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Short-lived climate forcers have been proven important both for the climate and human health. In particular, black carbon (BC) is an important climate forcer both as an aerosol and when deposited on snow and ice surface because of its strong light absorption. This paper presents measurements of elemental carbon (EC; a measurement-based definition of BC) in snow collected from western Siberia and northwestern European Russia during 2014, 2015 and 2016. The Russian Arctic is of great interest to the scientific community due to the large uncertainty of emission sources there. We have determined the major contributing sources of BC in snow in western Siberia and northwestern European Russia using a Lagrangian atmospheric transport model. For the first time, we use a recently developed feature that calculates deposition in backward (so-called retroplume) simulations allowing estimation of the specific locations of sources that contribute to the deposited mass. EC concentrations in snow from western Siberia and northwestern European Russia were highly variable depending on the sampling location. Modelled BC and measured EC were moderately correlated (R = 0.53-0.83) and a systematic region-specific model underestimation was found. The model underestimated observations by 42% (RMSED49 ngg-1) in 2014, 48% (RMSE=37 ngg-1) in 2015 and 27%(RMSE=43 ngg-1) in 2016. For EC sampled in northwestern European Russia the underestimation by the model was smaller (fractional bias, FB>-100 %). In this region, the major sources were transportation activities and domestic combustion in Finland. When sampling shifted to western Siberia, the model underestimation was more significant (FB<-100 %). There, the sources included emissions from gas flaring as a major contributor to snow BC. The accuracy of the model calculations was also evaluated using two independent datasets of BC measurements in snow covering the entire Arctic. The model underestimated BC concentrations in snow especially for samples collected in springtime. [ABSTRACT FROM AUTHOR]

There are very few large-scale observations of the chemical composition of the Siberian airshed. The Airborne Extensive Regional Observations in Siberia (YAK-AEROSIB) French-Russian research program aims to fill this gap by collecting repeated aircraft high-precision measurements of the vertical distribution of CO2, CO, O3, and aerosol size distribution in the Siberian troposphere on a transect of 4,000 km during campaigns lasting approximately one week. This manuscript gives an overview of the results from five campaigns executed in April 2006, September 2006, August 2007, and early and late July 2008. The dense set of CO2 vertical profiles, consisting of some 50 profiles in each campaign, is shown to constrain large-scale models of CO2 synoptic transport, in particular frontal transport processes. The observed seasonal cycle of CO2 in altitude reduces uncertainty on the seasonal covariance between vegetation fluxes and vertical mixing, known as the 'seasonal rectifier effect.' Regarding carbon dioxide, we illustrate the potential of the YAK-AEROSIB data to cross-validate a global CO2 transport model. When compared to the CO2 data, the model is likely to be biased toward too-weak mixing in winter, as it overestimates the CO2 vertical gradient compared to the observation. Regarding pollutants, we illustrate through case studies the occurence of CO enhancements of 30-50 ppb above background values, coincident with high O3. These high CO values correspond to large-scale transport of anthropogenic emissions from Europe, and to wildfires in the Caspian Sea area, over much cleaner Arctic air (September 2006). An occurence of extremely high CO values above 5,000 km in eastern Siberia is found to be related to the very fast transport and uplift of Chinese anthropogenic emissions caused by a cold front (April 2006). [ABSTRACT FROM AUTHOR]

We analysed results of three intensive aircraft campaigns above Siberia (April and September 2006, August 2007) with a total of ∼70 h of continuous CO2, CO and O3 measurements. The flight route consists of consecutive ascents and descents between Novosibirsk (55° N, 82° E) and Yakutsk (62° N, 129° E). We performed retroplume calculations with the Lagrangian particle dispersion model FLEXPART for many short segments along the flight tracks. To reduce the extremely rich information on source regions provided by the model calculation into a small number of distinct cases, we performed a statistical clustering - to our knowledge for the first time - into potential source regions of the footprint emission sensitivities obtained from the model calculations. This technique not only worked well to separate source region influences but also resulted in clearly distinct tracer concentrations for the various clusters obtained. High CO and O3 concentrations were found associated with agricultural fire plumes originating from Kazakhstan in September 2006. A statistical analysis indicates that summer uptake of CO2 is largely explained (∼50% of variance) by air mass exposure to uptake by Siberian and sub-arctic ecosystems. This resulted in an average 5 to 10 ppm difference with overlaying air masses. Stratosphere-troposphere exchange is found to strongly influence the observed O3 mixing ratios in spring, but not in summer. European emissions contributed to high O3 concentrations above Siberia in April 2006 and August 2007, while emissions from North Eastern China also contributed to higher O3 mixing ratios in summer, but tend to lower mixing ratios in spring, when the airmass aerosol burden is important. In the lower troposphere, large-scale deposition processes in the boreal and sub-arctic boundary layer is a large O3 sink, resulting in a ∼20 ppb difference with overlaying air masses. Lagrangian footprint clustering is very promising and could also be advantageously applied to the interpretation of ground based measurements including calculation of tracers' sources and sinks. [ABSTRACT FROM AUTHOR]

