0000000000953304
AUTHOR
Heiko Bozem
Summertime observations of ultrafine particles and cloud condensation nuclei from the boundary layer to the free troposphere in the Arctic
Abstract. The Arctic is extremely sensitive to climate change. Shrinking sea ice extent increases the area covered by open ocean during Arctic summer, which impacts the surface albedo and aerosol and cloud properties among many things. In this context extensive aerosol measurements (aerosol composition, particle number and size, cloud condensation nuclei, and trace gases) were made during 11 flights of the NETCARE July, 2014 airborne campaign conducted from Resolute Bay, Nunavut (74N, 94W). Flights routinely included vertical profiles from about 60 to 3000 m a.g.l. as well as several low-level horizontal transects over open ocean, fast ice, melt ponds, and polynyas. Here we discuss the vert…
Vertical profile of atmospheric dimethyl sulfide in the Arctic Spring and Summer
Abstract. Vertical distributions of atmospheric dimethyl sulfide (DMS(g)) were sampled aboard the research aircraft Polar 6 near Lancaster Sound, Nunavut, Canada in July 2014 and on pan-Arctic flights in April 2015 that started from Longyearbyen, Spitzbergen, and passed through Alert and Eureka, Nunavut and Inuvik, Northwest Territories. Larger mean DMS(g) mixing ratios were present during April 2015 (campaign-mean of 116±8 pptv) compared to July 2014 (campaign-mean of 20±6 pptv). Observations in July 2014 indicated a decrease in DMS(g) mixing ratios with altitude up to about 3 km, and the largest mixing ratios were found near the surface above ice-edge and open water, coincident with incre…
Trace gas composition in the Asian summer monsoon anticyclone: a case study based on aircraft observations and model simulations
We present in situ measurements of the trace gas composition of the upper tropospheric (UT) Asian summer monsoon anticyclone (ASMA) performed with the High Altitude and Long Range Research Aircraft (HALO) in the frame of the Earth System Model Validation (ESMVal) campaign. Air masses with enhanced O3 mixing ratios were encountered after entering the ASMA at its southern edge at about 150 hPa on 18 September 2012. This is in contrast to the presumption that the anticyclone's interior is dominated by recently uplifted air with low O3 in the monsoon season. We also observed enhanced CO and HCl in the ASMA, which are tracers for boundary layer pollution and tropopause layer (TL) air or stratosp…
Ship emissions measurement in the Arctic from plume intercepts of the Canadian Coast Guard <i>Amundsen</i> icebreaker from the <i>Polar 6</i> aircraft platform
Abstract. Decreasing sea ice and increasing marine navigability in northern latitudes have changed Arctic ship traffic patterns in recent years and are predicted to increase annual ship traffic in the Arctic in the future. Development of effective regulations to manage environmental impacts of shipping requires an understanding of ship emissions and atmospheric processing in the Arctic environment. As part of the summer 2014 NETCARE (Network on Climate and Aerosols) campaign, the plume dispersion and gas and particle emission factors of emissions originating from the Canadian Coast Guard Amundsen icebreaker operating near Resolute Bay, NU, Canada have been investigated. The Amundsen burnt d…
Boundary layer and free-tropospheric dimethyl sulfide in the Arctic spring and summer
Vertical distributions of atmospheric dimethyl sulfide (DMS(g)) were sampled aboard the research aircraft Polar 6 near Lancaster Sound, Nunavut, Canada, in July 2014 and on pan-Arctic flights in April 2015 that started from Longyearbyen, Spitzbergen, and passed through Alert and Eureka, Nunavut, and Inuvik, Northwest Territories. Larger mean DMS(g) mixing ratios were present during April 2015 (campaign mean of 116 ± 8 pptv) compared to July 2014 (campaign mean of 20 ± 6 pptv). During July 2014, the largest mixing ratios were found near the surface over the ice edge and open water. DMS(g) mixing ratios decreased with altitude up to about 3 km. During April 2015, profiles of DMS(g) were m…
Modelling Regional Air Quality in the Canadian Arctic: Simulation of an Arctic Summer Field Campaign
Model simulations of an Arctic summer field campaign were carried out. The model results were compared with observational data from both ground-based monitoring and in situ measurements on-board multiple mobile platforms. The model was able to well capture regional sources and transport affecting the Arctic air quality. It is shown that the study area was impacted by North American (NA) regional biomass burning emissions. The model-observation comparison also corroborates previous findings on possible roles of marine-biogenic sources in aerosol production in the Arctic MBL during summertime.
