In this study we present a qualitative and quantitative assessment of more than 10 yr of aerosol number size distribution data observed in the Arctic environment (Mt. Zeppelin (78°56' N, 11°53' E, ...474 m a.s.l.), Ny Ålesund, Svalbard). We provide statistics on both seasonal and diurnal characteristics of the aerosol observations and conclude that the Arctic aerosol number size distribution and related parameters such as integral mass and surface area exhibit a very pronounced seasonal variation. This seasonal variation seems to be controlled by both dominating source as well as meteorological conditions. Three distinctly different periods can be identified during the Arctic year: the haze period characterized by a dominating accumulation mode aerosol (March–May), followed by the sunlit summer period with low abundance of accumulation mode particles but high concentration of small particles which are likely to be recently and locally formed (June–August). The rest of the year is characterized by a comparably low concentration of accumulation mode particles and negligible abundance of ultrafine particles (September–February). A minimum in aerosol mass and number concentration is usually observed during September/October. We further show that the transition between the different regimes is fast, suggesting rapid change in the conditions defining their appearance. A source climatology based on trajectory analysis is provided, and it is shown that there is a strong seasonality of dominating source areas, with Eurasia dominating during the Autumn–Winter period and dominance of North Atlantic air during the summer months. We also show that new-particle formation events are rather common phenomena in the Arctic during summer, and this is the result of photochemical production of nucleating/condensing species in combination with low condensation sink. It is also suggested that wet removal may play a key role in defining the Arctic aerosol year, via the removal of accumulation mode size particles, which in turn have a pivotal role in facilitating the conditions favorable for new-particle formation events. In summary the aerosol Arctic year seems to be at least qualitatively predictable based on the knowledge of seasonality of transport paths and associated source areas, meteorological conditions and removal processes.
Sub-micrometer particle size distributions measured during four summer cruises of the Swedish icebreaker Oden 1991, 1996, 2001, and 2008 were combined with dimethyl sulfide gas data, back ...trajectories, and daily maps of pack ice cover in order to investigate source areas and aerosol formation processes of the boundary layer aerosol in the central Arctic. With a clustering algorithm, potential aerosol source areas were explored. Clustering of particle size distributions together with back trajectories delineated five potential source regions and three different aerosol types that covered most of the Arctic Basin: marine, newly formed and aged particles over the pack ice. Most of the pack ice area with < 15% of open water under the trajectories exhibited the aged aerosol type with only one major mode around 40 nm. For newly formed particles to occur, two conditions had to be fulfilled over the pack ice: the air had spent 10 days while traveling over ever more contiguous ice and had traveled over less than 30% open water during the last 5 days. Additionally, the air had experienced more open water (at least twice as much as in the cases of aged aerosol) during the last 4 days before arrival in heavy ice conditions at Oden. Thus we hypothesize that these two conditions were essential factors for the formation of ultrafine particles over the central Arctic pack ice. In a comparison the Oden data with summer size distribution data from Alert, Nunavut, and Mt. Zeppelin, Spitsbergen, we confirmed the Oden findings with respect to particle sources over the central Arctic. Future more frequent broken-ice or open water patches in summer will spur biological activity in surface water promoting the formation of biological particles. Thereby low clouds and fogs and subsequently the surface energy balance and ice melt may be affected.
