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    A novel rocket-borne ion mass spectrometer with large mass range: instrument description and first-flight results
    (Katlenburg-Lindau : European Geosciences Union, 2021) Stude, Joan; Aufmhoff, Heinfried; Schlager, Hans; Rapp, Markus; Arnold, Frank; Strelnikov, Boris
    We present a novel rocket-borne ion mass spectrometer named ROMARA (ROcket-borne MAss spectrometer for Research in the Atmosphere) for measuring atmospheric positive and negative ions (atomic, molecular and cluster ions) and positively and negatively charged meteor smoke particles. Our ROMARA instrument has, compared to previous rocket-borne ion mass spectrometers, a markedly larger mass range of up to m=z 2000 and a larger sensitivity, particularly for meteor smoke particle detection. The major objectives of this first ROMARA flight included the following: a functional test of the ROMARA instrument, measurements between 55 and 121 km in the mass range of atmospheric positive and negative ions, a first attempt to conduct mass spectrometric measurements in the mass range of meteor smoke particles with mass-to-charge ratios up to m=z 2000, and measurements inside a polar mesospheric winter echo layer as detected by ground-based radar. Our ROMARA measurements took place on the Arctic island of Andøya, Norway, at around noon in April 2018 and represented an integral part of the polar mesospheric winter radar echo (PMWE) rocket campaign. During the rocket flight, ROMARA was operated in a measurement mode, offering maximum sensitivity and the ability to qualitatively detect total ion signatures even beyond its mass-resolving mass range. On this first ROMARA flight we were able to meet all of our objectives. We detected atmospheric species including positive atomic, molecular and cluster ions along with negative molecular ions up to about m=z 100. Above m=z 2000, ROMARA measured strong negative-ion signatures, which are likely due to negatively charged meteor smoke particles. © 2021 Author(s).
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    VAHCOLI, a new concept for lidars: technical setup, science applications, and first measurements
    (Katlenburg-Lindau : European Geosciences Union, 2021) Lübken, Franz-Josef; Höffner, Josef
    A new concept for a cluster of compact lidar systems named VAHCOLI (Vertical And Horizontal COverage by LIdars) is presented, which allows for the measurement of temperatures, winds, and aerosols in the middle atmosphere (10 110 km) with high temporal and vertical resolution of minutes and some tens of meters, respectively, simultaneously covering horizontal scales from a few hundred meters to several hundred kilometers ( four-dimensional coverage ). The individual lidars ( units ) being used in VAHCOLI are based on a diode-pumped alexandrite laser, which is currently designed to detect potassium (D 770 nm), and on sophisticated laser spectroscopy measuring all relevant frequencies (seeder laser, power laser, backscattered light) with high temporal resolution (2 ms) and high spectral resolution applying Doppler-free spectroscopy. The frequency of the lasers and the narrowband filter in the receiving system are stabilized to typically 10 100 kHz, which is a factor of roughly 105 smaller than the Doppler-broadened Rayleigh signal. Narrowband filtering allows for the measurement of Rayleigh and/or resonance scattering separately from the aerosol (Mie) signal during both night and day. Lidars used for VAHCOLI are compact (volume: 1m3) and multi-purpose systems which employ contemporary electronic, optical, and mechanical components. The units are designed to autonomously operate under harsh field conditions in remote locations. An error analysis with parameters of the anticipated system demonstrates that temperatures and line-of-sight winds can be measured from the lower stratosphere to the upper mesosphere with an accuracy of (0.1 5)K and (0.1 10)ms1, respectively, increasing with altitude. We demonstrate that some crucial dynamical processes in the middle atmosphere, such as gravity waves and stratified turbulence, can be covered by VAHCOLI with sufficient temporal, vertical, and horizontal sampling and resolution. The four-dimensional capabilities of VAHCOLI allow for the performance of time-dependent analysis of the flow field, for example by employing Helmholtz decomposition, and for carrying out statistical tests regarding, for example, intermittency and helicity. The first test measurements under field conditions with a prototype lidar were performed in January 2020. The lidar operated successfully during a 6-week period (night and day) without any adjustment. The observations covered a height range of 5 100 km and demonstrated the capability and applicability of this unit for the VAHCOLI concept.
