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Article ; Online: Cloud condensation nuclei activity of internally mixed particle populations at a remote marine free troposphere site in the North Atlantic Ocean.

Cheng, Zezhen / Morgenstern, Megan / Henning, Silvia / Zhang, Bo / Roberts, Gregory C / Fraund, Matthew / Marcus, Matthew A / Lata, Nurun Nahar / Fialho, Paulo / Mazzoleni, Lynn / Wehner, Birgit / Mazzoleni, Claudio / China, Swarup

The Science of the total environment

2023 Volume 904, Page(s) 166865

Abstract: This study reports results from research conducted at the Observatory of Mount Pico (OMP), 2225 m above mean sea level on Pico Island in the Azores archipelago in June and July 2017. We investigated the chemical composition, mixing state, and cloud ... ...

Abstract	This study reports results from research conducted at the Observatory of Mount Pico (OMP), 2225 m above mean sea level on Pico Island in the Azores archipelago in June and July 2017. We investigated the chemical composition, mixing state, and cloud condensation nuclei (CCN) activities of long-range transported free tropospheric (FT) particles. FLEXible PARTicle Lagrangian particle dispersion model (FLEXPART) simulations reveal that most air masses that arrived at the OMP during the sampling period originated in North America and were highly aged (average plume age > 10 days). We probed size-resolved chemical composition, mixing state, and hygroscopicity parameter (κ) of individual particles using computer-controlled scanning electron microscopy with an energy-dispersive X-ray spectrometer (CCSEM-EDX). Based on the estimated individual particle mass from elemental composition, we calculated the mixing state index, χ. During our study, FT particle populations were internally mixed (χ of samples are between 53 % and 87 %), owing to the long atmospheric aging time. We used data from a miniature Cloud Condensation Nucleus Counter (miniCCNC) to derive the hygroscopicity parameter, κ
Language	English
Publishing date	2023-09-09
Publishing country	Netherlands
Document type	Journal Article
ZDB-ID	121506-1
ISSN	1879-1026 ; 0048-9697
ISSN (online)	1879-1026
ISSN	0048-9697
DOI	10.1016/j.scitotenv.2023.166865
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Book ; Online: Experimental study of the aerosol impact on fog microphysics

Mazoyer, Marie / Burnet, Frédéric / Denjean, Cyrielle / Roberts, Gregory C. / Haeffelin, Martial / Dupont, Jean-Charles / Elias, Thierry

eISSN: 1680-7324

2019

Abstract: Comprehensive field campaigns dedicated to fog life cycle observation were conducted during the winters of 2010–2013 at the Instrumented Site for Atmospheric Remote Sensing Research (SIRTA) observatory in a suburb of Paris. In order to document their ... ...

Abstract	Comprehensive field campaigns dedicated to fog life cycle observation were conducted during the winters of 2010–2013 at the Instrumented Site for Atmospheric Remote Sensing Research (SIRTA) observatory in a suburb of Paris. In order to document their properties, in situ microphysical measurements collected during 23 fog events induced by both radiative cooling and stratus lowering are examined here. They reveal large variability in number, concentration and size of both aerosol background before the fog onset and fog droplets according to the different cases. The objective of this paper is to evaluate the impact of aerosol particles on the fog microphysics. To derive an accurate estimation of the actual activated fog droplet number concentration N act , we determine the hygroscopicity parameter κ , the dry and the wet critical diameter and the critical supersaturation for each case by using an iterative procedure based on the κ -Köhler theory that combines cloud condensation nuclei (CCN), dry particle and droplet size distribution measurements. Our study reveals low values of the derived critical supersaturation occurring in fog with a median of 0.043 %. Consequently, the median dry and wet activation diameters are 0.39 and 3.79 µ m, respectively, leading to a minor fraction of the aerosol population activated into droplets. The corresponding N act values are low, with median concentrations of 53.5 and 111 cm −3 within the 75th percentile. The activated fraction of aerosols exhibits remarkably low correlation with κ values, which reflects the chemical composition of the aerosols. On the contrary, the activated fraction exhibits a strong correlation with the inferred critical diameter throughout the field campaigns. This suggests that the variability in the activated fraction is mostly driven by particle size, while variations in aerosol composition are of secondary importance. Moreover, our analysis suggests that the supersaturation reached in fog could be lowered by the aerosol number concentration, which could contribute to the sink term of water vapor during the radiative cooling. Although radiative fogs are usually associated with higher aerosol loading than stratus-lowering events, our analysis also reveals that the activated fraction at the beginning of the event is similar for both types of fog. However, the evolution of the droplet concentration during the fog life cycle shows significant differences between both types of fog. This work demonstrates that an accurate calculation of supersaturation is required to provide a realistic representation of fog microphysical properties in numerical models.
Subject code	660
Language	English
Publishing date	2019-04-04
Publishing country	de
Document type	Book ; Online
Database	BASE - Bielefeld Academic Search Engine (life sciences selection)

