scholarly journals Potential genesis and implications of calcium nitrate in Antarctic snow

2016 ◽  
Vol 10 (2) ◽  
pp. 825-836 ◽  
Author(s):  
Kanthanathan Mahalinganathan ◽  
Meloth Thamban

Abstract. Among the large variety of particulates in the atmosphere, calcic mineral dust particles have highly reactive surfaces that undergo heterogeneous reactions with atmospheric acids contiguously. The association between nssCa2+, an important proxy indicator of mineral dust, and NO3−, a dominant anion in the Antarctic snowpack, was analysed. A total of 41 snow cores ( ∼  1 m each) that represent snow deposited during 2008–2009 were studied along coastal–inland transects from two different regions in East Antarctica – the Princess Elizabeth Land (PEL) and central Dronning Maud Land (cDML). Correlation statistics showed a strong association (at 99 % significance level) between NO3− and nssCa2+ at the near-coastal sections of both PEL (r  =  0.74) and cDML (r  =  0.82) transects. Similarly, a strong association between these ions was also observed in snow deposits at the inland sections of PEL (r  =  0.73) and cDML (r  =  0.84). Such systematic associations between nssCa2+ and NO3− are attributed to the interaction between calcic mineral dust and nitric acid in the atmosphere, leading to the formation of calcium nitrate (Ca(NO3)2) aerosol. Principal component analysis revealed common transport and depositional processes for nssCa2+ and NO3− both in PEL and cDML. Forward- and back-trajectory analyses using HYSPLIT model v. 4 revealed that southern South America (SSA) was an important dust-emitting source to the study region, aided by the westerlies. Particle size distribution showed that over 90 % of the dust was in the range  <  4 µm, indicating that these dust particles reached the Antarctic region via long-range transport from the SSA region. We propose that the association between nssCa2+ and NO3− occurs during the long-range transport due to the formation of Ca(NO3)2 rather than to local neutralisation processes. However, the influence of local dust sources from the nunataks in cDML and the contribution of high sea salt in coastal PEL evidently mask such association in the mountainous and coastal regions respectively. Ionic balance calculations showed that 70–75 % of NO3− in the coastal sections was associated with nssCa2+ (to form Ca(NO3)2). However, in the inland sections, 50–55 % of NO3− was present as HNO3. The study indicates that the input of dust-bound NO3− contributes a significant fraction of the total NO3− deposited in coastal Antarctic snow.

2015 ◽  
Vol 9 (6) ◽  
pp. 6125-6151
Author(s):  
K. Mahalinganathan ◽  
M. Thamban

Abstract. Among the large variety of particulates in the atmosphere, calcic mineral dust particles have highly reactive surfaces that undergo heterogeneous reactions with nitrogen oxides contiguously. The association between Ca2+, an important proxy indicator of mineral dust and NO3–, a dominant anion in the Antarctic snow pack was analysed. A total of 41 snow cores (~ 1 m each) that represent snow deposited during 2008–2009 were studied along coastal–inland transects from two different regions – the Princess Elizabeth Land (PEL) and central Dronning Maud Land (cDML) in East Antarctica. Correlation statistics showed a strong association (at 99 % significance level) between NO3– and Ca2+ at the near-coastal sections of both PEL (r = 0.72) and cDML (r = 0.76) transects. Similarly, a strong association between these ions was also observed in snow deposits at the inland sections of PEL (r = 0.8) and cDML (r = 0.85). Such systematic associations between Ca2+ and NO3– is attributed to the interaction between calcic mineral dust and nitrogen oxides in the atmosphere, leading to the possible formation of calcium nitrate (Ca(NO3)2). Forward and back trajectory analyses using HYSPLIT model v. 4 revealed that Southern South America (SSA) was an important dust emitting source to the study region, aided by the westerlies. Particle size distribution showed that over 90 % of the dust was in the range < 4 μm, indicating that these dust particles reached the Antarctic region via long range transport from the SSA region. We propose that the association between Ca2+ and NO3– occurs during the long range transport due to the formation of Ca(NO3)2. The Ca(NO3)2 thus formed in the atmosphere undergo deposition over Antarctica under the influence of anticyclonic polar easterlies. However, influence of local dust sources from the nunataks in cDML evidently mask such association in the mountainous region. The study indicates that the input of dust-bound NO3– may contribute a significant fraction of the total NO3– deposited in Antarctic snow.


