Articles | Volume 23, issue 10
https://doi.org/10.5194/acp-23-5993-2023
© Author(s) 2023. 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-23-5993-2023
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Collision-sticking rates of acid–base clusters in the gas phase determined from atomistic simulation and a novel analytical interacting hard-sphere model
Huan Yang
CORRESPONDING AUTHOR
Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, P.O. Box 64, 00014 Helsinki, Finland
Ivo Neefjes
Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, P.O. Box 64, 00014 Helsinki, Finland
Valtteri Tikkanen
Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, P.O. Box 64, 00014 Helsinki, Finland
Jakub Kubečka
Department of Chemistry, iClimate, Aarhus University, Langelandsgade 140, 8000 Aarhus C, Denmark
Theo Kurtén
Institute for Atmospheric and Earth System Research/Chemistry, Faculty of Science, University of Helsinki, P.O. Box 55, 00014 Helsinki, Finland
Hanna Vehkamäki
Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, P.O. Box 64, 00014 Helsinki, Finland
Bernhard Reischl
Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, P.O. Box 64, 00014 Helsinki, Finland
Related authors
Ella Häkkinen, Huan Yang, Runlong Cai, and Juha Kangasluoma
Atmos. Meas. Tech., 17, 4211–4225, https://doi.org/10.5194/amt-17-4211-2024, https://doi.org/10.5194/amt-17-4211-2024, 2024
Short summary
Short summary
We report measurements of evaporation kinetics and surface equilibrium vapor pressures for various laboratory-generated organic nanoparticles using the dynamic-aerosol-size electrical mobility spectrometer (DEMS), a recent advancement in aerosol process characterization. Our findings align well with literature values, demonstrating DEMS's effectiveness. We suggest future improvements to DEMS and anticipate its potential for probing aerosol-related kinetic processes with unknown mechanisms.
Ivo Neefjes, Yosef Knattrup, Haide Wu, Georg Baadsgaard Trolle, Jonas Elm, and Jakub Kubečka
Aerosol Research Discuss., https://doi.org/10.5194/ar-2025-30, https://doi.org/10.5194/ar-2025-30, 2025
Preprint under review for AR
Short summary
Short summary
We investigated how water vapor affects the earliest steps of atmospheric aerosol formation, a key process influencing clouds and climate. By benchmarking quantum-chemical methods, we identified reliable approaches for modeling hydrated molecular clusters of common atmospheric acids and bases. We show that humidity moderately stabilizes certain clusters but only modestly alters particle formation rates. These findings sharpen our understanding of clusters and their role in aerosol formation.
Yosef Knattrup, Ivo Neefjes, Jakub Kubečka, and Jonas Elm
Aerosol Research, 3, 237–251, https://doi.org/10.5194/ar-3-237-2025, https://doi.org/10.5194/ar-3-237-2025, 2025
Short summary
Short summary
Aerosols, a large uncertainty in climate modeling, can be formed when gas vapors and particles begin sticking together. Traditionally, these particles are assumed to behave like hard spheres that only stick together upon head-on collisions. In reality, particles can attract each other over distances, leading to more frequent sticking events. We found that traditional models significantly undercount these events, with real sticking rates being up to 2.4 times higher.
Alfred W. Mayhew, Lauri Franzon, Kelvin H. Bates, Theo Kurtén, Felipe D. Lopez-Hilfiker, Claudia Mohr, Andrew R. Rickard, Joel A. Thornton, and Jessica D. Haskins
EGUsphere, https://doi.org/10.5194/egusphere-2025-1922, https://doi.org/10.5194/egusphere-2025-1922, 2025
Short summary
Short summary
This work outlines an investigation into an understudied atmospheric chemical reaction pathway with the potential to form particulate pollution that has important impacts on air quality and climate. We suggest that this chemical pathway is responsible for a large fraction of the atmospheric particulate matter observed in tropical forested regions, but we also highlight the need for further ambient and lab investigations to inform an accurate representation of this process in atmospheric models.
Yuanyuan Luo, Lauri Franzon, Jiangyi Zhang, Nina Sarnela, Neil M. Donahue, Theo Kurtén, and Mikael Ehn
Atmos. Chem. Phys., 25, 4655–4664, https://doi.org/10.5194/acp-25-4655-2025, https://doi.org/10.5194/acp-25-4655-2025, 2025
Short summary
Short summary
This study explores the formation of accretion products from reactions involving highly reactive compounds, Criegee intermediates. We focused on three types of terpenes, common in nature, and their reactions with specific acids. Our findings reveal that these reactions efficiently produce expected compounds. This research enhances our understanding of how these reactions affect air quality and climate by contributing to aerosol formation, crucial for atmospheric chemistry.
