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- ItemThe second ACTRIS inter-comparison (2016) for Aerosol Chemical Speciation Monitors (ACSM): Calibration protocols and instrument performance evaluations(Philadelphia, Pa.: Taylor & Francis, 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, OlivierThis 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.
- ItemQuantifying uncertainties in soil carbon responses to changes in global mean temperature and precipitation(München : European Geopyhsical Union, 2014) Nishina, K.; Ito, A.; Beerling, D.J.; Cadule, P.; Ciais, P.; Clark, D.B.; Friend, A.D.; Kahana, R.; Kato, E.; Keribin, R.; Lucht, W.; Lomas, M.; Rademacher, T.T.; Pavlick, R.; Schaphoff, S.; Vuichard, N.; Warszawaski, L.; Yokohata, T.Soil organic carbon (SOC) is the largest carbon pool in terrestrial ecosystems and may play a key role in biospheric feedbacks with elevated atmospheric carbon dioxide (CO2) in a warmer future world. We examined the simulation results of seven terrestrial biome models when forced with climate projections from four representative-concentration-pathways (RCPs)-based atmospheric concentration scenarios. The goal was to specify calculated uncertainty in global SOC stock projections from global and regional perspectives and give insight to the improvement of SOC-relevant processes in biome models. SOC stocks among the biome models varied from 1090 to 2650 Pg C even in historical periods (ca. 2000). In a higher forcing scenario (i.e., RCP8.5), inconsistent estimates of impact on the total SOC (2099–2000) were obtained from different biome model simulations, ranging from a net sink of 347 Pg C to a net source of 122 Pg C. In all models, the increasing atmospheric CO2 concentration in the RCP8.5 scenario considerably contributed to carbon accumulation in SOC. However, magnitudes varied from 93 to 264 Pg C by the end of the 21st century across biome models. Using the time-series data of total global SOC simulated by each biome model, we analyzed the sensitivity of the global SOC stock to global mean temperature and global precipitation anomalies (ΔT and ΔP respectively) in each biome model using a state-space model. This analysis suggests that ΔT explained global SOC stock changes in most models with a resolution of 1–2 °C, and the magnitude of global SOC decomposition from a 2 °C rise ranged from almost 0 to 3.53 Pg C yr−1 among the biome models. However, ΔP had a negligible impact on change in the global SOC changes. Spatial heterogeneity was evident and inconsistent among the biome models, especially in boreal to arctic regions. Our study reveals considerable climate uncertainty in SOC decomposition responses to climate and CO2 change among biome models. Further research is required to improve our ability to estimate biospheric feedbacks through both SOC-relevant and vegetation-relevant processes.
- ItemClimate Feedback on Aerosol Emission and Atmospheric Concentrations(Heidelberg : Springer, 2018) Tegen, Ina; Schepanski, KerstinPurpose of Review: Climate factors may considerably impact on natural aerosol emissions and atmospheric distributions. The interdependencies of processes within the aerosol-climate system may thus cause climate feedbacks that need to be understood. Recent findings on various major climate impacts on aerosol distributions are summarized in this review. Recent Findings: While generally atmospheric aerosol distributions are influenced by changes in precipitation, atmospheric mixing, and ventilation due to circulation changes, emissions from natural aerosol sources strongly depend on climate factors like wind speed, temperature, and vegetation. Aerosol sources affected by climate are desert sources of mineral dust, marine aerosol sources, and vegetation sources of biomass burning aerosol and biogenic volatile organic gases that are precursors for secondary aerosol formation. Different climate impacts on aerosol distributions may offset each other. Summary: In regions where anthropogenic aerosol loads decrease, the impacts of climate on natural aerosol variabilities will increase. Detailed knowledge of processes controlling aerosol concentrations is required for credible future projections of aerosol distributions.
