scholarly journals Aircraft-based measurements of High Arctic springtime aerosol show evidence for vertically varying sources, transport and composition

2019 ◽  
Vol 19 (1) ◽  
pp. 57-76 ◽  
Author(s):  
Megan D. Willis ◽  
Heiko Bozem ◽  
Daniel Kunkel ◽  
Alex K. Y. Lee ◽  
Hannes Schulz ◽  
...  

Abstract. The sources, chemical transformations and removal mechanisms of aerosol transported to the Arctic are key factors that control Arctic aerosol–climate interactions. Our understanding of sources and processes is limited by a lack of vertically resolved observations in remote Arctic regions. We present vertically resolved observations of trace gases and aerosol composition in High Arctic springtime, made largely north of 80∘ N, during the NETCARE campaign. Trace gas gradients observed on these flights defined the polar dome as north of 66–68∘ 30′ N and below potential temperatures of 283.5–287.5 K. In the polar dome, we observe evidence for vertically varying source regions and chemical processing. These vertical changes in sources and chemistry lead to systematic variation in aerosol composition as a function of potential temperature. We show evidence for sources of aerosol with higher organic aerosol (OA), ammonium and refractory black carbon (rBC) content in the upper polar dome. Based on FLEXPART-ECMWF calculations, air masses sampled at all levels inside the polar dome (i.e., potential temperature <280.5 K, altitude <∼3.5 km) subsided during transport over transport times of at least 10 days. Air masses at the lowest potential temperatures, in the lower polar dome, had spent long periods (>10 days) in the Arctic, while air masses in the upper polar dome had entered the Arctic more recently. Variations in aerosol composition were closely related to transport history. In the lower polar dome, the measured sub-micron aerosol mass was dominated by sulfate (mean 74 %), with lower contributions from rBC (1 %), ammonium (4 %) and OA (20 %). At higher altitudes and higher potential temperatures, OA, ammonium and rBC contributed 42 %, 8 % and 2 % of aerosol mass, respectively. A qualitative indication for the presence of sea salt showed that sodium chloride contributed to sub-micron aerosol in the lower polar dome, but was not detectable in the upper polar dome. Our observations highlight the differences in Arctic aerosol chemistry observed at surface-based sites and the aerosol transported throughout the depth of the Arctic troposphere in spring.

2018 ◽  
Author(s):  
Megan D. Willis ◽  
Heiko Bozem ◽  
Daniel Kunkel ◽  
Alex K. Y. Lee ◽  
Hannes Schulz ◽  
...  

Abstract. The sources, chemical transformations and removal mechanisms of aerosol transported to the Arctic are key factors that control Arctic aerosol-climate interactions. Our understanding of sources and processes is limited by a lack of vertically resolved observations in remote Arctic regions. We present vertically resolved observations of trace gases and aerosol composition in High Arctic springtime, made largely north of 80° N, during the NETCARE campaign. Trace gas gradients observed on these flights defined the polar dome as north of 66–68.5° N and below potential temperatures of 283.5–287.5 K (Bozem et al., 2018). In the polar dome, we observe evidence for vertically varying source regions and chemical processing. These vertical changes in sources and chemistry lead to systematic variation in aerosol composition as a function of potential temperature. We show evidence for sources of aerosol with higher organic aerosol (OA), ammonium (NH4) and refractory black carbon (rBC) content in the upper polar dome. Based on FLEXPART-ECMWF calculations, air masses sampled at all levels inside the polar dome (i.e., potential temperature


2019 ◽  
Vol 19 (23) ◽  
pp. 15049-15071
Author(s):  
Heiko Bozem ◽  
Peter Hoor ◽  
Daniel Kunkel ◽  
Franziska Köllner ◽  
Johannes Schneider ◽  
...  