Valtteri Tikkanen, Huan Yang, Hanna Vehkamäki, and Bernhard Reischl
EGUsphere, https://doi.org/10.5194/egusphere-2025-507, https://doi.org/10.5194/egusphere-2025-507, 2025
Short summary
Short summary
Collisions of neutral molecules and clusters is the prevalent pathway in atmospheric new particle formation. In heavily polluted urban areas, where clusters are formed rapidly and in large number, cluster-cluster collisions also become relevant. We calculate cluster-cluster collision rates from atomistic molecular dynamics simulations and an interacting hard sphere model. Not accounting for long-range attractive interactions underestimates collision and particle formation rates significantly.
Lauri Franzon, Marie Camredon, Richard Valorso, Bernard Aumont, and Theo Kurtén
Atmos. Chem. Phys., 24, 11679–11699, https://doi.org/10.5194/acp-24-11679-2024, https://doi.org/10.5194/acp-24-11679-2024, 2024
Short summary
Short summary
In this article we investigate the formation of large, sticky molecules from various organic compounds entering the atmosphere as primary emissions and the degree to which these processes may contribute to organic aerosol particle mass. More specifically, we qualitatively investigate a recently discovered chemical reaction channel for one of the most important short-lived radical compounds, peroxy radicals, and discover which of these reactions are most atmospherically important.
Ella Häkkinen, Huan Yang, Runlong Cai, and Juha Kangasluoma
Atmos. Meas. Tech., 17, 4211–4225, https://doi.org/10.5194/amt-17-4211-2024, https://doi.org/10.5194/amt-17-4211-2024, 2024
Short summary
Short summary
We report measurements of evaporation kinetics and surface equilibrium vapor pressures for various laboratory-generated organic nanoparticles using the dynamic-aerosol-size electrical mobility spectrometer (DEMS), a recent advancement in aerosol process characterization. Our findings align well with literature values, demonstrating DEMS's effectiveness. We suggest future improvements to DEMS and anticipate its potential for probing aerosol-related kinetic processes with unknown mechanisms.
Lukas Pichelstorfer, Pontus Roldin, Matti Rissanen, Noora Hyttinen, Olga Garmash, Carlton Xavier, Putian Zhou, Petri Clusius, Benjamin Foreback, Thomas Golin Almeida, Chenjuan Deng, Metin Baykara, Theo Kurten, and Michael Boy
EGUsphere, https://doi.org/10.5194/egusphere-2023-1415, https://doi.org/10.5194/egusphere-2023-1415, 2023
Preprint archived
Short summary
Short summary
Secondary organic aerosols (SOA) form effectively from gaseous precursors via a process called autoxidation. While key chemical reaction types seem to be known, no general description of autoxidation chemistry exists. In the present work, we present a method to create autoxidation chemistry schemes for any atmospherically relevant hydrocarbon. We exemplarily investigate benzene and its potential to form aerosols. We found that autoxidation, under some conditions, can dominate the SOA formation.
Melissa Meder, Otso Peräkylä, Jonathan G. Varelas, Jingyi Luo, Runlong Cai, Yanjun Zhang, Theo Kurtén, Matthieu Riva, Matti Rissanen, Franz M. Geiger, Regan J. Thomson, and Mikael Ehn
Atmos. Chem. Phys., 23, 4373–4390, https://doi.org/10.5194/acp-23-4373-2023, https://doi.org/10.5194/acp-23-4373-2023, 2023
Short summary
Short summary
We discuss and show the viability of a method where multiple isotopically labelled precursors are used for probing the formation pathways of highly oxygenated organic molecules (HOMs) from the oxidation of the monoterpene a-pinene. HOMs are very important for secondary organic aerosol (SOA) formation in forested regions, and monoterpenes are the single largest source of SOA globally. The fast reactions forming HOMs have thus far remained elusive despite considerable efforts over the last decade.
