Search Results
The second ACTRIS inter-comparison (2016) for Aerosol Chemical Speciation Monitors (ACSM): Calibration protocols and instrument performance evaluations
2019, Freney, Evelyn, Zhang, Yunjiang, Croteau, Philip, Amodeo, Tanguy, Williams, Leah, Truong, François, Petit, Jean-Eudes, Sciare, Jean, Sarda-Esteve, Roland, Bonnaire, Nicolas, Arumae, Tarvo, Aurela, Minna, Bougiatioti, Aikaterini, Mihalopoulos, Nikolaos, Coz, Esther, Artinano, Begoña, Crenn, Vincent, Elste, Thomas, Heikkinen, Liine, Poulain, Laurent, Wiedensohler, Alfred, Herrmann, Hartmut, Priestman, Max, Alastuey, Andres, Stavroulas, Iasonas, Tobler, Anna, Vasilescu, Jeni, Zanca, Nicola, Canagaratna, Manjula, Carbone, Claudio, Flentje, Harald, Green, David, Maasikmets, Marek, Marmureanu, Luminita, Cruz Minguillon, Maria, Prevot, Andre S.H., Gros, Valerie, Jayne, John, Favez, Olivier
This work describes results obtained from the 2016 Aerosol Chemical Speciation Monitor (ACSM) intercomparison exercise performed at the Aerosol Chemical Monitor Calibration Center (ACMCC, France). Fifteen quadrupole ACSMs (Q_ACSM) from the European Research Infrastructure for the observation of Aerosols, Clouds and Trace gases (ACTRIS) network were calibrated using a new procedure that acquires calibration data under the same operating conditions as those used during sampling and hence gets information representative of instrument performance. The new calibration procedure notably resulted in a decrease in the spread of the measured sulfate mass concentrations, improving the reproducibility of inorganic species measurements between ACSMs as well as the consistency with co-located independent instruments. Tested calibration procedures also allowed for the investigation of artifacts in individual instruments, such as the overestimation of m/z 44 from organic aerosol. This effect was quantified by the m/z (mass-to-charge) 44 to nitrate ratio measured during ammonium nitrate calibrations, with values ranging from 0.03 to 0.26, showing that it can be significant for some instruments. The fragmentation table correction previously proposed to account for this artifact was applied to the measurements acquired during this study. For some instruments (those with high artifacts), this fragmentation table adjustment led to an “overcorrection” of the f44 (m/z 44/Org) signal. This correction based on measurements made with pure NH4NO3, assumes that the magnitude of the artifact is independent of chemical composition. Using data acquired at different NH4NO3 mixing ratios (from solutions of NH4NO3 and (NH4)2SO4) we observe that the magnitude of the artifact varies as a function of composition. Here we applied an updated correction, dependent on the ambient NO3 mass fraction, which resulted in an improved agreement in organic signal among instruments. This work illustrates the benefits of integrating new calibration procedures and artifact corrections, but also highlights the benefits of these intercomparison exercises to continue to improve our knowledge of how these instruments operate, and assist us in interpreting atmospheric chemistry. © 2019, © 2019 Author(s). Published with license by Taylor & Francis Group, LLC.
