Physical aerosol properties and their relation to air mass origin at Monte Cimone (Italy) during the first MINATROC campaign

Abstract. Aerosol physical properties were measured at the Monte Cimone Observatory (Italy) from 1 June till 6 July 2000. The measurement site is located in the transition zone between the continental boundary layer and the free troposphere (FT), at the border between the Mediterranean area and Central Europe, and is exposed to a variety of air masses. Sub-μm number size distributions, aerosol hygroscopicity near 90% RH, refractory size distribution at 270°C and equivalent black carbon mass were continuously measured. Number size distributions and hygroscopic properties indicate that the site is exposed to aged continental air masses, however during daytime it is also affected by upslope winds. The mixing of this transported polluted boundary layer air masses with relatively clean FT air leads to frequent nucleation events around local noon. Night-time size distributions, including fine and coarse fractions for each air mass episode, have been parameterized by a 3-modal lognormal distribution. Number and volume concentrations in the sub-μm modes are strongly affected by the air mass origin, with highest levels in NW-European air masses, versus very clean, free tropospheric air coming from the N-European sector. During a brief but distinct dust episode, the coarse mode is clearly enhanced. The observed hygroscopic behavior of the aerosol is consistent with the chemical composition described by Putaud et al. (2004), but no closure between known chemical composition and measured hygroscopicity could be made because the hygroscopic properties of the water-soluble organic matter (WSOM) are not known. The data suggest that WSOM is slightly-to-moderately hygroscopic (hygroscopic growth factor GF at 90% relative humidity between 1.05 and 1.51), and that this property may well depend on the air mass origin and history. External mixing of aerosol particles is observed in all air masses through the occurrence of two hygroscopicity modes (average GF of 1.22 and 1.37, respectively). However, the presence of "less" hygroscopic particles has mostly such a low occurrence rate that the average growth factor distribution for each air mass sector actually appears as a single mode. This is not the case for the dust episode, where the external mixing between less hygroscopic and more hygroscopic particles is very prominent, and indicating clearly the occurrence of a dust accumulation mode, extending down to 50 nm particles, along with an anthropogenic pollution mode. The presented physical measurements finally allow us to provide a partitioning of the sub-μm aerosol in four non-overlapping fractions (soluble/volatile, non-soluble/volatile, refractory/non-black carbon, black carbon) which can be associated with separate groups of chemical compounds determined with chemical-analytical techniques (ions, non-water soluble organic matter, dust, elemental carbon). All air masses except the free-tropospheric N-European and Dust episodes show a similar composition within the uncertainty of the data (53%, 37%, 5% and 5% respectively for the four defined fractions). Compared to these sectors, the dust episode shows a clearly enhanced refractory-non-BC fraction (17%), attributed to dust in the accumulation mode, whereas for the very clean N-EUR sector, the total refractory fraction is 25%, of which 13% non-BC and 12% BC.

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Physical aerosol properties and their relation to air mass origin at Monte Cimone (Italy) during the first MINATROC campaign

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-5-1067-2005 ◽

2005 ◽

Vol 5 (1) ◽

pp. 1067-1114 ◽

Cited By ~ 3

Author(s):

R. Van Dingenen ◽

J.-P. Putaud ◽

S. Martins-Dos Santos ◽

F. Raes

Keyword(s):

