0000000000040767

AUTHOR

Christiane Voigt

0000-0001-8925-7731

Biofuel blending reduces particle emissions from aircraft engines at cruise conditions.

Aviation-related aerosol emissions contribute to the formation of contrail cirrus clouds that can alter upper tropospheric radiation and water budgets, and therefore climate1. The magnitude of air-traffic-related aerosol–cloud interactions and the ways in which these interactions might change in the future remain uncertain. Modelling studies of the present and future effects of aviation on climate require detailed information about the number of aerosol particles emitted per kilogram of fuel burned and the microphysical properties of those aerosols that are relevant for cloud formation. However, previous observational data at cruise altitudes are sparse for engines burning conventional fuel…

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Widespread persistent polar stratospheric ice clouds in the Arctic

Abstract. Despite a general decline in ozone depleting substances in the stratosphere due to the multi-national commitment to substantially reduce the emissions of their precursors, the magnitude of Arctic polar ozone loss has not decreased in recent years. Thus new observations at cold conditions can help to enhance our knowledge of polar stratospheric cloud (PSC) formation and life cycle which is of relevance for Arctic ozone loss. In the unique winter 2015/16, cold and persistent areas with temperatures below the ice frost point Tice developed in the Arctic stratosphere, caused by reduced perturbations of the polar vortex through planetary waves. Due to these extreme conditions, unpreced…

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Evidence for heterogeneous chlorine activation in the tropical UTLS

Airborne in-situ observations of ClO in the tropics were made during the TROCCINOX (Aracatuba, Brazil, February 2005) and SCOUT-O<sub>3</sub> (Darwin, Australia, November/December 2005) field campaigns. While during most flights significant amounts of ClO (≈10–20 parts per trillion, ppt) were present only in aged stratospheric air, instances of enhanced ClO mixing ratios of up to 40 ppt – significantly exceeding those expected from gas phase chemistry – were observed in air masses of a more tropospheric character. Most of these observations are associated with low temperatures or with the presence of cirrus clouds (often both), suggesting that cirrus ice particles and/or liquid …

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Comparing airborne and satellite retrievals of cloud optical thickness and particle effective radius using a spectral radiance ratio technique: two case studies for cirrus and deep convective clouds

Solar radiation reflected by cirrus and deep convective clouds (DCCs) was measured by the Spectral Modular Airborne Radiation Measurement System (SMART) installed on the German High Altitude and Long Range Research Aircraft (HALO) during the Mid-Latitude Cirrus (ML-CIRRUS) and the Aerosol, Cloud, Precipitation, and Radiation Interaction and Dynamic of Convective Clouds System – Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modelling and to the Global Precipitation Measurement (ACRIDICON-CHUVA) campaigns. On particular flights, HALO performed measurements closely collocated with overpasses of the Moderate Resolution Imaging Spectroradiometer (…

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Process-based microphysical characterization of a strong mid-latitude convective system using aircraft in situ cloud measurements

Clouds in the mixed-phase temperature regime impose a large uncertainty onto climate prediction models, in part due to incomplete knowledge of the degree of glaciation affecting cloud radiative properties. To achieve a better representation of these clouds, it is crucial to improve the understanding of ice nucleation and growth as well as microphysical properties determining the cloud phase. In this case study, we provide a rare data set of aircraft in situ measurements in a strong mid-latitude convective system extending from the boundary layer to the tropopause and aim to extend the sparse database of such measurements. Data were obtained with the research aircraft HALO and cloud properti…

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Global sensitivity of aviation NO<sub>x</sub> effects to the HNO<sub>3</sub>-forming channel of the HO<sub>2</sub> + NO reaction

Abstract. The impact of a recently proposed HNO3-forming channel of the HO2 + NO reaction on atmospheric ozone, methane and their precursors is assessed with the aim to investigate its effects on aviation NOx induced radiative forcing. The first part of the study addresses the differences in stratospheric and tropospheric HOx-NOx chemistry in general, by comparing a global climate simulation without the above reaction to two simulations with different rate coefficient parameterizations for HO2 + NO → HNO3. A possible enhancement of the reaction by humidity, as found by a laboratory study, particularly reduces the oxidation capacity of the atmosphere, increasing methane lifetime significantl…

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Evolution of CO2, SO2, HCl, and HNO3in the volcanic plumes from Etna

The volcanic plumes from degassing Etna (Italy) were extensively probed with instruments onboard the Deutsches Zentrum fur Luft- und Raumfahrt research aircraft Falcon during the contrail, volcano, and cirrus experiment CONCERT on 29/30 September 2011. Up to 10.4 ppmv SO2 and 0.3 ppmv HCl were detected with the atmospheric chemical ionization mass spectrometer AIMS at 3.1 km altitude and 20 km distance to the summit. HNO3 is the dominant reactive nitrogen component in the plumes. Linking aircraft and ground-based observations by Hybrid Single-Particle Lagrangian Integrated Trajectory dispersion modeling, we identify two crater plumes with different compositions primarily injected by the Boc…