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Book ; Online: Measurement report

Sanchez, Kevin J. / Roberts, Gregory C. / Saliba, Georges / Russell, Lynn M. / Twohy, Cynthia / Reeves, Michael J. / Humphries, Ruhi S. / Keywood, Melita D. / Ward, Jason P. / McRobert, Ian M.

eISSN: 1680-7324

Cloud processes and the transport of biological emissions affect southern ocean particle and cloud condensation nuclei concentrations

2021

Abstract: Long-range transport of biogenic emissions from the coast of Antarctica, precipitation scavenging, and cloud processing are the main processes that influence the observed variability in Southern Ocean (SO) marine boundary layer (MBL) condensation nuclei ( ...

Abstract	Long-range transport of biogenic emissions from the coast of Antarctica, precipitation scavenging, and cloud processing are the main processes that influence the observed variability in Southern Ocean (SO) marine boundary layer (MBL) condensation nuclei (CN) and cloud condensation nuclei (CCN) concentrations during the austral summer. Airborne particle measurements on the HIAPER GV from north–south transects between Hobart, Tasmania, and 62 ∘ S during the Southern Ocean Clouds, Radiation Aerosol Transport Experimental Study (SOCRATES) were separated into four regimes comprising combinations of high and low concentrations of CCN and CN. In 5 d HYSPLIT back trajectories, air parcels with elevated CCN concentrations were almost always shown to have crossed the Antarctic coast, a location with elevated phytoplankton emissions relative to the rest of the SO in the region south of Australia. The presence of high CCN concentrations was also consistent with high cloud fractions over their trajectory, suggesting there was substantial growth of biogenically formed particles through cloud processing. Cases with low cloud fraction, due to the presence of cumulus clouds, had high CN concentrations, consistent with previously reported new particle formation in cumulus outflow regions. Measurements associated with elevated precipitation during the previous 1.5 d of their trajectory had low CCN concentrations indicating CCN were effectively scavenged by precipitation. A coarse-mode fitting algorithm was used to determine the primary marine aerosol (PMA) contribution, which accounted for < 20 % of CCN (at 0.3 % supersaturation) and cloud droplet number concentrations. Vertical profiles of CN and large particle concentrations ( D p > 0.07 µ m) indicated that particle formation occurs more frequently above the MBL; however, the growth of recently formed particles typically occurs in the MBL, consistent with cloud processing and the condensation of volatile compound oxidation products. CCN measurements on the R/V Investigator as part of the second Clouds, Aerosols, Precipitation, Radiation and atmospheric Composition Over the southeRn Ocean (CAPRICORN-2) campaign were also conducted during the same period as the SOCRATES study. The R/V Investigator observed elevated CCN concentrations near Australia, likely due to continental and coastal biogenic emissions. The Antarctic coastal source of CCN from the south, CCN sources from the midlatitudes, and enhanced precipitation sink in the cyclonic circulation between the Ferrel and polar cells (around 60 ∘ S) create opposing latitudinal gradients in the CCN concentration with an observed minimum in the SO between 55 and 60 ∘ S. The SOCRATES airborne measurements are not influenced by Australian continental emissions but still show evidence of elevated CCN concentrations to the south of 60 ∘ S, consistent with biogenic coastal emissions. In addition, a latitudinal gradient in the particle composition, south of the Australian and Tasmanian coasts, is apparent in aerosol hygroscopicity derived from CCN spectra and aerosol particle size distribution. The particles are more hygroscopic to the north, consistent with a greater fraction of sea salt from PMA, and less hygroscopic to the south as there is more sulfate and organic particles originating from biogenic sources in coastal Antarctica.
Subject code	333
Language	English
Publishing date	2021-03-05
Publishing country	de
Document type	Book ; Online
Database	BASE - Bielefeld Academic Search Engine (life sciences selection)