Boundary Layer ◽

Organic Matter ◽

The Arctic ◽

Size Distributions ◽

Air Mass ◽

Air Masses ◽

Accumulation Mode ◽

Hygroscopic Properties ◽

Hygroscopic Particles ◽

Air Mass Origin

Abstract. Aerosol physical properties were measured at the Monte Cimone Observatory (Italy) from 1 June till 6 July 2000. The measurement site is located in the transition zone between continental boundary layer and the free troposphere (FT), at the border between the Mediterranean area and Central Europe, and is exposed to a variety of air masses. Sub-micrometer number size distributions, aerosol hygroscopicity at 90% RH, refractory size distribution at 270°C and black carbon mass were continuously measured. Number size distributions and hygroscopic properties indicate that the site is exposed to aged continental air masses, however during daytime it is also affected by upslope winds. The mixing of this transported polluted boundary layer air masses with relatively clean FT air leads to frequent nucleation events around local noon. Night-time size distributions including fine and coarse fractions for each air mass episode have been parameterized by a 3-modal lognormal distribution. Number and volume concentrations in the sub-micrometer modes are strongly affected by the air mass origin, with highest levels in NW-European air masses, versus very clean air in the ''Arctic'' episode. During the dust episode, the coarse mode is clearly enhanced. The observed hygroscopic behavior of the aerosol is consistent with the chemical composition described by Putaud et al. (2004a), but no closure could be made because the hygroscopic properties of the water-soluble organic matter is not known. The data suggest that WSOM is slightly-to-moderately hygroscopic, and that this property may well depend on the air mass origin and history. Although externally mixing is observed in all air masses, the occurrence of ''less'' hygroscopic particles has mostly such a low occurrence rate that the average growth factor distribution mostly appears as a single mode. This is not the case for the dust episode, where the external mixing between less hygroscopic and more hygroscopic particles is very prominent, and indicating clearly the occurrence of a dust accumulation mode, extending down to 50 nm particles, along with an anthropogenic pollution mode. The presented physical measurements finally allow us to provide a partitioning of the sub-µm aerosol in four non-overlapping fractions (soluble + volatile, non-soluble + volatile, refractory + non-BC, BC) which can be roughly associated with separate groups of chemical compounds (ions, organic matter, dust, BC). For what concerns the relative contributions of the fractions, all air masses except the free-tropospheric (FT) and Dust Episodes show a similar composition within the uncertainty of the data. The latter two have a significantly higher refractory fraction, which in the FT air mass is attributed to carbonaceous particles, and in the dust episode to a sub-µm accumulation mode of dust.

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Aerosol particle measurements at three stationary sites in the megacity of Paris during summer 2009: meteorology and air mass origin dominate aerosol particle composition and size distribution

Atmospheric Chemistry and Physics ◽

10.5194/acp-13-933-2013 ◽

2013 ◽

Vol 13 (2) ◽

pp. 933-959 ◽

Cited By ~ 83

Author(s):

F. Freutel ◽

J. Schneider ◽

F. Drewnick ◽

S.-L. von der Weiden-Reinmüller ◽

M. Crippa ◽

...

Keyword(s):

Particle Size ◽

Black Carbon ◽

Aerosol Particle ◽

Organic Aerosol ◽

Air Mass ◽

Air Masses ◽

Aerosol Mass ◽

The Impact ◽

Air Mass Origin ◽

Mass Concentrations

Abstract. During July 2009, a one-month measurement campaign was performed in the megacity of Paris. Amongst other measurement platforms, three stationary sites distributed over an area of 40 km in diameter in the greater Paris region enabled a detailed characterization of the aerosol particle and gas phase. Simulation results from the FLEXPART dispersion model were used to distinguish between different types of air masses sampled. It was found that the origin of air masses had a large influence on measured mass concentrations of the secondary species particulate sulphate, nitrate, ammonium, and oxygenated organic aerosol measured with the Aerodyne aerosol mass spectrometer in the submicron particle size range: particularly high concentrations of these species (about 4 μg m−3, 2 μg m−3, 2 μg m−3, and 7 μg m−3, respectively) were measured when aged material was advected from continental Europe, while for air masses originating from the Atlantic, much lower mass concentrations of these species were observed (about 1 μg m−3, 0.2 μg m−3, 0.4 μg m−3, and 1–3 μg m−3, respectively). For the primary emission tracers hydrocarbon-like organic aerosol, black carbon, and NOx it was found that apart from diurnal source strength variations and proximity to emission sources, local meteorology had the largest influence on measured concentrations, with higher wind speeds leading to larger dilution and therefore smaller measured concentrations. Also the shape of particle size distributions was affected by wind speed and air mass origin. Quasi-Lagrangian measurements performed under connected flow conditions between the three stationary sites were used to estimate the influence of the Paris emission plume onto its surroundings, which was found to be rather small. Rough estimates for the impact of the Paris emission plume on the suburban areas can be inferred from these measurements: Volume mixing ratios of 1–14 ppb of NOx, and upper limits for mass concentrations of about 1.5 μg m−3 of black carbon and of about 3 μg m−3 of hydrocarbon-like organic aerosol can be deduced which originate from both, local emissions and the overall Paris emission plume. The secondary aerosol particle phase species were found to be not significantly influenced by the Paris megacity, indicating their regional origin. The submicron aerosol mass concentrations of particulate sulphate, nitrate, and ammonium measured during time periods when air masses were advected from eastern central Europe were found to be similar to what has been found from other measurement campaigns in Paris and south-central France for this type of air mass origin, indicating that the results presented here are also more generally valid.