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Lagrangian matches between observations from aircraft, lidar and radar in a warm conveyor belt crossing orography

Warm conveyor belts (WCBs) are important airstreams in extratropical cyclones, often leading to the formation of intense precipitation and the amplification of upper-level ridges. This study presents a case study that involves aircraft, lidar and radar observations in a WCB ascending from western Europe towards the Baltic Sea during the Hydrological Cycle in the Mediterranean Experiment (HyMeX) and T-NAWDEX-Falcon in October 2012, a preparatory campaign for the THORPEX North Atlantic Waveguide and Downstream Impact Experiment (T-NAWDEX). Trajectories were used to link different observations along the WCB, that is, to establish so-called Lagrangian matches between observations. To this aim, …

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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…

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Airborne Measurements of Contrail Ice Properties—Dependence on Temperature and Humidity

The largest share in the climate impact of aviation results from cirrus clouds. Here, the dependence of microphysical contrail ice properties and extinction on temperature and humidity is investigated. Contrail measurements were performed at various altitudes during the 2018 ECLIF II/NDMAX campaign with the NASA DC-8 chasing the DLR A320. Ice number concentrations and contrail extinction coefficients are largest at altitudes near 9.5 km, typical for short- and medium-range air traffic. At higher altitudes near 11.5 km, low ambient water vapor concentrations lead to smaller contrail particle sizes and lower extinction coefficients. In addition, contrails were detected below 8.2 km near the S…

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Comparing Airborne and Satellite Retrievals of Optical and Microphysical Properties of Cirrus and Deep Convective Clouds using a Radiance Ratio Technique

Abstract. Solar radiation reflected by cirrus and deep convective clouds (DCCs) was measured by the Spectral Modular Airborne Radiation Measurement System (SMART) installed on the German HALO (High Altitude and Long Range Research Aircraft) during the ML-CIRRUS and the ACRIDICON-CHUVA campaigns. In particular flights, HALO performed closely collocated measurements with overpasses of the Moderate Resolution Imaging Spectroradiometer (MODIS) on board of Aqua satellite. Based on the nadir upward radiance, the optical thickness τ and bulk particle effective radius reff of cirrus and DCC are retrieved using a radiance ratio algorithm which considers the cloud thermodynamic phase, the cloud verti…

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The ACRIDICON-CHUVA campaign: Studying tropical deep convective clouds and precipitation over Amazonia using the new German research aircraft HALO

Abstract Between 1 September and 4 October 2014, a combined airborne and ground-based measurement campaign was conducted to study tropical deep convective clouds over the Brazilian Amazon rain forest. The new German research aircraft, High Altitude and Long Range Research Aircraft (HALO), a modified Gulfstream G550, and extensive ground-based instrumentation were deployed in and near Manaus (State of Amazonas). The campaign was part of the German–Brazilian Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems–Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the GPM (Global Precipitatio…

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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…

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Measurement of low-ppm mixing ratios of water vapor in the upper troposphere and lower stratosphere using chemical ionization mass spectrometry

A chemical ionization mass spectrometer (CIMS) instrument has been developed for the fast, precise, and accurate measurement of water vapor (H2O) at low mixing ratios in the upper troposphere and lower stratosphere (UT/LS). A low-pressure flow of sample air passes through an ionization volume containing an α-particle radiation source, resulting in a cascade of ion-molecule reactions that produce hydronium ions (H3O+) from ambient H2O. The production of H3O+ ions from ambient H2O depends on pressure and flow through the ion source, which were tightly controlled in order to maintain the measurement sensitivity independent of changes in the airborne sampling environment. The instrument w…

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Airborne measurements of the nitric acid partitioning in persistent contrails

This study reports the first systematic measurements of nitric acid (HNO3) uptake in contrail ice particles at typical aircraft cruise altitudes. During the CIRRUS-III campaign cirrus clouds and almost 40 persistent contrails were probed with in situ instruments over Germany and Northern Europe in November 2006. Besides reactive nitrogen, water vapor, cloud ice water content, ice particle size distributions, and condensation nuclei were measured during 6 flights. Contrails with ages up to 12 h were detected at altitudes 10–11.5 km and temperatures 211–220 K. These contrails had a larger ice phase fraction of total nitric acid (HNO3ice/HNO3tot = 6%) than the ambient cirrus layers (3%). On av…

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Contrail Formation: Analysis of Sublimation Mechanisms

We study losses of ice crystals in a persistent, soot-rich contra i l in the wake behind a medium-sized aircraft at cru i se. Constrain i n g a model covering ice nucleation, growth, and subl i m a t i o n phases with a n aircraft data set, we track the subl i m a t i o n history over two minutes of cont r a i l age and rela t e ice crystal numbers to the number of soot particles emitted by th e aircraft engines.