The HITRAN2020 molecular spectroscopic database
2022, Gordon, I.E., Rothman, L.S., Hargreaves, R.J., Hashemi, R., Karlovets, E.V., Skinner, F.M., Conway, E.K., Hill, C., Kochanov, R.V., Tan, Y., Wcisło, P., Finenko, A.A., Nelson, K., Bernath, P.F., Birk, M., Boudon, V., Campargue, A., Chance, K.V., Coustenis, A., Drouin, B.J., Flaud, J.M., Gamache, R.R., Hodges, J.T., Jacquemart, D., Mlawer, E.J., Nikitin, A.V., Perevalov, V.I., Rotger, M., Tennyson, J., Toon, G.C., Tran, H., Tyuterev, V.G., Adkins, E.M., Baker, A., Barbe, A., Canè, E., Császár, A.G., Dudaryonok, A., Egorov, O., Fleisher, A.J., Fleurbaey, H., Foltynowicz, A., Furtenbacher, T., Harrison, J.J., Hartmann, J.M., Horneman, V.M., Huang, X., Karman, T., Karns, J., Kassi, S., Kleiner, I., Kofman, V., Kwabia-Tchana, F., Lavrentieva, N.N., Lee, T.J., Long, D.A., Lukashevskaya, A.A., Lyulin, O.M., Makhnev, V.Yu., Matt, W., Massie, S.T., Melosso, M., Mikhailenko, S.N., Mondelain, D., Müller, H.S.P., Naumenko, O.V., Perrin, A., Polyansky, O.L., Raddaoui, E., Raston, P.L., Reed, Z.D., Rey, M., Richard, C., Tóbiás, R., Sadiek, I., Schwenke, D.W., Starikova, E., Sung, K., Tamassia, F., Tashkun, S.A., Vander Auwera, J., Vasilenko, I.A., Vigasin, A.A., Villanueva, G.L., Vispoel, B., Wagner, G., Yachmenev, A., Yurchenko, S.N.
The HITRAN database is a compilation of molecular spectroscopic parameters. It was established in the early 1970s and is used by various computer codes to predict and simulate the transmission and emission of light in gaseous media (with an emphasis on terrestrial and planetary atmospheres). The HITRAN compilation is composed of five major components: the line-by-line spectroscopic parameters required for high-resolution radiative-transfer codes, experimental infrared absorption cross-sections (for molecules where it is not yet feasible for representation in a line-by-line form), collision-induced absorption data, aerosol indices of refraction, and general tables (including partition sums) that apply globally to the data. This paper describes the contents of the 2020 quadrennial edition of HITRAN. The HITRAN2020 edition takes advantage of recent experimental and theoretical data that were meticulously validated, in particular, against laboratory and atmospheric spectra. The new edition replaces the previous HITRAN edition of 2016 (including its updates during the intervening years). All five components of HITRAN have undergone major updates. In particular, the extent of the updates in the HITRAN2020 edition range from updating a few lines of specific molecules to complete replacements of the lists, and also the introduction of additional isotopologues and new (to HITRAN) molecules: SO, CH3F, GeH4, CS2, CH3I and NF3. Many new vibrational bands were added, extending the spectral coverage and completeness of the line lists. Also, the accuracy of the parameters for major atmospheric absorbers has been increased substantially, often featuring sub-percent uncertainties. Broadening parameters associated with the ambient pressure of water vapor were introduced to HITRAN for the first time and are now available for several molecules. The HITRAN2020 edition continues to take advantage of the relational structure and efficient interface available at www.hitran.org and the HITRAN Application Programming Interface (HAPI). The functionality of both tools has been extended for the new edition.
Do new sea spray aerosol source functions improve the results of a regional aerosol model?