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Book ; Online: Measurement report

Sanchez, Kevin J. / Roberts, Gregory C. / Saliba, Georges / Russell, Lynn M. / Twohy, Cynthia / Reeves, Michael J. / Humphries, Ruhi S. / Keywood, Melita D. / Ward, Jason P. / McRobert, Ian M.

eISSN: 1680-7324

Cloud Processes and the Transport of Biological Emissions Regulate Southern Ocean Particle and Cloud Condensation Nuclei Concentrations

2020

Abstract	Long-range transport of biogenic emissions from the coast of Antarctica, precipitation scavenging, and cloud processing are the main processes that influence the observed variability in Southern Ocean (SO) marine boundary layer (MBL) condensation nuclei (CN) and cloud condensation nuclei (CCN) concentrations during the austral summer. Airborne particle measurements on the HIAPER GV from north-south transects between Hobart, Tasmania and 62° S during the Southern Ocean Clouds, Radiation Aerosol Transport Experimental Study (SOCRATES) were separated into four regimes comprising combinations of high and low concentrations of CCN and CN. In 5-day HYSPLIT back trajectories, air parcels with elevated CCN concentrations were almost always shown to have crossed the Antarctic coast, a location with elevated phytoplankton emissions relative to the rest of the SO. The presence of high CCN concentrations was also consistent with high cloud fractions over their trajectory, suggesting there was substantial growth of biogenically formed particles through cloud processing. Cases with low cloud fraction, due to the presence of cumulus clouds, had high CN concentrations, consistent with previously reported new particle formation in cumulus outflow regions. Measurements associated with elevated precipitation during the previous 1.5-days of their trajectory had low CCN concentrations indicating CCN were effectively scavenged by precipitation. A course-mode fitting algorithm was used to determine the primary marine aerosol (PMA) contribution which accounted for < 20 % of CCN (at 0.3 % supersaturation) and cloud droplet number concentrations. Vertical profiles of CN and large particle concentrations (D p > 0.07 µm) indicated that particle formation occurs more frequently above the MBL; however, the growth of recently formed particles typically occurs in the MBL, consistent with cloud processing and the condensation of volatile compound oxidation products. CCN measurements on the R/V Investigator as part of the second Clouds, Aerosols, Precipitation, Radiation and atmospheric Composition Over the southeRn Ocean (CAPRICORN-2) campaign were also conducted during the same period as the SOCRATES study. The R/V Investigator observed elevated CCN concentrations near Australia, likely due to continental and coastal biogenic emissions. The Antarctic coastal source of CCN from the south as well as CCN sources from the mid-latitudes create a latitudinal gradient in CCN concentration with an observed minimum in the SO between 55° S and 60° S. The SOCRATES airborne measurements are not influenced by Australian continental emissions, but still show evidence of elevated CCN concentrations to the south of 60° S, consistent with biogenic coastal emissions. In addition, a latitudinal gradient in the particle composition is observed; more hygroscopic particles to the north, consistent with a greater fraction of sea salt from PMA, and more sulfate and organic particles to the south, which are likely from biogenic sources in coastal Antarctica.
Subject code	551
Language	English
Publishing date	2020-09-11
Publishing country	de
Document type	Book ; Online
Database	BASE - Bielefeld Academic Search Engine (life sciences selection)

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Article ; Online: Multi-campaign ship and aircraft observations of marine cloud condensation nuclei and droplet concentrations.

