Origins of black carbon from anthropogenic emissions and open biomass burning transported to Xishuangbanna, Southwest China

Abstract. This study examines differences in the surface black carbon (BC) aerosol loading between the Bay of Bengal (BoB) and the Arabian Sea (AS) and identifies dominant sources of BC in South Asia and surrounding regions during March–May 2006 (Integrated Campaign for Aerosols, Gases and Radiation Budget, ICARB) period. A total of 13 BC tracers are introduced in the Weather Research and Forecasting Model coupled with Chemistry to address these objectives. The model reproduced the temporal and spatial variability of BC distribution observed over the AS and the BoB during the ICARB ship cruise and captured spatial variability at the inland sites. In general, the model underestimates the observed BC mass concentrations. However, the model–observation discrepancy in this study is smaller compared to previous studies. Model results show that ICARB measurements were fairly well representative of the AS and the BoB during the pre-monsoon season. Elevated BC mass concentrations in the BoB are due to 5 times stronger influence of anthropogenic emissions on the BoB compared to the AS. Biomass burning in Burma also affects the BoB much more strongly than the AS. Results show that anthropogenic and biomass burning emissions, respectively, accounted for 60 and 37% of the average ± standard deviation (representing spatial and temporal variability) BC mass concentration (1341 ± 2353 ng m−3) in South Asia. BC emissions from residential (61%) and industrial (23%) sectors are the major anthropogenic sources, except in the Himalayas where vehicular emissions dominate. We find that regional-scale transport of anthropogenic emissions contributes up to 25% of BC mass concentrations in western and eastern India, suggesting that surface BC mass concentrations cannot be linked directly to the local emissions in different regions of South Asia.

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Black carbon variability since preindustrial times in Eastern part of Europe reconstructed from Mt Elbrus, Caucasus ice cores

10.5194/acp-2016-804 ◽

2016 ◽

Author(s):

Saehee Lim ◽

Xavier Faïn ◽

Patrick Ginot ◽

Vladimir Mikhalenko ◽

Stanislav Kutuzov ◽

...

Keyword(s):

Black Carbon ◽

20Th Century ◽

Biomass Burning ◽

Mass Concentration ◽

Ice Core ◽

Ice Cores ◽

Anthropogenic Emissions ◽

Ice Core Record ◽

Summer Time ◽

Mass Concentrations

Abstract. Black carbon (BC), emitted by fossil fuel combustion and biomass burning, is the second largest man-made contributor to global warming after carbon dioxide (Bond et al., 2013). However, limited information exists on its past emissions and atmospheric variability. In this study, we present the first high-resolution record of refractory BC (rBC, including mass concentration and size) reconstructed from ice cores drilled at a high-altitude Eastern European site in Mt. Elbrus (ELB), Caucasus (5115 m a.s.l.). The ELB ice core record, covering the period 1825–2013, reflects the atmospheric load of rBC particles at the ELB site transported from the European continent with a larger rBC input from sources located in the Eastern part of Europe. In the first half of the 20th century, European anthropogenic emissions resulted in a 1.5-fold increase in the ice core rBC mass concentrations as respect to its level in the preindustrial era (before 1850). The rBC mass concentrations increased by a 5-fold in 1960–1980, followed by a decrease until ~ 2000. Over the last decade, the rBC signal for summer time slightly increased. We have compared the signal with the atmospheric BC load simulated using past BC emissions (ACCMIP and MACCity inventories) and taken into account the contribution of different geographical region to rBC distribution and deposition at the ELB site. Interestingly, the observed rBC variability in the ELB ice core record since the 1960s is not in perfect agreement with the simulated atmospheric BC load. Similar features between the ice core rBC record and the best scenarios for the atmospheric BC load support that anthropogenic BC increase in the 20th century is reflected in the ELB ice core record. However, the peak in BC mass concentration observed in ~ 1970 in the ice core is estimated to occur a decade later from past inventories. BC emission inventories for the period 1960s–1970s may be underestimating European anthropogenic emissions. Furthermore, for summer time snow layers of the last 2000s, the slightly increasing trend of rBC deposition likely reflects recent changes in anthropogenic and biomass burning BC emissions in the Eastern part of Europe. Our study highlights that the past changes in BC emissions of Eastern Europe need to be considered in assessing on-going air quality regulation.

