Articles | Volume 24, issue 1
https://doi.org/10.5194/acp-24-167-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-24-167-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
08 Jan 2024
Research article |
| 08 Jan 2024
| 08 Jan 2024
Impact of temperature on the role of Criegee intermediates and peroxy radicals in dimer formation from β-pinene ozonolysis
Yiwei Gong
CORRESPONDING AUTHOR
Department of Atmospheric and Oceanic Sciences, School of Physics, Peking University, Beijing, China
Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, Karlsruhe, Germany
Feng Jiang
Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, Karlsruhe, Germany
Yanxia Li
Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, Karlsruhe, Germany
Thomas Leisner
Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, Karlsruhe, Germany
Institute of Environmental Physics, Heidelberg University, Heidelberg, Germany
Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, Karlsruhe, Germany
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Linyu Gao, Junwei Song, Claudia Mohr, Wei Huang, Magdalena Vallon, Feng Jiang, Thomas Leisner, and Harald Saathoff
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Magdalena Vallon, Linyu Gao, Feng Jiang, Bianca Krumm, Jens Nadolny, Junwei Song, Thomas Leisner, and Harald Saathoff
Atmos. Meas. Tech., 15, 1795–1810, https://doi.org/10.5194/amt-15-1795-2022, https://doi.org/10.5194/amt-15-1795-2022, 2022
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Lucía Caudillo, Birte Rörup, Martin Heinritzi, Guillaume Marie, Mario Simon, Andrea C. Wagner, Tatjana Müller, Manuel Granzin, Antonio Amorim, Farnoush Ataei, Rima Baalbaki, Barbara Bertozzi, Zoé Brasseur, Randall Chiu, Biwu Chu, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Loïc Gonzalez Carracedo, Xu-Cheng He, Victoria Hofbauer, Weimeng Kong, Houssni Lamkaddam, Chuan P. Lee, Brandon Lopez, Naser G. A. Mahfouz, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Dario Massabò, Roy L. Mauldin, Bernhard Mentler, Ugo Molteni, Antti Onnela, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Meredith Schervish, Wiebke Scholz, Benjamin Schulze, Jiali Shen, Dominik Stolzenburg, Yuri Stozhkov, Mihnea Surdu, Christian Tauber, Yee Jun Tham, Ping Tian, António Tomé, Steffen Vogt, Mingyi Wang, Dongyu S. Wang, Stefan K. Weber, André Welti, Wang Yonghong, Wu Yusheng, Marcel Zauner-Wieczorek, Urs Baltensperger, Imad El Haddad, Richard C. Flagan, Armin Hansel, Kristina Höhler, Jasper Kirkby, Markku Kulmala, Katrianne Lehtipalo, Ottmar Möhler, Harald Saathoff, Rainer Volkamer, Paul M. Winkler, Neil M. Donahue, Andreas Kürten, and Joachim Curtius
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Larissa Lacher, Hans-Christian Clemen, Xiaoli Shen, Stephan Mertes, Martin Gysel-Beer, Alireza Moallemi, Martin Steinbacher, Stephan Henne, Harald Saathoff, Ottmar Möhler, Kristina Höhler, Thea Schiebel, Daniel Weber, Jann Schrod, Johannes Schneider, and Zamin A. Kanji
Atmos. Chem. Phys., 21, 16925–16953, https://doi.org/10.5194/acp-21-16925-2021, https://doi.org/10.5194/acp-21-16925-2021, 2021
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Ulrich Platt, Thomas Wagner, Jonas Kuhn, and Thomas Leisner
Atmos. Meas. Tech., 14, 6867–6883, https://doi.org/10.5194/amt-14-6867-2021, https://doi.org/10.5194/amt-14-6867-2021, 2021
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Julia Schneider, Kristina Höhler, Robert Wagner, Harald Saathoff, Martin Schnaiter, Tobias Schorr, Isabelle Steinke, Stefan Benz, Manuel Baumgartner, Christian Rolf, Martina Krämer, Thomas Leisner, and Ottmar Möhler
Atmos. Chem. Phys., 21, 14403–14425, https://doi.org/10.5194/acp-21-14403-2021, https://doi.org/10.5194/acp-21-14403-2021, 2021
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Naruki Hiranuma, Brent W. Auvermann, Franco Belosi, Jack Bush, Kimberly M. Cory, Dimitrios G. Georgakopoulos, Kristina Höhler, Yidi Hou, Larissa Lacher, Harald Saathoff, Gianni Santachiara, Xiaoli Shen, Isabelle Steinke, Romy Ullrich, Nsikanabasi S. Umo, Hemanth S. K. Vepuri, Franziska Vogel, and Ottmar Möhler
Atmos. Chem. Phys., 21, 14215–14234, https://doi.org/10.5194/acp-21-14215-2021, https://doi.org/10.5194/acp-21-14215-2021, 2021
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We present laboratory and field studies showing that an open-lot livestock facility is a substantial source of atmospheric ice-nucleating particles (INPs). The ambient concentration of INPs from livestock facilities in Texas is very high. It is up to several thousand INPs per liter below –20 °C and may impact regional aerosol–cloud interactions. About 50% of feedlot INPs were supermicron in diameter. No notable amount of known ice-nucleating microorganisms was found in our feedlot samples.
