Search Results
Results and recommendations from an intercomparison of six Hygroscopicity-TDMA systems
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.
Lessons learnt from the first EMEP intensive measurement periods
2012, Aas, W., Tsyro, S., Bieber, E., Bergström, R., Ceburnis, D., Ellermann, T., Fagerli, H., Frölich, M., Gehrig, R., Makkonen, U., Nemitz, E., Otjes, R., Perez, N., Perrino, C., Prévôt, A.S.H., Putaud, J.-P., Simpson, D., Spindler, G., Vana, M., Yttri, K.E.
The first EMEP intensive measurement periods were held in June 2006 and January 2007. The measurements aimed to characterize the aerosol chemical compositions, including the gas/aerosol partitioning of inorganic compounds. The measurement program during these periods included daily or hourly measurements of the secondary inorganic components, with additional measurements of elemental- and organic carbon (EC and OC) and mineral dust in PM1, PM2.5 and PM10. These measurements have provided extended knowledge regarding the composition of particulate matter and the temporal and spatial variability of PM, as well as an extended database for the assessment of chemical transport models. This paper summarise the first experiences of making use of measurements from the first EMEP intensive measurement periods along with EMEP model results from the updated model version to characterise aerosol composition. We investigated how the PM chemical composition varies between the summer and the winter month and geographically. The observation and model data are in general agreement regarding the main features of PM10 and PM2.5 composition and the relative contribution of different components, though the EMEP model tends to give slightly lower estimates of PM10 and PM2.5 compared to measurements. The intensive measurement data has identified areas where improvements are needed. Hourly concurrent measurements of gaseous and particulate components for the first time facilitated testing of modelled diurnal variability of the gas/aerosol partitioning of nitrogen species. In general, the modelled diurnal cycles of nitrate and ammonium aerosols are in fair agreement with the measurements, but the diurnal variability of ammonia is not well captured. The largest differences between model and observations of aerosol mass are seen in Italy during winter, which to a large extent may be explained by an underestimation of residential wood burning sources. It should be noted that both primary and secondary OC has been included in the calculations for the first time, showing promising results. Mineral dust is important, especially in southern Europe, and the model seems to capture the dust episodes well. The lack of measurements of mineral dust hampers the possibility for model evaluation for this highly uncertain PM component. There are also lessons learnt regarding improved measurements for future intensive periods. There is a need for increased comparability between the measurements at different sites. For the nitrogen compounds it is clear that more measurements using artefact free methods based on continuous measurement methods and/or denuders are needed. For EC/OC, a reference methodology (both in field and laboratory) was lacking during these periods giving problems with comparability, though measurement protocols have recently been established and these should be followed by the Parties to the EMEP Protocol. For measurements with no defined protocols, it might be a good solution to use centralised laboratories to ensure comparability across the network. To cope with the introduction of these new measurements, new reporting guidelines have been developed to ensure that all proper information about the methodologies and data quality is given.
GARRLiC and LIRIC: Strengths and limitations for the characterization of dust and marine particles along with their mixtures
2017, Tsekeri, Alexandra, Lopatin, Anton, Amiridis, Vassilis, Marinou, Eleni, Igloffstein, Julia, Siomos, Nikolaos, Solomos, Stavros, Kokkalis, Panagiotis, Engelmann, Ronny, Baars, Holger, Gratsea, Myrto, Raptis, Panagiotis I., Binietoglou, Ioannis, Mihalopoulos, Nikolaos, Kalivitis, Nikolaos, Kouvarakis, Giorgos, Bartsotas, Nikolaos, Kallos, George, Basart, Sara, Schuettemeyer, Dirk, Wandinger, Ulla, Ansmann, Albert, Chaikovsky, Anatoli P., Dubovik, Oleg
The Generalized Aerosol Retrieval from Radiometer and Lidar Combined data algorithm (GARRLiC) and the LIdar-Radiometer Inversion Code (LIRIC) provide the opportunity to study the aerosol vertical distribution by combining ground-based lidar and sun-photometric measurements. Here, we utilize the capabilities of both algorithms for the characterization of Saharan dust and marine particles, along with their mixtures, in the south-eastern Mediterranean during the CHARacterization of Aerosol mixtures of Dust and Marine origin Experiment (CHARADMExp). Three case studies are presented, focusing on dust-dominated, marinedominated and dust-marine mixing conditions. GARRLiC and LIRIC achieve a satisfactory characterization for the dust-dominated case in terms of particle microphysical properties and concentration profiles. The marine-dominated and the mixture cases are more challenging for both algorithms, although GARRLiC manages to provide more detailed microphysical retrievals compared to AERONET, while LIRIC effectively discriminates dust and marine particles in its concentration profile retrievals. The results are also compared with modelled dust and marine concentration profiles and surface in situ measurements.