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Alteration of the size distributions and mixing states of black carbon through transport in the boundary layer in east Asia

Atmospheric Chemistry and Physics ◽

10.5194/acp-17-5851-2017 ◽

2017 ◽

Vol 17 (9) ◽

pp. 5851-5864 ◽

Cited By ~ 17

Author(s):

Takuma Miyakawa ◽

Naga Oshima ◽

Fumikazu Taketani ◽

Yuichi Komazaki ◽

Ayako Yoshino ◽

...

Keyword(s):

Boundary Layer ◽

Black Carbon ◽

Water Solubility ◽

Southern China ◽

Source Region ◽

Size Distributions ◽

Air Masses ◽

Remote Island ◽

Mixing States ◽

Wet Removal

Abstract. Ground-based measurements of black carbon (BC) were performed near an industrial source region in the early summer of 2014 and at a remote island in Japan in the spring of 2015. Here, we report the temporal variations in the transport, size distributions, and mixing states of the BC-containing particles. These particles were characterized using a continuous soot monitoring system, a single particle soot photometer, and an aerosol chemical speciation monitor. The effects of aging on the growth of BC-containing particles were examined by comparing the ground-based observations between the near-source and remote island sites. Secondary formation of sulfate and organic aerosols strongly affected the increases in BC coating (i.e., enhancement of cloud condensation nuclei activity) with air mass aging from the source to the outflow regions. The effects of wet removal on BC microphysics were elucidated by classifying the continental outflow air masses depending on the enhancement ratios of BC to CO (ΔBC ∕ ΔCO), which were used as an indicator of the transport efficiency of BC. It was found that ΔBC ∕ ΔCO ratios were controlled mainly by the wet removal during transport in the planetary boundary layer (PBL) on the timescale of 1–2 days. The meteorological conditions and backward trajectory analyses suggested that air masses strongly affected by wet removal originated mainly from a region in southern China (20–35° N) in the spring of 2015. Removal of large and thickly coated BC-containing particles was detected in the air masses that were substantially affected by the wet removal in the PBL, as predicted by Köhler theory. The size and water solubility of BC-containing particles in the PBL can be altered by the wet removal as well as the condensation of non-BC materials.

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Aerosol particle measurements at three stationary sites in the megacity of Paris during summer 2009: meteorology and air mass origin dominate aerosol particle composition and size distribution

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-12-22199-2012 ◽

2012 ◽

Vol 12 (8) ◽

pp. 22199-22268 ◽

Cited By ~ 3

Author(s):

F. Freutel ◽

J. Schneider ◽

F. Drewnick ◽

S.-L. von der Weiden-Reinmüller ◽

M. Crippa ◽

...

Keyword(s):

Particle Size ◽

Black Carbon ◽

Aerosol Particle ◽

Organic Aerosol ◽

Air Mass ◽

Air Masses ◽

Aerosol Mass ◽

The Impact ◽

Air Mass Origin ◽

Mass Concentrations

Abstract. During July 2009, a one-month measurement campaign was performed in the megacity of Paris. Amongst other measurement platforms, three stationary sites distributed over an area of 40 km in diameter in the greater Paris region enabled a detailed characterization of the aerosol particle and gas phase. Simulation results from the FLEXPART dispersion model were used to distinguish between different types of air masses sampled. It was found that the origin of air masses had a large influence on measured mass concentrations of the secondary species particulate sulphate, nitrate, ammonium, and oxygenated organic aerosol measured with the Aerodyne aerosol mass spectrometer in the submicron particle size range: particularly high concentrations of these species (about 4 μg m−3, 2 μg m−3, 2 μg m−3, and 7 μg m−3, respectively) were measured when aged material was advected from continental Europe, while for air masses originating from the Atlantic, much lower mass concentrations of these species were observed (about 1 μg m−3, 0.2 μg m−3, 0.4 μg m−3, and 1–3 μg m−3, respectively). For the primary emission tracers hydrocarbon-like organic aerosol, black carbon, and NOx it was found that apart from diurnal source strength variations and proximity to emission sources, local meteorology had the largest influence on measured concentrations, with higher wind speeds leading to larger dilution and therefore smaller measured concentrations. Also the shape of particle size distributions was affected by wind speed and air mass origin. Quasi-Lagrangian measurements performed under connected flow conditions between the three stationary sites were used to estimate the influence of the Paris emission plume onto its surroundings, which was found to be rather small. Rough estimates for the impact of the Paris emission plume on the suburban areas can be inferred from these measurements: Volume mixing ratios of 1–14 ppb of NOx, and upper limits for mass concentrations of about 1.5 μg m−3 of black carbon and of about 3 μg m−3 of hydrocarbon-like organic aerosol can be deduced which originate from both, local emissions and the overall Paris emission plume. The secondary aerosol particle phase species were found to be not significantly influenced by the Paris megacity, indicating their regional origin. The submicron aerosol mass concentrations of particulate sulphate, nitrate, and ammonium measured during time periods when air masses were advected from eastern central Europe were found to be similar to what has been found from other measurement campaigns in Paris and South-Central France for this type of air mass origin, indicating that the results presented here are also more generally valid.

