scholarly journals Effects of Wegener-Bergeron-Findeisen Process on Global Black Carbon Distribution

Author(s):  
Ling Qi ◽  
Qinbin Li ◽  
Cenlin He ◽  
Xin Wang ◽  
Jianping Huang

Abstract. We systematically investigate the effects of Wegener-Bergeron-Findeisen (WBF) on BC scavenging efficiency, surface BCair, deposition flux, concentration in snow (BCsnow, ng g−1), and washout ratio using a global 3D chemical transport model (GEOS-Chem). We differentiate riming- versus WBF-dominated in-cloud scavenging based on liquid water content (LWC) and temperature. Specifically, we relate WBF to either temperature or ice mass fraction (IMF) in mixed-phase clouds. We find that at Jungfraujoch, Switzerland and Abisko, Sweden, where WBF dominates, the discrepancies of simulated BC scavenging efficiency and washout ratio are significantly reduced (from a factor of 3 to 10 % and from a factor of 4–5 to a factor of two). However, at Zeppelin, Norway, where riming dominates, simulation of BC scavenging efficiency, BCair, and washout ratio become worse (relative to observations) when WBF is included. There is thus an urgent need for extensive observations to distinguish and characterize riming- versus WBF-dominated aerosol scavenging in mixed-phase clouds and the associated BC scavenging efficiency. We find the reduction resulting from WBF to global BC scavenging efficiency varies substantially, from 8 % in the tropics to 76 % in the Arctic. The resulting annual mean BCair increases by up to 156 % at high altitudes and at northern high latitudes because of lower temperature and higher IMF. Overall, WBF halves the model-observation discrepancy (from −65 % to −30 %) of BCair across North America, Europe, China and the Arctic. Globally WBF increases BC burden from 0.22 to 0.29–0.35 mg m−2 yr−1, which partially explains the gap between observed and previous model simulated BC burdens over land. In addition, WBF significantly increases BC lifetime from 5.7 days to ~8 days. Additionally, WBF results in a significant redistribution of BC deposition in source and remote regions. Specifically, it lowers BC wet deposition (by 37–63 % at northern mid-latitudes and by 21–29 % in the Arctic) while increases dry deposition (by 3–16 % at mid-latitudes and by 81–159 % in the Arctic). The resulting total BC deposition is lower at mid-latitudes (by 12–34 %) but higher in the Arctic (by 2–29 %). We find that WBF decreases BCsnow at mid-latitudes (by ~15 %) but increases it in the Arctic (by 26 %) while improving model comparisons with observations. In addition, WBF dramatically reduces the model-observation discrepancy of washout ratios in winter (from a factor of 16 to 4). The remaining discrepancies in BCair, BCsnow and BC washout ratios suggest that in-cloud removal in mixed-phased clouds is likely still excessive over land.

2017 ◽  
Vol 17 (12) ◽  
pp. 7459-7479 ◽  
Author(s):  
Ling Qi ◽  
Qinbin Li ◽  
Cenlin He ◽  
Xin Wang ◽  
Jianping Huang

