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1. Current Role and Potential of Triple Quadrupole Mass Spectrometry in Biomedical Research and Clinical Applications.

Author

Tsakalof, Andreas, Sysoev, Alexey A., Vyatkina, Kira V., Eganov, Alexander A., Eroshchenko, Nikolay N., Kiryushin, Alexey N., Adamov, Alexey Yu., Danilova, Elena Yu., and Nosyrev, Alexander E.

Subjects
TANDEM mass spectrometry, DRUG monitoring, MASS spectrometry, FORENSIC toxicology, MEDICAL research
Abstract

Mass-spectrometry-based assays nowadays play an essential role in biomedical research and clinical applications. There are different types of commercial mass spectrometers on the market today, and triple quadrupole (QqQ) is one of the time-honored systems. Here, we overview the main areas of QqQ applications in biomedicine and assess the current level, evolution, and trends in the use of QqQ in these areas. Relevant data were extracted from the Scopus database using the specified terms and Boolean operators defined for each field of the QqQ application. We also discuss the recent advances in QqQ and QqQ-based analytical platforms, which promote the clinical application of these systems, and explain the indicated substantial increase in triple quadrupole use in biomedicine. The number of biomedical studies utilizing QqQ increased 2–3 times this decade. Triple quadrupole is most intensively used in the field of endocrine research and testing. On the contrary, the relative rate of immunoassay utilization—a major competitor of chromatography–mass spectrometry—decreased in this area as well as its use within Therapeutic drug monitoring (TDM) and forensic toxicology. Nowadays, the applications of high-resolution accurate mass (HRAM) mass spectrometers in the investigated areas represent only a small fraction of the total amount of research using mass spectrometry; however, their application substantially increased during the last decade in the untargeted search for new biomarkers. [ABSTRACT FROM AUTHOR]

Published
2024
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2. Neutral molecular cluster formation of sulfuric acid dimethylamine observed in real time under atmospheric conditions

Author

Kürten, Andreas, Jokinen, Tuija, Simon, Mario, Sipilä, Mikko, Sarnela, Nina, Junninen, Heikki, Adamov, Alexey, Almeida, João, Amorim, Antonio, Bianchi, Federico, Breitenlechner, Martin, Dommen, Josef, Donahue, Neil M., Duplissy, Jonathan, Ehrharta, Sebastian, Flagan, Richard C., Franchin, Alessandro, Hakala, Jani, Hansel, Armin, Heinritzia, Martin, Hutterli, Manuel, Kangasluoma, Juha, Kirkby, Jasper, Laaksonen, Ari, Lehtipalo, Katrianne, Leiminger, Markus, Makhmutov, Vladimir, Mathot, Serge, Onnela, Antti, Petäjä, Tuukka, Praplan, Arnaud P., Riccobono, Francesco, Rissanen, Matti P., Rondo, Linda, Schobesberger, Siegfried, Seinfeld, John H., Steiner, Gerhard, Tomé, António, Tröstl, Jasmin, Winkler, Paul M., Williamson, Christina, Wimmer, Daniela, Ye, Penglin, Baltensperger, Urs, Carslaw, Kenneth S., Kulmala, Markku, Worsnop, Douglas R., and Curtius, Joachim

Subjects
Physics - Atmospheric and Oceanic Physics, Physics - Chemical Physics
Abstract

For atmospheric sulfuric acid (SA) concentrations the presence of dimethylamine (DMA) at mixing ratios of several parts per trillion by volume can explain observed boundary layer new particle formation rates. However, the concentration and molecular composition of the neutral (uncharged) clusters have not been reported so far due to the lack of suitable instrumentation. Here we report on experiments from the Cosmics Leaving Outdoor Droplets chamber at the European Organization for Nuclear Research revealing the formation of neutral particles containing up to 14 SA and 16 DMA molecules, corresponding to a mobility diameter of about 2 nm, under atmospherically relevant conditions. These measurements bridge the gap between the molecular and particle perspectives of nucleation, revealing the fundamental processes involved in particle formation and growth. The neutral clusters are found to form at or close to the kinetic limit where particle formation is limited only by the collision rate of SA molecules. Even though the neutral particles are stable against evaporation from the SA dimer onward, the formation rates of particles at 1.7-nm size, which contain about 10 SA molecules, are up to 4 orders of magnitude smaller comparedwith those of the dimer due to coagulation and wall loss of particles before they reach 1.7 nm in diameter. This demonstrates that neither the atmospheric particle formation rate nor its dependence on SA can simply be interpreted in terms of cluster evaporation or the molecular composition of a critical nucleus., Comment: Main text plus SI