Mobility particle size spectrometers: Harmonization of technical standards and data structure to facilitate high quality long-term observations of atmospheric particle number size distributions
2012, Wiedensohler, A., Birmili, W., Nowak, A., Sonntag, A., Weinhold, K., Merkel, M., Wehner, B., Tuch, T., Pfeifer, S., Fiebig, M., Fjäraa, A.M., Asmi, E., Sellegri, K., Depuy, R., Venzac, H., Villani, P., Laj, P., Aalto, P., Ogren, J.A., Swietlick, E., Williams, P., Roldin, P., Quincey, P., Hüglin, C., Fierz-Schmidhauser, R., Gysel, M., Weingartner, E., Riccobono, F., Santos, S., Grüning, C., Faloon, K., Beddows, D., Harrison, R., Monahan, C., Jennings, S.G., O'Dowd, C.D., Marinoni, A., Horn, H.-G., Keck, L., Jiang, J., Scheckman, J., McMurry, P.H., Deng, Z., Zhao, C.S., Moerman, M., Henzing, B., de Leeuw, G., Löschau, G., Bastian, S.
Mobility particle size spectrometers often referred to as DMPS (Differential Mobility Particle Sizers) or SMPS (Scanning Mobility Particle Sizers) have found a wide range of applications in atmospheric aerosol research. However, comparability of measurements conducted world-wide is hampered by lack of generally accepted technical standards and guidelines with respect to the instrumental set-up, measurement mode, data evaluation as well as quality control. Technical standards were developed for a minimum requirement of mobility size spectrometry to perform long-term atmospheric aerosol measurements. Technical recommendations include continuous monitoring of flow rates, temperature, pressure, and relative humidity for the sheath and sample air in the differential mobility analyzer. We compared commercial and custom-made inversion routines to calculate the particle number size distributions from the measured electrical mobility distribution. All inversion routines are comparable within few per cent uncertainty for a given set of raw data. Furthermore, this work summarizes the results from several instrument intercomparison workshops conducted within the European infrastructure project EUSAAR (European Supersites for Atmospheric Aerosol Research) and ACTRIS (Aerosols, Clouds, and Trace gases Research InfraStructure Network) to determine present uncertainties especially of custom-built mobility particle size spectrometers. Under controlled laboratory conditions, the particle number size distributions from 20 to 200 nm determined by mobility particle size spectrometers of different design are within an uncertainty range of around ±10% after correcting internal particle losses, while below and above this size range the discrepancies increased. For particles larger than 200 nm, the uncertainty range increased to 30%, which could not be explained. The network reference mobility spectrometers with identical design agreed within ±4% in the peak particle number concentration when all settings were done carefully. The consistency of these reference instruments to the total particle number concentration was demonstrated to be less than 5%. Additionally, a new data structure for particle number size distributions was introduced to store and disseminate the data at EMEP (European Monitoring and Evaluation Program). This structure contains three levels: raw data, processed data, and final particle size distributions. Importantly, we recommend reporting raw measurements including all relevant instrument parameters as well as a complete documentation on all data transformation and correction steps. These technical and data structure standards aim to enhance the quality of long-term size distribution measurements, their comparability between different networks and sites, and their transparency and traceability back to raw data.