Alexei A. Kiselev, Alice Keinert, Tilia Gaedeke, Thomas Leisner, Christoph Sutter, Elena Petrishcheva, and Rainer Abart
Atmos. Chem. Phys., 21, 11801–11814, https://doi.org/10.5194/acp-21-11801-2021, https://doi.org/10.5194/acp-21-11801-2021, 2021
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Alkali feldspar is the most abundant mineral in the Earth's crust and is often present in mineral dust aerosols that are responsible for the formation of rain and snow in clouds. However, the cloud droplets containing pure potassium-rich feldspar would not freeze unless cooled down to a very low temperature. Here we show that partly replacing potassium with sodium would induce fracturing of feldspar, exposing a crystalline surface that could initiate freezing at higher temperature.
Hengheng Zhang, Frank Wagner, Harald Saathoff, Heike Vogel, Gholam Ali Hoshyaripour, Vanessa Bachmann, Jochen Förstner, and Thomas Leisner
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2021-193, https://doi.org/10.5194/amt-2021-193, 2021
Revised manuscript not accepted
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The evolution and the properties of Saharan dust plume were characterized by LIDARs, a sun photometer, and a regional transport model. Comparison between LIDAR measurements, sun photometer and ICON-ART predictions shows a good agreement for dust arrival time, dust layer height, and dust structure but also that the model overestimates the backscatter coefficients by a factor of (2.2 ± 0.16) and underestimate aerosol optical depth by a factor of (1.5 ± 0.11).
Barbara Bertozzi, Robert Wagner, Junwei Song, Kristina Höhler, Joschka Pfeifer, Harald Saathoff, Thomas Leisner, and Ottmar Möhler
Atmos. Chem. Phys., 21, 10779–10798, https://doi.org/10.5194/acp-21-10779-2021, https://doi.org/10.5194/acp-21-10779-2021, 2021
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Internally mixed particles composed of sulfate and organics are among the most abundant aerosol types. Their ice nucleation (IN) ability influences the formation of cirrus and, thus, the climate. We show that the presence of a thin organic coating suppresses the heterogeneous IN ability of crystalline ammonium sulfate particles. However, the IN ability of the same particle can substantially change if subjected to atmospheric processing, mainly due to differences in the resulting morphology.
Fritz Waitz, Martin Schnaiter, Thomas Leisner, and Emma Järvinen
Atmos. Meas. Tech., 14, 3049–3070, https://doi.org/10.5194/amt-14-3049-2021, https://doi.org/10.5194/amt-14-3049-2021, 2021
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A major challenge in the observations of mixed-phase clouds remains the phase discrimination and sizing of cloud droplets and ice crystals, especially for particles with diameters smaller than 0.1 mm. Here, we present a new method to derive the phase and size of single cloud particles using their angular-light-scattering information. Comparisons with other in situ instruments in three case studies show good agreement.
Julia Schneider, Kristina Höhler, Paavo Heikkilä, Jorma Keskinen, Barbara Bertozzi, Pia Bogert, Tobias Schorr, Nsikanabasi Silas Umo, Franziska Vogel, Zoé Brasseur, Yusheng Wu, Simo Hakala, Jonathan Duplissy, Dmitri Moisseev, Markku Kulmala, Michael P. Adams, Benjamin J. Murray, Kimmo Korhonen, Liqing Hao, Erik S. Thomson, Dimitri Castarède, Thomas Leisner, Tuukka Petäjä, and Ottmar Möhler
Atmos. Chem. Phys., 21, 3899–3918, https://doi.org/10.5194/acp-21-3899-2021, https://doi.org/10.5194/acp-21-3899-2021, 2021
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By triggering the formation of ice crystals, ice-nucleating particles (INP) strongly influence cloud formation. Continuous, long-term measurements are needed to characterize the atmospheric INP variability. Here, a first long-term time series of INP spectra measured in the boreal forest for more than 1 year is presented, showing a clear seasonal cycle. It is shown that the seasonal dependency of INP concentrations and prevalent INP types is driven by the abundance of biogenic aerosol.
Robert Wagner, Baptiste Testa, Michael Höpfner, Alexei Kiselev, Ottmar Möhler, Harald Saathoff, Jörn Ungermann, and Thomas Leisner
Atmos. Meas. Tech., 14, 1977–1991, https://doi.org/10.5194/amt-14-1977-2021, https://doi.org/10.5194/amt-14-1977-2021, 2021
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Michael Krayer, Agathe Chouippe, Markus Uhlmann, Jan Dušek, and Thomas Leisner
Atmos. Chem. Phys., 21, 561–575, https://doi.org/10.5194/acp-21-561-2021, https://doi.org/10.5194/acp-21-561-2021, 2021
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We address the phenomenon of ice enhancement in the vicinity of warm hydrometeors using highly accurate flow simulation techniques. It is found that the transiently supersaturated zones induced by the hydrometeor's wake are by far larger than what has been previously estimated. The ice enhancement is quantified on the micro- and macroscale, and its relevance is discussed. The results provided may contribute to a (currently unavailable) parametrization of the phenomenon.
Alexei Korolev and Thomas Leisner
Atmos. Chem. Phys., 20, 11767–11797, https://doi.org/10.5194/acp-20-11767-2020, https://doi.org/10.5194/acp-20-11767-2020, 2020
Short summary
Short summary
Secondary ice production (SIP) plays a key role in the formation of ice particles in tropospheric clouds. This work presents a critical review of the laboratory studies related to secondary ice production. It aims to identify gaps in our knowledge of SIP as well as to stimulate further laboratory studies focused on obtaining a quantitative description of efficiencies for each SIP mechanism.
