scholarly journals Corrigendum to "Size-resolved observations of refractory black carbon particles in cloud droplets at a marine boundary layer site" published in Atmos. Chem. Phys., 15, 1367–1383, 2015

2015 ◽  
Vol 15 (3) ◽  
pp. 1487-1487
Author(s):  
J. C. Schroder ◽  
S. J. Hanna ◽  
R. L. Modini ◽  
A. L. Corrigan ◽  
S. M. Kreidenweis ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Black Carbon ◽  
Marine Boundary Layer ◽  
Chem Phys ◽  
Cloud Droplets ◽  
Carbon Particles

scholarly journals Size-resolved observations of refractory black carbon particles in cloud droplets at a marine boundary layer site

2014 ◽  
Vol 14 (8) ◽  
pp. 11447-11491 ◽  
Author(s):  
J. C. Schroder ◽  
S. J. Hanna ◽  
R. L. Modini ◽  
A. L. Corrigan ◽  
A. M. Macdonald ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Black Carbon ◽  
Marine Boundary Layer ◽  
Back Trajectory ◽  
Cloud Droplets ◽  
Back Trajectories ◽  
Air Masses ◽  
Carbon Particles ◽  
Back Trajectory Analysis ◽  
La Jolla

Abstract. Size resolved observations of aerosol particles (including black carbon particles) and cloud residuals were studied at a marine boundary layer site (251 m a.m.s.l.) in La Jolla, CA during 2012. A counterflow virtual impactor was used to sample cloud residuals while a total inlet was used to sample both cloud residuals and interstitial particles. Two cloud events totaling ten hours of in-cloud sampling were analyzed. Since the CVI only sampled cloud droplets larger than ≈11 μm, less than 100% of the cloud droplets were sampled during the two cloud events (≈38% of the cloud droplets for the first cloud event and ≈24% of the cloud droplets for the second cloud were sampled). Back trajectories showed that air masses for both cloud events spent at least 96 h over the Pacific Ocean and traveled near, or over populated regions just before sampling. Based on bulk aerosol particle concentrations measured from the total inlet the two air masses sampled were classified as polluted marine air, a classification that was consistent with back trajectory analysis and the mass concentrations of refractory black carbon (rBC) measured from the total inlet. The activated fraction of rBC, estimated from the measurements, ranged from 0.01 to 0.1 for core diameters ranging from 70 to 220 nm. Since the fraction of cloud droplets sampled by the CVI was less than 100%, the measured activated fractions of rBC should be considered as lower limits to the total fraction of rBC activated during the two cloud events. Size distributions of rBC sampled from the residual inlet show that sub-100 nm rBC cores were incorporated into the droplets in both clouds. The coating analysis shows that the rBC cores had average coating thicknesses of 75 nm for core diameters of 70 nm and 29 nm for core diameters of 220 nm. The presence of sub-100 nm rBC cores in the cloud residuals is consistent with kappa-Köhler theory and the measured coating thicknesses of the rBC cores.

scholarly journals Size-resolved observations of refractory black carbon particles in cloud droplets at a marine boundary layer site

2015 ◽  
Vol 15 (3) ◽  
pp. 1367-1383 ◽  
Author(s):  
J. C. Schroder ◽  
S. J. Hanna ◽  
R. L. Modini ◽  
A. L. Corrigan ◽  
S. M. Kreidenwies ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Black Carbon ◽  
Marine Boundary Layer ◽  
Volume Fraction ◽  
Particle Diameter ◽  
Cloud Droplet ◽  
Cloud Droplets ◽  
Back Trajectories ◽  
Carbon Particles ◽  
La Jolla