- ItemImpact of cold atmospheric pressure plasma processing on storage of blueberries(Oxford [u.a.] : Wiley-Blackwell, 2020) Pathak, Namrata; Grossi Bovi, Graziele; Limnaios, Athanasios; Fröhling, Antje; Brincat, Jean-Pierre; Taoukis, Petros; Valdramidis, Vasilis P.; Schlüter, OliverThe current study aimed at investigating the impact of nitrogen (N)-generated cold atmospheric pressure plasma (CAPP) treatment on blueberries focusing on the overall impact on berry quality and microbial load along a storage period of 10 days. Blueberries were treated for 0 (control), 5, and 10 min. Assessment of fruit quality (°Bx, ascorbic acid, anthocyanins, titratable acidity, elasticity, and color parameters) and microbial analysis was performed. Results showed that CAPP treatment was more effective in inhibiting bacterial growth than fungal growth and during the subsequent storage, the quality parameters did not differ significantly from the control, under the same conditions. The study supports N-generated CAPP as a disinfection technique to reduce microbial load in blueberries without significantly impacting most quality parameters. Practical applications: Over the last decades, foodborne illness outbreaks around the world have been associated with berries. For that reason, due to the increasing consumption of berries it is paramount to study technologies that can eliminate pathogens responsible for such outbreaks. Cold atmospheric pressure plasma (CAPP) can be a promising technology to be used as an alternative to traditional decontamination methods of food. In this context, this study explored the effect and efficiency of this novel technology on reduction of native microflora and its impact on the physical and chemical properties of blueberries treated by nitrogen (N)-generated CAPP with subsequent storage of 10 days. Results of this work confirmed that such technology has high potential application for decontamination of berries without significantly impacting most quality parameters and thereby can be a potential technology for industrial applications. © 2020 The Authors. Journal of Food Processing and Preservation published by Wiley Periodicals LLC.
- ItemTreatment of Candida albicans biofilms with low-temperature plasma induced by dielectric barrier discharge and atmospheric pressure plasma jet(College Park, MD : Institute of Physics Publishing, 2010) Koban, I.; Matthes, R.; Hübner, N.-O.; Welk, A.; Meisel, P.; Holtfreter, B.; Sietmann, R.; Kindel, E.; Weltmann, K.-D.; Kramer, A.; Kocher, T.Because of some disadvantages of chemical disinfection in dental practice (especially denture cleaning), we investigated the effects of physical methods on Candida albicans biofilms. For this purpose, the antifungal efficacy of three different low-temperature plasma devices (an atmospheric pressure plasma jet and two different dielectric barrier discharges (DBDs)) on Candida albicans biofilms grown on titanium discs in vitro was investigated. As positive treatment controls, we used 0.1% Chlorhexidine digluconate (CHX) and 0.6% sodium hypochlorite (NaOCl). The corresponding gas streams without plasma ignition served as negative treatment controls. The efficacy of the plasma treatment was determined evaluating the number of colony-forming units (CFU) recovered from titanium discs. The plasma treatment reduced the CFU significantly compared to chemical disinfectants. While 10 min CHX or NaOCl exposure led to a CFU log 10 reduction factor of 1.5, the log10 reduction factor of DBD plasma was up to 5. In conclusion, the use of low-temperature plasma is a promising physical alternative to chemical antiseptics for dental practice. © IOP Publishing Ltd and Deutsche Physikalische Gesellschaft.
