scholarly journals Seasonal variations and vertical features of aerosol particles in the Antarctic troposphere

2011 ◽  
Vol 11 (3) ◽  
pp. 7555-7591 ◽  
Author(s):  
K. Hara ◽  
K. Osada ◽  
C. Nishita-Hara ◽  
T. Yamanouchi
Keyword(s):  
Seasonal Variations ◽  
Fine Particles ◽  
Austral Summer ◽  
Sea Salt ◽  
Coarse Particles ◽  
Free Troposphere ◽  
Syowa Station ◽  
Air Masses ◽  
Antarctic Expedition ◽  
The Antarctic

Abstract. Tethered balloon-borne aerosol measurements were conducted at Syowa Station, Antarctica during the 46th Japanese Antarctic expedition (2005–2006). The CN concentration reached a maximum in the summer, although the number concentrations of fine particles (Dp > 0.3 μm) and coarse particles (Dp > 2.0 μm) increased during the winter-spring. The CN concentration was 30–2200 cm−3 near the surface (surface – 500 m) and 7–7250 cm−3 in the lower free troposphere (>1500 m). During the austral summer, higher CN concentration was often observed in the lower free troposphere, where the number concentrations in fine and coarse modes were remarkably lower. The frequent appearance of higher CN concentrations in the free troposphere relative to continuous aerosol measurements at the ground strongly suggests that new particle formation is more likely to occur in the lower free troposphere in Antarctic regions. Seasonal variations of size distribution of fine-coarse particles show that the contribution of the coarse mode was greater in the winter-spring than in summer because of the dominance of sea-salt particles in the winter-spring. The number concentrations of fine and coarse particles were high in air masses from the ocean and mid-latitudes. Particularly, aerosol enhancement was observed not only in the boundary layer but also in the lower free troposphere during and immediately after Antarctic haze events occurring in May, July, and September.

scholarly journals Seasonal variations and vertical features of aerosol particles in the Antarctic troposphere

2011 ◽  
Vol 11 (11) ◽  
pp. 5471-5484 ◽  
Author(s):  
K. Hara ◽  
K. Osada ◽  
C. Nishita-Hara ◽  
T. Yamanouchi
Keyword(s):  
Seasonal Variations ◽  
Fine Particles ◽  
Austral Summer ◽  
Sea Salt ◽  
Coarse Particles ◽  
Free Troposphere ◽  
Syowa Station ◽  
Air Masses ◽  
Antarctic Expedition ◽  
The Antarctic

Abstract. Tethered balloon-borne aerosol measurements were conducted at Syowa Station, Antarctica during the 46th Japanese Antarctic expedition (2005–2006). The CN concentration reached a maximum in the summer, although the number concentrations of fine particles (Dp>0.3 μm) and coarse particles (Dp>2.0 μm) increased during the winter–spring. The CN concentration was 30–2200 cm−3 near the surface (surface – 500 m) and 7–7250 cm−3 in the lower free troposphere (>1500 m). During the austral summer, higher CN concentration was often observed in the lower free troposphere, where the number concentrations in fine and coarse modes were remarkably lower. The frequent appearance of higher CN concentrations in the free troposphere relative to continuous aerosol measurements at the ground strongly suggests that new particle formation is more likely to occur in the lower free troposphere in Antarctic regions. Seasonal variations of size distribution of fine-coarse particles show that the contribution of the coarse mode was greater in the winter–spring than in summer because of the dominance of sea-salt particles in the winter–spring. The number concentrations of fine and coarse particles were high in air masses from the ocean and mid-latitudes. Particularly, aerosol enhancement was observed not only in the boundary layer, but also in the lower free troposphere during and immediately after Antarctic haze events occurring in May, July and September.

scholarly journals Simultaneous aerosol measurements of unusual aerosol enhancement in the troposphere over Syowa Station, Antarctica

