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  • 1
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 15, No. 9 ( 2022-05-11), p. 2889-2921
    Abstract: Abstract. In this paper, we present the design, development, and characteristics of the novel aerosol mass spectrometer ERICA (ERC Instrument for Chemical composition of Aerosols; ERC – European Research Council) and selected results from the first airborne field deployment. The instrument combines two well-established methods of real-time in situ measurements of fine particle chemical composition. The first method is the laser desorption and ionization technique, or laser ablation technique, for single-particle mass spectrometry (here with a frequency-quadrupled Nd:YAG laser at λ = 266 nm). The second method is a combination of thermal particle desorption, also called flash vaporization, and electron impact ionization (like the Aerodyne aerosol mass spectrometer). The same aerosol sample flow is analyzed using both methods simultaneously, each using time-of-flight mass spectrometry. By means of the laser ablation, single particles are qualitatively analyzed (including the refractory components), while the flash vaporization and electron impact ionization technique provides quantitative information on the non-refractory components (i.e., particulate sulfate, nitrate, ammonia, organics, and chloride) of small particle ensembles. These techniques are implemented in two consecutive instrument stages within a common sample inlet and a common vacuum chamber. At its front end, the sample air containing the aerosol particles is continuously injected via an aerodynamic lens. All particles which are not ablated by the Nd:YAG laser in the first instrument stage continue their flight until they reach the second instrument stage and impact on the vaporizer surface (operated at 600 ∘C). The ERICA is capable of detecting single particles with vacuum aerodynamic diameters (dva) between ∼ 180 and 3170 nm (d50 cutoff). The chemical characterization of single particles is achieved by recording cations and anions with a bipolar time-of-flight mass spectrometer. For the measurement of non-refractory components, the particle size range extends from approximately 120 to 3500 nm (d50 cutoff; dva), and the cations are detected with a time-of-flight mass spectrometer. The compact dimensions of the instrument are such that the ERICA can be deployed on aircraft, at ground stations, or in mobile laboratories. To characterize the focused detection lasers, the ablation laser, and the particle beam, comprehensive laboratory experiments were conducted. During its first deployments the instrument was fully automated and operated during 11 research flights on the Russian high-altitude research aircraft M-55 Geophysica from ground pressure and temperature to 20 km altitude at 55 hPa and ambient temperatures as low as −86 ∘C. In this paper, we show that the ERICA is capable of measuring reliably under such conditions.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2022
    detail.hit.zdb_id: 2505596-3
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  • 2
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 16, No. 13 ( 2016-07-12), p. 8405-8421
    Abstract: Abstract. Stratospheric aerosol particles with diameters larger than about 10 nm were collected within the arctic vortex during two polar flight campaigns: RECONCILE in winter 2010 and ESSenCe in winter 2011. Impactors were installed on board the aircraft M-55 Geophysica, which was operated from Kiruna, Sweden. Flights were performed at a height of up to 21 km and some of the particle samples were taken within distinct polar stratospheric clouds (PSCs). The chemical composition, size and morphology of refractory particles were analyzed by scanning electron microscopy and energy-dispersive X-ray microanalysis. During ESSenCe no refractory particles with diameters above 500 nm were sampled. In total 116 small silicate, Fe-rich, Pb-rich and aluminum oxide spheres were found. In contrast to ESSenCe in early winter, during the late-winter RECONCILE mission the air masses were subsiding inside the Arctic winter vortex from the upper stratosphere and mesosphere, thus initializing a transport of refractory aerosol particles into the lower stratosphere. During RECONCILE, 759 refractory particles with diameters above 500 nm were found consisting of silicates, silicate ∕ carbon mixtures, Fe-rich particles, Ca-rich particles and complex metal mixtures. In the size range below 500 nm the presence of soot was also proven. While the data base is still sparse, the general tendency of a lower abundance of refractory particles during PSC events compared to non-PSC situations was observed. The detection of large refractory particles in the stratosphere, as well as the experimental finding that these particles were not observed in the particle samples (upper size limit ∼  5 µm) taken during PSC events, strengthens the hypothesis that such particles are present in the lower polar stratosphere in late winter and have provided a surface for heterogeneous nucleation during PSC formation.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2016
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 3
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 9, No. 10 ( 2016-10-20), p. 5135-5162