Abstract. The springtime composition of the Arctic lower troposphere is to a large extent controlled by the transport of midlatitude air masses into the Arctic. In contrast, precipitation and natural sources play the most important role during summer. Within the Arctic region sloping isentropes create a barrier to horizontal transport, known as the polar dome. The polar dome varies in space and time and exhibits a strong influence on the transport of air masses from midlatitudes, enhancing transport during winter and inhibiting transport during summer. We analyzed aircraft-based trace gas measurements in the Arctic from two NETCARE airborne field campaigns (July 2014 and April 2015) with the Alfred Wegener Institute Polar 6 aircraft, covering an area from Spitsbergen to Alaska (134 to 17∘ W and 68 to 83∘ N). Using these data we characterized the transport regimes of midlatitude air masses traveling to the high Arctic based on CO and CO2 measurements as well as kinematic 10 d back trajectories. We found that dynamical isolation of the high Arctic lower troposphere leads to gradients of chemical tracers reflecting different local chemical lifetimes, sources, and sinks. In particular, gradients of CO and CO2 allowed for a trace-gas-based definition of the polar dome boundary for the two measurement periods, which showed pronounced seasonal differences. Rather than a sharp boundary, we derived a transition zone from both campaigns. In July 2014 the polar dome boundary was at 73.5∘ N latitude and 299–303.5 K potential temperature. During April 2015 the polar dome boundary was on average located at 66–68.5∘ N and 283.5–287.5 K. Tracer–tracer scatter plots confirm different air mass properties inside and outside the polar dome in both spring and summer. Further, we explored the processes controlling the recent transport history of air masses within and outside the polar dome. Air masses within the springtime polar dome mainly experienced diabatic cooling while traveling over cold surfaces. In contrast, air masses in the summertime polar dome were diabatically heated due to insolation. During both seasons air masses outside the polar dome slowly descended into the Arctic lower troposphere from above through radiative cooling. Ascent to the middle and upper troposphere mainly took place outside the Arctic, followed by a northward motion. Air masses inside and outside the polar dome were also distinguished by different chemical compositions of both trace gases and aerosol particles. We found that the fraction of amine-containing particles, originating from Arctic marine biogenic sources, is enhanced inside the polar dome. In contrast, concentrations of refractory black carbon are highest outside the polar dome, indicating remote pollution sources. Synoptic-scale weather systems frequently disturb the transport barrier formed by the polar dome and foster exchange between air masses from midlatitudes and polar regions. During the second phase of the NETCARE 2014 measurements a pronounced low-pressure system south of Resolute Bay brought inflow from southern latitudes, which pushed the polar dome northward and significantly affected trace gas mixing ratios in the measurement region. Mean CO mixing ratios increased from 77.9±2.5 to 84.9±4.7 ppbv between these two regimes. At the same time CO2 mixing ratios significantly decreased from 398.16 ± 1.01 to 393.81 ± 2.25 ppmv. Our results demonstrate the utility of applying a tracer-based diagnostic to determine the polar dome boundary for interpreting observations of atmospheric composition in the context of transport history.


2011 ◽  
Vol 11 (3) ◽  
pp. 8801-8840
Author(s):  
M. Martin ◽  
R. Y.-W. Chang ◽  
B. Sierau ◽  
S. Sjogren ◽  
E. Swietlicki ◽  
...  

Abstract. We present an aerosol – cloud condensation nuclei CCN) closure study on summer high Arctic aerosol based on measurements that were carried out in summer 2008 during the Arctic Summer Cloud Ocean Study (ASCOS) on board the Swedish ice breaker Oden. The data presented here were collected during a three-week time period in the pack ice (>85° N) when the icebreaker Oden was moored to an ice floe and drifted passively during the most biological active period into autumn freeze up conditions. CCN number concentrations were obtained using two CCN counters measuring at different supersaturations. The directly measured CCN number concentration is then compared with a CCN number concentration calculated using both bulk aerosol mass composition data from an aerosol mass spectrometer and aerosol number size distributions obtained from a differential mobility particle sizer, assuming κ-Köhler theory and an internally mixed aerosol. For the two highest measured supersaturations, 0.73 and 0.41%, closure could not be achieved with the investigated settings concerning hygroscopicity and density. The calculated CCN number concentration was always higher than the measured one. One possible explanation is that the smaller particles that activate at these supersaturations have a relative larger insoluble organic mass fraction and thus are less good CCN than the larger particles. At 0.20, 0.15 and 0.10% supersaturation, the measured CCN number can be represented with different parameters for the hygroscopicity and density of the particles. For the best agreement of the calculated CCNnumber concentration with the measured one the organic fraction of the aerosol needs to be nearly insoluble (қorg=0.02). However, this is not unambigious and қorg=0.2 is found as an upper limit at 0.1% supersaturation.


