photochemical reaction in the afternoon. This is slightly different from the results of MAPS-Seoul 2015 campaign that showed two dominant peaks in the morning and afternoon.

Collection of Viable Aerosolized Influenza Virus and Other Respiratory Viruses in a Student Health Care Center through Water-Based Condensation Growth.

PubMed

Pan, Maohua; Bonny, Tania S; Loeb, Julia; Jiang, Xiao; Lednicky, John A; Eiguren-Fernandez, Arantzazu; Hering, Susanne; Fan, Z Hugh; Wu, Chang-Yu

2017-01-01

The dynamics and significance of aerosol transmission of respiratory viruses are still controversial, for the major reasons that virus aerosols are inefficiently collected by commonly used air samplers and that the collected viruses are inactivated by the collection method. Without knowledge of virus viability, infection risk analyses lack accuracy. This pilot study was performed to (i) determine whether infectious (viable) respiratory viruses in aerosols could be collected from air in a real world environment by the vi able v irus a erosol s ampler (VIVAS), (ii) compare and contrast the efficacy of the standard bioaerosol sampler, the BioSampler, with that of the VIVAS for the collection of airborne viruses in a real world environment, and (iii) gain insights for the use of the VIVAS for respiratory virus sampling. The VIVAS operates via a water vapor condensation process to enlarge aerosolized virus particles to facilitate their capture. A variety of viable human respiratory viruses, including influenza A H1N1 and H3N2 viruses and influenza B viruses, were collected by the VIVAS located at least 2 m from seated patients, during a late-onset 2016 influenza virus outbreak. Whereas the BioSampler when operated following our optimized parameters also collected virus aerosols, it was nevertheless overall less successful based on a lower frequency of virus isolation in most cases. This side-by-side comparison highlights some limitations of past studies based on impingement-based sampling, which may have generated false-negative results due to either poor collection efficiency and/or virus inactivation due to the collection process. IMPORTANCE The significance of virus aerosols in the natural transmission of respiratory diseases has been a contentious issue, primarily because it is difficult to collect or sample virus aerosols using currently available air sampling devices. We tested a new air sampler based on water vapor condensation for efficient sampling of viable

Seasonal variability of ice nuclei over Central Europe

NASA Astrophysics Data System (ADS)

Klein, Holger; Nickovic, Slobodan; Schuetz, Lothar; Weinbruch, Stephan; Levin, Zev; Andreae, Meinrat; Barrie, Leonard; Ebert, Martin; Bundke, Ulrich; Bingemer, Heinz

2010-05-01

The abundance of ice nuclei (IN) has been measured every day since April 2008 at the Taunus Observatory on Mt. Kleiner Feldberg (50.22°N, 8.45°E, 825 m. above sea level) at 20 km north of Frankfurt / M., Germany. Aerosol samples were collected on silicon wafers by an electrical aerosol precipitator and analyzed for IN number concentration (condensation and deposition freezing modes) using the static vapor diffusion chamber FRIDGE (Klein et al., Atmos. Res, doi:10.1016/j.atmosres.2009.08.002, 2009). Around 800 samples were analyzed so far. The IN number concentration shows a pronounced seasonal signal with about a factor of 10 higher ice nuclei in summer than in winter. Desert dust transported over long distances appears to be the dominant contributor to IN at the site. Episodes of Sahara dust transport are well represented by individual peaks in the IN record and identified by airmass trajectories, transport modelling and mineralogical analysis. The contribution of mineral dust to IN is further corroborated by the covariance of the individual IN concentrations with the aerosol optical depth (AOD) due to extinction by large particles, which was measured simultaneously at the AERONET site (Max-Planck-Institute for Chemistry) at Mainz, 20 km southwest of our site. The relation between IN and AOD not only holds for our individual daily measurements, but is also valid for the monthly means of our IN record, which are highly correlated to the multi-year monthly means of coarse and middle-sized dust AOD which is derived from the Multi-angle Imaging SpectroRadiometer (MISR) satellite instrument (http://eosweb.larc.nasa.gov/cgi-bin/misr_tools/clim_likely.cgi ) for the grid point closest to our site. Acknowledgements: We gratefully acknowledge funding of this work by the Deutsche Forschungsgemeinschaft (DFG) as part of the collaborative research centre Die troposphärische Eisphase (SFB641) and by the German-Israeli Foundation (GIF).

Aerosol measurements in the winter/spring Antarctic stratosphere. I - Correlative measurements with ozone. II - Impact on polar stratospheric cloud theories

NASA Technical Reports Server (NTRS)

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

1988-01-01

Aerosol measurements collected from August 25-November 3, 1986 at McMurdo Station using balloon-borne optical particle counters are examined in order to study the relationship between aerosol and ozone distribution and the formation of polar stratospheric clouds (PSCs). Ozone, aerosol, and condensation nuclei profiles, and pressure, temperature, and humidity measurements are analyzed. It is observed that the height of the stratospheric sulfate layer decreases over the period of measurement suggesting that upwelling in the votex is not important in the zone depletion process. Three theories on PSC formation are described, and the effects of the aerosol measurements on the theories are considered. The three theories are: (1) the original theory of water vapor pressure over a solution of H2SO4 of Steele et al. (1983) and Hamill and Mc Master (1984); (2) the nitric acid theory of PSCs of Toon et al. (1986) and Hamill et al. (1986); and (3) the quasi-cirrus cloud theory of Heymsfield (1986).

Simulating Aerosol Size Distribution and Mass Concentration with Simultaneous Nucleation, Condensation/Coagulation, and Deposition with the GRAPES-CUACE

NASA Astrophysics Data System (ADS)

Zhou, Chunhong; Shen, Xiaojing; Liu, Zirui; Zhang, Yangmei; Xin, Jinyuan

2018-04-01

A coupled aerosol-cloud model is essential for investigating the formation of haze and fog and the interaction of aerosols with clouds and precipitation. One of the key tasks of such a model is to produce correct mass and number size distributions of aerosols. In this paper, a parameterization scheme for aerosol size distribution in initial emission, which took into account the measured mass and number size distributions of aerosols, was developed in the GRAPES-CUACE [Global/Regional Assimilation and PrEdiction System-China Meteorological Administration (CMA) Unified Atmospheric Chemistry Environment model]—an online chemical weather forecast system that contains microphysical processes and emission, transport, and chemical conversion of sectional multi-component aerosols. In addition, the competitive mechanism between nucleation and condensation for secondary aerosol formation was improved, and the dry deposition was also modified to be in consistent with the real depositing length. Based on the above improvements, the GRAPES-CUACE simulations were verified against observational data during 1-31 January 2013, when a series of heavy regional haze-fog events occurred in eastern China. The results show that the aerosol number size distribution from the improved experiment was much closer to the observation, whereas in the old experiment the number concentration was higher in the nucleation mode and lower in the accumulation mode. Meanwhile, the errors in aerosol number size distribution as diagnosed by its sectional mass size distribution were also reduced. Moreover, simulations of organic carbon, sulfate, and other aerosol components were improved and the overestimation as well as underestimation of PM2.5 concentration in eastern China was significantly reduced, leading to increased correlation coefficient between simulated and observed PM2.5 by more than 70%. In the remote areas where bad simulation results were produced previously, the correlation coefficient

Effects of Ocean Ecosystem on Marine Aerosol-Cloud Interaction

DOE Office of Scientific and Technical Information (OSTI.GOV)

Meskhidze, Nicholas; Nenes, Athanasios

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

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

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.;

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

NASA Astrophysics Data System (ADS)

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

2014-06-01

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

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

NASA Astrophysics Data System (ADS)

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

2016-01-01

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

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.

Evidence for the existence of supercooled ethane droplets under conditions prevalent in Titan's atmosphere.

PubMed

Sigurbjörnsson, Omar F; Signorell, Ruth

2008-11-07

Recent evidence for ethane clouds and condensation in Titan's atmosphere raise the question whether liquid ethane condensation nuclei and supercooled liquid ethane droplets exist under the prevalent conditions. We present laboratory studies on the phase behaviour of pure ethane aerosols and ethane aerosols formed in the presence of other ice nuclei under conditions relevant to Titan's atmosphere. Combining bath gas cooling with infrared spectroscopy, we find evidence for the existence of supercooled liquid ethane aerosol droplets. The observed homogeneous freezing rates imply that supercooled ethane could be a long-lived species in ethane-rich regions of Titan's atmosphere similar to supercooled water in the Earth's atmosphere.

Intercomparison of aerosol-cloud-precipitation interactions in stratiform orographic mixed-phase clouds

NASA Astrophysics Data System (ADS)

Muhlbauer, A.; Hashino, T.; Xue, L.; Teller, A.; Lohmann, U.; Rasmussen, R. M.; Geresdi, I.; Pan, Z.

2010-09-01

Anthropogenic aerosols serve as a source of both cloud condensation nuclei (CCN) and ice nuclei (IN) and affect microphysical properties of clouds. Increasing aerosol number concentrations is hypothesized to retard the cloud droplet coalescence and the riming in mixed-phase clouds, thereby decreasing orographic precipitation. This study presents results from a model intercomparison of 2-D simulations of aerosol-cloud-precipitation interactions in stratiform orographic mixed-phase clouds. The sensitivity of orographic precipitation to changes in the aerosol number concentrations is analysed and compared for various dynamical and thermodynamical situations. Furthermore, the sensitivities of microphysical processes such as coalescence, aggregation, riming and diffusional growth to changes in the aerosol number concentrations are evaluated and compared. The participating numerical models are the model from the Consortium for Small-Scale Modeling (COSMO) with bulk microphysics, the Weather Research and Forecasting (WRF) model with bin microphysics and the University of Wisconsin modeling system (UWNMS) with a spectral ice habit prediction microphysics scheme. All models are operated on a cloud-resolving scale with 2 km horizontal grid spacing. The results of the model intercomparison suggest that the sensitivity of orographic precipitation to aerosol modifications varies greatly from case to case and from model to model. Neither a precipitation decrease nor a precipitation increase is found robustly in all simulations. Qualitative robust results can only be found for a subset of the simulations but even then quantitative agreement is scarce. Estimates of the aerosol effect on orographic precipitation are found to range from -19% to 0% depending on the simulated case and the model. Similarly, riming is shown to decrease in some cases and models whereas it increases in others, which implies that a decrease in riming with increasing aerosol load is not a robust result

Laboratory Experiments and Instrument Intercomparison Studies of Carbonaceous Aerosol Particles

DOE Office of Scientific and Technical Information (OSTI.GOV)

Davidovits, Paul

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 andmore » 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

Implementation of warm-cloud processes in a source-oriented WRF/Chem model to study the effect of aerosol mixing state on fog formation in the Central Valley of California

NASA Astrophysics Data System (ADS)

Lee, Hsiang-He; Chen, Shu-Hua; Kleeman, Michael J.; Zhang, Hongliang; DeNero, Steven P.; Joe, David K.

2016-07-01

The source-oriented Weather Research and Forecasting chemistry model (SOWC) was modified to include warm cloud processes and was applied to investigate how aerosol mixing states influence fog formation and optical properties in the atmosphere. SOWC tracks a 6-D chemical variable (X, Z, Y, size bins, source types, species) through an explicit simulation of atmospheric chemistry and physics. A source-oriented cloud condensation nuclei module was implemented into the SOWC model to simulate warm clouds using the modified two-moment Purdue Lin microphysics scheme. The Goddard shortwave and long-wave radiation schemes were modified to interact with source-oriented aerosols and cloud droplets so that aerosol direct and indirect effects could be studied. The enhanced SOWC model was applied to study a fog event that occurred on 17 January 2011, in the Central Valley of California. Tule fog occurred because an atmospheric river effectively advected high moisture into the Central Valley and nighttime drainage flow brought cold air from mountains into the valley. The SOWC model produced reasonable liquid water path, spatial distribution and duration of fog events. The inclusion of aerosol-radiation interaction only slightly modified simulation results since cloud optical thickness dominated the radiation budget in fog events. The source-oriented mixture representation of particles reduced cloud droplet number relative to the internal mixture approach that artificially coats hydrophobic particles with hygroscopic components. The fraction of aerosols activating into cloud condensation nuclei (CCN) at a supersaturation of 0.5 % in the Central Valley decreased from 94 % in the internal mixture model to 80 % in the source-oriented model. This increased surface energy flux by 3-5 W m-2 and surface temperature by as much as 0.25 K in the daytime.

Spatio-temporal aerosol particle distributions in the UT/LMS measured by the IAGOS-CARIBIC Observatory

NASA Astrophysics Data System (ADS)

Assmann, D. N.; Hermann, M.; Weigelt, A.; Martinsson, B. G.; Brenninkmeijer, C. A. M.; Rauthe-Schoech, A.; van Velthoven, P. J. F.; Boenisch, H.; Zahn, A.