    Abstract: Abstract. Particle concentration measurements with underwing probes on aircraft are impacted by air compression upstream of the instrument body as a function of flight velocity. In particular, for fast-flying aircraft the necessity arises to account for compression of the air sample volume. Hence, a correction procedure is needed to invert measured particle number concentrations to ambient conditions that is commonly applicable to different instruments to gain comparable results. In the compression region where the detection of particles occurs (i.e. under factual measurement conditions), pressure and temperature of the air sample are increased compared to ambient (undisturbed) conditions in certain distance away from the aircraft. Conventional procedures for scaling the measured number densities to ambient conditions presume that the air volume probed per time interval is determined by the aircraft speed (true air speed, TAS). However, particle imaging instruments equipped with pitot tubes measuring the probe air speed (PAS) of each underwing probe reveal PAS values systematically below those of the TAS. We conclude that the deviation between PAS and TAS is mainly caused by the compression of the probed air sample. From measurements during two missions in 2014 with the German Gulfstream G-550 (HALO – High Altitude LOng range) research aircraft we develop a procedure to correct the measured particle concentration to ambient conditions using a thermodynamic approach. With the provided equation, the corresponding concentration correction factor ξ is applicable to the high-frequency measurements of the underwing probes, each of which is equipped with its own air speed sensor (e.g. a pitot tube). ξ values of 1 to 0.85 are calculated for air speeds (i.e. TAS) between 60 and 250 m s−1. For different instruments at individual wing position the calculated ξ values exhibit strong consistency, which allows for a parameterisation of ξ as a function of TAS for the current HALO underwing probe configuration. The ability of cloud particles to adopt changes of air speed between ambient and measurement conditions depends on the cloud particles' inertia as a function of particle size (diameter Dp). The suggested inertia correction factor μ (Dp) for liquid cloud drops ranges between 1 (for Dp 〈 70 µm) and 0.8 (for 100 µm 〈 Dp 〈 225 µm) but it needs to be applied carefully with respect to the particles' phase and nature. The correction of measured concentration by both factors, ξ and μ (Dp), yields higher ambient particle concentration by about 10–25 % compared to conventional procedures – an improvement which can be considered as significant for many research applications. The calculated ξ values are specifically related to the considered HALO underwing probe arrangement and may differ for other aircraft. Moreover, suggested corrections may not cover all impacts originating from high flight velocities and from interferences between the instruments and e.g. the aircraft wings and/or fuselage. Consequently, it is important that PAS (as a function of TAS) is individually measured by each probe deployed underneath the wings of a fast-flying aircraft.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2016
    detail.hit.zdb_id: 2505596-3
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  • 4
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 17, No. 12 ( 2017-06-20), p. 7365-7386
    Abstract: Abstract. 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 cloud water content (CWC) derived from the different instruments generally shows good agreement within the instrumental uncertainties. To this end, the directly measured cloud drop concentrations (Nd) near cloud base were compared with inferred values based on the measured cloud base updraft velocity (Wb) and NCCN(S) spectra. The measurements of Nd at cloud base were also compared with drop concentrations (Na) derived on the basis of an adiabatic assumption and obtained from the vertical evolution of cloud drop effective radius (re) above cloud base. The measurements of NCCN(S) and Wb reproduced the observed Nd within the measurements uncertainties when the old (1959) Twomey's parameterization was used. The agreement between the measured and calculated Nd was only within a factor of 2 with attempts to use cloud base S, as obtained from the measured Wb, Nd, and NCCN(S). This underscores the yet unresolved challenge of aircraft measurements of S in clouds. Importantly, the vertical evolution of re with height reproduced the observation-based nearly adiabatic cloud base drop concentrations, Na. The combination of these results provides aircraft observational support for the various components of the satellite-retrieved methodology that was recently developed to retrieve NCCN(S) under the base of convective clouds. This parameterization can now be applied with the proper qualifications to cloud simulations and satellite retrievals.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2017
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 5
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 18, No. 13 ( 2018-07-12), p. 9803-9822
