Review of "Vertical profiles of aerosol and black carbon in the Arctic: a seasonal phenomenology along two years (2011-2012) of field campaign” by Ferrero et al.

2016 ◽  
Author(s):  
Anonymous
2016 ◽  
Author(s):  
Marianne T. Lund ◽  
Terje K. Berntsen ◽  
Bjørn H. Samset

Abstract. Despite recent improvements, significant uncertainties in global modeling of black carbon (BC) aerosols persist, posing important challenges for the design and evaluation of effective climate mitigation strategies targeted at BC emission reductions. Here we investigate the sensitivity of BC concentrations in the chemistry-transport model OsloCTM2 with the microphysical aerosol parameterization M7 (OsloCTM2-M7) to parameters controlling aerosol aging and scavenging. We focus on Arctic surface concentrations and remote region BC vertical profiles, and introduce a novel treatment of condensation of nitric acid on BC. The OsloCTM2-M7 underestimates annual averaged BC surface concentrations, with a mean normalized bias of −0.55. The seasonal cycle and magnitude of Arctic BC surface concentrations is improved compared to previous OsloCTM2 studies, but model-measurement discrepancies during spring remain. High-altitude BC over the Pacific is overestimated compared with measurements from the HIPPO campaigns. We find that a shorter global BC lifetime improves the agreement with HIPPO, in line with other recent studies. Several processes can achieve this, including allowing for convective scavenging of hydrophobic BC and reducing the amount of soluble material required for aging. Simultaneously, the concentrations in the Arctic are reduced, resulting in poorer agreement with measurements in part of the region. A first step towards inclusion of aging by nitrate in OsloCTM2-M7 is made by allowing for condensation of nitric acid on BC. This results in a faster aging and reduced lifetime, and in turn to a better agreement with the HIPPO measurements. On the other hand, model-measurement discrepancies in the Arctic are exacerbated. Work to further improve this parameterization is needed. The impact on global mean radiative forcing (RF) and surface temperature response (TS) in our experiments is estimated. Compared to the baseline, decreases in global mean direct RF on the order of 10–30 % of the total pre-industrial to present BC direct RF is estimated for the experiments that result in the largest changes in BC concentrations. We show that globally tuning parameters related to BC aging and scavenging can improve the representation of BC vertical profiles in the OsloCTM2-M7 compared with observations. Our results also show that such improvements can result from changes in several processes and often depend on assumptions about uncertain parameters such as the BC ice nucleating efficiency and the change in hygroscopicity with aging. It is also important to be aware of potential tradeoffs in model performance between different regions. Other important sources of uncertainty, particularly for Arctic BC, such as model resolution has not been investigated here. Our results underline the importance of more observations and experimental data to improve process understanding and thus further constrain models.


2016 ◽  
Vol 16 (16) ◽  
pp. 10441-10454 ◽  
Author(s):  
Liang Ran ◽  
Zhaoze Deng ◽  
Xiaobin Xu ◽  
Peng Yan ◽  
Weili Lin ◽  
...  

Abstract. Black carbon (BC) is a dominant absorber in the visible spectrum and a potent factor in climatic effects. Vertical profiles of BC were measured using a micro-aethalometer attached to a tethered balloon during the Vertical Observations of trace Gases and Aerosols (VOGA) field campaign, in summer 2014 at a semirural site in the North China Plain (NCP). The diurnal cycle of BC vertical distributions following the evolution of the mixing layer (ML) was investigated for the first time in the NCP region. Statistical parameters including identified mixing height (Hm) and average BC mass concentrations within the ML (Cm) and in the free troposphere (Cf) were obtained for a selected dataset of 67 vertical profiles. Hm was usually lower than 0.2 km in the early morning and rapidly rose thereafter due to strengthened turbulence. The maximum height of the ML was reached in the late afternoon. The top of a full developed ML exceeded 1 km on sunny days in summer, while it stayed much lower on cloudy  days. The sunset triggered the collapse of the ML, and a stable nocturnal boundary layer (NBL) gradually formed. Accordingly, the highest level Cm was found in the early morning and the lowest was found in the afternoon. In the daytime, BC was almost uniformly distributed within the ML and significantly decreased above the ML. During the field campaign, Cm averaged about 5.16 ± 2.49 µg m−3, with a range of 1.12 to 14.49 µg m−3, comparable with observational results in many polluted urban areas such as Milan in Italy and Shanghai in China. As evening approached, BC gradually built up near the surface and exponentially declined with height. In contrast to the large variability found both in Hm and Cm, Cf stayed relatively unaffected through the day. Cf was less than 10 % of the ground level under clean conditions, while it amounted to half of the ground level in some polluted cases. In situ measurements of BC vertical profiles would hopefully have an important implication for accurately estimating direct radiative forcing by BC and improving the retrieval of aerosol optical properties by remote sensing in this region.