Aircraft-based measurements of High Arctic springtime aerosol show evidence for vertically varying sources, transport and composition
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…
In situ detection of stratosphere-troposphere exchange of cirrus particles in the midlatitudes
Airborne trace gas, microphysical, and radiation measurements were performed during the AIRcraft TOwed Sensor Shuttle - Inhomogeneous Cirrus Experiment over northern Germany in 2013. Based on high-precision nitrous oxide (N2O) and carbon monoxide (CO) in situ data, stratospheric air could be identified, which contained cirrus cloud particles. Consistent with the stratospheric N2O data, backward trajectories indicate that the sampled air masses crossed the dynamical tropopause in the last 3 h before the measurement. These air masses contained cirrus particles, which were formed during slow ascent in the troposphere and subsequently mixed with stratospheric air. From the CO-N2O correlation th…
Frequent Ultrafine Particle Formation and Growth in the Canadian Arctic Marine Environment
Abstract. The source strength and capability of aerosol particles in the Arctic to act as cloud condensation nuclei have important implications for understanding the indirect aerosol-cloud effect within the polar climate system. It has been shown in several Arctic regions that ultrafine particle (UFP) formation and growth is a key contributor to aerosol number concentrations during the summer. This study uses aerosol number size distribution measurements from ship-board measurement expeditions aboard the research icebreaker CCGS Amundsen in the summers of 2014 and 2016 throughout the Canadian Arctic to gain a deeper understanding of the drivers of UFP formation and growth within this marine…
Comparison of Inorganic Chlorine in the Southern Hemispheric lowermost stratosphere during Late Winter 2019
Inorganic chlorine (Cly) is the sum of the degradation products of long-lived chlorinated source gases. These include the reservoir species (HCl and ClONO2) and active chlorine species (i.e. ClOx). The active chlorine species drive catalytic cycles that deplete ozone in the polar winter stratosphere. This work presents calculations of inorganic chlorine (Cly) derived from chlorinated source gas measurements on board the High Altitude and Long Range Research Aircraft (HALO) during the Southern hemisphere Transport, Dynamic and Chemistry (SouthTRAC) campaign in late winter and early spring 2019. Results are compared to Cly of the Northern Hemisphere derived from measurements of the POLSTRACC-…
Airborne observation of mixing across the entrainment zone during PARADE 2011
This study presents the analysis of the structure and air mass characteristics of the lower atmosphere during the field campaign PARADE (PArticles and RAdicals: Diel observations of the impact of urban and biogenic Emissions) on Mount Kleiner Feldberg in southwestern Germany during late summer 2011. We analysed measurements of meteorological variables (temperature, moisture, pressure, wind speed and direction) from radio soundings and of chemical tracers (carbon dioxide, ozone) from aircraft measurements. We focus on the thermodynamic and dynamic properties that control the chemical distribution of atmospheric constituents in the boundary layer. We show that the evolution of tracer profiles…
New insights into aerosol and climate in the Arctic
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 …
Temporally delineated sources of major chemical species in high Arctic snow
Long-range transport of aerosol from lower latitudes to the high Arctic may be a significant contributor to climate forcing in the Arctic. To identify the sources of key contaminants entering the Canadian High Arctic an intensive campaign of snow sampling was completed at Alert, Nunavut, from September 2014 to June 2015. Fresh snow samples collected every few days were analyzed for black carbon, major ions, and metals, and this rich data set provided an opportunity for a temporally refined source apportionment of snow composition via positive matrix factorization (PMF) in conjunction with FLEXPART (FLEXible PARTicle dispersion model) potential emission sensitivity analysis. Seven source fac…
Observations of atmospheric chemical deposition to high Arctic snow