Abstract. We systematically investigate the effects of Wegener–Bergeron–Findeisen process (hereafter WBF) on black carbon (BC) scavenging efficiency, surface BCair, deposition flux, concentration in snow (BCsnow, ng g−1), and washout ratio using a global 3-D chemical transport model (GEOS-Chem). We differentiate riming- versus WBF-dominated in-cloud scavenging based on liquid water content (LWC) and temperature. Specifically, we implement an implied WBF parameterization using either temperature or ice mass fraction (IMF) in mixed-phase clouds based on field measurements. We find that at Jungfraujoch, Switzerland, and Abisko, Sweden, where WBF dominates in-cloud scavenging, including the WBF effect strongly reduces the discrepancies of simulated BC scavenging efficiency and washout ratio against observations (from a factor of 3 to 10 % and from a factor of 4–5 to a factor of 2). However, at Zeppelin, Norway, where riming dominates, simulation of BC scavenging efficiency, BCair, and washout ratio become worse (relative to observations) when WBF is included. There is thus an urgent need for extensive observations to distinguish and characterize riming- versus WBF-dominated aerosol scavenging in mixed-phase clouds and the associated BC scavenging efficiency. Our model results show that including the WBF effect lowers global BC scavenging efficiency, with a higher reduction at higher latitudes (8 % in the tropics and up to 76 % in the Arctic). The resulting annual mean BCair increases by up to 156 % at high altitudes and at northern high latitudes because of lower temperature and higher IMF. Overall, WBF halves the model–observation discrepancy (from −65 to −30 %) of BCair across North America, Europe, China and the Arctic. Globally WBF increases BC burden from 0.22 to 0.29–0.35 mg m−2 yr−1, which partially explains the gap between observed and previous model-simulated BC burdens over land. In addition, WBF significantly increases BC lifetime from 5.7 to  ∼  8 days. Additionally, WBF results in a significant redistribution of BC deposition in source and remote regions. Specifically, it lowers BC wet deposition (by 37–63 % at northern mid-latitudes and by 21–29 % in the Arctic), while it increases dry deposition (by 3–16 % at mid-latitudes and by 81–159 % in the Arctic). The resulting total BC deposition is lower at mid-latitudes (by 12–34 %) but higher in the Arctic (by 2–29 %). We find that WBF decreases BCsnow at mid-latitudes (by  ∼  15 %) but increases it in the Arctic (by 26 %) while improving model comparisons with observations. In addition, WBF dramatically reduces the model–observation discrepancy of washout ratios in winter (from a factor of 16 to 4). The remaining discrepancies in BCair, BCsnow and BC washout ratios suggest that in-cloud removal in mixed-phased clouds is likely still excessive over land.


2017 ◽  
Vol 17 (20) ◽  
pp. 12779-12795 ◽  
Author(s):  
Meri M. Ruppel ◽  
Joana Soares ◽  
Jean-Charles Gallet ◽  
Elisabeth Isaksson ◽  
Tõnu Martma ◽  
...  

Abstract. The climate impact of black carbon (BC) is notably amplified in the Arctic by its deposition, which causes albedo decrease and subsequent earlier snow and ice spring melt. To comprehensively assess the climate impact of BC in the Arctic, information on both atmospheric BC concentrations and deposition is essential. Currently, Arctic BC deposition data are very scarce, while atmospheric BC concentrations have been shown to generally decrease since the 1990s. However, a 300-year Svalbard ice core showed a distinct increase in EC (elemental carbon, proxy for BC) deposition from 1970 to 2004 contradicting atmospheric measurements and modelling studies. Here, our objective was to decipher whether this increase has continued in the 21st century and to investigate the drivers of the observed EC deposition trends. For this, a shallow firn core was collected from the same Svalbard glacier, and a regional-to-meso-scale chemical transport model (SILAM) was run from 1980 to 2015. The ice and firn core data indicate peaking EC deposition values at the end of the 1990s and lower values thereafter. The modelled BC deposition results generally support the observed glacier EC variations. However, the ice and firn core results clearly deviate from both measured and modelled atmospheric BC concentration trends, and the modelled BC deposition trend shows variations seemingly independent from BC emission or atmospheric BC concentration trends. Furthermore, according to the model ca. 99 % BC mass is wet-deposited at this Svalbard glacier, indicating that meteorological processes such as precipitation and scavenging efficiency have most likely a stronger influence on the BC deposition trend than BC emission or atmospheric concentration trends. BC emission source sectors contribute differently to the modelled atmospheric BC concentrations and BC deposition, which further supports our conclusion that different processes affect atmospheric BC concentration and deposition trends. Consequently, Arctic BC deposition trends should not directly be inferred based on atmospheric BC measurements, and more observational BC deposition data are required to assess the climate impact of BC in Arctic snow.