Sanchez, Kevin J / Painemal, David / Brown, Matthew D / Crosbie, Ewan C / Gallo, Francesca / Hair, Johnathan W / Hostetler, Chris A / Jordan, Carolyn E / Robinson, Claire E / Scarino, Amy Jo / Shingler, Taylor J / Shook, Michael A / Thornhill, Kenneth L / Wiggins, Elizabeth B / Winstead, Edward L / Ziemba, Luke D / Chambers, Scott / Williams, Alastair / Humphries, Ruhi S /

Scientific data

2023 Volume 10, Issue 1, Page(s) 471

Abstract: In-situ marine cloud droplet number concentrations (CDNCs), cloud condensation nuclei (CCN), and CCN proxies, based on particle sizes and optical properties, are accumulated from seven field campaigns: ACTIVATE; NAAMES; ... ...

Abstract	In-situ marine cloud droplet number concentrations (CDNCs), cloud condensation nuclei (CCN), and CCN proxies, based on particle sizes and optical properties, are accumulated from seven field campaigns: ACTIVATE; NAAMES; CAMP
Language	English
Publishing date	2023-07-20
Publishing country	England
Document type	Dataset ; Journal Article
ZDB-ID	2775191-0
ISSN	2052-4463 ; 2052-4463
ISSN (online)	2052-4463
ISSN	2052-4463
DOI	10.1038/s41597-023-02372-z
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Article ; Online: Measurements of aerosol chemistry during new particle formation events at a remote rural mountain site.

Creamean, Jessie M / Ault, Andrew P / Ten Hoeve, John E / Jacobson, Mark Z / Roberts, Gregory C / Prather, Kimberly A

Environmental science & technology

2011 Volume 45, Issue 19, Page(s) 8208–8216

Abstract: Determining the major sources of particles that act as cloud condensation nuclei (CCN) represents a critical step in the development of a more fundamental understanding of aerosol impacts on cloud formation and climate. Reported herein are direct ... ...

Abstract	Determining the major sources of particles that act as cloud condensation nuclei (CCN) represents a critical step in the development of a more fundamental understanding of aerosol impacts on cloud formation and climate. Reported herein are direct measurements of the CCN activity of newly formed ambient particles, measured at a remote rural site in the Sierra Nevada Mountains of Northern California. Nucleation events in the winter of 2009 occurred during two pristine periods following precipitation, with higher gas-phase SO(2) concentrations during the second period, when faster particle growth occurred (7-8 nm/h). Amines, as opposed to ammonia, and sulfate were detected in the particle phase throughout new particle formation (NPF) events, increasing in number as the particles grew to larger sizes. Interestingly, long-range transport of SO(2) from Asia appeared to potentially play a role in NPF during faster particle growth. Understanding the propensity of newly formed particles to act as CCN is critical for predicting the effects of NPF on orographic cloud formation during winter storms along the Sierra Nevada Mountain range. The potential impact of newly formed particles in remote regions needs to be compared with that of transported urban aerosols when evaluating the impact of aerosols on clouds and climate.
MeSH term(s)	Aerosols/chemistry ; California ; Chemistry Techniques, Analytical/methods ; Ecosystem ; Gases/chemistry ; Mass Spectrometry ; Meteorological Concepts ; Particle Size ; Particulate Matter/chemistry ; Rural Population ; Sulfates/chemistry ; Time Factors
Chemical Substances	Aerosols ; Gases ; Particulate Matter ; Sulfates
Language	English
Publishing date	2011-10-01
Publishing country	United States
Document type	Journal Article
ISSN	1520-5851
ISSN (online)	1520-5851
DOI	10.1021/es103692f
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article: Effect of organic compounds on cloud condensation nuclei (CCN) activity of sea spray aerosol produced by bubble bursting

Moore, Meagan J.K / Furutani, Hiroshi / Roberts, Gregory C / Moffet, Ryan C / Gilles, Mary K / Palenik, Brian / Prather, Kimberly A

Atmospheric environment. 2011 Dec., v. 45, no. 39

2011

Abstract: The ocean comprises over 70% of the surface of the earth and thus sea spray aerosols generated by wave processes represent a critical component of our climate system. The manner in which different complex oceanic mixtures of organic species and inorganic ...