Published
2015
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3. The role of low-volatility organic compounds in initial particle growth in the atmosphere

Author

Tröstl, Jasmin, Chuang, Wayne K, Gordon, Hamish, Heinritzi, Martin, Yan, Chao, Molteni, Ugo, Ahlm, Lars, Frege, Carla, Bianchi, Federico, Wagner, Robert, Simon, Mario, Lehtipalo, Katrianne, Williamson, Christina, Craven, Jill S, Duplissy, Jonathan, Adamov, Alexey, Almeida, Joao, Bernhammer, Anne-Kathrin, Breitenlechner, Martin, Brilke, Sophia, Dias, Antònio, Ehrhart, Sebastian, Flagan, Richard C, Franchin, Alessandro, Fuchs, Claudia, Guida, Roberto, Gysel, Martin, Hansel, Armin, Hoyle, Christopher R, Jokinen, Tuija, Junninen, Heikki, Kangasluoma, Juha, Keskinen, Helmi, Kim, Jaeseok, Krapf, Manuel, Kürten, Andreas, Laaksonen, Ari, Lawler, Michael, Leiminger, Markus, Mathot, Serge, Möhler, Ottmar, Nieminen, Tuomo, Onnela, Antti, Petäjä, Tuukka, Piel, Felix M, Miettinen, Pasi, Rissanen, Matti P, Rondo, Linda, Sarnela, Nina, Schobesberger, Siegfried, Sengupta, Kamalika, Sipilä, Mikko, Smith, James N, Steiner, Gerhard, Tomè, Antònio, Virtanen, Annele, Wagner, Andrea C, Weingartner, Ernest, Wimmer, Daniela, Winkler, Paul M, Ye, Penglin, Carslaw, Kenneth S, Curtius, Joachim, Dommen, Josef, Kirkby, Jasper, Kulmala, Markku, Riipinen, Ilona, Worsnop, Douglas R, Donahue, Neil M, and Baltensperger, Urs

Subjects
General Science & Technology
Abstract

About half of present-day cloud condensation nuclei originate from atmospheric nucleation, frequently appearing as a burst of new particles near midday. Atmospheric observations show that the growth rate of new particles often accelerates when the diameter of the particles is between one and ten nanometres. In this critical size range, new particles are most likely to be lost by coagulation with pre-existing particles, thereby failing to form new cloud condensation nuclei that are typically 50 to 100 nanometres across. Sulfuric acid vapour is often involved in nucleation but is too scarce to explain most subsequent growth, leaving organic vapours as the most plausible alternative, at least in the planetary boundary layer. Although recent studies predict that low-volatility organic vapours contribute during initial growth, direct evidence has been lacking. The accelerating growth may result from increased photolytic production of condensable organic species in the afternoon, and the presence of a possible Kelvin (curvature) effect, which inhibits organic vapour condensation on the smallest particles (the nano-Köhler theory), has so far remained ambiguous. Here we present experiments performed in a large chamber under atmospheric conditions that investigate the role of organic vapours in the initial growth of nucleated organic particles in the absence of inorganic acids and bases such as sulfuric acid or ammonia and amines, respectively. Using data from the same set of experiments, it has been shown that organic vapours alone can drive nucleation. We focus on the growth of nucleated particles and find that the organic vapours that drive initial growth have extremely low volatilities (saturation concentration less than 10(-4.5) micrograms per cubic metre). As the particles increase in size and the Kelvin barrier falls, subsequent growth is primarily due to more abundant organic vapours of slightly higher volatility (saturation concentrations of 10(-4.5) to 10(-0.5) micrograms per cubic metre). We present a particle growth model that quantitatively reproduces our measurements. Furthermore, we implement a parameterization of the first steps of growth in a global aerosol model and find that concentrations of atmospheric cloud concentration nuclei can change substantially in response, that is, by up to 50 per cent in comparison with previously assumed growth rate parameterizations.