Isabelle Steinke, Naruki Hiranuma, Roger Funk, Kristina Höhler, Nadine Tüllmann, Nsikanabasi Silas Umo, Peter G. Weidler, Ottmar Möhler, and Thomas Leisner
Atmos. Chem. Phys., 20, 11387–11397, https://doi.org/10.5194/acp-20-11387-2020, https://doi.org/10.5194/acp-20-11387-2020, 2020
Short summary
Short summary
In this study, we highlight the potential impact of particles from certain terrestrial sources on the formation of ice crystals in clouds. In particular, we focus on biogenic particles consisting of various organic compounds, which makes it very difficult to predict the ice nucleation properties of complex ambient particles. We find that these ambient particles are often more ice active than individual components.
Cited articles
Ahrens, J., Carlsson, P. T. M., Hertl, N., Olzmann, M., Pfeifle, M., Wolf, J. L., and Zeuch, T.: Infrared Detection of Criegee Intermediates Formed during the Ozonolysis of β-Pinene and Their Reactivity towards Sulfur Dioxide, Angew. Chem. Int. Edit., 53, 715–719, https://doi.org/10.1002/anie.201307327, 2014.
Atkinson, R., Aschmann, S. M., Arey, J., and Shorees, B.: Formation of OH radicals in the gas phase reactions of O3 with a series of terpenes, J. Geophys. Res., 97, 6065–6073, https://doi.org/10.1029/92JD00062, 1992.
Atkinson, R., Baulch, D. L., Cox, R. A., Crowley, J. N., Hampson, R. F., Hynes, R. G., Jenkin, M. E., Rossi, M. J., Troe, J., and IUPAC Subcommittee: Evaluated kinetic and photochemical data for atmospheric chemistry: Volume II – gas phase reactions of organic species, Atmos. Chem. Phys., 6, 3625–4055, https://doi.org/10.5194/acp-6-3625-2006, 2006.
Bahreini, R., Keywood, M. D., Ng, N. L., Varutbangkul, V., Gao, S., Flagan, R. C., Seinfeld, J. H., Worsnop, D. R., and Jimenez, J. L.: Measurements of secondary organic aerosol from oxidation of cycloalkenes, terpenes, and m-xylene using an aerodyne aerosol mass spectrometer, Environ. Sci. Technol., 39, 5674–5688, https://doi.org/10.1021/es048061a, 2005.
Berndt, T., Jokinen, T., Sipilä, M., Mauldin III, R. L., Herrmann, H., Stratmann, F., Junninen, H., and Kulmala, M.: H2SO4 formation from the gas-phase reaction of stabilized Criegee Intermediates with SO2: Influence of water vapour content and temperature, Atmos. Environ., 89, 603–612, https://doi.org/10.1016/j.atmosenv.2014.02.062, 2014.
Berndt, T., Scholz, W., Mentler, B., Fischer, L., Herrmann, H., Kulmala, M., and Hansel, A.: Accretion product formation from self- and cross-reactions of RO2 radicals in the atmosphere, Angew. Chem. Int. Edit., 57, 3820–3824, https://doi.org/10.1002/anie.201710989, 2018a.
Berndt, T., Mentler, B., Scholz, W., Fischer, L., Herrmann, H., Kulmala, M., and Hansel, A.: Accretion Product Formation from Ozonolysis and OH Radical Reaction of αPinene: Mechanistic Insight and the Influence of Isoprene and Ethylene, Environ. Sci. Technol., 52, 11069–11077, https://doi.org/10.1021/acs.est.8b02210, 2018b.
Chen, L., Huang, Y., Xue, Y., Shen, Z., Cao, J., and Wang, W.: Mechanistic and kinetics investigations of oligomer formation from Criegee intermediate reactions with hydroxyalkyl hydroperoxides, Atmos. Chem. Phys., 19, 4075–4091, https://doi.org/10.5194/acp-19-4075-2019, 2019.
Chhantyal-Pun, R., McGillen, M. R., Beames, J. M., Khan, M. A. H., Percival, C. J., Shallcross, D. E., and Orr-Ewing, A. J.: Temperature-Dependence of the Rates of Reaction of Trifluoroacetic Acid with Criegee Intermediates, Angew. Chem. Int. Edit., 56, 9044–9047, https://doi.org/10.1002/anie.201703700, 2017.
Chhantyal-Pun, R., Khan, M. A. H., Taatjes, C. A., Percival, C. J., Orr-Ewing, A. J., and Shallcross, D. E.: Criegee intermediates: production, detection and reactivity, Int. Rev. Phys. Chem., 39, 385–424, https://doi.org/10.1080/0144235X.2020.1792104, 2020a.
Chhantyal-Pun, R., Khan, M. A. H., Zachhuber, N., Percival, C. J., Shallcross, D. E., and Orr-Ewing, A. J.: Impact of Criegee Intermediate Reactions with Peroxy Radicals on Tropospheric Organic Aerosol, ACS Earth Space Chem., 4, 1743–1755, https://doi.org/10.1021/acsearthspacechem.0c00147, 2020b.
Cox, R. A., Ammann, M., Crowley, J. N., Herrmann, H., Jenkin, M. E., McNeill, V. F., Mellouki, A., Troe, J., and Wallington, T. J.: Evaluated kinetic and photochemical data for atmospheric chemistry: Volume VII – Criegee intermediates, Atmos. Chem. Phys., 20, 13497–13519, https://doi.org/10.5194/acp-20-13497-2020, 2020.
DeCarlo, P. F., Slowik, J. G., Worsnop, D. R., Davidovits, P., and Jimenez, J. L.: Particle Morphology and Density Characterization by Combined Mobility and Aerodynamic Diameter Measurements. Part 1: Theory, Aerosol Sci. Tech., 38, 1185–1205, https://doi.org/10.1080/027868290903907, 2004.
