scholarly journals Importance of Supersaturation in Arctic Black Carbon Simulations

2021 ◽  
pp. 1-42
Author(s):  
Hitoshi Matsui ◽  
Mingxu Liu
Keyword(s):  
Black Carbon ◽  
Threshold Value ◽  
Climatic Conditions ◽  
The Arctic ◽  
Accurate Estimation ◽  
Cloud Droplets ◽  
Near Surface ◽  
Model Simulations ◽  
Microphysical Processes ◽  
Wet Removal

AbstractBlack carbon (BC) aerosol particles in the Arctic heat the atmosphere and snow/ice surfaces and may strengthen the snow-albedo feedback that amplifies Arctic warming. Model simulations of BC concentrations in the Arctic depend strongly on the representation of microphysical processes such as aging, activation, and wet removal. Most BC modeling studies have classified BC particles into hydrophobic BC, which cannot form cloud droplets, and hydrophilic BC, which can form cloud droplets, by assuming a globally constant critical supersaturation threshold value (Sthre), without considering its consistency with cloud maximum supersaturation (Smax). Here we show that it is essential to consider the consistency of Sthre with Smax in global model simulations to reduce uncertainties in near-surface ambient BC concentrations in the Arctic. Previous studies often obtained good agreement between simulated and observed near-surface Arctic BC mass concentrations when a low Sthre (~0.1%) was assumed in their models. However, this Sthre may be too low (activation and wet removal of BC may be underestimated) for the Arctic, because some recent observations and our model simulations suggest that Smax may actually be higher (~0.3%) there. We also demonstrate that spatially varying Sthre values and their consistency with Smax, which previous studies did not consider, must be represented in models for more accurate estimation of BC budget in the Arctic. Because both Smax and BC-aging speed depend on climatic conditions, our findings are an important step toward better simulations of BC impacts on past, present, and future Arctic climates.

scholarly journals Influence of cloud microphysical processes on black carbon wet removal, global distributions, and radiative forcing

2019 ◽  
Vol 19 (3) ◽  
pp. 1587-1603 ◽  
Author(s):  
Jiayu Xu ◽  
Jiachen Zhang ◽  
Junfeng Liu ◽  
Kan Yi ◽  
Songlin Xiang ◽  
...  
Keyword(s):  
Black Carbon ◽  
Wet Deposition ◽  
Radiative Forcing ◽  
Cloud Water ◽  
Ice Nucleation ◽  
The Arctic ◽  
Cloud Microphysical Processes ◽  
Vertical Distributions ◽  
Microphysical Processes ◽  
Wet Removal

Abstract. Parameterizations that impact wet removal of black carbon (BC) remain uncertain in global climate models. In this study, we enhance the default wet deposition scheme for BC in the Community Earth System Model (CESM) to (a) add relevant physical processes that were not resolved in the default model and (b) facilitate understanding of the relative importance of various cloud processes on BC distributions. We find that the enhanced scheme greatly improves model performance against HIPPO observations relative to the default scheme. We find that convection scavenging, aerosol activation, ice nucleation, evaporation of rain or snow, and below-cloud scavenging dominate wet deposition of BC. BC conversion rates for processes related to in-cloud water–ice conversion (i.e., riming, the Bergeron process, and evaporation of cloud water sedimentation) are relatively smaller, but have large seasonal variations. We also conduct sensitivity simulations that turn off each cloud process one at a time to quantify the influence of cloud processes on BC distributions and radiative forcing. Convective scavenging is found to have the largest impact on BC concentrations at mid-altitudes over the tropics and even globally. In addition, BC is sensitive to all cloud processes over the Northern Hemisphere at high latitudes. As for BC vertical distributions, convective scavenging greatly influences BC fractions at different altitudes. Suppressing BC droplet activation in clouds mainly decreases the fraction of column BC below 5 km, whereas suppressing BC ice nucleation increases that above 10 km. During wintertime, the Bergeron process also significantly increases BC concentrations at lower altitudes over the Arctic. Our simulation yields a global BC burden of 85 Gg; corresponding direct radiative forcing (DRF) of BC estimated using the Parallel Offline Radiative Transfer (PORT) is 0.13 W m−2, much lower than previous studies. The range of DRF derived from sensitivity simulations is large, 0.09–0.33 W m−2, corresponding to BC burdens varying from 73 to 151 Gg. Due to differences in BC vertical distributions among each sensitivity simulation, fractional changes in DRF (relative to the baseline simulation) are always higher than fractional changes in BC burdens; this occurs because relocating BC in the vertical influences the radiative forcing per BC mass. Our results highlight the influences of cloud microphysical processes on BC concentrations and radiative forcing.