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Source sector and region contributions to black carbon and PM<sub>2.5</sub> in the Arctic

Atmospheric Chemistry and Physics ◽

10.5194/acp-18-18123-2018 ◽

2018 ◽

Vol 18 (24) ◽

pp. 18123-18148 ◽

Cited By ~ 9

Author(s):

Negin Sobhani ◽

Sarika Kulkarni ◽

Gregory R. Carmichael

Keyword(s):

Black Carbon ◽

Biomass Burning ◽

Surface Concentration ◽

The Arctic ◽

Anthropogenic Emissions ◽

Economic Sectors ◽

Modeling Framework ◽

Source Regions ◽

Geographical Regions ◽

Chinese Industry

Abstract. The impacts of black carbon (BC) and particulate matter with aerodynamic diameters less than 2.5 µm (PM2.5) emissions from different source sectors (e.g., transportation, power, industry, residential, and biomass burning) and geographic source regions (e.g., Europe, North America, China, Russia, central Asia, south Asia, and the Middle East) to Arctic BC and PM2.5 concentrations are investigated through a series of annual sensitivity simulations using the Weather Research and Forecasting – sulfur transport and deposition model (WRF-STEM) modeling framework. The simulations are validated using observations at two Arctic sites (Alert and Barrow Atmospheric Baseline Observatory), the Interagency Monitoring of Protected Visual Environments (IMPROVE) surface sites over the US, and aircraft observations over the Arctic during spring and summer 2008. Emissions from power, industrial, and biomass burning sectors are found to be the main contributors to the Arctic PM2.5 surface concentration, with contributions of ∼ 30 %, ∼ 25 %, and ∼ 20 %, respectively. In contrast, the residential and transportation sectors are identified as the major contributors to Arctic BC, with contributions of ∼ 38 % and ∼ 30 %. Anthropogenic emissions are the most dominant contributors (∼ 88 %) to the BC surface concentration over the Arctic annually; however, the contribution from biomass burning is significant over the summer (up to ∼ 50 %). Among all geographical regions, Europe and China have the highest contributions to the BC surface concentrations, with contributions of ∼ 46 % and ∼ 25 %, respectively. Industrial and power emissions had the highest contributions to the Arctic sulfate (SO4) surface concentration, with annual contributions of ∼ 43 % and ∼ 41 %, respectively. Further sensitivity runs show that, among various economic sectors of all geographic regions, European and Chinese residential sectors contribute to ∼ 25 % and ∼ 14 % of the Arctic average surface BC concentration. Emissions from the Chinese industry sector and European power sector contribute ∼ 12 % and ∼ 18 % of the Arctic surface sulfate concentration. For Arctic PM2.5, the anthropogenic emissions contribute > ∼ 75 % at the surface annually, with contributions of ∼ 25 % from Europe and ∼ 20 % from China; however, the contributions of biomass burning emissions are significant in particular during spring and summer. The contributions of each geographical region to the Arctic PM2.5 and BC vary significantly with altitude. The simulations show that the BC from China is transported to the Arctic in the midtroposphere, while BC from European emission sources are transported near the surface under 5 km, especially during winter.

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FLEXPART v10.1 simulation of source contributions to Arctic black carbon

Atmospheric Chemistry and Physics ◽

10.5194/acp-20-1641-2020 ◽

2020 ◽

Vol 20 (3) ◽

pp. 1641-1656 ◽

Cited By ~ 3

Author(s):

Chunmao Zhu ◽

Yugo Kanaya ◽

Masayuki Takigawa ◽

Kohei Ikeda ◽

Hiroshi Tanimoto ◽

...