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Impact of rocket exhaust plumes on atmospheric composition and climate – an overview

Rockets are the only direct anthropogenic emission sources into the upper atmosphere. Gaseous rocket emissions include CO, N2, H2, H2O, and CO2, while solid rocket motors (SRM) additionally inject significant amounts of aluminum oxide (Al2O3) particles and gaseous chlorine species into the atmosphere. These emissions strongly perturb local at- mospheric trace gas and aerosol distributions. Here, the previous aircraft measurements in various rocket exhaust plumes including several large space shuttle launch vehicles are compiled. The observed changes of the lower stratospheric composition in the near field are summarized.

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Aerosol concentrations determine the height of warm rain and ice initiation in convective clouds over the Amazon basin

Abstract. We have investigated how pollution aerosols affect the height above cloud base of rain and ice hydrometeor initiation and the subsequent vertical evolution of cloud droplet size and number concentrations in growing convective cumulus. For this purpose we used in-situ data of hydrometeor size distributions measured with instruments mounted on HALO (High Altitude and Long Range Research Aircraft) during the ACRIDICON-CHUVA campaign over the Amazon during September 2014. The results show that the height of rain initiation by collision and coalescence processes (Dr, in units of meters above cloud base) is linearly correlated with the number concentration of droplets (Nd in cm−3) nucle…

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Lagrangian matches between observations from aircraft, lidar and radar in an orographic warm conveyor belt

Warm conveyor belts (WCBs) are important airstreams in extratropical cyclones, often leading to the formation of intense precipitation and the amplification of upper-level ridges. This study presents a case study that involves aircraft, lidar and radar observations in a WCB ascending from western Europe towards the Baltic Sea during the Hydrological Cycle in the Mediterranean Experiment (HyMeX) and T-NAWDEX-Falcon in October 2012, a preparatory campaign for the THORPEX North Atlantic Waveguide and Downstream Impact Experiment (T-NAWDEX). Trajectories were used to link different observations along the WCB, that is, to establish so-called Lagrangian matches between observations. To this aim, …

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Susceptibility of contrail ice crystal numbers to aircraft soot particle emissions

We develop an idealized, physically-based model describing combined effects of ice nucleation and sublimation on ice crystal number during persistent contrail formation. Our study represents the first effort to predict ice numbers at the point where contrails transition into contrail cirrus—several minutes past formation—by connecting them to aircraft soot particle emissions and atmospheric supersaturation with respect to ice. Results averaged over an observed exponential distribution of ice supersaturation (mean value 15%) indicate that large reductions in soot particle numbers are needed to lower contrail ice crystal numbers significantly for soot emission indices around 1015 (kg-fuel)−1,…

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Observed and Simulated Variability of Droplet Spectral Dispersion in Convective Clouds Over the Amazon

In this study, the variability of the spectral dispersion of droplet size distributions (DSDs) in convective clouds is investigated. Analyses are based on aircraft measurements of growing cumuli near the Amazon basin, and on numerical simulations of an idealized ice‐free cumulus. In cleaner clouds, the relative dispersion ϵ, defined as the ratio of the standard deviation to the mean value of the droplet diameter, is negatively correlated with the ratio of the cloud water content (qc) to the adiabatic liquid water content (qa), while no strong correlation between ϵ and qc/qa is seen in polluted clouds. Bin microphysics numerical simulations suggest that these contrasting behaviors are associ…

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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…

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The impact of mineral dust on cloud formation during the Saharan dust event in April 2014 over Europe

A regional modeling study on the impact of desert dust on cloud formation is presented for a major Saharan dust outbreak over Europe from 2 to 5 April 2014. The dust event coincided with an extensive and dense cirrus cloud layer, suggesting an influence of dust on atmospheric ice nucleation. Using interactive simulation with the regional dust model COSMO-MUSCAT, we investigate cloud and precipitation representation in the model and test the sensitivity of cloud parameters to dust–cloud and dust–radiation interactions of the simulated dust plume. We evaluate model results with ground-based and spaceborne remote sensing measurements of aerosol and cloud properties, as well as the in situ meas…

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ML-CIRRUS: The Airborne Experiment on Natural Cirrus and Contrail Cirrus with the High-Altitude Long-Range Research Aircraft HALO

Abstract The Midlatitude Cirrus experiment (ML-CIRRUS) deployed the High Altitude and Long Range Research Aircraft (HALO) to obtain new insights into nucleation, life cycle, and climate impact of natural cirrus and aircraft-induced contrail cirrus. Direct observations of cirrus properties and their variability are still incomplete, currently limiting our understanding of the clouds’ impact on climate. Also, dynamical effects on clouds and feedbacks are not adequately represented in today’s weather prediction models. Here, we present the rationale, objectives, and selected scientific highlights of ML-CIRRUS using the G-550 aircraft of the German atmospheric science community. The first combi…

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Mountain waves modulate the water vapor distribution in the UTLS

Abstract. The water vapor distribution in the upper troposphere–lower stratosphere (UTLS) region has a strong impact on the atmospheric radiation budget. Transport and mixing processes on different scales mainly determine the water vapor concentration in the UTLS. Here, we investigate the effect of mountain waves on the vertical transport and mixing of water vapor. For this purpose we analyze measurements of water vapor and meteorological parameters recorded by the DLR Falcon and NSF/NCAR Gulfstream V research aircraft taken during the Deep Propagating Gravity Wave Experiment (DEEPWAVE) in New Zealand. By combining different methods, we develop a new approach to quantify location, direction…