Published
2016

4. The effect of acid-base clustering and ions on the growth of atmospheric nano-particles.

Author

Lehtipalo, Katrianne, Rondo, Linda, Kontkanen, Jenni, Schobesberger, Siegfried, Jokinen, Tuija, Sarnela, Nina, Kürten, Andreas, Ehrhart, Sebastian, Franchin, Alessandro, Nieminen, Tuomo, Riccobono, Francesco, Sipilä, Mikko, Yli-Juuti, Taina, Duplissy, Jonathan, Adamov, Alexey, Ahlm, Lars, Almeida, João, 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, and Kulmala, Markku

Abstract

The 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.

Published
2016

5. Global atmospheric particle formation from CERN CLOUD measurements

Author

Dunne, Eimear M., Gordon, Hamish, Kürten, Andreas, Almeida, João, Duplissy, Jonathan, Williamson, Christina, Ortega, Ismael K., Pringle, Kirsty J., Adamov, Alexey, Baltensperger, Urs, Barmet, Peter, Benduhn, Francois, Bianchi, Federico, Breitenlechner, Martin, Clarke, Antony, Curtius, Joachim, Dommen, Josef, Donahue, Neil M., Ehrhart, Sebastian, Flagan, Richard C., Franchin, Alessandro, Guida, Roberto, Hakala, Jani, Hansel, Armin, Heinritzi, Martin, Jokinen, Tuija, Kangasluoma, Juha, Kirkby, Jasper, Kulmala, Markku, Kupc, Agnieszka, Lawler, Michael J., Lehtipalo, Katrianne, Makhmutov, Vladimir, Mann, Graham, Mathot, Serge, Merikanto, Joonas, Miettinen, Pasi, Nenes, Athanasios, Onnela, Antti, Rap, Alexandra, Reddington, Carly L. S., Riccobono, Francesco, Richards, Nigel A. D., Rissanen, Matti P., Rondo, Linda, Sarnela, Nina, Schobesberger, Siegfried, Sengupta, Kamalika, Simon, Mario, Sipilä, Mikko, Smith, James N., Stozkhov, Yuri, Tomé, Antonio, Tröstl, Jasmin, Wagner, Paul E., Wimmer, Daniela, Winkler, Paul M., Worsnop, Douglas R., and Carslaw, Kenneth S.

Published
2016

6. Reduced anthropogenic aerosol radiative forcing caused by biogenic new particle formation

Author

Gordon, Hamish, Sengupta, Kamalika, Rap, Alexandru, Duplissy, Jonathan, Frege, Carla, Williamson, Christina, Heinritzi, Martin, Simon, Mario, Yan, Chao, Almeida, João, Tröstl, Jasmin, Nieminen, Tuomo, Ortega, Ismael K., Wagner, Robert, Dunne, Eimear M., Adamov, Alexey, Amorim, Antonio, Bernhammer, Anne-Kathrin, Bianchi, Federico, Breitenlechner, Martin, Brilke, Sophia, Chen, Xuemeng, Craven, Jill S., Dias, Antonio, Ehrhart, Sebastian, Fischer, Lukas, Flagan, Richard C., Franchin, Alessandro, Fuchs, Claudia, Guida, Roberto, Hakala, Jani, Hoyle, Christopher R., Jokinen, Tuija, Junninen, Heikki, Kangasluoma, Juha, Kim, Jaeseok, Kirkby, Jasper, Krapf, Manuel, Kürten, Andreas, Laaksonen, Ari, Lehtipalo, Katrianne, Makhmutov, Vladimir, Mathot, Serge, Molteni, Ugo, Monks, Sarah A., Onnela, Antti, Peräkylä, Otso, Piel, Felix, Petäjä, Tuukka, Praplan, Arnaud P., Pringle, Kirsty J., Richards, Nigel A. D., Rissanen, Matti P., Rondo, Linda, Sarnela, Nina, Schobesberger, Siegfried, Scott, Catherine E., Seinfeld, John H., Sharma, Sangeeta, Sipilä, Mikko, Steiner, Gerhard, Stozhkov, Yuri, Stratmann, Frank, Tomé, Antonio, Virtanen, Annele, Vogel, Alexander Lucas, 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, Curtius, Joachim, and Carslaw, Kenneth S.

