Concentrations, composition, and sources of ice-nucleating particles in the Canadian High Arctic during spring 2016
Modelling studies suggest that the climate and the hydrological cycle are sensitive to the concentrations of ice-nucleating particles (INPs). However, the concentrations, composition, and sources of INPs in the atmosphere remain uncertain. Here, we report daily concentrations of INPs in the immersion freezing mode and tracers of mineral dust (Al, Fe, Ti, and Mn), sea spray aerosol (Na+ and Cl−), and anthropogenic aerosol (Zn, Pb, NO3-, NH4+, and non-sea-salt SO42-) at Alert, Canada, during a 3-week campaign in March 2016. In total, 16 daily measurements of INPs are reported. The average INP concentrations measured in the immersion freezing mode were 0.005±0.002, 0.020±0.004, and 0.186±0.040…
Evidence of small-scale quasi-isentropic mixing in ridges of extratropical baroclinic waves
Abstract. Stratosphere–troposphere exchange within extratropical cyclones provides the potential for anthropogenic and natural surface emissions to rapidly reach the stratosphere as well as for ozone from the stratosphere to penetrate deep into the troposphere, even down into the boundary layer. The efficiency of this process directly influences the surface climate, the chemistry in the stratosphere, the chemical composition of the extratropical transition layer, and surface pollution levels. Here, we present evidence for a mixing process within extratropical cyclones which has gained only a small amount of attention so far and which fosters the transport of tropospheric air masses into the…
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…
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…
In situ observations of new particle formation in the tropical upper troposphere: the role of clouds and the nucleation mechanism
New particle formation (NPF), which generates nucleation mode aerosol, was observed in the tropical Upper Troposphere (UT) and Tropical Tropopause Layer (TTL) by in situ airborne measurements over South America (January–March 2005), Australia (November–December 2005), West Africa (August 2006) and Central America (2004–2007). Particularly intense NPF was found at the bottom of the TTL. Measurements with a set of condensation particle counters (CPCs) with different <i>d</i><sub>p50</sub> (50% lower size detection efficiency diameter or "cut-off diameter") were conducted on board the M-55 <i>Geophysica</i> in the altitude range of 12.0–20.5 km and on board …
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…
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…
The tropopause inversion layer in baroclinic life-cycle experiments: the role of diabatic processes
Abstract. Recent studies on the formation of a quasi-permanent layer of enhanced static stability above the thermal tropopause revealed the contributions of dynamical and radiative processes. Dry dynamics leads to the evolution of a tropopause inversion layer (TIL), which is, however, too weak compared to observations and thus diabatic contributions are required. In this study we aim to assess the importance of diabatic processes in the understanding of TIL formation at midlatitudes. The non-hydrostatic model COSMO (COnsortium for Small-scale MOdelling) is applied in an idealized midlatitude channel configuration to simulate baroclinic life cycles. The effect of individual diabatic processe…
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…
Composite analysis of the tropopause inversion layer in extratropical baroclinic waves
Abstract. The variability and similarities in the evolution of the tropopause inversion (TIL) layer during cyclongenesis in the North Atlantic storm track are investigated using operational meteorological analysis data (Integrated Forecast System from the European Centre for Medium-Range Weather Forecasts). For this a total amount of 130 cyclones have been analysed which evolved during the months August through October between 2010–2014 over the North Atlantic. Their paths of migration along with associated flow features in the upper troposphere/lower stratosphere (UTLS) have been tracked using the mean sea level pressure. Subsets of the 130 cyclones have been used for composite analysis us…
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 …
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…
Cross-hemispheric transport of central African biomass burning pollutants: implications for downwind ozone production
