Search Results
Atomic oxygen number densities in the mesosphere–lower thermosphere region measured by solid electrolyte sensors onWADIS-2
2019, Eberhart, Martin, Löhle, Stefan, Strelnikov, Boris, Hedin, Jonas, Khaplanov, Mikhail, Fasoulas, Stefanos, Gumbel, Jörg, Lübken, Franz-Josef, Rapp, Markus
Absolute profiles of atomic oxygen number densities with high vertical resolution have been determined in the mesosphere-lower thermosphere (MLT) region from in situ measurements by several rocket-borne solid electrolyte sensors. The amperometric sensors were operated in both controlled and uncontrolled modes and with various orientations on the foredeck and aft deck of the payload. Calibration was based on mass spectrometry in a molecular beam containing atomic oxygen produced in a microwave discharge. The sensor signal is proportional to the number flux onto the electrodes, and the mass flow rate in the molecular beam was additionally measured to derive this quantity from the spectrometer reading. Numerical simulations provided aerodynamic correction factors to derive the atmospheric number density of atomic oxygen from the sensor data. The flight results indicate a preferable orientation of the electrode surface perpendicular to the rocket axis. While unstable during the upleg, the density profiles measured by these sensors show an excellent agreement with the atmospheric models and photometer results during the downleg of the trajectory. The high spatial resolution of the measurements allows for the identification of small-scale variations in the atomic oxygen concentration. © Author(s) 2019. This work is distributed under the Creative Commons Attribution 4.0 License.
Photocurrent modelling and experimental confirmation for meteoric smoke particle detectors on board atmospheric sounding rockets
2018-9-20, Giono, Gabriel, Strelnikov, Boris, Asmus, Heiner, Staszak, Tristan, Ivchenko, Nickolay, Lübken, Franz-Josef
Characterising the photoelectron current induced by the Sun's UV radiation is crucial to ensure accurate daylight measurements from particle detectors. This article lays out the methodology used to address this problem in the case of the meteoric smoke particle detectors (MSPDs), developed by the Leibniz Institute of Atmospheric Physics in Kühlungsborn (IAP) and flown on board the PMWEs (Polar Mesosphere Winter Echoes) sounding rockets in April 2018. The methodology focuses on two complementary aspects: modelling and experimental measurements. A detailed model of the MSPD photocurrent was created based on the expected solar UV flux, the atmospheric UV absorption as a function of height by molecular oxygen and ozone, the photoelectric yield of the material coating the MSPD as a function of wavelength, the index of refraction of these materials as a function of wavelength and the angle of incidence of the illumination onto the MSPD. Due to its complex structure, composed of a central electrode shielded by two concentric grids, extensive ray-tracing calculations were conducted to obtain the incidence angles of the illumination on the central electrode, and this was done for various orientations of the MSPD in respect to the Sun. Results of the modelled photocurrent at different heights and for different materials, as well as for different orientations of the detector, are presented. As a pre-flight confirmation, the model was used to reproduce the experimental measurements conducted by Robertson et al. (2014) and agrees within an order of magnitude. An experimental setup for the calibration of the MSPD photocurrent is also presented. The photocurrent induced by the Lyman-alpha line from a deuterium lamp was recorded inside a vacuum chamber using a narrowband filter, while a UV-sensitive photodiode was used to monitor the UV flux. These measurements were compared with the model prediction, and also matched within an order of magnitude. Although precisely modelling the photocurrent is a challenging task, this article quantitatively improved the understanding of the photocurrent on the MSPD and discusses possible strategies to untangle the meteoric smoke particles (MSPs) current from the photocurrent recorded in-flight.