2016-12-01

Submicrometer aerosol particles in the upper troposphere and lowermost stratosphere (UT/LMS) influence the Earth`s radiation budget directly and, more important, indirectly, by acting as cloud condensation nuclei and by changing trace gas concentrations through heterogeneous chemical processes. Since 1997, regular in situ UT/LMS aerosol particle measurements have been conducted by the Leibniz Institute for Tropospheric Research, Leipzig, Germany and the University of Lund, Sweden, using the the CARIBIC (now IAGOS-CARIBIC) observatory (www.caribic-atmospheric.com) onboard a passenger aircraft. Submicrometer aerosol particle number concentrations and the aerosol particle size distribution are measured using three condensation particle counters and one optical particle size spectrometer. Moreover, particle elemental composition is determined using an aerosol impactor sampler and post-flight ion beam analysis (PIXE, PESA) of the samples in the laboratory. Based on this unique data set, including meteorological analysis, we present representative spatio-temporal distributions of particle number, surface, volume, and elemental concentrations in an altitude of 8-12 km covering a large fraction of the northern hemisphere. We discuss the measured values in the different size regimes with respect to sources and sinks in different regions. Additionally, we calculated highly resolved latitudinal and longitudinal cross sections of the particle number size distribution, probability density functions and trends in particle number concentrations, but also in elemental composition, determined from our regular measurements over more than a decade. Moreover, we present the seasonality of particle number concentration in an equivelent latitude - potential temperature coordinate framework (see figure). The results are interpreted with respect to aerosol microphysics and transport using CARIBIC trace gas data like ozone and water vapour. The influence of clouds in the troposphere and

Biogenic influence on the composition and growth of summertime Arctic aerosol

NASA Astrophysics Data System (ADS)

Willis, M. D.; Burkart, J.; Thomas, J. L.; Koellner, F.; Schneider, J.; Bozem, H.; Hoor, P. M.; Aliabadi, A. A.; Schulz, H.; Herber, A. B.; Leaitch, R.; Abbatt, J.

2016-12-01

The summertime Arctic lower troposphere is a relatively pristine background aerosol environment dominated by nucleation and Aitken mode particles. Understanding the mechanisms that control the formation and growth of aerosol is crucial for our ability to predict cloud properties and therefore radiative balance and climate. We present aircraft-based observations of submicron aerosol composition from an aerosol mass spectrometer made during the NETCARE 2014 summertime arctic campaign, based in the Canadian High Arctic, at Resolute Bay, NU (74°N). Under stable and regionally influenced atmospheric conditions with low carbon monoxide and black carbon concentrations (< 100 ppbv and < 50 ng/m3, respectively), we observed organic aerosol (OA)-to-sulfate ratios ranging from 0.5 to > 6 with evidence for enhancement within the lower boundary layer. Methanesulfonic acid (MSA), a marker for the contribution of ocean-derived biogenic sulphur, was also observed in submicron aerosol. MSA-to-sulfate ratios ranged from near zero to 0.3 and tended to increase within the lower boundary layer, suggesting a contribution to aerosol loading from the ocean. In one notable case while flying in the lower boundary layer above open water in Lancaster Sound, we observed growth of small particles, <20 nm in diameter, into sizes above 50 nm. Aerosol growth was correlated with the presence of organic species, trimethylamine, and MSA in particles 80 nm and larger, where the organics were similar to those previously observed in marine settings. The organic-rich aerosol contributed significantly to particles active as cloud condensation nuclei (CCN, supersaturation = 0.6%). Our results highlight the potential importance of secondary organic aerosol formation and its role in growing nucleation mode aerosol into CCN-active sizes in this remote marine environment.

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.

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

NASA Astrophysics Data System (ADS)

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

2014-09-01

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

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

Matsui, H.; Koike, Makoto; Kondo, Yutaka

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 particlesmore » 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

Secondary Organic Aerosol Formation in the Captive Aerosol Growth and Evolution (CAGE) Chambers during the Southern Oxidant and Aerosol Study (SOAS) in Centreville, AL

NASA Astrophysics Data System (ADS)

Leong, Y.; Karakurt Cevik, B.; Hernandez, C.; Griffin, R. J.; Taylor, N.; Matus, J.; Collins, D. R.

2013-12-01

Secondary organic aerosol (SOA) represents a large portion of sub-micron particulate matter on a global scale. The composition of SOA and its formation processes are heavily influenced by anthropogenic and biogenic activity. Volatile organic compounds (VOCs) that are emitted naturally from forests or from human activity serve as precursors to SOA formation. Biogenic SOA (BSOA) is formed from biogenic VOCs and is prevalent in forested regions like the Southeastern United States. The formation and enhancement of BSOA under anthropogenic influences such as nitrogen oxides (NOx), sulfur dioxide (SO2), and oxygen radicals are still not well understood. The lack of information on anthropogenic BSOA enhancement and the reversibility of SOA formation could explain the underprediction of SOA in current models. To address some of these gaps in knowledge, this study was conducted as part of the Southern Oxidant and Aerosol Study (SOAS) in Centreville, AL during the summer of 2013. SOA growth experiments were conducted in two Captive Aerosol Growth and Evolution (CAGE) outdoor chambers located at the SEARCH site. Ambient trace gas concentrations were maintained in these chambers using semi-permeable gas-exchange membranes, while studying the growth of injected monodisperse seed aerosol. The control chamber was operated under ambient conditions; the relative humidity and oxidant and NOx levels were perturbed in the second chamber. This design allows experiments to capture the natural BSOA formation processes in the southeastern atmosphere and to study the influence of anthropogenic activity on aerosol chemistry. Chamber experiments were periodically monitored with physical and chemical instrumentation including a scanning mobility particle sizer (SMPS), a cloud condensation nuclei counter (CCNC), a humidified tandem differential mobility analyzer (H-TDMA), and an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). The CAGE experiments focused on SOA

Aerosol effect on cloud droplet size as monitored from surface-based remote sensing over East China Sea region

NASA Astrophysics Data System (ADS)

Pandithurai, G.; Takamura, T.; Yamaguchi, J.; Miyagi, K.; Takano, T.; Ishizaka, Y.; Dipu, S.; Shimizu, A.

2009-07-01

The effect of increased aerosol concentrations on the low-level, non-precipitating, ice-free stratus clouds is examined using a suite of surface-based remote sensing systems. Cloud droplet effective radius and liquid water path are retrieved using cloud radar and microwave radiometer. Collocated measurements of aerosol scattering coefficient, size distribution and cloud condensation nuclei (CCN) concentrations were used to examine the response of cloud droplet size and optical thickness to increased CCN proxies. During the episodic events of increase in aerosol accumulation-mode volume distribution, the decrease in droplet size and increase in cloud optical thickness is observed. The indirect effect estimates are made for both droplet effective radius and cloud optical thickness for different liquid water path ranges and they range 0.02-0.18 and 0.005-0.154, respectively. Data are also categorized into thin and thick clouds based on cloud geometric thickness (Δz) and estimates show IE values are relatively higher for thicker clouds.

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.

Intercomparison of aerosol-cloud-precipitation interactions in stratiform orographic mixed-phase clouds

NASA Astrophysics Data System (ADS)

Muhlbauer, A.; Hashino, T.; Xue, L.; Teller, A.; Lohmann, U.; Rasmussen, R. M.; Geresdi, I.; Pan, Z.

2010-04-01

Anthropogenic aerosols serve as a source of both cloud condensation nuclei (CCN) and ice nuclei (IN) and affect microphysical properties of clouds. Increasing aerosol number concentrations is hypothesized to retard the cloud droplet collision/coalescence and the riming in mixed-phase clouds, thereby decreasing orographic precipitation. This study presents results from a model intercomparison of 2-D simulations of aerosol-cloud-precipitation interactions in stratiform orographic mixed-phase clouds. The sensitivity of orographic precipitation to changes in the aerosol number concentrations is analyzed and compared for various dynamical and thermodynamical situations. Furthermore, the sensitivities of microphysical processes such as collision/coalescence, aggregation and riming to changes in the aerosol number concentrations are evaluated and compared. The participating models are the Consortium for Small-Scale Modeling's (COSMO) model with bulk-microphysics, the Weather Research and Forecasting (WRF) model with bin-microphysics and the University of Wisconsin modeling system (UWNMS) with a spectral ice-habit prediction microphysics scheme. All models are operated on a cloud-resolving scale with 2 km horizontal grid spacing. The results of the model intercomparison suggest that the sensitivity of orographic precipitation to aerosol modifications varies greatly from case to case and from model to model. Neither a precipitation decrease nor a precipitation increase is found robustly in all simulations. Qualitative robust results can only be found for a subset of the simulations but even then quantitative agreement is scarce. Estimates of the second indirect aerosol effect on orographic precipitation are found to range from -19% to 0% depending on the simulated case and the model. Similarly, riming is shown to decrease in some cases and models whereas it increases in others which implies that a decrease in riming with increasing aerosol load is not a robust result

Aerosol properties associated with air masses arriving into the North East Atlantic during the 2008 Mace Head EUCAARI intensive observing period: an overview

NASA Astrophysics Data System (ADS)

Dall'Osto, M.; Ceburnis, D.; Martucci, G.; Bialek, J.; Dupuy, R.; Jennings, S. G.; Berresheim, H.; Wenger, J. C.; Sodeau, J. R.; Healy, R. M.; Facchini, M. C.; Rinaldi, M.; Giulianelli, L.; Finessi, E.; Worsnop, D.; O'Dowd, C. D.

2009-12-01

As part of the EUCAARI Intensive Observing Period, a 4-week campaign to measure aerosol physical, chemical and optical properties, atmospheric structure, and cloud microphysics was conducted from mid-May to mid-June 2008 at the Mace Head Atmospheric Research Station, located at the interface of Western Europe and the NE Atlantic and centered on the west Irish coastline. During the campaign, continental air masses comprising both young and aged continental plumes were encountered, along with polar, Arctic and tropical air masses. Polluted-continental aerosol concentrations were of the order of 3000 cm-3, while background marine air aerosol concentrations were between 400-600 cm-3. The highest marine air concentrations occurred in polar air masses in which a 15 nm nucleation mode, with concentration of 1100 cm-3, was observed and attributed to open ocean particle formation. Black carbon concentrations in polluted air were between 300-400 ng m-3, and in clean marine air were less than 50 ng m-3. Continental air submicron chemical composition (excluding refractory sea salt) was dominated by organic matter, closely followed by sulphate mass. Although the concentrations and size distribution spectral shape were almost identical for the young and aged continental cases, hygroscopic growth factors (GF) and cloud condensation nuclei (CCN) to total condensation nuclei (CN) concentration ratios were significantly less in the younger pollution plume, indicating a more oxidized organic component to the aged continental plume. The difference in chemical composition and hygroscopic growth factor appear to result in a 40-50% impact on aerosol scattering coefficients and Aerosol Optical Depth, despite almost identical aerosol microphysical properties in both cases, with the higher values been recorded for the more aged case. For the CCN/CN ratio, the highest ratios were seen in the more age plume. In marine air, sulphate mass dominated the sub-micron component, followed by water

The Global Atmosphere Watch Aerosol Programme

NASA Astrophysics Data System (ADS)

Baltensperger, U.

2003-04-01

The Global Atmosphere Watch (GAW) programme is a WMO sponsored activity and currently supported by about 80 WMO member countries. It is the goal of GAW to develop and maintain long-term measurements of atmospheric constituents in order to detect trends, develop aerosol predictive capabilities and understand proc- esses. With respect to aerosols, the objective of GAW is to support a global network determining the spatio-temporal distribution of aerosol properties related to climate forcing and air quality up to multi-decadal time scales. The GAW network consists of 22 Global stations and some 300 Regional stations. The Scientific Advisory Group (SAG) for Aerosols will soon publish their recommendations for aerosol measurements. Each site should have an acceptable aerosol sampling inlet. Regional stations measure aerosol optical depth, as well as the aerosol light scattering and absorption coefficient. If possible these should be complemented by routine mass concentration and composition measurements in two aerosol size fractions. At Global stations, a larger number of measurements are desirable. These include the Regional parameters list above as well as the light scattering, hemispheric backscat- tering, and absorption coefficients at various wavelengths, aerosol number concen- tration, cloud condensation nuclei (CCN) concentration at 0.5% supersaturation, and diffuse, global and direct solar radiation. Additional parameters such as the aerosol size distribution, detailed size fractionated chemical composition, dependence of aerosol properties on relative humidity, CCN concentration at various supersatura- tions, and the vertical distribution of aerosol properties should be measured intermit- tently at Global stations. Examples from the Jungfraujoch (Swiss Alps, 3580 m asl) will be given, where many of the parameters listed above are measured. Data are delivered to and made available by the World Data Centre for Aerosols (WDCA, located in Ispra, Italy http

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.

The case against climate regulation via oceanic phytoplankton sulphur emissions.