scholarly journals A trajectory analysis of atmospheric transport of black carbon aerosols to Canadian High Arctic in winter and spring (1990–2005)

2010 ◽  
Vol 10 (2) ◽  
pp. 2221-2244 ◽  
Author(s):  
L. Huang ◽  
S. L. Gong ◽  
S. Sharma ◽  
D. Lavoué ◽  
C. Q. Jia
Keyword(s):  
Regression Model ◽  
Black Carbon ◽  
North American ◽  
Emission Intensity ◽  
Atmospheric Transport ◽  
High Arctic ◽  
The Arctic ◽  
Canadian High Arctic ◽  
Near Surface ◽  
Annual Variations

Abstract. Black carbon (BC) particles accumulated in the Arctic troposphere and deposited over snow have significant effects on radiative forcing of the Arctic regional climate. Applying cluster analysis technique on 10-day backward trajectories, transport pathways affecting Alert (82.5° N, 62.5° W), Nunavut in Canada are identified in this work, along with the associated transport frequency. Based on the atmospheric transport frequency and the estimated BC emission intensity from surrounding regions, a linear regression model is constructed to investigate the inter-annual variations of BC observed at Alert in January and April, representative of winter and spring respectively, between 1990 and 2005. Strong correlations are found between BC concentrations predicted with the regression model and measured at Alert for both seasons (R2 equals 0.77 and 0.81 for winter and spring, respectively). Results imply that atmospheric transport and BC emission are the major contributors to the inter-annual variations in BC concentrations observed at Alert in the cold seasons for the 16-year period. Based on the regression model the relative contributions of regional BC emissions affecting Alert are attributed to the Eurasian sector, composed of the European Union and the former USSR, and the North American sector. Considering both seasons, the model suggests that Eurasia is the major contributor to the near-surface BC levels at the Canadian High Arctic site with an average contribution of over 85% during the 16-year period. In winter, the atmospheric transport of BC aerosols from Eurasia is found to be even more predominant with a multi-year average of 94%. The model estimates smaller contribution from the Eurasian sector in spring (70%) than that in winter. It is also found that the change in Eurasian contributions depends mainly on the reduction of emission intensity, while the changes in both emission and atmospheric transport contributed to the inter-annual variation of North American contributions.

scholarly journals Arctic black carbon during PAMARCMiP 2018 and previous aircraft experiments in spring

2021 ◽  
Author(s):  
Sho Ohata ◽  
Makoto Koike ◽  
Atsushi Yoshida ◽  
Nobuhiro Moteki ◽  
Kouji Adachi ◽  
...  
Keyword(s):  
Numerical Model ◽  
Black Carbon ◽  
Biomass Burning ◽  
Base Station ◽  
Anthropogenic Sources ◽  
The Arctic ◽  
Core Diameter ◽  
Model Simulations ◽  
Anthropogenic Contributions ◽  
Mass Concentrations