2019 ◽  
Author(s):  
Heiko Bozem ◽  
Peter Hoor ◽  
Daniel Kunkel ◽  
Franziska Köllner ◽  
Johannes Schneider ◽  
...  

Abstract. The springtime composition of the Arctic lower troposphere is to a large extent controlled by transport of mid-latitude air masses into the Arctic, whereas during the summer precipitation and natural sources play the most important role. Within the Arctic region, there exists a transport barrier, known as the polar dome, which results from sloping isentropes. The polar dome, which varies in space and time, exhibits a strong influence on the transport of air masses from mid-latitudes, enhancing it during winter and inhibiting it during summer. Furthermore, a definition for the location of the polar dome boundary itself is quite sparse in the literature. We analyzed aircraft based trace gas measurements in the Arctic during two NETCARE airborne field camapigns (July 2014 and April 2015) with the Polar 6 aircraft of Alfred Wegener Institute Helmholtz Center for Polar and Marine Research (AWI), Bremerhaven, Germany, covering an area from Spitsbergen to Alaska (134° W to 17° W and 68° N to 83° N). For the spring (April 2015) and summer (July 2014) season we analyzed transport regimes of mid-latitude air masses travelling to the high Arctic based on CO and CO2 measurements as well as kinematic 10-day back trajectories. The dynamical isolation of the high Arctic lower troposphere caused by the transport barrier leads to gradients of chemical tracers reflecting different local chemical life times and sources and sinks. Particularly gradients of CO and CO2 allowed for a trace gas based definition of the polar dome boundary for the two measurement periods with pronounced seasonal differences. For both campaigns a transition zone rather than a sharp boundary was derived. For July 2014 the polar dome boundary was determined to be 73.5° N latitude and 299–303.5 K potential temperature, respectively. During April 2015 the polar dome boundary was on average located at 66–68.5° N and 283.5–287.5 K. Tracer-tracer scatter plots and probability density functions confirm different air mass properties inside and outside of the polar dome for the July 2014 and April 2015 data set. Using the tracer derived polar dome boundaries the analysis of aerosol data indicates secondary aerosol formation events in the clean summertime polar dome. Synoptic-scale weather systems frequently disturb this transport barrier and foster exchange between air masses from midlatitudes and polar regions. During the second phase of the NETCARE 2014 measurements a pronounced low pressure system south of Resolute Bay brought inflow from southern latitudes that pushed the polar dome northward and significantly affected trace gas mixing ratios in the measurement region. Mean CO mixing ratios increased from 77.9 ± 2.5 ppbv to 84.9 ± 4.7 ppbv from the first period to the second period. At the same time CO2 mixing ratios significantly dropped from 398.16 ± 1.01 ppmv to 393.81 ± 2.25 ppmv. We further analysed processes controlling the recent transport history of air masses within and outside the polar dome. Air masses within the spring time polar dome mainly experienced diabatic cooling while travelling over cold surfaces. In contrast air masses in the summertime polar dome were diabatically heated due to insolation. During both seasons air masses outside the polar dome slowly descended into the Arctic lower troposphere from above caused by radiative cooling. The ascent to the middle and upper troposphere mainly took place outside the Arctic, followed by a northward motion. Our results demonstrate the successful application of a tracer based diagnostic to determine the location of the polar dome boundary.


2018 ◽  
Author(s):  
Rishabh U. Shah ◽  
Ellis S. Robinson ◽  
Peishi Gu ◽  
Allen Robinson ◽  
Joshua S. Apte ◽  
...  