Ivo Neefjes, Roope Halonen, Hanna Vehkamäki, and Bernhard Reischl
Atmos. Chem. Phys., 22, 11155–11172, https://doi.org/10.5194/acp-22-11155-2022, https://doi.org/10.5194/acp-22-11155-2022, 2022
Short summary
Short summary
Collisions between ionic and dipolar molecules and clusters facilitate the formation of atmospheric aerosol particles, which affect global climate and air quality. We compared often-used classical approaches for calculating ion–dipole collision rates with robust atomistic computer simulations. While classical approaches work for simple ions and dipoles only, our modeling approach can also efficiently calculate reasonable collision properties for more complex systems.
Golnaz Roudsari, Olli H. Pakarinen, Bernhard Reischl, and Hanna Vehkamäki
Atmos. Chem. Phys., 22, 10099–10114, https://doi.org/10.5194/acp-22-10099-2022, https://doi.org/10.5194/acp-22-10099-2022, 2022
Short summary
Short summary
We use atomistic simulations to study heterogeneous ice nucleation on silver iodide surfaces in slit and wedge geometries at low supercooling which serve as a model of irregularities on real atmospheric aerosol particle surfaces. The revealed microscopic ice nucleation mechanisms in confined geometries strongly support the experimental evidence for the importance of surface features such as cracks or pits functioning as active sites for ice nucleation in the atmosphere.
Haiyan Li, Thomas Golin Almeida, Yuanyuan Luo, Jian Zhao, Brett B. Palm, Christopher D. Daub, Wei Huang, Claudia Mohr, Jordan E. Krechmer, Theo Kurtén, and Mikael Ehn
Atmos. Meas. Tech., 15, 1811–1827, https://doi.org/10.5194/amt-15-1811-2022, https://doi.org/10.5194/amt-15-1811-2022, 2022
Short summary
Short summary
This work evaluated the potential for PTR-based mass spectrometers to detect ROOR and ROOH peroxides both experimentally and through computations. Laboratory experiments using a Vocus PTR observed only noisy signals of potential dimers during α-pinene ozonolysis and a few small signals of dimeric compounds during cyclohexene ozonolysis. Quantum chemical calculations for model ROOR and ROOH systems showed that most of these peroxides should fragment partially following protonation.
Dina Alfaouri, Monica Passananti, Tommaso Zanca, Lauri Ahonen, Juha Kangasluoma, Jakub Kubečka, Nanna Myllys, and Hanna Vehkamäki
Atmos. Meas. Tech., 15, 11–19, https://doi.org/10.5194/amt-15-11-2022, https://doi.org/10.5194/amt-15-11-2022, 2022
Short summary
Short summary
To study what is happening in the atmosphere, it is important to be able to measure the molecules and clusters present in it. In our work, we studied an artifact that happens inside a mass spectrometer, in particular the fragmentation of clusters. We were able to quantify the fragmentation and retrieve the correct concentration and composition of the clusters using our dual (experimental and theoretical) approach.
Shahzad Gani, Lukas Kohl, Rima Baalbaki, Federico Bianchi, Taina M. Ruuskanen, Olli-Pekka Siira, Pauli Paasonen, and Hanna Vehkamäki
Geosci. Commun., 4, 507–516, https://doi.org/10.5194/gc-4-507-2021, https://doi.org/10.5194/gc-4-507-2021, 2021
Short summary
Short summary
In this article, we present authorship guidelines which also include a novel authorship form along with the documentation of the formulation process for a multidisciplinary and interdisciplinary center with more than 250 researchers. Our practical approach promotes fair authorship practices and, by focusing on clear, transparent, and timely communication, helps avoid late-stage authorship conflict.
Emma Lumiaro, Milica Todorović, Theo Kurten, Hanna Vehkamäki, and Patrick Rinke
Atmos. Chem. Phys., 21, 13227–13246, https://doi.org/10.5194/acp-21-13227-2021, https://doi.org/10.5194/acp-21-13227-2021, 2021
Short summary
Short summary
The study of climate change relies on climate models, which require an understanding of aerosol formation. We train a machine-learning model to predict the partitioning coefficients of atmospheric molecules, which govern condensation into aerosols. The model can make instant predictions based on molecular structures with accuracy surpassing that of standard computational methods. This will allow the screening of low-volatility molecules that contribute most to aerosol formation.