Abstract. Vertical profiles of the mass concentration of black carbon (BC) were measured at altitudes up to 5 km during the PAMARCMiP aircraft-based field experiment conducted around the Northern Greenland Sea (Fram Strait) during March and April 2018, with operation base Station Nord (81.6° N, 16.7° W). Median BC mass concentrations in individual altitude ranges were 7–18 ng m–3 at standard temperature and pressure at altitudes below 4.5 km. These concentrations were systematically lower than previous observations in the Arctic in spring conducted by ARCTAS-A in 2008 and NETCARE in 2015 and similar to those observed during HIPPO3 in 2010. Column amounts of BC for altitudes below 5 km in the Arctic (> 66.5° N, COLBC), observed during the ARCTAS-A and NETCARE experiments were higher by factors of 4.2 and 2.7, respectively, than those of the PAMARCMiP experiment. These differences could not be explained solely by the different locations of the experiments. The year-to-year variation of COLBC values generally corresponded to that of biomass burning activities in northern high latitudes over western and eastern Eurasia. Furthermore, numerical model simulations estimated the year-to-year variation of contributions from anthropogenic sources to be smaller than 30–40 %. These results suggest that the year-to-year variation of biomass burning activities likely affected BC amounts in the Arctic troposphere in spring, at least in the years examined in this study. The year-to-year variations in BC mass concentrations were also observed at the surface at high Arctic sites Ny-Ålesund and Barrow, although their magnitudes were slightly lower than those in COLBC. Numerical model simulations in general successfully reproduced the observed COLBC values for PAMARCMiP and HIPPO3 (within a factor of 2), whereas they markedly underestimated the values for ARCTAS-A and NETCARE by factors of 3.7–5.8 and 3.3–5.0, respectively. Because anthropogenic contributions account for nearly all of the COLBC (82–98 %) in PAMARCMiP and HIPPO3, the good agreements between the observations and calculations for these two experiments suggest that anthropogenic contributions were generally well reproduced. However, the significant underestimations of COLBC for ARCTAS-A and NETCARE suggest that biomass burning contributions were underestimated. In this study, we also investigated plumes with enhanced BC mass concentrations, which were affected by biomass burning emissions, observed at 5 km altitude. Interestingly, the mass-averaged diameter of BC (core) and the shell-to-core diameter ratio of BC-containing particles in the plumes were generally not very different from those in other air sampled, which were considered to be mostly aged anthropogenic BC. These observations provide useful bases to evaluate numerical model simulations of the BC radiative effect in the Arctic region in spring.

scholarly journals Vertical profiles of light absorption and scattering associated with black-carbon particle fractions in the springtime Arctic above 79° N

2019 ◽  
Author(s):  
W. Richard Leaitch ◽  
John K. Kodros ◽  
Megan D. Willis ◽  
Sarah Hanna ◽  
Hannes Schulz ◽  
...  
Keyword(s):  
Optical Properties ◽  
Absorption Coefficient ◽  
Black Carbon ◽  
Light Absorption ◽  
Single Scattering ◽  
Single Scattering Albedo ◽  
The Arctic ◽  
Vertical Profiles ◽  
Near Surface ◽  
Arctic Atmosphere

Abstract. Despite the potential importance of black carbon (BC) to radiative forcing of the Arctic atmosphere, vertically-resolved measurements of the particle light scattering coefficient (Bsp) and light absorption coefficient (Bap) in the springtime Arctic atmosphere are infrequent, especially measurements at latitudes at or above 80oN. Here, relationships among vertically-distributed aerosol optical properties Bap, Bsp, and single scattering albedo or SSA), particle microphysics and particle chemistry are examined for a region of the Canadian archipelago between 79.9oN and 83.4oN from near the surface to 500 hPa. Airborne data collected during April, 2015, are combined with ground-based observations from the observatory at Alert, Nunavut and simulations from the GEOS-Chem-TOMAS model (Kodros et al., 2018) to increase our knowledge of the effects of BC on light absorption in the Arctic troposphere. The results are constrained for Bsp less than 15 Mm-1, which represent 98% of the observed Bsp, because the single scattering albedo (SSA) has a tendency to be lower at lower Bsp, resulting in a larger relative contribution to Arctic warming. At 18.4 m2 g-1, the average BC mass absorption coefficient (MAC) from the combined airborne and Alert observations is substantially higher than the two averaged modelled MAC values (9.5 m2 g-1 and 7.0 m2 g-1) for two different internal mixing assumptions, the latter of which is based on previous observations. The higher observed MAC value may be explained by an underestimation of BC and possible differences in BC microphysics and morphologies between the observations and model. We present Bap and SSA based on the assumption that Bap is overestimated in the observations in addition to the assumption that the higher MAC is explained. Median values of the measured Bap, rBC and organic component of particles all increase by a factor of 1.8±0.1 going from near-surface to 750 hPa, and values higher than the surface persist to 600 hPa. Modelled BC, organics, and Bap agree with the near-surface measurements, but do not reproduce the higher values observed between 900 hPa and 600 hPa. The differences between modelled and observed optical properties follow the same trend as the differences between the modelled and observed concentrations of the carbonaceous components (black and organic). Some discrepancies in the model may be due to the use of a relatively low imaginary refractive index of BC as well as by the ejection of biomass burning particles only into the boundary layer at sources. For the assumption of the higher observed MAC value, the SSA range between 0.88 and 0.94, which is significantly lower than other recent estimates for the Arctic, in part reflecting the constraint of Bsp <15 Mm-1. The large uncertainties in measuring optical properties and BC as well as the large differences between measured and modelled values, here and in the literature, argue for improved measurements of BC and light absorption by BC as well as more vertical profiles of aerosol chemistry, microphysics, and other optical properties in the Arctic.