Keyword(s):

Black Carbon ◽

Biomass Burning ◽

Anthropogenic Sources ◽

The Arctic ◽

Anthropogenic Emissions ◽

High Altitudes ◽

Arctic Environment ◽

Gas Flaring ◽

Rapid Changes ◽

Arctic Surface

Abstract. The Arctic environment is undergoing rapid changes such as faster warming than the global average and exceptional melting of glaciers in Greenland. Black carbon (BC) particles, which are a short-lived climate pollutant, are one cause of Arctic warming and glacier melting. However, the sources of BC particles are still uncertain. We simulated the potential emission sensitivity of atmospheric BC present over the Arctic (north of 66∘ N) using the FLEXPART (FLEXible PARTicle) Lagrangian transport model (version 10.1). This version includes a new aerosol wet removal scheme, which better represents particle-scavenging processes than older versions did. Arctic BC at the surface (0–500 m) and high altitudes (4750–5250 m) is sensitive to emissions in high latitude (north of 60∘ N) and mid-latitude (30–60∘ N) regions, respectively. Geospatial sources of Arctic BC were quantified, with a focus on emissions from anthropogenic activities (including domestic biofuel burning) and open biomass burning (including agricultural burning in the open field) in 2010. We found that anthropogenic sources contributed 82 % and 83 % of annual Arctic BC at the surface and high altitudes, respectively. Arctic surface BC comes predominantly from anthropogenic emissions in Russia (56 %), with gas flaring from the Yamalo-Nenets Autonomous Okrug and Komi Republic being the main source (31 % of Arctic surface BC). These results highlight the need for regulations to control BC emissions from gas flaring to mitigate the rapid changes in the Arctic environment. In summer, combined open biomass burning in Siberia, Alaska, and Canada contributes 56 %–85 % (75 % on average) and 40 %–72 % (57 %) of Arctic BC at the surface and high altitudes, respectively. A large fraction (40 %) of BC in the Arctic at high altitudes comes from anthropogenic emissions in East Asia, which suggests that the rapidly growing economies of developing countries could have a non-negligible effect on the Arctic. To our knowledge, this is the first year-round evaluation of Arctic BC sources that has been performed using the new wet deposition scheme in FLEXPART. The study provides a scientific basis for actions to mitigate the rapidly changing Arctic environment.

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Influence of biomass burning and anthropogenic emissions on ozone, carbon monoxide and black carbon concentrations at the Mt. Cimone GAW-WMO global station (Italy, 2165 m a.s.l.)

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-12-21399-2012 ◽

2012 ◽

Vol 12 (8) ◽

pp. 21399-21435 ◽

Cited By ~ 2

Author(s):

P. Cristofanelli ◽

F. Fierli ◽

A. Marinoni ◽

R. Duchi ◽

J. Burkhart ◽

...

Keyword(s):