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In Situ Observations of Ice Particle Losses in a Young Persistent Contrail

We describe results of in situ observations of a 1 to 2-min old contrail in the vortex Phase generated from soot-rich exhaust (> 10^15 emitted soot particles per kg-fuel burned). Simultaneous measurements of soot (EIsoot) and apparent ice (AEIice) particle number emission indices show a pronounced anti-correlation in the vertical contrail profile. AEIice decrease by about 75% with increasing distance below the contrail-producing aircraft,while EIsoot increase by an equivalent relative fraction, therefore strongly suggesting sublimation causing the ice particle losses. Quantifying these losses in measurements helps to validate and improve contrail parameterizations used to estimate the clima…

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The airborne mass spectrometer AIMS – Part 1: AIMS-H<sub>2</sub>O for UTLS water vapor measurements

Abstract. In the upper troposphere and lower stratosphere (UTLS), the accurate quantification of low water vapor concentrations has presented a significant measurement challenge. The instrumental uncertainties are passed on to estimates of H2O transport, cloud formation and the role of H2O in the UTLS energy budget and resulting effects on surface temperatures. To address the uncertainty in UTLS H2O determination, the airborne mass spectrometer AIMS-H2O, with in-flight calibration, has been developed for fast and accurate airborne water vapor measurements. We present a new setup to measure water vapor by direct ionization of ambient air. Air is sampled via a backward facing inlet that inclu…

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Aerosol layers from the 2008 eruptions of Mount Okmok and Mount Kasatochi: In situ upper troposphere and lower stratosphere measurements of sulfate and organics over Europe

In 2008 Mount Okmok and Mount Kasatochi started erupting on 12 July and 7 August, respectively, in the Aleutians, depositing emissions of trace gases and aerosols as high as 15.2 km into the atmosphere. During an aircraft campaign, conducted over Europe in between 27 October and 2 November 2008, the volcanic aerosol was measured by an Aerodyne aerosol mass spectrometer, capable of particle chemical composition measurements covering a size diameter range between 40 nm and 1 mm. In the volcanic aerosol layer enhanced submicron particulate sulfate concentrations of up to 2.0 mg m−3 standard temperature and pressure (STP) were observed between 8 and 12 km altitude, while background values …

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Comparing calculated microphysical properties of tropical convective clouds at cloud base with measurements during the ACRIDICON-CHUVA campaign

Abstract. Reliable aircraft measurements of cloud microphysical properties are essential for understanding liquid convective cloud formation. In September 2014, the properties of convective clouds were measured with a Cloud Combination Probe (CCP), a Cloud and Aerosol Spectrometer (CAS-DPOL), and a cloud condensation nuclei (CCN) counter on board the HALO (High Altitude and Long Range Research Aircraft) aircraft during the ACRIDICON-CHUVA campaign over the Amazon region. An intercomparison of the cloud drop size distributions (DSDs) and the cloud water content derived from the different instruments generally shows good agreement within the instrumental uncertainties. The objective of this s…

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In-situ observations of young contrails – overview and selected results from the CONCERT campaign

Lineshaped contrails were detected with the research aircraft Falcon during the CONCERT – CONtrail and Cirrus ExpeRimenT – campaign in October/November 2008. The Falcon was equipped with a set of instruments to measure the particle size distribution, shape, extinction and chemical composition as well as trace gas mixing ratios of sulfur dioxide (SO<sub>2</sub>), reactive nitrogen and halogen species (NO, NO<sub>y</sub>, HNO<sub>3</sub>, HONO, HCl), ozone (O<sub>3</sub>) and carbon monoxide (CO). During 12 mission flights over Europe, numerous contrails, cirrus clouds and a volcanic aerosol layer were probed at altitudes between 8.5 and 11.6 km…

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Aviation Contrail Cirrus and Radiative Forcing Over Europe During 6 Months of COVID‐19

Abstract The COVID‐19 pandemic led to a 72% reduction of air traffic over Europe in March–August 2020 compared to 2019. Modeled contrail cover declined similarly, and computed mean instantaneous radiative contrail forcing dropped regionally by up to 0.7 W m−2. Here, model predictions of cirrus optical thickness and the top‐of‐atmosphere outgoing longwave and reflected shortwave irradiances are tested by comparison to Meteosat‐SEVIRI‐derived data. The agreement between observations and modeled data is slightly better when modeled contrail cirrus contributions are included. The spatial distributions and diurnal cycles of the differences in these data between 2019 and 2020 are partially caused…

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Sensitivities of Amazonian clouds to aerosols and updraft speed

