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…

Stratosphere-troposphere exchange in the vicinity of a tropopause fold

Abstract. Transport of air masses from the stratosphere to the troposphere along tropopause folds can lead to peaked ozone concentrations at ground level and hereby influence the long-term trend of tropospheric ozone. To improve the understanding of responsible processes and preferred regions of exchange, transient and reversible exchange processes in the vicinity of a tropopause fold are analysed on the basis of a case study. The global and regional atmospheric chemistry model system MECO(n), which couples the limited-area atmospheric chemistry and climate model COSMO-CLM/MESSy to the global model ECHAM5/MESSy for Atmospheric Chemistry (EMAC) is applied. Using similar process parametrisati…

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…

Highly resolved observations of trace gases in the lowermost stratosphere and upper troposphere from the Spurt project: an overview

International audience; During SPURT (Spurenstofftransport in der Tropopausenregion, trace gas transport in the tropopause region) we performed measurements of a wide range of trace gases with different lifetimes and sink/source characteristics in the northern hemispheric upper troposphere (UT) and lowermost stratosphere (LMS). A large number of in-situ instruments were deployed on board a Learjet 35A, flying at altitudes up to 13.7 km, at times reaching to nearly 380 K potential temperature. Eight measurement campaigns (consisting of a total of 36 flights), distributed over all seasons and typically covering latitudes between 35° N and 75° N in the European longitude sector (10° W?20° E), …

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…

Observed versus simulated mountain waves over Scandinavia – improvement of vertical winds, energy and momentum fluxes by enhanced model resolution?

Abstract. Two mountain wave events, which occurred over northern Scandinavia in December 2013 are analysed by means of airborne observations and global and mesoscale numerical simulations with horizontal mesh sizes of 16, 7.2, 2.4 and 0.8 km. During both events westerly cross-mountain flow induced upward-propagating mountain waves with different wave characteristics due to differing atmospheric background conditions. While wave breaking occurred at altitudes between 25 and 30 km during the first event due to weak stratospheric winds, waves propagated to altitudes above 30 km and interfacial waves formed in the troposphere at a stratospheric intrusion layer during the second event. Global an…

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…

Seasonality and extent of extratropical TST derived from in-situ CO measurements during SPURT

Abstract. We present airborne in-situ trace gas measurements which were performed on eight campaigns between November 2001 and July 2003 during the SPURT-project (SPURenstofftransport in der Tropopausenregion, trace gas transport in the tropopause region). The measurements on a quasi regular basis allowed an overview of the seasonal variations of the trace gas distribution in the tropopause region over Europe from 35°-75°N to investigate the influence of transport and mixing across the extratropical tropopause on the lowermost stratosphere. From the correlation of CO and O3 irreversible mixing of tropospheric air into the lowermost stratosphere is identified. The CO distribution indicates t…

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…

On the structural changes in the Brewer-Dobson circulation after 2000

In this paper we present evidence that the observed increase in tropical upwelling after the year 2000 may be attributed to a change in the Brewer-Dobson circulation pattern. For this purpose, we use the concept of transit times derived from residual circulation trajectories and different in-situ measurements of ozone and nitrous dioxide. Observations from the Canadian midlatitude ozone profile record, probability density functions of in-situ N<sub>2</sub>O observations and a shift of the N<sub>2</sub>O-O<sub>3</sub> correlation slopes, taken together, indicate that the increased upwelling in the tropics after the year 2000 appears to have triggered an in…

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…

Chlorine partitioning in the lowermost Arctic vortex during the cold winter 2015/2016

Activated chlorine compounds in the polar winter stratosphere drive catalytic cycles that deplete ozone and methane, whose abundances are highly relevant to the evolution of global climate. The present work introduces a novel dataset of in situ measurements of relevant chlorine species in the lowermost Arctic stratosphere from the aircraft mission POLSTRACC–GW-LCYCLE–SALSA during winter 2015/2016. The major stages of chemical evolution of the lower polar vortex are presented in a consistent series of high-resolution mass spectrometric observations of HCl and ClONO2. Simultaneous measurements of CFC-12 are used to derive total inorganic chlorine (Cly) and active chlorine (ClOx). The new data…

