scholarly journals Effects of mixing state on optical and radiative properties of black carbon in the European Arctic

Author(s):  
Marco Zanatta ◽  
Paolo Laj ◽  
Martin Gysel ◽  
Urs Baltensperger ◽  
Stergios Vratolis ◽  
...  

Abstract. Atmospheric aging promotes internal mixing of black carbon (BC) leading to an enhancement of light absorption and radiative forcing. The relationship between BC mixing state and consequent absorption enhancement was never estimated for BC found in the Arctic region. In the present work, we aim to quantify the absorption enhancement and its impact on radiative forcing as a function of microphysical properties and mixing state of BC observed in-situ at the Zeppelin Arctic station (78° N) in the spring of 2012 during the CLIMSLIP (Climate impacts of short-lived pollutants in the Arctic) project. Single particle soot photometer (SP2) measurements showed a mean mass concentration of refractory black carbon (rBC) of 39 ng m−3, while the rBC mass size distribution was of log-normal shape peaking at an rBC mass equivalent diameter (DrBC) of around 240 nm. On average, the number fraction of particles containing a BC core with DrBC > 80 nm was less than 5 % in the size range (overall optical particle diameter) from 150–500 nm. The BC cores were internally mixed with other particulate matter. The median coating thickness of BC cores with 220 nm 

2018 ◽  
Vol 18 (19) ◽  
pp. 14037-14057 ◽  
Author(s):  
Marco Zanatta ◽  
Paolo Laj ◽  
Martin Gysel ◽  
Urs Baltensperger ◽  
Stergios Vratolis ◽  
...  

Abstract. Atmospheric aging promotes internal mixing of black carbon (BC), leading to an enhancement of light absorption and radiative forcing. The relationship between BC mixing state and consequent absorption enhancement was never estimated for BC found in the Arctic region. In the present work, we aim to quantify the absorption enhancement and its impact on radiative forcing as a function of microphysical properties and mixing state of BC observed in situ at the Zeppelin Arctic station (78∘ N) in the spring of 2012 during the CLIMSLIP (Climate impacts of short-lived pollutants in the polar region) project. Single-particle soot photometer (SP2) measurements showed a mean mass concentration of refractory black carbon (rBC) of 39 ng m−3, while the rBC mass size distribution was of lognormal shape, peaking at an rBC mass-equivalent diameter (DrBC) of around 240 nm. On average, the number fraction of particles containing a BC core with DrBC>80 nm was less than 5 % in the size range (overall optical particle diameter) from 150 to 500 nm. The BC cores were internally mixed with other particulate matter. The median coating thickness of BC cores with 220 nm < DrBC< 260 nm was 52 nm, resulting in a core–shell diameter ratio of 1.4, assuming a coated sphere morphology. Combining the aerosol absorption coefficient observed with an Aethalometer and the rBC mass concentration from the SP2, a mass absorption cross section (MAC) of 9.8 m2 g−1 was inferred at a wavelength of 550 nm. Consistent with direct observation, a similar MAC value (8.4 m2 g−1 at 550 nm) was obtained indirectly by using Mie theory and assuming a coated-sphere morphology with the BC mixing state constrained from the SP2 measurements. According to these calculations, the lensing effect is estimated to cause a 54 % enhancement of the MAC compared to that of bare BC particles with equal BC core size distribution. Finally, the ARTDECO radiative transfer model was used to estimate the sensitivity of the radiative balance to changes in light absorption by BC as a result of a varying degree of internal mixing at constant total BC mass. The clear-sky noontime aerosol radiative forcing over a surface with an assumed wavelength-dependent albedo of 0.76–0.89 decreased, when ignoring the absorption enhancement, by −0.12 W m−2 compared to the base case scenario, which was constrained with mean observed aerosol properties for the Zeppelin site in Arctic spring. The exact magnitude of this forcing difference scales with environmental conditions such as the aerosol optical depth, solar zenith angle and surface albedo. Nevertheless, our investigation suggests that the absorption enhancement due to internal mixing of BC, which is a systematic effect, should be considered for quantifying the aerosol radiative forcing in the Arctic region.