2014 ◽  
Vol 14 (8) ◽  
pp. 4169-4183 ◽  
Author(s):  
K. Hara ◽  
M. Hayashi ◽  
M. Yabuki ◽  
M. Shiobara ◽  
C. Nishita-Hara
Keyword(s):  
Boundary Layer ◽  
Sea Ice ◽  
Sea Salt ◽  
Free Troposphere ◽  
Syowa Station ◽  
Particle Counter ◽  
Air Masses ◽  
Optical Particle Counter ◽  
Strong Winds ◽  
Storm Condition

Abstract. Unusual aerosol enhancement is often observed at Syowa Station, Antarctica, during winter and spring. Simultaneous aerosol measurements near the surface and in the upper atmosphere were conducted twice using a ground-based optical particle counter, a balloon-borne optical particle counter, and micropulse lidar (MPL) in August and September 2012. During 13–15 August, aerosol enhancement occurred immediately after a storm condition. A high backscatter ratio and high aerosol concentrations were observed from the surface to ca. 2.5 km over Syowa Station. Clouds appeared occasionally at the top of the aerosol-enhanced layer during the episode. Aerosol enhancement was terminated on 15 August by strong winds from a cyclone's approach. In the second case, on 5–7 September, aerosol number concentrations in Dp > 0.3 μm near the surface reached > 104 L−1 at about 15:00 UT (Universal Time) on 5 September despite calm wind conditions, whereas MPL measurement exhibited aerosols were enhanced at about 04:00 UT at 1000–1500 m above Syowa Station. The aerosol enhancement occurred near the surface to ca. 4 km. In both cases, air masses with high aerosol enhancement below 2.5–3 km were transported mostly from the boundary layer over the sea-ice area. In addition, air masses at 3–4 km in the second case came from the boundary layer over the open-sea area. This air mass history strongly suggests that dispersion of sea-salt particles from the sea-ice surface contributes considerably to aerosol enhancement in the lower free troposphere (about 3 km) and that the release of sea-salt particles from the ocean surface engenders high aerosol concentrations in the free troposphere (3–4 km). Continuous MPL measurements indicate that high aerosol enhancement occurred mostly in surface–lower free troposphere (3 km) during the period July–September.

scholarly journals Simultaneous aerosol measurements of unusual aerosol enhancement in troposphere over Syowa Station, Antarctica

2013 ◽  
Vol 13 (10) ◽  
pp. 26269-26303
Author(s):  
K. Hara ◽  
M. Hayashi ◽  
M. Yabuki ◽  
M. Shiobara ◽  
C. Nishita-Hara
Keyword(s):  
Boundary Layer ◽  
Sea Ice ◽  
Sea Salt ◽  
Free Troposphere ◽  
Syowa Station ◽  
Particle Counter ◽  
Air Masses ◽  
Optical Particle Counter ◽  
Strong Winds ◽  
Storm Condition

Abstract. Unusual aerosol enhancement is often observed at Syowa Station, Antarctica during winter through spring. Simultaneous aerosol measurements near the surface and in the upper atmosphere were conducted twice using a ground-based optical particle counter, a balloon-borne optical particle counter, and micro-pulse LIDAR (MPL) in August and September 2012. During 13–15 August, aerosol enhancement occurred immediately after a storm condition. A high backscatter ratio and aerosol concentrations were observed from the surface to ca. 2.5 km over Syowa Station. Clouds appeared occasionally at the top of aerosol-enhanced layer during the episode. Aerosol enhancement was terminated on 15 August by strong winds caused by a cyclone's approach. In the second case on 5–7 September, aerosol number concentrations in Dp > 0.3 μm near the surface reached > 104 L−1 at about 15:00 UT on 5 September in spite of calm wind conditions, whereas MPL measurement exhibited aerosols were enhanced at about 04:00 UT at 1000–1500 m above Syowa Station. The aerosol enhancement occurred near the surface–ca. 4 km. In both cases, air masses with high aerosol enhancement below 2.5–3 km were transported mostly from the boundary layer over the sea-ice area. In addition, air masses at 3–4 km in the second case came from the boundary layer over the open-sea area. This air mass history strongly suggests that dispersion of sea-salt particles from the sea-ice surface contributes considerably to the aerosol enhancement in the lower free troposphere (about 3 km) and that the release of sea-salt particles from the ocean surface engenders high aerosol concentrations in the free troposphere (3–4 km).