2016 ◽  
Author(s):  
Ling Qi ◽  
Qinbin Li ◽  
Yingrui Li ◽  
Cenlin He

Abstract. We investigate the sensitivity of black carbon (BC) in the Arctic, including BC in snow (BCsnow, ng g−1) and surface air (BCair, μg m−3), to emissions, dry deposition and wet scavenging using a global 3-D chemical transport model (CTM) GEOS-Chem. We find that the model underestimates BCsnow in the Arctic by 40 % on average (median = 11.8 ng g−1). Natural gas flaring substantially increases total BC emissions in the Arctic (by ~ 70 %). The flaring emissions lead to up to 49 % increases (0.1–8.5 ng g−1) in Arctic BCsnow, dramatically improving model comparison with observations (50 % reduction in discrepancy) near flaring source regions (Western Extreme North of Russia). Ample observations suggest that BC dry deposition velocities over snow and ice in current CTMs (0.03 cm s−1 in GEOS-Chem) are exceedingly small. We apply the resistance-in-series method to compute the dry deposition velocity that varies with local meteorological and surface conditions. The resulting velocity is significantly larger and varies by a factor of eight in the Arctic (0.03–0.24 cm s−1), increases the fraction of dry to total BC deposition (16 % to 25 %), yet leaves the total BC deposition and BCsnow in the Arctic unchanged. This is largely explained by the offsetting higher dry and lower wet deposition fluxes. Additionally, we account for the effect of the Wegener-Bergeron-Findeisen (WBF) process in mixed-phase clouds, which releases BC particles from condensed phases (water drops and ice crystals) back to the interstitial air and thereby substantially reduces the scavenging efficiency of BC (by 43–76 % in the Arctic). The resulting BCsnow is up to 80 % higher, BC loading is considerably larger (from 0.25 to 0.43 mg  m−2), and BC lifetime is markedly prolonged (from 9 to 16 days) in the Arctic. Over all, flaring emissions increase BCair in the Arctic (by ~ 20 ng m−3), the updated dry deposition velocity more than halves BCair (by ~ 20 ng  m−3), and the WBF effect increases BCair by 25–70 % during winter and early spring. The resulting model simulation of BCsnow is substantially improved (within 10 % of the observations) and the discrepancies of BCair are much smaller during snow season at Barrow, Alert and Summit (from −67 %–−47 % to −46 %–3 %). Our results point toward an urgent need for better characterization of flaring emissions of BC (e.g. the emission factors, temporal and spatial distribution), extensive measurements of both the dry deposition of BC over snow and ice, and the scavenging efficiency of BC in mixed-phase clouds.


2017 ◽  
Vol 17 (2) ◽  
pp. 1037-1059 ◽  
Author(s):  
Ling Qi ◽  
Qinbin Li ◽  
Yinrui Li ◽  
Cenlin He

Abstract. We investigate the sensitivity of black carbon (BC) in the Arctic, including BC concentration in snow (BCsnow, ng g−1) and surface air (BCair, ng m−3), as well as emissions, dry deposition, and wet scavenging using the global three-dimensional (3-D) chemical transport model (CTM) GEOS-Chem. We find that the model underestimates BCsnow in the Arctic by 40 % on average (median  =  11.8 ng g−1). Natural gas flaring substantially increases total BC emissions in the Arctic (by ∼ 70 %). The flaring emissions lead to up to 49 % increases (0.1–8.5 ng g−1) in Arctic BCsnow, dramatically improving model comparison with observations (50 % reduction in discrepancy) near flaring source regions (the western side of the extreme north of Russia). Ample observations suggest that BC dry deposition velocities over snow and ice in current CTMs (0.03 cm s−1 in the GEOS-Chem) are too small. We apply the resistance-in-series method to compute a dry deposition velocity (vd) that varies with local meteorological and surface conditions. The resulting velocity is significantly larger and varies by a factor of 8 in the Arctic (0.03–0.24 cm s−1), which increases the fraction of dry to total BC deposition (16 to 25 %) yet leaves the total BC deposition and BCsnow in the Arctic unchanged. This is largely explained by the offsetting higher dry and lower wet deposition fluxes. Additionally, we account for the effect of the Wegener–Bergeron–Findeisen (WBF) process in mixed-phase clouds, which releases BC particles from condensed phases (water drops and ice crystals) back to the interstitial air and thereby substantially reduces the scavenging efficiency of clouds for BC (by 43–76 % in the Arctic). The resulting BCsnow is up to 80 % higher, BC loading is considerably larger (from 0.25 to 0.43 mg m−2), and BC lifetime is markedly prolonged (from 9 to 16 days) in the Arctic. Overall, flaring emissions increase BCair in the Arctic (by ∼ 20 ng m−3), the updated vd more than halves BCair (by ∼ 20 ng m−3), and the WBF effect increases BCair by 25–70 % during winter and early spring. The resulting model simulation of BCsnow is substantially improved (within 10 % of the observations) and the discrepancies of BCair are much smaller during the snow season at Barrow, Alert, and Summit (from −67–−47 % to −46–3 %). Our results point toward an urgent need for better characterization of flaring emissions of BC (e.g., the emission factors, temporal, and spatial distribution), extensive measurements of both the dry deposition of BC over snow and ice, and the scavenging efficiency of BC in mixed-phase clouds. In addition, we find that the poorly constrained precipitation in the Arctic may introduce large uncertainties in estimating BCsnow. Doubling precipitation introduces a positive bias approximately as large as the overall effects of flaring emissions and the WBF effect; halving precipitation produces a similarly large negative bias.