Abstract	The ocean comprises over 70% of the surface of the earth and thus sea spray aerosols generated by wave processes represent a critical component of our climate system. The manner in which different complex oceanic mixtures of organic species and inorganic salts are distributed between individual particles in sea spray directly determines which particles will effectively form cloud nuclei. Controlled laboratory experiments were undertaken to better understand the full range of particle properties produced by bubbling solutions composed of simplistic model organic species, oleic acid and sodium dodecyl sulfate (SDS), mixed with NaCl to more complex artificial seawater mixed with complex organic mixtures produced by common oceanic microorganisms. Simple mixtures of NaCl and oleic acid or SDS had a significant effect on CCN activity, even in relatively small amounts. However, an artificial seawater (ASW) solution containing microorganisms, the common cyanobacteria (Synechococcus) and DMS-producing green algae (Ostreococcus), produced particles containing ∼34 times more carbon than the particles produced from pure ASW, yet no significant change was observed in the overall CCN activity. We hypothesize that these microorganisms produce diverse mixtures of organic species with a wide range of properties that produced offsetting effects, leading to no net change in the overall average measured hygroscopicity of the collection of sea spray particles. Based on these observations, changes in CCN activity due to “bloom” conditions would be predicted to lead to small changes in the average CCN activity, and thus have a negligible impact on cloud formation. However, each sea spray particle will contain a broad spectrum of different species, and thus further studies are needed of the CCN activity of individual sea spray particles and biological processes under a wide range of controllable conditions.
Keywords	Chlorophycota ; Synechococcus ; aerosols ; atmospheric chemistry ; carbon ; climate ; condensation ; hygroscopicity ; laboratory experimentation ; microorganisms ; oleic acid ; seawater ; sodium chloride ; sodium dodecyl sulfate
Language	English
Dates of publication	2011-12
Size	p. 7462-7469.
Publishing place	Elsevier Ltd
Document type	Article
ZDB-ID	216368-8
ISSN	0004-6981 ; 1352-2310
ISSN	0004-6981 ; 1352-2310
DOI	10.1016/j.atmosenv.2011.04.034
Database	NAL-Catalogue (AGRICOLA)

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Article ; Online: Bringing the ocean into the laboratory to probe the chemical complexity of sea spray aerosol.

Prather, Kimberly A / Bertram, Timothy H / Grassian, Vicki H / Deane, Grant B / Stokes, M Dale / Demott, Paul J / Aluwihare, Lihini I / Palenik, Brian P / Azam, Farooq / Seinfeld, John H / Moffet, Ryan C / Molina, Mario J / Cappa, Christopher D / Geiger, Franz M / Roberts, Gregory C / Russell, Lynn M / Ault, Andrew P / Baltrusaitis, Jonas / Collins, Douglas B /

Corrigan, Craig E / Cuadra-Rodriguez, Luis A / Ebben, Carlena J / Forestieri, Sara D / Guasco, Timothy L / Hersey, Scott P / Kim, Michelle J / Lambert, William F / Modini, Robin L / Mui, Wilton / Pedler, Byron E / Ruppel, Matthew J / Ryder, Olivia S / Schoepp, Nathan G / Sullivan, Ryan C / Zhao, Defeng

Proceedings of the National Academy of Sciences of the United States of America

2013 Volume 110, Issue 19, Page(s) 7550–7555

Abstract: The production, size, and chemical composition of sea spray aerosol (SSA) particles strongly depend on seawater chemistry, which is controlled by physical, chemical, and biological processes. Despite decades of studies in marine environments, a direct ... ...