2015 ◽  
Vol 15 (17) ◽  
pp. 10057-10070 ◽  
Author(s):  
T. Raatikainen ◽  
D. Brus ◽  
A.-P. Hyvärinen ◽  
J. Svensson ◽  
E. Asmi ◽  
...  

Abstract. Atmospheric aerosol composition was measured using a Single Particle Soot Photometer (SP2) in the Finnish Arctic during winter 2011–2012. The Sammaltunturi measurement site at the Pallas GAW (Global Atmosphere Watch) station receives air masses from different source regions including the Arctic Ocean and continental Europe. The SP2 provides detailed information about mass distributions and mixing state of refractory black carbon (rBC). The measurements showed widely varying rBC mass concentrations (0–120 ng m−3), which were related to varying contributions of different source regions and aerosol removal processes. The rBC mass was log-normally distributed showing a relatively constant rBC core mass mean diameter with an average of 194 nm (75–655 nm sizing range). On average, the number fraction of particles containing rBC was 0.24 (integrated over 350–450 nm particle diameter range) and the average particle diameter to rBC core volume equivalent diameter ratio was 2.0 (averaged over particles with 150–200 nm rBC core volume equivalent diameters). These average numbers mean that the observed rBC core mass mean diameter is similar to those of aged particles, but the observed particles seem to have unusually high particle to rBC core diameter ratios. Comparison of the measured rBC mass concentration with that of the optically detected equivalent black carbon (eBC) using an Aethalometer and a MAAP showed that eBC was larger by a factor of five. The difference could not be fully explained without assuming that only a part of the optically detected light absorbing material is refractory and absorbs light at the wavelength used by the SP2. Finally, climate implications of five different black carbon mixing state representations were compared using the Mie approximation and simple direct radiative forcing efficiency calculations. These calculations showed that the observed mixing state means significantly lower warming effect or even a net cooling effect when compared with that of a homogenous aerosol containing the same amounts of black carbon and non-absorbing material.


2018 ◽  
Vol 10 (10) ◽  
pp. 1634 ◽  
Author(s):  
Li Liu ◽  
Michael Mishchenko

This paper provides a thorough modeling-based overview of the scattering and radiative properties of a wide variety of morphologically complex carbonaceous aerosols. Using the numerically-exact superposition T-matrix method, we examine the absorption enhancement, absorption Ångström exponent (AAE), backscattering linear depolarization ratio (LDR), and scattering matrix elements of black-carbon aerosols with 11 different model morphologies ranging from bare soot to completely embedded soot–sulfate and soot–brown carbon mixtures. Our size-averaged results show that fluffy soot particles absorb more light than compact bare-soot clusters. For the same amount of absorbing material, the absorption cross section of internally mixed soot can be more than twice that of bare soot. Absorption increases as soot accumulates more coating material and can become saturated. The absorption enhancement is affected by particle size, morphology, wavelength, and the amount of coating. We refute the conventional belief that all carbonaceous aerosols have AAEs close to 1.0. Although LDRs caused by bare soot and certain carbonaceous particles are rather weak, LDRs generated by other soot-containing aerosols can reproduce strong depolarization measured by Burton et al. for aged smoke. We demonstrate that multi-wavelength LDR measurements can be used to identify the presence of morphologically complex carbonaceous particles, although additional observations can be needed for full characterization. Our results show that optical constants of the host/coating material can significantly influence the scattering and absorption properties of soot-containing aerosols to the extent of changing the sign of linear polarization. We conclude that for an accurate estimate of black-carbon radiative forcing, one must take into account the complex morphologies of carbonaceous aerosols in remote sensing studies as well as in atmospheric radiation computations.