2021 ◽  
Author(s):  
Fritz Waitz ◽  
Martin Schnaiter ◽  
Thomas Leisner ◽  
Emma Järvinen

Abstract. Mixed-phase clouds consist of both supercooled liquid water droplets and solid ice crystals. Despite having a significant impact on Earth‘s climate, mixed-phase clouds are poorly understood and not well represented in climate prediction models. One piece of the puzzle is understanding and parameterizing riming of mixed-phase cloud ice crystals, which is one of the main growth mechanisms of ice crystals via the accretion of small, supercooled droplets. Especially the extent of riming on ice crystals smaller than 500 μm is often overlooked in studies – mainly because observations are scarce. Here, we investigated riming in mixed-phase clouds during three airborne campaigns in the Arctic, the Southern Ocean and US east coast. Riming was observed from stereo-microscopic cloud particle images recorded with the Particle Habit Imaging and Polar Scattering (PHIPS) probe. We show that riming is most prevalent at temperatures around −7 °C, where, on average, 43 % of the investigated particles in a size range from 100 ≤ D ≤ 700 μm showed evidence of riming. We discuss the occurrence and properties of rimed ice particles and show correlation of the occurrence and the amount of riming with ambient meteorological parameters. We show that riming fraction increases with ice particle size (< 20 % for D ≤ 200 μm, 35–40 % for D ≥ 400 μm) and liquid water content (25 % for LWC ≤ 0.05 g m−3, up to 60 % for LWC = 0.5 g m−3). We investigate the ageing of rimed particles and the difference between "normal" and "epitaxial" riming based on a case study.


2017 ◽  
Author(s):  
Meri M. Ruppel ◽  
Joana Soares ◽  
Jean-Charles Gallet ◽  
Elisabeth Isaksson ◽  
Tõnu Martma ◽  
...  

Abstract. The climate impact of black carbon (BC) is notably amplified in the Arctic by its deposition that causes albedo decrease and subsequent earlier snow and ice spring melt. To comprehensively assess the climate impact of BC in the Arctic, information on both atmospheric BC concentrations and deposition are essential. Currently, Arctic BC deposition data are very scarce, while atmospheric BC concentrations have been shown to generally decrease since the 1990s. However, a 300-year Svalbard ice core showed a distinct increase in EC (elemental carbon, proxy for BC) deposition from 1970 to 2004 contradicting atmospheric measurements and modelling studies. Here, our objective was to decipher whether this increase has continued in the 21st century, and to investigate the drivers of the observed EC deposition trends. For this, a shallow firn core was collected from the same Svalbard glacier, and a regional-to-meso-scale chemical transport model (SILAM) was run from 1980 to 2015. The ice and firn core data indicate peaking EC deposition values at the end of the 1990s, and lower values thereafter. The modelled BC deposition results generally support the observed glacier EC variations. However, the ice and firn core results clearly deviate from both measured and modelled atmospheric BC concentration trends, and the modelled BC deposition trend shows variations seemingly independent from BC emission or atmospheric BC concentration trends. Furthermore, ca. 99 % BC mass is wet-deposited at this Svalbard glacier, indicating that meteorological processes such as precipitation and scavenging efficiency have most likely a stronger influence on the BC deposition trend than BC emission or atmospheric concentration trends. BC emission source sectors contribute differently to the modelled atmospheric BC concentrations and BC deposition, which further supports our conclusion that different processes affect atmospheric BC concentration and deposition trends. Consequently, Arctic BC deposition trends should not directly be inferred based on atmospheric BC measurements, and more observational BC deposition data are required to assess the climate impact of BC in Arctic snow.


