2016, Rusumdar, A.J., Wolke, R., Tilgner, A., Herrmann, H.

Ambient tropospheric deliquesced particles generally comprise a complex mixture of electrolytes, organic compounds, and water. Dynamic modeling of physical and chemical processes in this complex matrix is challenging. Thus, up-to-date multiphase chemistry models generally do not consider non-ideal solution effects. Therefore, the present study was aimed at presenting further development of the SPACCIM (Spectral Aerosol Cloud Chemistry Interaction Model) through treatment of solution non-ideality, which has not been considered before. The present paper firstly describes the model developments including (i) the implementation of solution non-ideality in aqueous-phase reaction kinetics in the SPACCIM framework, (ii) the advancements in the coupling scheme of microphysics and multiphase chemistry and (iii) the required adjustments of the numerical schemes, especially in the sparse linear solver and the calculation of the Jacobian. Secondly, results of sensitivity investigations are outlined, aiming at the evaluation of different activity coefficient modules and the examination of the contributions of different intermolecular forces to the overall activity coefficients. Finally, first results obtained with the new model framework are presented. The SPACCIM parcel model was developed and, so far, applied for the description of aerosol–cloud interactions. To advance SPACCIM also for modeling physical and chemical processes in deliquesced particles, the solution non-ideality has to be taken into account by utilizing activities in reaction terms instead of aqueous concentrations. The main goal of the extended approach was to provide appropriate activity coefficients for solved species. Therefore, an activity coefficient module was incorporated into the kinetic model framework of SPACCIM. Based on an intercomparison of different activity coefficient models and the comparison with experimental data, the AIOMFAC approach was implemented and extended by additional interaction parameters from the literature for mixed organic–inorganic systems. Moreover, the performance and the capability of the applied activity coefficient module were evaluated by means of water activity measurements, literature data and results of other activity coefficient models. Comprehensive comparison studies showed that the SpactMod (SPACCIM activity coefficient module) is valuable for predicting the thermodynamic behavior of complex mixtures of multicomponent atmospheric aerosol particles. First simulations with a detailed chemical mechanism have demonstrated the applicability of SPACCIM-SpactMod. The simulations indicate that the treatment of solution non-ideality might be needed for modeling multiphase chemistry processes in deliquesced particles. The modeled activity coefficients imply that chemical reaction fluxes of chemical processes in deliquesced particles can be both decreased and increased depending on the particular species involved in the reactions. For key ions, activity coefficients on the order of 0.1–0.8 and a strong dependency on the charge state as well as the RH conditions are modeled, implying a lowered chemical processing of ions in concentrated solutions. In contrast, modeled activity coefficients of organic compounds are in some cases larger than 1 under deliquesced particle conditions and suggest the possibility of an increased chemical processing of organic compounds. Moreover, the model runs have shown noticeable differences in the pH values calculated with and without consideration of solution non-ideality. On average, the predicted pH values of the simulations considering solution non-ideality are −0.27 and −0.44 pH units lower under 90 and 70 % RH conditions, respectively. More comprehensive results of detailed SPACCIM-SpactMod studies on the multiphase processing in organic–inorganic mixtures of deliquesced particles are described in a companion paper.

2009, Zecha, M., Röttger, J.

Observations of polar mesosphere summer echoes (PMSE) have been carried out during the summer periodes 1999–2001 and 2003–2004 at the very high latitude of 78° N using the SOUSY Svalbard Radar (53.5 MHz) at Longyearbyen. Although the measurements could not be done continuously in these seasons, PMSE have been detected over more than 6600 h of 9300 h of observation time overall. Using this data base, particular PMSE occurrence characteristics have been determined. PMSE at Svalbard appear from the middle of May to the end of August with an almost permanent total occurrence in June and July. Diurnal variations are observable in the height-depend occurrence rates and in PMSE thickness, they show a maximum around 09:00–10:00 UTC and a minimum around 21:00–22:00 UTC. PMSE occur nearly exclusively between a height of 80 km and 92 km with a maximum near 85 km. However, PMSE appear not simultaneously over the entire height range, the mean vertical PMSE extension is around 4–6 km in June and July. Furthermore, typically PMSE are separated into several layers, and only 30% of all PMSE are single layers. The probability of multiple layers is greater in June and July than at the beginning and the end of the PMSE season and shows a marked 5-day-variation. The same variation is noticeable in the seasonal dependence of the PMSE occurrence and the PMSE thickness. We finally discuss potential geophysical processes to explain our observational results.