Abstract. Size-resolved observations of aerosol particles and cloud droplet residuals were studied at a marine boundary layer site (251 m a.m.s.l.) in La Jolla, San Diego, California, during 2012. A counterflow virtual impactor (CVI) was used as the inlet to sample cloud residuals while a total inlet was used to sample both cloud residuals and interstitial particles. Two cloud events totaling 10 h of in-cloud sampling were analyzed. Based on bulk aerosol particle concentrations, mass concentrations of refractory black carbon (rBC), and back trajectories, the two air masses sampled were classified as polluted marine air. Since the fraction of cloud droplets sampled by the CVI was less than 100%, the measured activated fractions of rBC should be considered as lower limits to the total fraction of rBC activated during the two cloud events. Size distributions of rBC and a coating analysis showed that sub-100 nm rBC cores with relatively thick coatings were incorporated into the cloud droplets (i.e., 95 nm rBC cores with median coating thicknesses of at least 65 nm were incorporated into the cloud droplets). Measurements also show that the coating volume fraction of rBC cores is relatively large for sub-100 nm rBC cores. For example, the median coating volume fraction of 95 nm rBC cores incorporated into cloud droplets was at least 0.9, a result that is consistent with κ-Köhler theory. Measurements of the total diameter of the rBC-containing particles (rBC core and coating) suggest that the total diameter of rBC-containing particles needed to be at least 165 nm to be incorporated into cloud droplets when the core rBC diameter is ≥ 85 nm. This result is consistent with previous work that has shown that particle diameter is important for activation of non-rBC particles. The activated fractions of rBC determined from the measurements ranged from 0.01 to 0.1 for core rBC diameters ranging from 70 to 220 nm. This type of data is useful for constraining models used for predicting rBC concentrations in the atmosphere.

scholarly journals Modeling the smoky troposphere of the southeast Atlantic: a comparison to ORACLES airborne observations from September of 2016

2020 ◽  
Vol 20 (19) ◽  
pp. 11491-11526 ◽  
Author(s):  
Yohei Shinozuka ◽  
Pablo E. Saide ◽  
Gonzalo A. Ferrada ◽  
Sharon P. Burton ◽  
Richard Ferrare ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Optical Properties ◽  
Black Carbon ◽  
Marine Boundary Layer ◽  
Organic Aerosol ◽  
Airborne Lidar ◽  
Aerosol Mass ◽  
Wide Range ◽  
Smoke Layer ◽  
Mass Concentrations

Abstract. In the southeast Atlantic, well-defined smoke plumes from Africa advect over marine boundary layer cloud decks; both are most extensive around September, when most of the smoke resides in the free troposphere. A framework is put forth for evaluating the performance of a range of global and regional atmospheric composition models against observations made during the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) airborne mission in September 2016. A strength of the comparison is a focus on the spatial distribution of a wider range of aerosol composition and optical properties than has been done previously. The sparse airborne observations are aggregated into approximately 2∘ grid boxes and into three vertical layers: 3–6 km, the layer from cloud top to 3 km, and the cloud-topped marine boundary layer. Simulated aerosol extensive properties suggest that the flight-day observations are reasonably representative of the regional monthly average, with systematic deviations of 30 % or less. Evaluation against observations indicates that all models have strengths and weaknesses, and there is no single model that is superior to all the others in all metrics evaluated. Whereas all six models typically place the top of the smoke layer within 0–500 m of the airborne lidar observations, the models tend to place the smoke layer bottom 300–1400 m lower than the observations. A spatial pattern emerges, in which most models underestimate the mean of most smoke quantities (black carbon, extinction, carbon monoxide) on the diagonal corridor between 16∘ S, 6∘ E, and 10∘ S, 0∘ E, in the 3–6 km layer, and overestimate them further south, closer to the coast, where less aerosol is present. Model representations of the above-cloud aerosol optical depth differ more widely. Most models overestimate the organic aerosol mass concentrations relative to those of black carbon, and with less skill, indicating model uncertainties in secondary organic aerosol processes. Regional-mean free-tropospheric model ambient single scattering albedos vary widely, between 0.83 and 0.93 compared with in situ dry measurements centered at 0.86, despite minimal impact of humidification on particulate scattering. The modeled ratios of the particulate extinction to the sum of the black carbon and organic aerosol mass concentrations (a mass extinction efficiency proxy) are typically too low and vary too little spatially, with significant inter-model differences. Most models overestimate the carbonaceous mass within the offshore boundary layer. Overall, the diversity in the model biases suggests that different model processes are responsible. The wide range of model optical properties requires further scrutiny because of their importance for radiative effect estimates.

scholarly journals Black carbon in the marine boundary layer over the North Atlantic and seas of the Russian arctic in june-september 2017