In situ observations of CH2Cl2 and CHCl3 show efficient transport pathways for very short-lived species into the lower stratosphere via the Asian and the North American summer monsoon

Efficient transport pathways for ozone-depleting very short-lived substances (VSLSs) from their source regions into the stratosphere are a matter of current scientific debate; however they have yet to be fully identified on an observational basis. Understanding the increasing impact of chlorine-containing VSLSs (Cl-VSLSs) on stratospheric ozone depletion is important in order to validate and improve model simulations and future predictions. We report on a transport study using airborne in situ measurements of the Cl-VSLSs dichloromethane (CH2Cl2) and trichloromethane (chloroform, CHCl3) to derive a detailed description of two transport pathways from (sub)tropical source regions into the ext…

On the attribution of contributions of atmospheric trace gases to emissions in atmospheric model applications

Abstract. We present an improved tagging method, which describes the combined effect of emissions of various species from individual emission categories, e.g. the impact of both, nitrogen oxides and non-methane hydrocarbon emissions on ozone. This method is applied to two simplified chemistry schemes, which represent the main characteristics of atmospheric ozone chemistry. Analytical solutions are presented for this tagging approach. In the past, besides tagging approaches, sensitivity methods were used, which estimate the contributions from individual sources based on differences in two simulations, a base case and a simulation with a perturbation in the respective emission category. We ap…

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-…

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…

Tropical troposphere to stratosphere transport of carbon monoxide and long-lived trace species in the Chemical Lagrangian Model of the Stratosphere (CLaMS)

Variations in the mixing ratio of trace gases of tropospheric origin entering the stratosphere in the tropics are of interest for assessing both troposphere to stratosphere transport fluxes in the tropics and the impact of these transport fluxes on the composition of the tropical lower stratosphere. Anomaly patterns of carbon monoxide (CO) and long-lived tracers in the lower tropical stratosphere allow conclusions about the rate and the variability of tropical upwelling to be drawn. Here, we present a simplified chemistry scheme for the Chemical Lagrangian Model of the Stratosphere (CLaMS) for the simulation, at comparatively low numerical cost, of CO, ozone, and long-lived trace substances…

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…

SOUTHTRAC-GW: An airborne field campaign to explore gravity wave dynamics at the world’s strongest hotspot

The southern part of South America and the Antarctic peninsula are known as the world’s strongest hotspot region of stratospheric gravity wave (GW) activity. Large tropospheric winds are deflected by the Andes and the Antarctic Peninsula and excite GWs that might propagate into the upper mesosphere. Satellite observations show large stratospheric GW activity above the mountains, the Drake Passage, and in a belt centered along 60°S. This scientifically highly interesting region for studying GW dynamics was the focus of the Southern Hemisphere Transport, Dynamics, and Chemistry–Gravity Waves (SOUTHTRAC-GW) mission. The German High Altitude and Long Range Research Aircraft (HALO) was deployed …

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 …

Determination of eddy diffusivity in the lowermost stratosphere

[1] We present a 2D-advection-diffusion model that simulates the main transport pathways influencing tracer distributions in the lowermost stratosphere (LMS). The model describes slow diabatic descent of aged stratospheric air, vertical (cross-isentropic) and horizontal (along isentropes) diffusion within the LMS and across the tropopause using equivalent latitude and potential temperature coordinates. Eddy diffusion coefficients parameterize the integral effect of dynamical processes leading to small scale turbulence and mixing. They were specified by matching model simulations to observed CO distributions. Interestingly, the model suggests mixing across isentropes to be more important tha…

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…

Redistribution of total reactive nitrogen in the lowermost Arctic stratosphere during the cold winter 2015/2016

During winter 2015/2016 the Arctic stratosphere was characterized by extraordinarily low temperatures in connection with the occurrence of extensive polar stratospheric clouds. From mid of December 2015 until mid of March 2016 the German research aircraft HALO (High Altitude and Long–Range Research Aircraft) was deployed to probe the lowermost stratosphere in the Arctic region within the POLSTRACC (Polar Stratosphere in a Changing Climate) mission. More than twenty flights have been conducted out of Kiruna/Sweden and Oberpfaffenhofen/Germany, covering the whole winter period. Besides total reactive nitrogen (NOy), observations of nitrous oxide, nitric acid, ozone and water were used f…