Reactive Halogens in the Marine Boundary Layer (RHaMBLe): The tropical North Atlantic experiments
2010, Lee, J.D., McFiggans, G., Allan, J.D., Baker, A.R., Ball, S.M., Benton, A.K., Carpenter, L.J., Commane, R., Finley, B.D., Evans, M., Fuentes, E., Furneaux, K., Goddard, A., Good, N., Hamilton, J.F., Heard, D.E., Herrmann, H., Hollingsworth, A., Hopkins, J.R., Ingham, T., Irwin, M., Jones, C.E., Jones, R.L., Keene, W.C., Lawler, M.J., Lehmann, S., Lewis, A.C., Long, M.S., Mahajan, A., Methven, J., Moller, S.J., Müller, K., Müller, T., Niedermeier, N., O'Doherty, S., Oetjen, H., Plane, J.M.C., Pszenny, A.A.P., Read, K.A., Saiz-Lopez, A., Saltzman, E.S., Sander, R., von Glasow, R., Whalley, L., Wiedensohler, A., Young, D.
The NERC UK SOLAS-funded Reactive Halogens in the Marine Boundary Layer (RHaMBLe) programme comprised three field experiments. This manuscript presents an overview of the measurements made within the two simultaneous remote experiments conducted in the tropical North Atlantic in May and June 2007. Measurements were made from two mobile and one ground-based platforms. The heavily instrumented cruise D319 on the RRS Discovery from Lisbon, Portugal to São Vicente, Cape Verde and back to Falmouth, UK was used to characterise the spatial distribution of boundary layer components likely to play a role in reactive halogen chemistry. Measurements onboard the ARSF Dornier aircraft were used to allow the observations to be interpreted in the context of their vertical distribution and to confirm the interpretation of atmospheric structure in the vicinity of the Cape Verde islands. Long-term ground-based measurements at the Cape Verde Atmospheric Observatory (CVAO) on São Vicente were supplemented by long-term measurements of reactive halogen species and characterisation of additional trace gas and aerosol species during the intensive experimental period. This paper presents a summary of the measurements made within the RHaMBLe remote experiments and discusses them in their meteorological and chemical context as determined from these three platforms and from additional meteorological analyses. Air always arrived at the CVAO from the North East with a range of air mass origins (European, Atlantic and North American continental). Trace gases were present at stable and fairly low concentrations with the exception of a slight increase in some anthropogenic components in air of North American origin, though NOx mixing ratios during this period remained below 20 pptv (note the non-IUPAC adoption in this manuscript of pptv and ppbv, equivalent to pmol mol−1 and nmol mol−1 to reflect common practice). Consistency with these air mass classifications is observed in the time series of soluble gas and aerosol composition measurements, with additional identification of periods of slightly elevated dust concentrations consistent with the trajectories passing over the African continent. The CVAO is shown to be broadly representative of the wider North Atlantic marine boundary layer; measurements of NO, O3 and black carbon from the ship are consistent with a clean Northern Hemisphere marine background. Aerosol composition measurements do not indicate elevated organic material associated with clean marine air. Closer to the African coast, black carbon and NO levels start to increase, indicating greater anthropogenic influence. Lower ozone in this region is possibly associated with the increased levels of measured halocarbons, associated with the nutrient rich waters of the Mauritanian upwelling. Bromide and chloride deficits in coarse mode aerosol at both the CVAO and on D319 and the continuous abundance of inorganic gaseous halogen species at CVAO indicate significant reactive cycling of halogens. Aircraft measurements of O3 and CO show that surface measurements are representative of the entire boundary layer in the vicinity both in diurnal variability and absolute levels. Above the inversion layer similar diurnal behaviour in O3 and CO is observed at lower mixing ratios in the air that had originated from south of Cape Verde, possibly from within the ITCZ. ECMWF calculations on two days indicate very different boundary layer depths and aircraft flights over the ship replicate this, giving confidence in the calculated boundary layer depth.
