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Chemical composition of nanoparticles from α-pinene nucleation and the influence of isoprene and relative humidity at low temperature

Caudillo, Lucía and Rörup, Birte and Heinritzi, Martin and Marie, Guillaume and Simon, Mario and Wagner, Andrea C. and Müller, Tatjana and Granzin, Manuel and Amorim, Antonio and Ataei, Farnoush and Baalbaki, Rima and Bertozzi, Barbara and Brasseur, Zoé and Chiu, Randall and Chu, Biwu and Dada, Lubna and Duplissy, Jonathan and Finkenzeller, Henning and Gonzalez Carracedo, Loïc and He, Xu-Cheng and Hofbauer, Victoria and Kong, Weimeng and Lamkaddam, Houssni and Lee, Chuan P. and Lopez, Brandon and Mahfouz, Naser G. A. and Makhmutov, Vladimir and Manninen, Hanna E. and Marten, Ruby and Massabò, Dario and Mauldin, Roy L. and Mentler, Bernhard and Molteni, Ugo and Onnela, Antti and Pfeifer, Joschka and Philippov, Maxim and Piedehierro, Ana A. and Schervish, Meredith and Scholz, Wiebke and Schulze, Benjamin and Shen, Jiali and Stolzenburg, Dominik and Stozhkov, Yuri and Surdu, Mihnea and Tauber, Christian and Tham, Yee Jun and Tian, Ping and Tomé, António and Vogt, Steffen and Wang, Mingyi and Wang, Dongyu S. and Weber, Stefan K. and Welti, André and Yonghong, Wang and Yusheng, Wu and Zauner-Wieczorek, Marcel and Baltensperger, Urs and El Haddad, Imad and Flagan, Richard C. and Hansel, Armin and Höhler, Kristina and Kirkby, Jasper and Kulmala, Markku and Lehtipalo, Katrianne and Möhler, Ottmar and Saathoff, Harald and Volkamer, Rainer and Winkler, Paul M. and Donahue, Neil M. and Kürten, Andreas and Curtius, Joachim (2021) Chemical composition of nanoparticles from α-pinene nucleation and the influence of isoprene and relative humidity at low temperature. Atmospheric Chemistry and Physics, 21 (22). pp. 17099-17114. ISSN 1680-7324. doi:10.5194/acp-21-17099-2021. https://resolver.caltech.edu/CaltechAUTHORS:20211214-82816000

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Abstract

Biogenic organic precursors play an important role in atmospheric new particle formation (NPF). One of the major precursor species is α-pinene, which upon oxidation can form a suite of products covering a wide range of volatilities. Highly oxygenated organic molecules (HOMs) comprise a fraction of the oxidation products formed. While it is known that HOMs contribute to secondary organic aerosol (SOA) formation, including NPF, they have not been well studied in newly formed particles due to their very low mass concentrations. Here we present gas- and particle-phase chemical composition data from experimental studies of α-pinene oxidation, including in the presence of isoprene, at temperatures (−50 and −30 ∘C) and relative humidities (20 % and 60 %) relevant in the upper free troposphere. The measurements took place at the CERN Cosmics Leaving Outdoor Droplets (CLOUD) chamber. The particle chemical composition was analyzed by a thermal desorption differential mobility analyzer (TD-DMA) coupled to a nitrate chemical ionization–atmospheric pressure interface–time-of-flight (CI-APi-TOF) mass spectrometer. CI-APi-TOF was used for particle- and gas-phase measurements, applying the same ionization and detection scheme. Our measurements revealed the presence of