Atmosphere ◽  
2021 ◽  
Vol 12 (7) ◽  
pp. 814
Author(s):  
Sergey Kostrykin ◽  
Anastasia Revokatova ◽  
Alexey Chernenkov ◽  
Veronika Ginzburg ◽  
Polina Polumieva ◽  
...  

The work is devoted to the study of the climatic effects of black carbon (BC) transferred from forest fires to the Arctic zone. The HYSPLIT (The Hybrid Single-Particle Lagrangian Integrated Trajectory model) trajectory model was used to initially assess the potential for particle transport from fires. The results of the trajectory analysis of the 2019 fires showed that the probability of the transfer of particles to the Arctic ranges from 1% to 10%, and in some cases increases to 20%. Detailed studies of the possible influence of BC ejected as a result of fires became possible by using the climate model of the INMCM5 (Institute of Numerical Mathematics Climate Model). The results of the numerical experiments have shown that the maximum concentration of BC in the Arctic atmosphere is observed in July and August and is associated with emissions from fires. The deposition of BC in the Arctic increases by about 1.5–2 times in the same months, in comparison with simulation without forest fire emissions. This caused an average decrease in solar radiation forcing of 0.3–0.4 Wt/m2 and an increase in atmospheric radiation heating of up to 5–6 Wt/m2. To assess the radiation forcing from BC contaminated snow, we used the dependences of the change in the snow albedo on the snow depth, and the albedo of the underlying surface for a given amount of BC fallen on the snow. These dependences were constructed on the basis of the SNICAR (Snow, Ice, and Aerosol Radiative) model. According to our calculations, the direct radiative forcing from BC in the atmosphere with a clear sky is a maximum of 4–5 W/m2 in July and August.


2018 ◽  
Vol 18 (15) ◽  
pp. 11345-11361 ◽  
Author(s):  
John K. Kodros ◽  
Sarah J. Hanna ◽  
Allan K. Bertram ◽  
W. Richard Leaitch ◽  
Hannes Schulz ◽  
...  

Abstract. Transport of anthropogenic aerosol into the Arctic in the spring months has the potential to affect regional climate; however, modeling estimates of the aerosol direct radiative effect (DRE) are sensitive to uncertainties in the mixing state of black carbon (BC). A common approach in previous modeling studies is to assume an entirely external mixture (all primarily scattering species are in separate particles from BC) or internal mixture (all primarily scattering species are mixed in the same particles as BC). To provide constraints on the size-resolved mixing state of BC, we use airborne single-particle soot photometer (SP2) and ultrahigh-sensitivity aerosol spectrometer (UHSAS) measurements from the Alfred Wegener Institute (AWI) Polar 6 flights from the NETCARE/PAMARCMIP2015 campaign to estimate coating thickness as a function of refractory BC (rBC) core diameter and the fraction of particles containing rBC in the springtime Canadian high Arctic. For rBC core diameters in the range of 140 to 220 nm, we find average coating thicknesses of approximately 45 to 40 nm, respectively, resulting in ratios of total particle diameter to rBC core diameters ranging from 1.6 to 1.4. For total particle diameters ranging from 175 to 730 nm, rBC-containing particle number fractions range from 16 % to 3 %, respectively. We combine the observed mixing-state constraints with simulated size-resolved aerosol mass and number distributions from GEOS-Chem–TOMAS to estimate the DRE with observed bounds on mixing state as opposed to assuming an entirely external or internal mixture. We find that the pan-Arctic average springtime DRE ranges from −1.65 to −1.34 W m−2 when assuming entirely externally or internally mixed BC. This range in DRE is reduced by over a factor of 2 (−1.59 to −1.45 W m−2) when using the observed mixing-state constraints. The difference in DRE between the two observed mixing-state constraints is due to an underestimation of BC mass fraction in the springtime Arctic in GEOS-Chem–TOMAS compared to Polar 6 observations. Measurements of mixing state provide important constraints for model estimates of DRE.