Application of TXRF in monitoring trace metals in particulate matter and cloud water
2020, Fomba, Khanneh Wadinga, Deabji, Nabil, Barcha, Sayf El Islam, Ouchen, Ibrahim, Elbaramoussi, El Mehdi, El Moursli, Rajaa Cherkaoui, Harnafi, Mimoun, El Hajjaji, Souad, Mellouki, Abdelwahid, Herrmann, Hartmut
Trace metals in ambient particulate matter and cloud are considered key elements of atmospheric processes as they affect air quality, environmental ecosystems, and cloud formation. However, they are often available at trace concentrations in these media such that their analysis requires high-precision and sensitive techniques. In this study, different analytical methods were applied to quantify trace metals in particulate matter (PM) samples collected on quartz and polycarbonate filters as well as cloud water, using the Total reflection X-Ray Fluorescence (TXRF) technique. These methods considered the measurement of filter samples directly without and with chemical pretreatment. Direct measurements involved the analysis of PM samples collected on polycarbonate filters and cloud water samples after they are brought onto TXRF carrier substrates. The chemical treatment method involved the assessment of different acid digestion procedures on PM sampled on quartz filters. The solutions applied were reverse aqua regia, nitric acid, and a combination of nitric acid and hydrogen peroxide. The effect of cold-plasma treatment of samples on polycarbonate filters before TXRF measurements was also investigated. Digestion with the reverse aqua regia solution provided lower blanks and higher recovery in comparison to other tested procedures. The detection limits of the elements ranged from 0.3 to 44 ng cm−2. Ca, K, Zn, and Fe showed the highest detection limits of 44, 35, 6, and 1 ng cm−2, while As and Se had the lowest of 0.3 and 0.8 ng cm−2, respectively. The method showed higher recovery for most trace metals when applied to commercially available reference materials and field samples. TXRF measurements showed good agreement with results obtained from ion chromatography measurements for elements such as Ca and K. Cold-plasma treatment did not significantly lead to an increase in the detected concentration, and the results were element specific. Baking of the quartz filters prior to sampling showed a reduction of more than 20 % of the filter blanks for elements such as V, Sr, Mn, Zn, and Sb. The methods were applied successfully on ambient particulate matter and cloud water samples collected from the Atlas Mohammed V station in Morocco and the Cape Verde Atmospheric Observatory. The obtained concentrations were within the range reported using different techniques from similar remote and background regions elsewhere, especially for elements of anthropogenic origins such as V, Pb, and Zn with concentrations of up to 10, 19, and 28 ng m−3, respectively. Enrichment factor analysis indicated that crustal matter dominated the abundance of most of the elements, while anthropogenic activities also contributed to the abundance of elements such as Sb, Se, and Pb. The results confirm that TXRF is a useful complementary sensitive technique for trace metal analysis of particulate matter in the microgram range as well as in cloud water droplets.
A global analysis of climate-relevant aerosol properties retrieved from the network of Global Atmosphere Watch (GAW) near-surface observatories
2020, Laj, Paolo, Bigi, Alessandro, Rose, Clémence, Andrews, Elisabeth, Lund Myhre, Cathrine, Collaud Coen, Martine, Lin, Yong, Wiedensohler, Alfred, Schulz, Michael, Ogren, John A., Fiebig, Markus, Prenni, Anthony, Reisen, Fabienne, Romano, Salvatore, Sellegri, Karine, Sharma, Sangeeta, Schauer, Gerhard, Sheridan, Patrick, Sherman, James Patrick, Schütze, Maik, Schwerin, Andreas, Tuch, Thomas, Sohmer, Ralf, Sorribas, Mar, Steinbacher, Martin, Sun, Junying, Titos, Gloria, Toczko, Barbara, Tulet, Pierre, Tunved, Peter, Vakkari, Ville, Velarde, Fernando, Velasquez, Patricio, Villani, Paolo, Vratolis, Sterios, Wang, Sheng-Hsiang, Weinhold, Kay, Gliß, Jonas, Weller, Rolf, Yela, Margarita, Yus-Diez, Jesus, Zdimal, Vladimir, Zieger, Paul, Zikova, Nadezda, Mortier, Augustin, Pandolfi, Marco, Petäja, Tuukka, Kim, Sang-Woo, Aas, Wenche, Putaud, Jean-Philippe, Mayol-Bracero, Olga, Keywood, Melita, Labrador, Lorenzo, Aalto, Pasi, Ahlberg, Erik, Alados Arboledas, Lucas, Alastuey, Andrés, Andrade, Marcos, Artíñano, Begoña, Ausmeel, Stina, Arsov, Todor, Asmi, Eija, Backman, John, Baltensperger, Urs, Bastian, Susanne, Bath, Olaf, Beukes, Johan