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- ItemOptimizing 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, StephanThe 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.
- ItemAerosol 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-PaulInfrared 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.