Abstract. We investigated spatial and temporal patterns in concentration and composition of sub-micron particulate matter (PM1) in Oakland, California in the summer of 2017 using an aerosol mass spectrometer mounted in a mobile laboratory. We performed ∼ 160 hours of mobile sampling in the city over a 20-day period. Measurements are compared for three adjacent neighborhoods with distinct land uses: a central business district (downtown), a residential district (West Oakland), and a major shipping port. The average organic aerosol (OA) concentration is 5.3 μgm−3 and contributes ∼ 50 % of the PM1 mass. OA concentrations in downtown are, on average, 1.5 μgm−3 higher than in West Oakland and Port. We decomposed OA into three factors using positive matrix factorization: hydrocarbon-like OA (HOA; 20 % average contribution), cooking OA (COA; 25 %) and semi-volatile oxidized OA (SV-OOA; 55 %). The collective 45 % contribution from primary OA (HOA + COA) emphasizes the importance of primary emissions in Oakland. The dominant source of primary OA shifts from HOA-rich in the morning to COA-rich after lunch time. COA in downtown is consistently higher than West Oakland and Port due to a large number of restaurants. HOA exhibits variability in space and time. Morning-time HOA concentration in downtown is twice that in Port, but Port HOA increases more than two-fold during mid-day, likely because trucking activity at the Port peaks at that time. Despite the expectation of being spatially uniform, SV-OOA also exhibits spatial differences. Morning-time SV-OOA in downtown is roughly 25 % (∼ 0.6 μgm−3) higher than the rest of Oakland. Even as the entire domain approaches a more uniform photo-chemical state in the afternoon, downtown SV-OOA remains statistically higher than West Oakland and Port, suggesting that downtown is a microenvironment with higher photochemical activity. Higher concentrations of particulate sulfate (also of secondary origin) with no direct sources in Oakland further reflect higher photochemical activity in downtown. A combination of several factors (poor ventilation of air masses in street canyons, higher concentrations of precursor gases, higher concentrations of the hydroxyl radical) likely result in the proposed high photochemical activity in downtown. Lastly, through Van Krevelen analysis of elemental ratios (H/C, O/C) of the OA, we show that OA in Oakland is more chemically reduced than several other urban areas. This underscores the importance of primary emissions in Oakland. We also show that mixing of oceanic air masses with these primary emissions in Oakland is an important processing mechanism that governs the overall OA composition in Oakland. The findings of this study are important because the pollutants we find contributing the most to OA variability, both of primary and secondary origin, are ubiquitous in other urban locations.


2007 ◽  
Vol 7 (1) ◽  
pp. 107-119 ◽  
Author(s):  
A. Karpechko ◽  
A. Lukyanov ◽  
E. Kyrö ◽  
S. Khaikin ◽  
L. Korshunov ◽  
...  

Abstract. Balloon-borne water vapour measurements during January and February 2004, which were obtained as part of the LAUTLOS campaign at Sodankylä, Finland, 67° N, were used to analyse the water vapour distribution in the wintertime Arctic lowermost stratosphere. A 2.5 km thick layer (or 30 K in the potential temperature scale) above the tropopause is characterized by a significant water vapour variability on a synoptic timescale with values between stratospheric and tropospheric, which is in good agreement with previously reported measurements. A cross-correlation analysis of ozone and water vapour confirms that this layer contains a mixture of stratospheric and tropospheric air masses. Some of the flights sampled laminae of enhanced water vapour above the tropopause. Meteorological analyses and backward trajectory calculations show that these features were related to filaments that had developed along the flanks of cut-off anticyclones, which had been active at this time over the Northern Atlantic. The role of the filaments was however not to transport water vapour from the troposphere to the stratosphere but rather to transport it within the stratosphere away from regions where intensive two-way stratosphere-troposphere exchange (STE) was identified. Intensive STE occurred around cut-off anticyclones in regions of strong winds, where calculations suggest the presence of clear-air turbulence (CAT). Evidences that CAT contributes to the troposphere-to-stratosphere transport (TST) are presented. However, statistically, relation between TST and CAT during the studied period is weak.


2011 ◽  
Vol 11 (22) ◽  
pp. 11335-11350 ◽  
Author(s):  
M. Martin ◽  
R. Y.-W. Chang ◽  
B. Sierau ◽  
S. Sjogren ◽  
E. Swietlicki ◽  
...  