2013 ◽  
Vol 13 (4) ◽  
pp. 1941-1955 ◽  
Author(s):  
S. B. Dalsøren ◽  
B. H. Samset ◽  
G. Myhre ◽  
J. J. Corbett ◽  
R. Minjares ◽  
...  

Abstract. We quantify the concentrations changes and Radiative Forcing (RF) of short-lived atmospheric pollutants due to shipping emissions of NOx, SOx, CO, NMVOCs, BC and OC. We use high resolution ship emission inventories for the Arctic that are more suitable for regional scale evaluation than those used in former studies. A chemical transport model and a RF model are used to evaluate the time period 2004–2030, when we expect increasing traffic in the Arctic region. Two datasets for ship emissions are used that characterize the potential impact from shipping and the degree to which shipping controls may mitigate impacts: a high (HIGH) scenario and a low scenario with Maximum Feasible Reduction (MFR) of black carbon in the Arctic. In MFR, BC emissions in the Arctic are reduced with 70% representing a combination technology performance and/or reasonable advances in single-technology performance. Both scenarios result in moderate to substantial increases in concentrations of pollutants both globally and in the Arctic. Exceptions are black carbon in the MFR scenario, and sulfur species and organic carbon in both scenarios due to the future phase-in of current regulation that reduces fuel sulfur content. In the season with potential transit traffic through the Arctic in 2030 we find increased concentrations of all pollutants in large parts of the Arctic. Net global RFs from 2004–2030 of 53 mW m−2 (HIGH) and 73 mW m−2 (MFR) are similar to those found for preindustrial to present net global aircraft RF. The found warming contrasts with the cooling from historical ship emissions. The reason for this difference and the higher global forcing for the MFR scenario is mainly the reduced future fuel sulfur content resulting in less cooling from sulfate aerosols. The Arctic RF is largest in the HIGH scenario. In the HIGH scenario ozone dominates the RF during the transit season (August–October). RF due to BC in air, and snow and ice becomes significant during Arctic spring. For the HIGH scenario the net Arctic RF during spring is 5 times higher than in winter.


2018 ◽  
Author(s):  
Hannes Schulz ◽  
Heiko Bozem ◽  
Marco Zanatta ◽  
W. Richard Leaitch ◽  
Andreas B. Herber ◽  
...  

Abstract. The vertical distribution of black carbon (BC) particles in the Arctic atmosphere is one of the key parameters controlling its radiative forcing. Hence, this work investigates the presence and properties of BC over the high Canadian Arctic. Airborne campaigns were performed as part of the NETCARE project and provided insights into the variability of the vertical distributions of BC particles in summer 2014 and spring 2015. The observation periods covered evolutions of cyclonic disturbances to the polar dome that caused and changed transport of air pollution into the High–Arctic, as otherwise the airmass boundary largely impedes entrainment of pollution from lower latitudes. A total of 48 vertical profiles of refractory BC (rBC) mass concentration and particle size, extending from 0.1 to 5.5 km altitude, were obtained with a Single–Particle Soot Photometer (SP2). Generally, the rBC mass concentration decreased from spring to summer by a factor 10. Such depletion was associated with a decrease of the mean rBC particle diameter, from approximately 200 nm to 130 nm at low altitude. Due to the very low number fraction, rBC particles did not substantially contribute to the total aerosol population in summer. Profiles analysed with potential temperature as vertical coordinate revealed characteristic variability patterns due to different balances of supply and removal of rBC in specific levels of the stable atmosphere. Kinematic back–trajectories were used to investigate transport pathways into these levels. The lower polar dome was influenced by low–level transport from sources within the cold central and marginal Arctic. During the spring campaign, a cold air outbreak over eastern Europe additionally caused northward transport of air from a corridor over western Russia to Central Asia that was affected by emissions from gas flaring, industrial activity and wildfires. This caused rBC concentrations between about 500 to 1800 m altitude to gradually increase from 32 to 49 ng m−3. The temporal development of transport to the level above, at around 2500 m, caused the initially low concentration to increase from


2019 ◽  
Vol 19 (4) ◽  
pp. 2361-2384 ◽  
Author(s):  
Hannes Schulz ◽  
Marco Zanatta ◽  
Heiko Bozem ◽  
W. Richard Leaitch ◽  
Andreas B. Herber ◽  
...  