Aerosol particle measurements at three stationary sites in the megacity of Paris during summer 2009: Meteorology and air mass origin dominate aerosol particle composition and size distribution
2013, Freutel, F., Schneider, J., Drewnick, F., Weiden-Reinmüller, S.-L., Crippa, M., Prévôt, A.S.H., Baltensperger, U., Poulain, L., Wiedensohler, R.A., Sciare, J., Sarda-Estève, R., Burkhart, J.F., Eckhardt, S., Stohl, A., Gros, V., Colomb, A., Michoud, V., Doussin, J.F., Borbon, A., Haeffelin, M., Morille, Y., Beekmann, M., Borrmann, S.
During July 2009, a one-month measurement campaign was performed in the megacity of Paris. Amongst other measurement platforms, three stationary sites distributed over an area of 40 km in diameter in the greater Paris region enabled a detailed characterization of the aerosol particle and gas phase. Simulation results from the FLEXPART dispersion model were used to distinguish between different types of air masses sampled. It was found that the origin of air masses had a large influence on measured mass concentrations of the secondary species particulate sulphate, nitrate, ammonium, and oxygenated organic aerosol measured with the Aerodyne aerosol mass spectrometer in the submicron particle size range: particularly high concentrations of these species (about 4 μg m−3, 2 μg m−3, 2 μg m−3, and 7 μg m−3, respectively) were measured when aged material was advected from continental Europe, while for air masses originating from the Atlantic, much lower mass concentrations of these species were observed (about 1 μg m−3, 0.2 μg m−3, 0.4 μg m−3, and 1–3 μg m−3, respectively). For the primary emission tracers hydrocarbon-like organic aerosol, black carbon, and NOx it was found that apart from diurnal source strength variations and proximity to emission sources, local meteorology had the largest influence on measured concentrations, with higher wind speeds leading to larger dilution and therefore smaller measured concentrations. Also the shape of particle size distributions was affected by wind speed and air mass origin. Quasi-Lagrangian measurements performed under connected flow conditions between the three stationary sites were used to estimate the influence of the Paris emission plume onto its surroundings, which was found to be rather small. Rough estimates for the impact of the Paris emission plume on the suburban areas can be inferred from these measurements: Volume mixing ratios of 1–14 ppb of NOx, and upper limits for mass concentrations of about 1.5 μg m−3 of black carbon and of about 3 μg m−3 of hydrocarbon-like organic aerosol can be deduced which originate from both, local emissions and the overall Paris emission plume. The secondary aerosol particle phase species were found to be not significantly influenced by the Paris megacity, indicating their regional origin. The submicron aerosol mass concentrations of particulate sulphate, nitrate, and ammonium measured during time periods when air masses were advected from eastern central Europe were found to be similar to what has been found from other measurement campaigns in Paris and south-central France for this type of air mass origin, indicating that the results presented here are also more generally valid.
The Ice Selective Inlet: A novel technique for exclusive extraction of pristine ice crystals in mixed-phase clouds
2015, Kupiszewski, P., Weingartner, E., Vochezer, P., Schnaiter, M., Bigi, A., Gysel, M., Rosati, B., Toprak, E., Mertes, S., Baltensperger, U.