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Multivariate statistical air mass classification for the high-alpine observatory at the Zugspitze Mountain, Germany

Atmospheric Chemistry and Physics ◽

10.5194/acp-19-12477-2019 ◽

2019 ◽

Vol 19 (19) ◽

pp. 12477-12494 ◽

Cited By ~ 2

Author(s):

Armin Sigmund ◽

Korbinian Freier ◽

Till Rehm ◽

Ludwig Ries ◽

Christian Schunk ◽

...

Keyword(s):

Boundary Layer ◽

Real Time ◽

Statistical Approach ◽

Free Troposphere ◽

Time Data ◽

Detection Scheme ◽

Air Mass ◽

Thermally Induced ◽

Air Masses ◽

Mechanistic Approach

Abstract. To assist atmospheric monitoring at high-alpine sites, a statistical approach for distinguishing between the dominant air masses was developed. This approach was based on a principal component analysis using five gas-phase and two meteorological variables. The analysis focused on the Schneefernerhaus site at Zugspitze Mountain, Germany. The investigated year was divided into 2-month periods, for which the analysis was repeated. Using the 33.3 % and 66.6 % percentiles of the first two principal components, nine air mass regimes were defined. These regimes were interpreted with respect to vertical transport and assigned to the BL (recent contact with the boundary layer), UFT/SIN (undisturbed free troposphere or stratospheric intrusion), and HYBRID (influences of both the boundary layer and the free troposphere or ambiguous) air mass classes. The input data were available for 78 % of the investigated year. BL accounted for 31 % of the cases with similar frequencies in all seasons. UFT/SIN comprised 14 % of the cases but was not found from April to July. HYBRID (55 %) mostly exhibited intermediate characteristics, whereby 17 % of the HYBRID class suggested an influence from the marine boundary layer or the lower free troposphere. The statistical approach was compared to a mechanistic approach using the ceilometer-based mixing layer height from a nearby valley site and a detection scheme for thermally induced mountain winds. Due to data gaps, only 25 % of the cases could be classified using the mechanistic approach. Both approaches agreed well, except in the rare cases of thermally induced uplift. The statistical approach is a promising step towards a real-time classification of air masses. Future work is necessary to assess the uncertainty arising from the standardization of real-time data.

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Particle size distributions in the Eastern Mediterranean troposphere

Atmospheric Chemistry and Physics ◽

10.5194/acp-8-6729-2008 ◽

2008 ◽

Vol 8 (22) ◽

pp. 6729-6738 ◽

Cited By ~ 29

Author(s):

N. Kalivitis ◽

W. Birmili ◽

M. Stock ◽

B. Wehner ◽

A. Massling ◽

...

Keyword(s):

Boundary Layer ◽

Particle Size ◽

Eastern Mediterranean ◽

Particle Formation ◽

Particle Nucleation ◽

Size Distributions ◽

Particle Size Distributions ◽

Air Masses ◽

Crete Island ◽

Particle Sizer

Abstract. Atmospheric particle size distributions were measured on Crete island, Greece in the Eastern Mediterranean during an intensive field campaign between 28 August and 20 October, 2005. Our instrumentation combined a differential mobility particle sizer (DMPS) and an aerodynamic particle sizer (APS) and measured number size distributions in the size range 0.018 μm–10 μm. Four time periods with distinct aerosol characteristics were discriminated, two corresponding to marine and polluted air masses, respectively. In marine air, the sub-μm size distributions showed two particle modes centered at 67 nm and 195 nm having total number concentrations between 900 and 2000 cm−3. In polluted air masses, the size distributions were mainly unimodal with a mode typically centered at 140 nm, with number concentrations varying between 1800 and 2900 cm−3. Super-μm particles showed number concentrations in the range from 0.01 to 2.5 cm−3 without any clear relation to air mass origin. A small number of short-lived particle nucleation events were recorded, where the calculated particle formation rates ranged between 1.1–1.7 cm−3 s−1. However, no particle nucleation and growth events comparable to those typical for the continental boundary layer were observed. Particles concentrations (Diameter <50 nm) were low compared to continental boundary layer conditions with an average concentration of 300 cm−3. The production of sulfuric acid and its subsequently condensation on preexisting particles was examined with the use of a simplistic box model. These calculations suggested that the day-time evolution of the Aitken particle population was governed mainly by coagulation and that particle formation was absent during most days.