Abstract. The vertical distribution of black carbon (BC) particles in the Arctic atmosphere is one of the key parameters controlling their radiative forcing and thus role in Arctic climate change. This work investigates the presence and properties of these light-absorbing aerosols over the High Canadian Arctic (>70∘ N). Airborne campaigns were performed as part of the NETCARE project (Network on Climate and Aerosols: Addressing Key Uncertainties in Remote Canadian Environments) and provided insights into the variability of the vertical distributions of BC particles in summer 2014 and spring 2015. The observation periods covered evolutions of cyclonic disturbances at the polar front, which favoured the transport of air pollution into the High Canadian Arctic, as otherwise this boundary between the air masses largely impedes entrainment of pollution from lower latitudes. A total of 48 vertical profiles of refractory BC (rBC) mass concentration and particle size, extending from 0.1 to 5.5 km altitude were obtained with a Single-Particle Soot Photometer (SP2). Generally, the rBC mass concentration decreased from spring to summer by a factor of 10. Such depletion was associated with a decrease in the mean rBC particle diameter, from approximately 200 to 130 nm at low altitude. Due to the very low number fraction, rBC particles did not substantially contribute to the total aerosol population in summer. The analysis of profiles with potential temperature as vertical coordinate revealed characteristic variability patterns within specific levels of the cold and stably stratified, dome-like, atmosphere over the polar region. The associated history of transport trajectories into each of these levels showed that the variability was induced by changing rates and efficiencies of rBC import. Generally, the source areas affecting the polar dome extended southward with increasing potential temperature (i.e. altitude) level in the dome. While the lower dome was mostly only influenced by low-level transport from sources within the cold central and marginal Arctic, for the mid-dome and upper dome during spring it was found that a cold air outbreak over eastern Europe caused intensified northward transport of air from a corridor over western Russia to central Asia. This sector was affected by emissions from gas flaring, industrial activity and wildfires. The development of transport caused rBC concentrations in the second lowest level to gradually increase from 32 to 49 ng m−3. In the third level this caused the initially low rBC concentration to increase from <15 to 150 ng m−3. A shift in rBC mass-mean diameter, from above 200 nm in the lower polar dome dominated by low-level transport to <190 nm at higher levels, may indicate that rBC was affected by wet removal mechanisms preferential to larger particle diameters when lifting processes were involved during transport. The summer polar dome had limited exchange with the mid-latitudes. Air pollution was supplied from sources within the marginal Arctic as well as by long-range transport, but in both cases rBC was largely depleted in absolute and relative concentrations. Near the surface, rBC concentrations were <2 ng m−3, while concentrations increased to <10 ng m−3 towards the upper boundary of the polar dome. The mass mean particle diameter of 132 nm was smaller than in spring; nonetheless the summer mean mass size distribution resembled the spring distribution from higher levels, with depletion of particles >300 nm. Our work provides vertical, spatial and seasonal information of rBC characteristics in the polar dome over the High Canadian Arctic, offering a more extensive dataset for evaluation of chemical transport models and for radiative forcing assessments than those obtained before by other Arctic aircraft campaigns.


2012 ◽  
Vol 12 (10) ◽  
pp. 26647-26684 ◽  
Author(s):  
S. B. Dalsøren ◽  
B. H. Samset ◽  
G. Myhre ◽  
J. J. Corbett ◽  
R. Minjares ◽  
...  