Paul, Brem, Benjamin T., Bukowiecki, Nicolas, Conil, Sébastien, Couret, Cedric, Day, Derek, Dayantolis, Wan, Degorska, Anna, Eleftheriadis, Konstantinos, Fetfatzis, Prodromos, Favez, Olivier, Flentje, Harald, Gini, Maria I., Gregorič, Asta, Gysel-Beer, Martin, Hallar, A. Gannet, Hand, Jenny, Hoffer, Andras, Hueglin, Christoph, Hooda, Rakesh K., Hyvärinen, Antti, Kalapov, Ivo, Kalivitis, Nikos, Kasper-Giebl, Anne, Kim, Jeong Eun, Kouvarakis, Giorgos, Kranjc, Irena, Krejci, Radovan, Kulmala, Markku, Labuschagne, Casper, Lee, Hae-Jung, Lihavainen, Heikki, Lin, Neng-Huei, Löschau, Gunter, Luoma, Krista, Marinoni, Angela, Martins Dos Santos, Sebastiao, Meinhardt, Frank, Merkel, Maik, Metzger, Jean-Marc, Mihalopoulos, Nikolaos, Nguyen, Nhat Anh, Ondracek, Jakub, Pérez, Noemi, Perrone, Maria Rita, Petit, Jean-Eudes, Picard, David, Pichon, Jean-Marc, Pont, Veronique, Prats, Natalia
Aerosol particles are essential constituents of the Earth's atmosphere, impacting the earth radiation balance directly by scattering and absorbing solar radiation, and indirectly by acting as cloud condensation nuclei. In contrast to most greenhouse gases, aerosol particles have short atmospheric residence times, resulting in a highly heterogeneous distribution in space and time. There is a clear need to document this variability at regional scale through observations involving, in particular, the in situ near-surface segment of the atmospheric observation system. This paper will provide the widest effort so far to document variability of climate-relevant in situ aerosol properties (namely wavelength dependent particle light scattering and absorption coefficients, particle number concentration and particle number size distribution) from all sites connected to the Global Atmosphere Watch network. High-quality data from almost 90 stations worldwide have been collected and controlled for quality and are reported for a reference year in 2017, providing a very extended and robust view of the variability of these variables worldwide. The range of variability observed worldwide for light scattering and absorption coefficients, single-scattering albedo, and particle number concentration are presented together with preliminary information on their long-term trends and comparison with model simulation for the different stations. The scope of the present paper is also to provide the necessary suite of information, including data provision procedures, quality control and analysis, data policy, and usage of the ground-based aerosol measurement network. It delivers to users of the World Data Centre on Aerosol, the required confidence in data products in the form of a fully characterized value chain, including uncertainty estimation and requirements for contributing to the global climate monitoring system.
A new method of inferring the size, number density, and charge of mesospheric dust from its in situ collection by the DUSTY probe
2019, Havnes, Ove, Antonsen, Tarjei, Baumgarten, Gerd, Hartquist, Thomas W., Biebricher, Alexander, Fredriksen, Åshild, Friedrich, Martin, Hedin, Jonas
We present a new method of analyzing measurements of mesospheric dust made with DUSTY rocket-borne Faraday cup probes. It can yield the variation in fundamental dust parameters through a mesospheric cloud with an altitude resolution down to 10 cm or less if plasma probes give the plasma density variations with similar height resolution. A DUSTY probe was the first probe that unambiguously detected charged dust and aerosol particles in the Earth's mesosphere. DUSTY excluded the ambient plasma by various biased grids, which however allowed dust particles with radii above a few nanometers to enter, and it measured the flux of charged dust particles. The flux measurements directly yielded the total ambient dust charge density. We extend the analysis of DUSTY data by using the impact currents on its main grid and the bottom plate as before, together with a dust charging model and a secondary charge production model, to allow the determination of fundamental parameters, such as dust radius, charge number, and total dust density. We demonstrate the utility of the new analysis technique by considering observations made with the DUSTY probes during the MAXIDUSTY rocket campaign in June-July 2016 and comparing the results with those of other instruments (lidar and photometer) also used in the campaign. In the present version we have used monodisperse dust size distributions.© Author(s) 2019.