PubMed

Quinn, P K; Bates, T S

2011-11-30

More than twenty years ago, a biological regulation of climate was proposed whereby emissions of dimethyl sulphide from oceanic phytoplankton resulted in the formation of aerosol particles that acted as cloud condensation nuclei in the marine boundary layer. In this hypothesis--referred to as CLAW--the increase in cloud condensation nuclei led to an increase in cloud albedo with the resulting changes in temperature and radiation initiating a climate feedback altering dimethyl sulphide emissions from phytoplankton. Over the past two decades, observations in the marine boundary layer, laboratory studies and modelling efforts have been conducted seeking evidence for the CLAW hypothesis. The results indicate that a dimethyl sulphide biological control over cloud condensation nuclei probably does not exist and that sources of these nuclei to the marine boundary layer and the response of clouds to changes in aerosol are much more complex than was recognized twenty years ago. These results indicate that it is time to retire the CLAW hypothesis.

Reactive Heterogeneous Chemistry on Organic Aerosols: Two Case Studies

NASA Astrophysics Data System (ADS)

Abbatt, J.; Braban, C.; Broekhuizen, K.; Thornberry, T.; Thornton, J.

2003-12-01

Two sets of laboratory studies will be discussed to illustrate the impact that heterogeneous chemistry involving tropospheric organic aerosols may have on both the gas-phase composition of the atmosphere and the chemical nature of the particles themselves. In the first case, the reactive uptake coefficient for the hydrolysis of dinitrogen pentoxide (N2O5) on organic aerosols has been measured in an entrained aerosol flow tube coupled to a Chemical-Ionization Mass Spectrometer (CIMS). The general observation is that the reaction on aqueous malonic acid aerosols behaves in an analogous manner to that on aqueous inorganic salts, i.e. the uptake coefficient shows a linear dependence on the particle water content up to 50% relative humidity (RH), at which point the effect saturates. In addition, there is evidence for the kinetics being dependent on both the size of the particles and the levels of dissolved nitrate. By contrast, the N2O5 hydrolysis kinetics on solid azelaic acid particles are too slow to be atmospherically significant, even at 85% RH. In the second case, the kinetics and product yields from the oxidation of liquid oleic acid by ozone have been studied in considerable detail, with emphasis on the quantification of gas-phase products (nonanal) by CIMS and water-soluble species by HPLC/Electrospray-Ionization Mass Spectrometry (azelaic acid, nonanoic acid). The atmospheric importance of these results will be discussed, in particular with respect to the role of organic aerosol oxidation as a source of cloud condensation nuclei.

Carbonaceous Aerosol Removal During Precipitation Events: Climate Implications

NASA Astrophysics Data System (ADS)

Gaffney, J. S.; Marley, N. A.; Bridges, G. L.; Marchany-Rivera, A.; Begum, M.

2009-12-01

Atmospheric aerosols and their links to clouds are one of the main focus areas of the Department of Energy’s Atmospheric Systems Research, due to the fact that aerosols and clouds constitute the major uncertainties in radiative forcing that need to be reduced for more accurate modeling of climate, particularly regional climate. The impact of absorbing aerosols on radiative balance of the atmosphere will depend on their atmospheric lifetimes as well as their UV-visible absorption profiles. Aerosol lifetimes depend on the aerosols ability to take up water and grow to sufficient size to be either removed by gravitational settling or to act as cloud condensation nuclei and be removed by precipitation scavenging. The investigation of uv-visible absorbing aerosols is underway using a seven-channel aethalometer to evaluate the change in aerosol optical absorption during precipitation events. Angstrom absorption exponents (AAEs) are determined before, during, and after rain events to examine the impact on the aerosol absorption profiles anticipated by removal of the water soluble short-wave absorbing species (i.e. HULIS) that can be produced by photochemical oxidation of biogenic emissions (isoprene, monoterpenes, sesquiterpenes). Aerosol absorption data are presented from observations made at the University of Arkansas at Little Rock and other sites, which clearly show that a significant amount of absorbing carbon is not removed during rain events, and that the organic matter removed is likely secondary organics produced from biogenic precursors. The dissolved organic carbon measured in precipitation samples along with determinations of natural radionuclide tracers are also used to help examine the extent of carbonaceous aerosol removal by precipitation. The data are discussed in terms of the potential impacts of anthropogenic enhancement of aerosol absorption by secondary organic aerosols adding to atmospheric heating and changes in atmospheric dynamics. The potential

Cloud condensation nucleus activity of internally mixed ammonium sulfate/organic acid aerosol particles

NASA Astrophysics Data System (ADS)

Abbatt, J. P. D.; Broekhuizen, K.; Pradeep Kumar, P.

The ability of mixed ammonium sulfate/organic acid particles to act as cloud condensation nuclei (CCN) has been studied in the laboratory using a continuous flow, thermal-gradient diffusion chamber operated at supersaturations between 0.3% and 0.6%. The organic acids studied were malonic acid, azelaic acid, hexanoic acid, cis-pinonic acid, oleic acid and stearic acid, and the particles were largely prepared by condensation of the organic vapor onto a dry ammonium sulfate core. For malonic acid and hexanoic acid, the mixed particles activated as predicted by a simple Köhler theory model where both species are assumed to be fully soluble and the droplet has the surface tension of water. Three low-solubility species, cis-pinonic acid, azelaic acid and oleic acid, are well modeled where the acid was assumed to be either partially or fully insoluble. Interestingly, although thin coats of stearic acid behaved in a manner similar to that displayed by oleic and cis-pinonic acid, we observed that thick coats led to a complete deactivation of the ammonium sulfate, presumably because the water vapor could not diffuse through the solid stearic acid. We observed no CCN behavior that could be clearly attributed to a lowering of the surface tension of the growing droplet by the presence of the organic constituents, some of which are highly surface active.

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

The function and response of an improved stratospheric condensation nucleus counter

NASA Technical Reports Server (NTRS)

Wilson, J. C.; Hyun, J. H.; Blackshear, E. D.

1983-01-01

An improved condensation nucleus counter (CNC) for use in the stratosphere is described. The University of Minnesota CNC (UMCNC) has a sequential saturator and condenser and uses n-butyl alcohol as the working fluid. The use of a coaxial saturator flow, with aerosol in the center and filtered, alcohol-laden air around it, speeds the response of this instrument and improves its stability as pressure changes. The counting efficiency has been studied as a function of particle size and pressure. The UMCNC provides an accurate measure of submicron aerosol concentration as long as the number distribution is not dominated by sub-0.02 micron diameter aerosol. The response of the UMCNC is compared with that of other stratospheric condensation nucleus counters, and the results of a (near) comparison with a balloon-borne condensation nucleus counter are presented. The UMCNC has operated 14 times on a NASA U-2 aircraft at altitudes from 8 to 21.5 km.

Reduced anthropogenic aerosol radiative forcing caused by biogenic new particle formation

NASA Astrophysics Data System (ADS)

Gordon, Hamish; Sengupta, Kamalika; Rap, Alexandru; Duplissy, Jonathan; Frege, Carla; Williamson, Christina; Heinritzi, Martin; Simon, Mario; Yan, Chao; Almeida, João; Tröstl, Jasmin; Nieminen, Tuomo; Ortega, Ismael K.; Wagner, Robert; Dunne, Eimear M.; Adamov, Alexey; Amorim, Antonio; Bernhammer, Anne-Kathrin; Bianchi, Federico; Breitenlechner, Martin; Brilke, Sophia; Chen, Xuemeng; Craven, Jill S.; Dias, Antonio; Ehrhart, Sebastian; Fischer, Lukas; Flagan, Richard C.; Franchin, Alessandro; Fuchs, Claudia; Guida, Roberto; Hakala, Jani; Hoyle, Christopher R.; Jokinen, Tuija; Junninen, Heikki; Kangasluoma, Juha; Kim, Jaeseok; Kirkby, Jasper; Krapf, Manuel; Kürten, Andreas; Laaksonen, Ari; Lehtipalo, Katrianne; Makhmutov, Vladimir; Mathot, Serge; Molteni, Ugo; Monks, Sarah A.; Onnela, Antti; Peräkylä, Otso; Piel, Felix; Petäjä, Tuukka; Praplan, Arnaud P.; Pringle, Kirsty J.; Richards, Nigel A. D.; Rissanen, Matti P.; Rondo, Linda; Sarnela, Nina; Schobesberger, Siegfried; Scott, Catherine E.; Seinfeld, John H.; Sharma, Sangeeta; Sipilä, Mikko; Steiner, Gerhard; Stozhkov, Yuri; Stratmann, Frank; Tomé, Antonio; Virtanen, Annele; Vogel, Alexander Lucas; Wagner, Andrea C.; Wagner, Paul E.; Weingartner, Ernest; Wimmer, Daniela; Winkler, Paul M.; Ye, Penglin; Zhang, Xuan; Hansel, Armin; Dommen, Josef; Donahue, Neil M.; Worsnop, Douglas R.; Baltensperger, Urs; Kulmala, Markku; Curtius, Joachim; Carslaw, Kenneth S.

2016-10-01

The magnitude of aerosol radiative forcing caused by anthropogenic emissions depends on the baseline state of the atmosphere under pristine preindustrial conditions. Measurements show that particle formation in atmospheric conditions can occur solely from biogenic vapors. Here, we evaluate the potential effect of this source of particles on preindustrial cloud condensation nuclei (CCN) concentrations and aerosol-cloud radiative forcing over the industrial period. Model simulations show that the pure biogenic particle formation mechanism has a much larger relative effect on CCN concentrations in the preindustrial atmosphere than in the present atmosphere because of the lower aerosol concentrations. Consequently, preindustrial cloud albedo is increased more than under present day conditions, and therefore the cooling forcing of anthropogenic aerosols is reduced. The mechanism increases CCN concentrations by 20-100% over a large fraction of the preindustrial lower atmosphere, and the magnitude of annual global mean radiative forcing caused by changes of cloud albedo since 1750 is reduced by 0.22 W m-2 (27%) to -0.60 W m-2. Model uncertainties, relatively slow formation rates, and limited available ambient measurements make it difficult to establish the significance of a mechanism that has its dominant effect under preindustrial conditions. Our simulations predict more particle formation in the Amazon than is observed. However, the first observation of pure organic nucleation has now been reported for the free troposphere. Given the potentially significant effect on anthropogenic forcing, effort should be made to better understand such naturally driven aerosol processes.

Hygroscopicity of Early Earth and Titan Laboratory Aerosol Analogs

NASA Astrophysics Data System (ADS)

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

2009-12-01

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

Evidence for Limited Indirect Aerosol Forcing in Stratocumulus

NASA Technical Reports Server (NTRS)

Ackerman, Andrew S.; Toon, O. B.; Stevens, D. E.

2003-01-01

Increases in cloud cover and condensed water contribute more than half of the indirect aerosol effect in an ensemble of general circulation model (GCM) simulations estimating the global radiative forcing of anthropogenic aerosols. We use detailed simulations of marine stratocumulus clouds and airborne observations of ship tracks to show that increases in cloud cover and condensed water in reality are far less than represented by the GCM ensemble. Our results offer an explanation for recent simplified inverse climate calculations indicating that indirect aerosol effects are greatly exaggerated in GCMs.

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

Sea Spray Aerosol Production in the North Atlantic: A Comparison from 4 Cruises in 3 Seasons

NASA Astrophysics Data System (ADS)

Bates, T. S.; Quinn, P.

2016-12-01

Breaking waves on the ocean surface generate air bubbles that scavenge organic matter from the surrounding seawater. When injected into the atmosphere, these bubbles burst, yielding sea spray aerosol (SSA), a mixture of organic and inorganic compounds with the organic matter enriched relative to seawater. SSA mass is well documented as the dominant component of aerosol light scattering over the remote oceans. The importance of SSA number to marine boundary layer cloud condensation nuclei (CCN) is much less certain. During the Western Atlantic Climate Study cruises (WACS-1 - August 2012 and WACS-2 - May-June 2014) and the North Atlantic Aerosols and Marine Ecosystem Study cruises (NAAMES-1 - November 2015, NAAMES-2 - May 2016, and NAAMES-3 - September 2017), we generated and measured freshly emitted SSA using the Sea Sweep SSA generator. During the 2017 cruise we also generated SSA with a Marine Aerosol Reference Tank (MART). Using the data generated on these 5 cruises and a large database of remote marine boundary layer aerosol measurements we will address three questions during this presentation: 1 - Do phytoplankton ecosystems affect the organic enrichment of freshly emitted SSA?, 2 - Do plankton ecosystems affect the number production flux of SSA?, and 3 - Is SSA a significant source of atmospheric CCN?

Contact ice nucleation by submicron atmospheric aerosols

NASA Technical Reports Server (NTRS)

Deshler, T.