We use a global aerosol microphysics model in combination with an offline radiative transfer model to quantify the radiative effect of biogenic secondary organic aerosol (SOA) in the present-day ...atmosphere. Through its role in particle growth and ageing, the presence of biogenic SOA increases the global annual mean concentration of cloud condensation nuclei (CCN; at 0.2% supersaturation) by 3.6-21.1%, depending upon the yield of SOA production from biogenic volatile organic compounds (BVOCs), and the nature and treatment of concurrent primary carbonaceous emissions. This increase in CCN causes a rise in global annual mean cloud droplet number concentration (CDNC) of 1.9-5.2%, and a global mean first aerosol indirect effect (AIE) of between +0.01 W m-2 and -0.12 W m-2. The radiative impact of biogenic SOA is far greater when biogenic oxidation products also contribute to the very early stages of new particle formation; using two organically mediated mechanisms for new particle formation, we simulate global annual mean first AIEs of -0.22 W m-2 and -0.77 W m-2. The inclusion of biogenic SOA substantially improves the simulated seasonal cycle in the concentration of CCN-sized particles observed at three forested sites. The best correlation is found when the organically mediated nucleation mechanisms are applied, suggesting that the first AIE of biogenic SOA could be as large as -0.77 W m-2. The radiative impact of SOA is sensitive to the presence of anthropogenic emissions. Lower background aerosol concentrations simulated with anthropogenic emissions from 1750 give rise to a greater fractional CCN increase and a more substantial first AIE from biogenic SOA. Consequently, the anthropogenic indirect radiative forcing between 1750 and the present day is sensitive to assumptions about the amount and role of biogenic SOA. We also calculate an annual global mean direct radiative effect of between -0.08 W m-2 and -0.78 W m-2 in the present day, with uncertainty in the amount of SOA produced from the oxidation of BVOCs accounting for most of this range.
Atmospheric new particle formation (NPF) and growth significantly influences climate by supplying new seeds for cloud condensation and brightness. Currently, there is a lack of understanding of ...whether and how marine biota emissions affect aerosol-cloud-climate interactions in the Arctic. Here, the aerosol population was categorised via cluster analysis of aerosol size distributions taken at Mt Zeppelin (Svalbard) during a 11 year record. The daily temporal occurrence of NPF events likely caused by nucleation in the polar marine boundary layer was quantified annually as 18%, with a peak of 51% during summer months. Air mass trajectory analysis and atmospheric nitrogen and sulphur tracers link these frequent nucleation events to biogenic precursors released by open water and melting sea ice regions. The occurrence of such events across a full decade was anti-correlated with sea ice extent. New particles originating from open water and open pack ice increased the cloud condensation nuclei concentration background by at least ca. 20%, supporting a marine biosphere-climate link through sea ice melt and low altitude clouds that may have contributed to accelerate Arctic warming. Our results prompt a better representation of biogenic aerosol sources in Arctic climate models.
Long‐term measurements of the light absorption coefficient (babs) obtained with a particle soot absorption photometer (PSAP), babs (PSAP), have been previously reported for Barrow, Alaska, and ...Ny‐Ålesund, Spitsbergen, in the Arctic. However, the effects on babs of other aerosol chemical species coexisting with black carbon (BC) have not been critically evaluated. Furthermore, different mass absorption cross section (MAC) values have been used to convert babs to BC mass concentration (MBC = babs/MAC). We used a continuous soot monitoring system (COSMOS), which uses a heated inlet to remove volatile aerosol compounds, to measure babs (babs (COSMOS)) at these sites during 2012–2015. Field measurements and laboratory experiments have suggested that babs (COSMOS) is affected by about 9% on average by sea‐salt aerosols. MBC values derived by COSMOS (MBC (COSMOS)) using a MAC value obtained by our previous studies agreed to within 9% with elemental carbon concentrations at Barrow measured over 11 months. babs (PSAP) was higher than babs (COSMOS), by 22% at Barrow (PM1) and by 43% at Ny‐Ålesund (PM10), presumably due to the contribution of volatile aerosol species to babs (PSAP). Using babs (COSMOS) as a reference, we derived MBC (PSAP) from babs (PSAP) measured since 1998. We also established the seasonal variations of MBC at these sites. Seasonally averaged MBC (PSAP) decreased at a rate of about 0.55 ± 0.30 ng m−3 yr−1. We also compared MBC (COSMOS) and scaled MBC (PSAP) values with previously reported data and evaluated the degree of inconsistency in the previous data.