2018, Barthel, Stefan, Tegen, Ina, Wolke, Ralf
Sea spray aerosol particle is a dominating part of the global aerosol mass load of natural origin. Thus, it strongly influences the atmospheric radiation balance and cloud properties especially over the oceans. Uncertainties of the estimated climate impacts by this aerosol type are partly caused by the uncertainties in the particle size dependent emission fluxes of sea spray aerosol particle. We present simulations with a regional aerosol transport model system in two domains, for three months and compared the model results to measurements at four stations using various sea spray aerosol particle source source functions. Despite these limitations we found the results using different source functions are within the range of most model uncertainties. Especially the model's ability to produce realistic wind speeds is crucial. Furthermore, the model results are more affected by a function correcting the emission flux for the effect of the sea surface temperature than by the use of different source functions. © 2018 The Authors
Phenomenology of ultrafine particle concentrations and size distribution across urban Europe
2023, Trechera, Pedro, Garcia-Marlès, Meritxell, Liu, Xiansheng, Reche, Cristina, Pérez, Noemí, Savadkoohi, Marjan, Beddows, David, Salma, Imre, Vörösmarty, Máté, Casans, Andrea, Casquero-Vera, Juan Andrés, Hueglin, Christoph, Marchand, Nicolas, Chazeau, Benjamin, Gille, Grégory, Kalkavouras, Panayiotis, Mihalopoulos, Nikos, Ondracek, Jakub, Zikova, Nadia, Niemi, Jarkko V., Manninen, Hanna E., Green, David C., Tremper, Anja H., Norman, Michael, Vratolis, Stergios, Eleftheriadis, Konstantinos, Gómez-Moreno, Francisco J., Alonso-Blanco, Elisabeth, Gerwig, Holger, Wiedensohler, Alfred, Weinhold, Kay, Merkel, Maik, Bastian, Susanne, Petit, Jean-Eudes, Favez, Olivier, Crumeyrolle, Suzanne, Ferlay, Nicolas, Martins Dos Santos, Sebastiao, Putaud, Jean-Philippe, Timonen, Hilkka, Lampilahti, Janne, Asbach, Christof, Wolf, Carmen, Kaminski, Heinz, Altug, Hicran, Hoffmann, Barbara, Rich, David Q., Pandolfi, Marco, Harrison, Roy M., Hopke, Philip K., Petäjä, Tuukka, Alastuey, Andrés, Querol, Xavier
The 2017–2019 hourly particle number size distributions (PNSD) from 26 sites in Europe and 1 in the US were evaluated focusing on 16 urban background (UB) and 6 traffic (TR) sites in the framework of Research Infrastructures services reinforcing air quality monitoring capacities in European URBAN & industrial areaS (RI-URBANS) project. The main objective was to describe the phenomenology of urban ultrafine particles (UFP) in Europe with a significant air quality focus. The varying lower size detection limits made it difficult to compare PN concentrations (PNC), particularly PN10-25, from different cities. PNCs follow a TR > UB > Suburban (SUB) order. PNC and Black Carbon (BC) progressively increase from Northern Europe to Southern Europe and from Western to Eastern Europe. At the UB sites, typical traffic rush hour PNC peaks are evident, many also showing midday-morning PNC peaks anti-correlated with BC. These peaks result from increased PN10-25, suggesting significant PNC contributions from nucleation, fumigation and shipping. Site types to be identified by daily and seasonal PNC and BC patterns are: (i) PNC mainly driven by traffic emissions, with marked correlations with BC on different time scales; (ii) marked midday/morning PNC peaks and a seasonal anti-correlation with PNC/BC; (iii) both traffic peaks and midday peaks without marked seasonal patterns. Groups (ii) and (iii) included cities with high insolation. PNC, especially PN25-800, was positively correlated with BC, NO2, CO and PM for several sites. The variable correlation of PNSD with different urban pollutants demonstrates that these do not reflect the variability of UFP in urban environments. Specific monitoring of PNSD is needed if nanoparticles and their associated health impacts are to be assessed. Implementation of the CEN-ACTRIS recommendations for PNSD measurements would provide comparable measurements, and measurements of <10 nm PNC are needed for full evaluation of the health effects of this size fraction.
Highly Oxygenated Organic Molecules (HOM) from Gas-Phase Autoxidation Involving Peroxy Radicals: A Key Contributor to Atmospheric Aerosol
2019, Bianchi, Federico, Kurtén, Theo, Riva, Matthieu, Mohr, Claudia, Rissanen, Matti P., Roldin, Pontus, Berndt, Torsten, Crounse, John D., Wennberg, Paul O., Mentel, Thomas F., Wildt, Jürgen, Junninen, Heikki, Jokinen, Tuija, Kulmala, Markku, Worsnop, Douglas R., Thornton, Joel A., Donahue, Neil, Kjaergaard, Henrik G., Ehn, Mikael
Highly oxygenated organic molecules (HOM) are formed in the atmosphere via autoxidation involving peroxy radicals arising from volatile organic compounds (VOC). HOM condense on pre-existing particles and can be involved in new particle formation. HOM thus contribute to the formation of secondary organic aerosol (SOA), a significant and ubiquitous component of atmospheric aerosol known to affect the Earth's radiation balance. HOM were discovered only very recently, but the interest in these compounds has grown rapidly. In this Review, we define HOM and describe the currently available techniques for their identification/quantification, followed by a summary of the current knowledge on their formation mechanisms and physicochemical properties. A main aim is to provide a common frame for the currently quite fragmented literature on HOM studies. Finally, we highlight the existing gaps in our understanding and suggest directions for future HOM research. © 2019 American Chemical Society.