1982-01-01

An apparatus designed to measure the concentrations of submicron contact ice nuclei is described. Here, natural forces transfer nuclei to supercooled sample drops suspended in an aerosol stream. Experimental measurements of the scavenging rate of the sample drops for several humidities and aerosol sizes are found to be in agreement with theory to within a factor of two. This fact, together with the statistical tests showing a difference between the data and control samples, is seen as indicating that a reliable measurement of the concentrations of submicron contact ice nuclei has been effected. A figure is included showing the ice nucleus concentrations as a function of temperature and assumed aerosol radius. For a 0.01 micron radius, the average is 1/liter at -15 C and 3/liter at -18 C. It is noted that the measurements are in fair agreement with ice crystal concentrations in stable winter clouds measured over Elk Mountain, WY (Vali et al., 1982).

Growth rates of fine aerosol particles at a site near Beijing in June 2013

NASA Astrophysics Data System (ADS)

Zhao, Chuanfeng; Li, Yanan; Zhang, Fang; Sun, Yele; Wang, Pucai

2018-02-01

Growth of fine aerosol particles is investigated during the Aerosol-CCN-Cloud Closure Experiment campaign in June 2013 at an urban site near Beijing. Analyses show a high frequency (˜ 50%) of fine aerosol particle growth events, and show that the growth rates range from 2.1 to 6.5 nm h-1 with a mean value of ˜ 5.1 nm h-1. A review of previous studies indicates that at least four mechanisms can affect the growth of fine aerosol particles: vapor condensation, intramodal coagulation, extramodal coagulation, and multi-phase chemical reaction. At the initial stage of fine aerosol particle growth, condensational growth usually plays a major role and coagulation efficiency generally increases with particle sizes. An overview of previous studies shows higher growth rates over megacity, urban and boreal forest regions than over rural and oceanic regions. This is most likely due to the higher condensational vapor, which can cause strong condensational growth of fine aerosol particles. Associated with these multiple factors of influence, there are large uncertainties for the aerosol particle growth rates, even at the same location.

Characteristics of regional aerosols: Southern Arizona and eastern Pacific Ocean

NASA Astrophysics Data System (ADS)

Prabhakar, Gouri

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

Aerosol Generation by Modern Flush Toilets.

PubMed

Johnson, David; Lynch, Robert; Marshall, Charles; Mead, Kenneth; Hirst, Deborah

A microbe-contaminated toilet will produce bioaerosols when flushed. We assessed toilet plume aerosol from high efficiency (HET), pressure-assisted high efficiency (PAT), and flushometer (FOM) toilets with similar bowl water and flush volumes. Total and droplet nuclei "bioaerosols" were assessed. Monodisperse 0.25-1.9- μ m fluorescent microspheres served as microbe surrogates in separate trials in a mockup 5 m 3 water closet (WC). Bowl water seeding was approximately 10 12 particles/mL. Droplet nuclei were sampled onto 0.2- μ m pore size mixed cellulose ester filters beginning 15 min after the flush using open-face cassettes mounted on the WC walls. Pre- and postflush bowl water concentrations were measured. Filter particle counts were analyzed via fluorescent microscopy. Bowl headspace droplet count size distributions were bimodal and similar for all toilet types and flush conditions, with 95% of droplets < 2 μ m diameter and > 99% < 5 μ m. Up to 145,000 droplets were produced per flush, with the high-energy flushometer producing over three times as many as the lower energy PAT and over 12 times as many as the lowest energy HET despite similar flush volumes. The mean numbers of fluorescent droplet nuclei particles aerosolized and remaining airborne also increased with flush energy. Fluorescent droplet nuclei per flush decreased with increasing particle size. These findings suggest two concurrent aerosolization mechanisms-splashing for large droplets and bubble bursting for the fine droplets that form droplet nuclei.

Aerosol Generation by Modern Flush Toilets

PubMed Central

Johnson, David; Lynch, Robert; Marshall, Charles; Mead, Kenneth; Hirst, Deborah

2015-01-01

A microbe-contaminated toilet will produce bioaerosols when flushed. We assessed toilet plume aerosol from high efficiency (HET), pressure-assisted high efficiency (PAT), and flushometer (FOM) toilets with similar bowl water and flush volumes. Total and droplet nuclei “bioaerosols” were assessed. Monodisperse 0.25–1.9-μm fluorescent microspheres served as microbe surrogates in separate trials in a mockup 5 m3 water closet (WC). Bowl water seeding was approximately 1012 particles/mL. Droplet nuclei were sampled onto 0.2-μm pore size mixed cellulose ester filters beginning 15 min after the flush using open-face cassettes mounted on the WC walls. Pre- and postflush bowl water concentrations were measured. Filter particle counts were analyzed via fluorescent microscopy. Bowl headspace droplet count size distributions were bimodal and similar for all toilet types and flush conditions, with 95% of droplets <2 μm diameter and >99% <5 μm. Up to 145,000 droplets were produced per flush, with the high-energy flushometer producing over three times as many as the lower energy PAT and over 12 times as many as the lowest energy HET despite similar flush volumes. The mean numbers of fluorescent droplet nuclei particles aerosolized and remaining airborne also increased with flush energy. Fluorescent droplet nuclei per flush decreased with increasing particle size. These findings suggest two concurrent aerosolization mechanisms—splashing for large droplets and bubble bursting for the fine droplets that form droplet nuclei. PMID:26635429

Radiative Importance of Aerosol-Cloud Interaction

NASA Technical Reports Server (NTRS)

Tsay, Si-Chee

1999-01-01

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

Impact of Aerosols on Convective Clouds and Precipitation

NASA Technical Reports Server (NTRS)

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

2012-01-01

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

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wood, R.

2016-01-01

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

Aerosol-cloud interactions in mixed-phase convective clouds - Part 1: Aerosol perturbations

NASA Astrophysics Data System (ADS)

Miltenberger, Annette K.; Field, Paul R.; Hill, Adrian A.; Rosenberg, Phil; Shipway, Ben J.; Wilkinson, Jonathan M.; Scovell, Robert; Blyth, Alan M.

2018-03-01

Changes induced by perturbed aerosol conditions in moderately deep mixed-phase convective clouds (cloud top height ˜ 5 km) developing along sea-breeze convergence lines are investigated with high-resolution numerical model simulations. The simulations utilise the newly developed Cloud-AeroSol Interacting Microphysics (CASIM) module for the Unified Model (UM), which allows for the representation of the two-way interaction between cloud and aerosol fields. Simulations are evaluated against observations collected during the COnvective Precipitation Experiment (COPE) field campaign over the southwestern peninsula of the UK in 2013. The simulations compare favourably with observed thermodynamic profiles, cloud base cloud droplet number concentrations (CDNC), cloud depth, and radar reflectivity statistics. Including the modification of aerosol fields by cloud microphysical processes improves the correspondence with observed CDNC values and spatial variability, but reduces the agreement with observations for average cloud size and cloud top height. Accumulated precipitation is suppressed for higher-aerosol conditions before clouds become organised along the sea-breeze convergence lines. Changes in precipitation are smaller in simulations with aerosol processing. The precipitation suppression is due to less efficient precipitation production by warm-phase microphysics, consistent with parcel model predictions. In contrast, after convective cells organise along the sea-breeze convergence zone, accumulated precipitation increases with aerosol concentrations. Condensate production increases with the aerosol concentrations due to higher vertical velocities in the convective cores and higher cloud top heights. However, for the highest-aerosol scenarios, no further increase in the condensate production occurs, as clouds grow into an upper-level stable layer. In these cases, the reduced precipitation efficiency (PE) dominates the precipitation response and no further

Long-term observation of aerosol cloud relationships in the Mid-Atlantic region

NASA Astrophysics Data System (ADS)

Li, S.; Joseph, E.; Min, Q.; Yin, B.

2013-12-01

Long-term ground-based observations of aerosol and cloud properties derived from measurements of Multifilter Rotating Shadow Band Radiometer and microwave radiometer at an atmospheric measurement field station in the Baltimore-Washington corridor operated by Howard University are used to examine the temporal variation of aerosol and cloud properties and moreover aerosol indirect effect on clouds. Through statistical analysis of five years (from 2006 to 2010) of these observations, the proportion of polluted cases is found larger in 2006 and 2007 and the proportion of optically thick clouds cases is also larger in 2006 and 2007 than that in 2008, 2009 and 2010. Both the mean aerosol optical depth (AOD) and cloud optical depth (COD) are observed decreasing from 2006 to 2010 but there is no obvious trend observed on cloud liquid water path (LWP). Because of the limit of AOD retrievals under cloudy conditions surface measurements of fine particle particulate matter 2.5 (PM2.5) were used for assessing aerosol indirect effect. A positive relationship between LWP and cloud droplets effective radius (Re) and a negative relationship between PM2.5 and Re are observed based on a stringent case selection method which is used to reduce the uncertainties from retrieval and meteorological impacts. The total 5 years summer time observations are segregated according to the value of PM2.5. Examination of distributions of COD, cloud condensation nuclei (CCN), cloud droplets effective radius and LWP under polluted and pristine conditions further confirm that the high aerosol loading decreases cloud droplets effective radius and increases cloud optical depth.

Effect of phytoplackton-derived organic matter on the behavior of marine aerosols

NASA Astrophysics Data System (ADS)

Fuentes, E.; Coe, H.; McFiggans, G.; Green, D.

2009-04-01

The presence of significant concentrations of organic material in marine aerosols has been appreciated for several decades; however, only recently has significant progress been made towards demonstrating that this organic content is biogenically formed. Biogenic organics of placktonic life origin are incorporated in marine aerosol composition as a result of bubble bursting/breaking waves mechanisms that occur at the ocean surface. The presence of organic surfactants in the marine aerosol composition might have a significant impact on the properties of the generated aerosols by affecting the particles surface tension and solution balance properties. Nevertheless, it remains uncertain the role of such organics on the physical-chemical behavior of marine aerosols. In this work an experimental study was performed in order to determine the influence of biogenic marine organic compounds on the size distribution, hygroscopicity and cloud-nucleating properties of marine aerosols. For the experimental study a laboratory water recirculation system (bubble tank), designed for the simulation of bubble-burst aerosol formation, was used as marine aerosol generator. The bubble spectra produced by such system was characterized by means of an optical bubble measuring device (BMS) and it was found to be consistent with oceanic bubble spectra properties. Seawater proxy solutions were prepared from laboratory biologically-synthesized exudates produced by oceanic representative algal species and introduced in the tank for the generation of marine aerosol by bubble bursting. Two experimental methods were employed for seawater proxies preparation: the formation of surface monolayers from the biogenic surfactants extracted by a solid phase extraction technique (monolayer method) and the mixing of the exudates in the sea salt water bulk (bulk mixing method). Particle size distribution, hygroscopicity and cloud condensation nuclei experiments for different monolayers, and exudate mixtures

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.

Shipborne measurements of aerosol number size distribution and hygroscopicity over the North Pacific Ocean

NASA Astrophysics Data System (ADS)

Royalty, T. M.; Phillips, B.; Dawson, K. W.; Reed, R. E.; Meskhidze, N.

2016-12-01

We report aerosol number size distribution and hygroscopicity data collected over the Pacific Ocean near the Hawaii Ocean Timeseries (HOT) Station ALOHA (centered near 22°N, 158°W). From June 25 to July 3, 2016 our hygroscopicity tandem differential mobility analyzer (HTDMA)/scanning mobility particle sizer (SMPS) system was deployed onboard of NOAA Ship Hi'ialakai that participated in mooring operations associated with the Woods Hole Oceanographic Institution WHOTS project. The ambient aerosol data was collected during the ship's planned operations. The inlet was located at the bow of the ship and the air samples were drawn (using 3/8 inch stainless steel tubing) inside a dry, air-conditioned lab. The region north of Oahu was very clean, with total particle number approximately 200 cm-3, occasionally dropping below 100 cm-3. We compare our particle number size distribution and hygroscopicity data with previously reported estimates. Our measurements contribute to process-level understanding of the role of sea spray aerosol in marine boundary layer cloud condensation nuclei (CCN) budget and provide crucial information to the community interested in studying and projecting climate change using Earth System Models.

On the competition among aerosol number, size and composition in predicting CCN variability: a multi-annual field study in an urbanized desert.