2018 ◽  
Vol 18 (8) ◽  
pp. 5371-5389 ◽  
Author(s):  
Silvia Bucci ◽  
Paolo Cristofanelli ◽  
Stefano Decesari ◽  
Angela Marinoni ◽  
Silvia Sandrini ◽  
...  

Abstract. Studying the vertical distribution of aerosol particle physical and chemical properties in the troposphere is essential to understand the relative importance of local emission processes vs. long-range transport for column-integrated aerosol properties (e.g. the aerosol optical depth, AOD, affecting regional climate) as well as for the aerosol burden and its impacts on air quality at the ground. The main objective of this paper is to investigate the transport of desert dust in the middle troposphere and its intrusion into the planetary boundary layer (PBL) over the Po Valley (Italy), a region considered one of the greatest European pollution hotspots for the frequency that particulate matter (PM) limit values are exceeded. Events of mineral aerosol uplift from local (soil) sources and phenomena of hygroscopic growth at the ground are also investigated, possibly affecting the PM concentration in the region as well. During the PEGASOS 2012 field campaign, an integrated observing–modelling system was set up based on near-surface measurements (particle concentration and chemistry), vertical profiling (backscatter coefficient profiles from lidar and radiosoundings) and Lagrangian air mass transport simulations by FLEXPART model. Measurements were taken at the San Pietro Capofiume supersite (44°39′ N, 11°37′ E; 11 m a.s.l.), located in a rural area relatively close to some major urban and industrial emissive areas in the Po Valley. Mt. Cimone (44°12′ N, 10°42′ E; 2165 m a.s.l.) WMO/GAW station observations are also included in the study to characterize regional-scale variability. Results show that, in the Po Valley, aerosol is detected mainly below 2000 m a.s.l. with a prevalent occurrence of non-depolarizing particles ( > 50 % throughout the campaign) and a vertical distribution modulated by the PBL daily evolution. Two intense events of mineral dust transport from northern Africa (19–21 and 29 June to 2 July) are observed, with layers advected mainly above 2000 m, but subsequently sinking and mixing in the PBL. As a consequence, a non-negligible occurrence of mineral dust is observed close to the ground ( ∼ 7 % of occurrence during a 1-month campaign). The observations unambiguously show Saharan dust layers intruding the Po Valley mixing layer and directly affecting the aerosol concentrations near the surface. Finally, lidar observations also indicate strong variability in aerosol on shorter timescales (hourly). Firstly, these highlight events of hygroscopic growth of anthropogenic aerosol, visible as shallow layers of low depolarization near the ground. Such events are identified during early morning hours at high relative humidity (RH) conditions (RH  > 80 %). The process is observed concurrently with high PM1 nitrate concentration (up to 15 µg cm−3) and hence mainly explicable by deliquescence of fine anthropogenic particles, and during mineral dust intrusion episodes, when water condensation on dust particles could instead represent the dominant contribution. Secondly, lidar images show frequent events (mean daily occurrence of  ∼  22 % during the whole campaign) of rapid uplift of mineral depolarizing particles in afternoon–evening hours up to 2000 m a.s.l. height. The origin of such particles cannot be directly related to long-range transport events, being instead likely linked to processes of soil particle resuspension from agricultural lands.


2017 ◽  
Author(s):  
Silvia Bucci ◽  
Paolo Cristofanelli ◽  
Stefano Decesari ◽  
Angela Marinoni ◽  
Silvia Sandrini ◽  
...  

