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- ItemResults and recommendations from an intercomparison of six Hygroscopicity-TDMA systems(München : European Geopyhsical Union, 2011) Massling, A.; Niedermeier, N.; Hennig, T.; Fors, E.O.; Swietlicki, E.; Ehn, M.; Hämeri, K.; Villani, P.; Laj, P.; Good, N.; McFiggans, G.; Wiedensohler, A.The performance of six custom-built Hygrocopicity-Tandem Differential Mobility Analyser (H-TDMA) systems was investigated in the frame of an international calibration and intercomparison workshop held in Leipzig, February 2006. The goal of the workshop was to harmonise H-TDMA measurements and develop recommendations for atmospheric measurements and their data evaluation. The H-TDMA systems were compared in terms of the sizing of dry particles, relative humidity (RH) uncertainty, and consistency in determination of number fractions of different hygroscopic particle groups. The experiments were performed in an air-conditioned laboratory using ammonium sulphate particles or an external mixture of ammonium sulphate and soot particles. The sizing of dry particles of the six H-TDMA systems was within 0.2 to 4.2% of the selected particle diameter depending on investigated size and individual system. Measurements of ammonium sulphate aerosol found deviations equivalent to 4.5% RH from the set point of 90% RH compared to results from previous experiments in the literature. Evaluation of the number fraction of particles within the clearly separated growth factor modes of a laboratory generated externally mixed aerosol was done. The data from the H-TDMAs was analysed with a single fitting routine to investigate differences caused by the different data evaluation procedures used for each H-TDMA. The differences between the H-TDMAs were reduced from +12/−13% to +8/−6% when the same analysis routine was applied. We conclude that a common data evaluation procedure to determine number fractions of externally mixed aerosols will improve the comparability of H-TDMA measurements. It is recommended to ensure proper calibration of all flow, temperature and RH sensors in the systems. It is most important to thermally insulate the aerosol humidification unit and the second DMA and to monitor these temperatures to an accuracy of 0.2 °C. For the correct determination of external mixtures, it is necessary to take into account size-dependent losses due to diffusion in the plumbing between the DMAs and in the aerosol humidification unit.
- Item3+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)?(Katlenburg-Lindau : Copernicus, 2019) Tesche, Matthias; Kolgotin, Alexei; Haarig, Moritz; Burton, Sharon P.; Ferrare, Richard A.; Hostetler, Chris A.; Müller, DetlefThe 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).
- ItemA statistical proxy for sulphuric acid concentration(München : European Geopyhsical Union, 2011) Mikkonen, S.; Romakkaniemi, S.; Smith, J.N.; Korhonen, H.; Petäjä, T.; Plass-Duelmer, C.; Boy, M.; McMurry, P.H.; Lehtinen, K.E.J.; Joutsensaari, J.; Hamed, A.; Mauldin III, R.L.; Birmili, W.; Spindler, G.; Arnold, F.; Kulmala, M.; Laaksonen, A.Gaseous sulphuric acid is a key precursor for new particle formation in the atmosphere. Previous experimental studies have confirmed a strong correlation between the number concentrations of freshly formed particles and the ambient concentrations of sulphuric acid. This study evaluates a body of experimental gas phase sulphuric acid concentrations, as measured by Chemical Ionization Mass Spectrometry (CIMS) during six intensive measurement campaigns and one long-term observational period. The campaign datasets were measured in Hyytiälä, Finland, in 2003 and 2007, in San Pietro Capofiume, Italy, in 2009, in Melpitz, Germany, in 2008, in Atlanta, Georgia, USA, in 2002, and in Niwot Ridge, Colorado, USA, in 2007. The long term data were obtained in Hohenpeissenberg, Germany, during 1998 to 2000. The measured time series were used to construct proximity measures ("proxies") for sulphuric acid concentration by using statistical analysis methods. The objective of this study is to find a proxy for sulfuric acid that is valid in as many different atmospheric environments as possible. Our most accurate and universal formulation of the sulphuric acid concentration proxy uses global solar radiation, SO2 concentration, condensation sink and relative humidity as predictor variables, yielding a correlation measure (R) of 0.87 between observed concentration and the proxy predictions. Interestingly, the role of the condensation sink in the proxy was only minor, since similarly accurate proxies could be constructed with global solar radiation and SO2 concentration alone. This could be attributed to SO2 being an indicator for anthropogenic pollution, including particulate and gaseous emissions which represent sinks for the OH radical that, in turn, is needed for the formation of sulphuric acid.