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.

2016, Wandinger, Ulla, Freudenthaler, Volker, Baars, Holger, Amodeo, Aldo, Engelmann, Ronny, Mattis, Ina, Groß, Silke, Pappalardo, Gelsomina, Giunta, Aldo, D'Amico, Giuseppe, Chaikovsky, Anatoli, Osipenko, Fiodor, Slesar, Alexander, Nicolae, Doina, Belegante, Livio, Talianu, Camelia, Serikov, Ilya, Linné, Holger, Jansen, Friedhelm, Apituley, Arnoud, Wilson, Keith M., de Graaf, Martin, Trickl, Thomas, Giehl, Helmut, Adam, Mariana, Comerón, Adolfo, Muñoz-Porcar, Constantino, Rocadenbosch, Francesc, Sicard, Michaël, Tomás, Sergio, Lange, Diego, Kumar, Dhiraj, Pujadas, Manuel, Molero, Francisco, Fernández, Alfonso J., Alados-Arboledas, Lucas, Bravo-Aranda, Juan Antonio, Navas-Guzmán, Francisco, Guerrero-Rascado, Juan Luis, Granados-Muñoz, María José, Preißler, Jana, Wagner, Frank, Gausa, Michael, Grigorov, Ivan, Stoyanov, Dimitar, Iarlori, Marco, Rizi, Vincenco, Spinelli, Nicola, Boselli, Antonella, Wang, Xuan, Feudo, Teresa Lo, Perrone, Maria Rita, De Tomas, Ferdinando, Burlizzi, Pasquale

This paper introduces the recent European Aerosol Research Lidar Network (EARLINET) quality-assurance efforts at instrument level. Within two dedicated campaigns and five single-site intercomparison activities, 21 EARLINET systems from 18 EARLINET stations were intercompared between 2009 and 2013. A comprehensive strategy for campaign setup and data evaluation has been established. Eleven systems from nine EARLINET stations participated in the EARLINET Lidar Intercomparison 2009 (EARLI09). In this campaign, three reference systems were qualified which served as traveling standards thereafter. EARLINET systems from nine other stations have been compared against these reference systems since 2009. We present and discuss comparisons at signal and at product level from all campaigns for more than 100 individual measurement channels at the wavelengths of 355, 387, 532, and 607 nm. It is shown that in most cases, a very good agreement of the compared systems with the respective reference is obtained. Mean signal deviations in predefined height ranges are typically below ±2 %. Particle backscatter and extinction coefficients agree within ±2  ×  10−4 km−1 sr−1 and ± 0.01 km−1, respectively, in most cases. For systems or channels that showed larger discrepancies, an in-depth analysis of deficiencies was performed and technical solutions and upgrades were proposed and realized. The intercomparisons have reinforced confidence in the EARLINET data quality and allowed us to draw conclusions on necessary system improvements for some instruments and to identify major challenges that need to be tackled in the future.

2016, Heinold, Bernd, Tegen, Ina, Schepanski, Kerstin, Banks, Jamie R.

In the aerosol-climate model ECHAM6-HAM2, dust source activation (DSA) observations from Meteosat Second Generation (MSG) satellite are proposed to replace the original source area parameterization over the Sahara Desert. The new setup is tested in nudged simulations for the period 2007 to 2008. The evaluation is based on comparisons to dust emission events inferred from MSG dust index imagery, Aerosol Robotic Network (AERONET) sun photometer observations, and satellite retrievals of aerosol optical thickness (AOT). The model results agree well with AERONET measurements especially in terms of seasonal variability, and a good spatial correlation was found between model results and MSG-SEVIRI (Spinning-Enhanced Visible and InfraRed Imager) dust AOT as well as Multi-angle Imaging SpectroRadiometer (MISR) AOT. ECHAM6-HAM2 computes a more realistic geographical distribution and up to 20 % higher annual Saharan dust emissions, using the MSG-based source map. The representation of dust AOT is partly improved in the southern Sahara and Sahel. In addition, the spatial variability is increased towards a better agreement with observations depending on the season. Thus, using the MSG DSA map can help to circumvent the issue of uncertain soil input parameters. An important issue remains the need to improve the model representation of moist convection and stable nighttime conditions. Compared to sub-daily DSA information from MSG-SEVIRI and results from a regional model, ECHAM6-HAM2 notably underestimates the important fraction of morning dust events by the breakdown of the nocturnal low-level jet, while a major contribution is from afternoon-to-evening emissions.