Xiaolong Fan, Jing Cai, Chao Yan, Jian Zhao, Yishuo Guo, Chang Li, Kaspar R. Dällenbach, Feixue Zheng, Zhuohui Lin, Biwu Chu, Yonghong Wang, Lubna Dada, Qiaozhi Zha, Wei Du, Jenni Kontkanen, Theo Kurtén, Siddhart Iyer, Joni T. Kujansuu, Tuukka Petäjä, Douglas R. Worsnop, Veli-Matti Kerminen, Yongchun Liu, Federico Bianchi, Yee Jun Tham, Lei Yao, and Markku Kulmala
Atmos. Chem. Phys., 21, 11437–11452, https://doi.org/10.5194/acp-21-11437-2021, https://doi.org/10.5194/acp-21-11437-2021, 2021
Short summary
Short summary
We observed significant concentrations of gaseous HBr and HCl throughout the winter and springtime in urban Beijing, China. Our results indicate that gaseous HCl and HBr are most likely originated from anthropogenic emissions such as burning activities, and the gas–aerosol partitioning may play a crucial role in contributing to the gaseous HCl and HBr. These observations suggest that there is an important recycling pathway of halogen species in inland megacities.
Mingyi Wang, Xu-Cheng He, Henning Finkenzeller, Siddharth Iyer, Dexian Chen, Jiali Shen, Mario Simon, Victoria Hofbauer, Jasper Kirkby, Joachim Curtius, Norbert Maier, Theo Kurtén, Douglas R. Worsnop, Markku Kulmala, Matti Rissanen, Rainer Volkamer, Yee Jun Tham, Neil M. Donahue, and Mikko Sipilä
Atmos. Meas. Tech., 14, 4187–4202, https://doi.org/10.5194/amt-14-4187-2021, https://doi.org/10.5194/amt-14-4187-2021, 2021
Short summary
Short summary
Atmospheric iodine species are often short-lived with low abundance and have thus been challenging to measure. We show that the bromide chemical ionization mass spectrometry, compatible with both the atmospheric pressure and reduced pressure interfaces, can simultaneously detect various gas-phase iodine species. Combining calibration experiments and quantum chemical calculations, we quantify detection sensitivities to HOI, HIO3, I2, and H2SO4, giving detection limits down to < 106 molec. cm-3.
Georgia Michailoudi, Jack J. Lin, Hayato Yuzawa, Masanari Nagasaka, Marko Huttula, Nobuhiro Kosugi, Theo Kurtén, Minna Patanen, and Nønne L. Prisle
Atmos. Chem. Phys., 21, 2881–2894, https://doi.org/10.5194/acp-21-2881-2021, https://doi.org/10.5194/acp-21-2881-2021, 2021
Short summary
Short summary
This study provides insight into hydration of two significant atmospheric compounds, glyoxal and methylglyoxal. Using synchrotron radiation excited X-ray absorption spectroscopy, we confirm that glyoxal is fully hydrated in water, and for the first time, we experimentally detect enol structures in aqueous methylglyoxal. Our results support the contribution of these compounds to secondary organic aerosol formation, known to have a large uncertainty in atmospheric models and climate predictions.
Anna Shcherbacheva, Tracey Balehowsky, Jakub Kubečka, Tinja Olenius, Tapio Helin, Heikki Haario, Marko Laine, Theo Kurtén, and Hanna Vehkamäki
Atmos. Chem. Phys., 20, 15867–15906, https://doi.org/10.5194/acp-20-15867-2020, https://doi.org/10.5194/acp-20-15867-2020, 2020
Short summary
Short summary
Atmospheric new particle formation and cluster growth to aerosol particles is an important field of research, in particular due to the climate change phenomenon. Evaporation rates are very difficult to account for but they are important to explain the formation and growth of particles. Different quantum chemistry (QC) methods produce substantially different values for the evaporation rates. We propose a novel approach for inferring evaporation rates of clusters from available measurements.
Noora Hyttinen, Reyhaneh Heshmatnezhad, Jonas Elm, Theo Kurtén, and Nønne L. Prisle
Atmos. Chem. Phys., 20, 13131–13143, https://doi.org/10.5194/acp-20-13131-2020, https://doi.org/10.5194/acp-20-13131-2020, 2020
Short summary
Short summary
We present aqueous solubilities and activity coefficients of mono- and dicarboxylic acids (C1–C6 and C2–C8, respectively) estimated using the COSMOtherm program. In addition, we have calculated effective equilibrium constants of dimerization and hydration of the same acids in the condensed phase. We were also able to improve the agreement between experimental and estimated properties of monocarboxylic acids in aqueous solutions by including clustering reactions in COSMOtherm calculations.