2010 ◽  
Vol 10 (6) ◽  
pp. 15167-15196
Author(s):  
J. R. Spackman ◽  
R. S. Gao ◽  
W. D. Neff ◽  
J. P. Schwarz ◽  
L. A. Watts ◽  
...  

Abstract. Understanding the processes controlling black carbon (BC) in the Arctic is crucial for evaluating the impact of anthropogenic and natural sources of BC on Arctic climate. Vertical profiles of BC mass were observed from the surface to near 7-km altitude in April 2008 using a Single-Particle Soot Photometer (SP2) during flights on the NOAA WP-3D research aircraft from Fairbanks, Alaska. These measurements were conducted during the NOAA-sponsored Aerosol, Radiation, and Cloud Processes affecting Arctic Climate (ARCPAC) project as part of POLARCAT, an International Polar Year (IPY) activity. In the free troposphere, the Arctic air mass was influenced by long-range transport from biomass-burning and anthropogenic source regions at lower latitudes especially during the latter part of the campaign. Maximum average BC mass loadings of 150 ng kg−1 were observed near 5.5-km altitude in the aged Arctic air mass. In biomass-burning plumes, BC was enhanced from near the top of the Arctic boundary layer (ABL) to 5.5 km compared to the aged Arctic air mass. At the bottom of some of the profiles, positive vertical gradients in BC were observed in the vicinity of open leads in the sea-ice. BC mass loadings increased by about a factor of two across the boundary layer transition in the ABL in these cases while carbon monoxide (CO) remained constant, evidence for depletion of BC in the ABL. BC mass loadings were positively correlated with O3 in ozone depletion events (ODEs) for all the observations in the ABL suggesting that BC was removed by dry deposition of BC on the snow or ice because molecular bromine, Br2, which photolyzes and catalytically destroys O3, is thought to be released near the open leads in regions of ice formation. We estimate the deposition flux of BC mass to the snow using a box model constrained by the vertical profiles of BC in the ABL. The open leads may increase vertical mixing in the ABL and entrainment of pollution from the free troposphere possibly enhancing the deposition of BC to the snow.


2019 ◽  
Author(s):  
W. Richard Leaitch ◽  
John K. Kodros ◽  
Megan D. Willis ◽  
Sarah Hanna ◽  
Hannes Schulz ◽  
...  

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.


2014 ◽  
Vol 14 (5) ◽  
pp. 2399-2417 ◽  
Author(s):  
C. Jiao ◽  
M. G. Flanner ◽  
Y. Balkanski ◽  
S. E. Bauer ◽  
N. Bellouin ◽  
...  