Abstract. Rapidly rising temperatures and loss of snow and ice cover have demonstrated the unique vulnerability of the high Arctic to climate change. There are major uncertainties in modelling the chemical depositional and scavenging processes of Arctic snow. To that end, fresh snow samples collected on average every 4 days at Alert, Nunavut, from September 2014 to June 2015 were analyzed for black carbon, major ions, and metals, and their concentrations and fluxes were reported. Comparison with simultaneous measurements of atmospheric aerosol mass loadings yields effective deposition velocities that encompass all processes by which the atmospheric species are transferred to the snow. It is…
Observations of Atmospheric Chemical Deposition to High Arctic Snow
Abstract. Rapidly rising temperatures and loss of snow and ice cover have demonstrated the unique vulnerability of the high Arctic to climate change. There are major uncertainties in modelling the chemical depositional and scavenging processes of Arctic snow. To that end, fresh snow samples collected on average every four days at Alert, Nunavut, from September 2014 to June 2015 were analyzed for black carbon, major ions, and metals, and their concentrations and fluxes reported. Comparison with simultaneous measurements of atmospheric aerosol mass loadings yields effective deposition velocities which encompass all processes by which the atmospheric species are transferred to the snow. It is …
Transport of Antarctic stratospheric strongly dehydrated air into the troposphere observed during the HALO-ESMVal campaign 2012
Abstract. Dehydration in the Antarctic winter stratosphere is a well-known phenomenon that is annually observed by satellites and occasionally observed by balloon-borne measurements. However, in situ measurements of dehydrated air masses in the Antarctic vortex are very rare. Here, we present detailed observations with the in situ and GLORIA remote sensing instrument payload aboard the German aircraft HALO. Strongly dehydrated air masses down to 1.6 ppmv of water vapor were observed as far north as 47° S in an altitude between 12 and 13 km in the lowermost stratosphere. The dehydration can be traced back to individual ice formation events above the Antarctic Peninsula and Plateau, where ice…
Frequent ultrafine particle formation and growth in Canadian Arctic marine and coastal environments
The source strength and capability of aerosol particles in the Arctic to act as cloud condensation nuclei have important implications for understanding the indirect aerosol–cloud effect within the polar climate system. It has been shown in several Arctic regions that ultrafine particle (UFP) formation and growth is a key contributor to aerosol number concentrations during the summer. This study uses aerosol number size distribution measurements from shipboard expeditions aboard the research icebreaker CCGS Amundsen in the summers of 2014 and 2016 throughout the Canadian Arctic to gain a deeper understanding of the drivers of UFP formation and growth within this marine boundary layer. UFP nu…
Evidence for marine biogenic influence on summertime Arctic aerosol
International audience; We present vertically-resolved observations of aerosol composition during pristine summertime Arctic background conditions. The methansulfonic acid (MSA)-to-sulfate ratio peaked near the surface (mean 0.10), indicating a contribution from ocean-derived biogenic sulfur. Similarly, the organic aerosol (OA)-to-sulfate ratio increased towards the surface (mean 2.0). Both MSA-to-sulfate and OA-to-sulfate ratios were significantly correlated with FLEXPART-WRF-predicted airmass residence time over open water, indicating marine influenced OA. External mixing of sea salt aerosol from a larger number fraction of organic, sulfate and amine-containing particles, together with lo…
Synoptic development during the ACLOUD/PASCAL field campaign near Svalbard in spring 2017
Abstract. The two concerted field campaigns Arctic CLoud Observations Using airborne measurements during polar Day (ACLOUD) and the Physical feedbacks of Arctic planetary boundary level Sea ice, Cloud and AerosoL (PASCAL) took place near Svalbard from 23 May to 26 June 2017. They were focused on studying Arctic mixed-phase clouds and involved observations from two airplanes (ACLOUD), an icebreaker (PASCAL), as well as surface-based stations, a tethered balloon, and satellites. Here, we present the synoptic development during the 35 day period of the campaigns, using classical near-surface and upper-air meteorological observations, as well as operational satellite and model data. Over the ca…
