scholarly journals Vertical profiles of aerosol and black carbon in the Arctic: a seasonal phenomenology along two years (2011–2012) of field campaign

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.

2016 ◽  
Vol 16 (19) ◽  
pp. 12601-12629 ◽  
Author(s):  
Luca Ferrero ◽  
David Cappelletti ◽  
Maurizio Busetto ◽  
Mauro Mazzola ◽  
Angelo Lupi ◽  
...  

Abstract. 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 by means of a tethered balloon (up to 1200 m a.g.l.) 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. The collected experimental data allowed a classification of the vertical profiles into different typologies, which allowed us to describe the seasonal phenomenology of vertical aerosol properties in the Arctic. During spring, four main types of profiles were found and their behavior 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 as a function of size. During the summer season, the impact from shipping caused aerosol and BC pollution plumes to be constrained close to the ground, indicating that increasing shipping emissions in the Arctic could bring anthropogenic aerosol and BC in the Arctic summer, affecting the climate.


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.


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.


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.


2010 ◽  
Vol 10 (19) ◽  
pp. 9667-9680 ◽  
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 loadings 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. 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. Average BC mass mixing ratios peaked at about 150 ng BC (kg dry air )−1 near 5.5 km altitude in the aged Arctic air mass and 250 ng kg−1 at 4.5 km in biomass-burning influenced air. BC mass loadings were enhanced by up to a factor of 5 in biomass-burning influenced air compared to the aged Arctic air mass. At the bottom of some of the profiles, positive vertical gradients in BC were observed over the sea-ice. The vertical profiles generally occurred in the vicinity of open leads in the sea-ice. In the aged Arctic air mass, BC mass loadings more than doubled with increasing altitude within the ABL and across the boundary layer transition while carbon monoxide (CO) remained constant. This is evidence for depletion of BC mass in the ABL. BC mass loadings were positively correlated with O3 in ozone depletion events (ODEs) for all the observations in the ABL. Since bromine catalytically destroys ozone in the ABL after being released as molecular bromine in regions of new sea-ice formation at the surface, the BC–O3 correlation suggests that BC particles were removed by a surface process such as dry deposition. We develop a box model to estimate the dry deposition flux of BC mass to the snow constrained by the vertical profiles of BC mass in the ABL. Open leads in the sea-ice may increase vertical mixing and entrainment of pollution from the free troposphere possibly enhancing the deposition of BC aerosol to the snow.


2011 ◽  
Vol 11 (12) ◽  
pp. 32499-32534 ◽  
Author(s):  
M. T. Lund ◽  
T. Berntsen

Abstract. A critical parameter for the atmospheric lifetime of black carbon (BC) aerosols, and hence for the range over which the particles can be transported, is the aging time, i.e. the time before the aerosols become available for removal by wet deposition. This study compares two different parameterizations of BC aging in the chemistry transport model OsloCTM2: (i) a bulk parameterization (BULK) where aging is represented by a constant transfer to hydrophilic mode and (ii) a microphysical module (M7) where aging occurs through particle interaction and where the particle size distribution is accounted for. We investigate the effect of including microphysics on the distribution of BC globally and in the Arctic. We also focus on the impact on estimated contributions to Arctic BC from selected emission source regions. With more detailed microphysics (M7) there are regional and seasonal variations in aging. The aging is slower during high-latitude winter, when the production of sulfate is lower, than in lower latitudes and during summer. High-latitude concentrations of BC are significantly increased during winter compared to BULK. Furthermore, M7 improves the model performance at high Arctic surface stations, especially the accumulation of BC during winter. A proper representation of vertical BC load is important because the climate effects of the aerosols depend on their altitude in the atmosphere. Comparisons with measured vertical profiles indicate that the model generally overestimates the BC load, particularly at higher altitudes, and this overestimation is exacerbated with M7 compared to BULK. Both parameterizations show that north of 65° N emissions in Europe contribute most to atmospheric BC concentration and to BC in snow and ice. M7 leads to a pronounced seasonal pattern in contributions and contributions from Europe and Russia increase strongly during winter compared to BULK. There is generally a small increase in the amount of BC in snow and ice with M7 compared to BULK, but concentrations are still underestimated relative to measurements.


2016 ◽  
Vol 16 (14) ◽  
pp. 9435-9455 ◽  
Author(s):  
Matthew J. Alvarado ◽  
Chantelle R. Lonsdale ◽  
Helen L. Macintyre ◽  
Huisheng Bian ◽  
Mian Chin ◽  
...  