Published
2016

7. Neutral molecular cluster formation of sulfuric acid-dimethylamine observed in real time under atmospheric conditions

Author

Kürten, Andreas, Jokinen, Tuija, Simon, Mario, Sipilä, Mikko, Sarnela, Nina, Junninen, Heikki, Adamov, Alexey, Almeida, João, Amorim, Antonio, Bianchi, Federico, Breitenlechner, Martin, Dommen, Josef, Donahue, Neil M., Duplissy, Jonathan, Ehrhart, Sebastian, Flagan, Richard C., Franchin, Alessandro, Hakala, Jani, Hansel, Armin, Heinritzi, Martin, Hutterli, Manuel, Kangasluoma, Juha, Kirkby, Jasper, Laaksonen, Ari, Lehtipalo, Katrianne, Leiminger, Markus, Makhmutov, Vladimir, Mathot, Serge, Onnela, Antti, Petäjä, Tuukka, Praplan, Arnaud P., Riccobono, Francesco, Rissanen, Matti P., Rondo, Linda, Schobesberger, Siegfried, Seinfeld, John H., Steiner, Gerhard, Tomé, António, Tröstl, Jasmin, Winkler, Paul M., Williamson, Christina, Wimmer, Daniela, Ye, Penglin, Baltensperger, Urs, Carslaw, Kenneth S., Kulmala, Markku, Worsnop, Douglas R., and Curtius, Joachim

Published
2014

8. Ion-induced nucleation of pure biogenic particles

Author

Kirkby, Jasper, Duplissy, Jonathan, Sengupta, Kamalika, Frege, Carla, 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., and Curtius, Joachim

Published
2016
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12. Molecular understanding of sulphuric acid–amine particle nucleation in the atmosphere

Author

Almeida, João, Schobesberger, Siegfried, Kürten, Andreas, Ortega, Ismael K., Kupiainen-Määttä, Oona, Praplan, Arnaud P., Adamov, Alexey, Amorim, Antonio, Bianchi, Federico, Breitenlechner, Martin, David, André, Dommen, Josef, Donahue, Neil M., Downard, Andrew, Dunne, Eimear, Duplissy, Jonathan, Ehrhart, Sebastian, Flagan, Richard C., Franchin, Alessandro, Guida, Roberto, Hakala, Jani, Hansel, Armin, Heinritzi, Martin, Henschel, Henning, Jokinen, Tuija, Junninen, Heikki, Kajos, Maija, Kangasluoma, Juha, Keskinen, Helmi, Kupc, Agnieszka, Kurtén, Theo, Kvashin, Alexander N., Laaksonen, Ari, Lehtipalo, Katrianne, Leiminger, Markus, Leppä, Johannes, Loukonen, Ville, Makhmutov, Vladimir, Mathot, Serge, McGrath, Matthew J., Nieminen, Tuomo, Olenius, Tinja, Onnela, Antti, Petäjä, Tuukka, Riccobono, Francesco, Riipinen, Ilona, Rissanen, Matti, Rondo, Linda, Ruuskanen, Taina, Santos, Filipe D., Sarnela, Nina, Schallhart, Simon, Schnitzhofer, Ralf, Seinfeld, John H., Simon, Mario, Sipilä, Mikko, Stozhkov, Yuri, Stratmann, Frank, Tomé, Antonio, Tröstl, Jasmin, Tsagkogeorgas, Georgios, Vaattovaara, Petri, Viisanen, Yrjo, Virtanen, Annele, Vrtala, Aron, Wagner, Paul E., Weingartner, Ernest, Wex, Heike, Williamson, Christina, Wimmer, Daniela, Ye, Penglin, Yli-Juuti, Taina, Carslaw, Kenneth S., Kulmala, Markku, Curtius, Joachim, Baltensperger, Urs, Worsnop, Douglas R., Vehkamäki, Hanna, and Kirkby, Jasper

Published
2013
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15. EMS912194 Supplemental Material - Supplemental material for Investigation by simulation of the RF carpets for the transport of ions at atmospheric pressures

Author

Poteshin, Sergey, Burykina, Anna, Adamov, Alexey, and Sysoev, Alexey

Subjects
FOS: Materials engineering, 91299 Materials Engineering not elsewhere classified
Abstract