    Abstract: Abstract. Air traffic affects cloudiness, and thus climate, by emitting exhaust gases and particles. The study of the evolution of contrail properties is very challenging due to the complex interplay of vortex dynamics and the atmospheric environment (e.g. temperature, supersaturation). Despite substantial progress in recent years, the optical, microphysical, and macrophysical properties of contrails and ambient cirrus during contrail formation and subsequent ageing are still subject to large uncertainties due to instrumental and observational limitations and the large number of variables influencing the contrail life cycle. In this study, various contrail cases corresponding to different aircraft types and atmospheric conditions are investigated using a statistical method based on the in situ optical measurements performed during the Contrail and Cirrus Experiments (CONCERT) campaigns 2008 and 2011. The two aircraft campaigns encompass more than 17 aircraft contrail cases. A principal component analysis (PCA) of the angular scattering coefficients measured by the polar nephelometer is implemented. The goal is to classify the sampled ice cloud measurements in several clusters representative of different contrail development stages (primary wake, young contrail, aged contrail, and cirrus). Extinction and asymmetry coefficients, nitrogen oxide concentrations, and relative humidity with respect to ice and particle size distributions are analysed for each cluster to characterize the evolution of ice cloud properties during the contrail to cirrus evolution. The PCA demonstrates that contrail optical properties are well suited to identify and discriminate between the different contrail growth stages and to characterize the evolution of contrail properties.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2018
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 6
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 13, No. 7 ( 2020-07-08), p. 3651-3660
    Abstract: Abstract. We present a novel and compact design of a constant-pressure inlet (CPI) developed for use in airborne aerosol mass spectrometry. In particular, the inlet system is optimized for aerodynamic lenses commonly used in aerosol mass spectrometers, in which efficient focusing of aerosol particles into a vacuum chamber requires a precisely controlled lens pressure, typically of a few hectopascals. The CPI device can also be used in condensation particle counters (CPCs), cloud condensation nucleus counters (CCNCs), and gas-phase sampling instruments across a wide range of altitudes and inlet pressures. The constant pressure is achieved by changing the inner diameter of a properly scaled O-ring that acts as a critical orifice. The CPI control keeps air pressure and thereby mass flow rate (≈0.1 L min−1) upstream of an aerodynamic lens constant, deviating at most by only ±2 % from a preset value. In our setup, a pressure sensor downstream of the O-ring maintains control of the pinch mechanism via a feedback loop and setpoint conditions are reached within seconds. The device was implemented in a few instruments, which were successfully operated on different research aircraft covering a wide range of ambient pressures, from sea level up to about 55 hPa. Details of operation and the quality of aerosol particle transmission were evaluated by laboratory experiments and in-flight data with a single-particle mass spectrometer.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2020
    detail.hit.zdb_id: 2505596-3
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  • 7
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 17, No. 23 ( 2017-12-11), p. 14727-14746
    Abstract: Abstract. The behavior of tropical clouds remains a major open scientific question, resulting in poor representation by models. One challenge is to realistically reproduce cloud droplet size distributions (DSDs) and their evolution over time and space. Many applications, not limited to models, use the gamma function to represent DSDs. However, even though the statistical characteristics of the gamma parameters have been widely studied, there is almost no study dedicated to understanding the phase space of this function and the associated physics. This phase space can be defined by the three parameters that define the DSD intercept, shape, and curvature. Gamma phase space may provide a common framework for parameterizations and intercomparisons. Here, we introduce the phase space approach and its characteristics, focusing on warm-phase microphysical cloud properties and the transition to the mixed-phase layer. We show that trajectories in this phase space can represent DSD evolution and can be related to growth processes. Condensational and collisional growth may be interpreted as pseudo-forces that induce displacements in opposite directions within the phase space. The actually observed movements in the phase space are a result of the combination of such pseudo-forces. Additionally, aerosol effects can be evaluated given their significant impact on DSDs. The DSDs associated with liquid droplets that favor cloud glaciation can be delimited in the phase space, which can help models to adequately predict the transition to the mixed phase. We also consider possible ways to constrain the DSD in two-moment bulk microphysics schemes, in which the relative dispersion parameter of the DSD can play a significant role. Overall, the gamma phase space approach can be an invaluable tool for studying cloud microphysical evolution and can be readily applied in many scenarios that rely on gamma DSDs.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2017
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 8
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 16, No. 18 ( 2016-09-23), p. 11883-11897