- ItemOrganic aerosol components derived from 25 AMS data sets across Europe using a consistent ME-2 based source apportionment approach(München : European Geopyhsical Union, 2014) Crippa, M.; Canonaco, F.; Lanz, V.A.; Äijälä, M.; Allan, J.D.; Carbone, S.; Capes, G.; Ceburnis, D.; Dall'Osto, M.; Day, D.A.; DeCarlo, P.F.; Ehn, M.; Eriksson, A.; Freney, E.; Hildebrandt Ruiz, L.; Hillamo, R.; Jimenez, J.L.; Junninen, H.; Kiendler-Scharr, A.; Kortelainen, A.-M.; Kulmala, M.; Laaksonen, A.; Mensah, A.A.; Mohr, C.; Nemitz, E.; O'Dowd, C.; Ovadnevaite, J.; Pandis, S.N.; Petäjä, T.; Poulain, L.; Saarikoski, S.; Sellegri, K.; Swietlicki, E.; Tiitta, P.; Worsnop, D.R.; Baltensperger, U.; Prévôt, A.S.H.Organic aerosols (OA) represent one of the major constituents of submicron particulate matter (PM1) and comprise a huge variety of compounds emitted by different sources. Three intensive measurement field campaigns to investigate the aerosol chemical composition all over Europe were carried out within the framework of the European Integrated Project on Aerosol Cloud Climate and Air Quality Interactions (EUCAARI) and the intensive campaigns of European Monitoring and Evaluation Programme (EMEP) during 2008 (May–June and September–October) and 2009 (February–March). In this paper we focus on the identification of the main organic aerosol sources and we define a standardized methodology to perform source apportionment using positive matrix factorization (PMF) with the multilinear engine (ME-2) on Aerodyne aerosol mass spectrometer (AMS) data. Our source apportionment procedure is tested and applied on 25 data sets accounting for two urban, several rural and remote and two high altitude sites; therefore it is likely suitable for the treatment of AMS-related ambient data sets. For most of the sites, four organic components are retrieved, improving significantly previous source apportionment results where only a separation in primary and secondary OA sources was possible. Generally, our solutions include two primary OA sources, i.e. hydrocarbon-like OA (HOA) and biomass burning OA (BBOA) and two secondary OA components, i.e. semi-volatile oxygenated OA (SV-OOA) and low-volatility oxygenated OA (LV-OOA). For specific sites cooking-related (COA) and marine-related sources (MSA) are also separated. Finally, our work provides a large overview of organic aerosol sources in Europe and an interesting set of highly time resolved data for modeling purposes.