Carbon Monoxide ◽

Black Carbon ◽

Biomass Burning ◽

Dispersion Model ◽

Anthropogenic Pollution ◽

Global Scale ◽

Local Source ◽

Anthropogenic Emissions ◽

Large Variability ◽

Air Masses

Abstract. This work investigates the variability of ozone (O3), carbon monoxide (CO) and equivalent black carbon (BC) concentrations at the Italian Climate Observatory "O. Vittori" (ICO-OV), part of the Mt. Cimone global GAW-WMO station (Italy). For this purpose, ICO-OV observations carried out in the period January 2007–June 2009, have been analysed and correlated with the output of the FLEXPART Lagrangian dispersion model to specifically evaluate the influence of biomass burning (BB) and anthropogenic emissions younger than 20 days. During the investigation period, the average O3, CO and BC concentrations at ICO-OV were 54 ± 3 ppbv, 122 ± 7 ppbv and 213 ± 34 ng m−3 (mean ± expanded uncertainty with p<95%), with clear seasonal cycles characterized by summer maxima and winter minima for O3 and BC and spring maximum and summer minimum for CO. According to FLEXPART output, BB impact is maximized during the warm months from July to September but appeared to have a significant contribution to the observed tracer concentrations only during specific transport events. We characterised in detail five major events with respect to transport scales (i.e. global, regional and local), source regions and O3, CO and BC variations. For these events, very large variability of enhancement ratios O3/CO (from −0.22 to 0.71) and BC/CO (from 2.69 to 29.83 ng m−3 ppbv−1) were observed. CO related with anthropogenic emissions (COant) contributed to 17.4% of the mean CO value observed at ICO-OV, with the warm months appearing particularly affected by transport events of air-masses rich in anthropogenic pollution. The proportion of tracer variability that is described by FLEXPART COant peaked to 37% (in May–September) for CO, 19% (in May–September) for O3 and 32% (in January–April) for BC. During May–September, the analysis of the correlation among CO, O3 and BC as a function of the COant indicated that ICO-OV was influenced by air-masses rich in anthropogenic pollution transported from the regional to the global scale. On the other side, CO and O3 were negatively correlated during October–December, when FLEXPART does not show significant presence of recent anthropogenic emissions and only a few observations are characterized by enhanced BC. Such behaviour may be attributed to an ensemble of processes concurrent in enhancing O3 with low CO (upper troposphere/lower stratosphere intrusions) and O3 titration by NO in polluted air-masses along with lower photochemical activity. An intermediate situation occurs in January–April when CO and O3 were almost uncorrelated and BC enhancements were associated to relatively old (10 days) anthropogenic emissions.

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Flexpart v10.1 simulation of source contributions to Arctic black carbon

10.5194/acp-2019-590 ◽

2019 ◽

Author(s):

Chunmao Zhu ◽

Yugo Kanaya ◽

Masayuki Takigawa ◽

Kohei Ikeda ◽

Hiroshi Tanimoto ◽

...

Keyword(s):

Black Carbon ◽

Biomass Burning ◽

Anthropogenic Sources ◽

The Arctic ◽

Anthropogenic Emissions ◽

High Altitudes ◽

Arctic Environment ◽

Gas Flaring ◽

Rapid Changes ◽

Arctic Surface

Abstract. The Arctic environment is undergoing rapid changes such as faster warming than the global average and exceptional melting of glaciers in Greenland. Black carbon (BC) particles, which are a short-lived climate pollutant, are one cause of Arctic warming and glacier melting. However, the sources of BC particles are still uncertain. We simulated the potential emission sensitivity of atmospheric BC present over the Arctic (north of 66° N) using the Flexpart Lagrangian transport model (version 10.1). This version includes a new aerosol wet removal scheme, which better represents particle-scavenging processes than older versions did. Arctic BC at the surface (0–500 m) and high altitudes (4750–5250 m) is sensitive to emissions in high latitude (> 60° N) and mid-latitude (30–60° N) regions, respectively. Geospatial sources of Arctic BC were quantified, with a focus on emissions from anthropogenic activities and biomass burning in 2010. We found that anthropogenic sources contributed 82 % and 83 % of annual Arctic BC at the surface and high altitudes, respectively. Arctic surface BC comes predominantly from anthropogenic emissions in Russia (56 %), with gas flaring from the Yamalo-Nenets Autonomous Okrug and Komi Republic being the main source (31 % of Arctic surface BC). These results highlight the need for regulations to control BC emissions from gas flaring to mitigate the rapid changes in the Arctic environment. In summer, combined biomass burning in Siberia, Alaska, and Canada contributes 56–85 % (75 % on average) and 40–72 % (57 %) of Arctic BC at the surface and high altitudes, respectively. A large fraction (40 %) of BC in the Arctic at high altitudes comes from anthropogenic emissions in East Asia, which suggests that the rapidly growing economies of developing countries could have a non-negligible effect on the Arctic. To our knowledge, this is the first year-round evaluation of Arctic BC sources that has been performed using the new wet deposition scheme in Flexpart. The study provides a scientific basis for actions to mitigate the rapidly changing Arctic environment.