Supplementary material to "A convolution of observational and model data to estimate age of air spectra in the northern hemispheric lower stratosphere"

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…

Contribution of Asian emissions to upper tropospheric CO over the remote Pacific

Abstract. Upon analysing the global distribution of the highest 2 % of daily CO mixing ratios at 400 hPa derived from the MOPITT satellite instrument for 20 years (2000–2019), we very regularly detect regions with very high CO values (i.e. mixing ratios belonging to the globally highest 2 %) over the remote Northern Hemispheric (NH) Pacific. Such events of elevated CO over the upper tropospheric NH Pacific occur throughout the year with surprisingly high regularity and frequency (70 % of all days during winter, 80 % of all days during spring). During winter, most of these pollution events are detected over the north-eastern and central NH Pacific, during spring over the central NH Pacific, …

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…

Aircraft-based observation of meteoric material in lower-stratospheric aerosol particles between 15 and 68° N

We analyse aerosol particle composition measurements from five research missions between 2014 and 2018 to assess the meridional extent of particles containing meteoric material in the upper troposphere and lower stratosphere (UTLS). Measurements from the Jungfraujoch mountaintop site and a low-altitude aircraft mission show that meteoric material is also present within middle- and lower-tropospheric aerosol but within only a very small proportion of particles. For both the UTLS campaigns and the lower- and mid-troposphere observations, the measurements were conducted with single-particle laser ablation mass spectrometers with bipolar-ion detection, which enabled us to measure the chemical c…

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…

Transport timescales and tracer properties in the extratropical UTLS

A comprehensive evaluation of seasonal backward trajectories initialized in the northern hemisphere lowermost stratosphere (LMS) has been performed to investigate the factors that determine the temporal and spatial structure of troposphere-to-stratosphere-transport (TST) and it's impact on the LMS. In particular we explain the fundamental role of the transit time since last TST (tTST) for the chemical composition of the LMS. According to our results the structure of the LMS can be characterized by a layer with tTST<40 days forming a narrow band around the local tropopause. This layer extends about 30 K above the local dynamical tropopause, corresponding to the extratropical tropopause trans…

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…

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&thinsp;km above the surface up to 25&thinsp;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&thinsp;=&thinsp;4&thinsp;&middot;&…

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…

Bioaerosols in the Earth system: Climate, health, and ecosystem interactions

Abstract Aerosols of biological origin play a vital role in the Earth system, particularly in the interactions between atmosphere, biosphere, climate, and public health. Airborne bacteria, fungal spores, pollen, and other bioparticles are essential for the reproduction and spread of organisms across various ecosystems, and they can cause or enhance human, animal, and plant diseases. Moreover, they can serve as nuclei for cloud droplets, ice crystals, and precipitation, thus influencing the hydrological cycle and climate. The sources, abundance, composition, and effects of biological aerosols and the atmospheric microbiome are, however, not yet well characterized and constitute a large gap i…

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…

A convolution of observational and model data to estimate age of air spectra in the northern hemispheric lower stratosphere

Abstract. Derivation of mean age of air (AoA) and age spectra from atmospheric measurements remains a challenge and often requires data from atmospheric models. This study tries to minimize the direct influence of model data and presents an extension and application of a previously established inversion method to derive age spectra from mixing ratios of long- and short-lived trace gases. For a precise description of cross-tropopause transport processes, the inverse method is extended to incorporate air entrainment into the stratosphere across the tropical and extratropical tropopause. We first use simulations with the Chemical Lagrangian Model of the Stratosphere (CLaMS) to provide a genera…

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…

Fast transport from Southeast Asia boundary layer sources to northern Europe: rapid uplift in typhoons and eastward eddy shedding of the Asian monsoon anticyclone