scholarly journals CCN measurements at the Princess Elisabeth Antarctica Research Station during three austral summers

2018 ◽  
Author(s):  
Paul Herenz ◽  
Heike Wex ◽  
Alexander Mangold ◽  
Quentin Laffineur ◽  
Irina V. Gorodestkaya ◽  
...  
Keyword(s):  
Southern Ocean ◽  
Aerosol Particle ◽  
Aerosol Particles ◽  
Source Region ◽  
Austral Summer ◽  
Research Station ◽  
Air Masses ◽  
Potential Source ◽  
The Antarctic ◽  
Aitken Mode

Abstract. For three austral summer seasons (2013–2016, each from December to February) aerosol particles arriving at the Belgian Antarctic research station Princess Elisabeth (PE), in Dronning Maud Land in East Antarctica were characterized in terms of number concentrations of total aerosol particles (NCN) and cloud condensation nuclei (NCCN), the particle number size distribution (PNSD), the aerosol particle hygroscopicity and the influence of the air mass origin on NCN and NCCN. In general NCN was found to range from 40 to 6700 cm−3 with a median of 333 cm−3, while NCCN was found to cover a range between less than 10 and 1300 cm−3 for supersaturations (SS) between 0.1 and 0.7 %. It is shown that the aerosol is Aitken mode dominated and is characterized by a significant amount of freshly, secondarily formed aerosol particles, with 94 % and 36 % of the aerosol particles are smaller than 90 nm and ≈ 35 nm, respectively. Measurements of the basic meteorological parameters as well as the history of the air masses arriving at the measurement station indicate that the station is influenced by both, continental air masses originating from the Antarctic inland ice sheet (continental events – CE) and marine air masses originating from the Southern Ocean (marine events – ME). CEs came along with rather constant NCN and NCCN values, which we denote to be Antarctic continental background concentrations. MEs however cause large fluctuations in NCN and NCCN caused by scavenging due to precipitation or new particle formation based on marine precursors. The application of Hysplit back trajectories in form of the potential source contribution function (PSCF) analysis indicate, that the region of the Southern Ocean is a potential source of Aitken mode particles. For particles larger than ≈ 110 nm (CCN measured at SS of 0.1 %) the Antarctic ice shelf regions were found to be a potential source region, most likely due to the emission of sea salt aerosol particles, released from snow particles from surface snow layers by sublimation, e.g., during periods of high wind speed, leading to drifting or blowing snow. On the basis of the PNSDs and NCCN, the critical diameter for cloud droplet activation and the aerosol particle hygroscopicity parameter κ were determined to be 110 nm and 1, respectively, for a SS of 0.1 %. The region of the Antarctic inland plateau however was not found to feature a significant source region for CN and CCN measured at the PE station in austral summer.

scholarly journals The Weddell Sea region: an important precipitation channel to the interior of the Antarctic ice sheet as revealed by glaciochemical investigation of surface snow along the longest trans-Antarctic route

1999 ◽  
Vol 29 ◽  
pp. 55-60 ◽  
Author(s):  
Qin Dahe ◽  
Paul A. Mayewski ◽  
Ren Jiawen ◽  
Xiao Cunde ◽  
Sun Junying
Keyword(s):  
Ice Sheet ◽  
Weddell Sea ◽  
Sea Salt ◽  
East Antarctica ◽  
Antarctic Ice Sheet ◽  
Air Masses ◽  
Antarctic Plateau ◽  
Salt Ions ◽  
Surface Snow ◽  
The Antarctic