DeVault, M. P. and Ziemann, P. J.: Gas- and Particle-Phase Products and Their Mechanisms of Formation from the Reaction of Δ-3-Carene with NO3 Radicals, J. Phys. Chem. A, 125, 10207–10222, 2021.
Docherty, K. S. and Ziemann, P. J.: Effects of Stabilized Criegee Intermediate and OH Radical Scavengers on Aerosol Formation from Reactions of β-Pinene with O3, Aerosol Sci. Tech., 37, 877–891, https://doi.org/10.1080/02786820300930, 2003.
Donahue, N. M., Kroll, J. H., Pandis, S. N., and Robinson, A. L.: A two-dimensional volatility basis set – Part 2: Diagnostics of organic-aerosol evolution, Atmos. Chem. Phys., 12, 615–634, https://doi.org/10.5194/acp-12-615-2012, 2012.
Ehn, M., Thornton, J. A., Kleist, E., Sipilä, M., Junninen, H., Pullinen, I., Springer, M., Rubach, F., Tillmann, R., Lee, B., Lopez-Hilfiker, F., Andres, S., Acir, I.-H., Rissanen, M., Jokinen, T., Schobesberger, S., Kangasluoma, J., Kontkanen, J., Nieminen, T., Kurtén, T., Nielsen, L. B., Jørgensen, S., Kjaergaard, H. G., Canagaratna, M., Dal Maso, M., Berndt, T., Petäjä, T., Wahner, A., Kerminen, V.-M., Kulmala, M., Worsnop, D. R., Wildt, J., and Mentel, T. F.: A large source of low-volatility secondary organic aerosol, Nature, 506, 476–479, https://doi.org/10.1038/nature13032, 2014.
Elayan, I. A., Almatarneh, M. H., and Hollett, J. W.: Reactivity of the anti-Criegee intermediate of β-pinene with prevalent atmospheric species, Struct. Chem., 30, 1353–1364, https://doi.org/10.1007/s11224-019-1288-4, 2019.
Eskola, A. J., Döntgen, M., Rotavera, B., Caravan, R. L., Welz, O., Savee, J. D., Osborn, D. L., Shallcross, D. E., Percival, C. J., and Taatjes, C. A.: Direct kinetics study of CH2OO + methyl vinyl ketone and CH2OO + methacrolein reactions and an upper limit determination for CH2OO + CO reaction, Phys. Chem. Chem. Phys., 20, 19373–19381, https://doi.org/10.1039/c8cp03606c, 2018.
Fahey, D. W., Gao, R.-S., Möhler, O., Saathoff, H., Schiller, C., Ebert, V., Krämer, M., Peter, T., Amarouche, N., Avallone, L. M., Bauer, R., Bozóki, Z., Christensen, L. E., Davis, S. M., Durry, G., Dyroff, C., Herman, R. L., Hunsmann, S., Khaykin, S. M., Mackrodt, P., Meyer, J., Smith, J. B., Spelten, N., Troy, R. F., Vömel, H., Wagner, S., and Wienhold, F. G.: The AquaVIT-1 intercomparison of atmospheric water vapor measurement techniques, Atmos. Meas. Tech., 7, 3177–3213, https://doi.org/10.5194/amt-7-3177-2014, 2014.
Gao, L., Song, J., Mohr, C., Huang, W., Vallon, M., Jiang, F., Leisner, T., and Saathoff, H.: Kinetics, SOA yields, and chemical composition of secondary organic aerosol from β-caryophyllene ozonolysis with and without nitrogen oxides between 213 and 313 K, Atmos. Chem. Phys., 22, 6001–6020, https://doi.org/10.5194/acp-22-6001-2022, 2022.
Gao, L., Buchholz, A., Li, Z., Song, J., Vallon, M., Jiang, F., Möhler, O., Leisner, T., and Saathoff, H.: Volatility of secondary organic aerosol from β-caryophyllene ozonolysis over a wide tropospheric temperature range, Environ. Sci. Technol., 57, 8965–8974, https://doi.org/10.1021/acs.est.3c01151, 2023.
Gong, Y. and Chen, Z.: Quantification of the role of stabilized Criegee intermediates in the formation of aerosols in limonene ozonolysis, Atmos. Chem. Phys., 21, 813–829, https://doi.org/10.5194/acp-21-813-2021, 2021.
Gong, Y., Jiang, F., Li, Y., Leisner, T., and Saathoff, H.: Impact of temperature on the role of Criegee intermediates and peroxy radicals in dimers formation from ß-pinene ozonolysis, RADAR KIT [data set], https://doi.org/10.35097/1828, 2023.
Guenther, A. B., Jiang, X., Heald, C. L., Sakulyanontvittaya, T., Duhl, T., Emmons, L. K., and Wang, X.: The Model of Emissions of Gases and Aerosols from Nature version 2.1 (MEGAN2.1): an extended and updated framework for modeling biogenic emissions, Geosci. Model Dev., 5, 1471–1492, https://doi.org/10.5194/gmd-5-1471-2012, 2012.
Hallquist, M., Wenger, J. C., Baltensperger, U., Rudich, Y., Simpson, D., Claeys, M., Dommen, J., Donahue, N. M., George, C., Goldstein, A. H., Hamilton, J. F., Herrmann, H., Hoffmann, T., Iinuma, Y., Jang, M., Jenkin, M. E., Jimenez, J. L., Kiendler-Scharr, A., Maenhaut, W., McFiggans, G., Mentel, Th. F., Monod, A., Prévôt, A. S. H., Seinfeld, J. H., Surratt, J. D., Szmigielski, R., and Wildt, J.: The formation, properties and impact of secondary organic aerosol: current and emerging issues, Atmos. Chem. Phys., 9, 5155–5236, https://doi.org/10.5194/acp-9-5155-2009, 2009.
