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Application of a Thermal Desorption-Differential Mobility Analyzer (TD-DMA) coupled to a nitrate chemical ionization-atmospheric pressure interface-time-of-flight (CI-APi-TOF) for measuring nanoparticles at the CLOUD Chamber at CERN

  • Atmospheric particles play an important role in the radiative balance of the Earth, as well as they affect human health and air quality. Hence, the chemical characterization constitutes a crucial task to determinate their properties, sources and fate. Particularly, the analysis of nanoparticles (d<100 nm) represents an analytical challenge, since these particles are abundant in number but have very little mass. This accumulative thesis focuses on the chemical characterization of nanoparticles, performed in both laboratory and field studies. Here, I present four manuscripts, two of which are my main project as a lead author. The first manuscript (Caudillo et al., 2021) focuses on the gas and the particle phase originated from biogenic precursor gases (α-pinene and isoprene). The experiments were performed in the CLOUD chamber at CERN to simulate pure biogenic new particle formation. Both gas and particle phases are measured with a nitrate CI-APi-TOF mass spectrometer, while the TD-DMA is coupled to it for particle-phase measurements, this setup allows a direct comparison as both measurements use the identical chemical ionization and detector. This study demonstrates the suitability of the TD-DMA for measuring newly formed nanoparticles and it confirms that isoprene suppresses new particle formation but contributes to the growth of newly formed particles. The second manuscript (Caudillo et al., 2022) presents an intercomparison of four different techniques (including the TD-DMA) for measuring the chemical composition of SOA nanoparticles. The measurements were conducted in the CLOUD chamber. The intercomparison was done by contrasting the observed chemical composition, the calculated volatility, and the thermal desorption behavior (for the thermal desorption techniques). The methods generally agreed on the most important compounds that are found in the nanoparticles. However, they did see different parts of the organic spectrum. Potential explanations for these differences are suggested. The third manuscript (Ungeheuer al., 2022) presents both laboratory and ambient measurements to investigate the ability of lubricant oil to form new particles. These new particles are an important source of ultrafine particles in the areas nearby large airports. The ambient measurements were performed downwind of Frankfurt International Airport, and it was found that the fraction of lubricant oil is largest in the smallest particles. In the laboratory, the main finding was that evaporated lubricant oil nucleates and forms new particles rapidly. The results suggest that nucleation of lubricant oil and subsequent particle growth can occur in the cooling exhaust plumes of aircraft-turbofans. The fourth manuscript (Wang et al., 2022) is a new particle formation study in the CLOUD chamber at CERN. This study shows that nitric acid, sulfuric acid, and ammonia interact synergistically and rapidly form particles under upper free tropospheric conditions. These particles can grow by condensation (driven by the availability of ammonia) up to CCN sizes and INP particles. The ability of these particles to act as a CCN and INP was also investigated and it was found to be as efficient as for desert dust. This mechanism constitutes an important finding and it can account for previous observations of high concentrations of ammonia and ammonium nitrate over the Asia monsoon region.

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Metadaten
Author:Lucía Caudillo MurilloGND
URN:urn:nbn:de:hebis:30:3-749814
DOI:https://doi.org/10.21248/gups.74981
Place of publication:Frankfurt am Main
Referee:Joachim CurtiusORCiD, Katrianne LehtipaloORCiDGND
Document Type:Doctoral Thesis
Language:English
Date of Publication (online):2023/09/20
Year of first Publication:2022
Publishing Institution:Universitätsbibliothek Johann Christian Senckenberg
Granting Institution:Johann Wolfgang Goethe-Universität
Date of final exam:2023/06/07
Release Date:2023/09/25
Page Number:156
Note:
Kumulative Dissertation
enthält die Verlagsversionen (Version of Record) der folgenden ArtikeL

Caudillo, Lucía; Rörup, Birte; Heinritzi, Martin; Marie, Guillaume; Simon, Mario; Wagner, Andrea C.; Müller, Tatjana; Granzin, Manuel; Amorim, Antonio; Ataei, Farnoush; Baalbaki, Rima; Bertozzi, Barbara; Brasseur, Zoé; Chiu, Randall; Chu, Biwu; Dada, Lubna; Duplissy, Jonathan; Finkenzeller, Henning; Gonzalez Carracedo, Loic; He, Xu-Cheng; Hofbauer, Victoria; Kong, Weimeng, Lamkaddam, Houssni; Lee, Chua P.; Lopez, Brando; Mahfouz, Naser G.A.; Makhmutov, Vladimir; Manninen, Hanna E.; Marten, Ruby; Massabò, Dario; Mauldin, Roy L.; Mentler, Bernhard; Molteni, Ugo; Onnela, Antti; Pfeifer, Joschka; Philippov, Maxim; Piedehierro, Ana A.; Schervish, Meredith; Scholz, Wiebke; Schulze, Benjamin; Shen, Jiali; Stolzenburg, Dominik; Stozhkov, Yuri; Surdu, Mihnea; Tauber, Christian; Tham, Yee Jun; Tian, Ping; Tomé; Anónio, Vogt, Steffen; Wang, Mingyi; Wang, Dongyu S.; Weber, Stefan K.; Welit; André; Yonghong, Wang; Yusheng, Wu; Zauner-Wieczorek, Marcel; Baltensperger, Urs; El Haddad, Imad; Flagan, Richard C.; Hansel, Armin; Höhler, Kristina; Kirkby, Jasper; Kulmala, Markku; Lehtipalo, Katrianne; Möhler, Ottmar; Saathoff, Harald; Vokamer, Rainer; Winkler, Paul M.; Danahue, Neil M.; Kürten, Andreas; Curtius, Joachim (2021): Chemical composition of nanoparticles from α-α-pinene nucleation and the influence of isoprene and relative humidity at low temperature. Atmospheric Chemistry and Physics 2021, Vol 21 (22), Seite 17099-17114, ISSN 1680-7316. DOI 10.5194/acp-21-17099-2021