Key Points
We evaluated the accuracy of black carbon (BC) measurements at Barrow, Alaska, and Ny‐Ålesund, Spitsbergen, in the Arctic
At Barrow, seasonally averaged BC mass concentrations decreased in winter and summer at a rate of 0.55 ± 0.30 ng m−3 yr−1 during 1998–2015
We established seasonal variations of BC at the two sites and evaluated the causes of the inconsistency of the previously reported data
Samples of rainwater (RW) were collected to characterize the chemistry and sources in two representative megacities at Pune (Southwest) and Delhi (Northern) India from 2011 to 2014 across two ...seasons: monsoon (MN) and non-monsoon (NMN). Collected RW samples were analyzed for major chemical constituents (F−, Cl−, SO42−, NO3−, NH4+, Na+, K+, Ca2+, and Mg2+), pH and conductivity. In addition, bicarbonate (HCO3−) was also estimated. The mean pH values of the RW were >6 at Pune and <6 at Delhi and 4% and 26% were acidic, respectively. The mean sum of all measured ionic species in Pune and Delhi was 304.7 and 536.4 μeq/l, respectively, indicating that significant atmospheric pollution effects in these Indian mega cities. Both the Ca2+ and SO42− were the dominant ions, accounting for 43% (Pune) and 54% (Delhi) of the total ions. The sum of measured ions during the NMN period was greater than the NM period by a factor of 1.5 for Pune (278.4: NM and 412.1: NMN μeq/l) and a factor of about 2.5 for Delhi (406 and 1037.7 μeq/l). The contributions of SO42− and NO3− to the RW acidity were ∼40% and 60%, respectively, at Pune and correspondingly, 36% and 64% at Delhi. The concentrations of secondary aerosols (SO42−and NO3−) were higher by a factor of two and three when the air masses were transported to Pune from the continental side. At Delhi, the concentrations of SO42−, NO3−, Ca2+, and Mg2+ were significantly higher when the air masses arrive from Punjab, Haryana, and Pakistan indicating the greater atmospheric pollution over the Indo-Gangetic Plain. Positive matrix factorization was applied to the source apportionment of the deposition fluxes of these ions. Three factors were obtained for Pune and four for Delhi. The sources at Pune were secondary aerosols from fossil fuel combustion, soil dust, and marine, whereas, at Delhi, the sources were soil, fossil fuel combustion, biomass burning, and industrial chlorine.
•76% higher loading of chemical constituents over Delhi than Pune.•Higher secondary aerosols in RW over Delhi from NW direction.•∼4 and 26% acidic samples were observed in Pune and Delhi.•Lower concentrations of ions from the Arabian Sea.
In recent decades much attention has been given to the Arctic environment, where climate change is happening rapidly. Black carbon (BC) has been shown to be a major component of Arctic pollution that ...also affects the radiative balance. In the present study, we focused on how vegetation fires that occurred in northern Eurasia during the period of 2002–2013 influenced the budget of BC in the Arctic. For simulating the transport of fire emissions from northern Eurasia to the Arctic, we adopted BC fire emission estimates developed independently by GFED3 (Global Fire Emissions Database) and FEI-NE (Fire Emission Inventory – northern Eurasia). Both datasets were based on fire locations and burned areas detected by MODIS (Moderate resolution Imaging Spectroradiometer) instruments on NASA's (National Aeronautics and Space Administration) Terra and Aqua satellites. Anthropogenic sources of BC were adopted from the MACCity (Monitoring Atmospheric Composition and Climate and megacity Zoom for the Environment) emission inventory.During the 12-year period, an average area of 250 000 km2 yr−1 was burned in northern Eurasia (FEI-NE) and the global emissions of BC ranged between 8.0 and 9.5 Tg yr−1 (FEI-NE+MACCity). For the BC emitted in the Northern Hemisphere (based on