Hasan, G., Valiev, R. R., Salo, V.-T., and Kurtén, T.: Computational Investigation of the Formation of Peroxide (ROOR) Accretion Products in the OH- and NO3-Initiated Oxidation of α-Pinene, J. Phys. Chem. A, 125, 10632–10639, https://doi.org/10.1021/acs.jpca.1c08969, 2021.
Huang, W., Saathoff, H., Pajunoja, A., Shen, X., Naumann, K.-H., Wagner, R., Virtanen, A., Leisner, T., and Mohr, C.: α-Pinene secondary organic aerosol at low temperature: chemical composition and implications for particle viscosity, Atmos. Chem. Phys., 18, 2883–2898, https://doi.org/10.5194/acp-18-2883-2018, 2018.
Jenkin, M. E.: Modelling the formation and composition of secondary organic aerosol from α- and β-pinene ozonolysis using MCM v3, Atmos. Chem. Phys., 4, 1741–1757, https://doi.org/10.5194/acp-4-1741-2004, 2004.
Jonsson, Å. M., Hallquist, M., and Ljungström, E.: The effect of temperature and water on secondary organic aerosol formation from ozonolysis of limonene, Δ3-carene and α-pinene, Atmos. Chem. Phys., 8, 6541–6549, https://doi.org/10.5194/acp-8-6541-2008, 2008.
Kanakidou, M., Seinfeld, J. H., Pandis, S. N., Barnes, I., Dentener, F. J., Facchini, M. C., Van Dingenen, R., Ervens, B., Nenes, A., Nielsen, C. J., Swietlicki, E., Putaud, J. P., Balkanski, Y., Fuzzi, S., Horth, J., Moortgat, G. K., Winterhalter, R., Myhre, C. E. L., Tsigaridis, K., Vignati, E., Stephanou, E. G., and Wilson, J.: Organic aerosol and global climate modelling: a review, Atmos. Chem. Phys., 5, 1053–1123, https://doi.org/10.5194/acp-5-1053-2005, 2005.
Kenseth, C. M., Huang, Y. L., Zhao, R., Dalleska, N. F., Hethcox, J. C., Stoltz, B. M., and Seinfeld, J. H.: Synergistic O3 + OH oxidation pathway to extremely low-volatility dimers revealed in β-pinene secondary organic aerosol, P. Natl. Acad. Sci. USA, 115, 8301–8306, https://doi.org/10.1073/pnas.1804671115, 2018.
Kostenidou, E., Pathak, R. K., and Pandis, S. N.: An Algorithm for the Calculation of Secondary Organic Aerosol Density Combining AMS and SMPS Data, Aerosol Sci. Tech., 41, 1002–1010, https://doi.org/10.1080/02786820701666270, 2007.
Kristensen, K., Enggrob, K. L., King, S. M., Worton, D. R., Platt, S. M., Mortensen, R., Rosenoern, T., Surratt, J. D., Bilde, M., Goldstein, A. H., and Glasius, M.: Formation and occurrence of dimer esters of pinene oxidation products in atmospheric aerosols, Atmos. Chem. Phys., 13, 3763–3776, https://doi.org/10.5194/acp-13-3763-2013, 2013.
Kristensen, K., Cui, T., Zhang, H., Gold, A., Glasius, M., and Surratt, J. D.: Dimers in α-pinene secondary organic aerosol: effect of hydroxyl radical, ozone, relative humidity and aerosol acidity, Atmos. Chem. Phys., 14, 4201–4218, https://doi.org/10.5194/acp-14-4201-2014, 2014.
Kristensen, K., Jensen, L. N., Glasius, M., and Bilde, M.: The effect of sub-zero temperature on the formation and composition of secondary organic aerosol from ozonolysis of alpha-pinene, Environ. Sci., 19, 1220–1234, https://doi.org/10.1039/c7em00231a, 2017.
Kristensen, K., Jensen, L. N., Quéléver, L. L. J., Christiansen, S., Rosati, B., Elm, J., Teiwes, R., Pedersen, H. B., Glasius, M., Ehn, M., and Bilde, M.: The Aarhus Chamber Campaign on Highly Oxygenated Organic Molecules and Aerosols (ACCHA): particle formation, organic acids, and dimer esters from α-pinene ozonolysis at different temperatures, Atmos. Chem. Phys., 20, 12549–12567, https://doi.org/10.5194/acp-20-12549-2020, 2020.
Kumar, M., Busch, D. H., Subramaniam, B., and Thompson, W. H.: Criegee Intermediate Reaction with CO: Mechanism, Barriers, Conformer-Dependence, and Implications for Ozonolysis Chemistry, J. Phys. Chem. A, 118, 1887–1894, https://doi.org/10.1021/jp500258h, 2014.
Kumar, A., Mallick, S., and Kumar, P.: Effect of water on the oxidation of CO by a Criegee intermediate, Phys. Chem. Chem. Phys., 22, 21257–21266, https://doi.org/10.1039/d0cp02682d, 2020.
Lee, A., Goldstein, A. H., Keywood, M. D., Gao, S., Varutbangkul, V., Bahreini, R., Ng, N. L., Flagan, R. C., and Seinfeld, J. H.: Gas-phase products and secondary aerosol yields from the ozonolysis of ten different terpenes, J. Geophys. Res.-Atmos., 111, D07302, https://doi.org/10.1029/2005JD006437, 2006.