Cited articles
Barducci, A., Bussi, G., and Parrinello, M.: Well-Tempered Metadynamics: A
Smoothly Converging and Tunable Free-Energy Method, Phys. Rev. Lett., 100,
020603, https://doi.org/10.1103/PhysRevLett.100.020603, 2008. a
Becker, R. and Döring, W.: Kinetische Behandlung der Keimbildung in
übersättigten Dämpfen, Ann. Phys., 416, 719–752,
https://doi.org/10.1002/andp.19354160806, 1935. a
Clary, D.: Calculations of rate constants for ion-molecule reactions using a
combined capture and centrifugal sudden approximation, Mol. Phys., 54,
605–618, https://doi.org/10.1080/00268978500100461, 1985. a
Elm, J., Jen, C. N., Kurtén, T., and Vehkamäki, H.: Strong Hydrogen Bonded
Molecular Interactions between Atmospheric Diamines and Sulfuric Acid,
J. Phys. Chem. A, 120, 3693–3700, https://doi.org/10.1021/acs.jpca.6b03192, 2016. a
Farkas, L.: Keimbildungsgeschwindigkeit in übersättigten Dämpfen,
Z. Phys. Chem., 125U, 236–242, https://doi.org/10.1515/zpch-1927-12513, 1927. a
Fuchs, N. and Sutugin, A.: Coagulation rate of highly dispersed aerosols,
J. Colloid Sci., 20, 492–500, https://doi.org/10.1016/0095-8522(65)90031-0, 1965. a, b
Gioumousis, G. and Stevenson, D. P.: Reactions of Gaseous Molecule Ions with
Gaseous Molecules. V. Theory, J. Chem. Phys., 29, 294–299,
https://doi.org/10.1063/1.1744477, 1958. a
Guo, S., Hu, M., Zamora, M. L., Peng, J., Shang, D., Zheng, J., Du, Z., Wu, Z.,
Shao, M., Zeng, L., Molina, M. J., and Zhang, R.: Elucidating severe urban
haze formation in China, P. Natl. Acad. Sci. USA, 111,
17373–17378, https://doi.org/10.1073/pnas.1419604111, 2014. a
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. a
Halonen, R., Zapadinsky, E., Kurtén, T., Vehkamäki, H., and Reischl, B.: Rate enhancement in collisions of sulfuric acid molecules due to long-range intermolecular forces, Atmos. Chem. Phys., 19, 13355–13366, https://doi.org/10.5194/acp-19-13355-2019, 2019. a, b, c, d
Hamaker, H.: The London—van der Waals attraction between spherical particles,
Physica, 4, 1058–1072, https://doi.org/10.1016/S0031-8914(37)80203-7, 1937. a, b
Jorgensen, W. L., Maxwell, D. S., and Tirado-Rives, J.: Development and Testing
of the OPLS All-Atom Force Field on Conformational Energetics and Properties
of Organic Liquids, J. Am. Chem. Soc., 118, 11225–11236,
https://doi.org/10.1021/ja9621760, 1996. a
Kirkby, J., Curtius, J., Almeida, J., Dunne, E., Duplissy, J., Ehrhart, S.,
Franchin, A., Gagné, S., Ickes, L., Kürten, A., Kupc, A., Metzger, A.,
Riccobono, F., Rondo, L., Schobesberger, S., Tsagkogeorgas, G., Wimmer, D.,
Amorim, A., Bianchi, F., Breitenlechner, M., David, A., Dommen, J., Downard,
A., Ehn, M., Flagan, R. C., Haider, S., Hansel, A., Hauser, D., Jud, W.,
Junninen, H., Kreissl, F., Kvashin, A., Laaksonen, A., Lehtipalo, K., Lima,
J., Lovejoy, E. R., Makhmutov, V., Mathot, S., Mikkilä, J., Minginette, P.,
Mogo, S., Nieminen, T., Onnela, A., Pereira, P., Petäjä, T., Schnitzhofer,
R., Seinfeld, J. H., Mikko Sipilä, Y. S., Stratmann, F., Tomé, A.,
Vanhanen, J., Viisanen, Y., Vrtala, A., Wagner, P. E., Walther, H.,
Weingartner, E., Wex, H., Winkler, P. M., Carslaw, K. S., Worsnop, D. R.,
Baltensperger, U., and Kulmala, M.: Role of sulphuric acid, ammonia and
galactic cosmic rays in atmospheric aerosol nucleation, Nature, 476,