C₈₋₁₀ monomers and C₁₈₋₂₀ dimers as the major compounds in the particles (diameter up to ∼ 100 nm). Particularly, for the system with isoprene added, C₅ (C₅H₁₀O₅₋₇) and C₁₅ compounds (C₁₅H₂₄O₅₋₁₀) were detected. This observation is consistent with the previously observed formation of such compounds in the gas phase. However, although the C₅ and C₁₅ compounds do not easily nucleate, our measurements indicate that they can still contribute to the particle growth at free tropospheric conditions. For the experiments reported here, most likely isoprene oxidation products enhance the growth of particles larger than 15 nm. Additionally, we report on the nucleation rates measured at 1.7 nm (J_(1.7 nm)) and compared with previous studies, we found lower J_(1.7 nm) values, very likely due to the higher α-pinene and ozone mixing ratios used in the present study.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.5194/acp-21-17099-2021DOIArticle
https://acp.copernicus.org/articles/21/17099/2021/acp-21-17099-2021-supplement.pdfPublisherSupporting Information
ORCID:
AuthorORCID
Rörup, Birte0000-0001-8755-9453
Heinritzi, Martin0000-0002-9171-8127
Marie, Guillaume0000-0003-1454-0908
Simon, Mario0000-0002-4900-7460
Wagner, Andrea C.0000-0003-3159-9434
Müller, Tatjana0000-0001-6453-9134
Amorim, Antonio0000-0003-0638-2321
Ataei, Farnoush0000-0001-8038-649X
Baalbaki, Rima0000-0002-4480-2107
Bertozzi, Barbara0000-0003-2571-6585
Brasseur, Zoé0000-0001-5387-018X
Chiu, Randall0000-0002-9892-2761
Chu, Biwu0000-0002-7548-5669
Dada, Lubna0000-0003-1105-9043
Duplissy, Jonathan0000-0001-8819-0264
Finkenzeller, Henning0000-0002-8349-3714
He, Xu-Cheng0000-0002-7416-306X
Hofbauer, Victoria0000-0001-9036-4446
Kong, Weimeng0000-0002-9432-2857
Lamkaddam, Houssni0000-0001-5166-6353
Lee, Chuan P.0000-0003-0051-8179
Mahfouz, Naser G. A.0000-0002-7097-1430
Makhmutov, Vladimir0000-0002-2242-1055
Manninen, Hanna E.0000-0002-0419-4020
Marten, Ruby0000-0003-0417-4350
Massabò, Dario0000-0001-7445-0328
Mauldin, Roy L.0000-0002-8569-8561
Mentler, Bernhard0000-0003-3852-0397
Molteni, Ugo0000-0002-1623-1933
Onnela, Antti0000-0001-9946-9762
Pfeifer, Joschka0000-0002-9172-4447
Philippov, Maxim0000-0003-4302-0020
Scholz, Wiebke0000-0003-2617-620X
Schulze, Benjamin0000-0002-6405-8872
Stolzenburg, Dominik0000-0003-1014-1360
Stozhkov, Yuri0000-0003-1917-0328
Surdu, Mihnea0000-0003-1815-2750
Tauber, Christian0000-0003-1453-1067
Tham, Yee Jun0000-0001-7924-5841
Tomé, António0000-0001-9144-7120
Wang, Mingyi0000-0001-5782-2513
Wang, Dongyu S.0000-0001-7549-1578
Weber, Stefan K.0000-0001-7408-9069
Welti, André0000-0002-3549-1212
Yonghong, Wang0000-0003-2498-9143
Zauner-Wieczorek, Marcel0000-0002-0867-665X
Baltensperger, Urs0000-0003-0079-8713
El Haddad, Imad0000-0002-2461-7238
Flagan, Richard C.0000-0001-5690-770X
Hansel, Armin0000-0002-1062-2394
Höhler, Kristina0000-0001-5503-9816
Kirkby, Jasper0000-0003-2341-9069
Kulmala, Markku0000-0003-3464-7825
Lehtipalo, Katrianne0000-0002-1660-2706
Möhler, Ottmar0000-0002-7551-9814
Volkamer, Rainer0000-0002-0899-1369
Winkler, Paul M.0000-0001-6861-6029
Donahue, Neil M.0000-0003-3054-2364
Kürten, Andreas0000-0002-8955-4450
Curtius, Joachim0000-0003-3153-4630