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Influence of biomass burning and anthropogenic emissions on ozone, carbon monoxide and black carbon at the Mt. Cimone GAW-WMO global station (Italy, 2165 m a.s.l.)

Atmospheric Chemistry and Physics ◽

10.5194/acp-13-15-2013 ◽

2013 ◽

Vol 13 (1) ◽

pp. 15-30 ◽

Cited By ~ 49

Author(s):

P. Cristofanelli ◽

F. Fierli ◽

A. Marinoni ◽

F. Calzolari ◽

R. Duchi ◽

...

Keyword(s):

Carbon Monoxide ◽

Black Carbon ◽

Biomass Burning ◽

Dispersion Model ◽

Anthropogenic Pollution ◽

Global Scale ◽

Local Source ◽

Anthropogenic Emissions ◽

Large Variability ◽

Air Masses

Abstract. This work investigates the variability of ozone (O3), carbon monoxide (CO) and equivalent black carbon (BC) at the Italian Climate Observatory "O. Vittori" (ICO-OV), part of the Mt. Cimone global GAW-WMO station (Italy). For this purpose, ICO-OV observations carried out in the period January 2007–June 2009, have been analyzed and correlated with the outputs of the FLEXPART Lagrangian dispersion model to specifically evaluate the influence of biomass burning (BB) and anthropogenic emissions younger than 20 days. During the investigation period, the average O3, CO and BC at ICO-OV were 54 ± 3 ppb, 122 ± 7 ppb and 213 ± 34 ng m−3 (mean ± expanded uncertainty with p < 95%), with clear seasonal cycles characterized by summer maxima and winter minima for O3 and BC and spring maximum and summer minimum for CO. According to FLEXPART outputs, BB impact is maximized during the warm months from July to September but appeared to have a significant contribution to the observed tracers only during specific transport events. We characterised in detail five "representative" events with respect to transport scales (i.e. global, regional and local), source regions and O3, CO and BC variations. For these events, very large variability of enhancement ratios O3/CO (from −0.22 to 0.71) and BC/CO (from 2.69 to 29.83 ng m−3 ppb−1) were observed. CO contributions related with anthropogenic emissions (COant) contributed to 17.4% of the mean CO value observed at ICO-OV, with the warm months appearing particularly affected by transport events of air-masses rich in anthropogenic pollution. The proportion of tracer variability that is described by FLEXPART COant peaked to 37% (in May–September) for CO, 19% (in May–September) for O3 and 32% (in January–April) for BC. During May–September, the analysis of the correlation among CO, O3 and BC as a function of the COant indicated that ICO-OV was influenced by air-masses rich in anthropogenic pollution transported from the regional to the global scale. On the other side, CO and O3 were negatively correlated during October–December, when FLEXPART does not show significant presence of recent anthropogenic emissions and only a few observations are characterized by enhanced BC. Such behaviour may be attributed to an ensemble of processes concurrent in enhancing O3 with low CO (upper troposphere/lower stratosphere intrusions) and to O3 titration by NO in polluted air-masses along with lower photochemical activity. An intermediate situation occurs in January–April when CO and O3 were almost uncorrelated and BC enhancements were associated to relatively old (10 days) anthropogenic emissions.

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Black carbon variability since preindustrial times in the eastern part of Europe reconstructed from Mt. Elbrus, Caucasus, ice cores

Atmospheric Chemistry and Physics ◽

10.5194/acp-17-3489-2017 ◽

2017 ◽

Vol 17 (5) ◽

pp. 3489-3505 ◽

Cited By ~ 17

Author(s):

Saehee Lim ◽

Xavier Faïn ◽

Patrick Ginot ◽

Vladimir Mikhalenko ◽

Stanislav Kutuzov ◽

...