429–433, https://doi.org/10.1038/nature10343, 2011. a
Kulmala, M., Pirjola, L., and Mäkelä, J. M.: Elucidating severe urban haze
formation in China, P. Natl. Acad. Sci. USA, 404, 66–69,
https://doi.org/10.1038/35003550, 2000. a
Kulmala, M., Kontkanen, J., Junninen, H., Lehtipalo, K., Manninen, H. E.,
Nieminen, T., Petäjä, T., Sipilä, M., Schobesberger, S., Rantala, P.,
Franchin, A., Jokinen, T., Järvinen, E., Äijälä, M., Kangasluoma, J.,
Hakala, J., Aalto, P. P., Paasonen, P., Mikkilä, J., Vanhanen, J., Aalto,
J., Hakola, H., Makkonen, U., Ruuskanen, T., Mauldin, R. L., Duplissy, J.,
Vehkamäki, H., Bäck, J., Kortelainen, A., Riipinen, I., Kurtén, T.,
Johnston, M. V., Smith, J. N., Ehn, M., Mentel, T. F., Lehtinen, K. E. J.,
Laaksonen, A., Kerminen, V.-M., and Worsnop, D. R.: Direct Observations of
Atmospheric Aerosol Nucleation, Science, 339, 943–946,
https://doi.org/10.1126/science.1227385, 2013. a
Kurtén, T., Loukonen, V., Vehkamäki, H., and Kulmala, M.: Amines are likely to enhance neutral and ion-induced sulfuric acid-water nucleation in the atmosphere more effectively than ammonia, Atmos. Chem. Phys., 8, 4095–4103, https://doi.org/10.5194/acp-8-4095-2008, 2008. a
Landau, L. D. and Lifshitz, E. M.: Mechanics, vol. 1, Butterworth-Heinemann,
https://doi.org/10.1016/C2009-0-25569-3, 1976. a
Lehtipalo, K., Rondo, L., Kontkanen, J., Schobesberger, S., Jokinen, T.,
Sarnela, N., Kürten, A., Ehrhart, S., Franchin, A., Nieminen, T., Riccobono,
F., Sipilä, M., Yli-Juuti, T., Duplissy, J., Adamov, A., Ahlm, L., Almeida,
J., Amorim, A., Bianchi, F., Breitenlechner, M., Dommen, J., Downard, A. J.,
Dunne, E. M., Flagan, R. C., Guida, R., Hakala, J., Hansel, A., Jud, W.,
Kangasluoma, J., Kerminen, V.-M., Keskinen, H., Kim, J., Kirkby, J., Kupc,
A., Kupiainen-Määttä, O., Laaksonen, A., Lawler, M. J., Leiminger, M.,
Mathot, S., Olenius, T., Ortega, I. K., Onnela, A., Petäjä, T., Praplan,
A., Rissanen, M. P., Ruuskanen, T., Santos, F. D., Schallhart, S.,
Schnitzhofer, R., Simon, M., Smith, J. N., Tröstl, J., Tsagkogeorgas, G.,
Tomé, A., Vaattovaara, P., Vehkamäki, H., Vrtala, A. E., Wagner, P. E.,
Williamson, C., Wimmer, D., Winkler, P. M., Virtanen, A., Donahue, N. M.,
Carslaw, K. S., Baltensperger, U., Riipinen, I., Curtius, J., Worsnop, D. R.,
and Kulmala, M.: The effect of acid–base clustering and ions on the growth
of atmospheric nano-particles, Nat. Commun., 7, 11594,
https://doi.org/10.1038/ncomms11594, 2016. a
Leite, F. L., Bueno, C. C., Da Róz, A. L., Ziemath, E. C., and Oliveira,
O. N.: Theoretical Models for Surface Forces and Adhesion and Their
Measurement Using Atomic Force Microscopy, Int. J. Mol. Sci., 13,
12773–12856, https://doi.org/10.3390/ijms131012773, 2012. a
Loukonen, V., Kurtén, T., Ortega, I. K., Vehkamäki, H., Pádua, A. A. H., Sellegri, K., and Kulmala, M.: Enhancing effect of dimethylamine in sulfuric acid nucleation in the presence of water – a computational study, Atmos. Chem. Phys., 10, 4961–4974, https://doi.org/10.5194/acp-10-4961-2010, 2010. a, b
Moran, T. F. and Hamill, W. H.: Cross Sections of Ion–Permanent-Dipole
Reactions by Mass Spectrometry, J. Chem. Phys., 39, 1413–1422,
https://doi.org/10.1063/1.1734457, 1963. a
Myllys, N., Olenius, T., Kurtén, T., Vehkamäki, H., Riipinen, I., and Elm,
J.: Effect of Bisulfate, Ammonia, and Ammonium on the Clustering of Organic