Additional Information:© Author(s) 2021. This work is distributed under the Creative Commons Attribution 4.0 License. Received: 16 Jun 2021 – Discussion started: 07 Jul 2021 – Revised: 15 Oct 2021 – Accepted: 17 Oct 2021 – Published: 25 Nov 2021. We thank CERN for providing the CLOUD facility to perform the experiments and the CLOUD community for supporting this study. We especially would like to thank Katja Ivanova, Timo Keber, Frank Malkemper, Robert Sitals, Hanna Elina Manninen, Antti Onnela, and Robert Kristic for their contributions to the experiment. This research has been supported by the European Commission, Research Executive Agency (grant no. CLOUD-MOTION (764991)), the Bundesministerium für Bildung und Forschung (grant no. CLOUD-16, 01LK1601A), the National Science Foundation (grant nos. AGS-1801280, AGS-1801574, and AGS-1801897), and the Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung (grant nos. 20020_172602 and BSSGI0_155846). This open-access publication was funded by the Goethe University Frankfurt. Data availability. Data related to this article are available upon request to the corresponding authors. The supplement related to this article is available online at: https://doi.org/10.5194/acp-21-17099-2021-supplement. The contact author has declared that neither they nor their co-authors have any competing interests. The contact author has declared that neither they nor their co-authors have any competing interests.
Funders:
Funding AgencyGrant Number
Marie Curie Fellowship764991
Bundesministerium für Bildung und Forschung (BMBF)CLOUD-16, 01LK1601A
NSFAGS-1801280
NSFAGS-1801574
NSFAGS-1801897
Swiss National Science Foundation (SNSF)20020_172602
Swiss National Science Foundation (SNSF)BSSGI0_155846
Issue or Number:22
DOI:10.5194/acp-21-17099-2021
Record Number:CaltechAUTHORS:20211214-82816000
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20211214-82816000
Official Citation:Caudillo, L., Rörup, B., Heinritzi, M., Marie, G., Simon, M., Wagner, A. C., Müller, T., Granzin, M., Amorim, A., Ataei, F., Baalbaki, R., Bertozzi, B., Brasseur, Z., Chiu, R., Chu, B., Dada, L., Duplissy, J., Finkenzeller, H., Gonzalez Carracedo, L., He, X.-C., Hofbauer, V., Kong, W., Lamkaddam, H., Lee, C. P., Lopez, B., Mahfouz, N. G. A., Makhmutov, V., Manninen, H. E., Marten, R., Massabò, D., Mauldin, R. L., Mentler, B., Molteni, U., Onnela, A., Pfeifer, J., Philippov, M., Piedehierro, A. A., Schervish, M., Scholz, W., Schulze, B., Shen, J., Stolzenburg, D., Stozhkov, Y., Surdu, M., Tauber, C., Tham, Y. J., Tian, P., Tomé, A., Vogt, S., Wang, M., Wang, D. S., Weber, S. K., Welti, A., Yonghong, W., Yusheng, W., Zauner-Wieczorek, M., Baltensperger, U., El Haddad, I., Flagan, R. C., Hansel, A., Höhler, K., Kirkby, J., Kulmala, M., Lehtipalo, K., Möhler, O., Saathoff, H., Volkamer, R., Winkler, P. M., Donahue, N. M., Kürten, A., and Curtius, J.: Chemical composition of nanoparticles from α-pinene nucleation and the influence of isoprene and relative humidity at low temperature, Atmos. Chem. Phys., 21, 17099–17114, https://doi.org/10.5194/acp-21-17099-2021, 2021.
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:112440
Collection:CaltechAUTHORS
Deposited By: George Porter
Deposited On:15 Dec 2021 15:04
Last Modified:01 Feb 2022 22:54

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