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 ◽  
...  

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.

2015 ◽  
Vol 15 (3) ◽  
pp. 1367-1383 ◽  
Author(s):  
J. C. Schroder ◽  
S. J. Hanna ◽  
R. L. Modini ◽  
A. L. Corrigan ◽  
S. M. Kreidenwies ◽  
...  

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.


2019 ◽  
Vol 59 (5) ◽  
pp. 771-776
Author(s):  
V. P. Shevchenko ◽  
V. M. Kopeikin ◽  
A. N. Novigatsky ◽  
G. V. Malafeev

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).


2006 ◽  
Vol 6 (6) ◽  
pp. 11209-11246
Author(s):  
L. Sogacheva ◽  
A. Hamed ◽  
M. C. Facchini ◽  
M. Kulmala ◽  
A. Laaksonen

Abstract. In this paper, we study the transport of air mass to San Pietro Capofiume (SPC) in Po Valley, Italy, by means of back trajectory analysis. Our main aim is to investigate whether air masses originate from different regions on nucleation event days and on nonevent days, during three years when nucleation events have been continuously recorded at SPC. The results indicate that nucleation events occur frequently in air masses arriving form Central Europe, whereas event frequency is much lower in air transported from southern directions and from the Atlantic Ocean. We also analyzed the behaviour of meteorological parameters during 96 h transport to SPC, and found that on average, event trajectories undergo stronger subsidence during the last 12 h before the arrival at SPC than nonevent trajectories. This causes a reversal in the temperature and relative humidity (RH) differences between event and nonevent trajectories: between 96 and 12 h back time, temperatures are lower and RH's higher for event than nonevent trajectories and between 12 and 0 h vice versa. Boundary layer mixing is stronger along the event trajectories compared to nonevent trajectories. The absolute humidity (AH) is similar for the event and nonevent trajectories between about 96 h and about 60 h back time, but after that, the event trajectories AH becomes lower due to stronger rain. We also studied transport of SO2 to SPC, and conclude that although sources in Po Valley most probably dominate the measured concentrations, certain Central and Eastern European sources can also have a non-negligible contribution.


2015 ◽  
Vol 96 (3) ◽  
pp. 419-440 ◽  
Author(s):  
Robert Wood ◽  
Matthew Wyant ◽  
Christopher S. Bretherton ◽  
Jasmine Rémillard ◽  
Pavlos Kollias ◽  
...  

Abstract The Clouds, Aerosol, and Precipitation in the Marine Boundary Layer (CAP-MBL) deployment at Graciosa Island in the Azores generated a 21-month (April 2009–December 2010) comprehensive dataset documenting clouds, aerosols, and precipitation using the Atmospheric Radiation Measurement Program (ARM) Mobile Facility (AMF). The scientific aim of the deployment is to gain improved understanding of the interactions of clouds, aerosols, and precipitation in the marine boundary layer. Graciosa Island straddles the boundary between the subtropics and midlatitudes in the northeast Atlantic Ocean and consequently experiences a great diversity of meteorological and cloudiness conditions. Low clouds are the dominant cloud type, with stratocumulus and cumulus occurring regularly. Approximately half of all clouds contained precipitation detectable as radar echoes below the cloud base. Radar and satellite observations show that clouds with tops from 1 to 11 km contribute more or less equally to surface-measured precipitation at Graciosa. A wide range of aerosol conditions was sampled during the deployment consistent with the diversity of sources as indicated by back-trajectory analysis. Preliminary findings suggest important two-way interactions between aerosols and clouds at Graciosa, with aerosols affecting light precipitation and cloud radiative properties while being controlled in part by precipitation scavenging. The data from Graciosa are being compared with short-range forecasts made with a variety of models. A pilot analysis with two climate and two weather forecast models shows that they reproduce the observed time-varying vertical structure of lower-tropospheric cloud fairly well but the cloud-nucleating aerosol concentrations less well. The Graciosa site has been chosen to be a permanent fixed ARM site that became operational in October 2013.


2011 ◽  
Vol 11 (1) ◽  
pp. 681-744 ◽  
Author(s):  
G. Allen ◽  
H. Coe ◽  
A. Clarke ◽  
C. Bretherton ◽  
R. Wood ◽  
...  