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    Multi-year ACSM measurements at the central European research station Melpitz (Germany)-Part 1: Instrument robustness, quality assurance, and impact of upper size cutoff diameter
    (Katlenburg-Lindau : Copernicus, 2020) Poulain, Laurent; Spindler, Gerald; Grüner, Achim; Tuch, Thomas; Stieger, Bastian; van Pinxteren, Dominik; Petit, Jean-Eudes; Favez, Olivier; Herrmann, Hartmut; Wiedensohler, Alfred
    The aerosol chemical speciation monitor (ACSM) is nowadays widely used to identify and quantify the main components of fine particles in ambient air. As such, its deployment at observatory platforms is fully incorporated within the European Aerosol, Clouds and Trace Gases Research Infrastructure (ACTRIS). Regular intercomparisons are organized at the Aerosol Chemical Monitoring Calibration Center (ACMCC; part of the European Center for Aerosol Calibration, Paris, France) to ensure the consistency of the dataset, as well as instrumental performance and variability. However, in situ quality assurance remains a fundamental aspect of the instrument's stability. Here, we present and discuss the main outputs of long-term quality assurance efforts achieved for ACSM measurements at the research station Melpitz (Germany) since 2012 onwards. In order to validate the ACSM measurements over the years and to characterize seasonal variations, nitrate, sulfate, ammonium, organic, and particle mass concentrations were systematically compared against the collocated measurements of daily offline high-volume PM1 and PM2:5 filter samples and particle number size distribution (PNSD) measurements. Mass closure analysis was made by comparing the total particle mass (PM) concentration obtained by adding the mass concentration of equivalent black carbon (eBC) from the multi-angle absorption photometer (MAAP) to the ACSM chemical composition, to that of PM1 and PM2:5 during filter weighing, as well as to the derived mass concentration of PNSD. A combination of PM1 and PM2:5 filter samples helped identifying the critical importance of the upper size cutoff of the ACSM during such exercises. The ACSM-MAAP-derived mass concentrations systematically deviated from the PM1 mass when the mass concentration of the latter represented less than 60% of PM2:5, which was linked to the transmission efficiency of the aerodynamic lenses of the ACSM. The best correlations are obtained for sulfate (slopeD 0:96; R2 D 0:77) and total PM (slopeD 1:02; R2 D 0:90). Although, sulfate did not exhibit a seasonal dependency, total PM mass concentration revealed a small seasonal variability linked to the increase in non-water-soluble fractions. The nitrate suffers from a loss of ammonium nitrate during filter collection, and the contribution of organo-nitrate compounds to the ACSM nitrate signal make it difficult to directly compare the two methods. The contribution of m=z 44 (f44) to the total organic mass concentration was used to convert the ACSM organic mass (OM) to organic carbon (OC) by using a similar approach as for the aerosol mass spectrometer (AMS). The resulting estimated OCACSM was compared with the measured OCPM1 (slopeD 0:74; R2 D 0:77), indicating that the f44 signal was relatively free of interferences during this period. The PM2:5 filter samples use for the ACSM data quality might suffer from a systematic bias due to a size truncation effect as well as to the presence of chemical species that cannot be detected by the ACSM in coarse mode (e.g., sodium nitrate and sodium sulfate). This may lead to a systematic underestimation of the ACSM particle mass concentration and/or a positive artifact that artificially decreases the discrepancies between the two methods. Consequently, ACSM data validation using PM2:5 filters has to be interpreted with extreme care. The particle mass closure with the PNSD was satisfying (slopeD 0:77; R2 D 0:90 over the entire period), with a slight overestimation of the mobility particle size spectrometer (MPSS)-derived mass concentration in winter. This seasonal variability was related to a change on the PNSD and a larger contribution of the supermicrometer particles in winter. This long-term analysis between the ACSM and other collocated instruments confirms the robustness of the ACSM and its suitability for long-term measurements. Particle mass closure with the PNSD is strongly recommended to ensure the stability of the ACSM. A near-real-time mass closure procedure within the entire ACTRIS-ACSM network certainly represents an optimal quality control and assurance of both warranting the quality assurance of the ACSM measurements as well as identifying cross-instrumental biases. © Author(s) 2020.