FEI-NE+MACCity), about 70 % originated from anthropogenic sources and the rest from biomass burning (BB). Using the FEI-NE+MACCity inventory, we found that 102 ± 29 kt yr−1 BC was deposited in the Arctic (defined here as the area north of 67° N) during the 12 years simulated, which was twice as much as when using the MACCity inventory (56 ± 8 kt yr−1). The annual mass of BC deposited in the Arctic from all sources (FEI-NE in northern Eurasia, MACCity elsewhere) is significantly higher by about 37 % in 2009 (78 vs. 57 kt yr−1) to 181 % in 2012 (153 vs. 54 kt yr−1), compared to the BC deposited using just the MACCity emission inventory. Deposition of BC in the Arctic from BB sources in the Northern Hemisphere thus represents 68 % of the BC deposited from all BC sources (the remaining being due to anthropogenic sources). Northern Eurasian vegetation fires (FEI-NE) contributed 85 % (79–91 %) to the BC deposited over the Arctic from all BB sources in the Northern Hemisphere.We estimate that about 46 % of the BC deposited over the Arctic from vegetation fires in northern Eurasia originated from Siberia, 6 % from Kazakhstan, 5 % from Europe, and about 1 % from Mongolia. The remaining 42 % originated from other areas in northern Eurasia. About 42 % of the BC released from northern Eurasian vegetation fires was deposited over the Arctic (annual average: 17 %) during spring and summer.
Sources, composition and occurrence of secondary organic aerosols in the Arctic were investigated at Zeppelin Mountain, Svalbard, and Station Nord, northeastern Greenland, during the full annual ...cycle of 2008 and 2010, respectively. Speciation of organic acids, organosulfates and nitrooxy organosulfates – from both anthropogenic and biogenic precursors were in focus. A total of 11 organic acids (terpenylic acid, benzoic acid, phthalic acid, pinic acid, suberic acid, azelaic acid, adipic acid, pimelic acid, pinonic acid, diaterpenylic acid acetate and 3-methyl-1,2,3-butanetricarboxylic acid), 12 organosulfates and 1 nitrooxy organosulfate were identified in aerosol samples from the two sites using a high-performance liquid chromatograph (HPLC) coupled to a quadrupole Time-of-Flight mass spectrometer. At Station Nord, compound concentrations followed a distinct annual pattern, where high mean concentrations of organosulfates (47 ± 14 ng m−3) and organic acids (11.5 ± 4 ng m−3) were observed in January, February and March, contrary to considerably lower mean concentrations of organosulfates (2 ± 3 ng m−3) and organic acids (2.2 ± 1 ng m−3) observed during the rest of the year. At Zeppelin Mountain, organosulfate and organic acid concentrations remained relatively constant during most of the year at a mean concentration of 15 ± 4 ng m−3 and 3.9 ± 1 ng m−3, respectively. However during four weeks of spring, remarkably higher concentrations of total organosulfates (23–36 ng m−3) and total organic acids (7–10 ng m−3) were observed. Elevated organosulfate and organic acid concentrations coincided with the Arctic haze period at both stations, where northern Eurasia was identified as the main source region. Air mass transport from northern Eurasia to Zeppelin Mountain was associated with a 100% increase in the number of detected organosulfate species compared with periods of air mass transport from the Arctic Ocean, Scandinavia and Greenland. The results from this study suggested that the presence of organic acids and organosulfates at Station Nord was mainly due to long-range transport, whereas indications of local sources were found for some compounds at Zeppelin Mountain. Furthermore, organosulfates contributed significantly to organic matter throughout the year at Zeppelin Mountain (annual mean of 13 ± 8%) and during Arctic haze at Station Nord (7 ± 2%), suggesting organosulfates to be important compounds in Arctic aerosols.