- ItemThe effect of acid-base clustering and ions on the growth of atmospheric nano-particles(London : Nature Publishing Group, 2016) Lehtipalo, Katrianne; Rondo, Linda; Kontkanen, Jenni; Schobesberger, Siegfried; Jokinen, Tuija; Sarnela, Nina; Kürten, Andreas; Ehrhart, Sebastian; Franchin, Alessandro; Nieminen, Tuomo; Kulmala, Markku; Riccobono, Francesco; Sipila, Mikko; Yli-Juuti, Taina; Duplissy, Jonathan; Adamov, Alexey; Ahlm, Lars; Almeida, Joa˜o; Amorim, Antonio; Bianchi, Federico; Breitenlechner, Martin; Dommen, Josef; Downard, Andrew J.; Dunne, Eimear M.; Flagan, Richard C.; Guida, Roberto; Hakala, Jani; Hansel, Armin; Jud, Werner; Kangasluoma, Juha; Kerminen, Veli-Matti; Keskinen, Helmi; Kim, Jaeseok; Kirkby, Jasper; Kupc, Agnieszka; Kupiainen-Määttä, Oona; Laaksonen, Ari; Lawler, Michael J.; Leiminger, Markus; Mathot, Serge; Olenius, Tinja; Ortega, Ismael K.; Onnela, Antti; Petäjä, Tuukka; Praplan, Arnaud; Rissanen, Matti P.; Ruuskanen, Taina; Santos, Filipe D.; Schallhart, Simon; Schnitzhofer, Ralf; Simon, Mario; Smith, James N.; Tröstl, Jasmin; Tsagkogeorgas, Georgios; Tomé, António; Vaattovaara, Petri; Vehkamäki, Hanna; Vrtala, Aron E.; Wagner, Paul E.; Williamson, Christina; Wimmer, Daniela; Winkler, Paul M.; Virtanen, Annele; Donahue, Neil M.; Carslaw, Kenneth S.; Baltensperger, Urs; Riipinen, Ilona; Curtius, Joachim; Worsnop, Douglas R.; Kulmala, MarkkuThe growth of freshly formed aerosol particles can be the bottleneck in their survival to cloud condensation nuclei. It is therefore crucial to understand how particles grow in the atmosphere. Insufficient experimental data has impeded a profound understanding of nano-particle growth under atmospheric conditions. Here we study nano-particle growth in the CLOUD (Cosmics Leaving OUtdoors Droplets) chamber, starting from the formation of molecular clusters. We present measured growth rates at sub-3 nm sizes with different atmospherically relevant concentrations of sulphuric acid, water, ammonia and dimethylamine. We find that atmospheric ions and small acid-base clusters, which are not generally accounted for in the measurement of sulphuric acid vapour, can participate in the growth process, leading to enhanced growth rates. The availability of compounds capable of stabilizing sulphuric acid clusters governs the magnitude of these effects and thus the exact growth mechanism. We bring these observations into a coherent framework and discuss their significance in the atmosphere.
- ItemIon-induced nucleation of pure biogenic particles(London : Nature Publishing Group, 2016) Kirkby, Jasper; Duplissy, Jonathan; Sengupta, Kamalika; Gordon, Hamish; Williamson, Christina; Heinritzi, Martin; Simon, Mario; Yan, Chao; Almeida, João; Tröstl, Jasmin; Nieminen, Tuomo; Ortega, Ismael K.; Wagner, Robert; Adamov, Alexey; Amorim, Antonio; Bernhammer, Anne-Kathrin; Bianchi, Federico; Breitenlechner, Martin; Brilke, Sophia; Chen, Xuemeng; Craven, Jill; Dias, Antonio; Ehrhart, Sebastian; Flagan, Richard C.; Franchin, Alessandro; Fuchs, Claudia; Guida, Roberto; Hakala, Jani; Hoyle, Christopher R.; Jokinen, Tuija; Junninen, Heikki; Kangasluoma, Juha; Kim, Jaeseok; Krapf, Manuel; Kürten, Andreas; Laaksonen, Ari; Lehtipalo, Katrianne; Makhmutov, Vladimir; Mathot, Serge; Molteni, Ugo; Onnela, Antti; Peräkylä, Otso; Piel, Felix; Petäjä, Tuukka; Praplan, Arnaud P.; Pringle, Kirsty; Rap, Alexandru; Richards, Nigel A.D.; Riipinen, Ilona; Rissanen, Matti P.; Rondo, Linda; Sarnela, Nina; Schobesberger, Siegfried; Scott, Catherine E.; Seinfeld, John H.; Sipilä, Mikko; Steiner, Gerhard; Stozhkov, Yuri; Stratmann, Frank; Tomé, Antonio; Virtanen, Annele; Vogel, Alexander L.; Wagner, Andrea C.; Wagner, Paul E.; Weingartner, Ernest; Wimmer, Daniela; Winkler, Paul M.; Ye, Penglin; Zhang, Xuan; Hansel, Armin; Dommen, Josef; Donahue, Neil M.; Worsnop, Douglas R.; Baltensperger, Urs; Kulmala, Markku; Carslaw, Kenneth S.; Curtius, JoachimAtmospheric aerosols and their effect on clouds are thought to be important for anthropogenic radiative forcing of the climate, yet remain poorly understood1. Globally, around half of cloud condensation