Abstract. The effects of aerosol particles and updraft speed on warm-phase cloud microphysical properties are studied in the Amazon region as part of the ACRIDICON-CHUVA experiment. Here we expand the sensitivity analysis usually found in the literature by concomitantly considering cloud evolution, putting the sensitivity quantifications into perspective in relation to in-cloud processing, and by considering the effects on droplet size distribution (DSD) shape. Our in situ aircraft measurements over the Amazon Basin cover a wide range of particle concentration and thermodynamic conditions, from the pristine regions over coastal and forested areas to the southern Amazon, which is highly poll…

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In situ measurements of ice saturation in young contrails

Relative humidity with respect to ice (RHi) is a major factor controlling the evolution of aircraft contrails. High-resolution airborne H2O measurements in and near contrails were made at a rate of 4.2 Hz using the novel water vapor mass spectrometer AIMS-H2O with in-flight calibration during the CONtrail, volcano, and Cirrus ExpeRimenT (CONCERT) 2011. Three 2 min old contrails were sampled near 11 km altitude. Independent of the ambient supersaturation or subsaturation over ice, the mean of the RHi frequency distribution within each contrail is shifted toward ice saturation. This shift can be explained by the high ice surface area densities with corresponding RHi relaxation times on the or…

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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…

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Comparing parameterized versus measured microphysical properties of tropical convective cloud bases during the ACRIDICON–CHUVA campaign

The objective of this study is to validate parameterizations that were recently developed for satellite retrievals of cloud condensation nuclei supersaturation spectra, NCCN(S), at cloud base alongside more traditional parameterizations connecting NCCN(S) with cloud base updrafts and drop concentrations. This was based on the HALO aircraft measurements during the ACRIDICON–CHUVA campaign over the Amazon region, which took place in September 2014. The properties of convective clouds were measured with a cloud combination probe (CCP), a cloud and aerosol spectrometer (CAS-DPOL), and a CCN counter onboard the HALO aircraft. An intercomparison of the cloud drop size distributions (DSDs) and the…

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Contrail ice particles in aircraft wakes and their climatic importance

[1] Measurements of gaseous (NO, NOy, SO2, HONO) and ice particle concentrations in young contrails in primary and secondary wakes of aircraft of different sizes (B737, A319, A340, A380) are used to investigate ice particle formation behind aircraft. The gas concentrations are largest in the primary wake and decrease with increasing altitude in the secondary wake, as expected for passive trace gases and aircraft-dependent dilution. In contrast, the measured ice particle concentrations were found larger in the secondary wake than in the primary wake. The contrails contain more ice particles than expected for previous black carbon (soot) estimates. The ice concentrations may result from soot-…

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The airborne mass spectrometer AIMS – Part 2: Measurements of trace gases with stratospheric or tropospheric origin in the UTLS

Understanding the role of climate-sensitive trace gas variabilities in the upper troposphere and lower stratosphere region (UTLS) and their impact on its radiative budget requires accurate measurements. The composition of the UTLS is governed by transport and chemistry of stratospheric and tropospheric constituents, such as chlorine, nitrogen oxide and sulfur compounds. The Atmospheric chemical Ionization Mass Spectrometer AIMS has been developed to accurately measure a set of these constituents on aircraft by means of chemical ionization. Here we present a setup using SF5− reagent ions for the simultaneous measurement of trace gas concentrations of HCl, HNO3 and SO2 in the  pptv to ppmv (1…

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Cloud droplet number closure for tropical convective clouds during the ACRIDICON–CHUVA campaign

The main objective of the ACRIDICON-CHUVA (Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems–Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the Global Precipitation measurements) campaign in September 2014 was the investigation of aerosol-cloud-interactions in the Amazon Basin. Cloud properties near cloud base of growing convective cumuli were characterized by cloud droplet size distribution measurements using a cloud combination probe (CCP) and a cloud and aerosol spectrometer (CAS-DPOL). In the current study, an adiabatic parcel model was used to perform cloud droplet number (N…

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Characterization of a Newly Developed Aircraft-Based Laser Ablation Aerosol Mass Spectrometer (ALABAMA) and First Field Deployment in Urban Pollution Plumes over Paris During MEGAPOLI 2009

We present here the development and first field deployment of a novel Aircraft-based Laser ABlation Aerosol MAss spectrometer (ALABAMA), which is capable of measuring the chemical composition and size of individual ambient aerosol particles in the size range between 150 and 900 nm. The instrument uses a continuous wave 532 nm laser to size and detect the particles, a pulsed 266 nm laser to ablate and ionize the particles, and a bipolar, Z-shaped time-of-flight mass spectrometer to detect positive and negative ions. The ALABAMA fits into a 19"-aircraft rack of 150 cm height and has a total weight of 140 kg, thus currently being one of the smallest and lightest-weight instruments of its type.…

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Linear relationship between effective radius and precipitation water content near the top of convective clouds

Quantifying the precipitation within clouds is a crucial challenge to improve our current understanding of the Earth’s hydrological cycle. We have investigated the relationship between the effective radius of droplets and ice particles (re) and precipitation water content (PWC) measured by cloud probes near the top of growing convective cumuli. The data for this study were collected by aircraft measurements in clean and polluted conditions over the Amazon Basin and over the western tropical Atlantic in September 2014. Our results indicate a threshold of re ∼ 13 μm for warm rain initiation in convective clouds, which is in agreement with previous studies. In…