Abstract. We present an aerosol – cloud condensation nuclei (CCN) closure study on summer high Arctic aerosol based on measurements that were carried out in 2008 during the Arctic Summer Cloud Ocean Study (ASCOS) on board the Swedish ice breaker Oden. The data presented here were collected during a three-week time period in the pack ice (>85° N) when the icebreaker Oden was moored to an ice floe and drifted passively during the most biological active period into autumn freeze up conditions. CCN number concentrations were obtained using two CCN counters measuring at different supersaturations. The directly measured CCN number concentration was then compared with a CCN number concentration calculated using both bulk aerosol mass composition data from an aerosol mass spectrometer (AMS) and aerosol number size distributions obtained from a differential mobility particle sizer, assuming κ-Köhler theory, surface tension of water and an internally mixed aerosol. The last assumption was supported by measurements made with a hygroscopic tandem differential mobility analyzer (HTDMA) for particles >70 nm. For the two highest measured supersaturations, 0.73 and 0.41%, closure could not be achieved with the investigated settings concerning hygroscopicity and density. The calculated CCN number concentration was always higher than the measured one for those two supersaturations. This might be caused by a relative larger insoluble organic mass fraction of the smaller particles that activate at these supersaturations, which are thus less good CCN than the larger particles. On average, 36% of the mass measured with the AMS was organic mass. At 0.20, 0.15 and 0.10% supersaturation, closure could be achieved with different combinations of hygroscopic parameters and densities within the uncertainty range of the fit. The best agreement of the calculated CCN number concentration with the observed one was achieved when the organic fraction of the aerosol was treated as nearly water insoluble (κorg=0.02), leading to a mean total κ, κtot, of 0.33 ± 0.13. However, several settings led to closure and κorg=0.2 is found to be an upper limit at 0.1% supersaturation. κorg≤0.2 leads to a κtot range of 0.33 ± 013 to 0.50 ± 0.11. Thus, the organic material ranges from being sparingly soluble to effectively insoluble. These results suggest that an increase in organic mass fraction in particles of a certain size would lead to a suppression of the Arctic CCN activity.


2021 ◽  
Vol 21 (17) ◽  
pp. 13287-13309
Author(s):  
Jakob Boyd Pernov ◽  
Bjarne Jensen ◽  
Andreas Massling ◽  
Daniel Charles Thomas ◽  
Henrik Skov

Abstract. While much research has been devoted to the subject of gaseous elemental mercury (GEM) and gaseous oxidized mercury (GOM) in the Arctic spring during atmospheric mercury depletion events, few studies have examined the behavior of GOM in the High Arctic summer. GOM, once deposited and incorporated into the ecosystem, can pose a threat to human and wildlife health, though there remain large uncertainties regarding the transformation, deposition, and assimilation of mercury into the food web. Therefore, to further our understanding of the dynamics of GOM in the High Arctic during the late summer, we performed measurements of GEM and GOM, along with meteorological parameters and atmospheric constituents, and utilized modeled air mass history during two summer campaigns in 2019 and 2020 at Villum Research Station (Villum) in northeastern Greenland. Seven events of enhanced GOM concentrations were identified and investigated in greater detail. In general, the common factors associated with event periods at ground level were higher levels of radiation and lower H2O mixing ratios, accumulated precipitation, and relative humidity (RH), although none were connected with cold temperatures. Non-event periods at ground level each displayed a different pattern in one or more parameters when compared to event periods. Generally, air masses during event periods for both campaigns were colder and drier, arrived from higher altitudes, and spent more time above the mixed layer and less time in a cloud compared to non-events, although some events deviated from this general pattern. Non-event air masses displayed a different pattern in one or more parameters when compared to event periods, although they were generally warmer and wetter and arrived from lower altitudes with little radiation. Coarse-mode aerosols were hypothesized to provide the heterogenous surface for halogen propagation during some of the events, while for others the source is unknown. While these general patterns were observed for event and non-event periods, analysis of individual events showed more specific origins. Five of the seven events were associated with air masses that experienced similar conditions: transported from the cold, dry, and sunlit free troposphere. However, two events experienced contrasting conditions, with air masses being warm and wet with surface layer contact under little radiation. Two episodes of extremely high levels of NCoarse and BC, which appear to originate from flaring emissions in Russia, did not contribute to enhanced GOM levels. This work aims to provide a better understanding of the dynamics of GOM during the High Arctic summer.


2019 ◽  
Vol 12 (6) ◽  
pp. 3081-3099 ◽  
Author(s):  
Charles A. Brock ◽  
Christina Williamson ◽  
Agnieszka Kupc ◽  
Karl D. Froyd ◽  
Frank Erdesz ◽  
...  