- ItemFour-dimensional distribution of the 2010 Eyjafjallajökull volcanic cloud over Europe observed by EARLINET(München : European Geopyhsical Union, 2013) Pappalardo, G.; Mona, L.; D'Amico, G.; Wandinger, U.; Adam, M.; Amodeo, A.; Ansmann, A.; Apituley, A.; Alados Arboledas, L.; Balis, D.; Boselli, A.; Bravo-Aranda, J.A.; Chaikovsky, A.; Comeron, A.; Cuesta, J.; De Tomasi, F.; Freudenthaler, V.; Gausa, M.; Giannakaki, E.; Giehl, H.; Giunta, A.; Grigorov, I.; Groß, S.; Haeffelin, M.; Hiebsch, A.; Iarlori, M.; Lange, D.; Linné, H.; Madonna, F.; Mattis, I.; Mamouri, R.-E.; McAuliffe, M.A.P.; Mitev, V.; Molero, F.; Navas-Guzman, F.; Nicolae, D.; Papayannis, A.; Perrone, M.R.; Pietras, C.; Pietruczuk, A.; Pisani, G.; Preißler, J.; Pujadas, M.; Rizi, V.; Ruth, A.A.; Schmidt, J.; Schnell, F.; Seifert, P.; Serikov, I.; Sicard, M.; Simeonov, V.; Spinelli, N.; Stebel, K.; Tesche, M.; Trickl, T.; Wang, X.; Wagner, F.; Wiegner, M.; Wilson, K.M.The eruption of the Icelandic volcano Eyjafjallajökull in April–May 2010 represents a "natural experiment" to study the impact of volcanic emissions on a continental scale. For the first time, quantitative data about the presence, altitude, and layering of the volcanic cloud, in conjunction with optical information, are available for most parts of Europe derived from the observations by the European Aerosol Research Lidar NETwork (EARLINET). Based on multi-wavelength Raman lidar systems, EARLINET is the only instrument worldwide that is able to provide dense time series of high-quality optical data to be used for aerosol typing and for the retrieval of particle microphysical properties as a function of altitude. In this work we show the four-dimensional (4-D) distribution of the Eyjafjallajökull volcanic cloud in the troposphere over Europe as observed by EARLINET during the entire volcanic event (15 April–26 May 2010). All optical properties directly measured (backscatter, extinction, and particle linear depolarization ratio) are stored in the EARLINET database available at http://www.earlinet.org. A specific relational database providing the volcanic mask over Europe, realized ad hoc for this specific event, has been developed and is available on request at http://www.earlinet.org. During the first days after the eruption, volcanic particles were detected over Central Europe within a wide range of altitudes, from the upper troposphere down to the local planetary boundary layer (PBL). After 19 April 2010, volcanic particles were detected over southern and south-eastern Europe. During the first half of May (5–15 May), material emitted by the Eyjafjallajökull volcano was detected over Spain and Portugal and then over the Mediterranean and the Balkans. The last observations of the event were recorded until 25 May in Central Europe and in the Eastern Mediterranean area. The 4-D distribution of volcanic aerosol layering and optical properties on European scale reported here provides an unprecedented data set for evaluating satellite data and aerosol dispersion models for this kind of volcanic events.
- ItemModeling the global emission, transport and deposition of trace elements associated with mineral dust(München : European Geopyhsical Union, 2015) Zhang, Y.; Mahowald, N.; Scanza, R.A.; Journet, E.; Desboeufs, K.; Albani, S.; Kok, J.F.; Zhuang, G.; Chen, Y.; Cohen, D.D.; Paytan, A.; Patey, M.D.; Achterberg, E.P.; Engelbrecht, J.P.; Fomba, K.W.Trace element deposition from desert dust has important impacts on ocean primary productivity, the quantification of which could be useful in determining the magnitude and sign of the biogeochemical feedback on radiative forcing. However, the impact of elemental deposition to remote ocean regions is not well understood and is not currently included in global climate models. In this study, emission inventories for eight elements primarily of soil origin, Mg, P, Ca, Mn, Fe, K, Al, and Si are determined based on a global mineral data set and a soil data set. The resulting elemental fractions are used to drive the desert dust model in the Community Earth System Model (CESM) in order to simulate the elemental concentrations of atmospheric dust. Spatial variability of mineral dust elemental fractions is evident on a global scale, particularly for Ca. Simulations of global variations in the Ca / Al ratio, which typically range from around 0.1 to 5.0 in soils, are consistent with observations, suggesting that this ratio is a good signature for dust source regions. The simulated variable fractions of chemical elements are sufficiently different; estimates of deposition should include elemental variations, especially for Ca, Al and Fe. The model results have been evaluated with observations of elemental aerosol concentrations from desert regions and dust events in non-dust regions, providing insights into uncertainties in the modeling approach. The ratios between modeled and observed elemental fractions range from 0.7 to 1.6, except for Mg and Mn (3.4 and 3.5, respectively). Using the soil database improves the correspondence of the spatial heterogeneity in the modeling of several elements (Ca, Al and Fe) compared to observations. Total and soluble dust element fluxes to different ocean basins and ice sheet regions have been estimated, based on the model results. The annual inputs of soluble Mg, P, Ca, Mn, Fe and K associated with dust using the mineral data set are 0.30 Tg, 16.89 Gg, 1.32 Tg, 22.84 Gg, 0.068 Tg, and 0.15 Tg to global oceans and ice sheets.