Abstract. Studying the vertical distribution of aerosol particles physical and chemical properties in the troposphere is essential to understand the relative importance of local emissions processes vs. long-range transport on column-integrated aerosol properties (e.g. the aerosol optical depth (AOD), affecting regional climate) as well as on the aerosol burden and its impacts on air quality at the ground. The main objective of this paper is to investigate the transport of desert dust in the middle troposphere and its intrusion into the planetary boundary layer (PBL) over the Po Valley (Italy), a region considered one of the major European pollution hot-spots for the frequency of particulate matter (PM) limit values exceedances. Events of mineral aerosol uplift from local (soil) sources and phenomena of hygroscopic growth at the ground are also investigated, possibly affecting the PM concentration in the region as well. During the PEGASOS 2012 field campaign, an integrated observing-modeling system was set up based on near-surface measurements (particle concentration and chemistry), vertical profiling (backscatter coefficient profiles from LiDAR and radiosoundings) and Lagrangian air masses transport simulations by FLEXPART model. Measurements were taken at the San Pietro Capofiume supersite (44°39' N, 11°37'0 E, 11 m a.s.l.), located in a rural area relatively close to some major urban and industrial emissive areas in the Po Valley. Mt. Cimone (44°12' N, 10°42' E, 2165 m a.s.l.) WMO/GAW station observations are also included in the study to characterize regional-scale variability. Results show that, in the Po Valley, aerosol is detected mainly below 2000 m a.s.l. with a prevalent occurrence of non-depolarizing particles (>50 % throughout the campaign) and a vertical distribution modulated by the PBL daily evolution. Two intense events of mineral dust transport from Northern Africa (19–21 June and 29 June to 2 July) are observed, with layers advected mainly above 2000 m height, but lately sinking and mixing in the PBL. As a consequence, a non-negligible occurrence of mineral dust is observed close to the ground (∼7 % of occurrence during a 1-month campaign). The observations unambiguously show Saharan dust layers intruding the Po Valley summertime mixing layer and directly affecting the aerosol concentrations near the surface. Finally, LiDAR observations indicate also strong variability in aerosol on shorter timescales (hourly) highlighting: a) events of hygroscopic growth of anthropogenic aerosol, visible in shallow layers of low depolarization near the ground. Such events are identified during early morning hours at high relative humidity (RH) conditions (RH > 80 %). The process is observed concurrently with high PM1 nitrate concentration (up to 15 µg cm−3), hence mainly explicable by deliquescence of fine anthropogenic particles, and during mineral dust intrusion episodes, when water condensation on dust particles could instead represent the dominant contribution; b) frequent events (mean diurnal occurrence of ∼22 % during the whole campaign) of rapid uplift of mineral depolarizing particles in afternoon-evening hours up to 2000 m a.s.l. height. The origin of such particles cannot be directly related to long-range transport events, being instead likely linked to processes of soil particles resuspension from agricultural lands.


2018 ◽  
Author(s):  
Xue Wu ◽  
Sabine Griessbach ◽  
Lars Hoffmann

Abstract. Volcanic sulfate aerosol is an important source of sulfur for Antarctica where other local sources of sulfur are rare. Mid- and high latitude volcanic eruptions can directly influence the aerosol budget of the polar stratosphere. However, tropical eruptions can also enhance polar aerosol load following long-range transport. In the present work, we analyze the volcanic plume of a tropical eruption, Mount Merapi in October 2010, using the Lagrangian particle dispersion model Massive-Parallel Trajectory Calculations (MPTRAC), Atmospheric Infrared Sounder (AIRS) SO2 observations and Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) aerosol observations. We investigate the pathway and transport efficiency of the volcanic aerosol from the tropical tropopause layer (TTL) to the lower stratosphere over Antarctica. We first estimated the time- and height-resolved SO2 injection time series over Mount Merapi during the explosive eruption using the AIRS SO2 observations and a backward trajectory approach. Then the SO2 injections were tracked for up to 6 months using the MPTRAC model. The Lagrangian transport simulation of the volcanic plume was compared to MIPAS aerosol observations and showed good agreement. Both of the simulation and the observations presented in this study suggest that a significant amount of aerosols of the volcanic plume from the Merapi eruption was transported from the tropics to the south of 60 °S within one month after the eruption and even further to Antarctica in the following two months. This relatively fast meridional transport of volcanic aerosol was mainly driven by quasi-horizontal mixing from the TTL to the extratropical lower stratosphere, which was facilitated by the weakening of the subtropical jet during the seasonal transition from austral spring to summer and linked to the westerly phase of the quasi-biennial oscillation (QBO). When the plume went to southern high latitudes, the polar vortex was displaced from the south pole, so the volcanic plume was carried to the south pole without penetrating the polar vortex. Based on the model results, the most efficient pathway for the quasi-horizontal mixing was in between the isentropic surfaces of 360 and 430 K. Although only 4 % of the initial SO2 load was transported into the lower stratosphere south of 60 °S, the Merapi eruption contributed about 8800 tons of sulfur to the Antarctic lower stratosphere. This indicates that the long-range transport under favorable meteorological conditions enables tropical volcanic eruptions to be an important remote source of sulfur for the Antarctic stratosphere.