Pollutant plumes with enhanced concentrations of trace gases and aerosols were observed over the southern coast of West Africa during August 2006 as part of the AMMA wet season field campaign. Plumes were observed both in the mid and upper troposphere. In this study we examined the origin of these pollutant plumes, and their potential to photochemically produce ozone (O<sub>3</sub>) downwind over the Atlantic Ocean. Their possible contribution to the Atlantic O<sub>3</sub> maximum is also discussed. Runs using the BOLAM mesoscale model including biomass burning carbon monoxide (CO) tracers were used to confirm an origin from central African biomass burning fires. The…
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…
High gas-phase mixing ratios of formic and acetic acid in the High Arctic
Abstract. Formic and acetic acid are ubiquitous and abundant in the Earth's atmosphere and are important contributors to cloud water acidity, especially in remote regions. Their global sources are not well understood, as evidenced by the inability of models to reproduce the magnitude of measured mixing ratios, particularly at high northern latitudes. The scarcity of measurements at those latitudes is also a hindrance to understanding these acids and their sources. Here, we present ground-based gas-phase measurements of formic acid (FA) and acetic acid (AA) in the Canadian Arctic collected at 0.5 Hz with a high-resolution chemical ionization time-of-flight mass spectrometer using the iodide …
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…
On the occurrence of enhanced vertical wind shear in the tropopause region: A ten year ERA5 northern hemispheric study
A climatology of the occurrence of enhanced wind shear in the UTLS is presented, which gives rise to define a tropopause shear layer (TSL). Enhanced wind shear in the tropopause region is of interest because it can generate turbulence which can lead to cross-tropopause mixing. The analysis is based on ten years of daily northern hemispheric ECMWF ERA-5 reanalysis data. The vertical extent of the region analysed is limited to the altitudes from 1.5 km above the surface up to 25 km, to exclude the planetary boundary layer as well as enhanced wind shear in higher atmospheric layers like the mesosphere/lower thermosphere. A threshold value of S2t = 4 ·&…
The impact of overshooting deep convection on local transport and mixing in the tropical upper troposphere/lower stratosphere (UTLS)
Abstract. In this study we examine the simulated downward transport and mixing of stratospheric air into the upper tropical troposphere as observed on a research flight during the SCOUT-O3 campaign in connection to a deep convective system. We use the Advanced Research Weather and Research Forecasting (WRF-ARW) model with a horizontal resolution of 333 m to examine this downward transport. The simulation reproduces the deep convective system, its timing and overshooting altitudes reasonably well compared to radar and aircraft observations. Passive tracers initialised at pre-storm times indicate the downward transport of air from the stratosphere to the upper troposphere as well as upward tr…
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…
On the occurrence of strong vertical wind shear in the tropopause region: a 10-year ERA5 northern hemispheric study
A climatology of the occurrence of strong wind shear in the upper troposphere–lower stratosphere (UTLS) is presented, which gives rise to defining a tropopause shear layer (TSL). Strong wind shear in the tropopause region is of interest because it can generate turbulence, which can lead to cross-tropopause mixing. The analysis is based on 10 years of daily northern hemispheric ECMWF ERA5 reanalysis data. The vertical extent of the region analyzed is limited to the altitudes from 1.5 km above the surface up to 25 km, to exclude the planetary boundary layer as well as strong wind shear in higher atmospheric layers like the mesosphere–lower thermosphere. A threshold value of St2=4×10-4s-2 of t…
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…
Can inertia-gravity waves persistently alter the tropopause inversion layer?
Previous simulations of baroclinic life cycles have shown, among many other features, the evolution of a tropopause inversion layer (TIL) as well as the spontaneous emission of inertia-gravity waves (IGWs). This study suggests that the latter two are related to each other, i.e., that IGWs may affect the TIL in a persistent manner. The IGWs are emitted along the jet and grow to large amplitudes, leading to the appearance of low-gradient Richardson numbers that indicate Kelvin-Helmholtz instability. Ensuing energy dissipation, local heating, and turbulence may persistently alter the thermodynamical structure of the tropopause region and, therefore, contribute to TIL formation or alter an exis…
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…