    Abstract: Abstract. Aerosols of the volcanic degassing plumes from Mt. Etna and Mt. Stromboli were probed with in situ instruments on board the Deutsches Zentrum für Luft- und Raumfahrt research aircraft Falcon during the contrail, volcano, and cirrus experiment CONCERT in September 2011. Aerosol properties were analyzed using angular-scattering intensities and particle size distributions measured simultaneously with the Polar Nephelometer and the Forward Scattering Spectrometer probes (FSSP series 100 and 300), respectively. Aerosols of degassing plumes are characterized by low values of the asymmetry parameter (between 0.6 and 0.75); the effective diameter was within the range of 1.5–2.8 µm and the maximal diameter was lower than 20 µm. A principal component analysis applied to the Polar Nephelometer data indicates that scattering features of volcanic aerosols of different crater origins are clearly distinctive from angular-scattering intensities of cirrus and contrails. Retrievals of aerosol properties revealed that the particles were "optically spherical" and the estimated values of the real part of the refractive index are within the interval from 1.35 to 1.38. The interpretation of these results leads to the conclusion that the degassing plume aerosols were porous with air voids. Our estimates suggest that aerosol particles contained about 18 to 35 % of air voids in terms of the total volume.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2016
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 9
    In: Bulletin of the American Meteorological Society, American Meteorological Society, Vol. 98, No. 2 ( 2017-02-01), p. 271-288
    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 combined in situ–remote sensing cloud mission with HALO united state-of-the-art cloud probes, a lidar and novel ice residual, aerosol, trace gas, and radiation instrumentation. The aircraft observations were accompanied by remote sensing from satellite and ground and by numerical simulations. In spring 2014, HALO performed 16 flights above Europe with a focus on anthropogenic contrail cirrus and midlatitude cirrus induced by frontal systems including warm conveyor belts and other dynamical regimes (jet streams, mountain waves, and convection). Highlights from ML-CIRRUS include 1) new observations of microphysical and radiative cirrus properties and their variability in meteorological regimes typical for midlatitudes, 2) insights into occurrence of in situ–formed and lifted liquid-origin cirrus, 3) validation of cloud forecasts and satellite products, 4) assessment of contrail predictability, and 5) direct observations of contrail cirrus and their distinction from natural cirrus. Hence, ML-CIRRUS provides a comprehensive dataset on cirrus in the densely populated European midlatitudes with the scope to enhance our understanding of cirrus clouds and their role for climate and weather.
    Type of Medium: Online Resource
    ISSN: 0003-0007 , 1520-0477
    Language: English
    Publisher: American Meteorological Society
    Publication Date: 2017
    detail.hit.zdb_id: 2029396-3
    detail.hit.zdb_id: 419957-1
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  • 10
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 21, No. 2 ( 2021-01-26), p. 989-1013
    Abstract: Abstract. 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 composition of particles in a diameter range of approximately 150 nm to 3 µm. The five UTLS aircraft missions cover a latitude range from 15 to 68∘ N, altitudes up to 21 km, and a potential temperature range from 280 to 480 K. In total, 338 363 single particles were analysed, of which 147 338 were measured in the stratosphere. Of these total particles, 50 688 were characterized by high abundances of magnesium and iron, together with sulfuric ions, the vast majority (48 610) in the stratosphere, and are interpreted as meteoric material immersed or dissolved within sulfuric acid. It must be noted that the relative abundance of such meteoric particles may be overestimated by about 10 % to 30 % due to the presence of pure sulfuric acid particles in the stratosphere which are not detected by the instruments used here. Below the tropopause, the observed fraction of the meteoric particle type decreased sharply with 0.2 %–1 % abundance at Jungfraujoch, and smaller abundances (0.025 %–0.05 %) were observed during the lower-altitude Canadian Arctic aircraft measurements. The size distribution of the meteoric sulfuric particles measured in the UTLS campaigns is consistent with earlier aircraft-based mass-spectrometric measurements, with only 5 %–10 % fractions in the smallest particles detected (200–300 nm diameter) but with substantial (〉 40 %) abundance fractions for particles from 300–350 up to 900 nm in diameter, suggesting sedimentation is the primary loss mechanism. In the tropical lower stratosphere, only a small fraction (〈 10 %) of the analysed particles contained meteoric material. In contrast, in the extratropics the observed fraction of meteoric particles reached 20 %–40 % directly above the tropopause. At potential temperature levels of more than 40 K above the thermal tropopause, particles containing meteoric material were observed in much higher relative abundances than near the tropopause, and, at these altitudes, they occurred at a similar abundance fraction across all latitudes and seasons measured. Above 440 K, the observed fraction of meteoric particles is above 60 % at latitudes between 20 and 42∘ N. Meteoric smoke particles are transported from the mesosphere into the stratosphere within the winter polar vortex and are subsequently distributed towards low latitudes by isentropic mixing, typically below a potential temperature of 440 K. By contrast, the findings from the UTLS measurements show that meteoric material is found in stratospheric aerosol particles at all latitudes and seasons, which suggests that either isentropic mixing is effective also above 440 K or that meteoric fragments may be the source of a substantial proportion of the observed meteoric material.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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