Abstract	The production, size, and chemical composition of sea spray aerosol (SSA) particles strongly depend on seawater chemistry, which is controlled by physical, chemical, and biological processes. Despite decades of studies in marine environments, a direct relationship has yet to be established between ocean biology and the physicochemical properties of SSA. The ability to establish such relationships is hindered by the fact that SSA measurements are typically dominated by overwhelming background aerosol concentrations even in remote marine environments. Herein, we describe a newly developed approach for reproducing the chemical complexity of SSA in a laboratory setting, comprising a unique ocean-atmosphere facility equipped with actual breaking waves. A mesocosm experiment was performed in natural seawater, using controlled phytoplankton and heterotrophic bacteria concentrations, which showed SSA size and chemical mixing state are acutely sensitive to the aerosol production mechanism, as well as to the type of biological species present. The largest reduction in the hygroscopicity of SSA occurred as heterotrophic bacteria concentrations increased, whereas phytoplankton and chlorophyll-a concentrations decreased, directly corresponding to a change in mixing state in the smallest (60-180 nm) size range. Using this newly developed approach to generate realistic SSA, systematic studies can now be performed to advance our fundamental understanding of the impact of ocean biology on SSA chemical mixing state, heterogeneous reactivity, and the resulting climate-relevant properties.
MeSH term(s)	Aerosols/chemistry ; Atmosphere/chemistry ; Bacteria/metabolism ; Chlorophyll/chemistry ; Chlorophyll A ; Ecology ; Oceanography ; Oceans and Seas ; Phytoplankton/metabolism ; Seawater/chemistry
Chemical Substances	Aerosols ; Chlorophyll (1406-65-1) ; Chlorophyll A (YF5Q9EJC8Y)
Language	English
Publishing date	2013-04-25
Publishing country	United States
Document type	Journal Article ; Research Support, Non-U.S. Gov't ; Research Support, U.S. Gov't, Non-P.H.S.
ZDB-ID	209104-5
ISSN	1091-6490 ; 0027-8424
ISSN (online)	1091-6490
ISSN	0027-8424
DOI	10.1073/pnas.1300262110
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Article: Effect of organic compounds on cloud condensation nuclei (CCN) activity of sea spray aerosol produced by bubble bursting

Moore, Meagan J.K. / Furutani, Hiroshi / Roberts, Gregory C. / Moffet, Ryan C. / Gilles, Mary K. / Palenik, Brian / Prather, Kimberly A.

Atmospheric environment

Volume v. 45,, Issue no. 3

Abstract	The ocean comprises over 70% of the surface of the earth and thus sea spray aerosols generated by wave processes represent a critical component of our climate system. The manner in which different complex oceanic mixtures of organic species and inorganic salts are distributed between individual particles in sea spray directly determines which particles will effectively form cloud nuclei. Controlled laboratory experiments were undertaken to better understand the full range of particle properties produced by bubbling solutions composed of simplistic model organic species, oleic acid and sodium dodecyl sulfate (SDS), mixed with NaCl to more complex artificial seawater mixed with complex organic mixtures produced by common oceanic microorganisms. Simple mixtures of NaCl and oleic acid or SDS had a significant effect on CCN activity, even in relatively small amounts. However, an artificial seawater (ASW) solution containing microorganisms, the common cyanobacteria (Synechococcus) and DMS-producing green algae (Ostreococcus), produced particles containing ∼34 times more carbon than the particles produced from pure ASW, yet no significant change was observed in the overall CCN activity. We hypothesize that these microorganisms produce diverse mixtures of organic species with a wide range of properties that produced offsetting effects, leading to no net change in the overall average measured hygroscopicity of the collection of sea spray particles. Based on these observations, changes in CCN activity due to “bloom” conditions would be predicted to lead to small changes in the average CCN activity, and thus have a negligible impact on cloud formation. However, each sea spray particle will contain a broad spectrum of different species, and thus further studies are needed of the CCN activity of individual sea spray particles and biological processes under a wide range of controllable conditions.
Keywords	seawater ; sodium chloride ; condensation ; oleic acid ; Synechococcus ; atmospheric chemistry ; sodium dodecyl sulfate ; carbon ; aerosols ; laboratory experimentation ; Chlorophycota ; climate ; hygroscopicity ; microorganisms
Language	English
Document type	Article
ISSN	1352-2310
Database	AGRIS - International Information System for the Agricultural Sciences and Technology

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