Abstract. The VAMOS Ocean-Climate-Atmosphere-Land Regional Experiment (VOCALS-REx) was conducted from 15 October to 15 November 2008 in the South East Pacific region to investigate interactions between land, sea and atmosphere in this unique tropical eastern ocean environment and to improve the skill of global and regional models in representing the region. This study synthesises selected aircraft, ship and surface site observations from VOCALS-REx to statistically summarise and characterise the atmospheric composition and variability of the Marine Boundary Layer (MBL) and Free Troposphere (FT) along the 20° S parallel between 70° W and 85° W. Significant zonal gradients in mean MBL sub-micron aerosol particle size and composition, carbon monoxide, ozone and sulphur dioxide were seen over the campaign, with a generally more variable and polluted coastal environment and a less variable, more pristine remote maritime regime. Gradients are observed to be associated with strong gradients in cloud droplet number. The FT is often more polluted in terms of trace gases than the MBL in the mean; however increased variability in the FT composition suggests an episodic nature to elevated concentrations. This is consistent with a complex vertical interleaving of airmasses with diverse sources and hence pollutant concentrations as seen by generalised back trajectory analysis, which suggests contributions from both local and long-range sources. Furthermore, back trajectory analysis demonstrates that the observed zonal gradients both in the boundary layer and the free troposphere are characteristic of marked changes in airmass history with distance offshore – coastal boundary layer airmasses having been in recent contact with the local land surface and remote maritime airmasses having resided over ocean for in excess of ten days. Boundary layer composition to the east of 75° W was observed to be dominated by coastal emissions from sources to the west of the Andes, with evidence for diurnal pumping of the Andean boundary layer above the height of the marine capping inversion. The climatology presented here aims to provide a valuable dataset to inform model simulation and future process studies, particularly in the context of aerosol-cloud interaction and further evaluation of dynamical processes in the SEP region for conditions analogous to those during VOCALS-REx.


Atmosphere ◽  
2019 ◽  
Vol 10 (9) ◽  
pp. 539
Author(s):  
Abdelhaleem Khader ◽  
Randal S. Martin

Few air pollutant studies within the Palestinian territories have been reported in the literature. In March–April and May–June of 2018, three low-cost, locally calibrated particulate monitors (AirU’s) were deployed at different elevations and source areas throughout the city of Nablus in Northern West Bank, Palestine. During each of the three-week periods, high but site-to-site similar particulate matter less than 2.5 µm in aerodynamic diameter (PM2.5) and less than 10 µm (PM10) concentrations were observed. The PM2.5 concentrations at the three sampling locations and during both sampling periods averaged 38.2 ± 3.6 µg/m3, well above the World Health Organization’s (WHO) 24 h guidelines. Likewise, the PM10 concentrations exceeded or were just below the WHO’s 24 h guidelines, averaging 48.5 ± 4.3 µg/m3. During both periods, short episodes were identified in which the particulate levels at all three sites increased substantially (≈2×) above the regional baseline. Air mass back trajectory analyses using U.S. National Oceanic and Atmospheric Administration’s (NOAA) Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model suggested that, during these peak episodes, the arriving air masses spent recent days over desert areas (e.g., the Saharan Desert in North Africa). On days with regionally low PM2.5 concentrations (≈20 µg/m3), back trajectory analysis showed that air masses were directed in from the Mediterranean Sea area. Further, the lower elevation (downtown) site often recorded markedly higher particulate levels than the valley wall sites. This would suggest locally derived particulate sources are significant and may be beneficial in the identification of potential remediation options.


2003 ◽  
Vol 3 (1) ◽  
pp. 1017-1049
Author(s):  
M. de Reus ◽  
H. Fischer ◽  
F. Arnold ◽  
J. de Gouw ◽  
R. Holzinger ◽  
...  

Abstract. Carbon monoxide and acetone measurements are presented for five aircraft measurement campaigns at mid-latitudes, polar and tropical regions in the northern hemisphere. Throughout all campaigns, free tropospheric air masses, which were influenced by anthropogenic emissions, showed a similar linear relation between CO and acetone, with a slope of 21–25 pptv acetone/ppbv CO. Measurements in the anthropogenically influenced marine boundary layer revealed a slope of 13–16 pptv acetone/ppbv CO. The different slopes observed in the marine boundary layer and the free troposphere indicate that acetone is emitted by the ocean in relatively clean air masses and taken up by the ocean in polluted air masses. In the lowermost stratosphere, a good correlation between CO and acetone was observed as well, however, with a much smaller slope (~5 pptv acetone/ppbv CO) compared to the troposphere. This is caused by the longer photochemical lifetime of CO compared to acetone in the lower stratosphere, due to the increasing photolytic loss of acetone and the decreasing OH concentration with altitude. No significant correlation between CO and acetone was observed over the tropical rain forest due to the large direct and indirect biogenic emissions of acetone. The common slopes of the linear acetone-CO relation in various layers of the atmosphere, during five field experiments, makes them useful for model calculations. Often a single observation of the CO-acetone correlation, determined from stratospheric measurements, has been used in box model applications. This study shows that different slopes have to be considered for marine boundary layer, free tropospheric and stratospheric air masses, and that the CO-acetone relation cannot be used for air masses which are strongly influenced by biogenic emissions.