We examine the relationship between the number concentration of boundary-layer cloud condensation nuclei (CCN) and light extinction to investigate underlying aerosol processes and satellite-based CCN ...estimates. For a variety of airborne and ground-based observations not dominated by dust, regression identifies the CCN (cm-3) at 0.4 plus or minus 0.1% supersaturation with 100.3 alpha +1.3 sigma 0.75 where sigma (Mm-1) is the 500 nm extinction coefficient by dried particles and alpha is the Angstrom exponent. The deviation of 1 km horizontal average data from this approximation is typically within a factor of 2.0. partial differential logCCN / partial differential log sigma is less than unity because, among other explanations, growth processes generally make aerosols scatter more light without increasing their number. This, barring special meteorology-aerosol connections, associates a doubling of aerosol optical depth with less than a doubling of CCN, contrary to previous studies based on heavily averaged measurements or a satellite algorithm.
Black carbon (BC) is an important atmospheric aerosol constituent that affects the climate by absorbing (directly) the sunlight and modifying cloud characteristics (indirectly). Here, we present ...first time yearlong measurements of BC and carbon monoxide (CO) from an urban location of Guwahati located in the Brahmaputra River valley (BRV) in the northeast region of India from 1st July 2013 to 30th June 2014. Daily BC concentrations varied within the range of 2.86 to 11.56μgm−3 with an annual average of 7.17±1.89μgm−3, while, CO varied from 0.19 to 1.20ppm with a mean value of 0.51±0.19ppm during the study period. The concentrations of BC (8.37μgm−3) and CO (0.67ppm) were ~39% and ~55% higher during the dry months (October to March) than the wet months (April to September) suggesting that seasonal changes in meteorology and emission sources play an important role in controlling these species. The seasonal ΔBC/ΔCO ratios were highest (lowest) in the pre-monsoon (winter) 18.1±1.4μgm−3ppmv−1 (12.6±2.2μgm−3ppmv−1) which indicate the combustion of biofuel/biomass as well as direct emissions from fossil fuel during the pre-monsoon season. The annual BC emission was estimated to be 2.72Gg in and around Guwahati which is about 44% lower than the mega city ‘Delhi’ (4.86Gg). During the study period, the annual mean radiative forcing (RF) at the top of the atmosphere (TOA) for clear skies of BC was +9.5Wm−2, however, the RF value at the surface (SFC) was −21.1Wm−2 which indicates the net warming and cooling effects, respectively. The highest RF at SFC was in the month of April (−30Wm−2) which is coincident with the highest BC mass level. The BC atmospheric radiative forcing (ARF) was +30.16 (annual mean) Wm−2 varying from +23.1 to +43.8Wm−2. The annual mean atmospheric heating rate (AHR) due to the BC aerosols was 0.86Kday−1 indicates the enhancement in radiation effect over the study region. The Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) captured the seasonal cycle of observed BC fairly well but underestimated the observed BC during the month of May–August. Model results show that BC at Guwahati is controlled mainly by anthropogenic emissions except during the pre-monsoon season when open biomass burning also makes a similar contribution.
Figure: The monthly mean radiative forcing (RF) at the top of the atmosphere (TOA) due to BC aerosols for clear skies over Guwahati, northeast region of India from 1st July 2013 to 30th June 2014. The RFs values at TOA are varying between +7.2 and +13.5Wm−2 with annual mean (+9.5Wm−2), however, at surface (SFC), the RFs values are −15.9 to −30.3Wm−2 with mean (−21.1Wm−2), which indicate the net warming and cooling effects respectively. The Atmosphere radiative forcing (ARF) due to BC was +30.16Wm−2 indicates warming effect to the atmosphere over Guwahati. Display omitted
•The first time yearlong BC (mean: 7.2μgm−3) measurement over BRV•Higher atmosphere forcing (+30.16Wm−2) & heating (0.86Kday−1) over BRV•Annual BC emissions are 2.72Gg.•39% (BC) and 46% (CO) were higher during the dry period than wet period.•Highest ΔBC/ΔCO ratio (18.1μgm−3ppmv−1) in the pre-monsoon season
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