Abstract. Though many global aerosols models prognose surface deposition, only a few models have been used to directly simulate the radiative effect from black carbon (BC) deposition to snow and sea ice. Here, we apply aerosol deposition fields from 25 models contributing to two phases of the Aerosol Comparisons between Observations and Models (AeroCom) project to simulate and evaluate within-snow BC concentrations and radiative effect in the Arctic. We accomplish this by driving the offline land and sea ice components of the Community Earth System Model with different deposition fields and meteorological conditions from 2004 to 2009, during which an extensive field campaign of BC measurements in Arctic snow occurred. We find that models generally underestimate BC concentrations in snow in northern Russia and Norway, while overestimating BC amounts elsewhere in the Arctic. Although simulated BC distributions in snow are poorly correlated with measurements, mean values are reasonable. The multi-model mean (range) bias in BC concentrations, sampled over the same grid cells, snow depths, and months of measurements, are −4.4 (−13.2 to +10.7) ng g−1 for an earlier phase of AeroCom models (phase I), and +4.1 (−13.0 to +21.4) ng g−1 for a more recent phase of AeroCom models (phase II), compared to the observational mean of 19.2 ng g−1. Factors determining model BC concentrations in Arctic snow include Arctic BC emissions, transport of extra-Arctic aerosols, precipitation, deposition efficiency of aerosols within the Arctic, and meltwater removal of particles in snow. Sensitivity studies show that the model–measurement evaluation is only weakly affected by meltwater scavenging efficiency because most measurements were conducted in non-melting snow. The Arctic (60–90° N) atmospheric residence time for BC in phase II models ranges from 3.7 to 23.2 days, implying large inter-model variation in local BC deposition efficiency. Combined with the fact that most Arctic BC deposition originates from extra-Arctic emissions, these results suggest that aerosol removal processes are a leading source of variation in model performance. The multi-model mean (full range) of Arctic radiative effect from BC in snow is 0.15 (0.07–0.25) W m−2 and 0.18 (0.06–0.28) W m−2 in phase I and phase II models, respectively. After correcting for model biases relative to observed BC concentrations in different regions of the Arctic, we obtain a multi-model mean Arctic radiative effect of 0.17 W m−2 for the combined AeroCom ensembles. Finally, there is a high correlation between modeled BC concentrations sampled over the observational sites and the Arctic as a whole, indicating that the field campaign provided a reasonable sample of the Arctic.


2020 ◽  
Vol 20 (17) ◽  
pp. 10545-10563 ◽  
Author(s):  
W. Richard Leaitch ◽  
John K. Kodros ◽  
Megan D. Willis ◽  
Sarah Hanna ◽  
Hannes Schulz ◽  
...  

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.


2016 ◽  
Author(s):  
Luca Ferrero ◽  
David Cappelletti ◽  
Maurizio Busetto ◽  
Mauro Mazzola ◽  
Angelo Lupi ◽  
...  

Abstract. In this paper we present results from a systematic study of vertical profiles of aerosol number size distribution and black carbon (BC) concentrations conducted in the Arctic, over Ny-Ålesund (Svalbard). The campaign lasted 2 years (2011–2012) and resulted in 200 vertical profiles measured during the spring and summer seasons. In addition, chemical analysis of filter samples, aerosol size distribution and a full set of meteorological parameters were determined at ground to put on a firmer grounds the analysis of the vertical profiles. The collected experimental data allowed a classification of the vertical profiles into different typologies which allowed to describe a seasonal phenomenology of vertical aerosol properties in the Arctic. During spring, four main types of profiles were found and their behaviour was related to the main aerosol and atmospheric dynamics occurring at the measuring site. Background conditions generated homogenous profiles. Transport events caused an increase of aerosol concentration with altitude. High Arctic haze pollution trapped below thermal inversions promoted a decrease of aerosol concentration with altitude. Finally, ground-based plumes of locally formed secondary aerosol determined profiles with decreasing aerosol concentration located at different altitude in function of size. During the summer season, the impact from shipping caused aerosol and BC pollution plumes constrained close to the ground, indicating that increasing shipping emissions in the Arctic could bring anthropogenic aerosol and BC in the summer Arctic affecting the climate.