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Measurements of HONO, NO, NOyand SO2in aircraft exhaust plumes at cruise

Measurements of gaseous nitrogen and sulfur oxide emissions in young aircraft exhaust plumes give insight into chemical oxidation processes inside aircraft engines. Particularly, the OHA¢Â�Â�induced formation of nitrous acid (HONO) from nitrogen oxide (NO) and sulfuric acid (H2SO4) from sulfur dioxide (SO2) inside the turbine which is highly uncertain, need detailed analysis to address the climate impact of aviation. We report on airborne in situ measurements at cruise altitudes of HONO, NO, NOy, and SO2 in 9 wakes of 8 different types of modern jet airliners, including for the first time also an A380. Measurements of HONO and SO2 were made with an ITCIMS (Ion Trap Chemical Ionization Mass …

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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…

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The challenge of simulating the sensitivity of the Amazonian clouds microstructure to cloud condensation nuclei number concentrations

The realistic representation of cloud-aerosol interactions is of primary importance for accurate climate model projections. The investigation of these interactions in strongly contrasting clean and polluted atmospheric conditions in the Amazon area has been one of the motivations for several field observations, including the airborne Aerosol, Cloud, Precipitation, and Radiation Interactions and DynamIcs of CONvective cloud systems – Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the GPM (Global Precipitation Measurement) (ACRIDICON-CHUVA) campaign based in Manaus, Brazil in September 2014. In this work we combine in situ …

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The Pagami Creek smoke plume after long-range transport to the upper troposphere over Europe – aerosol properties and black carbon mixing state

Abstract. During the CONCERT 2011 field experiment with the DLR research aircraft Falcon, an enhanced aerosol layer with particle linear depolarization ratios of 6–8% at 532 nm was observed at altitudes above 10 km over northeast Germany on 16 September 2011. Dispersion simulations with HYSPILT suggest that the elevated aerosol layer originated from the Pagami Creek forest fire in Minnesota, USA, which caused pyro-convective uplift of particles and gases. The 3–4 day-old smoke plume had high total refractory black carbon (rBC) mass concentrations of 0.03–0.35 μg m−3 at standard temperature and pressure (STP) with rBC mass equivalent diameter predominantly smaller than 130 nm. Assuming a cor…

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The evolution of microphysical and optical properties of an A380 contrail in the vortex phase

A contrail from a large-body A380 aircraft at cruise in the humid upper troposphere has been probed with in-situ instruments onboard the DLR research aircraft Falcon. The contrail was sampled during 700 s measurement time at contrail ages of about 1–4 min. The contrail was in the vortex regime during which the primary wake vortices were sinking 270 m below the A380 flight level while the secondary wake remained above. Contrail properties were sampled separately in the primary wake at 90 and 115 s contrail age and nearly continously in the secondary wake at contrail ages from 70 s to 220 s. The scattering phase functions of the contrail particles were measured with a polar nephelometer. The …

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Linear relationship between effective radius and precipitation water content near the top of convective clouds: measurement results from ACRIDICON–CHUVA campaign

Quantifying the precipitation within clouds is a crucial challenge to improve our current understanding of the Earth's hydrological cycle. We have investigated the relationship between the effective radius of droplets and ice particles (re) and precipitation water content (PWC) measured by cloud probes near the top of growing convective cumuli. The data for this study were collected during the ACRIDICON–CHUVA campaign on the HALO research aircraft in clean and polluted conditions over the Amazon Basin and over the western tropical Atlantic in September 2014. Our results indicate a threshold of re∼13 µm for warm rain initiation in convective clouds, which is in agreement with previous studie…

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Air traffic and contrail changes during COVID-19 over Europe: A model study

The strong reduction of air traffic during the COVID-19 pandemic provides a test case for the relation between air traffic density, contrails, and their radiative forcing of climate change. Air traffic and contrail cirrus changes are quantified for a European domain for March to August 2020 and compared to the same period in 2019. Traffic data show a 72 % reduction in flight distance compared with 2019. This paper investigates the induced contrail changes in a model study. The contrail model results depend on various methodological details tested in parameter studies. In the reference case, the reduced traffic caused an even stronger reduction in contrail length, partly because the w…

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Nitric Acid Trihydrate (NAT) formation at low NAT supersaturation in Polar Stratospheric Clouds (PSCs)

International audience; A PSC was detected on 6 February 2003 in the Arctic stratosphere by in-situ measurements onboard the high-altitude research aircraft Geophysica. Low number densities (~10-4cm-3) of small nitric acid (HNO3) containing particles (dTNAT, these NAT particles have the potential to grow further and to remove HNO3 from the stratosphere, thereby enhancing polar ozone loss. Interestingly, the NAT particles formed in less than a day at temperatures just slightly below TNAT (T>TNAT-3.1K). This unique measurement of PSC formation at extremely low NAT saturation ratios (SNAT?10) constrains current NAT nucleation theories. We suggest, that the NAT particles have formed heterogeneo…