PubMed

Crosbie, E; Youn, J-S; Balch, B; Wonaschütz, A; Shingler, T; Wang, Z; Conant, W C; Betterton, E A; Sorooshian, A

2015-02-10

A 2-year data set of measured CCN (cloud condensation nuclei) concentrations at 0.2 % supersaturation is combined with aerosol size distribution and aerosol composition data to probe the effects of aerosol number concentrations, size distribution and composition on CCN patterns. Data were collected over a period of 2 years (2012-2014) in central Tucson, Arizona: a significant urban area surrounded by a sparsely populated desert. Average CCN concentrations are typically lowest in spring (233 cm -3 ), highest in winter (430 cm -3 ) and have a secondary peak during the North American monsoon season (July to September; 372 cm -3 ). There is significant variability outside of seasonal patterns, with extreme concentrations (1 and 99 % levels) ranging from 56 to 1945 cm -3 as measured during the winter, the season with highest variability. Modeled CCN concentrations based on fixed chemical composition achieve better closure in winter, with size and number alone able to predict 82% of the variance in CCN concentration. Changes in aerosol chemical composition are typically aligned with changes in size and aerosol number, such that hygroscopicity can be parameterized even though it is still variable. In summer, models based on fixed chemical composition explain at best only 41% (pre-monsoon) and 36% (monsoon) of the variance. This is attributed to the effects of secondary organic aerosol (SOA) production, the competition between new particle formation and condensational growth, the complex interaction of meteorology, regional and local emissions and multi-phase chemistry during the North American monsoon. Chemical composition is found to be an important factor for improving predictability in spring and on longer timescales in winter. Parameterized models typically exhibit improved predictive skill when there are strong relationships between CCN concentrations and the prevailing meteorology and dominant aerosol physicochemical processes, suggesting that similar findings could

Seed maturation in Arabidopsis thaliana is characterized by nuclear size reduction and increased chromatin condensation.

PubMed

van Zanten, Martijn; Koini, Maria A; Geyer, Regina; Liu, Yongxiu; Brambilla, Vittoria; Bartels, Dorothea; Koornneef, Maarten; Fransz, Paul; Soppe, Wim J J

2011-12-13

Most plant species rely on seeds for their dispersal and survival under unfavorable environmental conditions. Seeds are characterized by their low moisture content and significantly reduced metabolic activities. During the maturation phase, seeds accumulate storage reserves and become desiccation-tolerant and dormant. Growth is resumed after release of dormancy and the occurrence of favorable environmental conditions. Here we show that embryonic cotyledon nuclei of Arabidopsis thaliana seeds have a significantly reduced nuclear size, which is established at the beginning of seed maturation. In addition, the chromatin of embryonic cotyledon nuclei from mature seeds is highly condensed. Nuclei regain their size and chromatin condensation level during germination. The reduction in nuclear size is controlled by the seed maturation regulator ABSCISIC ACID-INSENSITIVE 3, and the increase during germination requires two predicted nuclear matrix proteins, LITTLE NUCLEI 1 and LITTLE NUCLEI 2. Our results suggest that the specific properties of nuclei in ripe seeds are an adaptation to desiccation, independent of dormancy. We conclude that the changes in nuclear size and chromatin condensation in seeds are independent, developmentally controlled processes.

Marine Stratocumulus Properties from the FPDR - PDI as a Function of Aerosol during ORACLES

NASA Astrophysics Data System (ADS)

Small Griswold, J. D.; Heikkila, A.

2016-12-01

Aerosol-cloud interactions in the southeastern Atlantic (SEA) region were investigated during year 1 of the ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) field project in Aug-Sept 2016. This region is of interest due to seasonally persistent marine stratocumulus cloud decks that are an important component of the climate system due to their radiative and hydrologic impacts. The SEA deck is unique due to the interactions between these clouds and transported biomass burning aerosol during the July-October fire season. These biomass burning aerosol play multiple roles in modifying the cloud deck through interactions with radiation as absorbing aerosol and through modifications to cloud microphysical properties as cloud condensation nuclei. This work uses in situcloud data obtained with a Flight Probe Dual Range - Phase Doppler Interferometer (FPDR - PDI), standard aerosol instrumentation on board the NASA P-3, and reanalysis data to investigate Aerosol-Cloud Interactions (ACI). The FPDR - PDI provides unique cloud microphysical observations of individual cloud drop arrivals allowing for the computation of a variety of microphysical cloud properties including individual drop size, cloud drop number concentration, cloud drop size distributions, liquid water content, and cloud thickness. The FPDR - PDI measurement technique also provides droplet spacing and drop velocity information which is used to investigate turbulence and entrainment mixing processes. We use aerosol information such as average background aerosol amount (low, mid, high) and location relative to cloud (above or mixing) to sort FPDR - PDI cloud properties. To control for meteorological co-variances we further sort the data within aerosol categories by lower tropospheric stability, vertical velocity, and surface wind direction. We then determine general marine stratocumulus cloud characteristics under each of the various aerosol categories to investigate ACI in the SEA.

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

PubMed

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

2016-07-29

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.

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

PubMed Central

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

2016-01-01

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. PMID:27470588

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.

Potential indirect effects of aerosol on tropical cyclone intensity: convective fluxes and cold-pool activity

NASA Astrophysics Data System (ADS)

Krall, G. M.; Cottom, W. R.

2012-01-01

Observational and model evidence suggest that a 2008 Western Pacific typhoon (NURI) ingested elevated concentrations of aerosol as it neared the Chinese coast. This study uses a regional model with two-moment bin-emulating microphysics to simulate the typhoon as it enters the field of elevated aerosol concentrations. A clean maritime field of cloud condensation nuclei (CCN) was prescribed as marine background CCN concentrations and then based on satellite and global aerosol model output, increased to pollution levels and further enhanced in sensitivity tests. The typhoon was simulated for 96 h beginning 17 August 2008. During the final 60 h CCN concentrations were enhanced as it neared the Philippines and coastal China. The model was initialized with both global reanalysis model data and irregularly spaced dropsonde data from the 2008 T-PARC observational campaign using an objective analysis routine. At 36 h, the internal nudging of the model was switched off and allowed to freely evolve on its own. As the typhoon encountered the elevated CCN in the sensitivity tests, a significant perturbation of windspeed, convective fluxes, and hydrometeor species behavior was simulated. Early during the ingestion of enhanced CCN, precipitation was reduced due to suppressed collision and coalescence, and storm winds increased in strength. Subsequently, owing to reduced fall speeds of the smaller drops, greater amounts of condensate were thrust into supercooled levels where the drops froze releasing greater amounts of latent heat of freezing. Convection thereby intensified which resulted in enhanced rainfall and more vigorous convectively-produced downdrafts. As the convection intensified in the outer rainbands the storm drifted over the developing cold-pools. The enhanced cold-pools blocked the inflow of warm, moist air into the core of the typhoon which led to a weakening of the typhoon with significantly reduced low level wind speeds. The very high amounts of pollution

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.;

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

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

Global distribution and sources of volatile and nonvolatile aerosol in the remote troposphere

NASA Astrophysics Data System (ADS)

Singh, Hanwant B.; Anderson, B. E.; Avery, M. A.; Viezee, W.; Chen, Y.; Tabazadeh, A.; Hamill, P.; Pueschel, R.; Fuelberg, H. E.; Hannan, J. R.

2002-06-01

Airborne measurements of aerosol (condensation nuclei, CN) and selected trace gases made over areas of the North Atlantic Ocean during Subsonic Assessment (SASS) Ozone and Nitrogen Oxide Experiment (SONEX) (October/November 1997), the south tropical Pacific Ocean during Pacific Exploratory Mission (PEM)-Tropics A (September/October 1996), and PEM-Tropics B (March/April 1999) have been analyzed. The emphasis is on interpreting variations in the number densities of fine (>17 nm) and ultrafine (>8 nm) aerosol in the upper troposphere (8-12 km). These data suggest that large number densities of highly volatile CN (104 - 105 cm-3) are present in the upper troposphere and particularly over the tropical/subtropical region. CN number densities in all regions are largest when the atmosphere is devoid of nonvolatile particles. 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 aerosols behave in a manner similar to tracers of combustion (CO) and photochemical pollution (peroxyacetylnitrate (PAN)), implying a continental pollution source from industrial emissions or biomass burning. In the upper troposphere we find that volatile and nonvolatile aerosol number densities are inversely correlated. Results from an aerosol microphysical model suggest that the coagulation of fine volatile particles with fewer but larger nonvolatile particles, of principally anthropogenic origin, is one possible explanation for this relationship. In some instances the larger nonvolatile particles may also directly remove precursors (e.g., H2SO4) and effectively stop nucleation.

Potential sea salt aerosol sources from frost flowers in the pan-Arctic region

DOE Office of Scientific and Technical Information (OSTI.GOV)

Xu, Li; Russell, Lynn M.; Burrows, Susannah M.

In order to better represent observed wintertime aerosol concentrations at Barrow, Alaska, we implemented an observationally-based parameterization for estimating sea salt production from frost flowers in the Community Earth System Model (CESM). In this work, we evaluate the potential influence of this sea salt source on the pan-Arctic (60ºN-90ºN) climate. Results show that frost flower salt emissions substantially increase the modeled surface sea salt aerosol concentration in the winter months when new sea ice and frost flowers are present. The parameterization reproduces both the magnitude and seasonal variation of the observed submicron sea salt aerosol concentration at surface in Barrowmore » during winter much better than the standard CESM simulation without a frost-flower salt particle source. Adding these frost flower salt particle emissions increases aerosol optical depth by 10% and results in a small cooling at surface. The increase in salt particle mass concentrations of a factor of 8 provides nearly two times the cloud condensation nuclei concentration, as well as 10% increases in cloud droplet number and 40% increases in liquid water content near coastal regions adjacent to continents. These cloud changes reduce longwave cloud forcing by 3% and cause a small surface warming, increasing the downward longwave flux at the surface by 2 W m-2 in the pan-Arctic under the present-day climate.« less

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

Nonequilibrium atmospheric secondary organic aerosol formation and growth

PubMed Central

Perraud, Véronique; Bruns, Emily A.; Ezell, Michael J.; Johnson, Stanley N.; Yu, Yong; Alexander, M. Lizabeth; Zelenyuk, Alla; Imre, Dan; Chang, Wayne L.; Dabdub, Donald; Pankow, James F.; Finlayson-Pitts, Barbara J.

2012-01-01

Airborne particles play critical roles in air quality, health effects, visibility, and climate. Secondary organic aerosols (SOA) formed from oxidation of organic gases such as α-pinene account for a significant portion of total airborne particle mass. Current atmospheric models typically incorporate the assumption that SOA mass is a liquid into which semivolatile organic compounds undergo instantaneous equilibrium partitioning to grow the particles into the size range important for light scattering and cloud condensation nuclei activity. We report studies of particles from the oxidation of α-pinene by ozone and NO3 radicals at room temperature. SOA is primarily formed from low-volatility ozonolysis products, with a small contribution from higher volatility organic nitrates from the NO3 reaction. Contrary to expectations, the particulate nitrate concentration is not consistent with equilibrium partitioning between the gas phase and a liquid particle. Rather the fraction of organic nitrates in the particles is only explained by irreversible, kinetically determined uptake of the nitrates on existing particles, with an uptake coefficient that is 1.6% of that for the ozonolysis products. If the nonequilibrium particle formation and growth observed in this atmospherically important system is a general phenomenon in the atmosphere, aerosol models may need to be reformulated. The reformulation of aerosol models could impact the predicted evolution of SOA in the atmosphere both outdoors and indoors, its role in heterogeneous chemistry, its projected impacts on air quality, visibility, and climate, and hence the development of reliable control strategies. PMID:22308444

Contributions of Organic Sources to Atmospheric Aerosol Particle Concentrations and Growth

NASA Astrophysics Data System (ADS)

Russell, L. M.

2017-12-01

emissions to particles, addressing the persistent question of the sources of cloud condensation nuclei in clean marine conditions.

Reactivity of liquid and semisolid secondary organic carbon with chloride and nitrate in atmospheric aerosols

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Bingbing; O'Brien, Rachel E.; Univ. of the Pacific, Stockton, CA

2015-05-14

Constituents of secondary organic carbon (SOC) in atmospheric aerosols are often mixed with inorganic components and compose a significant mass fraction of fine particulate matter in the atmosphere. Interactions between SOC and other condensed-phase species are not well understood. Here, we investigate the reactions of liquid-like and semi-solid SOC from ozonolysis of limonene (LSOC) and α-pinene (PSOC) with NaCl using a set of complementary micro-spectroscopic analyses. These reactions result in chloride depletion in the condensed phase, release of gaseous HCl, and formation of organic salts. The reactions attributed to acid displacement by SOC acidic components are driven by the highmore » volatility of HCl. Similar reactions can take place in SOC/NaNO₃ particles. The results show that an increase in SOC mass fraction in the internally mixed SOC/NaCl particles leads to higher chloride depletion. Glass transition temperatures and viscosity of PSOC were estimated for atmospherically relevant conditions. Data show that the reaction extent depends on SOC composition, particle phase state and viscosity, mixing state, temperature, relative humidity (RH), and reaction time. LSOC shows slightly higher potential to deplete chloride than PSOC. Higher particle viscosity at low temperatures and RH can hinder these acid displacement reactions. Formation of organic salts from these overlooked reactions can alter particle physiochemical properties and may affect their reactivity and ability to act as cloud condensation and ice nuclei. The release and potential recycling of HCl and HNO₃ from reacted aerosol particles may have important implications for atmospheric chemistry.« less

Reactivity of liquid and semisolid secondary organic carbon with chloride and nitrate in atmospheric aerosols.