2020 ◽  
Vol 20 (6) ◽  
pp. 3415-3438 ◽  
Author(s):  
Hendrik Andersen ◽  
Jan Cermak ◽  
Julia Fuchs ◽  
Peter Knippertz ◽  
Marco Gaetani ◽  
...  

Abstract. Fog is a defining characteristic of the climate of the Namib Desert, and its water and nutrient input are important for local ecosystems. In part due to sparse observation data, the local mechanisms that lead to fog occurrence in the Namib are not yet fully understood, and to date, potential synoptic-scale controls have not been investigated. In this study, a recently established 14-year data set of satellite observations of fog and low clouds in the central Namib is analyzed in conjunction with reanalysis data in order to identify synoptic-scale patterns associated with fog and low-cloud variability in the central Namib during two seasons with different spatial fog occurrence patterns. It is found that during both seasons, mean sea level pressure and geopotential height at 500 hPa differ markedly between fog/low-cloud and clear days, with patterns indicating the presence of synoptic-scale disturbances on fog and low-cloud days. These regularly occurring disturbances increase the probability of fog and low-cloud occurrence in the central Namib in two main ways: (1) an anomalously dry free troposphere in the coastal region of the Namib leads to stronger longwave cooling of the marine boundary layer, increasing low-cloud cover, especially over the ocean where the anomaly is strongest; (2) local wind systems are modulated, leading to an onshore anomaly of marine boundary-layer air masses. This is consistent with air mass back trajectories and a principal component analysis of spatial wind patterns that point to advected marine boundary-layer air masses on fog and low-cloud days, whereas subsiding continental air masses dominate on clear days. Large-scale free-tropospheric moisture transport into southern Africa seems to be a key factor modulating the onshore advection of marine boundary-layer air masses during April, May, and June, as the associated increase in greenhouse gas warming and thus surface heating are observed to contribute to a continental heat low anomaly. A statistical model is trained to discriminate between fog/low-cloud and clear days based on information on large-scale dynamics. The model accurately predicts fog and low-cloud days, illustrating the importance of large-scale pressure modulation and advective processes. It can be concluded that regional fog in the Namib is predominantly of an advective nature and that fog and low-cloud cover is effectively maintained by increased cloud-top radiative cooling. Seasonally different manifestations of synoptic-scale disturbances act to modify its day-to-day variability and the balance of mechanisms leading to its formation and maintenance. The results are the basis for a new conceptual model of the synoptic-scale mechanisms that control fog and low-cloud variability in the Namib Desert and will guide future studies of coastal fog regimes.


2008 ◽  
Vol 8 (16) ◽  
pp. 4711-4728 ◽  
Author(s):  
S. R. Zorn ◽  
F. Drewnick ◽  
M. Schott ◽  
T. Hoffmann ◽  
S. Borrmann

Abstract. Measurements of the submicron fraction of the atmospheric aerosol in the marine boundary layer were performed from January to March 2007 (Southern Hemisphere summer) onboard the French research vessel Marion Dufresne in the Southern Atlantic and Indian Ocean (20° S–60° S, 70° W–60° E). We used an Aerodyne High-Resolution-Time-of-Flight AMS to characterize the chemical composition and to measure species-resolved size distributions of non-refractory aerosol components in the submicron range. Within the "standard" AMS compounds (ammonium, chloride, nitrate, sulfate, organics) "sulfate" is the dominant species in the marine boundary layer with concentrations ranging between 50 ng m−3 and 3 μg m−3. Furthermore, what is seen as "sulfate" by the AMS is likely comprised mostly of sulfuric acid. Another sulfur containing species that is produced in marine environments is methanesulfonic acid (MSA). There have been previously measurements of MSA using an Aerodyne AMS. However, due to the use of an instrument equipped with a quadrupole detector with unit mass resolution it was not possible to physically separate MSA from other contributions to the same m/z. In order to identify MSA within the HR-ToF-AMS raw data and to extract mass concentrations for MSA from the field measurements the standard high-resolution MSA fragmentation patterns for the measurement conditions during the ship campaign (e.g. vaporizer temperature) needed to be determined. To identify characteristic air masses and their source regions backwards trajectories were used and averaged concentrations for AMS standard compounds were calculated for each air mass type. Sulfate mass size distributions were measured for these periods showing a distinct difference between oceanic air masses and those from African outflow. While the peak in the mass distribution was roughly at 250 nm (vacuum aerodynamic diameter) in marine air masses, it was shifted to 470 nm in African outflow air. Correlations between the mass concentrations of sulfate, organics and MSA show a narrow correlation for MSA with sulfate/sulfuric acid coming from the ocean, but not with continental sulfate.


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