Supplemental material, EMS912194 Supplemental Material for Investigation by simulation of the RF carpets for the transport of ions at atmospheric pressures by Sergey Poteshin, Anna Burykina, Alexey Adamov and Alexey Sysoev in European Journal of Mass Spectrometry

Published
2020
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18. The effect of acid-base clustering and ions on the growth of atmospheric nano-particles

Author

University of Helsinki, Department of Physics, University of Helsinki, Helsinki Institute of Physics, Lehtipalo, Katrianne, Rondo, Linda, Kontkanen, Jenni, Schobesberger, Siegfried, Jokinen, Tuija, Sarnela, Nina, Kuerten, Andreas, Ehrhart, Sebastian, Franchin, Alessandro, Nieminen, Tuomo, Riccobono, Francesco, Sipilä, Mikko, Yli-Juuti, Taina, Duplissy, Jonathan, Adamov, Alexey, Ahlm, Lars, Almeida, Joao, 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., Trostl, Jasmin, Tsagkogeorgas, Georgios, Tome, Antonio, 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, Markku, University of Helsinki, Department of Physics, University of Helsinki, Helsinki Institute of Physics, Lehtipalo, Katrianne, Rondo, Linda, Kontkanen, Jenni, Schobesberger, Siegfried, Jokinen, Tuija, Sarnela, Nina, Kuerten, Andreas, Ehrhart, Sebastian, Franchin, Alessandro, Nieminen, Tuomo, Riccobono, Francesco, Sipilä, Mikko, Yli-Juuti, Taina, Duplissy, Jonathan, Adamov, Alexey, Ahlm, Lars, Almeida, Joao, 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., Trostl, Jasmin, Tsagkogeorgas, Georgios, Tome, Antonio, 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., and Kulmala, Markku

Abstract

The 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.

Published
2016

19. Development of atmospheric pressure ionization ion mobility spectrometry and ion mobility spectrometry mass spectrometry

Author

Adamov, Alexey, University of Helsinki, Faculty of Science, Department of Chemistry, Laboratory of Analytical Chemistry, Helsingin yliopisto, matemaattis-luonnontieteellinen tiedekunta, kemian laitos, Helsingfors universitet, matematisk-naturvetenskapliga fakulteten, kemiska institutionen, Thomas, Paul, Kotiaho, Tapio, and Sysoev, Alexey

Subjects
analyyttinen kemia
Abstract

This study is focused on the development and evaluation of ion mobility instrumentation with various atmospheric pressure ionization techniques and includes the following work. First, a high-resolution drift tube ion mobility spectrometer (IMS), coupled with a commercial triple quadrupole mass spectrometer (MS), was developed. This drift tube IMS is compatible with the front-end of commercial Sciex mass spectrometers (e.g., Sciex API-300, 365, and 3000) and also allows easy (only minor modifications are needed) installation between the original atmospheric pressure ion source and the triple quadrupole mass spectrometer. Performance haracteristics (e.g.,resolving power, detection limit, transmission efficiency of ions) of this IMS-MS instrument were evaluated. Development of the IMS-MS instrument also led to a study where a proposal was made that tetraalkylammonium ions can be used as chemical standards for ESI-IMS. Second, the same drift tube design was also used to build a standalone ion mobility spectrometer equipped with a Faraday plate detector. For this highresolution (resolving power about 100 shown) IMS device, a multi-ion source platform was built, which allows the use of a range of atmospheric pressure ionization methods, such as: corona discharge chemical ionization (CD-APCI), atmospheric pressure photoionization (APPI), and radioactive atmospheric pressure chemical ionization (R-APCI). The multi-ion source platform provides easy switching between ionization methods and both positive and negative ionization modes can be used. Third, a simple desorpion/ionization on silicon (DIOS) ion source set-up for use with the developed IMS and IMS-MS instruments was built and its operation demonstrated. Fourth, a prototype of a commercial aspiration-type ion mobility spectrometer was mounted in front of a commercial triple quadrupole mass spectrometer. The set-up, which is simple, easy to install, and requires no major modifications to the MS, provides the possibility of gathering fundamental information about aspiration mobility spectrometry. Not available.