2019 ◽  
Vol 59 (5) ◽  
pp. 771-776
Author(s):  
V. P. Shevchenko ◽  
V. M. Kopeikin ◽  
A. N. Novigatsky ◽  
G. V. Malafeev
Keyword(s):  
Boundary Layer ◽  
Black Carbon ◽  
North Atlantic ◽  
Marine Boundary Layer ◽  
The Arctic ◽  
Air Masses ◽  
South Eastern ◽  
The North ◽  
The North Atlantic ◽  
Eastern Baltic

The paper presents the results of a study of the concentrations of black carbon in the marine boundary layer over the Baltic and North Seas, the North Atlantic, the Norwegian, the Barents, the Kara and the Laptev seas from June 30 to September 29, 2017 in the 68th and 69th voyages of research vessel "Akademik Mstislav Keldysh". Black carbon has a significant impact on climate change and the degree of pollution of the Arctic. Black carbon is formed as a result of incomplete combustion of fossil fuels (primarily coal, oil) and biomass or biofuel. It consists of submicron particles and their aggregates and can be transported a great distance from the source. Samples were taken by pumping air for 46 hours through quartz filters Hahnemule at an altitude of 10 m above sea level in a headwind to prevent smoke of the vessel from entering the filters. Subsequently, the black carbon content was determined in the laboratory by the aetalometric method. The backward trajectories of the air mass transfer and the black carbon particles transported by them to the sampling points were calculated using the HYSPLIT (Hybrid Single-Particle Lagrangian Integrated Trajectory) model at http://www.arl.noaa.gov/ready.html. The conducted studies show low values of black carbon concentrations (50 ng/m3) along the expedition route when air masses came from the background areas of the North Atlantic and the Arctic. High concentrations of black carbon (100200 ng/m3 and higher) are characteristic for areas with active navigation (the South-Eastern Baltic, the North Sea) and near ports (eg Reykjavik), as well as for incoming air masses from the industrialized regions of Europe to South-Eastern Baltic and from areas of oil and gas fields where associated gas is flared (the North, the Norwegian and the Kara seas).

scholarly journals Black carbon concentrations and sources in the marine boundary layer of the tropical Atlantic Ocean using four methodologies

2014 ◽  
Vol 14 (14) ◽  
pp. 7431-7443 ◽  
Author(s):  
K. Pohl ◽  
M. Cantwell ◽  
P. Herckes ◽  
R. Lohmann
Keyword(s):  
Boundary Layer ◽  
South America ◽  
Atlantic Ocean ◽  
Black Carbon ◽  
Marine Boundary Layer ◽  
Caribbean Sea ◽  
Tropical Atlantic ◽  
Carbonaceous Aerosols ◽  
The Caribbean ◽  
Carbon Concentrations

Abstract. Combustion-derived aerosols in the marine boundary layer have been poorly studied, especially in remote environments such as the open Atlantic Ocean. The tropical Atlantic has the potential to contain a high concentration of aerosols, such as black carbon, due to the African emission plume of biomass and agricultural burning products. Atmospheric particulate matter samples across the tropical Atlantic boundary layer were collected in the summer of 2010 during the southern hemispheric dry season when open fire events were frequent in Africa and South America. The highest black carbon concentrations were detected in the Caribbean Sea and within the African plume, with a regional average of 0.6 μg m−3 for both. The lowest average concentrations were measured off the coast of South America at 0.2 to 0.3 μg m−3. Samples were quantified for black carbon using multiple methods to provide insights into the form and stability of the carbonaceous aerosols (i.e., thermally unstable organic carbon, soot like, and charcoal like). Soot-like aerosols composed up to 45% of the carbonaceous aerosols in the Caribbean Sea to as little as 4% within the African plume. Charcoal-like aerosols composed up to 29% of the carbonaceous aerosols over the oligotrophic Sargasso Sea, suggesting that non-soot-like particles could be present in significant concentrations in remote environments. To better apportion concentrations and forms of black carbon, multiple detection methods should be used, particularly in regions impacted by biomass burning emissions.

scholarly journals Ultraclean Layers and Optically Thin Clouds in the Stratocumulus-to-Cumulus Transition. Part II: Depletion of Cloud Droplets and Cloud Condensation Nuclei through Collision–Coalescence