Lee, B. H., Lopez-Hilfiker, F. D., Mohr, C., Kurtén, T., Worsnop, D. R., and Thornton, J. A.: An iodide-adduct high-resolution time-of-flight chemical-ionization mass spectrometer: Application to atmospheric inorganic and organic compounds, Environ. Sci. Technol., 48, 6309–6317, https://doi.org/10.1021/es500362a, 2014.
Lin, J. J.-M. and Chao, W.: Structure-dependent reactivity of Criegee intermediates studied with spectroscopic methods, Chem. Soc. Rev., 46, 7483–7497, https://doi.org/10.1039/c7cs00336f, 2017.
Lopez-Hilfiker, F. D., Mohr, C., Ehn, M., Rubach, F., Kleist, E., Wildt, J., Mentel, Th. F., Carrasquillo, A. J., Daumit, K. E., Hunter, J. F., Kroll, J. H., Worsnop, D. R., and Thornton, J. A.: Phase partitioning and volatility of secondary organic aerosol components formed from α-pinene ozonolysis and OH oxidation: the importance of accretion products and other low volatility compounds, Atmos. Chem. Phys., 15, 7765–7776, https://doi.org/10.5194/acp-15-7765-2015, 2015.
Ma, Y. and Marston, G.: Multifunctional acid formation from the gas-phase ozonolysis of β-pinene, Phys. Chem. Chem. Phys., 10, 6115–6126, https://doi.org/10.1039/b807863g, 2008.
Mohr, C., Lopez-Hilfiker, F. D., Yli-Juuti, T., Heitto, A., Lutz, A., Hallquist, M., D'Ambro, E. L., Rissanen, M. P., Hao, L. Q., Schobesberger, S., Kulmala, M., Mauldin III, R. L., Makkonen, U., Sipilä, M., Petäjä, T., and Thornton, J. A.: Ambient observations of dimers from terpene oxidation in the gas phase: Implications for new particle formation and growth, Geophys. Res. Lett., 44, 2958–2966, https://doi.org/10.1002/2017GL072718, 2017.
Müller, L., Reinnig, M.-C., Warnke, J., and Hoffmann, Th.: Unambiguous identification of esters as oligomers in secondary organic aerosol formed from cyclohexene and cyclohexene/α-pinene ozonolysis, Atmos. Chem. Phys., 8, 1423–1433, https://doi.org/10.5194/acp-8-1423-2008, 2008.
Naumann, K. H.: COSIMA – a computer program simulating the dynamics of fractal aerosols, J. Aerosol Sci., 34, 1371–1397, 2003.
Nguyen, T., Peeters, J., and Vereecken, L.: Theoretical study of the gas-phase ozonolysis of β-pinene (C10H16), Phys. Chem. Chem. Phys., 11, 5643–5656, https://doi.org/10.1039/b822984h, 2009.
Onel, L., Lade, R., Mortiboy, J., Blitz, M. A., Seakins, P. W., Heard, D. E., and Stone, D.: Kinetics of the gas phase reaction of the Criegee intermediate CH2OO with SO2 as a function of temperature, Phys. Chem. Chem. Phys., 23, 19415–19423, https://doi.org/10.1039/d1cp02932k, 2021.
Orlando, J. J. and Tyndall, G. S.: Laboratory studies of organic peroxy radical chemistry: An overview with emphasis on recent issues of atmospheric significance, Chem. Soc. Rev., 41, 6294–6317, https://doi.org/10.1039/c2cs35166h, 2012.
Pathak, R., Stanier, C. O., Donahue, N. M., and Pandis, S. N.: Ozonolysis of α-pinene at atmospherically relevant concentrations: Temperature dependence of aerosol mass fractions (yields), J. Geophys. Res., 112, D03201, https://doi.org/10.1029/2006JD007436, 2007.
Pathak, R., Donahue, N. M., and Pandis, S. N.: Ozonolysis of β-pinene: Temperature dependence of secondary organic aerosol mass fraction, Environ. Sci. Technol., 42, 5081–5086, https://doi.org/10.1021/es070721z, 2008.
Peltola, J., Seal, P., Inkilä, A., and Eskola, A.: Time-resolved, broadband UV-absorption spectrometry measurements of Criegee intermediate kinetics using a new photolytic precursor: unimolecular decomposition of CH2OO and its reaction with formic acid, Phys. Chem. Chem. Phys., 22, 11797–11808, https://doi.org/10.1039/D0CP00302F, 2020.
Peng, W. H., Le, C., Porter, W. C., and Cocker III, D. R.: Variability in Aromatic Aerosol Yields under Very Low NOx Conditions at Different HO
Percival, C. J., Welz, O., Eskola, A. J., Savee, J. D., Osborn, D. L., Topping, D. O., Lowe, D., Utembe, S. R., Bacak, A., Mcfiggans, G., Cooke, M. C., Xiao, P., Archibald, A. T., Jenkin, M. E., Derwent, R. G., Riipinen, I., Mok, D. W. K., Lee, E. P. F., Dyke, J. M., Taatjes, C. A., and Shallcross, D. E.: Regional and global impacts of Criegee intermediates on atmospheric sulphuric acid concentrations and first steps of aerosol formation, Faraday Discuss., 165, 45–73, https://doi.org/10.1039/c3fd00048f, 2013.
Porter, W. C., Jimenez, J. L., and Barsanti, K. C.: Quantifying Atmospheric Parameter Ranges for Ambient Secondary Organic Aerosol Formation, ACS Earth Space Chem., 5, 2380–2397, https://doi.org/10.1021/acsearthspacechem.1c00090, 2021.