Abstract. Enhanced tropospheric trace gases such as CO, CH4 and H2O and reduced stratospheric O3 were measured in situ in the lowermost stratosphere over northern Europe on 26 September 2012 during the TACTS aircraft campaign. The measurements indicate that these air masses clearly differ from the stratospheric background. The calculation of 40-day backward trajectories with the trajectory module of the CLaMS model shows that these air masses are affected by the Asian monsoon anticyclone. Some air masses originate from the boundary layer in Southeast Asia/West Pacific and are rapidly lifted (1–2 days) within a typhoon up to the outer edge of the Asian monsoon anticyclone. Afterwards, the ai…

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…

Mixing and ageing in the polar lower stratosphere in winter 2015–2016

We present data from winter 2015–2016, which were measured during the POLSTRACC (The Polar Stratosphere in a Changing Climate) aircraft campaign between December 2015 and March 2016 in the Arctic upper troposphere and lower stratosphere (UTLS). The focus of this work is on the role of transport and mixing between aged and potentially chemically processed air masses from the stratosphere which have midlatitude and low-latitude air mass fractions with small transit times originating at the tropical lower stratosphere. By combining measurements of CO, N2O and SF6 we estimate the evolution of the relative contributions of transport and mixing to the UTLS composition over the course of the winte…

On the structure of the extra-tropical transition layer from in-situ observations

Abstract. In-situ observations of atmospheric tracers from multiple measurement campaigns over the period 1994–2007 were combined to investigate the Extra-tropical Transition Layer (ExTL) region and the properties of large scale meridional transport. We used potential temperature, equivalent latitude and distance relative to the local dynamical tropopause as vertical coordinates to highlight the behaviour of trace gases in the tropopause region. Vertical coordinates based on constant PV surfaces allowed us to relate the dynamical definition of the tropopause with trace gases distributions and vertical gradients and hence analyse its latitudinal dependence and seasonal variability. Analysis …

Quantifying transport into the lowermost stratosphere using simultaneous in-situ measurements of SF&amp;lt;sub&amp;gt;6&amp;lt;/sub&amp;gt; and CO&amp;lt;sub&amp;gt;2&amp;lt;/sub&amp;gt;

Abstract. The seasonality of transport and mixing of air into the lowermost stratosphere (LMS) is studied using distributions of mean age of air and a mass balance approach, based on in-situ observations of SF6 and CO2 during the SPURT (Spurenstofftransport in der Tropopausenregion, trace gas transport in the tropopause region) aircraft campaigns. Combining the information of the mean age of air and the water vapour distributions we demonstrate that the tropospheric air transported into the LMS above the extratropical tropopause layer (ExTL) originates predominantly from the tropical tropopause layer (TTL). The concept of our mass balance is based on simultaneous measurements of the two pas…

In situ observations of CH&amp;lt;sub&amp;gt;2&amp;lt;/sub&amp;gt;Cl&amp;lt;sub&amp;gt;2&amp;lt;/sub&amp;gt; and CHCl&amp;lt;sub&amp;gt;3&amp;lt;/sub&amp;gt; show efficient transport pathways for very short-lived species into the lower stratosphere via the Asian and the North American summer monsoon

Abstract. Efficient transport pathways for ozone-depleting very short-lived substances (VSLSs) from their source regions into the stratosphere are a matter of current scientific debate; however they have yet to be fully identified on an observational basis. Understanding the increasing impact of chlorine-containing VSLSs (Cl-VSLSs) on stratospheric ozone depletion is important in order to validate and improve model simulations and future predictions. We report on a transport study using airborne in situ measurements of the Cl-VSLSs dichloromethane (CH2Cl2) and trichloromethane (chloroform, CHCl3) to derive a detailed description of two transport pathways from (sub)tropical source regions in…

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 tandem approach for collocated in-situ measurements of microphysical and radiative cirrus properties

Abstract. Microphysical and radiation measurements were collected with the unique AIRcraft TOwed Sensor Shuttle (AIRTOSS) – Learjet tandem platform. It is a combination of a Learjet 35A research aircraft and an instrumented aerodynamic body, which can be detached from and retracted back to the aircraft during flight. Both platforms are equipped with radiative, cloud microphysical, trace gas (CO, N2O, O3 and H2O) and meteorological instruments to study the inhomogeneity of cirrus as well as other layer clouds. Sophisticated numerical flow simulations were conducted in advance in order to optimally integrate a Cloud Combination Probe (CCP) inside the AIRTOSS. The tandem platform was used for …