Abstract. From 2016 to 2018 a DC-8 aircraft operated by the US National Aeronautics and Space Administration (NASA) made four series of flights, profiling the atmosphere from 180 m to ∼12 km above sea level (km a.s.l.) from the Arctic to the Antarctic over both the Pacific and Atlantic oceans. This program, the Atmospheric Tomography Mission (ATom), sought to sample the troposphere in a representative manner, making measurements of atmospheric composition in each season. This paper describes the aerosol microphysical measurements and derived quantities obtained during this mission. Dry size distributions from 2.7 nm to 4.8 µm in diameter were measured in situ at 1 Hz using a battery of instruments: 10 condensation particle counters with different nucleation diameters, two ultra-high-sensitivity aerosol size spectrometers (UHSASs), one of which measured particles surviving heating to 300 ∘C, and a laser aerosol spectrometer (LAS). The dry aerosol measurements were complemented by size distribution measurements from 0.5 to 930 µm diameter at near-ambient conditions using a cloud, aerosol, and precipitation spectrometer (CAPS) mounted under the wing of the DC-8. Dry aerosol number, surface area, and volume, and optical scattering and asymmetry parameters at several wavelengths from the near-UV to the near-IR ranges were calculated from the measured dry size distributions (2.7 nm to 4.8 µm). Dry aerosol mass was estimated by combining the size distribution data with particle density estimated from independent measurements of aerosol composition with a high-resolution aerosol mass spectrometer and a single-particle soot photometer. We describe the instrumentation and fully document the aircraft inlet and flow distribution system, the derivation of uncertainties, and the calculation of data products from combined size distributions. Comparisons between the instruments and direct measurements of some aerosol properties confirm that in-flight performance was consistent with calibrations and within stated uncertainties for the two deployments analyzed. The unique ATom dataset contains accurate, precise, high-resolution in situ measurements of dry aerosol size distributions, and integral parameters, and estimates and measurements of optical properties, for particles < 4.8 µm in diameter that can be used to evaluate aerosol abundance and processes in global models.


2020 ◽  
Author(s):  
Lukas Papritz

&lt;p align=&quot;justify&quot;&gt;Recent decades have revealed dramatic changes in the high Arctic (&gt; 80&amp;#176;N) related to natural variability and anthropogenic climate change. In particular, episodes of extremely warm temperatures in the lower troposphere and their role for sea ice melting have gained considerable attention. While it has been recognized that injections of warm and humid air masses contribute to wintertime warm anomalies, summertime warm anomalies have also been linked to blocking anticyclones within the high Arctic. Yet, the relative importance of the various thermodynamic and atmospheric dynamical processes that can contribute to the formation of extreme warm anomalies in the high Arctic is poorly understood.&lt;/p&gt;&lt;p align=&quot;justify&quot;&gt;In this work, we present a systematic analysis of the processes leading to the formation of winter- and summertime lower tropospheric warm extremes in the high Arctic by means of kinematic backward trajectories based on the ERA-Interim reanalysis. The trajectories enable us to quantify the relative contributions of poleward transport from (potentially) warmer regions, adiabatic warming due to subsidence, and diabatic heating associated with surface sensible heat fluxes and latent heat release. Furthermore, we relate these processes to atmospheric dynamical flow features such as atmospheric blocking and extratropical cyclones.&lt;/p&gt;&lt;p align=&quot;justify&quot;&gt;Our analyses reveal that subsidence in blocking anticyclones over the Barents and Kara Seas and diabatic warming by surface sensible heat fluxes are the dominant mechanisms leading to wintertime warm extremes (contributing about 40% each), whereas the transport from southerly latitudes &amp;#8211; predominantly accomplished by the injection of warm and humid air masses associated with an intensified and westward displaced storm track in the Nordic Seas - is of secondary importance (20%). Summertime warm anomalies, in contrast, are essentially the result of subsidence in blocking anticyclones (70%) that are located within the high Arctic. Thus, our findings point towards a rich, seasonally varying spectrum of dynamical and thermodynamic processes contributing to Arctic warm extremes that result from a complex interplay between transport induced by dynamical weather systems and diabatic processes. Furthermore, they emphasize the importance of processes within the Arctic for the formation of warm extremes.&lt;/p&gt;&lt;p align=&quot;justify&quot;&gt;Papritz, L., 2019: Arctic lower tropospheric warm and cold extremes: horizontal and vertical transport, diabatic processes, and linkage to synoptic circulation features, &lt;em&gt;J. Climate&lt;/em&gt;, doi: 10.1175/JCLI-D-19-0638.1&lt;/p&gt;


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