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Cloud droplet formation at the base of tropical convective clouds: closure between modeling and measurement results of ACRIDICON–CHUVA

Aerosol–cloud interactions contribute to the large uncertainties in current estimates of climate forcing. We investigated the effect of aerosol particles on cloud droplet formation by model calculations and aircraft measurements over the Amazon and over the western tropical Atlantic during the ACRIDICON–CHUVA campaign in September 2014. On the HALO (High Altitude Long Range Research) research aircraft, cloud droplet number concentrations (Nd) were measured near the base of clean and polluted growing convective cumuli using a cloud combination probe (CCP) and a cloud and aerosol spectrometer (CAS-DPOL). An adiabatic parcel model was used to perform cloud droplet number closure studies for fl…

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Design, construction and commissioning of the Braunschweig Icing Wind Tunnel

Beyond its physical importance in both fundamental and climate research, atmospheric icing is considered as a severe operational condition in many engineering applications like aviation, electrical power transmission and wind-energy production. To reproduce such icing conditions in a laboratory environment, icing wind tunnels are frequently used. In this paper, a comprehensive overview on the design, construction and commissioning of the Braunschweig Icing Wind Tunnel is given. The tunnel features a test section of 0.5 m  ×  0.5 m with peak velocities of up to 40 m s−1. The static air temperature ranges from −25 to +30 °C. Supercooled droplet icing with liquid water contents up to 3 g m−3 c…

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Long-lived contrails and convective cirrus above the tropical tropopause

Abstract. This study has two objectives: (1) it characterizes contrails at very low temperatures and (2) it discusses convective cirrus in which the contrails occurred. (1) Long-lived contrails and cirrus from overshooting convection are investigated above the tropical tropopause at low temperatures down to −88 °C from measurements with the Russian high-altitude research aircraft M-55 Geophysica, as well as related observations during the SCOUT-O3 field experiment near Darwin, Australia, in 2005. A contrail was observed to persist below ice saturation at low temperatures and low turbulence in the stratosphere for nearly 1 h. The contrail occurred downwind of the decaying convective system H…

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Contrail formation in the tropopause region caused by emissions from an Ariane 5 rocket

Rockets directly inject water vapor and aerosol into the atmosphere, which promotes the formation of ice clouds in ice supersaturated layers of the atmosphere. Enhanced mesospheric cloud occurrence has frequently been detected near 80 km altitude a few days after rocket launches. Here, we present unique evidence for cirrus formation in the tropopause region caused by ice nucleation in the exhaust plume from an Ariane 5-ECA rocket. Meteorological reanalysis data from the European Centre for Medium-Range Weather Forecasts show significant ice supersaturation at the 100 hPa level in the American tropical tropopause region on 26 November 2011. Near 17 km altitudes temperatures are below the Sch…

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Aircraft type influence on contrail properties

The investigation of the impact of aircraft parameters on contrail properties helps to better understand the climate impact from aviation. Yet, in observations, it is a challenge to separate aircraft and meteorological influences on contrail formation. During the CONCERT campaign in November 2008, contrails from 3 Airbus passenger aircraft of types A319-111, A340-311 and A380-841 were probed at cruise under similar meteorological conditions with in situ instruments on board DLR research aircraft Falcon. Within the 2 min-old contrails detected near ice saturation, we find similar effective diameters Deff (5.2–5.9 μm), but differences in particle number densities nice (162–235 cm−3) and…

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Potential of airborne lidar measurements for cirrus cloud studies

Abstract. Aerosol and water vapour measurements were performed with the lidar system WALES of Deutsches Zentrum für Luft- und Raumfahrt (DLR) in October and November 2010 during the first mission with the new German research aircraft G55-HALO. Curtains composed of lidar profiles beneath the aircraft show the vertical and horizontal distribution and variability of water vapour mixing ratio and backscatter ratio above Germany. Two missions on 3 and 4 November 2010 were selected to derive the water vapour mixing ratio inside cirrus clouds from the lidar instrument. A good agreement was found with in situ observations performed on a second research aircraft flying below HALO. ECMWF analysis tem…

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Extinction and optical depth of contrails

[1] One factor limiting the understanding of the climate impact from contrails and aircraft induced cloud modifications is the accurate determination of their optical depth. To this end, 14 contrails were sampled for 2756 s with instruments onboard the research aircraft Falcon during the CONCERT (CONtrail and Cirrus ExpeRimenT) campaign in November 2008. The young (<10 min old) contrails were produced by 9 commercial aircraft with weights of 47 to 508 t, among them the largest operating passenger aircraft, the Airbus A380. The contrails were observed at temperatures between 214 and 224 K and altitudes between 8.8 and 11.1 km. The measured mean in-contrail relative humidity with respect to i…

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Detection of reactive nitrogen containing particles in the tropopause region? Evidence for a tropical nitric acid trihydrage (NAT) belt