2021 ◽  
Author(s):  
Ramina Alwarda ◽  
Kristof Bognar ◽  
Kimberly Strong ◽  
Martyn Chipperfield ◽  
Sandip Dhomse ◽  
...  

&lt;p&gt;The Arctic winter of 2019-2020 was characterized by an unusually persistent polar vortex and temperatures in the lower stratosphere that were consistently below the threshold for the formation of polar stratospheric clouds (PSCs). These conditions led to ozone loss that is comparable to the Antarctic ozone hole. Ground-based measurements from a suite of instruments at the Polar Environment Atmospheric Research Laboratory (PEARL) in Eureka, Canada (80.05&amp;#176;N, 86.42&amp;#176;W) were used to investigate chemical ozone depletion. The vortex was located above Eureka longer than in any previous year in the 20-year dataset and lidar measurements provided evidence of polar stratospheric clouds (PSCs) above Eureka. Additionally, UV-visible zenith-sky Differential Optical Absorption Spectroscopy (DOAS) measurements showed record ozone loss in the 20-year dataset, evidence of denitrification along with the slowest increase of NO&lt;sub&gt;2&lt;/sub&gt; during spring, as well as enhanced reactive halogen species (OClO and BrO). Complementary measurements of HCl and ClONO&lt;sub&gt;2&lt;/sub&gt; (chlorine reservoir species) from a Fourier transform infrared (FTIR) spectrometer showed unusually low columns that were comparable to 2011, the previous year with significant chemical ozone depletion. Record low values of HNO&lt;sub&gt;3&lt;/sub&gt; in the FTIR dataset are in accordance with the evidence of PSCs and a denitrified atmosphere. Estimates of chemical ozone loss were derived using passive ozone from the SLIMCAT offline chemical transport model to account for dynamical contributions to the stratospheric ozone budget.&lt;/p&gt;


2012 ◽  
Vol 12 (15) ◽  
pp. 7073-7085 ◽  
Author(s):  
J. Kuttippurath ◽  
S. Godin-Beekmann ◽  
F. Lefèvre ◽  
G. Nikulin ◽  
M. L. Santee ◽  
...  

Abstract. We present a detailed discussion of the chemical and dynamical processes in the Arctic winters 1996/1997 and 2010/2011 with high resolution chemical transport model (CTM) simulations and space-based observations. In the Arctic winter 2010/2011, the lower stratospheric minimum temperatures were below 195 K for a record period of time, from December to mid-April, and a strong and stable vortex was present during that period. Simulations with the Mimosa-Chim CTM show that the chemical ozone loss started in early January and progressed slowly to 1 ppmv (parts per million by volume) by late February. The loss intensified by early March and reached a record maximum of ~2.4 ppmv in the late March–early April period over a broad altitude range of 450–550 K. This coincides with elevated ozone loss rates of 2–4 ppbv sh−1 (parts per billion by volume/sunlit hour) and a contribution of about 30–55% and 30–35% from the ClO-ClO and ClO-BrO cycles, respectively, in late February and March. In addition, a contribution of 30–50% from the HOx cycle is also estimated in April. We also estimate a loss of about 0.7–1.2 ppmv contributed (75%) by the NOx cycle at 550–700 K. The ozone loss estimated in the partial column range of 350–550 K exhibits a record value of ~148 DU (Dobson Unit). This is the largest ozone loss ever estimated in the Arctic and is consistent with the remarkable chlorine activation and strong denitrification (40–50%) during the winter, as the modeled ClO shows ~1.8 ppbv in early January and ~1 ppbv in March at 450–550 K. These model results are in excellent agreement with those found from the Aura Microwave Limb Sounder observations. Our analyses also show that the ozone loss in 2010/2011 is close to that found in some Antarctic winters, for the first time in the observed history. Though the winter 1996/1997 was also very cold in March–April, the temperatures were higher in December–February, and, therefore, chlorine activation was moderate and ozone loss was average with about 1.2 ppmv at 475–550 K or 42 DU at 350–550 K, as diagnosed from the model simulations and measurements.