A tandem approach for collocated measurements of microphysical and radiative cirrus properties

Microphysical and radiation measurements were collected with the novel AIRcraft TOwed Sensor Shuttle (AIRTOSS) – Learjet tandem platform. The platform is a combination of an instrumented Learjet 35A research aircraft and an aerodynamic bird, which is detached from and retracted back to the aircraft during flight via a steel wire with a length of 4000 m. Both platforms are equipped with radiative, cloud microphysical, trace gas, and meteorological instruments. The purpose of the development of this tandem set-up is to study the inhomogeneity of cirrus as well as other stratiform clouds. Sophisticated numerical flow simulations were conducted in order to optimally integrate an axially asymmet…

Observed versus simulated mountain waves over Scandinavia – improvement by enhanced model resolution?

Abstract. Two mountain wave events, which occured over northern Scandinavia in December 2013 are analysed by means of airborne observations and global and mesoscale numerical simulations with horizontal mesh sizes of 16 km, 7.2 km, 2.4 km and 0.8 km. During both events westerly cross-mountain flow induced upward propagating waves in the troposphere and stratosphere and trapped waves in the lee of the mountains. Despite similar forcing conditions gravity wave breaking occured during the first event at altitudes between 25 km to 30 km due to weak stratospheric background winds, while waves propagated to altitudes above 30 km during the second event. In the lower troposphere trapped lee waves …

A quasi chemistry-transport model mode for EMAC

Abstract. A quasi chemistry-transport model mode (QCTM) is presented for the numerical chemistry-climate simulation system ECHAM/MESSy Atmospheric Chemistry (EMAC). It allows for a quantification of chemical signals through suppression of any feedback between chemistry and dynamics. Noise would otherwise interfere too strongly. The signal is calculated from the difference of two QCTM simulations, a reference simulation and a sensitivity simulation. In order to avoid the feedbacks, the simulations adopt the following offline chemical fields: (a) offline mixing ratios of radiatively active substances enter the radiation scheme, (b) offline mixing ratios of nitric acid enter the scheme for re-…

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…

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 …

Pollution patterns in the upper troposphere over Europe and Asia observed by CARIBIC

Abstract Between May 2005 and March 2008 the CARIBIC (Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container) observatory was deployed to make atmospheric observations on 42 flights between Frankfurt, Germany and Manila, the Philippines. This nearly 3 year flight series provides information about atmospheric composition in the upper troposphere over Europe and Asia during all seasons and was used to investigate seasonal and regional differences in trace gas distributions and the influence of long range transport and local convection on composition. The flight route was separated into three different regions having characteristic differences in transp…

Water vapor increase in the northern lower stratosphere by the Asian monsoon anticyclone observed during TACTS/ESMVal campaigns

Abstract. The impact of air masses from Asia influenced by the Asian monsoon anticyclone on the northern hemispheric stratosphere is investigated based on in-situ measurements. An statistical significant increase in water vapor of about 0.5 ppmv (11 %) and methane up to 20 ppbv (1.2 %) in the extra-tropical stratosphere above a potential temperature of 380 K was detected between August and September 2012 by in-situ instrumentation in the northern hemisphere during the HALO aircraft mission TACTS and ESMVal. We investigate the origin of this water vapor and methane increase with the help of the three-dimensional Lagrangian chemistry transport model CLaMS. We assign the source of the moist ai…

Aircraft-based observation of meteoric material in lower stratospheric aerosol particles between 15 and 68&deg;&thinsp;N

In this paper we analyze aerosol particle composition measurements from five research missions conducted between 2014 and 2018 sampling the upper troposphere and lower stratosphere (UTLS), to assess the meridional extent of particles containing meteoric material. Additional data sets from a ground based study and from a low altitude aircraft mission are used to confirm the existence of meteoric material in lower tropospheric particles. Single particle laser ablation techniques with bipolar ion detection were used to measure the chemical composition of particles in a size range of approximately 150&thinsp;nm to 3&thinsp;μm. The five UTLS aircraft missions cover a latitude range from 15 to 68…