Published
2012

20. Insight into Acid–Base Nucleation Experiments by Comparison of the Chemical Composition of Positive, Negative, and Neutral Clusters

Author

Bianchi, Federico, primary, Praplan, Arnaud P., additional, Sarnela, Nina, additional, Dommen, Josef, additional, Kürten, Andreas, additional, Ortega, Ismael K., additional, Schobesberger, Siegfried, additional, Junninen, Heikki, additional, Simon, Mario, additional, Tröstl, Jasmin, additional, Jokinen, Tuija, additional, Sipilä, Mikko, additional, Adamov, Alexey, additional, Amorim, Antonio, additional, Almeida, Joao, additional, Breitenlechner, Martin, additional, Duplissy, Jonathan, additional, Ehrhart, Sebastian, additional, Flagan, Richard C., additional, Franchin, Alessandro, additional, Hakala, Jani, additional, Hansel, Armin, additional, Heinritzi, Martin, additional, Kangasluoma, Juha, additional, Keskinen, Helmi, additional, Kim, Jaeseok, additional, Kirkby, Jasper, additional, Laaksonen, Ari, additional, Lawler, Michael J., additional, Lehtipalo, Katrianne, additional, Leiminger, Markus, additional, Makhmutov, Vladimir, additional, Mathot, Serge, additional, Onnela, Antti, additional, Petäjä, Tuukka, additional, Riccobono, Francesco, additional, Rissanen, Matti P., additional, Rondo, Linda, additional, Tomé, António, additional, Virtanen, Annele, additional, Viisanen, Yrjö, additional, Williamson, Christina, additional, Wimmer, Daniela, additional, Winkler, Paul M., additional, Ye, Penglin, additional, Curtius, Joachim, additional, Kulmala, Markku, additional, Worsnop, Douglas R., additional, Donahue, Neil M., additional, and Baltensperger, Urs, additional

Published
2014
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21. Evolution of alpha-pinene oxidation products in the presence of varying oxidizers: CI-APi-TOF point of view

Author

DeMott, P. J., ODowd, C. D., Rissanen, Matti P., Jokinen, Tuija, Schobesberger, Siegfried, Praplan, Arnaud P., Sipilä, Mikko, Sarnela, Nina, Junninen, Heikki, Duplissy, Jonathan, Kangasluoma, Juha, Hakala, Jani, Wimmer, Daniela, Adamov, Alexey, Lehtipalo, Katrianne, Nieminen, Tuomo, Kulmala, Markku, Worsnop, Douglas R., DeMott, P. J., ODowd, C. D., Rissanen, Matti P., Jokinen, Tuija, Schobesberger, Siegfried, Praplan, Arnaud P., Sipilä, Mikko, Sarnela, Nina, Junninen, Heikki, Duplissy, Jonathan, Kangasluoma, Juha, Hakala, Jani, Wimmer, Daniela, Adamov, Alexey, Lehtipalo, Katrianne, Nieminen, Tuomo, Kulmala, Markku, and Worsnop, Douglas R.

Abstract

Alpha-pinene oxidation was studied in the CERN CLOUD chamber under near atmospheric conditions using varying levels of different oxidizers (i.e., O_3 , HO_x and NO_x with differing gas mixture compositions) in the presence and absence of UV-radiation, SO_2 and additional organic traces; ammonia (NH_3) and dimethylamine (DMA). The oxidation products and their evolution due to aging in the chamber were studied using a novel CI-APi-TOF technique, with the nitrate ion (NO^−_3 ) based chemical ionization (CI) scheme. We aimed to the results that would indicate how different oxidizing pathways lead to different product distributions in the product clusters detected.

Published
2013

22. Cluster Measurements at CLOUD using a High Resolution Ion Mobility Spectrometer - Mass Spectrometer Combination

Author

DeMott, Paul J., ODowd, C. D., Adamov, Alexey, Junninen, Heikki, Duplissy, Jonathan, Sipilä, Mikko, Kulmala, Markku, DeMott, Paul J., ODowd, C. D., Adamov, Alexey, Junninen, Heikki, Duplissy, Jonathan, Sipilä, Mikko, and Kulmala, Markku

Abstract

Mass spectrometry is powerful tool for environmental and atmospheric chemistry analysis. Modern mass spectrometers demonstrate low detection limits, high sensitivity, and high resolving power. However, such high performance is not always enough to identify ambient ion clusters due to the clusters braking at the atmospheric pressure-to-vacuum interface of mass spectrometer. This study presents a high resolution ion mobility spectrometer-time-of-flight mass spectrometer (IMS-TOF) in the CLOUD experiment. This combination of orthogonal analytical techniques allows obtaining structural information in addition to mass-to-charge separation.