2009, Brattli, A., Lie-Svendsen, Ø., Svenes, K., Hoppe, U.-P., Strelnikova, I., Rapp, M., Latteck, R., Torkar, K., Gumbel, J., Megner, L., Baumgarten, G.

The ECOMA series of rocket payloads use a set of aerosol particle, plasma, and optical instruments to study the properties of aerosol particles and their interaction with the ambient plasma environment in the polar mesopause region. In August 2007 the ECOMA-3 payload was launched into a region with Polar Mesosphere Summer Echoes (PMSE) and noctilucent clouds (NLC). An electron depletion was detected in a broad region between 83 and 88 km, coincident with enhanced density of negatively charged aerosol particles. We also find evidence for positive ion depletion in the same region. Charge neutrality requires that a population of positively charged particles smaller than 2 nm and with a density of at least 2×108 m−3 must also have been present in the layer, undetected by the instruments. A numerical model for the charging of aerosol particles and their interaction with the ambient plasma is used to analyse the results, showing that high aerosol particle densities are required in order to explain the observed ion density depletion. The model also shows that a very high photoionisation rate is required for the particles smaller than 2 nm to become positively charged, indicating that these may have a lower work function than pure water ice.

2016, Engelmann, Ronny, Kanitz, Thomas, Baars, Holger, Heese, Birgit, Althausen, Dietrich, Skupin, Annett, Wandinger, Ulla, Komppula, Mika, Stachlewska, Iwona S., Amiridis, Vassilis, Marinou, Eleni, Mattis, Ina, Linné, Holger, Ansmann, Albert

The atmospheric science community demands autonomous and quality-assured vertically resolved measurements of aerosol and cloud properties. For this purpose, a portable lidar called Polly was developed at TROPOS in 2003. The lidar system was continuously improved with gained experience from the EARLINET community, involvement in worldwide field campaigns, and international institute collaborations within the last 10 years. Here we present recent changes of the setup of the portable multiwavelength Raman and polarization lidar PollyXT and discuss the improved capabilities of the system by means of a case study. The latest system developments include an additional near-range receiver unit for Raman measurements of the backscatter and extinction coefficient down to 120 m above ground, a water-vapor channel, and channels for simultaneous measurements of the particle linear depolarization ratio at 355 and 532 nm. Quality improvements were achieved by systematically following the EARLINET guidelines and the international PollyNET quality assurance developments. A modified ship radar ensures measurements in agreement with air-traffic safety regulations and allows for 24∕7 monitoring of the atmospheric state with PollyXT.

2017, Meinshausen, Malte, Vogel, Elisabeth, Nauels, Alexander, Lorbacher, Katja, Meinshausen, Nicolai, Etheridge, David M., Fraser, Paul J., Montzka, Stephen A., Rayner, Peter J., Trudinger, Cathy M., Krummel, Paul B., Beyerle, Urs, Canadell, Josep G., Daniel, John S., Enting, Ian G., Law, Rachel M. Law, Lunder, Chris R., O'Doherty, Simon, Prinn, Ron G., Reimann, Stefan, Rubino, Mauro, Velders, Guus J.M., Vollmer, Martin K., Wang, Ray H.J., Weiss, Ray

Atmospheric greenhouse gas (GHG) concentrations are at unprecedented, record-high levels compared to the last 800000 years. Those elevated GHG concentrations warm the planet and – partially offset by net cooling effects by aerosols – are largely responsible for the observed warming over the past 150 years. An accurate representation of GHG concentrations is hence important to understand and model recent climate change. So far, community efforts to create composite datasets of GHG concentrations with seasonal and latitudinal information have focused on marine boundary layer conditions and recent trends since the 1980s. Here, we provide consolidated datasets of historical atmospheric concentrations (mole fractions) of 43 GHGs to be used in the Climate Model Intercomparison Project – Phase 6 (CMIP6) experiments. The presented datasets are based on AGAGE and NOAA networks, firn and ice core data, and archived air data, and a large set of published studies. In contrast to previous intercomparisons, the new datasets are latitudinally resolved and include seasonality. We focus on the period 1850–2014 for historical CMIP6 runs, but data are also provided for the last 2000 years. We provide consolidated datasets in various spatiotemporal resolutions for carbon dioxide (CO2), methane (CH4) and nitrous oxide (N2O), as well as 40 other GHGs, namely 17 ozone-depleting substances, 11 hydrofluorocarbons (HFCs), 9 perfluorocarbons (PFCs), sulfur hexafluoride (SF6), nitrogen trifluoride (NF3) and sulfuryl fluoride (SO2F2). In addition, we provide three equivalence species that aggregate concentrations of GHGs other than CO2, CH4 and N2O, weighted by their radiative forcing efficiencies. For the year 1850, which is used for pre-industrial control runs, we estimate annual global-mean surface concentrations of CO2 at 284.3ppm, CH4 at 808.2ppb and N2O at 273.0ppb. The data are available at https://esgf-node.llnl.gov/search/input4mips/ and http://www.climatecollege.unimelb.edu.au/cmip6. While the minimum CMIP6 recommendation is to use the global- and annual-mean time series, modelling groups can also choose our monthly and latitudinally resolved concentrations, which imply a stronger radiative forcing in the Northern Hemisphere winter (due to the latitudinal gradient and seasonality).