AbstractGlaciochemical analysis of surface snow samples, collected along a profile crossing the Antarctic ice sheet from the Larsen Ice Shelf, Antarctic Peninsula, via the Antarctic Plateau through South Pole, Vostok and Komsomolskaya to Mirny station (at the east margin of East Antarctica), shows that the Weddell Sea region is an important channel for air masses to the high plateau of the Antarctic ice sheet (>2000 m a.s.l.). This opinion is supported by the following. (1) The fluxes of sea-salt ions such as Na+, Mg2 + and CF display a decreasing trend from the west to the east of interior Antarctica. In |eneral, as sea-salt aerosols are injected into the atmosphere over the Antarctic ice sheet from the Weddell Sea, large aerosols tend to decrease. For the inland plateau, few large particles of sea-salt aerosol reach the area, and the sea-salt concentration levels are low (2) The high altitude of the East Antarctic plateau, as well as the polar cold high-pressure system, obstruct the intrusive air masses mainly from the South Indian Ocean sector. (3) For the coastal regions of the East Antarctic ice sheet, the elevation rises to 2000 m over a distance from several to several tens of km. High concentrations of sea salt exist in snow in East Antarctica but are limited to a narrow coastal zone. (4) Fluxes of calcium and non-sea-salt sulfate in snow from the interior plateau do not display an eastward-decreasing trend. Since calcium is mainly derived from crustal sources, and nssSO42- is a secondary aerosol, this again confirms that the eastward-declining tendency of sea-salt ions indicates the transfer direction of precipitation vapor.

scholarly journals New particle formation events observed at the King Sejong Station, Antarctic Peninsula – Part 2: Link with the oceanic biological activities

2019 ◽  
Vol 19 (11) ◽  
pp. 7595-7608 ◽  
Author(s):  
Eunho Jang ◽  
Ki-Tae Park ◽  
Young Jun Yoon ◽  
Tae-Wook Kim ◽  
Sang-Bum Hong ◽  
...  
Keyword(s):  
Austral Summer ◽  
Particle Formation ◽  
Taxonomic Composition ◽  
Weddell Sea ◽  
Marine Biota ◽  
New Particle Formation ◽  
Air Masses ◽  
Bellingshausen Sea ◽  
The Antarctic ◽  
New Particles

Abstract. Marine biota is an important source of atmospheric aerosol particles in the remote marine atmosphere. However, the relationship between new particle formation and marine biota is poorly quantified. Long-term observations (from 2009 to 2016) of the physical properties of atmospheric aerosol particles measured at the Antarctic Peninsula (King Sejong Station; 62.2∘ S, 58.8∘ W) and satellite-derived estimates of the biological characteristics were analyzed to identify the link between new particle formation and marine biota. New particle formation events in the Antarctic atmosphere showed distinct seasonal variations, with the highest values occurring when the air mass originated from the ocean domain during the productive austral summer (December, January and February). Interestingly, new particle formation events were more frequent in the air masses that originated from the Bellingshausen Sea than in those that originated from the Weddell Sea. The monthly mean number concentration of nanoparticles (2.5–10 nm in diameter) was >2-fold higher when the air masses passed over the Bellingshausen Sea than the Weddell Sea, whereas the biomass of phytoplankton in the Weddell Sea was more than ∼70 % higher than that of the Bellingshausen Sea during the austral summer period. Dimethyl sulfide (DMS) is of marine origin and its oxidative products are known to be one of the major components in the formation of new particles. Both satellite-derived estimates of the biological characteristics (dimethylsulfoniopropionate, DMSP; precursor of DMS) and phytoplankton taxonomic composition and in situ methanesulfonic acid (84 daily measurements during the summer period in 2013 and 2014) analysis revealed that DMS(P)-rich phytoplankton were more dominant in the Bellingshausen Sea than in the Weddell Sea. Furthermore, the number concentration of nanoparticles was positively correlated with the biomass of phytoplankton during the period when DMS(P)-rich phytoplankton predominate. These results indicate that oceanic DMS emissions could play a key role in the formation of new particles; moreover, the taxonomic composition of phytoplankton could affect the formation of new particles in the Antarctic Ocean.