Published
2013

23. Adjusting mobility scales of ion mobility spectrometers using 2,6-DtBP as a reference compound

Author

Viitanen, Anna-Kaisa, Mauriala, Tiimo, Mattila, Terhi, Adamov, Alexey, Pedersen, Christian Schack, Mäkelä, Jyrki M., Marjamäki, Marko, Sysoev, Alexey, keskinen, Jorma, Kotiaho, Tapio, Viitanen, Anna-Kaisa, Mauriala, Tiimo, Mattila, Terhi, Adamov, Alexey, Pedersen, Christian Schack, Mäkelä, Jyrki M., Marjamäki, Marko, Sysoev, Alexey, keskinen, Jorma, and Kotiaho, Tapio

Abstract

Udgivelsesdato: 29-05-08

Published
2008

24. Particle nucleation events at the high Alpine station Jungfraujoch

Author

Bianchi, Federico, primary, Junninen, Heikki, additional, Tröstl, Jasmin, additional, Duplissy, Jonathan, additional, Rondo, Linda, additional, Simon, Mario, additional, Kürten, Andreas, additional, Adamov, Alexey, additional, Curtius, Joachim, additional, Dommen, Josef, additional, Weingartner, Ernest, additional, Worsnop, Douglas R., additional, Kulmala, Markku, additional, and Baltensperger, Urs, additional

Published
2013
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28. Cluster measurements at CLOUD using a high resolution ion mobility spectrometer-mass spectrometer combination.

Author

Adamov, Alexey, Junninen, Heikki, Duplissy, Jonathan, Sipilä, Mikko, Kulmala, Markku, and CLOUD Collaboration

Subjects
*CLOUDS, *ION mobility spectroscopy, *ENVIRONMENTAL chemistry, *ATMOSPHERIC chemistry, *SENSITIVITY analysis, *ATMOSPHERIC pressure, *HIGH resolution spectroscopy, *CHARGE transfer
Abstract

Mass spectrometry is powerful tool for environmental and atmospheric chemistry analysis. Modern mass spectrometers demonstrate low detection limits, high sensitivity, and high resolving power. However, such high performance is not always enough to identify ambient ion clusters due to the clusters braking at the atmospheric pressure-to-vacuum interface of mass spectrometer. This study presents a high resolution ion mobility spectrometer-time-of-flight mass spectrometer (IMS-TOF) in the CLOUD experiment. This combination of orthogonal analytical techniques allows obtaining structural information in addition to mass-to-charge separation. [ABSTRACT FROM AUTHOR]

Published
2013
Full Text
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31. Neutral molecular cluster formation of sulfuric acid-dimethylamine observed in real time under atmospheric conditions.

Author

Kürtena, Andreas, Jokinen, Tuija, Simon, Mario, Sipilä, Mikko, Sarnela, Nina, Junninen, Heikki, Adamov, Alexey, Almeida, João, Amorim, Antonio, Bianchi, Federico, Breitenlechner, Martin, Dommen, Josef, Donahue, Neil M., Duplissy, Jonathan, Ehrhart, Sebastian, Flagan, Richard C., Franchin, Alessandro, Hakala, Jani, Hansel, Armin, and Heinritzi, Martin

Subjects
MOLECULAR clusters, SULFURIC acid, DIMETHYLAMINE, BOUNDARY layer (Aerodynamics), EVAPORATION (Chemistry)
Abstract

For atmospheric sulfuric acid (SA) concentrations the presence of dimethyiamine (DMA) at mixing ratios of several parts per trillion by volume can explain observed boundary layer new particle formation rates. However, the concentration and molecular composition of the neutral (uncharged) clusters have not been reported so far due to the lack of suitable instrumentation. Here we report on experiments from the Cosmics Leaving Outdoor Droplets chamber at the European Organization for Nuclear Research revealing the formation of neutral particles containing up to 14 SA and 16 DMA molecules, corresponding to a mobility diameter of about 2 nm, under atmospherically relevant conditions. These measurements bridge the gap between the molecular and particle perspectives of nucleation, revealing the fundamental processes involved in particle formation and growth. The neutral clusters are found to form at or close to the kinetic limit where particle formation is limited only by the collision rate of SA molecules. Even though the neutral particles are stable against evaporation from the SA dimer onward, the formation rates of particles at 1.7-nm size, which contain about 10 SA molecules, are up to 4 orders of magnitude smaller compared with those of the dimer due to coagulation and wall loss of particles before they reach 1.7 nm in diameter. This demonstrates that neither the atmospheric particle formation rate nor its dependence on SA can simply be interpreted in terms of cluster evaporation or the molecular composition of a critical nucleus. [ABSTRACT FROM AUTHOR]