The Arctic Cloud Puzzle: Using ACLOUD/PASCAL Multiplatform Observations to Unravel the Role of Clouds and Aerosol Particles in Arctic Amplification
A consortium of polar scientists combined observational forces in a field campaign of unprecedented complexity to uncover the secrets of clouds and their role in Arctic amplification. Two research aircraft, an icebreaker research vessel, an ice-floe camp including an instrumented tethered balloon, and a permanent ground-based measurement station were employed in this endeavour. Clouds play an important role in Arctic amplification. This term represents the recently observed enhanced warming of the Arctic relative to the global increase of near-surface air temperature. However, there are still important knowledge gaps regarding the interplay between Arctic clouds and aerosol particles, surfa…
Investigation of the mixing layer height derived from ceilometer measurements in the Kathmandu Valley and implications for local air quality
Abstract. In this study 1 year of ceilometer measurements taken in the Kathmandu Valley, Nepal, in the framework of the SusKat project (A Sustainable Atmosphere for the Kathmandu Valley) were analysed to investigate the diurnal variation of the mixing layer height (MLH) and its dependency on the meteorological conditions. In addition, the impact of the MLH on the temporal variation and the magnitude of the measured black carbon concentrations are analysed for each season. Based on the assumption that black carbon aerosols are vertically well mixed within the mixing layer and the finding that the mixing layer varies only little during night time and morning hours, black carbon emission fluxe…
A quantitative analysis of stratospheric HCl, HNO3, and O3 in the tropopause region near the subtropical jet
The effects of chemical two-way mixing on the Extratropical Transition Layer (ExTL) near the subtropical jet are investigated by stratospheric tracer-tracer correlations. To this end, in situ measurements were performed west of Africa (25-32 ◦ N) during the Transport and Composition of the Upper Troposphere Lower Stratosphere (UTLS)/Earth System Model Validation (TACTS/ESMVal) mission in August/September 2012. The Atmospheric chemical Ionization Mass Spectrometer sampling HCl and HNO3 was for the first time deployed on the new German High Altitude and Long range research aircraft (HALO). Measurements of O3, CO, European Centre for Medium-Range Weather Forecasts (ECMWF) analysis, and the tig…
Particulate trimethylamine in the summertime Canadian high Arctic lower troposphere
Abstract. Size-resolved and vertical profile measurements of single particle chemical composition (sampling altitude range 50–3000 m) were conducted in July 2014 in the Canadian high Arctic during the aircraft-based measurement campaign NETCARE 2014. We deployed the single particle laser ablation aerosol mass spectrometer ALABAMA (vacuum aerodynamic diameter range approximately 200–1000 nm) to identify different particle types and their mixing states. On basis of the single particle analysis, we found that a significant fraction (23 %) of all analyzed particles (in total: 7412) contained trimethylamine (TMA). The identification of TMA in ambient mass spectra was confirmed by laboratory meas…
Ship emissions measurement in the Arctic by plume intercepts of the Canadian Coast Guard icebreaker <i>Amundsen</i> from the <i>Polar 6</i> aircraft platform
Abstract. Decreasing sea ice and increasing marine navigability in northern latitudes have changed Arctic ship traffic patterns in recent years and are predicted to increase annual ship traffic in the Arctic in the future. Development of effective regulations to manage environmental impacts of shipping requires an understanding of ship emissions and atmospheric processing in the Arctic environment. As part of the summer 2014 NETCARE (Network on Climate and Aerosols) campaign, the plume dispersion and gas and particle emission factors of effluents originating from the Canadian Coast Guard icebreaker Amundsen operating near Resolute Bay, NU, Canada, were investigated. The Amundsen burned dist…
Comparison of inorganic chlorine in the Antarctic and Arctic lowermost stratosphere by separate late winter aircraft measurements