Pospisilova, V., Lopez-Hilfiker, F. D., Bell, D. M., El Haddad, I., Mohr, C., Huang, W., Heikkinen, L., Xiao, M., Dommen, J., Prevot, A., Baltensperger, U., and Slowik, J.: On the fate of oxygenated organic molecules in atmospheric aerosol particles, Sci. Adv., 6, eaax8922, https://doi.org/10.1126/sciadv.aax8922, 2020.
Renbaum-Wolff, L., Grayson, J. W., Bateman, A. P., Kuwata, M., Sellier, M., Murray, B. J., Shilling, J. E., Martin, S. T., and Bertram, A. K.: Viscosity of α-pinene secondary organic material and implications for particle growth and reactivity, P. Natl. Acad. Sci. USA, 110, 8014–8019, https://doi.org/10.1073/pnas.1219548110, 2013.
Praske, E., Otkjær, R. V., Crounse, J. D., Hethcox, J. C., Stoltz, B. M., Kjaergaard, H. G., and Wennberg, P. O.: Atmospheric autoxidation is increasingly important in urban and suburban North America, P. Natl. Acad. Sci. USA, 115, 64–69, https://doi.org/10.1073/pnas.1715540115, 2017.
Robinson, C., Onel, L., Newman, J., Lade, R., Au, K., Sheps, L., Heard, D. E., Seakins, P. W., Blitz, M. A., and Stone, D.: Unimolecular Kinetics of Stabilized CH3CHOO Criegee Intermediates: syn-CH3CHOO Decomposition and anti-CH3CHOO Isomerization, J. Phys. Chem. A, 126, 6984–6994, https://doi.org/10.1021/acs.jpca.2c05461, 2022.
Saathoff, H., Naumann, K.-H., Möhler, O., Jonsson, Å. M., Hallquist, M., Kiendler-Scharr, A., Mentel, Th. F., Tillmann, R., and Schurath, U.: Temperature dependence of yields of secondary organic aerosols from the ozonolysis of α-pinene and limonene, Atmos. Chem. Phys., 9, 1551–1577, https://doi.org/10.5194/acp-9-1551-2009, 2009.
Sakamoto, Y., Yajima, R., Inomata, S., and Hirokawa, J.: Water vapour effects on secondary organic aerosol formation in isoprene ozonolysis, Phys. Chem. Chem. Phys., 19, 3165–3175, https://doi.org/10.1039/c6cp04521a, 2017.
Smith, M. C., Chang, C.-H., Chao, W., Lin, L.-C., Takahashi, K., Boering, K. A., and Lin, J. J.-M.: Strong negative temperature dependence of the simplest Criegee intermediate CH2OO reaction with water dimer, J. Phys. Chem. Lett., 6, 2708–2713, https://doi.org/10.1021/acs.jpclett.5b01109, 2015.
Smith, M. C., Chao, W., Takahashi, K., Boering, K. A., and Lin, J. J.-M.: Unimolecular Decomposition Rate of the Criegee Intermediate (CH3)2COO Measured Directly with UV Absorption Spectroscopy, J. Phys. Chem. A, 120, 4789–4798, https://doi.org/10.1021/acs.jpca.5b12124, 2016.
Simon, M., Dada, L., Heinritzi, M., Scholz, W., Stolzenburg, D., Fischer, L., Wagner, A. C., Kürten, A., Rörup, B., He, X.-C., Almeida, J., Baalbaki, R., Baccarini, A., Bauer, P. S., Beck, L., Bergen, A., Bianchi, F., Bräkling, S., Brilke, S., Caudillo, L., Chen, D., Chu, B., Dias, A., Draper, D. C., Duplissy, J., El-Haddad, I., Finkenzeller, H., Frege, C., Gonzalez-Carracedo, L., Gordon, H., Granzin, M., Hakala, J., Hofbauer, V., Hoyle, C. R., Kim, C., Kong, W., Lamkaddam, H., Lee, C. P., Lehtipalo, K., Leiminger, M., Mai, H., Manninen, H. E., Marie, G., Marten, R., Mentler, B., Molteni, U., Nichman, L., Nie, W., Ojdanic, A., Onnela, A., Partoll, E., Petäjä, T., Pfeifer, J., Philippov, M., Quéléver, L. L. J., Ranjithkumar, A., Rissanen, M. P., Schallhart, S., Schobesberger, S., Schuchmann, S., Shen, J., Sipilä, M., Steiner, G., Stozhkov, Y., Tauber, C., Tham, Y. J., Tomé, A. R., Vazquez-Pufleau, M., Vogel, A. L., Wagner, R., Wang, M., Wang, D. S., Wang, Y., Weber, S. K., Wu, Y., Xiao, M., Yan, C., Ye, P., Ye, Q., Zauner-Wieczorek, M., Zhou, X., Baltensperger, U., Dommen, J., Flagan, R. C., Hansel, A., Kulmala, M., Volkamer, R., Winkler, P. M., Worsnop, D. R., Donahue, N. M., Kirkby, J., and Curtius, J.: Molecular understanding of new-particle formation from α-pinene between −50 and +25 ∘C, Atmos. Chem. Phys., 20, 9183–9207, https://doi.org/10.5194/acp-20-9183-2020, 2020.
Sindelarova, K., Granier, C., Bouarar, I., Guenther, A., Tilmes, S., Stavrakou, T., Müller, J.-F., Kuhn, U., Stefani, P., and Knorr, W.: Global data set of biogenic VOC emissions calculated by the MEGAN model over the last 30 years, Atmos. Chem. Phys., 14, 9317–9341, https://doi.org/10.5194/acp-14-9317-2014, 2014.