PubMed

Wang, Bingbing; O'Brien, Rachel E; Kelly, Stephen T; Shilling, John E; Moffet, Ryan C; Gilles, Mary K; Laskin, Alexander

2015-05-14

Constituents of secondary organic carbon (SOC) in atmospheric aerosols are often mixed with inorganic components and compose a significant mass fraction of fine particulate matter in the atmosphere. Interactions between SOC and other condensed-phase species are not well understood. Here, we investigate the reactions of liquid-like and semisolid SOC from ozonolysis of limonene (LSOC) and α-pinene (PSOC) with NaCl using a set of complementary microspectroscopic analyses. These reactions result in chloride depletion in the condensed phase, release of gaseous HCl, and formation of organic salts. The reactions attributed to acid displacement by SOC acidic components are driven by the high volatility of HCl. Similar reactions can take place in SOC/NaNO3 particles. The results show that an increase in SOC mass fraction in the internally mixed SOC/NaCl particles leads to higher chloride depletion. Glass transition temperatures and viscosity of PSOC were estimated for atmospherically relevant conditions. Data show that the reaction extent depends on SOC composition, particle phase state and viscosity, mixing state, temperature, relative humidity (RH), and reaction time. LSOC shows slightly higher potential to deplete chloride than PSOC. Higher particle viscosity at low temperatures and RH can hinder these acid displacement reactions. Formation of organic salts from these overlooked reactions can alter particle physiochemical properties and may affect their reactivity and ability to act as cloud condensation and ice nuclei. The release and potential recycling of HCl and HNO3 from reacted aerosol particles may have important implications for atmospheric chemistry.

Nascent Marine Aerosol Acting as Ultra-Efficient Cloud Nuclei

NASA Astrophysics Data System (ADS)

Ovadnevaite, J.; Zuend, A.; Laaksonen, A.; Sanchez, K.; Roberts, G.; Ceburnis, D.; Decesari, S.; Rinaldi, M.; Hodas, N.; Facchini, C.; Seinfeld, J.; O'Dowd, C. D. D.

2017-12-01

Marine aerosol is an important part of the natural aerosol and often dominates the total burden in remote locations. Moreover, it contributes significantly to the global radiative budget through the formation of haze and cloud layers. Even if these layers are optically-thin at times, they can have a profound impact on the radiative budget as they overly a dark and extensive ocean surface. Since the postulation of marine aerosol global importance several decades ago1, understanding has progressed from evaluation of the nss-sulphate and sea salt effects to the acknowledgement of a significant role of organic aerosol2. Dependence of organic matter (OM) fraction enrichment in sea spray on phytoplankton biomass has been shown3 as well as an apparent dichotomous OM behaviour in terms of water uptake4. Hygroscopicity of organic aerosol in sub-saturated humidity fields is typically less than most common salts found in the atmospheric aerosol; however, the ability of organic aerosol to activate cloud droplets is predicted to be greatly increased in supersaturated air due a lowering of the droplets surface tension5. While this phenomenon has been acknowledged for some time, it has yet to be demonstrated in the real atmosphere. Here, we present evidence that recently-formed secondary organic aerosol particles, in marine air, lead to enhanced cloud droplet activation resulting from surface tension reduction. Whilst the surface tension lowering is expected to be negated by a concomitant reduction in the Raoult effect, driven by the displacement of solute ions by surfactant molecules at the droplet-vapour interface, we present new observational and theoretical evidence illustrating that, in ambient air, the former can prevail over the latter. Consideration of liquid-liquid phase-separation, leading to complete or partial engulfing of a hygroscopic particle core by a hydrophobic organic-rich phase, explains the lack of suppression of the Raoult effect, while maintaining

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

NASA Technical Reports Server (NTRS)

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

1990-01-01

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

Giant aerosol observations with cloud radar: methodology and effects

NASA Astrophysics Data System (ADS)

Guma Claramunt, Pilar; Madonna, Fabio; Amodeo, Aldo; Bauer-Pfundstein, Matthias; Papagiannopoulos, Nikolaos; Pappalardo, Gelsomina

2017-04-01

Giant aerosol particles can act as Giant Cloud Condensation Nuclei (GCCN), and determine the droplet concentration at the cloud formation, the clouds albedo and lifetime, and the precipitation formation. In addition, depending on their composition, they can also act as IN. It is not yet clear if they can also expedite rain processes. The main techniques used nowadays in measuring aerosols, which are lidar and sun photometer, cannot retrieve aerosol microphysical properties for particles bigger than a few microns, which means that they do not account for giant aerosols. Therefore, the distribution and impact in the atmosphere and climate of these particles is not well known and the aerosol transport models largely underestimate them. Recent studies have demonstrated that cloud radars are able to detect ultragiant volcanic aerosols also at a large distance from the source. In this study, an innovative methodology for the observation of giant aerosols using the millimeter wavelength radar has been developed and applied to 6 years of measurements carried out at CNR-IMAA Atmospheric Observatory (CIAO), in Potenza, South Italy, finding more than 40 giant aerosol events per year and a good agreement with the aerosol climatologic data. Besides, the effects of giant aerosols in the local and regional meteorology have been studied by correlating several atmospheric variables in the time period following the observation of giant particles. The meteorological situation has been assessed through the data classification into cases characterized by different pressure vertical velocities at the upper atmosphere (400 hPa), Giant aerosols are correlated to lower values of the Cloud Optical Depth (COD) in presence of stable or unstable atmospheric conditions while higher values are found for an intermediate stability. The giant aerosols effects on the Liquid Water Path (LWP) are closely linked to those in the Aerosol Optical Thickness (AOD). The highest increases in the LWP occurs

Sea-Salt Aerosol Forecasts Compared with Wave and Sea-Salt Measurements in the Open Mediterranean Sea

NASA Astrophysics Data System (ADS)

Kishcha, P.; Starobinets, B.; Bozzano, R.; Pensieri, S.; Canepa, E.; Nickovie, S.; di Sarra, A.; Udisti, R.; Becagli, S.; Alpert, P.

2012-03-01

Sea-salt aerosol (SSA) could influence the Earth's climate acting as cloud condensation nuclei. However, there were no regular measurements of SSA in the open sea. At Tel-Aviv University, the DREAM-Salt prediction system has been producing daily forecasts of 3-D distribution of sea-salt aerosol concentrations over the Mediterranean Sea (http://wind.tau.ac.il/saltina/ salt.html). In order to evaluate the model performance in the open sea, daily modeled concentrations were compared directly with SSA measurements taken at the tiny island of Lampedusa, in the Central Mediterranean. In order to further test the robustness of the model, the model performance over the open sea was indirectly verified by comparing modeled SSA concentrations with wave height measurements collected by the ODAS Italia 1 buoy and the Llobregat buoy. Model-vs.-measurement comparisons show that the model is capable of producing realistic SSA concentrations and their day-today variations over the open sea, in accordance with observed wave height and wind speed.

Redistribution of ice nuclei between cloud and rain droplets: Parameterization and application to deep convective clouds

NASA Astrophysics Data System (ADS)

Paukert, M.; Hoose, C.; Simmel, M.

2017-03-01

In model studies of aerosol-dependent immersion freezing in clouds, a common assumption is that each ice nucleating aerosol particle corresponds to exactly one cloud droplet. In contrast, the immersion freezing of larger drops—"rain"—is usually represented by a liquid volume-dependent approach, making the parameterizations of rain freezing independent of specific aerosol types and concentrations. This may lead to inconsistencies when aerosol effects on clouds and precipitation shall be investigated, since raindrops consist of the cloud droplets—and corresponding aerosol particles—that have been involved in drop-drop-collisions. Here we introduce an extension to a two-moment microphysical scheme in order to account explicitly for particle accumulation in raindrops by tracking the rates of selfcollection, autoconversion, and accretion. This provides a direct link between ice nuclei and the primary formation of large precipitating ice particles. A new parameterization scheme of drop freezing is presented to consider multiple ice nuclei within one drop and effective drop cooling rates. In our test cases of deep convective clouds, we find that at altitudes which are most relevant for immersion freezing, the majority of potential ice nuclei have been converted from cloud droplets into raindrops. Compared to the standard treatment of freezing in our model, the less efficient mineral dust-based freezing results in higher rainwater contents in the convective core, affecting both rain and hail precipitation. The aerosol-dependent treatment of rain freezing can reverse the signs of simulated precipitation sensitivities to ice nuclei perturbations.

The hygroscopicity parameter (κ) of ambient organic aerosol at a field site subject to biogenic and anthropogenic influences: relationship to degree of aerosol oxidation

NASA Astrophysics Data System (ADS)

Chang, R. Y.-W.; Slowik, J. G.; Shantz, N. C.; Vlasenko, A.; Liggio, J.; Sjostedt, S. J.; Leaitch, W. R.; Abbatt, J. P. D.

2010-06-01

Cloud condensation nuclei (CCN) concentrations were measured at Egbert, a rural site in Ontario, Canada during the spring of 2007. The CCN concentrations were compared to values predicted from the aerosol chemical composition and size distribution using κ-Köhler theory, with the specific goal of this work being to determine the hygroscopic parameter (κ) of the oxygenated organic component of the aerosol, assuming that oxygenation drives the hygroscopicity for the entire organic fraction of the aerosol. The hygroscopicity of the oxygenated fraction of the organic component, as determined by an Aerodyne aerosol mass spectrometer (AMS), was characterised by two methods. First, positive matrix factorization (PMF) was used to separate oxygenated and unoxygenated organic aerosol factors. By assuming that the unoxygenated factor is completely non-hygroscopic and by varying κ of the oxygenated factor so that the predicted and measured CCN concentrations are internally consistent and in good agreement, κ of the oxygenated organic factor was found to be 0.22±0.04 for the suite of measurements made during this five-week campaign. In a second, equivalent approach, we continue to assume that the unoxygenated component of the aerosol, with a mole ratio of atomic oxygen to atomic carbon (O/C) ≈ 0, is completely non-hygroscopic, and we postulate a simple linear relationship between κorg and O/C. Under these assumptions, the κ of the entire organic component for bulk aerosols measured by the AMS can be parameterised as κorg=(0.29±0.05)·(O/C), for the range of O/C observed in this study (0.3 to 0.6). These results are averaged over our five-week study at one location using only the AMS for composition analysis. Empirically, our measurements are consistent with κorg generally increasing with increasing particle oxygenation, but high uncertainties preclude us from testing this hypothesis. Lastly, we examine select periods of different aerosol composition, corresponding

Air-Sea exchange of biogenic volatile organic compounds and the impact on aerosol particle size distributions

NASA Astrophysics Data System (ADS)

Kim, Michelle J.; Novak, Gordon A.; Zoerb, Matthew C.; Yang, Mingxi; Blomquist, Byron W.; Huebert, Barry J.; Cappa, Christopher D.; Bertram, Timothy H.

2017-04-01

We report simultaneous, underway eddy covariance measurements of the vertical flux of isoprene, total monoterpenes, and dimethyl sulfide (DMS) over the Northern Atlantic Ocean during fall. Mean isoprene and monoterpene sea-to-air vertical fluxes were significantly lower than mean DMS fluxes. While rare, intense monoterpene sea-to-air fluxes were observed, coincident with elevated monoterpene mixing ratios. A statistically significant correlation between isoprene vertical flux and short wave radiation was not observed, suggesting that photochemical processes in the surface microlayer did not enhance isoprene emissions in this study region. Calculations of secondary organic aerosol production rates (PSOA) for mean isoprene and monoterpene emission rates sampled here indicate that PSOA is on average <0.1 μg m-3 d-1. Despite modest PSOA, low particle number concentrations permit a sizable role for condensational growth of monoterpene oxidation products in altering particle size distributions and the concentration of cloud condensation nuclei during episodic monoterpene emission events from the ocean.

MCS precipitation and downburst intensity response to increased aerosol concentrations

NASA Astrophysics Data System (ADS)

Clavner, M.; Cotton, W. R.; van den Heever, S. C.

2015-12-01

Mesoscale convective systems (MCSs) are important contributors to rainfall in the High Plains of the United States as well as producers of severe weather such as hail, tornados and straight-line wind events known as derechos. Past studies have shown that changes in aerosol concentrations serving as cloud condensation nuclei (CCN) alter the MCS hydrometeor characteristics which in turn modify precipitation yield, downdraft velocity, cold-pool strength, storm propagation and the potential for severe weather to occur. In this study, the sensitivity of MCS precipitation characteristics and convective downburst velocities associated with a derecho to changes in CCN concentrations were examined by simulating a case study using the Regional Atmospheric Modeling System (RAMS). The case study of the 8 May 2009 "Super-Derecho" MCS was chosen since it produced a swath of widespread wind damage in association with an embedded large-scale bow echo, over a broad region from the High Plains of western Kansas to the foothills of the Appalachians. The sensitivity of the storm to changes in CCN concentrations was examined by conducting a set of three simulations which differed in the initial aerosol concentration based on output from the 3D chemical transport model, GEOS-Chem. Results from this study indicate that while increasing CCN concentrations led to an increase in precipitation rates, the changes to the derecho strength were not linear. A moderate increase in aerosol concentration reduced the derecho strength, while the simulation with the highest aerosol concentrations increased the derecho intensity. These changes are attributed to the impact of enhanced CCN concentration on the production of convective downbursts. An analysis of aerosol loading impacts on these MCS features will be presented.