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    Optimizing the detection, ablation, and ion extraction efficiency of a single-particle laser ablation mass spectrometer for application in environments with low aerosol particle concentrations
    (Katlenburg-Lindau : Copernicus, 2020) Clemen, Hans-Christian; Schneider, Johannes; Klimach, Thomas; Helleis, Frank; Köllner, Franziska; Hünig, Andreas; Rubach, Florian; Mertes, Stephan; Wex, Heike; Stratmann, Frank; Welti, André; Kohl, Rebecca; Frank, Fabian; Borrmann, Stephan
    The aim of this study is to show how a newly developed aerodynamic lens system (ALS), a delayed ion extraction (DIE), and better electric shielding improve the efficiency of the Aircraft-based Laser ABlation Aerosol MAss spectrometer (ALABAMA). These improvements are applicable to single-particle laser ablation mass spectrometers in general. To characterize the modifications, extensive sizeresolved measurements with spherical polystyrene latex particles (PSL; 150-6000 nm) and cubic sodium chloride particles (NaCl; 400-1700 nm) were performed. Measurements at a fixed ALS position show an improved detectable particle size range of the new ALS compared to the previously used Liu-type ALS, especially for supermicron particles. At a lens pressure of 2.4 hPa, the new ALS achieves a PSL particle size range from 230 to 3240 nm with 50% detection efficiency and between 350 and 2000 nm with 95% detection efficiency. The particle beam divergence was determined by measuring the detection efficiency at variable ALS positions along the laser cross sections and found to be minimal for PSL at about 800 nm. Compared to measurements by singleparticle mass spectrometry (SPMS) instruments using Liutype ALSs, the minimum particle beam divergence is shifted towards larger particle sizes. However, there are no disadvantages compared to the Liu-type lenses for particle sizes down to 200 nm. Improvements achieved by using the DIE and an additional electric shielding could be evaluated by size-resolved measurements of the hit rate, which is the ratio of laser pulses yielding a detectable amount of ions to the total number of emitted laser pulses. In particular, the hit rate for multiply charged particles smaller than 500 nm is significantly improved by preventing an undesired deflection of these particles in the ion extraction field. Moreover, it was found that by using the DIE the ion yield of the ablation, ionization, and ion extraction process could be increased, resulting in up to 7 times higher signal intensities of the cation spectra. The enhanced ion yield results in a larger effective width of the ablation laser beam, which in turn leads to a hit rate of almost 100% for PSL particles in the size range from 350 to 2000 nm. Regarding cubic NaCl particles the modifications of the ALABAMA result in an up to 2 times increased detection efficiency and an up to 5 times increased hit rate. The need for such instrument modifications arises in particular for measurements of particles that are present in low number concentrations such as ice-nucleating particles (INPs) in general, but also aerosol particles at high altitudes or in pristine environments. Especially for these low particle number concentrations, improved efficiencies help to overcome the statistical limitations of single-particle mass spectrometer measurements. As an example, laboratory INP measurements carried out in this study show that the appli- cation of the DIE alone increases the number of INP mass spectra per time unit by a factor of 2 to 3 for the sampled substances. Overall, the combination of instrument modifications presented here resulted in an increased measurement efficiency of the ALABAMA for different particle types and particles shape as well as for highly charged particles. © 2020 Copernicus GmbH. All rights reserved.
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    Aerosol and cloud top height information of Envisat MIPAS measurements
    (Katlenburg-Lindau : Copernicus, 2020) Griessbach, Sabine; Hoffmann, Lars; Spang, Reinhold; Achtert, Peggy; von Hobe, Marc; Mateshvili, Nina; Müller, Rolf; Riese, Martin; Rolf, Christian; Seifert, Patric; Vernier, Jean-Paul
    Infrared limb emission instruments have a long history in measuring clouds and aerosol. In particular, the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument aboard ESA's Envisat provides 10 years of altitude-resolved global measurements. Previous studies found systematic overestimations and underestimations of cloud top heights for cirrus and polar stratospheric clouds. To assess the cloud top height information and to characterise its uncertainty for the MIPAS instrument we performed simulations for ice clouds, volcanic ash, and sulfate aerosol. From the simulation results we found that in addition to the known effects of the field-of-view that can lead to a cloud top height overestimation, and broken cloud conditions that can lead to underestimation, the cloud extinction also plays an important role. While for optically thick clouds the possible cloud top height overestimation for MIPAS reaches up to 1.6 km due to the field-of-view, for optically thin clouds and aerosol the systematic underestimation reaches 5.1 km. For the detection sensitivity and the degree of underestimation of the MIPAS measurements, the cloud layer thickness also plays a role; 1 km thick clouds are detectable down to extinctions of 5×10-4 km-1 and 6 km thick clouds are detectable down to extinctions of 1×10-4 km-1, where the largest underestimations of the cloud top height occur for the optically thinnest clouds with a vertical extent of 6 km. The relation between extinction coefficient, cloud top height estimate, and layer thickness is confirmed by a comparison of MIPAS cloud top heights of the volcanic sulfate aerosol from the Nabro eruption in 2011 with space-and ground-based lidar measurements and twilight measurements between June 2011 and February 2012. For plumes up to 2 months old, where the extinction was between 1×10-4 and 7×10-4 km-1 and the layer thickness mostly below 4 km, we found for MIPAS an average underestimation of 1.1 km. In the aged plume with extinctions down to 5 × 10-5 km-1 and layer thicknesses of up to 9.5 km, the underestimation was higher, reaching up to 7.2 km. The dependency of the cloud top height overestimations or underestimations on the extinction coefficient can explain seemingly contradictory results of previous studies. In spite of the relatively large uncertainty range of the cloud top height, the comparison of the detection sensitivity towards sulfate aerosol between MIPAS and a suite of widely used UV/VIS limb and IR nadir satellite aerosol measurements shows that MIPAS provides complementary information in terms of detection sensitivity. © Author(s) 2020.