Stratospheric inorganic chlorine (Cly) is predominantly released from long-lived chlorinated source gases and, to a small extent, very short-lived chlorinated substances. Cly includes the reservoir species (HCl and ClONO2) and active chlorine species (i.e., ClOx). The active chlorine species drive catalytic cycles that deplete ozone in the polar winter stratosphere. This work presents calculations of inorganic chlorine (Cly) derived from chlorinated source gas measurements on board the High Altitude and Long Range Research Aircraft (HALO) during the Southern Hemisphere Transport, Dynamic and Chemistry (SouthTRAC) campaign in austral late winter and early spring 2019. Results are compared to…
Measurements of aerosol and CCN properties in the Mackenzie River delta (Canadian Arctic) during spring–summer transition in May 2014
Within the framework of the RACEPAC (Radiation–Aerosol–Cloud Experiment in the Arctic Circle) project, the Arctic aerosol, arriving at a ground-based station in Tuktoyaktuk (Mackenzie River delta area, Canada), was characterized during a period of 3 weeks in May 2014. Basic meteorological parameters and particle number size distributions (PNSDs) were observed and two distinct types of air masses were found. One type were typical Arctic haze air masses, termed accumulation-type air masses, characterized by a monomodal PNSD with a pronounced accumulation mode at sizes above 100 nm. These air masses were observed during a period when back trajectories indicate an air mass origin in the north-e…
Depletion of ozone and reservoir species of chlorine and nitrogen oxide in the lower Antarctic polar vortex measured from aircraft
Novel airborne in situ measurements of inorganic chlorine, nitrogen oxide species, and ozone were performed inside the lower Antarctic polar vortex and at its edge in September 2012. We focus on one flight during the Transport and Composition of the LMS/Earth System Model Validation (TACTS/ESMVal) campaign with the German research aircraft HALO (High-Altitude LOng range research aircraft), reaching latitudes of 65°S and potential temperatures up to 405 K. Using the early winter correlations of reactive trace gases with N2O from the Atmospheric Chemistry Experiment-Fourier Transform Spectrometer (ACE-FTS), we find high depletion of chlorine reservoir gases up to ∼40% (0.8 ppbv) at 12 km to 1…
Characterization of transport regimes and the polar dome during Arctic spring and summer using in situ aircraft measurements
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 W…
Airborne survey of trace gases and aerosols over the Southern Baltic Sea: from clean marine boundary layer to shipping corridor effect
The influence of shipping on air quality over the Southern Baltic Sea was investigated by characterizing the horizontal and vertical distribution of aerosols and trace gases using airborne measurements in the summer of 2015. Generally, continental and anthropogenic emissions affected the vertical distribution of atmospheric pollutants, leading to pronounced stratification in and above the marine boundary layer and controlling the aerosol extinction. Marine traffic along the shipping corridor “Kadet Fairway” in the Arkona Basin is shown to influence the presence and properties of both trace gases and aerosol particles in the lowest atmospheric layer. Total particle number concentration and N…
Airborne observations of far-infrared upwelling radiance in the Arctic
Abstract. The first airborne measurements of the Far-InfraRed Radiometer (FIRR) were performed in April 2015 during the panarctic NETCARE campaign. Vertical profiles of spectral upwelling radiance in the range 8–50 μm were measured in clear and cloudy conditions from the surface up to 6 km. The clear-sky profiles highlight the strong dependence of radiative fluxes to the temperature inversion typical of the Arctic. Measurements acquired for total column water vapor from 1.5 to 10.5 mm also underline the sensitivity of the far-infrared greenhouse effect to specific humidity. The cloudy cases show that optically thin ice clouds increase the cooling rate of the atmosphere by a factor up to thr…
Effects of 20–100 nm particles on liquid clouds in the clean summertime Arctic