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Particle size distributions in the Eastern Mediterranean troposphere

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-8-6571-2008 ◽

2008 ◽

Vol 8 (2) ◽

pp. 6571-6601

Author(s):

N. Kalivitis ◽

W. Birmili ◽

M. Stock ◽

B. Wehner ◽

A. Massling ◽

...

Keyword(s):

Boundary Layer ◽

Particle Size ◽

Eastern Mediterranean ◽

Particle Formation ◽

Particle Nucleation ◽

Size Distributions ◽

Particle Size Distributions ◽

Air Masses ◽

Crete Island ◽

Particle Sizer

Abstract. Atmospheric particle size distributions were measured on Crete island, Greece in the Eastern Mediterranean during an intensive field campaign between 28 August and 20 October 2005. Our instrumentation combined a differential mobility particle sizer (DMPS) and an aerodynamic particle sizer (APS) and measured number size distributions in the size range 0.018 μm–10 μm. Four time periods with distinct aerosol characteristics were discriminated, two corresponding to marine and polluted air masses, respectively. In marine air, the sub-μm size distributions showed two particle modes centered at 67 nm and 195 nm having total number concentrations between 900 and 2000 cm−3. In polluted air masses, the size distributions were mainly unimodal with a mode typically centered at 140 nm, with number concentrations varying between 1800 and 2900 cm−3. Super-μm particles showed number concentrations in the range from 0.01 to 2.5 cm−3 without any clear relation to air mass origin. A small number of short-lived particle nucleation events were recorded, where the calculated particle formation rates ranged between 1.1–1.7 cm−3 s−1. However, no particle nucleation and growth events comparable to those typical for the continental boundary layer were observed. Particles concentrations (Diameter <50 nm) were low compared to continental boundary layer conditions with an average concentration of 300 cm−3. The production of sulfuric acid and its subsequently condensation on preexisting particles was examined with the use of a simplistic box model. These calculations suggested that the day-time evolution of the Aitken particle population was governed mainly by coagulation and that particle formation was absent during most days.

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Long-term real-time chemical characterization of submicron aerosols at Montsec (southern Pyrenees, 1570 m a.s.l.)

Atmospheric Chemistry and Physics ◽

10.5194/acp-15-2935-2015 ◽

2015 ◽

Vol 15 (6) ◽

pp. 2935-2951 ◽

Cited By ~ 36

Author(s):

A. Ripoll ◽

M. C. Minguillón ◽

J. Pey ◽

J. L. Jimenez ◽

D. A. Day ◽

...

Keyword(s):