scholarly journals Unexpectedly high ultrafine aerosol concentrations above East Antarctic sea ice

2016 ◽  
Vol 16 (4) ◽  
pp. 2185-2206 ◽  
Author(s):  
R. S. Humphries ◽  
A. R. Klekociuk ◽  
R. Schofield ◽  
M. Keywood ◽  
J. Ward ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Southern Ocean ◽  
Sea Ice ◽  
Radiative Forcing ◽  
Free Troposphere ◽  
Radiative Balance ◽  
Air Masses ◽  
Antarctic Sea Ice ◽  
Ocean Region ◽  
The Antarctic

Abstract. Better characterisation of aerosol processes in pristine, natural environments, such as Antarctica, have recently been shown to lead to the largest reduction in uncertainties in our understanding of radiative forcing. Our understanding of aerosols in the Antarctic region is currently based on measurements that are often limited to boundary layer air masses at spatially sparse coastal and continental research stations, with only a handful of studies in the vast sea-ice region. In this paper, the first observational study of sub-micron aerosols in the East Antarctic sea ice region is presented. Measurements were conducted aboard the icebreaker Aurora Australis in spring 2012 and found that boundary layer condensation nuclei (CN3) concentrations exhibited a five-fold increase moving across the polar front, with mean polar cell concentrations of 1130 cm−3 – higher than any observed elsewhere in the Antarctic and Southern Ocean region. The absence of evidence for aerosol growth suggested that nucleation was unlikely to be local. Air parcel trajectories indicated significant influence from the free troposphere above the Antarctic continent, implicating this as the likely nucleation region for surface aerosol, a similar conclusion to previous Antarctic aerosol studies. The highest aerosol concentrations were found to correlate with low-pressure systems, suggesting that the passage of cyclones provided an accelerated pathway, delivering air masses quickly from the free troposphere to the surface. After descent from the Antarctic free troposphere, trajectories suggest that sea-ice boundary layer air masses travelled equatorward into the low-albedo Southern Ocean region, transporting with them emissions and these aerosol nuclei which, after growth, may potentially impact on the region's radiative balance. The high aerosol concentrations and their transport pathways described here, could help reduce the discrepancy currently present between simulations and observations of cloud and aerosol over the Southern Ocean.

scholarly journals DMS and MSA measurements in the Antarctic boundary layer: impact of BrO on MSA production

2008 ◽  
Vol 8 (1) ◽  
pp. 2657-2694 ◽  
Author(s):  
K. A. Read ◽  
A. C. Lewis ◽  
S. Bauguitte ◽  
A. M. Rankin ◽  
R. A. Salmon ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Austral Summer ◽  
Atmospheric Concentration ◽  
Air Masses ◽  
Average Value ◽  
Number Of Factors ◽  
Spatial Coverage ◽  
Antarctic Boundary Layer ◽  
The Antarctic

Abstract. In situ measurements of dimethyl sulphide (DMS) and methane sulphonic acid (MSA) were made at Halley Station, Antarctica (75°35´S, 26°19W) during February 2004–February 2005 as part of the CHABLIS (Chemistry of the Antarctic boundary layer and the interface with snow) project. DMS was present in the atmosphere at Halley all year (average 38.1±43 pptV) with a maximum monthly average value of 113.6±52 pptV in February 2004 coinciding temporally with a minimum in sea extent. Whilst seasonal variability and interannual variability can be attributed to a number of factors, short term variability appeared strongly dependent on air mass origin and trajectory pressure height. The MSA and derived non-sea salt sulphate (nss-SO42−) measurements showed no correlation with those of DMS (regression R2=0.039, and R2=0.001, respectively) in-line with the complexity of DMS fluxes, conflicting oxidation routes, transport of air masses and variable spatial coverage of both sea-ice and phytoplankton. MSA was generally low throughout the year, with an annual average of 42 ng m−3 (9.8±13.2 pptV), however MSA: nss-SO42− ratios were high implying a dominance of the addition oxidation route for DMS. Including BrO measurements into MSA production calculations demonstrated the significance of BrO on DMS oxidation within this region of the atmosphere in austral summer. Assuming an 80% yield of DMSO from the reaction of DMS+BrO, an atmospheric concentration of BrO equal to 3 pptV increased the calculated MSA production from DMS by a factor of 9 above that obtained when considering only reaction with the hydroxyl radical.