Acids and Sulfuric Acid, J. Phys. Chem. A, 121, 4812–4824,
https://doi.org/10.1021/acs.jpca.7b03981, 2017. a
Neefjes, I., Halonen, R., Vehkamäki, H., and Reischl, B.: Modeling approaches for atmospheric ion–dipole collisions: all-atom trajectory simulations and central field methods, Atmos. Chem. Phys., 22, 11155–11172, https://doi.org/10.5194/acp-22-11155-2022, 2022. a, b, c
Ortega, I. K., Kupiainen, O., Kurtén, T., Olenius, T., Wilkman, O., McGrath, M. J., Loukonen, V., and Vehkamäki, H.: From quantum chemical formation free energies to evaporation rates, Atmos. Chem. Phys., 12, 225–235, https://doi.org/10.5194/acp-12-225-2012, 2012. a
Ouyang, H., Gopalakrishnan, R., and Hogan, C. J.: Nanoparticle collisions in
the gas phase in the presence of singular contact potentials, J. Chem. Phys.,
137, 064316, https://doi.org/10.1063/1.4742064, 2012. a
Plimpton, S.: Fast Parallel Algorithms for Short-Range Molecular Dynamics,
J. Comput. Phys., 117, 1–19, https://doi.org/10.1006/jcph.1995.1039, 1995. a, b
Pope III, C. A. and Dockery, D. W.: Aerosols, Climate, and the Hydrological
Cycle, J. Air Waste Manage., 56, 709–742,
https://doi.org/10.1080/10473289.2006.10464485, 2006. a
Pöschl, U.: Atmospheric Aerosols: Composition, Transformation, Climate and
Health Effects, Angew. Chem. Int. Edit., 44, 7520–7540,
https://doi.org/10.1002/anie.200501122, 2005. a
Ramanathan, V., Crutzen, P. J., Kiehl, J. T., and Rosenfeld, D.: Aerosols,
Climate, and the Hydrological Cycle, Science, 294, 2119–2124,
https://doi.org/10.1126/science.1064034, 2001. a
Sceats, M. G.: Brownian coagulation in aerosols—the role of long range
forces, J. Colloid Interface Sci., 129, 105–112,
https://doi.org/10.1016/0021-9797(89)90419-0, 1989. a
Schenter, G. K., Kathmann, S. M., and Garrett, B. C.: Dynamical Nucleation
Theory: A New Molecular Approach to Vapor-Liquid Nucleation,
Phys. Rev. Lett., 82, 3484–3487, https://doi.org/10.1103/PhysRevLett.82.3484, 1999. a
Seinfeld, J. H., Bretherton, C., Carslaw, K. S., Coe, H., DeMott, P. J.,
Dunlea, E. J., Feingold, G., Ghan, S., Guenther, A. B., Kahn, R., Kraucunas,
I., Kreidenweis, S. M., Molina, M. J., Nenes, A., Penner, J. E., Prather,
K. A., Ramanathan, V., Ramaswamy, V., Rasch, P. J., Ravishankara, A. R.,
Rosenfeld, D., Stephens, G., and Wood, R.: Improving our fundamental
understanding of the role of aerosol-cloud interactions in the climate
system, P. Natl. Acad. Sci. USA, 113, 5781–5790,
https://doi.org/10.1073/pnas.1514043113, 2016. a
Sipilä, M., Berndt, T., Petäjä, T., Brus, D., Vanhanen, J., Stratmann, F.,
Patokoski, J., Mauldin, R. L., Hyvärinen, A.-P., Lihavainen, H., and
Kulmala, M.: The Role of Sulfuric Acid in Atmospheric Nucleation, Science,
327, 1243–1246, https://doi.org/10.1126/science.1180315, 2010. a
Stolzenburg, D., Simon, M., Ranjithkumar, A., Kürten, A., Lehtipalo, K., Gordon, H., Ehrhart, S., Finkenzeller, H., Pichelstorfer, L., Nieminen, T., He, X.