Intercomparison study and optical asphericity measurements of small ice particles in the CERN CLOUD experiment
2017, Nichman, Leonid, Järvinen, Emma, Dorsey, James, Connolly, Paul, Duplissy, Jonathan, Fuchs, Claudia, Ignatius, Karoliina, Sengupta, Kamalika, Stratmann, Frank, Möhler, Ottmar, Schnaiter, Martin, Gallagher, Martin
Optical probes are frequently used for the detection of microphysical cloud particle properties such as liquid and ice phase, size and morphology. These properties can eventually influence the angular light scattering properties of cirrus clouds as well as the growth and accretion mechanisms of single cloud particles. In this study we compare four commonly used optical probes to examine their response to small cloud particles of different phase and asphericity. Cloud simulation experiments were conducted at the Cosmics Leaving OUtdoor Droplets (CLOUD) chamber at European Organisation for Nuclear Research (CERN). The chamber was operated in a series of multi-step adiabatic expansions to produce growth and sublimation of ice particles at super- and subsaturated ice conditions and for initial temperatures of -30, -40 and -50°C. The experiments were performed for ice cloud formation via homogeneous ice nucleation. We report the optical observations of small ice particles in deep convection and in situ cirrus simulations. Ice crystal asphericity deduced from measurements of spatially resolved single particle light scattering patterns by the Particle Phase Discriminator mark 2 (PPD-2K, Karlsruhe edition) were compared with Cloud and Aerosol Spectrometer with Polarisation (CASPOL) measurements and image roundness captured by the 3View Cloud Particle Imager (3V-CPI). Averaged path light scattering properties of the simulated ice clouds were measured using the Scattering Intensity Measurements for the Optical detectioN of icE (SIMONE) and single particle scattering properties were measured by the CASPOL. We show the ambiguity of several optical measurements in ice fraction determination of homogeneously frozen ice in the case where sublimating quasi-spherical ice particles are present. Moreover, most of the instruments have difficulties of producing reliable ice fraction if small aspherical ice particles are present, and all of the instruments cannot separate perfectly spherical ice particles from supercooled droplets. Correlation analysis of bulk averaged path depolarisation measurements and single particle measurements of these clouds showed higher R2 values at high concentrations and small diameters, but these results require further confirmation. We find that none of these instruments were able to determine unambiguously the phase of the small particles. These results have implications for the interpretation of atmospheric measurements and parametrisations for modelling, particularly for low particle number concentration clouds.
3+2 + X : what is the most useful depolarization input for retrieving microphysical properties of non-spherical particles from lidar measurements using the spheroid model of Dubovik et al. (2006)?