2018 ◽  
Vol 75 (5) ◽  
pp. 1653-1673 ◽  
Author(s):  
Kuan-Ting O ◽  
Robert Wood ◽  
Christopher S. Bretherton
Keyword(s):  
Boundary Layer ◽  
Marine Boundary Layer ◽  
Cloud Condensation Nuclei ◽  
Cloud Droplet ◽  
Liquid Water Content ◽  
Cloud Base ◽  
Condensation Nuclei ◽  
Cloud Droplets ◽  
Droplet Concentration ◽  
Cloud Thickness

In Part I, aircraft observations are used to show that ultraclean layers (UCLs) in the marine boundary layer (MBL) are a common feature of the stratocumulus-to-cumulus transition (SCT) region over the northeast Pacific. The ultraclean layers are defined as layers of either cloud or clear air in which the concentration of particles with diameter larger than 0.1 μm is below 10 cm−3. Here, idealized microphysical parcel modeling shows that in the cumulus regime, collision–coalescence can strongly deplete cloud droplet concentration in cumulus (Cu) updrafts, thereby removing cloud condensation nuclei (CCN) from the atmosphere, suggesting that collision scavenging is likely the key process causing the low particle concentration in UCLs. Furthermore, the model results suggest that the stratocumulus regime is typically not favorable for UCL formation, because condensate amounts are generally not large enough to deplete drops in the time it takes to loft air to the upper planetary boundary layer (PBL). A bulk parameterization of the coalescence-scavenging rate is derived based on in situ measurements. The fractional coalescence-scavenging rate is found to be strongly dependent upon liquid water content (LWC) and, hence, the height above cloud base, indicating that a higher cloud top and thus a greater cloud thickness in a Cu updraft is an important factor accounting for the observed sharp rise of UCL coverage in the SCT region. An important implication is that PBL height, which controls maximum cloud thickness, and therefore LWC in updrafts, could be a crucial factor constraining coalescence scavenging and thus the formation of UCLs in the MBL.

scholarly journals The first steps of iodine gas-to-particle conversion as seen in the lab: constraints on the role of iodine oxides and oxyacids

2020 ◽  
Author(s):  
Juan Carlos Gomez Martin ◽  
Tom Lewis ◽  
Manoj Kumar ◽  
John Plane ◽  
Joseph Francisco ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Gas Phase ◽  
Marine Boundary Layer ◽  
Oxide Particle ◽  
Molecular Iodine ◽  
Chem Phys ◽  
Particle Formation ◽  
Atmospheric Modeling ◽  
Atmospheric Environment ◽  
Iodine Oxides

<p>The photooxidation of gas phase iodine-bearing molecules emitted by marine biota leads to intense particle nucleation events in the coastal and polar marine boundary layer<sup>1-3</sup>. The ubiquity of iodine in the marine atmospheric environment<sup>4-7</sup> has suggested that this may be a previously unrecognized global source of new aerosol particles<sup>8</sup>. Atmospheric modeling is required in order to evaluate the importance of this process, but a substantial lack of understanding of the gas-to-particle conversion mechanism is hindering this effort, especially regarding the gas phase chemistry of the nucleating molecules (iodine oxides<sup>9</sup><sup>,</sup><sup>10</sup> and/or oxyacids<sup>7</sup>) and the formation kinetics of molecular clusters. To address this problem, we have conducted new flow tube laboratory experiments where pulsed laser photolysis or continuous broad-band photolysis of I<sub>2</sub>/O<sub>3</sub> mixtures  in air are used to generate iodine radicals in the presence of atmospherically representative mixing ratios of water vapor. The molecular reactants and the resulting molecular products are detected by time-resolved VUV laser photo-ionization time-of-flight mass spectrometry. High-level quantum chemistry and master equation calculations and gas kinetics modelling are used to analyse the experimental data. In this presentation we discuss our results and their implications for the interpretation of field meassurements and for the implementatiion of an iodine oxide particle formation mechanism in atmospheric models.</p><p>References:</p><p>1. Hoffmann, T., O'Dowd, C. D. & Seinfeld, J. H. Iodine oxide homogeneous nucleation: An explanation for coastal new particle production. Geophys. Res. Lett. <strong>28</strong>, 1949-1952 (2001).</p><p>2. McFiggans, G. et al. Direct evidence for coastal iodine particles from Laminaria macroalgae - linkage to emissions of molecular iodine. Atmos. Chem. Phys. <strong>4</strong>, 701-713 (2004).</p><p>3. O'Dowd, C. D. et al. Marine aerosol formation from biogenic iodine emissions. Nature <strong>417</strong>, 632-636 (2002).</p><p>4. Prados-Roman, C. et al. Iodine oxide in the global marine boundary layer. Atmos. Chem. Phys. <strong>15</strong>, 583-593, doi:10.5194/acp-15-583-2015 (2015).</p><p>5. Schönhardt, A. et al. Simultaneous satellite observations of IO and BrO over Antarctica. Atmos. Chem. Phys. <strong>12</strong>, 6565-6580, doi:10.5194/acp-12-6565-2012 (2012).</p><p>6. Mahajan, A. S. et al. Concurrent observations of atomic iodine, molecular iodine and ultrafine particles in a coastal environment. Atmos. Chem. Phys. <strong>10</strong>, 27227-27253 (2010).</p><p>7. Sipilä, M. et al. Molecular-scale evidence of aerosol particle formation via sequential addition of HIO3. Nature <strong>537</strong>, 532-534, doi:10.1038/nature19314 (2016).</p><p>8. Saiz-Lopez, A. et al. Atmospheric Chemistry of Iodine. Chem. Rev. <strong>112</strong>, 1773–1804, doi:DOI: 10.1021/cr200029u (2012).</p><p>9. Gómez Martín, J. C. et al. On the mechanism of iodine oxide particle formation. Phys. Chem. Chem. Phys. <strong>15</strong>, 15612-15622, doi:10.1039/c3cp51217g (2013).</p><p>10. Saunders, R. W., Mahajan, A. S., Gómez Martín, J. C., Kumar, R. & Plane, J. M. C. Studies of the Formation and Growth of Aerosol from Molecular Iodine Precursor. Z. Phys. Chem. <strong>224</strong>, 1095-1117 (2010).</p>