scholarly journals Climatic and Chemical Studies in James Ross Island Snow (Antarctic Peninsula) (Abstract only)

1982 ◽  
Vol 3 ◽  
pp. 347-347
Author(s):  
A Aristarain ◽  
M Briat ◽  
R Delmas ◽  
M Pourchet ◽  
J Jouzel
Keyword(s):  
Antarctic Peninsula ◽  
Seasonal Variations ◽  
Ice Core ◽  
Sea Salt ◽  
Eastern Coast ◽  
Mean Annual Temperature ◽  
Ice Cap ◽  
James Ross Island ◽  
The Mean ◽  
The Antarctic

James Ross Island (mean diameter 50 km) is located near the north-eastern coast of the Antarctic Peninsula. An ice cap, covering nearly the entire island, rises to a height of ~1 600 m. Three summer expeditions with glaciological purposes were recently achieved on this ice cap by the Instituto Antártico Argentino, two of them with the scientific participation of the Laboratoire de Glaciologie et Geophysique de I'Environnement, Grenoble.We present results of climatic and chemical investigations performed on recent snow layers dating back about 25 a. The studied samples were collected at different sites on the upper part of the ice dome. Detailed measurements (deuterium, oxygen 18 and total β activity) were performed on more than 1000 selected samples. The relationship between stable isotope and mean annual temperature fits very well with the one previously obtained in the Antarctic Peninsula.An ice core 22 m deep drilled on Dome Dalinqer (elevation 1600 m, mean annual temperature -15˚C) showed well-preserved seasonal variations in deuterium all along the profile, thus providing a yearly dating of the samples which was confirmed by β activity reference levels. The mean annual accumulation thus deduced is 500 kg m−2 between 1955 and 1979, with values significantly lower (30%) in the 1955–65 decade than in 1965–79. The same trend earlier observed in east and central parts of Antarctica thus appears to have a very large geographical extent.This well-dated core allows us to undertake a year-to-year comparison between isotopic and climatological data over the 1953–78 period. The mean annual values of the deuterium content are well correlated with the average surface temperature taken over the whole Antarctic Peninsula (δD = (3.4±2.0)T - (98±32))These data and the experimentally derived δD/δ180 relationship obtained on James Ross Island allow us to deduce a δ180 temperature gradient of 0.44‰°C−1. This low value is discussed in view of a new isotopic model taking into account the partial removal of precipitation and the possible variation of the oceanic source. James Ross Island thus appears suitable as a potential site for reconstructing past climatic changes of the Antarctic Peninsula beyond existing data.Contamination-free techniques were used for sampling and analysing the snow samples. Na, K, Ca, and Al (by atomic absorption), H+ (by titrimetric measurements), SO42- and NO3− (by ion chromatography), and conductivity were determined on more than 100 samples collected in a 4.3 m deep pit. Some of these parameters were also measured on ice-core samples or additional pit samples.Snow impurities are contributed by different aerosol sources: sea salt, continental particles and the small-size particles produced by the conversion of various atmospheric gases. The relative importance of these sources has been estimated.James Ross snow was found always to be slightly acid (1 to 10 μEquiv. l−1 of H+, mainly as sulphuric acid). Nitrate concentrations are much smaller (0.4 μEquiv. l−1). Strong seasonal variations are observed for H2SO4 deposition, probably in relation to its formation in the Antarctic atmosphere.Sea-salt deposition exhibits also seasonal variations which can be correlated with storm frequency in the Weddell Sea area. The continental aerosol contribution is weak as indicated by very low Al values.The influence of Deception Island volcanism on the regional aerosol chemistry is examined. A marked increase of snow acidity was detected after the 1967 eruption of this volcano, but no ash layers were observed.The strong variations of the conductivity of melt water are interpreted: it is shown that this parameter is not representative of the extent of sea ice

scholarly journals Contribution of combustion Fe in marine aerosols over the northwestern Pacific estimated by Fe stable isotope ratios

