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  • Clemen, Hans-Christian  (4)
  • Schneider, Johannes  (4)
  • 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 Measurement Techniques, Copernicus GmbH, Vol. 13, No. 11 ( 2020-11-09), p. 5923-5953
    Abstract: Abstract. 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 size-resolved 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 single-particle mass spectrometry (SPMS) instruments using Liu-type 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 application 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.
    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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  • 3
    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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  • 4
    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
    Location Call Number Limitation Availability
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