Supplement of Chemical composition of nanoparticles from α-α-pinene nucleation and the influence of isoprene and relative humidity at low temperature. DOI 10.5194/acp-21-17099-2021-supplement

Die eingereichte Manuskriptversion der folgenden Artikel:
Caudillo, Lucía; Surdu, Mihnea; Lopez, Brandon; Wang, Mingyi; Thoma, Markus; Bräkling, Steffen; Buchholz, Angela; Simon, Mario; Wagner, Andrea C.; Müller, Tatjana; Granzin, Manuel; Heinritzi, Martin; Amorim, Antonio, Bell, David M.; Brasseur, Zoé; Dada, Lubna; Duplissy, Jonathan; Finkenzeller, Henning; He, Xu-Cheng; Lamkaddam, Houssni; Mahfouz, Naser G.A.; Makhmutov, Vladimir; Manninen, Hanna E.; Mari, Guillaume; Marten, Ruby; Mauldin, Roy L.; Mentler, Bernhard; Onnela, Antti; Petäjä, Tuukka; Pfeifer, Joschka; Philippov, Maxim; Piedehierro, Ana A.; Rörup, Birte; Scholz, Wiebke; Shen, Jiali; Stolzenburg, Dominik; Tauber, Christian; Tian, Ping; Tomé, António, Umo, Nsikanabasi Silas; Wang, Dongyu S.; Wang, Yonghong; Weber, Stefan K.; Welti, André; Zauner-Wieczorek, Marcel; Baltensperger, Urs; Flagan, Richard C.; Hansel, Armin; Kirkby, Jasper; Kulmala, Markku; Lehtipalo, Katrianne; Worsnop, Douglas R.; El Haddad, Imad; Donahue, Neil M.; Vogel, Alexander L.; Kürten, Andreas; Curtius, Joachim (2022): An intercomparison study of four different techniques for measuring the chemical composition of nanoparticles. Atmospheric Chemistry and Physics. ISSN 1680-7316, DOI 10.5194/acp-2022-498

Ungeheuer, Florian; Caudillo, Lucia; Ditas, Florian; Simon, Mario; Pinxteren, Dominik van; Kilic, Dogushan; Rose, Diana; Jacobi, Stefan; Kürten, Andreas; Curtius, Joachim; Vogel, Alexander L. (2022) Nucleation of jet engine oil vapors is a large source of aviation-related ultrafine particles

Die Verlagsversion des folgenden Artikels:
Wang, Mingyi, Xiao, Mao; Bertozzi, Barbara; Marie, Guillaume, Rörup, Birte; Schulze, Benjamin; Bardakov, Roman; He, Xu-Cheng; Shen, Jiali; Scholz, Wiebke; Marten, Ruby; Dada, Lubna; Baalbaki, Rima; Lopez, Brandon; Lamkaddam, Houssni; Manninen, Hanna E.; Amorim, António; Ataei, Farnoush; Bogert, Pia; Brasseru, Zoé; Caudillo, Lucía; De Menezes, Louis-Philippe; Duplissy, Jonathan; Ekman, Annica M.L; Finkenzeller, Henning; Gonzalez Carracedo, Loic; Granzin, Manuel; Guida, Roberto; Heinritzi, Martin; Hofbauer, Victoria; Höhler, Kristina; Korhonen, Kimmo; Krechmer, Jordan E.; Kürten, Andreas; Lehtipalo, Katrianne; Mahfouz, Naser G.A.; Makhmutov, Vladimir; Massabò, Dario; Mathot, Serge; Mauldin, Roy L.; Mentler, Bernhard; Müller, Tatjana; Onnela, Antti; Petäjä, Tuukka; Philippov, Maxim; Piedehierro, Ana A.; Pozzer, Andrea; Ranjithkumar, Ananth; Schervish, Meredith; Schobesberger, Siegfried; Simon, Mario; Stozhkov, Yuri; Tomé, António; Umo, Nsikanabasi Silas; Vogel, Franziska; Wagner, Robert; Wang, Dongyu S.; Weber, Stefan K.; Welti, André; Wu, Yusheng; Zauner-Wieczorek, Marcel; Sipilä, Mikko; Winkler, Paul M.; Hansel, Armin; Baltensperger, Urs; Kulmala, Markku; Flagan, Richard C.; Curtius, Joachim; Riipinen, Ilona; Gordon, Hamish; Lelieveld, Jos; El-Haddad, Imad; Volkamer, Rainer; Worsnop, Douglas, R; Christoudis, Theodoros; Kirkby, Jasper; Möhler, Ottmar; Donahue, Neil M. (2021): Synergistic HNO3–H2SO4–NH3 upper tropospheric particle formation. Nature 2022, Vol. 605, Seite 483-489, DOI 10.1038/s41586-022-04605-4
HeBIS-PPN:511878273
Institutes:Geowissenschaften / Geographie
Dewey Decimal Classification:5 Naturwissenschaften und Mathematik / 55 Geowissenschaften, Geologie / 550 Geowissenschaften
Sammlungen:Universitätspublikationen
Licence (German):License LogoDeutsches Urheberrecht