nuclei originate from nucleation of atmospheric vapours2. It is thought that sulfuric acid is essential to initiate most particle formation in the atmosphere3,4, and that ions have a relatively minor role5. Some laboratory studies, however, have reported organic particle formation without the intentional addition of sulfuric acid, although contamination could not be excluded6,7. Here we present evidence for the formation of aerosol particles from highly oxidized biogenic vapours in the absence of sulfuric acid in a large chamber under atmospheric conditions. The highly oxygenated molecules (HOMs) are produced by ozonolysis of α-pinene. We find that ions from Galactic cosmic rays increase the nucleation rate by one to two orders of magnitude compared with neutral nucleation. Our experimental findings are supported by quantum chemical calculations of the cluster binding energies of representative HOMs. Ion-induced nucleation of pure organic particles constitutes a potentially widespread source of aerosol particles in terrestrial environments with low sulfuric acid pollution.
- ItemHydroxyl radical-induced formation of highly oxidized organic compounds(London : Nature Publishing Group, 2016) Berndt, Torsten; Richters, Stefanie; Jokinen, Tuija; Hyttinen, Noora; Kurtén, Theo; Otkjær, Rasmus V.; Kjaergaard, Henrik G.; Stratmann, Frank; Herrmann, Hartmut; Sipila, Mikko; Kulmala, Markku; Ehn, MikaelExplaining the formation of secondary organic aerosol is an intriguing question in atmospheric sciences because of its importance for Earth’s radiation budget and the associated effects on health and ecosystems. A breakthrough was recently achieved in the understanding of secondary organic aerosol formation from ozone reactions of biogenic emissions by the rapid formation of highly oxidized multifunctional organic compounds via autoxidation. However, the important daytime hydroxyl radical reactions have been considered to be less important in this process. Here we report measurements on the reaction of hydroxyl radicals with a- and b-pinene applying improved mass spectrometric methods. Our laboratory results prove that the formation of highly oxidized products from hydroxyl radical reactions proceeds with considerably higher yields than previously reported. Field measurements support these findings. Our results allow for a better description of the diurnal behaviour of the highly oxidized product formation and subsequent secondary organic aerosol formation in the atmosphere.
- ItemEURODELTA III exercise: An evaluation of air quality models’ capacity to reproduce the carbonaceous aerosol(Amsterdam : Elsevier, 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, SamaraThe 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
- ItemFirst global observations of the mesospheric potassium layer(Hoboken, NJ : Wiley-Blackwell Publishing Ltd, 2014) Dawkins, E.C.M.; Plane, J.M.C.; Chipperfield, M.P.; Feng, W.; Gumbel, J.; Hedin, J.; Höffner, J.; Friedman, J.S.Metal species, produced by meteoric ablation, act as useful tracers of upper atmosphere dynamics and chemistry. Of these meteoric metals, K is an enigma: at extratropical latitudes, limited available lidar data show that the K layer displays a semiannual seasonal variability, rather than the annual pattern seen in other metals such as Na and Fe. Here we present the first near-global K retrieval, where K atom number density profiles are derived from dayglow measurements made by the Optical Spectrograph and Infrared Imager System spectrometer on board the Odin satellite. This robust retrieval produces density profiles with typical layer peak errors of ±15% and a 2km vertical grid resolution. We demonstrate that these retrieved profiles compare well with available lidar data and show for the first time that the unusual semiannual behavior is near-global in extent. This new data set has wider applications for improving understanding of the K chemistry and of related upper atmosphere processes. Key Points First quantitative retrieval of the terrestrial K layer from space The unusual semiannual behavior of K is near global in extent.