2020 ◽  
Author(s):  
Eemeli Holopainen ◽  
Harri Kokkola ◽  
Anton Laakso ◽  
Thomas Kühn

Abstract. In this study we introduce an in-cloud wet deposition scheme for liquid and ice phase clouds for global aerosol-climate models which use a size-segregated aerosol description. For in-cloud nucleation scavenging, the scheme uses cloud droplet activation and ice nucleation rates obtained from the host model. For in-cloud impaction scavenging, we used a method where the removal rate depends on the aerosol size and cloud droplet radii. The scheme was compared to a scheme that uses fixed scavenging coefficients. The comparison included vertical profiles and mass and number distributions of wet deposition fluxes of different aerosol compounds and for different latitude bands. Using the scheme presented here, mass concentrations for black carbon, organic carbon, sulfate, and the number concentration of particles with diameters larger than 100 nm are higher than using fixed scavenging coefficients, with the largest differences in the vertical profiles in the Arctic. On the other hand, the number concentrations of small particles show a decrease, especially in the Arctic region. These results indicate that, compared to using fixed scavenging coefficients, nucleation scavenging is less efficient and impaction scavenging is increased in the scheme introduced here. Without further adjustments in the host model, our wet deposition scheme produced unrealistically high aerosol concentrations, especially at high altitudes. This also leads to a spuriously long lifetime of black carbon aerosol. To find a better setup for simulating aerosol vertical profiles and transport, sensitivity simulations were conducted where aerosol emission distribution and hygroscopicity were altered. The simulated vertical profiles of aerosol in these sensitivity studies were evaluated against aircraft observations. The lifetimes of different aerosol compounds were also evaluated against the ensemble mean of models involved in the Aerosol Comparisons between Observations and Models (AEROCOM) project. The best comparison between the observations and the model was achieved with the new wet deposition scheme when black carbon was emitted internally mixed with soluble compounds instead of keeping it externally mixed. This also produced atmospheric lifetimes for the other species which were comparable to the AEROCOM model means.


2020 ◽  
Vol 13 (12) ◽  
pp. 6215-6235
Author(s):  
Eemeli Holopainen ◽  
Harri Kokkola ◽  
Anton Laakso ◽  
Thomas Kühn

Abstract. In this study we introduce an in-cloud wet deposition scheme for liquid and ice phase clouds for global aerosol–climate models which use a size-segregated aerosol description. For in-cloud nucleation scavenging, the scheme uses cloud droplet activation and ice nucleation rates obtained from the host model. For in-cloud impaction scavenging, we used a method where the removal rate depends on the wet aerosol size and cloud droplet radii. We used the latest release version of ECHAM-HAMMOZ (ECHAM6.3-HAM2.3-MOZ1.0) with the Sectional Aerosol module for Large Scale Applications version 2.0 (SALSA) microphysics package to test and compare our scheme. The scheme was compared to a scheme that uses fixed scavenging coefficients. The comparison included vertical profiles and mass and number distributions of wet deposition fluxes of different aerosol compounds and for different latitude bands. Using the scheme presented here, mass concentrations for black carbon, organic carbon, sulfate, and the number concentration of particles with diameters larger than 100 nm are higher than using fixed scavenging coefficients, with the largest differences in the vertical profiles in the Arctic. On the other hand, the number concentrations of particles smaller than 100 nm in diameter show a decrease, especially in the Arctic region. These results could indicate that, compared to fixed scavenging coefficients, nucleation scavenging is less efficient, resulting in an increase in the number concentration of particles larger than 100 nm. In addition, changes in rates of impaction scavenging and new particle formation (NPF) can be the main cause of reduction in the number concentrations of particles smaller than 100 nm. Without further adjustments in the host model, our wet deposition scheme produced unrealistically high aerosol concentrations, especially at high altitudes. This also leads to a spuriously long lifetime of black carbon aerosol. To find a better setup for simulating aerosol vertical profiles and transport, sensitivity simulations were conducted where aerosol emission distribution and hygroscopicity were altered. Vertical profiles of aerosol species simulated with the scheme which uses fixed scavenging rates and the abovementioned sensitivity simulations were evaluated against vertical profiles from aircraft observations. The lifetimes of different aerosol compounds were also evaluated against the ensemble mean of models involved in the Aerosol Comparisons between Observations and Models (AEROCOM) project. The best comparison between the observations and the model was achieved with our wet deposition scheme when black carbon was emitted internally mixed with soluble compounds instead of keeping it externally mixed. This also produced atmospheric lifetimes for the other species which were comparable to the AEROCOM model means.


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