Real Time ◽

Long Range ◽

Chemical Characterization ◽

Western Mediterranean ◽

Continuous Increase ◽

Air Mass ◽

Air Masses ◽

Diurnal Cycles ◽

Western Mediterranean Basin ◽

Air Mass Origin

Abstract. Real-time measurements of inorganic (sulfate, nitrate, ammonium, chloride and black carbon (BC)) and organic submicron aerosols (particles with an aerodynamic diameter of less than 1 μm) from a continental background site (Montsec, MSC, 1570 m a.s.l.) in the western Mediterranean Basin (WMB) were conducted for 10 months (July 2011–April 2012). An aerosol chemical speciation monitor (ACSM) was co-located with other online and offline PM1 measurements. Analyses of the hourly, diurnal, and seasonal variations are presented here, for the first time, for this region. Seasonal trends in PM1 components are attributed to variations in evolution of the planetary boundary layer (PBL) height, air mass origin, and meteorological conditions. In summer, the higher temperature and solar radiation increases convection, enhancing the growth of the PBL and the transport of anthropogenic pollutants towards high altitude sites. Furthermore, the regional recirculation of air masses over the WMB creates a continuous increase in the background concentrations of PM1 components and causes the formation of reservoir layers at relatively high altitudes. The combination of all these atmospheric processes results in a high variability of PM1 components, with poorly defined daily patterns, except for the organic aerosols (OA). OA was mostly composed (up to 90%) of oxygenated organic aerosol (OOA), split in two types: semivolatile (SV-OOA) and low-volatility (LV-OOA), the rest being hydrocarbon-like OA (HOA). The marked diurnal cycles of OA components regardless of the air mass origin indicates that they are not only associated with anthropogenic and long-range-transported secondary OA (SOA) but also with recently produced biogenic SOA. Very different conditions drive the aerosol phenomenology in winter at MSC. The thermal inversions and the lower vertical development of the PBL leave MSC in the free troposphere most of the day, being affected by PBL air masses only after midday, when the mountain breezes transport emissions from the adjacent valleys and plains to the top of the mountain. This results in clear diurnal patterns of both organic and inorganic concentrations. OA was also mainly composed (71%) of OOA, with contributions from HOA (5%) and biomass burning OA (BBOA; 24%). Moreover, in winter sporadic long-range transport from mainland Europe is observed. The results obtained in the present study highlight the importance of SOA formation processes at a remote site such as MSC, especially in summer. Additional research is needed to characterize the sources and processes of SOA formation at remote sites.

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Characterization of the South Atlantic marine boundary layer aerosol using an aerodyne aerosol mass spectrometer

Atmospheric Chemistry and Physics ◽

10.5194/acp-8-4711-2008 ◽

2008 ◽

Vol 8 (16) ◽

pp. 4711-4728 ◽

Cited By ~ 98

Author(s):

S. R. Zorn ◽

F. Drewnick ◽

M. Schott ◽

T. Hoffmann ◽

S. Borrmann

Keyword(s):

Boundary Layer ◽

Sulfuric Acid ◽

High Resolution ◽

Marine Boundary Layer ◽

Methanesulfonic Acid ◽

Field Measurements ◽

Size Distributions ◽

Air Masses ◽

Unit Mass Resolution ◽

Mass Concentrations

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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Aircraft observations of enhancement and depletion of black carbon mass in the springtime Arctic

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-10-15167-2010 ◽

2010 ◽

Vol 10 (6) ◽

pp. 15167-15196

Author(s):

J. R. Spackman ◽

R. S. Gao ◽

W. D. Neff ◽

J. P. Schwarz ◽

L. A. Watts ◽

...

Keyword(s):

Boundary Layer ◽

Black Carbon ◽

Biomass Burning ◽

Boundary Layer Transition ◽

Arctic Climate ◽

The Arctic ◽

Vertical Profiles ◽

Free Troposphere ◽

Air Mass ◽

The Impact

Abstract. Understanding the processes controlling black carbon (BC) in the Arctic is crucial for evaluating the impact of anthropogenic and natural sources of BC on Arctic climate. Vertical profiles of BC mass were observed from the surface to near 7-km altitude in April 2008 using a Single-Particle Soot Photometer (SP2) during flights on the NOAA WP-3D research aircraft from Fairbanks, Alaska. These measurements were conducted during the NOAA-sponsored Aerosol, Radiation, and Cloud Processes affecting Arctic Climate (ARCPAC) project as part of POLARCAT, an International Polar Year (IPY) activity. In the free troposphere, the Arctic air mass was influenced by long-range transport from biomass-burning and anthropogenic source regions at lower latitudes especially during the latter part of the campaign. Maximum average BC mass loadings of 150 ng kg−1 were observed near 5.5-km altitude in the aged Arctic air mass. In biomass-burning plumes, BC was enhanced from near the top of the Arctic boundary layer (ABL) to 5.5 km compared to the aged Arctic air mass. At the bottom of some of the profiles, positive vertical gradients in BC were observed in the vicinity of open leads in the sea-ice. BC mass loadings increased by about a factor of two across the boundary layer transition in the ABL in these cases while carbon monoxide (CO) remained constant, evidence for depletion of BC in the ABL. BC mass loadings were positively correlated with O3 in ozone depletion events (ODEs) for all the observations in the ABL suggesting that BC was removed by dry deposition of BC on the snow or ice because molecular bromine, Br2, which photolyzes and catalytically destroys O3, is thought to be released near the open leads in regions of ice formation. We estimate the deposition flux of BC mass to the snow using a box model constrained by the vertical profiles of BC in the ABL. The open leads may increase vertical mixing in the ABL and entrainment of pollution from the free troposphere possibly enhancing the deposition of BC to the snow.

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