Tomaz, S., Wang, D., Zabalegui, N., Li, D., Lamkaddam, H., Bachmeier, F., Vogel, A., Monge, M., Perrier, S., Baltensperger, U., George, C., Rissanen, M., Ehn, M., El Haddad, I., and Riva, M.: Structures and reactivity of peroxy radicals and dimeric products revealed by online tandem mass spectrometry, Nat. Commun., 12, 300, https://doi.org/10.1038/s41467-020-20532-2, 2021.
Valiev, R., Hasan, G., Salo, V.-T., Kubečka, J., and Kurten, T.: Intersystem Crossings Drive Atmospheric Gas-Phase Dimer Formation, J. Phys. Chem. A, 123, 6596–6604, https://doi.org/10.1021/acs.jpca.9b02559, 2019.
Vereecken, L., Rickard, A. R., Newland, M. J., and Bloss, W. J.: Theoretical study of the reactions of Criegee intermediates with ozone, alkylhydroperoxides, and carbon monoxide, Phys. Chem. Chem. Phys., 17, 23847–23858, https://doi.org/10.1039/c5cp03862f, 2015.
von Hessberg, C., von Hessberg, P., Pöschl, U., Bilde, M., Nielsen, O. J., and Moortgat, G. K.: Temperature and humidity dependence of secondary organic aerosol yield from the ozonolysis of β-pinene, Atmos. Chem. Phys., 9, 3583–3599, https://doi.org/10.5194/acp-9-3583-2009, 2009.
Wang, P.-B., Truhlar, D. G., Xia, Y., and Long, B.: Temperature-dependent kinetics of the atmospheric reaction between CH2OO and acetone, Phys. Chem. Chem. Phys., 24, 13066–13073, https://doi.org/10.1039/d2cp01118b, 2022.
Winterhalter, R., Neeb, P., Grossmann, D., Kolloff, A., Horie, O., and Moortgat, G.: Products and Mechanism of the Gas Phase Reaction of Ozone with β-Pinene, J. Atmos. Chem., 35, 165–197, https://doi.org/10.1023/A:1006257800929, 2000.
Yasmeen, F., Vermeylen, R., Szmigielski, R., Iinuma, Y., Böge, O., Herrmann, H., Maenhaut, W., and Claeys, M.: Terpenylic acid and related compounds: precursors for dimers in secondary organic aerosol from the ozonolysis of α- and β-pinene, Atmos. Chem. Phys., 10, 9383–9392, https://doi.org/10.5194/acp-10-9383-2010, 2010.
Ye, Q., Wang, M., Hofbauer, V., Stolzenburg, D., Chen, D., Schervish, M., Vogel, A., Mauldin, R., Baalbaki, R., Brilke, S., Dada, L., Dias, A., Duplissy, J., El Haddad, I., Finkenzeller, H., Fischer, L., He, X., Kim, C., Kürten, A., Lamkaddam, H., Lee, C., Lehtipalo, K., Leiminger, M., Manninen, H., Marten, R., Mentler, B., Partoll, E., Petäjä, T., Rissanen, M., Schobesberger, S., Schuchmann, S., Simon, M., Tham, Y., Vazquez-Pufleau, M., Wagner, A., Wang, Y., Wu, Y., Xiao, M., Baltensperger, U., Curtius, J., Flagan, R., Kirkby, J., Kulmala, M., Volkamer, R., Winkler, P., Worsnop, D., and Donahue, N.: Molecular composition and volatility of nucleated particles from α-pinene oxidation between −50 ∘C and +25 ∘C, Environ. Sci. Technol., 53, 12357–12365, https://doi.org/10.1021/acs.est.9b03265, 2019.
Zhang, D. and Zhang, R. Y.: Ozonolysis of α-pinene and β-pinene: Kinetics and mechanism, J. Chem. Phys., 122, 114308, https://doi.org/10.1063/1.1862616, 2005.
Zhang, X., McVay, R. C., Huang, D. D., Dalleska, N. F., Aumont, B., Flagan, R., and Seinfeld, J. H.: Formation and evolution of molecular products in α-pinene secondary organic aerosol, P. Natl. Acad. Sci. USA, 112, 14168–14173, https://doi.org/10.1073/pnas.1517742112, 2015.
Zhao, Q. L., Liu, F. Y., Wang, W. N., Li, C. Y., Lü, J., and Wang, W. L.: Reactions between hydroxyl-substituted alkylperoxy radicals and Criegee intermediates: correlations of the electronic characteristics of methyl substituents and the reactivity, Phys. Chem. Chem. Phys., 19, 15073–15083, https://doi.org/10.1039/c7cp00869d, 2017.
Zhao, Y., Thornton, J. A., and Pye, H. O. T.: Quantitative constraints on autoxidation and dimer formation from direct probing of monoterpene-derived peroxy radical chemistry, P. Natl. Acad. Sci. USA, 115, 12142–12147, https://doi.org/10.1073/pnas.1812147115, 2018.
Short summary
This study investigates the role of the important atmospheric reactive intermediates in the formation of dimers and aerosol in monoterpene ozonolysis at different temperatures. Through conducting a series of chamber experiments and utilizing chemical kinetic and aerosol dynamic models, the SOA formation processes are better described, especially for colder regions. The results can be used to improve the chemical mechanism modeling of monoterpenes and SOA parameterization in transport models.
This study investigates the role of the important atmospheric reactive intermediates in the...
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