scholarly journals Heterogeneous nucleation of water vapor on different types of black carbon particles

2020 ◽  
Author(s):  
Ari Laaksonen ◽  
Jussi Malila ◽  
Athanasios Nenes
Keyword(s):  
Water Vapor ◽  
Black Carbon ◽  
Heterogeneous Nucleation ◽  
Hydrological Cycle ◽  
Quantitative Description ◽  
Nucleation Theory ◽  
Cloud Formation ◽  
Cloud Droplets ◽  
Carbon Particles ◽  
Different Types

Abstract. Heterogeneous nucleation of water vapor on insoluble particles affects cloud formation, precipitation, the hydrological cycle and climate. Despite its importance, heterogeneous nucleation remains a poorly understood phenomenon that relies heavily on empirical information for its quantitative description. Here, we examine heterogeneous nucleation of water vapor on and cloud drop activation of different types of soots, both pure black carbon particles, and black carbon particles mixed with secondary organic matter. We show that the recently developed adsorption nucleation theory quantitatively predicts the nucleation of water and droplet formation upon particles of the various soot types. A surprising consequence of this new understanding is that, with sufficient adsorption site density, soot particles can activate into cloud droplets – even when completely lacking any soluble material.

scholarly journals Heterogeneous nucleation of water vapor on different types of black carbon particles

2020 ◽  
Vol 20 (21) ◽  
pp. 13579-13589
Author(s):  
Ari Laaksonen ◽  
Jussi Malila ◽  
Athanasios Nenes
Keyword(s):  
Water Vapor ◽  
Black Carbon ◽  
Heterogeneous Nucleation ◽  
Hydrological Cycle ◽  
Quantitative Description ◽  
Nucleation Theory ◽  
Cloud Formation ◽  
Cloud Droplets ◽  
Carbon Particles ◽  
Different Types

Abstract. The heterogeneous nucleation of water vapor on insoluble particles affects cloud formation, precipitation, the hydrological cycle, and climate. Despite its importance, heterogeneous nucleation remains a poorly understood phenomenon that relies heavily on empirical information for its quantitative description. Here, we examine the heterogeneous nucleation of water vapor on different types of soots as well as cloud drop activation of different types of soots, including both pure black carbon particles and black carbon particles mixed with secondary organic matter. We show that the recently developed adsorption nucleation theory quantitatively predicts the nucleation of water and droplet formation upon particles of the various soot types. A surprising consequence of this new understanding is that, with sufficient adsorption site density, soot particles can activate into cloud droplets – even when completely lacking any soluble material.

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