- ItemA concept of an automated function control for ambient aerosol measurements using mobility particle size spectrometers(München : European Geopyhsical Union, 2014) Schladitz, A.; Merkel, M.; Bastian, S.; Birmili, W.; Weinhold, K.; Löschau, G.; Wiedensohler, A.An automated function control unit was developed to regularly check the ambient particle number concentration derived from a mobility particle size spectrometer as well as its zero-point behaviour. The function control allows unattended quality assurance experiments at remote air quality monitoring or research stations under field conditions. The automated function control also has the advantage of being able to get a faster system stability response than the recommended on-site comparisons with reference instruments. The method is based on a comparison of the total particle number concentration measured by a mobility particle size spectrometer and a condensation particle counter while removing diffusive particles smaller than 20 nm in diameter. In practice, the small particles are removed by a set of diffusion screens, as traditionally used in a diffusion battery. Another feature of the automated function control is to check the zero-point behaviour of the ambient aerosol passing through a high-efficiency particulate air (HEPA) filter. The performance of the function control is illustrated with the aid of a 1-year data set recorded at Annaberg-Buchholz, a station in the Saxon air quality monitoring network. During the period of concern, the total particle number concentration derived from the mobility particle size spectrometer slightly overestimated the particle number concentration recorded by the condensation particle counter by 2 % (grand average). Based on our first year of experience with the function control, we developed tolerance criteria that allow a performance evaluation of a tested mobility particle size spectrometer with respect to the total particle number concentration. We conclude that the automated function control enhances the quality and reliability of unattended long-term particle number size distribution measurements. This will have beneficial effects for intercomparison studies involving different measurement sites, and help provide a higher data accuracy for cohort health and climate research studies.
- ItemApplication of linear polarized light for the discrimination of frozen and liquid droplets in ice nucleation experiments(München : European Geopyhsical Union, 2013) Clauss, T.; Kiselev, A.; Hartmann, S.; Augustin, S.; Pfeifer, S.; Niedermeier, D.; Wex, H.; Stratmann, F.We report on the development and test results of the new optical particle counter TOPS-Ice (Thermo-stabilized Optical Particle Spectrometer for the detection of Ice). The instrument uses measurements of the cross-polarized scattered light by single particles into the near-forward direction (42.5° ± 12.7°) to distinguish between spherical and non-spherical particles. This approach allows the differentiation between liquid water droplets (spherical) and ice particles (non-spherical) having similar volume-equivalent sizes and therefore can be used to determine the fraction of frozen droplets in a typical immersion freezing experiment. We show that the numerical simulation of the light scattered on non-spherical particles (spheroids in random orientation) considering the actual scattering geometry used in the instrument supports the validity of the approach, even though the cross-polarized component of the light scattered by spherical droplets does not vanish in this scattering angle. For the separation of the ice particle mode from the liquid droplet mode, we use the width of the pulse detected in the depolarization channel instead of the pulse height. Exploiting the intrinsic relationship between pulse height and pulse width for Gaussian pulses allows us to calculate the fraction of frozen droplets even if the liquid droplet mode dominates the particle ensemble. We present test results obtained with TOPS-Ice in the immersion freezing experiments at the laminar diffusion chamber LACIS (Leipzig Aerosol Cloud Interaction Simulator) and demonstrate the excellent agreement with the data obtained in similar experiments with a different optical instrument. Finally, the advantages of using the cross-polarized light measurements for the differentiation of liquid and frozen droplets in the realistic immersion freezing experiments are discussed.