2021 ◽  
Vol 21 (20) ◽  
pp. 16027-16050
Author(s):  
Minako Kurisu ◽  
Kohei Sakata ◽  
Mitsuo Uematsu ◽  
Akinori Ito ◽  
Yoshio Takahashi
Keyword(s):  
East Asia ◽  
Fine Particles ◽  
Isotope Ratios ◽  
The Other ◽  
Northwestern Pacific ◽  
Large Contribution ◽  
Coarse Particles ◽  
Marine Aerosols ◽  
Air Masses ◽  
Surface Ocean

Abstract. The source apportionment of aerosol iron (Fe), including natural and combustion Fe, is an important issue because aerosol Fe can enhance oceanic primary production in the surface ocean. Based on our previous finding that combustion Fe emitted by evaporation processes has Fe isotope ratios (δ56Fe) that are approximately 4 ‰ lower than those of natural Fe, this study aimed to distinguish aerosol Fe sources over the northwestern Pacific using two size-fractionated marine aerosols. The δ56Fe values of fine and coarse particles from the eastern or northern Pacific were found to be similar to each other, ranging from 0.0 ‰ to 0.4 ‰. Most of them were close to the crustal average, suggesting the dominance of natural Fe. On the other hand, particles from the direction of East Asia demonstrated lower δ56Fe values in fine particles (−0.5 ‰ to −2.2 ‰) than in coarse particles (on average −0.02 ± 0.12 ‰). The correlations between the δ56Fe values and the enrichment factors of lead and vanadium suggested that the low δ56Fe values obtained were due to the presence of combustion Fe. The δ56Fe values of the soluble component of fine particles in this region were lower than the total, indicating the preferential dissolution of combustion Fe. In addition, we found a negative correlation between the δ56Fe value and the fractional Fe solubility in air masses from the direction of East Asia. These results suggest that the presence of combustion Fe is an important factor in controlling the fractional Fe solubility in air masses from the direction of East Asia, whereas other factors are more important in the other areas. By assuming typical δ56Fe values for combustion and natural Fe, the contribution of combustion Fe to the total (acid-digested) Fe in aerosols was estimated to reach up to 50 % of fine and 21 % of bulk (coarse + fine) particles in air masses from the direction of East Asia, whereas its contribution was small in the other areas. The contribution of combustion Fe to the soluble Fe component estimated for one sample was approximately twice as large as the total, indicating the importance of combustion Fe as a soluble Fe source despite lower emissions than the natural. These isotope-based estimates were compared with those estimated using an atmospheric chemical transport model (IMPACT), in which the fractions of combustion Fe in fine particles, especially in air masses from the direction of East Asia, were consistent with each other. In contrast, the model estimated a relatively large contribution from combustion Fe in coarse particles, probably because of the different characteristics of combustion Fe that are included in the model calculation and the isotope-based estimation. This highlights the importance of observational data on δ56Fe for size-fractionated aerosols to scale the combustion Fe emission by the model. The average deposition fluxes of soluble Fe to the surface ocean were 1.4 and 2.9 nmol m−2 d−1 from combustion and natural aerosols, respectively, in air masses from the direction of East Asia, which suggests that combustion Fe could be an important Fe source to the surface seawater among other Fe sources. Distinguishing Fe sources using the δ56Fe values of marine aerosols and seawater is anticipated to lead to a more quantitative understanding of the Fe cycle in the atmosphere and surface ocean.

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