Climate predictions are affected by high uncertainties partially due to an insufficient knowledge of aerosol–cloud interactions. One of the poorly understood processes is formation of mixed-phase clouds (MPCs) via heterogeneous ice nucleation. Field measurements of the atmospheric ice phase in MPCs are challenging due to the presence of much more numerous liquid droplets. The Ice Selective Inlet (ISI), presented in this paper, is a novel inlet designed to selectively sample pristine ice crystals in mixed-phase clouds and extract the ice residual particles contained within the crystals for physical and chemical characterization. Using a modular setup composed of a cyclone impactor, droplet evaporation unit and pumped counterflow virtual impactor (PCVI), the ISI segregates particles based on their inertia and phase, exclusively extracting small ice particles between 5 and 20 μm in diameter. The setup also includes optical particle spectrometers for analysis of the number size distribution and shape of the sampled hydrometeors. The novelty of the ISI is a droplet evaporation unit, which separates liquid droplets and ice crystals in the airborne state, thus avoiding physical impaction of the hydrometeors and limiting potential artefacts. The design and validation of the droplet evaporation unit is based on modelling studies of droplet evaporation rates and computational fluid dynamics simulations of gas and particle flows through the unit. Prior to deployment in the field, an inter-comparison of the optical particle size spectrometers and a characterization of the transmission efficiency of the PCVI was conducted in the laboratory. The ISI was subsequently deployed during the Cloud and Aerosol Characterization Experiment (CLACE) 2013 and 2014 – two extensive international field campaigns encompassing comprehensive measurements of cloud microphysics, as well as bulk aerosol, ice residual and ice nuclei properties. The campaigns provided an important opportunity for a proof of concept of the inlet design. In this work we present the setup of the ISI, including the modelling and laboratory characterization of its components, as well as field measurements demonstrating the ISI performance and validating the working principle of the inlet. Finally, measurements of biological aerosol during a Saharan dust event (SDE) are presented, showing a first indication of enrichment of bio-material in sub-2 μm ice residuals.
The chemistry of OH and HO2 radicals in the boundary layer over the tropical Atlantic Ocean
2010, Whalley, L.K., Furneaux, K.L., Goddard, A., Lee, J.D., Mahajan, A., Oetjen, H., Read, K.A., Kaaden, N., Carpenter, L.J., Lewis, A.C., Plane, J.M.C., Saltzman, E.S., Wiedensohler, A., Heard, D.E.
Fluorescence Assay by Gas Expansion (FAGE) has been used to detect ambient levels of OH and HO2 radicals at the Cape Verde Atmospheric Observatory, located in the tropical Atlantic marine boundary layer, during May and June 2007. Midday radical concentrations were high, with maximum concentrations of 9 ×106 molecule cm−3 and 6×108 molecule cm−3 observed for OH and HO2, respectively. A box model incorporating the detailed Master Chemical Mechanism, extended to include halogen chemistry, heterogeneous loss processes and constrained by all available measurements including halogen and nitrogen oxides, has been used to assess the chemical and physical parameters controlling the radical chemistry. The model was able to reproduce the daytime radical concentrations to within the 1 σ measurement uncertainty of 20% during the latter half of the measurement period but significantly under-predicted [HO2] by 39% during the first half of the project. Sensitivity analyses demonstrate that elevated [HCHO] (~2 ppbv) on specific days during the early part of the project, which were much greater than the mean [HCHO] (328 pptv) used to constrain the model, could account for a large portion of the discrepancy between modelled and measured [HO2] at this time. IO and BrO, although present only at a few pptv, constituted ~19% of the instantaneous sinks for HO2, whilst aerosol uptake and surface deposition to the ocean accounted for a further 23% of the HO2 loss at noon. Photolysis of HOI and HOBr accounted for ~13% of the instantaneous OH formation. Taking into account that halogen oxides increase the oxidation of NOx (NO → NO2), and in turn reduce the rate of formation of OH from the reaction of HO2 with NO, OH concentrations were estimated to be 9% higher overall due to the presence of halogens. The increase in modelled OH from halogen chemistry gives an estimated 9% shorter lifetime for methane in this region, and the inclusion of halogen chemistry is necessary to model the observed daily cycle of O3 destruction that is observed at the surface. Due to surface losses, we hypothesise that HO2 concentrations increase with height and therefore contribute a larger fraction of the O3 destruction than at the surface.
A concept of an automated function control for ambient aerosol measurements using mobility particle size spectrometers
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.
Target categorization of aerosol and clouds by continuous multiwavelength-polarization lidar measurements
2017, Baars, Holger, Seifert, Patric, Engelmann, Ronny, Wandinger, Ulla
Absolute 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.
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