2019, Tesche, Matthias, Kolgotin, Alexei, Haarig, Moritz, Burton, Sharon P., Ferrare, Richard A., Hostetler, Chris A., Müller, Detlef
The typical multiwavelength aerosol lidar data set for inversion of optical to microphysical parameters is composed of three backscatter coefficients (β) at 355, 532, and 1064 nm and two extinction coefficients (α) at 355 and 532 nm. This data combination is referred to as a 3β C 2α or 3 + 2 data set. This set of data is sufficient for retrieving some important microphysical particle parameters if the particles have spherical shape. Here, we investigate the effect of including the particle linear depolarization ratio (δ) as a third input parameter for the inversion of lidar data. The inversion algorithm is generally not used if measurements show values of d that exceed 0.10 at 532 nm, i.e. in the presence of nonspherical particles such as desert dust, volcanic ash, and, under special circumstances, biomass-burning smoke. We use experimental data collected with instruments that are capable of measuring d at all three lidar wavelengths with an inversion routine that applies the spheroidal light-scattering model of Dubovik et al. (2006) with a fixed axis-ratio distribution to replicate scattering properties of non-spherical particles. The inversion gives the fraction of spheroids required to replicate the optical data as an additional output parameter. This is the first systematic test of the effect of using all theoretically possible combinations of d taken at 355, 532, and 1064 nm as input in the lidar data inversion. We find that depolarization information of at least one wavelength already provides useful information for the inversion of optical data that have been collected in the presence of non-spherical mineral dust particles. However, any choice of d will give lower values of the single-scattering albedo than the traditional 3 + 2 data set. We find that input data sets that include d355 give a spheroid fraction that closely resembles the dust ratio we obtain from using β532 and d532 in a methodology applied in aerosol-type separation. The use of d355 in data sets of two or three d? reduces the spheroid fraction that is retrieved when using d532 and d1064. Use of the latter two parameters without accounting for d355 generally leads to high spheroid fractions that we consider not trustworthy. The use of three d instead of two δ, including the constraint that one of these is measured at 355 nm does not provide any advantage over using 3 + 2 + d355 for the observations with varying contributions of mineral dust considered here. However, additional measurements at wavelengths different from 355 nm would be desirable for application to a wider range of aerosol scenarios that may include non-spherical smoke particles, which can have values of d355 that are indistinguishable from those found for mineral dust. We therefore conclude that - depending on measurement capability - the future standard input for inversion of lidar data taken in the presence of mineral dust particles and using the spheroid model of Dubovik et al. (2006) might be 3+2Cδ355 or 3 + 2 + δ355 + δ532. © 2019 The Author(s).
Increasing the spatial resolution of cloud property retrievals from Meteosat SEVIRI by use of its high-resolution visible channel: Evaluation of candidate approaches with MODIS observations
2020, Werner, Frank, Deneke, Hartwig
This study presents and evaluates several candidate approaches for downscaling observations from the Spinning Enhanced Visible and Infrared Imager (SEVIRI) in order to increase the horizontal resolution of subsequent cloud optical thickness (τ) and effective droplet radius (reff) retrievals from the native ≈ 3km×3km spatial resolution of the narrowband channels to ≈ 1km×1km. These methods make use of SEVIRI's coincident broadband high-resolution visible (HRV) channel. For four example cloud fields, the reliability of each downscaling algorithm is evaluated by means of collocated 1km×1km MODIS radiances, which are reprojected to the horizontal grid of the HRV channel and serve as reference for the evaluation. By using these radiances, smoothed with the modulation transfer function of the native SEVIRI channels, as retrieval input, the accuracy at the SEVIRI standard resolution can be evaluated and an objective comparison of the accuracy of the different downscaling algorithms can be made. For the example scenes considered in this study, it is shown that neglecting high-frequency variations below the SEVIRI standard resolution results in significant random absolute deviations of the retrieved τ and reff of up to ≈ 14 and ≈ 6μm, respectively, as well as biases. By error propagation, this also negatively impacts the reliability of the subsequent calculation of liquid water path (WL) and cloud droplet number concentration (ND), which exhibit deviations of up to ≈ 89gm-2 and ≈ 177cm-3, respectively. For τ , these deviations can be almost completely mitigated by the use of the HRV channel as a physical constraint and by applying most of the presented downscaling schemes. Uncertainties in retrieved reff at the native SEVIRI resolution are smaller, and the improvements from downscaling the observations are less obvious than for τ. Nonetheless, the right choice of downscaling scheme yields noticeable improvements in the retrieved reff. Furthermore, the improved reliability in retrieved cloud products results in significantly reduced uncertainties in derived WL and ND. In particular, one downscaling approach provides clear improvements for all cloud products compared to those obtained from SEVIRI's standard resolution and is recommended for future downscaling endeavors. This work advances efforts to mitigate impacts of scale mismatches among channels of multiresolution instruments on cloud retrievals. © Author(s) 2020.