2013 ◽  
Vol 13 (11) ◽  
pp. 31079-31125 ◽  
Author(s):  
J. Sedlar ◽  
M. D. Shupe

Abstract. Over the Arctic Ocean, little is known, observationally, on cloud-generated buoyant overturning vertical motions within mixed-phase stratocumulus clouds. Characteristics of such motions are important for understanding the diabatic processes associated with the vertical motions, the lifetime of the cloud layer and its micro- and macrophysical characteristics. In this study, we exploit a suite of surface-based remote sensors over the high Arctic sea ice during a week-long period of persistent stratocumulus in August 2008 to derive the in-cloud vertical motion characteristics. In-cloud vertical velocity skewness and variance profiles are found to be strikingly different from observations within lower-latiatude stratocumulus, suggesting these Arctic mixed-phase clouds interact differently with the atmospheric thermodynamics (cloud tops extending above a stable temperature inversion base) and with a different coupling state between surface and cloud. We find evidence of cloud-generated vertical mixing below cloud base, regardless of surface-cloud coupling state, although a decoupled surface-cloud state occurred most frequently. Detailed case studies are examined focusing on 3 levels within the cloud layer, where wavelet and power spectral analyses are applied to characterize the dominant temporal and horizontal scales associated with cloud-generated vertical motions. In general, we find a positively-correlated vertical motion signal across the full cloud layer depth. The coherency is dependent upon other non-cloud controlled factors, such as larger, mesoscale weather passages and radiative shielding of low-level stratocumulus by multiple cloud layers above. Despite the coherency in vertical velocity across the cloud, the velocity variances were always weaker near cloud top, relative to cloud mid and base. Taken in combination with the skewness, variance and thermodynamic profile characteristics, we observe vertical motions near cloud-top that behave differently than those from lower within the cloud layer. Spectral analysis indicates peak cloud-generated w variance timescales slowed only modestly during decoupled cases relative to coupled; horizontal wavelengths only slightly increased when transitioning from coupling to decoupling. The similarities in scales suggests that perhaps the dominant forcing for all cases is generated from the cloud layer, and it is not the surface forcing that characterizes the time and space scales of in-cloud vertical velocity variance. This points toward the resilient nature of Arctic mixed-phase clouds to persist when characterized by thermodynamic regimes unique to the Arctic.


2013 ◽  
Vol 52 (5) ◽  
pp. 1277-1293 ◽  
Author(s):  
Greg M. McFarquhar ◽  
Junshik Um ◽  
Robert Jackson

AbstractThe shapes of cloud particles with maximum dimensions Dmax between 35 and 60 μm in mixed-phase clouds were studied using high-resolution particle images collected by a cloud particle imager (CPI) during the Mixed-Phase Arctic Cloud Experiment (M-PACE) and the Indirect and Semi-Direct Aerosol Campaign (ISDAC). The area ratio α, the projected area of a particle divided by the area of a circle with diameter Dmax, quantified particle shape. The differing optical characteristics of CPIs used in M-PACE and ISDAC had no effect on derived α provided that Dmax > 35 μm and CPI focus > 45. The fraction of particles with 35 < Dmax < 60 μm with α > 0.8 increased with the ratio of liquid water content (LWC) to total water content (TWC). The average αmean of small particles in each 10-s interval in mixed-phase clouds was correlated with LWC/TWC with a correlation coefficient of 0.60 for M-PACE and 0.43 for ISDAC. The stronger correlation seen during M-PACE was most likely associated with the presence of more liquid droplets that were larger than the CPI detection threshold contributing to αmean; the modal effective radius was larger (11 vs 6 μm), and drops with D > 35 μm had concentrations during M-PACE that were 6 times as large as those of ISDAC. This study hence suggests that area ratio can be used to identify the phase of particles with 35 < Dmax < 60 μm and questions the assumption used in previous studies that all particles in this size range are supercooled droplets.


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