scholarly journals Influence of cloud microphysical processes on black carbon wet removal, global distributions, and radiative forcing

2018 ◽  
Author(s):  
Jiayu Xu ◽  
Jiachen Zhang ◽  
Junfeng Liu ◽  
Kan Yi ◽  
Songlin Xiang ◽  
...  
Keyword(s):  
Black Carbon ◽  
Wet Deposition ◽  
Radiative Forcing ◽  
Cloud Water ◽  
Ice Nucleation ◽  
Cloud Microphysical Processes ◽  
Vertical Distributions ◽  
Microphysical Processes ◽  
Aerosol Activation ◽  
Wet Removal

Abstract. Parameterizations that impact wet removal of black carbon remain uncertain in global climate models. In this study, we enhance the default wet deposition scheme for BC in the Community Earth System Model (CESM) to (a) add relevant physical processes that were not resolved in the default model, and (b) facilitate understanding of the relative importance of various cloud processes on BC distributions. We find that the enhanced scheme greatly improves model performance against HIPPO observations relative to the default scheme. We find that convection scavenging, aerosol activation, ice nucleation, evaporation of rain/snow, and below cloud scavenging dominate wet deposition of BC. BC conversion rates for processes related to in-cloud water/ice conversion (i.e., riming, the Bergeron processes, and evaporation of cloud water sedimentation) are relatively smaller, but have large seasonal variations. We also conduct sensitivity simulations that turn off each cloud process one at a time to quantify the influence of cloud processes on BC distributions and radiative forcing. Convective scavenging is found to most significantly influence BC concentrations at mid-altitudes over the tropics and even globally. In addition, BC is sensitive to all cloud processes over the Northern Hemisphere at high latitudes. As for BC vertical distributions, convective scavenging has a dominant influence. Aerosol activation mainly increases the fraction of column BC below 5 km whereas ice nucleation decreases that above 10 km. During wintertime, the Bergeron process also significantly increases BC concentrations at lower altitudes over the Arctic. Our simulation yields a global BC burden of 85 Gg; corresponding direct radiative forcing (DRF) of BC estimated using the Parallel Offline Radiative Transfer (PORT) is 0.13 W m−2, much lower than previous studies. The range of DRF derived from sensitivity simulations is large, 0.09–0.33 W m−2, corresponding to BC burdens varying from 73 Gg to 151 Gg. Due to differences in BC vertical distributions among each sensitivity simulation, fractional changes in DRF (relative to the baseline simulation) are always higher than fractional changes in BC burdens; this occurs because relocating BC in the vertical influences the radiative forcing per BC mass. Our results highlight the influences of cloud microphysical processes on BC concentrations and radiative forcing.

scholarly journals Four-dimensional variational inversion of black carbon emissions during ARCTAS-CARB with WRFDA-Chem

2017 ◽  
Vol 17 (12) ◽  
pp. 7605-7633 ◽  
Author(s):  
Jonathan J. Guerrette ◽  
Daven K. Henze
Keyword(s):  
Black Carbon ◽  
Biomass Burning ◽  
Atmospheric Aerosols ◽  
Degrees Of Freedom ◽  
Variance Reduction ◽  
Regional Climate ◽  
The Arctic ◽  
Near Surface ◽  
Fire Emissions ◽  
Aircraft Observations