The detection of nitric acid trihydrate (NAT, HNO&lt;sub&gt;3&lt;/sub&gt;&amp;times;3H&lt;sub&gt;2&lt;/sub&gt;O) particles in the tropical transition layer (TTL) harmonizes our understanding of polar stratospheric cloud formation. Large reactive nitrogen (NO&lt;sub&gt;y&lt;/sub&gt;) containing particles were observed on 8 August 2006 by instruments onboard the high altitude research aircraft M55-Geophysica near and below the tropical tropopause. The particles, most likely NAT, have diameters less than 6 &amp;mu;m and concentrations below 10&lt;sup&gt;-4&lt;/sup&gt; cm&lt;sup&gt;&amp;minus;3&lt;/sup&gt;. The NAT particle layer was repeatedly detected at altitudes between 15.1 and 17.5 km ove…

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Evaluation of simulated CO2 power plant plumes from six high-resolution atmospheric transport models

Power plants and large industrial facilities contribute more than half of global anthropogenic CO2 emissions. Quantifying the emissions of these point sources is therefore one of the main goals of the planned constellation of anthropogenic CO2 monitoring satellites (CO2M) of the European Copernicus program. Atmospheric transport models may be used to study the capabilities of such satellites through observing system simulation experiments and to quantify emissions in an inverse modeling framework. How realistically the CO2 plumes of power plants can be simulated and how strongly the results may depend on model type and resolution, however, is not well known due to a lack of observations ava…

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Further evidence for CCN aerosol concentrations determining the height of warm rain and ice initiation in convective clouds over the Amazon basin

We have investigated how aerosols affect the height above cloud base of rain and ice hydrometeor initiation and the subsequent vertical evolution of cloud droplet size and number concentrations in growing convective cumulus. For this purpose we used in situ data of hydrometeor size distributions measured with instruments mounted on HALO aircraft during the ACRIDICON–CHUVA campaign over the Amazon during September 2014. The results show that the height of rain initiation by collision and coalescence processes (Dr, in units of meters above cloud base) is linearly correlated with the number concentration of droplets (Nd in cm−3) nucleated at cloud base (Dr ≈ 5 ⋅ Nd). Additional cloud processes…

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Properties of individual contrails: a compilation of observations and some comparisons

International audience; Mean properties of individual contrails are characterized for a wide range of jet aircraft as a function of age during their life cycle from seconds to 11.5 h (7.4-18.7 km altitude, -88 to -31 °C ambient temperature), based on a compilation of about 230 previous in situ and remote sensing measurements. The airborne, satellite, and ground-based observations encompass exhaust contrails from jet aircraft from 1972 onwards, as well as a few older data for propeller aircraft. The contrails are characterized by mean ice particle sizes and concentrations, extinction, ice water content, optical depth, geometrical depth, and contrail width. Integral contrail properties includ…

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Enhanced sulfur in the upper troposphere and lower stratosphere in spring 2020

Sulfur compounds in the upper troposphere and lower stratosphere (UTLS) impact the atmosphere radiation budget, either directly as particles or indirectly as precursor gas for new particle formation. In situ measurements in the UTLS are rare but are important to better understand the impact of the sulfur budget on climate. The BLUESKY mission in May and June 2020 explored an unprecedented situation. (1) The UTLS experienced extraordinary dry conditions in spring 2020 over Europe, in comparison to previous years, and (2) the first lockdown of the COVID-19 pandemic caused major emission reductions from industry, ground, and airborne transportation. With the two research aircraft HALO and Falc…

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In-situ observations and modeling of small nitric acid-containing ice crystals

Measurements in nascent ice forming regions are very rare and help understand cirrus cloud formation and the interactions of trace gases with ice crystals. A tenuous cirrus cloud has been probed with in-situ and remote sensing instruments onboard the high altitude research aircraft Geophysica M55 in the tropical upper troposphere. Besides microphysical and optical particle properties, water (H&lt;sub&gt;2&lt;/sub&gt;O) and reactive nitrogen species (NO&lt;sub&gt;y&lt;/sub&gt;) have been measured. In slightly ice supersaturated air between 14.2 and 14.9 km altitude, an unusually low ice water content of 0.031 mg m&lt;sup&gt;&amp;minus;3&lt;/sup&gt; and small ice crystals with mean radii of 5…

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Sensitivity of low-level clouds and precipitation to anthropogenic aerosol emission in southern West Africa: a DACCIWA case study

Abstract. During the West African summer monsoon, pollutants emitted in urbanized coastal areas modify cloud cover and precipitation patterns. The Dynamics-Aerosol-Chemistry-Cloud-Interactions in West Africa (DACCIWA) field campaign provided numerous aircraft-based and ground-based observations, which are used here to evaluate two experiments made with the coupled WRF-CHIMERE model, integrating both the direct and indirect aerosol effect on meteorology. During one well-documented week (1–7 July 2016), the impacts of anthropogenic aerosols on the diurnal cycle of low-level clouds and precipitation are analyzed in detail using high and moderate intensity of anthropogenic emissions in the expe…

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