Abstract. Accurate modeling of the scattering and absorption of ultraviolet and visible radiation by aerosols is essential for accurate simulations of atmospheric chemistry and climate. Closure studies using in situ measurements of aerosol scattering and absorption can be used to evaluate and improve models of aerosol optical properties without interference from model errors in aerosol emissions, transport, chemistry, or deposition rates. Here we evaluate the ability of four externally mixed, fixed size distribution parameterizations used in global models to simulate submicron aerosol scattering and absorption at three wavelengths using in situ data gathered during the 2008 Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) campaign. The four models are the NASA Global Modeling Initiative (GMI) Combo model, GEOS-Chem v9-02, the baseline configuration of a version of GEOS-Chem with online radiative transfer calculations (called GC-RT), and the Optical Properties of Aerosol and Clouds (OPAC v3.1) package. We also use the ARCTAS data to perform the first evaluation of the ability of the Aerosol Simulation Program (ASP v2.1) to simulate submicron aerosol scattering and absorption when in situ data on the aerosol size distribution are used, and examine the impact of different mixing rules for black carbon (BC) on the results. We find that the GMI model tends to overestimate submicron scattering and absorption at shorter wavelengths by 10–23 %, and that GMI has smaller absolute mean biases for submicron absorption than OPAC v3.1, GEOS-Chem v9-02, or GC-RT. However, the changes to the density and refractive index of BC in GC-RT improve the simulation of submicron aerosol absorption at all wavelengths relative to GEOS-Chem v9-02. Adding a variable size distribution, as in ASP v2.1, improves model performance for scattering but not for absorption, likely due to the assumption in ASP v2.1 that BC is present at a constant mass fraction throughout the aerosol size distribution. Using a core-shell mixing rule in ASP overestimates aerosol absorption, especially for the fresh biomass burning aerosol measured in ARCTAS-B, suggesting the need for modeling the time-varying mixing states of aerosols in future versions of ASP.


Ocean Science ◽  
2014 ◽  
Vol 10 (6) ◽  
pp. 967-975 ◽  
Author(s):  
A. J. G. Nurser ◽  
S. Bacon

Abstract. The first (and second) baroclinic deformation (or Rossby) radii are presented north of ~60° N, focusing on deep basins and shelf seas in the high Arctic Ocean, the Nordic seas, Baffin Bay, Hudson Bay and the Canadian Arctic Archipelago, derived from climatological ocean data. In the high Arctic Ocean, the first Rossby radius increases from ~5 km in the Nansen Basin to ~15 km in the central Canadian Basin. In the shelf seas and elsewhere, values are low (1–7 km), reflecting weak density stratification, shallow water, or both. Seasonality strongly impacts the Rossby radius only in shallow seas, where winter homogenization of the water column can reduce it to below 1 km. Greater detail is seen in the output from an ice–ocean general circulation model, of higher resolution than the climatology. To assess the impact of secular variability, 10 years (2003–2012) of hydrographic stations along 150° W in the Beaufort Gyre are also analysed. The first-mode Rossby radius increases over this period by ~20%. Finally, we review the observed scales of Arctic Ocean eddies.


2017 ◽  
Author(s):  
Zilin Wang ◽  
Xin Huang ◽  
Aijun Ding

Abstract. Black carbon (BC) has been identified to play a critical role in aerosol-planet boundary layer (PBL) interaction and further deterioration of near-surface air pollution in megacities, which has been named as its dome effect. However, the impacts of key factors that influence this effect, such as the vertical distribution and aging processes of BC, and also the underlying land surface, have not been quantitatively explored yet. Here, based on available in-situ measurements of meteorology and atmospheric aerosols together with the meteorology-chemistry online coupled model, WRF-Chem, we conduct a set of parallel simulations to quantify the roles of these factors in influencing the BC's dome effect and surface haze pollution, and discuss the main implications of the results to air pollution mitigation in China. We found that the impact of BC on PBL is very sensitive to the altitude of aerosol layer. The upper level BC, especially those near the capping inversion, is more essential in suppressing the PBL height and weakening the turbulence mixing. The dome effect of BC tends to be significantly intensified as BC aerosol mixed with scattering aerosols during winter haze events, resulting in a decrease of PBL height by more than 25 %. In addition, the dome effect is more substantial (up to 15 %) in rural areas than that in the urban areas with the same BC loading, indicating an unexpected regional impact of such kind of effect to air quality in countryside. This study suggests that China's regional air pollution would greatly benefit from BC emission reductions, especially those from the elevated sources from the chimneys and also the domestic combustions in rural areas, through weakening the aerosol-boundary layer interactions that triggered by BC.


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