Keyword(s):

Black Carbon ◽

20Th Century ◽

Biomass Burning ◽

Mass Concentration ◽

Ice Core ◽

Ice Cores ◽

Anthropogenic Emissions ◽

Geographical Regions ◽

Ice Core Record ◽

Mass Concentrations

Abstract. Black carbon (BC), emitted by fossil fuel combustion and biomass burning, is the second largest man-made contributor to global warming after carbon dioxide (Bond et al., 2013). However, limited information exists on its past emissions and atmospheric variability. In this study, we present the first high-resolution record of refractory BC (rBC, including mass concentration and size) reconstructed from ice cores drilled at a high-altitude eastern European site in Mt. Elbrus (ELB), Caucasus (5115 m a.s.l.). The ELB ice core record, covering the period 1825–2013, reflects the atmospheric load of rBC particles at the ELB site transported from the European continent with a larger rBC input from sources located in the eastern part of Europe. In the first half of the 20th century, European anthropogenic emissions resulted in a 1.5-fold increase in the ice core rBC mass concentrations with respect to its level in the preindustrial era (before 1850). The summer (winter) rBC mass concentrations increased 5-fold (3.3-fold) in 1960–1980, followed by a decrease until ∼  2000. Over the last decade, the rBC signal for summertime slightly increased. We have compared the signal with the atmospheric BC load simulated using past BC emissions (ACCMIP and MACCity inventories) and taken into account the contribution of different geographical regions to rBC distribution and deposition at the ELB site. Interestingly, the observed rBC variability in the ELB ice core record since the 1960s is not in perfect agreement with the simulated atmospheric BC load. Similar features between the ice core rBC record and the best scenarios for the atmospheric BC load support anthropogenic BC increase in the 20th century being reflected in the ELB ice core record. However, the peak in BC mass concentration observed in ∼  1970 in the ice core is estimated to occur a decade later from past inventories. BC emission inventories for the period 1960s–1970s may be underestimating European anthropogenic emissions. Furthermore, for summertime snow layers of the 2000s, the slightly increasing trend of rBC deposition likely reflects recent changes in anthropogenic and biomass burning BC emissions in the eastern part of Europe. Our study highlights that the past changes in BC emissions of eastern Europe need to be considered in assessing ongoing air quality regulation.

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Anthropogenic, biomass burning, and volcanic emissions of black carbon, organic carbon, and SO<sub>2</sub> from 1980 to 2010 for hindcast model experiments

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-12-24895-2012 ◽

2012 ◽

Vol 12 (9) ◽

pp. 24895-24954 ◽

Cited By ~ 158

Author(s):

T. Diehl ◽

A. Heil ◽

M. Chin ◽

X. Pan ◽

D. Streets ◽

...

Keyword(s):