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

NASA Technical Reports Server (NTRS)

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

2012-01-01

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

In Place Calibration of Aerosol Optical Depth Instruments.

NASA Astrophysics Data System (ADS)

Denn, F. M.; Fabbri, B. E.; Schuster, G. L.

2016-12-01

Aerosol Optical Depth (AOD) is important because aerosols determine atmospheric energy deposition and cloud condensation nuclei. AOD can be determined with a narrow band sun photometer. The first step in determining AOD is calibration, which is the determination of the top of atmosphere values (V0). The sun photometer considered here is a Yankee Environmental Multi-Filter Rotating Shadowband Radiometer (MFRSR). Four methods of determining the top of atmosphere values are examined and applied to data taken during the Third Filter Radiometer Comparison (FRC-III), held in Davos, Switzerland during September and October of 2015. Data from a set of three Physikalisch Meteorologisches Observatorium Davos (PMOD) manufactured Precision Filter Radiometers (PFRs), known as the PFR Triad, were used as the reference data set. Data were collected over a five year period at two Baseline Surface Radiation Network Sites: CLH (Chesapeake Light House, 25 kilometers off the Virginia coast); LRC (located in southeast Virginia); at PMOD; and at Mauna Loa, Hawaii. AODs determined using in place calibration agree with values determined by the Triad as well as or better than AODs determined using mountain calibrations, but determination of the V0s takes longer. Also, there is no possibility of instrument damage during shipping.

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

PubMed

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

2008-12-28

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

Effect of Morphology and Composition on the Hygroscopicity of Soot Aerosols

NASA Astrophysics Data System (ADS)

Williams, L.; Slowik, J.; Davidovits, P.; Jayne, J.; Kolb, C.; Worsnop, D.; Rudich, Y.

2003-12-01

Freshly generated soot aerosols are initially hydrophobic and unlikely to act as cloud condensation nuclei (CCN). However, during combustion many low vapor pressure gas products are formed that may then condense on existing soot aerosols. Additionally, soot particles may acquire coatings as they age, such as acids, salts, and oxygenated organics. An understanding of this aging process and its effect on soot hygroscopicity is necessary to address the potential of soot to act as a CCN. The transformation of soot from hydrophobic to hydrophilic is the focus of this work. An aim here is to determine the minimum coating required for hygroscopic growth. Soot particles produced by combustion of mixtures of fuel and air are size selected by a Differential Mobility Analyzer (DMA) and entrained in a laminar flow passing through a flow tube. The size selected soot particles are mixed with a controlled amount of the gas phase precursors to produce the coatings to be studied. Initial studies are focused on coatings of H2SO4, NH4NO3, and selected organics. The number of particles per unit volume of air is counted by a Condensation Particle Counter (CPC) and the particles are isokinetically sampled into an Aerosol Mass Spectrometer (AMS). Two distinct types of soot aerosols have been observed depending on the type of fuel and air mixture. With soot produced by the combustion of propane and air, the AMS shows a polydisperse particle size distribution with aerodynamic diameters ranging from 100 nm to 400 nm. The aerodynamic diameter is linearly related to the DMA-determined mobility diameter with the product density x shape factor = 1.2. The organic molecules in this soot are mostly PAH compounds. However, when kerosene is added to the propane flame, the soot particle morphology and composition is strikingly altered. While the DMA shows an essentially unchanged mobility diameter distribution, in the range 100 nm to 400, aerodynamic particle diameter is constant at about 100 nm

Interannual Variations in Aerosol Sources and Their Impact on Orographic Precipitation Over California's Central Sierra Nevada

NASA Technical Reports Server (NTRS)

Creamean, J. M.; Ault, A. P.; White, A. B.; Neiman, P. J.; Ralph, F. M.; Minnis, Patrick; Prather, K. A.

2014-01-01

Aerosols that serve as cloud condensation nuclei (CCN) and ice nuclei (IN) have the potential to profoundly influence precipitation processes. Furthermore, changes in orographic precipitation have broad implications for reservoir storage and flood risks. As part of the CalWater I field campaign (2009-2011), the impacts of aerosol sources on precipitation were investigated in the California Sierra Nevada. In 2009, the precipitation collected on the ground was influenced by both local biomass burning (up to 79% of the insoluble residues found in precipitation) and long-range transported dust and biological particles (up to 80% combined), while in 2010, by mostly local sources of biomass burning and pollution (30-79% combined), and in 2011 by mostly long-range transport from distant sources (up to 100% dust and biological). Although vast differences in the source of residues was observed from year-to-year, dust and biological residues were omnipresent (on average, 55% of the total residues combined) and were associated with storms consisting of deep convective cloud systems and larger quantities of precipitation initiated in the ice phase. Further, biological residues were dominant during storms with relatively warm cloud temperatures (up to -15 C), suggesting these particles were more efficient IN compared to mineral dust. On the other hand, lower percentages of residues from local biomass burning and pollution were observed (on average 31% and 9%, respectively), yet these residues potentially served as CCN at the base of shallow cloud systems when precipitation quantities were low. The direct connection of the source of aerosols within clouds and precipitation type and quantity can be used in models to better assess how local emissions versus long-range transported dust and biological aerosols play a role in impacting regional weather and climate, ultimately with the goal of more accurate predictive weather forecast models and water resource management.

Interannual Variations in Aerosol Sources and Their Impact on Orographic Precipitation over California's Central Sierra Nevada

NASA Astrophysics Data System (ADS)

Creamean, J.; Ault, A. P.; White, A. B.; Neiman, P. J.; Minnis, P.; Prather, K. A.

2014-12-01

Aerosols that serve as cloud condensation nuclei (CCN) and ice nuclei (IN) have the potential to profoundly influence precipitation processes. Furthermore, changes in orographic precipitation have broad implications for reservoir storage and flood risks. As part of the CalWater I field campaign (2009-2011), the impacts of aerosol sources on precipitation were investigated in the California Sierra Nevada Mountains. In 2009, the precipitation collected on the ground was influenced by both local biomass burning and long-range transported dust and biological particles, while in 2010, by mostly local sources of biomass burning and pollution, and in 2011 by mostly long-range transport of dust and biological particles from distant sources. Although vast differences in the sources of residues were observed from year-to-year, dust and biological residues were omnipresent (on average, 55% of the total residues combined) and were associated with storms consisting of deep convective cloud systems and larger quantities of precipitation initiated in the ice phase. Further, biological residues were dominant during storms with relatively warm cloud temperatures (up to -15°C), suggesting biological components were more efficient IN than mineral dust. On the other hand, when precipitation quantities were lower, local biomass burning and pollution residues were observed (on average 31% and 9%, respectively), suggesting these residues potentially served as CCN at the base of shallow cloud systems and that lower level polluted clouds of storm systems produced less precipitation than non-polluted (i.e., marine) clouds. The direct connection of the sources of aerosols within clouds and precipitation type and quantity can be used in models to better assess how local emissions versus long-range transported dust and biological aerosols play a role in impacting regional weather and climate, ultimately with the goal of more accurate predictive weather forecast models and water resource

Investigation of aerosol indirect effects on simulated flash-flood heavy rainfall over Korea

NASA Astrophysics Data System (ADS)

Lim, Kyo-Sun Sunny; Hong, Song-You

2012-11-01

This study investigates aerosol indirect effects on the development of heavy rainfall near Seoul, South Korea, on 12 July 2006, focusing on precipitation amount. The impact of the aerosol concentration on simulated precipitation is evaluated by varying the initial cloud condensation nuclei (CCN) number concentration in the Weather Research and Forecasting (WRF) Double-Moment 6-class (WDM6) microphysics scheme. The simulations are performed under clean, semi-polluted, and polluted conditions. Detailed analysis of the physical processes that are responsible for surface precipitation, including moisture and cloud microphysical budgets shows enhanced ice-phase processes to be the primary driver of increased surface precipitation under the semi-polluted condition. Under the polluted condition, suppressed auto-conversion and the enhanced evaporation of rain cause surface precipitation to decrease. To investigate the role of environmental conditions on precipitation response under different aerosol number concentrations, a set of sensitivity experiments are conducted with a 5 % decrease in relative humidity at the initial time, relative to the base simulations. Results show ice-phase processes having small sensitivity to CCN number concentration, compared with the base simulations. Surface precipitation responds differently to CCN number concentration under the lower humidity initial condition, being greatest under the clean condition, followed by the semi-polluted and polluted conditions.

Aerosol Size, CCN, and Black Carbon Properties at a Coastal Site in the Eastern U.S.

NASA Astrophysics Data System (ADS)

Royalty, T. M.; Petters, M. D.; Grieshop, A. P.; Meskhidze, N.; Reed, R. E.; Phillips, B.; Dawson, K. W.

2015-12-01

Atmospheric aerosols play an important role in regulating the global radiative budget through direct and indirect effects. To date, the role of sea spray aerosols in modulating climate remains poorly understood. Here we present results from measurements performed at the United States Army Corps of Engineers' Field Research Facility in Duck, North Carolina, USA. Aerosol mobility size distributions (10-600 nm), refractory black carbon (rBC) and scattering particle size distributions (200-620 nm), and size resolved cloud condensation nuclei distributions (.07% - .6% supersaturation) were collected at the end of a 560m pier. Aerosol characteristics associated with northerly, high wind speed (15+ m s-1) flow originating from an oceanic trajectory are contrasted with aerosol properties observed during a weak to moderate westerly flow originating from a continental trajectory. Both marine and continental air masses had aerosol with bi-modal number size distributions with modes centered at 30nm and 140nm. In the marine air-mass, the CCN concentration at supersaturation of 0.4%, total aerosol number, surface, and volume concentration were low. rBC number concentration (D > 200 nm) associated with the marine air-mass was an order of magnitude less than continental number concentration and indicative of relatively unpolluted air. These measurements are consistent with measurements from other coastal sites under marine influence. The relative proportion of Aitken mode size particles increased from 1:2 to 2:1 while aerosol surface area was < 25 μm2 cm-3, suggesting that conditions upwind were potentially conducive to new particle formation. Overall, these results will contribute a better understanding to composition and size variation of marine aerosols.

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fast, JD; Berg, LK

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 moremore » 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.« less

Variation in aerosol nucleation and growth in coal-fired power plant plumes due to background aerosol, meteorology and emissions: sensitivity analysis and parameterization.

NASA Astrophysics Data System (ADS)

Stevens, R. G.; Lonsdale, C. L.; Brock, C. A.; Reed, M. K.; Crawford, J. H.; Holloway, J. S.; Ryerson, T. B.; Huey, L. G.; Nowak, J. B.; Pierce, J. R.

2012-04-01

New-particle formation in the plumes of coal-fired power plants and other anthropogenic sulphur sources may be an important source of particles in the atmosphere. It remains unclear, however, how best to reproduce this formation in global and regional aerosol models with grid-box lengths that are 10s of kilometres and larger. The predictive power of these models is thus limited by the resultant uncertainties in aerosol size distributions. In this presentation, we focus on sub-grid sulphate aerosol processes within coal-fired power plant plumes: the sub-grid oxidation of SO2 with condensation of H2SO4 onto newly-formed and pre-existing particles. Based on the results of the System for Atmospheric Modelling (SAM), a Large-Eddy Simulation/Cloud-Resolving Model (LES/CRM) with online TwO Moment Aerosol Sectional (TOMAS) microphysics, we develop a computationally efficient, but physically based, parameterization that predicts the characteristics of aerosol formed within coal-fired power plant plumes based on parameters commonly available in global and regional-scale models. Given large-scale mean meteorological parameters, emissions from the power plant, mean background condensation sink, and the desired distance from the source, the parameterization will predict the fraction of the emitted SO2 that is oxidized to H2SO4, the fraction of that H2SO4 that forms new particles instead of condensing onto preexisting particles, the median diameter of the newly-formed particles, and the number of newly-formed particles per kilogram SO2 emitted. We perform a sensitivity analysis of these characteristics of the aerosol size distribution to the meteorological parameters, the condensation sink, and the emissions. In general, new-particle formation and growth is greatly reduced during polluted conditions due to the large preexisting aerosol surface area for H2SO4 condensation and particle coagulation. The new-particle formation and growth rates are also a strong function of the

The competition between mineral dust and soot ice nuclei in mixed-phase clouds (Invited)

NASA Astrophysics Data System (ADS)

Murray, B. J.; Atkinson, J.; Umo, N.; Browse, J.; Woodhouse, M. T.; Whale, T.; Baustian, K. J.; Carslaw, K. S.; Dobbie, S.; O'Sullivan, D.; Malkin, T. L.