Abstract. Observations addressing effects of aerosol particles on summertime Arctic clouds are limited. An airborne study, carried out during July 2014 from Resolute Bay, Nunavut, Canada, as part of the Canadian NETCARE project, provides a comprehensive in situ look into some effects of aerosol particles on liquid clouds in the clean environment of the Arctic summer. Median cloud droplet number concentrations (CDNC) from 62 cloud samples are 10 cm−3 for low-altitude cloud (clouds topped below 200 m) and 101 cm−3 for higher-altitude cloud (clouds based above 200 m). The lower activation size of aerosol particles is ≤ 50 nm diameter in about 40 % of the cases. Particles as small as 20 nm ac…
A comprehensive in situ and remote sensing data set from the Arctic CLoud Observations Using airborne measurements during polar Day (ACLOUD) campaign
The Arctic CLoud Observations Using airborne measurements during polar Day (ACLOUD) campaign was carried out north-west of Svalbard (Norway) between 23 May and 6 June 2017. The objective of ACLOUD was to study Arctic boundary layer and mid-level clouds and their role in Arctic amplification. Two research aircraft (Polar 5 and 6) jointly performed 22 research flights over the transition zone between open ocean and closed sea ice. Both aircraft were equipped with identical instrumentation for measurements of basic meteorological parameters, as well as for turbulent and radiative energy fluxes. In addition, on Polar 5 active and passive remote sensing instruments were installed, while Polar 6 …
Chemical composition and source attribution of sub-micrometre aerosol particles in the summertime Arctic lower troposphere
Aerosol particles impact the Arctic climate system both directly and indirectly by modifying cloud properties, yet our understanding of their vertical distribution, chemical composition, mixing state, and sources in the summertime Arctic is incomplete. In situ vertical observations of particle properties in the high Arctic combined with modelling analysis on source attribution are in short supply, particularly during summer. We thus use airborne measurements of aerosol particle composition to demonstrate the strong contrast between particle sources and composition within and above the summertime Arctic boundary layer. In situ measurements from two complementary aerosol mass spectrometers, t…
Meteorological conditions during the ACLOUD/PASCAL field campaign near Svalbard in early summer 2017
Abstract. The two concerted field campaigns, Arctic CLoud Observations Using airborne measurements during polar Day (ACLOUD) and the Physical feedbacks of Arctic planetary boundary level Sea ice, Cloud and AerosoL (PASCAL), took place near Svalbard from 23 May to 26 June 2017. They were focused on studying Arctic mixed-phase clouds and involved observations from two airplanes (ACLOUD), an icebreaker (PASCAL) and a tethered balloon, as well as ground-based stations. Here, we present the synoptic development during the 35-day period of the campaigns, using near-surface and upper-air meteorological observations, as well as operational satellite, analysis, and reanalysis data. Over the campaign…
Impact of the Asian monsoon on the extratropical lower stratosphere: trace gas observations during TACTS over Europe 2012
Abstract. The transport of air masses originating from the Asian monsoon anticyclone into the extratropical upper troposphere and lower stratosphere (Ex-UTLS) above potential temperatures Θ = 380 K was identified during the HALO aircraft mission TACTS in August and September 2012. In situ measurements of CO, O3 and N2O during TACTS flight 2 on 30 August 2012 show the irreversible mixing of aged stratospheric air masses with younger (recently transported from the troposphere) ones within the Ex-UTLS. Backward trajectories calculated with the trajectory module of CLaMS indicate that these tropospherically affected air masses originate from the Asian monsoon anticyclone. These air masses are …
Measurements of aerosol and CCN properties in the Mackenzie River delta (Arctic) during RACEPAC
Within the framework of the RACEPAC (Radiation-Aerosol-Cloud Experiment in the Arctic Circle) project, the Arctic aerosol, arriving at a ground-based station in Tuktoyaktuk (Mackenzie River delta area, Canada), was characterized during a period of 3 weeks in May 2014. Basic meteorological parameters and particle number size distributions (PNSDs) were observed and two distinct types of air masses were found. One type were typical Arctic haze air masses, termed accumulation-type air masses, characterized by a monomodal PNSD with a pronounced accumulation mode at sizes above 100 nm. These air masses were observed during a period when back trajectories indicate an air mass origin in the north-e…