Abstract. Biomass burning emissions of atmospheric aerosols, including black carbon, are growing due to increased global drought, and comprise a large source of uncertainty in regional climate and air quality studies. We develop and apply new incremental four-dimensional variational (4D-Var) capabilities in WRFDA-Chem to find optimal spatially and temporally distributed biomass burning (BB) and anthropogenic black carbon (BC) aerosol emissions. The constraints are provided by aircraft BC concentrations from the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites in collaboration with the California Air Resources Board (ARCTAS-CARB) field campaign and surface BC concentrations from the Interagency Monitoring of PROtected Visual Environment (IMPROVE) network on 22, 23, and 24 June 2008. We consider three BB inventories, including Fire INventory from NCAR (FINN) v1.0 and v1.5 and Quick Fire Emissions Database (QFED) v2.4r8. On 22 June, aircraft observations are able to reduce the spread between a customized QFED inventory and FINNv1.0 from a factor of 3. 5 ( × 3. 5) to only × 2. 1. On 23 and 24 June, the spread is reduced from × 3. 4 to × 1. 4. The posterior corrections to emissions are heterogeneous in time and space, and exhibit similar spatial patterns of sign for both inventories. The posterior diurnal BB patterns indicate that multiple daily emission peaks might be warranted in specific regions of California. The US EPA's 2005 National Emissions Inventory (NEI05) is used as the anthropogenic prior. On 23 and 24 June, the coastal California posterior is reduced by × 2, where highway sources dominate, while inland sources are increased near Barstow by × 5. Relative BB emission variances are reduced from the prior by up to 35 % in grid cells close to aircraft flight paths and by up to 60 % for fires near surface measurements. Anthropogenic variance reduction is as high as 40 % and is similarly limited to sources close to observations. We find that the 22 June aircraft observations are able to constrain approximately 14 degrees of freedom of signal (DOF), while surface and aircraft observations together on 23/24 June constrain 23 DOF. Improving hourly- to daily-scale concentration predictions of BC and other aerosols during BB events will require more comprehensive and/or targeted measurements and a more complete accounting of sources of error besides the emissions.

scholarly journals Responses of Arctic black carbon and surface temperature to multi-region emission reductions: a Hemispheric Transport of Air Pollution Phase 2 (HTAP2) ensemble modeling study

2021 ◽  
Vol 21 (11) ◽  
pp. 8637-8654
Author(s):  
Na Zhao ◽  
Xinyi Dong ◽  
Kan Huang ◽  
Joshua S. Fu ◽  
Marianne Tronstad Lund ◽  
...  
Keyword(s):  
Air Pollution ◽  
Surface Temperature ◽  
Black Carbon ◽  
The Arctic ◽  
Ensemble Modeling ◽  
Phase 2 ◽  
Emission Reductions ◽  
Near Surface ◽  
Source Regions ◽  
The Impact

Abstract. Black carbon (BC) emissions play an important role in regional climate change in the Arctic. It is necessary to pay attention to the impact of long-range transport from regions outside the Arctic as BC emissions from local sources in the Arctic were relatively small. The task force Hemispheric Transport of Air Pollution Phase 2 (HTAP2) set up a series of simulation scenarios to investigate the response of BC in a given region to different source regions. This study investigated the responses of Arctic BC concentrations and surface temperature to 20 % anthropogenic emission reductions from six regions in 2010 within the framework of HTAP2 based on ensemble modeling results. Emission reductions from East Asia (EAS) had the most (monthly contributions: 0.2–1.5 ng m−3) significant impact on the Arctic near-surface BC concentrations, while the monthly contributions from Europe (EUR), Middle East (MDE), North America (NAM), Russia–Belarus–Ukraine (RBU), and South Asia (SAS) were 0.2–1.0, 0.001–0.01, 0.1–0.3, 0.1–0.7, and 0.0–0.2 ng m−3, respectively. The responses of the vertical profiles of the Arctic BC to the six regions were found to be different due to multiple transport pathways. Emission reductions from NAM, RBU, EUR, and EAS mainly influenced the BC concentrations in the low troposphere of the Arctic, while most of the BC in the upper troposphere of the Arctic derived from SAS. The response of the Arctic BC to emission reductions in six source regions became less significant with the increase in the latitude. The benefit of BC emission reductions in terms of slowing down surface warming in the Arctic was evaluated by using absolute regional temperature change potential (ARTP). Compared to the response of global temperature to BC emission reductions, the response of Arctic temperature was substantially more sensitive, highlighting the need for curbing global BC emissions.