2018 ◽  
Author(s):  
Jonathan P. D. Abbatt ◽  
W. Richard Leaitch ◽  
Amir A. Aliabadi ◽  
Alan K. Bertram ◽  
Jean-Pierre Blanchet ◽  
...  

Abstract. Motivated by the need to predict how the Arctic atmosphere will change in a warming world, this article summarizes recent advances made by the research consortium NETCARE (Network on Climate and Aerosols: Addressing Key Uncertainties in Remote Canadian Environments) that contribute to our fundamental understanding of Arctic aerosol particles as they relate to climate forcing. The overall goal of NETCARE research has been to use an interdisciplinary approach encompassing extensive field observations and a range of chemical transport, earth system, and biogeochemical models. Several major findings and advances have emerged from NETCARE since its formation in 2013 . (1) Unexpectedly high summertime dimethyl sulfide (DMS) levels were identified in ocean water and the overlying atmosphere in the Canadian Arctic Archipelago (CAA). Furthermore, melt ponds, which are widely prevalent, were identified as an important DMS source. (2) Evidence was found of widespread particle nucleation and growth in the marine boundary layer in the CAA in the summertime. DMS-oxidation-driven nucleation is facilitated by the presence of atmospheric ammonia arising from sea bird colony emissions, and potentially also from coastal regions, tundra, and biomass burning. Via accumulation of secondary organic material (SOA), a significant fraction of the new particles grow to sizes that are active in cloud droplet formation. Although the gaseous precursors to Arctic marine SOA remain poorly defined, the measured levels of common continental SOA precursors (isoprene and monoterpenes) were low, whereas elevated mixing ratios of oxygenated volatile organic compounds were inferred to arise via processes involving the sea surface microlayer. (3) The variability in the vertical distribution of black carbon (BC) under both springtime Arctic haze and more pristine summertime aerosol conditions was observed. Measured particle size distributions and mixing states were used to constrain, for the first time, calculations of aerosol–climate interactions under Arctic conditions. Aircraft- and ground-based measurements were used to better establish the BC source regions that supply the Arctic via long-range transport mechanisms. (4) Measurements of ice nucleating particles (INPs) in the Arctic indicate that a major source of these particles is mineral dust, likely derived from local sources in the summer and long-range transport in the spring. In addition, INPs are abundant in the sea surface microlayer in the Arctic, and possibly play a role in ice nucleation in the atmosphere when mineral dust concentrations are low. (5) Amongst multiple aerosol components, BC was observed to have the smallest effective deposition velocities to high Arctic snow.


2019 ◽  
Vol 19 (4) ◽  
pp. 2527-2560 ◽  
Author(s):  
Jonathan P. D. Abbatt ◽  
W. Richard Leaitch ◽  
Amir A. Aliabadi ◽  
Allan K. Bertram ◽  
Jean-Pierre Blanchet ◽  
...  