2013-12-01

The amount of ice present in mixed-phase clouds, which contain both supercooled liquid water droplets and ice particles, affects cloud extent, lifetime, particle size and radiative properties. The freezing of cloud droplets can be catalysed by the presence of aerosol particles known as ice nuclei. In this talk our recent laboratory and global aerosol modelling work on mineral dust and soot ice nuclei will be presented. We have performed immersion mode experiments to quantify ice nucleation by the individual minerals which make up desert mineral dusts and have shown that the feldspar component, rather than the clay component, is most important for ice nucleation (Atkinson et al. 2013). Experiments with well-characterised soot generated with eugenol, an intermediate in biomass burning, and n-decane show soot has a significant ice nucleation activity in mixed-phase cloud conditions. Our results for soot are in good agreement with previous results for acetylene soot (DeMott, 1990), but extend the efficiency to much higher temperatures. We then use a global aerosol model (GLOMAP) to map the distribution of soot and feldspar particles on a global basis. We show that below about -15oC that dust and soot together can explain most observed ice nuclei in the Earth's atmosphere, while at warmer temperatures other ice nuclei types are needed. We show that in some regions soot is the most important ice nuclei (below -15oC), while in others feldspar dust dominates. Our results suggest that there is a strong anthropogenic contribution to the ice nuclei population, since a large proportion of soot aerosol in the atmosphere results from human activities. Atkinson, J. D., Murray, B. J., Woodhouse, M. T., Carslaw, K. S., Whale, T. F., Baustian, K. J., Dobbie, S., O'Sullivan, D., and Malkin, T. L.: The importance of feldspar for ice nucleation by mineral dust in mixed-phase clouds, Nature, 10.1038/nature12278, (2013). Demott, P. J. 1990. An Exploratory-Study of Ice Nucleation by Soot

Long-term cloud condensation nuclei number concentration, particle number size distribution and chemical composition measurements at regionally representative observatories

NASA Astrophysics Data System (ADS)

Schmale, Julia; Henning, Silvia; Decesari, Stefano; Henzing, Bas; Keskinen, Helmi; Sellegri, Karine; Ovadnevaite, Jurgita; Pöhlker, Mira L.; Brito, Joel; Bougiatioti, Aikaterini; Kristensson, Adam; Kalivitis, Nikos; Stavroulas, Iasonas; Carbone, Samara; Jefferson, Anne; Park, Minsu; Schlag, Patrick; Iwamoto, Yoko; Aalto, Pasi; Äijälä, Mikko; Bukowiecki, Nicolas; Ehn, Mikael; Frank, Göran; Fröhlich, Roman; Frumau, Arnoud; Herrmann, Erik; Herrmann, Hartmut; Holzinger, Rupert; Kos, Gerard; Kulmala, Markku; Mihalopoulos, Nikolaos; Nenes, Athanasios; O'Dowd, Colin; Petäjä, Tuukka; Picard, David; Pöhlker, Christopher; Pöschl, Ulrich; Poulain, Laurent; Prévôt, André Stephan Henry; Swietlicki, Erik; Andreae, Meinrat O.; Artaxo, Paulo; Wiedensohler, Alfred; Ogren, John; Matsuki, Atsushi; Yum, Seong Soo; Stratmann, Frank; Baltensperger, Urs; Gysel, Martin

2018-02-01

Aerosol-cloud interactions (ACI) constitute the single largest uncertainty in anthropogenic radiative forcing. To reduce the uncertainties and gain more confidence in the simulation of ACI, models need to be evaluated against observations, in particular against measurements of cloud condensation nuclei (CCN). Here we present a data set - ready to be used for model validation - of long-term observations of CCN number concentrations, particle number size distributions and chemical composition from 12 sites on 3 continents. Studied environments include coastal background, rural background, alpine sites, remote forests and an urban surrounding. Expectedly, CCN characteristics are highly variable across site categories. However, they also vary within them, most strongly in the coastal background group, where CCN number concentrations can vary by up to a factor of 30 within one season. In terms of particle activation behaviour, most continental stations exhibit very similar activation ratios (relative to particles > 20 nm) across the range of 0.1 to 1.0 % supersaturation. At the coastal sites the transition from particles being CCN inactive to becoming CCN active occurs over a wider range of the supersaturation spectrum. Several stations show strong seasonal cycles of CCN number concentrations and particle number size distributions, e.g. at Barrow (Arctic haze in spring), at the alpine stations (stronger influence of polluted boundary layer air masses in summer), the rain forest (wet and dry season) or Finokalia (wildfire influence in autumn). The rural background and urban sites exhibit relatively little variability throughout the year, while short-term variability can be high especially at the urban site. The average hygroscopicity parameter, κ, calculated from the chemical composition of submicron particles was highest at the coastal site of Mace Head (0.6) and lowest at the rain forest station ATTO (0.2-0.3). We performed closure studies based on κ

A Study of The Direct Aerosol Forcing At Ground Level For A Pollution Event During The Escompte Campaign

NASA Astrophysics Data System (ADS)

Mallet, M.; Roger, J. C.; Dubuisson, P.; Putaud, J. P.; van Dingenen, R.; Despiau, S.

Radiative forcing by aerosol particles is one of the largest source of uncertainties in predicting climate change (IPCC, 2001). Indeed, quantitative estimates of this effect are still uncertain due to little knowledge of these atmospheric particles. Atmospheric particles influence the Earth's radiation balance both directly and indirectly. The indi- rect effect denotes the effect of aerosols acting as cloud condensation nuclei, possibly modifying cloud albedo and cloud lifetime. The direct effect is due to scattering and absorption of radiation and each of these processes depends mainly on the refractive index and the size distribution of aerosol particles. During the ESCOMPTE campaign, which took place in coastal Mediterranean area during the summer 2001, we estimated these aerosol micro-physical properties during a pollution event at two different sites. The first is an urban site (the city of Marseille), and the second is a rural area located fifty kilometers inland. The aerosol size distribution was measured with an SMPS for the particles with radii < 1 µm, and an optical counter for r > 1 µm. The chemi- cal composition (including different ionic compounds , dust, elemental and organic carbon) was deduced from chromatography analysis. The aerosol optical properties calculated from measured aerosol physical and chemical properties at ground level (from Mie theory) are used as input to a shortwave radiative transfer model. Then, this model is used to calculate the diurnally averaged direct aerosol forcing at surface and to compare this values with those measured from the ARAT aircraft and surface pyranometer during the campaign.

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

Quantifying the microphysical impacts of fire aerosols on clouds in Indonesia using remote sensing observations

NASA Astrophysics Data System (ADS)

Tosca, M. G.; Diner, D. J.; Garay, M. J.; Kalashnikova, O. V.

2012-12-01

Fire-emitted aerosols modify cloud and precipitation dynamics by acting as cloud condensation nuclei in what is known as the first and second aerosol indirect effect. The cloud response to the indirect effect varies regionally and is not well understood in the highly convective tropics. We analyzed nine years (2003-2011) of aerosol data from the Multi-angle Imaging SpectroRadiometer (MISR), and fire emissions data from the Global Fire Emissions Database, version 3 (GFED3) over southeastern tropical Asia (Indonesia), and identified scenes that contained both a high atmospheric aerosol burden and large surface fire emissions. We then collected scenes from the Cloud Profiling Radar (CPR) on board the CLOUDSAT satellite that corresponded both spatially and temporally to the high-burning scenes from MISR, and identified differences in convective cloud dynamics over areas with varying aerosol optical depths. Differences in overpass times (MISR in the morning, CLOUDSAT in the afternoon) improved our ability to infer that changes in cloud dynamics were a response to increased or decreased aerosol emissions. Our results extended conclusions from initial studies over the Amazon that used remote sensing techniques to identify cloud fraction reductions in high burning areas (Koren et al., 2004; Rosenfeld, 1999) References Koren, I., Y.J. Kaufman, L.A. Remer and J.V. Martins (2004), Measurement of the effect of Amazon smoke on inhibition of cloud formation, Science, 303, 1342-1345 Rosenfeld, D. (1999), TRMM observed first direct evidence of smoke from forest fires inhibiting rainfall, Gephys. Res. Lett., 26, 3105.

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

DOE PAGES

Zhang, Shipeng; Wang, Minghuai; Ghan, Steven J.; ...

2016-03-04

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

A new chemistry option in WRF/Chem v. 3.4 for the simulation of direct and indirect aerosol effects using VBS: evaluation against IMPACT-EUCAARI data

NASA Astrophysics Data System (ADS)

Tuccella, P.; Curci, G.; Grell, G. A.; Visconti, G.; Crumeroylle, S.; Schwarzenboeck, A.; Mensah, A. A.

2015-02-01

A parameterization for secondary organic aerosol (SOA) production based on the volatility basis set (VBS) approach has been coupled with microphysics and radiative scheme in WRF/Chem model. The new chemistry option called "RACM/MADE/VBS" was evaluated on a cloud resolving scale against ground-based and aircraft measurements collected during the IMPACT-EUCAARI campaign, and complemented with satellite data from MODIS. The day-to-day variability and the diurnal cycle of ozone (O3) and nitrogen oxides (NOx) at the surface is captured by the model. Surface aerosol mass of sulphate (SO4), nitrate (NO3), ammonium (NH4), and organic matter (OM) is simulated with a correlation larger than 0.55. WRF/Chem captures the vertical profile of the aerosol mass in both the planetary boundary layer (PBL) and free troposphere (FT) as a function of the synoptic condition, but the model does not capture the full range of the measured concentrations. Predicted OM concentration is at the lower end of the observed mass. The bias may be attributable to the missing aqueous chemistry processes of organic compounds, the uncertainties in meteorological fields, the assumption on the deposition velocity of condensable organic vapours, and the uncertainties in the anthropogenic emissions of primary organic carbon. Aerosol particle number concentration (condensation nuclei, CN) is overestimated by a factor 1.4 and 1.7 within PBL and FT, respectively. Model bias is most likely attributable to the uncertainties of primary particle emissions (mostly in the PBL) and to the nucleation rate. The overestimation of simulated cloud condensation nuclei (CCN) is more contained with respect to that of CN. The CCN efficiency, which is a measure of the ability of aerosol particles to nucleate cloud droplets, is underestimated by a factor of 1.5 and 3.8 in the PBL and FT, respectively. The comparison with MODIS data shows that the model overestimates the aerosol optical thickness (AOT). The domain averages (for

Effect of relative humidity on soot - secondary organic aerosol mixing: A case study from the Soot Aerosol Aging Study (PNNL-SAAS)

NASA Astrophysics Data System (ADS)

Sharma, N.; China, S.; Zaveri, R. A.; Shilling, J. E.; Pekour, M. S.; Liu, S.; Aiken, A. C.; Dubey, M. K.; Wilson, J. M.; Zelenyuk, A.; OBrien, R. E.; Moffet, R.; Gilles, M. K.; Gourihar, K.; Chand, D.; Sedlacek, A. J., III; Subramanian, R.; Onasch, T. B.; Laskin, A.; Mazzoleni, C.

2014-12-01

Atmospheric processing of fresh soot particles emitted by anthropogenic as well as natural sources alters their physical and chemical properties. For example, fresh and aged soot particles interact differently with incident solar radiation, resulting in different overall radiation budgets. Varying atmospheric chemical and meteorological conditions can result in complex soot mixing states. The Soot Aerosol Aging Study (SAAS) was conducted at the Pacific Northwest National Laboratory in November 2013 and January 2014 as a step towards understanding the evolution of mixing state of soot and its impact on climate-relevant properties. Aging experiments on diesel soot were carried out in a controlled laboratory chamber, and the effects of condensation and coagulation processes were systematically explored in separate sets of experiments. In addition to online measurement of aerosol properties, aerosol samples were collected for offline single particle analysis to investigate the evolution of the morphology, elemental composition and fine structure of sample particles from different experiments. Condensation experiments focused on the formation of α-pinene secondary organic aerosol on diesel soot aerosol seeds. Experiments were conducted to study the aging of soot under dry (RH < 2%) and humid conditions (RH ~ 80%). We present an analysis of the morphology of soot, its evolution, and its correlation with optical properties, as the condensation of α-pinene SOA is carried out for the two different RH conditions. The analysis was performed by using scanning electron microscopy, transmission electron microscopy, scanning transmission x-ray microscopy and atomic force microscopy for single particle characterization. In addition, particle size, mass, composition, shape, and density were characterized in-situ, as a function of organics condensed on soot seeds, using single particle mass spectrometer.