2012, Pietikäinen, J.-P., O'Donnell, D., Teichmann, C., Karstens, U., Pfeifer, S., Kazil, J., Podzun, R., Fiedler, S., Kokkola, H., Birmili, W., O'Dowd, C., Baltensperger, U., Weingartner, E., Gehrig, R., Spindler, G., Kulmala, M., Feichter, J., Jacob, D., Laaksonen, A.

REMO-HAM is a new regional aerosol-climate model. It is based on the REMO regional climate model and includes most of the major aerosol processes. The structure for aerosol is similar to the global aerosol-climate model ECHAM5-HAM, for example the aerosol module HAM is coupled with a two-moment stratiform cloud scheme. On the other hand, REMO-HAM does not include an online coupled aerosol-radiation nor a secondary organic aerosol module. In this work, we evaluate the model and compare the results against ECHAM5-HAM and measurements. Four different measurement sites were chosen for the comparison of total number concentrations, size distributions and gas phase sulfur dioxide concentrations: Hyytiälä in Finland, Melpitz in Germany, Mace Head in Ireland and Jungfraujoch in Switzerland. REMO-HAM is run with two different resolutions: 50 × 50 km2 and 10 × 10 km2. Based on our simulations, REMO-HAM is in reasonable agreement with the measured values. The differences in the total number concentrations between REMO-HAM and ECHAM5-HAM can be mainly explained by the difference in the nucleation mode. Since we did not use activation nor kinetic nucleation for the boundary layer, the total number concentrations are somewhat underestimated. From the meteorological point of view, REMO-HAM represents the precipitation fields and 2 m temperature profile very well compared to measurement. Overall, we show that REMO-HAM is a functional aerosol-climate model, which will be used in further studies.

2015, D'Amico, Giuseppe, Amodeo, A., Baars, H., Binietoglou, I., Freudenthaler, V., Mattis, I., Wandinger, U., Pappalardo, G.

In this paper we describe the EARLINET Single Calculus Chain (SCC), a tool for the automatic analysis of lidar measurements. The development of this tool started in the framework of EARLINET-ASOS (European Aerosol Research Lidar Network – Advanced Sustainable Observation System); it was extended within ACTRIS (Aerosol, Clouds and Trace gases Research InfraStructure Network), and it is continuing within ACTRIS-2. The main idea was to develop a data processing chain that allows all EARLINET stations to retrieve, in a fully automatic way, the aerosol backscatter and extinction profiles starting from the raw lidar data of the lidar systems they operate. The calculus subsystem of the SCC is composed of two modules: a pre-processor module which handles the raw lidar data and corrects them for instrumental effects and an optical processing module for the retrieval of aerosol optical products from the pre-processed data. All input parameters needed to perform the lidar analysis are stored in a database to keep track of all changes which may occur for any EARLINET lidar system over the time. The two calculus modules are coordinated and synchronized by an additional module (daemon) which makes the whole analysis process fully automatic. The end user can interact with the SCC via a user-friendly web interface. All SCC modules are developed using open-source and freely available software packages. The final products retrieved by the SCC fulfill all requirements of the EARLINET quality assurance programs on both instrumental and algorithm levels. Moreover, the manpower needed to provide aerosol optical products is greatly reduced and thus the near-real-time availability of lidar data is improved. The high-quality of the SCC products is proven by the good agreement between the SCC analysis, and the corresponding independent manual retrievals. Finally, the ability of the SCC to provide high-quality aerosol optical products is demonstrated for an EARLINET intense observation period.