Abstract. Motivated by the need to predict how the Arctic atmosphere will change in a warming world, this article summarizes recent advances made by the research consortium NETCARE (Network on Climate and Aerosols: Addressing Key Uncertainties in Remote Canadian Environments) that contribute to our fundamental understanding of Arctic aerosol particles as they relate to climate forcing. The overall goal of NETCARE research has been to use an interdisciplinary approach encompassing extensive field observations and a range of chemical transport, earth system, and biogeochemical models. Several major findings and advances have emerged from NETCARE since its formation in 2013. (1) Unexpectedly high summertime dimethyl sulfide (DMS) levels were identified in ocean water (up to 75 nM) and the overlying atmosphere (up to 1 ppbv) in the Canadian Arctic Archipelago (CAA). Furthermore, melt ponds, which are widely prevalent, were identified as an important DMS source (with DMS concentrations of up to 6 nM and a potential contribution to atmospheric DMS of 20 % in the study area). (2) Evidence of widespread particle nucleation and growth in the marine boundary layer was found in the CAA in the summertime, with these events observed on 41 % of days in a 2016 cruise. As well, at Alert, Nunavut, particles that are newly formed and grown under conditions of minimal anthropogenic influence during the months of July and August are estimated to contribute 20 % to 80 % of the 30–50 nm particle number density. DMS-oxidation-driven nucleation is facilitated by the presence of atmospheric ammonia arising from seabird-colony emissions, and potentially also from coastal regions, tundra, and biomass burning. Via accumulation of secondary organic aerosol (SOA), a significant fraction of the new particles grow to sizes that are active in cloud droplet formation. Although the gaseous precursors to Arctic marine SOA remain poorly defined, the measured levels of common continental SOA precursors (isoprene and monoterpenes) were low, whereas elevated mixing ratios of oxygenated volatile organic compounds (OVOCs) were inferred to arise via processes involving the sea surface microlayer. (3) The variability in the vertical distribution of black carbon (BC) under both springtime Arctic haze and more pristine summertime aerosol conditions was observed. Measured particle size distributions and mixing states were used to constrain, for the first time, calculations of aerosol–climate interactions under Arctic conditions. Aircraft- and ground-based measurements were used to better establish the BC source regions that supply the Arctic via long-range transport mechanisms, with evidence for a dominant springtime contribution from eastern and southern Asia to the middle troposphere, and a major contribution from northern Asia to the surface. (4) Measurements of ice nucleating particles (INPs) in the Arctic indicate that a major source of these particles is mineral dust, likely derived from local sources in the summer and long-range transport in the spring. In addition, INPs are abundant in the sea surface microlayer in the Arctic, and possibly play a role in ice nucleation in the atmosphere when mineral dust concentrations are low. (5) Amongst multiple aerosol components, BC was observed to have the smallest effective deposition velocities to high Arctic snow (0.03 cm s−1).


2016 ◽  
Author(s):  
Leonardo A. Mingari ◽  
Estela A. Collini ◽  
Arnau Folch ◽  
Walter Báez ◽  
Emilce Bustos ◽  
...  

Abstract. On the 13 June 2015, the London Volcanic Ash Advisory Centre (VAAC) warned the Buenos Aires VAAC about a possible volcanic eruption from the Nevados Ojos del Salado volcano (6879 m), located in the Andes mountain range on the border between Chile and Argentina. A volcanic ash cloud was detected by the SEVIRI instrument on board the Meteosat Second Generation (MSG) satellites from 14:00 UTC on 13 June. Further studies concluded that the phenomenon was caused by remobilization of ancient pyroclastic deposits (circa 4.5 Ka Cerro Blanco eruption) from the Bolsón de Fiambalá (Fiambalá Basin) in northwestern Argentina. In this paper, we provide the first comprehensive description of the dust episode through observations and numerical simulations. We have investigated the spatio-temporal distribution of aerosols and the emission process over complex terrain to gain insight into the key role played by the orography and the condition that triggered the long-range transport episode. Numerical simulations of windblown dust were performed using the WRF-ARW/FALL3D modeling system with meteorological fields downscaled to a spatial resolution of 2 km in order to resolve the complex orography of the area. Results indicated that favourable conditions to generate dust uplifting occurred in northern Fiambalá Basin, where orographic effects caused strong surface winds. According to short-range numerical simulations, dust particles were confined to near-ground layers around the emission areas. On the other hand, dust aerosols were injected up to 5–6 km high in central and southern regions of the Fiambalá Basin, where intense ascending airflows are driven by horizontal convergence. Long-range transport numerical simulations were also performed to model dust cloud spreading over northern Argentina. Results of simulated vertical particle column mass were compared with the MSG-SEVIRI retrieval product. We tested two numerical schemes: with the default configuration of the FALL3D model, we found difficulties to simulate transport through orographic barriers, whereas an alternative configuration, using a numerical scheme to more accurately compute the horizontal advection in abrupt terrains, substantially improved the model performance.