Nano-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) for investigating hygroscopic properties of sub-10nm aerosol nanoparticles
2020, Lei, Ting, Ma, Nan, Hong, Juan, Tuch, Thomas, Wang, Xin, Wang, Zhibin, Pöhlker, Mira, Ge, Maofa, Wang, Weigang, Mikhailov, Eugene, Hoffmann, Thorsten, Pöschl, Ulrich, Su, Hang, Wiedensohler, Alfred, Cheng, Yafang
Interactions between water and nanoparticles are relevant for atmospheric multiphase processes, physical chemistry, and materials science. Current knowledge of the hygroscopic and related physicochemical properties of nanoparticles, however, is restricted by the limitations of the available measurement techniques. Here, we present the design and performance of a nano-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) apparatus that enables high accuracy and precision in hygroscopic growth measurements of aerosol nanoparticles with diameters less than 10 nm. Detailed methods of calibration and validation are provided. Besides maintaining accurate and stable sheath and aerosol flow rates (1 %), high accuracy of the differential mobility analyzer (DMA) voltage (0:1 %) in the range of 0-50V is crucial for achieving accurate sizing and small sizing offsets between the two DMAs (1:4 %). To maintain a stable relative humidity (RH), the humidification system and the second DMA are placed in a well-insulated and air conditioner housing (0:1 K). We also tested and discussed different ways of preventing predeliquescence in the second DMA. Our measurement results for ammonium sulfate nanoparticles are in good agreement with Biskos et al. (2006b), with no significant size effect on the deliquescence and efflorescence relative humidity (DRH and ERH, respectively) at diameters down to 6 nm. For sodium sulfate nanoparticles, however, we find a pronounced size dependence of DRH and ERH between 20 and 6 nm nanoparticles. © Author(s) 2020. This work is distributed under the Creative Commons Attribution 4.0 License.
Characterization and first results from LACIS-T : a moist-air wind tunnel to study aerosol–cloud–turbulence interactions
2020, Niedermeier, Dennis, Voigtländer, Jens, Schmalfuß, Silvio, Busch, Daniel, Schumacher, Jörg, Shaw, Raymond A., Stratmann, Frank
The interactions between turbulence and cloud microphysical processes have been investigated primarily through numerical simulation and field measurements over the last 10 years. However, only in the laboratory we can be confident in our knowledge of initial and boundary conditions and are able to measure under statistically stationary and repeatable conditions. In the scope of this paper, we present a unique turbulent moist-air wind tunnel, called the Turbulent Leipzig Aerosol Cloud Interaction Simulator (LACIS-T) which has been developed at TROPOS in order to study cloud physical processes in general and interactions between turbulence and cloud microphysical processes in particular. The investigations take place under well-defined and reproducible turbulent and thermodynamic conditions covering the temperature range of warm, mixed-phase and cold clouds (25∘C>T>−40∘C ). The continuous-flow design of the facility allows for the investigation of processes occurring on small temporal (up to a few seconds) and spatial scales (micrometer to meter scale) and with a Lagrangian perspective. The here-presented experimental studies using LACIS-T are accompanied and complemented by computational fluid dynamics (CFD) simulations which help us to design experiments as well as to interpret experimental results. In this paper, we will present the fundamental operating principle of LACIS-T, the numerical model, and results concerning the thermodynamic and flow conditions prevailing inside the wind tunnel, combining both characterization measurements and numerical simulations. Finally, the first results are depicted from deliquescence and hygroscopic growth as well as droplet activation and growth experiments. We observe clear indications of the effect of turbulence on the investigated microphysical processes.