- ItemCalibration of Raman lidar water vapor profiles by means of AERONET photometer observations and GDAS meteorological data(München : European Geopyhsical Union, 2018) Dai, Guangyao; Althausen, Dietrich; Hofer, Julian; Engelmann, Ronny; Seifert, Patric; Bühl, Johannes; Mamouri, Rodanthi-Elisavet; Wu, Songhua; Ansmann, AlbertWe present a practical method to continuously calibrate Raman lidar observations of water vapor mixing ratio profiles. The water vapor profile measured with the multiwavelength polarization Raman lidar PollyXT is calibrated by means of co-located AErosol RObotic NETwork (AERONET) sun photometer observations and Global Data Assimilation System (GDAS) temperature and pressure profiles. This method is applied to lidar observations conducted during the Cyprus Cloud Aerosol and Rain Experiment (CyCARE) in Limassol, Cyprus. We use the GDAS temperature and pressure profiles to retrieve the water vapor density. In the next step, the precipitable water vapor from the lidar observations is used for the calibration of the lidar measurements with the sun photometer measurements. The retrieved calibrated water vapor mixing ratio from the lidar measurements has a relative uncertainty of 11 % in which the error is mainly caused by the error of the sun photometer measurements. During CyCARE, nine measurement cases with cloud-free and stable meteorological conditions are selected to calculate the precipitable water vapor from the lidar and the sun photometer observations. The ratio of these two precipitable water vapor values yields the water vapor calibration constant. The calibration constant for the PollyXT Raman lidar is 6.56 g kg−1 ± 0.72 g kg−1 (with a statistical uncertainty of 0.08 g kg−1 and an instrumental uncertainty of 0.72 g kg−1). To check the quality of the water vapor calibration, the water vapor mixing ratio profiles from the simultaneous nighttime observations with Raman lidar and Vaisala radiosonde sounding are compared. The correlation of the water vapor mixing ratios from these two instruments is determined by using all of the 19 simultaneous nighttime measurements during CyCARE. Excellent agreement with the slope of 1.01 and the R2 of 0.99 is found. One example is presented to demonstrate the full potential of a well-calibrated Raman lidar. The relative humidity profiles from lidar, GDAS (simulation) and radiosonde are compared, too. It is found that the combination of water vapor mixing ratio and GDAS temperature profiles allow us to derive relative humidity profiles with the relative uncertainty of 10–20 %.
- ItemTarget categorization of aerosol and clouds by continuous multiwavelength-polarization lidar measurements(Katlenburg-Lindau : Copernicus, 2017) Baars, Holger; Seifert, Patric; Engelmann, Ronny; Wandinger, UllaAbsolute calibrated signals at 532 and 1064 nm and the depolarization ratio from a multiwavelength lidar are used to categorize primary aerosol but also clouds in high temporal and spatial resolution. Automatically derived particle backscatter coefficient profiles in low temporal resolution (30 min) are applied to calibrate the lidar signals. From these calibrated lidar signals, new atmospheric parameters in temporally high resolution (quasi-particle-backscatter coefficients) are derived. By using thresholds obtained from multiyear, multisite EARLINET (European Aerosol Research Lidar Network) measurements, four aerosol classes (small; large, spherical; large, non-spherical; mixed, partly nonspherical) and several cloud classes (liquid, ice) are defined. Thus, particles are classified by their physical features (shape and size) instead of by source. The methodology is applied to 2 months of continuous observations (24 h a day, 7 days a week) with the multiwavelength-Raman-polarization lidar PollyXT during the High-Definition Clouds and Precipitation for advancing Climate Prediction (HD(CP)2) Observational Prototype Experiment (HOPE) in spring 2013. Cloudnet equipment was operated continuously directly next to the lidar and is used for comparison. By discussing three 24 h case studies, it is shown that the aerosol discrimination is very feasible and informative and gives a good complement to the Cloudnet target categorization. Performing the categorization for the 2-month data set of the entire HOPE campaign, almost 1 million pixel (5 min×30 m) could be analysed with the newly developed tool. We find that the majority of the aerosol trapped in the planetary boundary layer (PBL) was composed of small particles as expected for a heavily populated and industrialized area. Large, spherical aerosol was observed mostly at the top of the PBL and close to the identified cloud bases, indicating the importance of hygroscopic growth of the particles at high relative humidity. Interestingly, it is found that on several days non-spherical particles were dispersed from the ground into the atmosphere.