Organic Carbon ◽

Black Carbon ◽

Biomass Burning ◽

Sharp Decrease ◽

Emission Factors ◽

Horizontal Resolution ◽

Anthropogenic Sources ◽

Anthropogenic Emissions ◽

Volcanic Emissions ◽

So2 Emissions

Abstract. Two historical emission inventories of black carbon (BC), primary organic carbon (OC), and SO2 emissions from land-based anthropogenic sources, ocean-going vessels, air traffic, biomass burning, and volcanoes are presented and discussed for the period 1980–2010. These gridded inventories are provided to the internationally coordinated AeroCom Phase II multi-model hindcast experiments. The horizontal resolution is 0.5°×0.5° and 1.0°×1.0°, while the temporal resolution varies from daily for volcanoes to monthly for biomass burning and aircraft emissions, and annual averages for land-based and ship emissions. One inventory is based on inter-annually varying activity rates of land-based anthropogenic emissions and shows strong variability within a decade, while the other one is derived from interpolation between decadal endpoints and thus exhibits linear trends within a decade. Both datasets capture the major trends of decreasing anthropogenic emissions over the USA and Western Europe since 1980, a sharp decrease around 1990 over Eastern Europe and the former USSR, and a steep increase after 2000 over East and South Asia. The inventory differences for the combined anthropogenic and biomass burning emissions in the year 2005 are 34% for BC, 46% for OC, and 13% for SO2. They vary strongly depending on species, year and region, from about 10% to 40% in most cases, but in some cases the inventories differ by 100% or more. Differences in emissions from wild-land fires are caused only by different choices of the emission factors for years after 1996 which vary by a factor of about 1 to 2 for OC depending on region, and by a combination of emission factors and the amount of dry mass burned for years up to 1996. Volcanic SO2 emissions, which are only provided in one inventory, include emissions from explosive, effusive, and quiescent degassing events for 1167 volcanoes.

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Source attribution of Arctic black carbon constrained by aircraft and surface measurements

10.5194/acp-2017-236 ◽

2017 ◽

Author(s):

Junwei Xu ◽

Randall V. Martin ◽

Andrew Morrow ◽

Sangeeta Sharma ◽

Lin Huang ◽

...

Keyword(s):

North America ◽

Black Carbon ◽

Biomass Burning ◽

Western Siberia ◽

The Arctic ◽

Anthropogenic Emissions ◽

Northern Asia ◽

Airborne Measurements ◽

Gas Flaring ◽

Southern Asia

Abstract. Black carbon (BC) contributes to both degraded air quality and Arctic warming, however sources of Arctic BC and their geographic contributions remain uncertain. We interpret a series of recent airborne and ground-based measurements with the GEOS-Chem global chemical transport model and its adjoint to attribute the sources of Arctic BC. The springtime airborne measurements performed by the NETCARE campaign in 2015 and the PAMARCMiP campaigns in 2009 and 2011 offer BC vertical profiles extending to > 6 km across the Arctic and include profiles above Arctic ground monitoring stations. Long-term ground-based measurements are examined from multiple methods (thermal, laser incandescence and light absorption) at Alert (2011–2013), Barrow (2009–2015) and Ny-Ålesund (2009–2014) stations. Our simulations with the addition of gas flaring emissions are consistent with ground-based measurements of BC concentrations at Alert and Barrow in winter and spring (rRMSE < 13 %), and with airborne measurements of BC vertical profile across the Arctic (rRMSE = 17 %). Sensitivity simulations suggest that anthropogenic emissions in eastern and southern Asia are the largest source of the Arctic BC column both in spring (56 %) and annually (37 %), with larger contributions aloft than near the surface (e.g. a contribution of 66 % between 400–700 hPa and of 46 % below 900 hPa in spring). Anthropogenic emissions from northern Asia contribute considerable BC to the lower troposphere (a contribution of 27 % in spring and of 43 % annually below 900 hPa). Biomass burning has a substantial contribution to Arctic BC below 400 hPa of 25 % annually, despite minor influence in spring ( 50 %) in winter and those from eastern and southern Asia are the largest in spring (~ 40 %). At Ny-Ålesund, anthropogenic emissions from Europe (~ 30 %) and northern Asia (~ 30 %) are major sources in winter and early spring. Biomass burning from North America is the most important contributor to surface BC at all stations in summer, especially at Barrow where North American biomass burning contributes more than 90 % of BC in July and August. Our adjoint simulations indicate pronounced spatial and seasonal heterogeneity in the contribution of emissions to the Arctic BC column concentrations with noteworthy contributions from emissions in eastern China (15 %) and western Siberia (6.5 %). Although uncertain, gas flaring emissions from oilfields in western Siberia could have a striking impact (13 %) on Arctic BC loadings in January, comparable to the total influence of continental Europe and North America (6.5 % each in January).

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