2020 ◽  
Author(s):  
Stefanos Samaras ◽  
Christine Böckmann ◽  
Moritz Haarig ◽  
Albert Ansmann ◽  
Adrian Walser ◽  
...  

Abstract. Saharan dust is a major natural atmospheric aerosol component with significant impact on the Earth radiation budget. In this work we determine the microphysical properties of dust particles after a long-range transport over the Atlantic Ocean, using input from three depolarization channels of a multi-wavelength polarization Raman lidar. The measurements were performed at Barbados in the framework of the Saharan Aerosol Long-Range Transport and Aerosol–Cloud-Interaction Experiment (SALTRACE) in the summers of 2013 and 2014. The microphysical retrievals are performed with the software tool SphInX (Spheroidal Inversion Experiments) which uses regularization for the inversion process and a new two-dimensional (2-D) extension of the Mie model approximating dust with spheroids. The method allows us to simultaneously retrieve shape- and size-dependent particle distributions. Because dust particles are mostly non-spherical this software tool fills the gap in estimating the non-spherical particle fraction. Two cases measured on 10 July 2013 and 20 June 2014 are discussed. 2-D radius-bimodal shape-size distribution are retrieved. The ratio of spherical-to-non-spherical contributions to the particle number concentration was found to be about 3/7. A volume-weighted effective aspect ratio of 1.1 was obtained, indicating slightly prolate particles. The total effective radius for the two cases in the preselected radius range from 0.01–2.2 μm was found to be, on average, 0.75 μm. The stronger dust event (10 July 2013) showed about 24 % higher values for the total surface-area and volume concentration. Finally, we compare our results with the ones from the polarization lidar-photometer networking (POLIPHON) method and ground-based photometers as well as with airborne in situ particle counters. Considering all differences in these independent approaches, we find a qualitatively good agreement between the different results and a consistent description of the dust cases. Such an extensive comparison is a novel and fruitful exercise and corroborates that the mathematical retrieval based on Raman lidar data of particle backscattering, extinction, and depolarization is a powerful tool even in the case of dust particles.


2020 ◽  
Vol 20 (16) ◽  
pp. 10047-10062 ◽  
Author(s):  
Samantha J. Kramer ◽  
Claudia Alvarez ◽  
Anne E. Barkley ◽  
Peter R. Colarco ◽  
Lillian Custals ◽  
...  

Abstract. North African dust reaches the southeastern United States every summer. Size-resolved dust mass measurements taken in Miami, Florida, indicate that more than one-half of the surface dust mass concentrations reside in particles with geometric diameters less than 2.1 µm, while vertical profiles of micropulse lidar depolarization ratios show dust reaching above 4 km during pronounced events. These observations are compared to the representation of dust in the Modern-Era Retrospective analysis for Research and Applications, version 2 (MERRA-2) aerosol reanalysis and closely related Goddard Earth Observing System model version 5 (GEOS-5) Forward Processing (FP) aerosol product, both of which assimilate satellite-derived aerosol optical depths using a similar protocol and inputs. These capture the day-to-day variability in aerosol optical depth well, in a comparison to an independent sun-photometer-derived aerosol optical depth dataset. Most of the modeled dust mass resides in diameters between 2 and 6 µm, in contrast to the measurements. Model-specified mass extinction efficiencies equate light extinction with approximately 3 times as much aerosol mass, in this size range, compared to the measured dust sizes. GEOS-5 FP surface-layer sea salt mass concentrations greatly exceed observed values, despite realistic winds and relative humidities. In combination, these observations help explain why, despite realistic total aerosol optical depths, (1) free-tropospheric model volume extinction coefficients are lower than those retrieved from the micro-pulse lidar, suggesting too-low model dust loadings in the free troposphere, and (2) model dust mass concentrations near the surface can be higher than those measured. The modeled vertical distribution of dust, when captured, is reasonable. Large, aspherical particles exceeding the modeled dust sizes are also occasionally present, but dust particles with diameters exceeding 10 µm contribute little to the measured total dust mass concentrations after such long-range transport. Remaining uncertainties warrant a further integrated assessment to confirm this study's interpretations.


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