Published
2014
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32. Evolution of alpha-pinene oxidation products in the presence of varying oxidizers: CI-APi-TOF point of view.

Author

Rissanen, Matti P., Jokinen, Tuija, Schobesberger, Siegfried, Praplan, Arnaud P., Sipilä, Mikko, Sarnela, Nina, Junninen, Heikki, Duplissy, Jonathan, Kangasluoma, Juha, Hakala, Jani, Wimmer, Daniela, Adamov, Alexey, Lehtipalo, Katrianne, Nieminen, Tuomo, Kulmala, Markku, Worsnop, Douglas R., and CLOUD Collaboration

Subjects
OXIDIZING agents, CLOUD chambers, ULTRAVIOLET radiation, PINENE, DIMETHYLAMINE, AMMONIA
Abstract

Alpha-pinene oxidation was studied in the CERN CLOUD chamber under near atmospheric conditions using varying levels of different oxidizers (i.e., O3, HOx and NOx with differing gas mixture compositions) in the presence and absence of UV-radiation, SO2 and additional organic traces; ammonia (NH3) and dimethylamine (DMA). The oxidation products and their evolution due to aging in the chamber were studied using a novel CI-APi-TOF technique, with the nitrate ion (NO3-) based chemical ionization (CI) scheme. We aimed to the results that would indicate how different oxidizing pathways lead to different product distributions in the product clusters detected. [ABSTRACT FROM AUTHOR]

Published
2013
Full Text
View/download PDF

33. Elemental composition and clustering behaviour of α-pinene oxidation products for different oxidation conditions

Author

Praplan, Arnaud P., Schobesberger, Siegfried, Bianchi, Frederico, Rissanen, Matti P., Ehn, Mikael, Jokinen, Tuija, Junninen, Heikki, Adamov, Alexey, Amorim, Antonio, Dommen, Josef, Duplissy, Jonathan, Hakala, Jani, Hansel, Armin, Heinritzi, Martin, Kangasluoma, Juha, Kirkby, Jasper, Krapf, Manuel, Kürten, Andreas, Lehtipalo, Katrianne, Riccobono, Francesco, Rondo, Linda, Sarnela, Nina, Simon, Mario, Tomé, António, Tröstl, Jasmin, Winkler, Paul M., Williamson, Christina, Ye, Penglin, Curtius, Joachim, Baltensperger, Urs, Donahue, Neil M., Kulmala, Markku, and Worsnop, Douglas R.

Subjects
13. Climate action, 3. Good health
Abstract

This study presents the difference between oxidised organic compounds formed by α-pinene oxidation under various conditions in the CLOUD environmental chamber: (1) pure ozonolysis (in the presence of hydrogen as hydroxyl radical (OH) scavenger) and (2) OH oxidation (initiated by nitrous acid (HONO) photolysis by ultraviolet light) in the absence of ozone. We discuss results from three Atmospheric Pressure interface Time-of-Flight (APi-TOF) mass spectrometers measuring simultaneously the composition of naturally charged as well as neutral species (via chemical ionisation with nitrate). Natural chemical ionisation takes place in the CLOUD chamber and organic oxidised compounds form clusters with nitrate, bisulfate, bisulfate/sulfuric acid clusters, ammonium, and dimethylaminium, or get protonated. The results from this study show that this process is selective for various oxidised organic compounds with low molar mass and ions, so that in order to obtain a comprehensive picture of the elemental composition of oxidation products and their clustering behaviour, several instruments must be used. We compare oxidation products containing 10 and 20 carbon atoms and show that highly oxidised organic compounds are formed in the early stages of the oxidation., Atmospheric Chemistry and Physics, 15 (8), ISSN:1680-7375, ISSN:1680-7367

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