scholarly journals Vertical profiles of light absorption and scattering associated with black carbon particle fractions in the springtime Arctic above 79° N

2020 ◽  
Vol 20 (17) ◽  
pp. 10545-10563 ◽  
Author(s):  
W. Richard Leaitch ◽  
John K. Kodros ◽  
Megan D. Willis ◽  
Sarah Hanna ◽  
Hannes Schulz ◽  
...  
Keyword(s):  
Optical Properties ◽  
Absorption Coefficient ◽  
Black Carbon ◽  
Light Absorption ◽  
Single Scattering ◽  
Single Scattering Albedo ◽  
The Arctic ◽  
Vertical Profiles ◽  
Near Surface ◽  
Arctic Atmosphere

Abstract. Despite the potential importance of black carbon (BC) for radiative forcing of the Arctic atmosphere, vertically resolved measurements of the particle light scattering coefficient (σsp) and light absorption coefficient (σap) in the springtime Arctic atmosphere are infrequent, especially measurements at latitudes at or above 80∘ N. Here, relationships among vertically distributed aerosol optical properties (σap, σsp and single scattering albedo or SSA), particle microphysics and particle chemistry are examined for a region of the Canadian archipelago between 79.9 and 83.4∘ N from near the surface to 500 hPa. Airborne data collected during April 2015 are combined with ground-based observations from the observatory at Alert, Nunavut and simulations from the Goddard Earth Observing System (GEOS) model, GEOS-Chem, coupled with the TwO-Moment Aerosol Sectional (TOMAS) model (collectively GEOS-Chem–TOMAS; Kodros et al., 2018) to further our knowledge of the effects of BC on light absorption in the Arctic troposphere. The results are constrained for σsp less than 15 Mm−1, which represent 98 % of the observed σsp, because the single scattering albedo (SSA) has a tendency to be lower at lower σsp, resulting in a larger relative contribution to Arctic warming. At 18.4 m2 g−1, the average BC mass absorption coefficient (MAC) from the combined airborne and Alert observations is substantially higher than the two averaged modelled MAC values (13.6 and 9.1 m2 g−1) for two different internal mixing assumptions, the latter of which is based on previous observations. The higher observed MAC value may be explained by an underestimation of BC, the presence of small amounts of dust and/or possible differences in BC microphysics and morphologies between the observations and model. In comparing the observations and simulations, we present σap and SSA, as measured, and σap∕2 and the corresponding SSA to encompass the lower modelled MAC that is more consistent with accepted MAC values. Median values of the measured σap, rBC and the organic component of particles all increase by a factor of 1.8±0.1, going from near-surface to 750 hPa, and values higher than the surface persist to 600 hPa. Modelled BC, organics and σap agree with the near-surface measurements but do not reproduce the higher values observed between 900 and 600 hPa. The differences between modelled and observed optical properties follow the same trend as the differences between the modelled and observed concentrations of the carbonaceous components (black and organic). Model-observation discrepancies may be mostly due to the modelled ejection of biomass burning particles only into the boundary layer at the sources. For the assumption of the observed MAC value, the SSA range between 0.88 and 0.94, which is significantly lower than other recent estimates for the Arctic, in part reflecting the constraint of σsp<15 Mm−1. The large uncertainties in measuring optical properties and BC, and the large differences between measured and modelled values here and in the literature, argue for improved measurements of BC and light absorption by BC and more vertical profiles of aerosol chemistry, microphysics and other optical properties in the Arctic.

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