-C., Brilke, S., Xiao, M., Amorim, A., Baalbaki, R., Baccarini, A., Beck, L., Bräkling, S., Caudillo Murillo, L., Chen, D., Chu, B., Dada, L., Dias, A., Dommen, J., Duplissy, J., El Haddad, I., Fischer, L., Gonzalez Carracedo, L., Heinritzi, M., Kim, C., Koenig, T. K., Kong, W., Lamkaddam, H., Lee, C. P., Leiminger, M., Li, Z., Makhmutov, V., Manninen, H. E., Marie, G., Marten, R., Müller, T., Nie, W., Partoll, E., Petäjä, T., Pfeifer, J., Philippov, M., Rissanen, M. P., Rörup, B., Schobesberger, S., Schuchmann, S., Shen, J., Sipilä, M., Steiner, G., Stozhkov, Y., Tauber, C., Tham, Y. J., Tomé, A., Vazquez-Pufleau, M., Wagner, A. C., Wang, M., Wang, Y., Weber, S. K., Wimmer, D., Wlasits, P. J., Wu, Y., Ye, Q., Zauner-Wieczorek, M., Baltensperger, U., Carslaw, K. S., Curtius, J., Donahue, N. M., Flagan, R. C., Hansel, A., Kulmala, M., Lelieveld, J., Volkamer, R., Kirkby, J., and Winkler, P. M.: Enhanced growth rate of atmospheric particles from sulfuric acid, Atmos. Chem. Phys., 20, 7359–7372, https://doi.org/10.5194/acp-20-7359-2020, 2020.
a
Su, T. and Bowers, M. T.: Theory of ion‐polar molecule collisions. Comparison
with experimental charge transfer reactions of rare gas ions to geometric
isomers of difluorobenzene and dichloroethylene, J. Chem. Phys., 58,
3027–3037, https://doi.org/10.1063/1.1679615, 1973. a
Su, T., Su, E. C., and Bowers, M. T.: Ion–polar molecule collisions.
Conservation of angular momentum in the average dipole orientation theory.
The AADO theory, J. Chem. Phys., 69, 2243–2250, https://doi.org/10.1063/1.436783,
1978. a
Temelso, B., Phan, T. N., and Shields, G. C.: Computational Study of the
Hydration of Sulfuric Acid Dimers: Implications for Acid Dissociation and
Aerosol Formation, J. Phys. Chem. A, 116, 9745–9758,
https://doi.org/10.1021/jp3054394, 2012. a
Tribello, G. A., Bonomi, M., Branduardi, D., Camilloni, C., and Bussi, G.:
PLUMED 2: New feathers for an old bird, Comput. Phys. Commun., 185, 604–613,
https://doi.org/10.1016/j.cpc.2013.09.018, 2014. a
Vehkamäki, H. and Riipinen, I.: Thermodynamics and kinetics of atmospheric
aerosol particle formation and growth, Chem. Soc. Rev., 41, 5160–5173,
https://doi.org/10.1039/C2CS00002D, 2012. a
Yang, H., Goudeli, E., and Hogan, C. J.: Condensation and dissociation rates
for gas phase metal clusters from molecular dynamics trajectory calculations,
J. Chem. Phys., 148, 164304, https://doi.org/10.1063/1.5026689, 2018. a, b
Yang, H., Drossinos, Y., and Hogan, C. J.: Excess thermal energy and latent
heat in nanocluster collisional growth, J. Chem. Phys., 151, 224304,
https://doi.org/10.1063/1.5129918, 2019. a
Yang, H., Song, G., and Hogan, C. J.: A molecular dynamics study of collisional
heat transfer to nanoclusters in the gas phase, J. Aerosol Sci., 159,
105891, https://doi.org/10.1016/j.jaerosci.2021.105891, 2022. a, b
Zhang, R., Khalizov, A., Wang, L., Hu, M., and Xu, W.: Nucleation and Growth of
Nanoparticles in the Atmosphere, Chem. Rev., 112, 1957–2011,
https://doi.org/10.1021/cr2001756, 2012. a
Short summary
We present a new analytical model for collision rates between molecules and clusters of arbitrary sizes, accounting for long-range interactions. The model is verified against atomistic simulations of typical acid–base clusters participating in atmospheric new particle formation (NPF). Compared to non-interacting models, accounting for long-range interactions leads to 2–3 times higher collision rates for small clusters, indicating the necessity of including such interactions in NPF modeling.
We present a new analytical model for collision rates between molecules and clusters of...
Altmetrics
Final-revised paper
Preprint