We present airborne measurements of carbon dioxide (CO2), carbon monoxide (CO), ozone (O3), equivalent black carbon (EBC) and ultra fine particles over North- Eastern Siberia in July 2008 performed during the YAKAEROSIB/ POLARCAT experiment. During a "golden day" (11 July 2008) a number of biomass burning plumes were encountered with CO mixing ratio enhancements of up to 500 ppb relative to a background of 90 ppb. Number concentrations of aerosols in the size range 3.5-200 nm peaked at 4000 cm-3 and the EBC content reached 1.4 μgm-3. These high concentrations were caused by forest fires in the vicinity of the landing airport in Yakutsk where measurements in fresh smoke could be made during the descent. We estimate a combustion efficiency of 90±3% based on CO and CO2 measurements and a CO emission factor of 65.5±10.8 gCO per kilogram of dry matter burned. This suggests a potential increase in the average northern hemispheric CO mixing ratio of 3.0-7.2 ppb per million hectares of Siberian forest burned. For BC, we estimate an emission factor of 0.52±0.07 gBC kg-1, comparable to values reported in the literature. The emission ratio of ultra-fine particles (3.5-200 nm) was 26 cm-3 (ppb CO)-1, consistent with other airborne studies. The transport of identified biomass burning plumes was investigated using the FLEXPART Lagrangian model. Based on sampling of wildfire plumes from the same source but with different atmospheric ages derived from FLEXPART, we estimate that the e-folding lifetimes of EBC and ultra fine particles (between 3.5 and 200 nm in size) against removal and growth processes are 5.1 and 5.5 days respectively, supporting lifetime estimates used in various modelling studies. [ABSTRACT FROM AUTHOR]

Two airborne campaigns were carried out to measure the tropospheric concentrations and variability of CO2, CO and O3 over Siberia. In order to quantify the influence of remote and regional natural and anthropogenic sources, we analysed a total of 52 vertical profiles of these species collected in April and September 2006, every ∼200 km and up to 7 km altitude. CO2 and CO concentrations were high in April 2006 (respectively 385–390 ppm CO2 and 160–200 ppb CO) compared to background values. CO concentrations up to 220 ppb were recorded above 3.5 km over eastern Siberia, with enhancements in 500–1000 m thick layers. The presence of CO enriched air masses resulted from a quick frontal uplift of a polluted air mass exposed to northern China anthropogenic emissions and to fire emissions in northern Mongolia. A dominant Asian origin for CO above 4 km (71.0%) contrasted with a dominant European origin below this altitude (70.9%) was deduced both from a transport model analysis, and from the contrasted ΔCO/ΔCO2 ratio vertical distribution. In September 2006, a significant O3 depletion (∼–30 ppb) was repeatedly observed in the boundary layer, as diagnosed from virtual potential temperature profiles and CO2 gradients, compared to the free troposphere aloft, suggestive of a strong O3 deposition over Siberian forests. [ABSTRACT FROM AUTHOR]

Understanding the role of short-lived climate forcers such as black carbon (BC) at high northern latitudes in climate change is hampered by the scarcity of surface observations in the Russian Arctic. In this study, highly time-resolved Equivalent BC (EBC) measurements during a ship campaign in the White, Barents, and Kara Seas in October 2015 are presented. The measured EBC concentrations are compared with BC concentrations simulated with a Lagrangian particle dispersion model coupled with a recently completed global emission inventory to quantify the origin of the Arctic BC. EBC showed increased values (100-400 ng m-3) in the Kara Strait, Kara Sea, and Kola Peninsula and an extremely high concentration (1000 ng m-3) in the White Sea. Assessment of BC origin throughout the expedition showed that gas-flaring emissions from the Yamal-Khanty-Mansiysk and Nenets-Komi regions contributed the most when the ship was close to the Kara Strait, north of 70° N. Near Arkhangelsk (White Sea), biomass burning in mid-latitudes, surface transportation, and residential and commercial combustion from Central and Eastern Europe were found to be important BC sources. The model reproduced observed EBC concentrations efficiently, building credibility in the emission inventory for BC emissions at high northern latitudes. [ABSTRACT FROM AUTHOR]

Black carbon (BC) particles contribute to climate warming by heating the atmosphere and reducing the albedo of snow/ice surfaces. The available Arctic BC deposition records are restricted to the Atlantic and North American sectors, for which previous studies suggest considerable spatial differences in trends. Here, we present first long-term BC deposition and radiocarbon-based source apportionment data from Russia using four lake sediment records from western Arctic Russia, a region influenced by BC emissions from oil and gas production. The records consistently indicate increasing BC fluxes between 1800 and 2014. The radiocarbon analyses suggest mainly (∼70%) biomass sources for BC with fossil fuel contributions peaking around 1960-1990. Backward calculations with the atmospheric transport model FLEXPART show emission source areas and indicate that modeled BC deposition between 1900 and 1999 is largely driven by emission trends. Comparison of observed and modeled data suggests the need to update anthropogenic BC emission inventories for Russia, as these seem to underestimate Russian BC emissions and since 1980s potentially inaccurately portray their trend. Additionally, the observations may indicate underestimation of wildfire emissions in inventories. Reliable information on BC deposition trends and sources is essential for design of efficient and effective policies to limit climate warming.