Abstract. We quantify the concentrations change of atmospheric pollutants and Radiative Forcing (RF) of short-lived components due to shipping emissions of NOx, SOx, CO, NMVOCs, BC and OC. A set of models is used to evaluate the period 2004–2030. This time period reflects expected increasing traffic in the Arctic region. Two datasets for ship emissions are used that may characterize the potential impact from shipping and the degree to which shipping controls may mitigate impacts: A high (HIGH) scenario and a low scenario with Maximum Feasible Reduction (MFR) of black carbon in the Arctic. In MFR, BC emissions in the Arctic are reduced with 70% representing a combination technology performance and/or reasonable advances in single-technology performance. Both scenarios result in moderate to substantial increases in concentrations of pollutants both globally and in the Arctic. Exceptions are black carbon in the MFR scenario, and sulfur species and organic carbon in both scenarios due to the future phase-in of current regulation that reduces fuel sulfur content. In the season with potential transit traffic through the Arctic in 2030 significant increases occur for all pollutants in large parts of the Arctic. Net global RFs from 2004–2030 of 53 mW m−2 (HIGH) and 73 mW m−2 (MFR) are similar to those found for preindustrial to present net global aircraft RF. The found warming contrasts the cooling from historical ship emissions. The reason for this difference and the higher global forcing for the MFR scenario is mainly the reduced future fuel sulfur content resulting in less cooling from sulfate aerosols. Arctic regional forcing is largest in the HIGH scenario because other components become locally more important in polar latitudes. In the HIGH scenario ozone dominates the RF during Arctic summer and the transit season. RF due to BC in air, and snow and ice becomes of significance in Arctic spring. For the HIGH scenario the net Arctic RF during spring is 5 times higher than in winter.


2017 ◽  
Vol 17 (9) ◽  
pp. 6003-6022 ◽  
Author(s):  
Marianne T. Lund ◽  
Terje K. Berntsen ◽  
Bjørn H. Samset

Abstract. Accurate representation of black carbon (BC) concentrations in climate models is a key prerequisite for understanding its net climate impact. BC aging and scavenging are treated very differently in current models. Here, we examine the sensitivity of three-dimensional (3-D), temporally resolved BC concentrations to perturbations to individual model processes in the chemistry transport model OsloCTM2–M7. The main goals are to identify processes related to aerosol aging and scavenging where additional observational constraints may most effectively improve model performance, in particular for BC vertical profiles, and to give an indication of how model uncertainties in the BC life cycle propagate into uncertainties in climate impacts. Coupling OsloCTM2 with the microphysical aerosol module M7 allows us to investigate aging processes in more detail than possible with a simpler bulk parameterization. Here we include, for the first time in this model, a treatment of condensation of nitric acid on BC. Using kernels, we also estimate the range of radiative forcing and global surface temperature responses that may result from perturbations to key tunable parameters in the model. We find that BC concentrations in OsloCTM2–M7 are particularly sensitive to convective scavenging and the inclusion of condensation by nitric acid. The largest changes are found at higher altitudes around the Equator and at low altitudes over the Arctic. Convective scavenging of hydrophobic BC, and the amount of sulfate required for BC aging, are found to be key parameters, potentially reducing bias against HIAPER Pole-to-Pole Observations (HIPPO) flight-based measurements by 60 to 90  %. Even for extensive tuning, however, the total impact on global-mean surface temperature is estimated to less than 0.04 K. Similar results are found when nitric acid is allowed to condense on the BC aerosols. We conclude, in line with previous studies, that a shorter atmospheric BC lifetime broadly improves the comparison with measurements over the Pacific. However, we also find that the model–measurement discrepancies can not be uniquely attributed to uncertainties in a single process or parameter. Model development therefore needs to be focused on improvements to individual processes, supported by a broad range of observational and experimental data, rather than tuning of individual, effective parameters such as the global BC lifetime.


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