The ocean's vital skin: Toward an integrated understanding of the sea surface microlayer
2017, Engel, Anja, Bange, Hermann W., Cunliffe, Michael, Burrows, Susannah M., Friedrichs, Gernot, Galgani, Luisa, Herrmann, Hartmut, Hertkorn, Norbert, Johnson, Martin, Liss, Peter S., Quinn, Patricia K., Schartau, Markus, Soloviev, Alexander, Stolle, Christian, Upstill-Goddard, Robert C., van Pinxteren, Manuela, Zäncker, Birthe
Despite the huge extent of the ocean's surface, until now relatively little attention has been paid to the sea surface microlayer (SML) as the ultimate interface where heat, momentum and mass exchange between the ocean and the atmosphere takes place. Via the SML, large-scale environmental changes in the ocean such as warming, acidification, deoxygenation, and eutrophication potentially influence cloud formation, precipitation, and the global radiation balance. Due to the deep connectivity between biological, chemical, and physical processes, studies of the SML may reveal multiple sensitivities to global and regional changes. Understanding the processes at the ocean's surface, in particular involving the SML as an important and determinant interface, could therefore provide an essential contribution to the reduction of uncertainties regarding ocean-climate feedbacks. This review identifies gaps in our current knowledge of the SML and highlights a need to develop a holistic and mechanistic understanding of the diverse biological, chemical, and physical processes occurring at the ocean-atmosphere interface. We advocate the development of strong interdisciplinary expertise and collaboration in order to bridge between ocean and atmospheric sciences. Although this will pose significant methodological challenges, such an initiative would represent a new role model for interdisciplinary research in Earth System sciences.
EURODELTA III exercise: An evaluation of air quality models’ capacity to reproduce the carbonaceous aerosol
2019, Mircea, Mihaela, Bessagnet, Bertrand, D'Isidoro, Massimo, Pirovano, Guido, Aksoyoglu, Sebnem, Ciarelli, Giancarlo, Tsyro, Svetlana, Manders, Astrid, Bieser, Johannes, Stern, Rainer, Vivanco, Marta García, Cuvelier, Cornelius, Aas, Wenche, Prévôt, André S.H., Aulinger, Armin, Briganti, Gino, Calori, Giuseppe, Cappelletti, Andrea, Colette, Augustin, Couvidat, Florian, Fagerli, Hilde, Finardi, Sandro, Kranenburg, Richard, Rouïl, Laurence, Silibello, Camillo, Spindler, Gerald, Poulain, Laurent, Herrmann, Hartmut, Jimenez, Jose L., Day, Douglas A., Tiitta, Petri, Carbone, Samara
The carbonaceous aerosol accounts for an important part of total aerosol mass, affects human health and climate through its effects on physical and chemical properties of the aerosol, yet the understanding of its atmospheric sources and sinks is still incomplete. This study shows the state-of-the-art in modelling carbonaceous aerosol over Europe by comparing simulations performed with seven chemical transport models (CTMs) currently in air quality assessments in Europe: CAMx, CHIMERE, CMAQ, EMEP/MSC-W, LOTOS-EUROS, MINNI and RCGC. The simulations were carried out in the framework of the EURODELTA III modelling exercise and were evaluated against field measurements from intensive campaigns of European Monitoring and Evaluation Programme (EMEP) and the European Integrated Project on Aerosol Cloud Climate and Air Quality Interactions (EUCAARI). Model simulations were performed over the same domain, using as much as possible the same input data and covering four seasons: summer (1–30 June 2006), winter (8 January – 4 February 2007), autumn (17 September- 15 October 2008) and spring (25 February - 26 March 2009). The analyses of models’ performances in prediction of elemental carbon (EC) for the four seasons and organic aerosol components (OA) for the last two seasons show that all models generally underestimate the measured concentrations. The maximum underestimation of EC is about 60% and up to about 80% for total organic matter (TOM). The underestimation of TOM outside of highly polluted area is a consequence of an underestimation of secondary organic aerosol (SOA), in particular of its main contributor: biogenic secondary aerosol (BSOA). This result is independent on the SOA modelling approach used and season. The concentrations and daily cycles of total primary organic matter (TPOM) are generally better reproduced by the models since they used the same anthropogenic emissions. However, the combination of emissions and model formulation leads to overestimate TPOM concentrations in 2009 for most of the models. All models capture relatively well the SOA daily cycles at rural stations mainly due to the spatial resolution used in the simulations. For the investigated carbonaceous aerosol compounds, the differences between the concentrations simulated by different models are lower than the differences between the concentrations simulated with a model for different seasons. © 2019 The Authors
Tropospheric aqueous-phase chemistry: kinetics, mechanisms, and its coupling to a changing gas phase
2015, Herrmann, Hartmut, Schaefer, Thomas, Tilgner, Andreas, Styler, Sarah A., Weller, Christian, Teich, Monique, Otto, Tobias
[no abstract available]
Variability of black carbon mass concentrations, sub-micrometer particle number concentrations and size distributions: results of the German Ultrafine Aerosol Network ranging from city street to High Alpine locations
2018, Sun, J., Birmili, W., Hermann, M., Tuch, T., Weinhold, K., Spindler, G., Schladitz, A., Bastian, S., Löschau, G., Cyrys, J., Gu, J., Flentje, H., Briel, B., Asbac, C., Kaminski, H., Ries, L., Sohme, R., Gerwig, H., Wirtz, K., Meinhardt, F., Schwerin, A., Bath, O., Ma, N., Wiedensohler, A.
This work reports the first statistical analysis of multi-annual data on tropospheric aerosols from the German Ultrafine Aerosol Network (GUAN). Compared to other networks worldwide, GUAN with 17 measurement locations has the most sites equipped with particle number size distribution (PNSD) and equivalent black carbon (eBC) instruments and the most site categories in Germany ranging from city street/roadside to High Alpine. As we know, the variations of eBC and particle number concentration (PNC) are influenced by several factors such as source, transformation, transport and deposition. The dominant controlling factor for different pollutant parameters might be varied, leading to the different spatio-temporal variations among the measured parameters. Currently, a study of spatio-temporal variations of PNSD and eBC considering the influences of both site categories and spatial scale is still missing. Based on the multi-site dataset of GUAN, the goal of this study is to investigate how pollutant parameters may interfere with spatial characteristics and site categories. © 2019 The Authors
The Importance of the Representation of DMS Oxidation in Global Chemistry‐Climate Simulations
2021, Hoffmann, Erik Hans, Heinold, Bernd, Kubin, Anne, Tegen, Ina, Herrmann, Hartmut
The oxidation of dimethyl sulfide (DMS) is key for the natural sulfate aerosol formation and its climate impact. Multiphase chemistry is an important oxidation pathway but neglected in current chemistry-climate models. Here, the DMS chemistry in the aerosol-chemistry-climate model ECHAM-HAMMOZ is extended to include multiphase methane sulfonic acid (MSA) formation in deliquesced aerosol particles, parameterized by reactive uptake. First simulations agree well with observed gas-phase MSA concentrations. The implemented formation pathways are quantified to contribute up to 60% to the sulfate aerosol burden over the Southern Ocean and Arctic/Antarctic regions. While globally the impact on the aerosol radiative forcing almost levels off, a significantly more positive solar radiative forcing of up to +0.1 W m−2 is computed in the Arctic (>60°N). The findings imply the need of both further laboratory and model studies on the atmospheric multiphase oxidation of DMS.