Articles | Volume 2, issue 1
https://doi.org/10.5194/ar-2-123-2024
© 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/ar-2-123-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
A cluster-of-functional-groups approach for studying organic enhanced atmospheric cluster formation
Astrid Nørskov Pedersen
Department of Chemistry, Aarhus University, Langelandsgade 140, 8000 Aarhus C, Denmark
Yosef Knattrup
Department of Chemistry, Aarhus University, Langelandsgade 140, 8000 Aarhus C, Denmark
Department of Chemistry, Aarhus University, Langelandsgade 140, 8000 Aarhus C, Denmark
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Haide Wu, Yosef Knattrup, Andreas Buchgraitz Jensen, and Jonas Elm
Aerosol Research, 2, 303–314, https://doi.org/10.5194/ar-2-303-2024, https://doi.org/10.5194/ar-2-303-2024, 2024
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The exact point at which a given assembly of molecules represents an atmospheric molecular cluster or a particle remains ambiguous. Using quantum chemical methods, here we explore a cluster-to-particle transition point. Based on our results, we deduce a property-based criterion for defining freshly nucleated particles (FNPs) that act as a boundary between discrete cluster configurations and bulk particles.
Yosef Knattrup and Jonas Elm
Aerosol Research Discuss., https://doi.org/10.5194/ar-2024-37, https://doi.org/10.5194/ar-2024-37, 2024
Preprint under review for AR
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Using quantum chemical methods we studied the uptake of first generation oxidation products onto freshly nucleated particles (FNPs). We find that pinic acid can condense on these small FNPs at realistic atmospheric conditions, thereby contributing to the early particle growth. The mechanism involves two pinic acid molecules interacting with each other, showing that direct organic-organic interactions during co-condensation onto the particle contributes to the growth.
Galib Hasan, Haide Wu, Yosef Knattrup, and Jonas Elm
Aerosol Research Discuss., https://doi.org/10.5194/ar-2024-28, https://doi.org/10.5194/ar-2024-28, 2024
Preprint under review for AR
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Aerosol formation is an important process for our global climate. However, there are large uncertainties associated with the formation of new aerosol particles. We present quantum chemical calculations of large atmospheric molecular cluster composed of sulfuric acid (SA), ammonia (AM) and dimethyl amine (DMA). We find that mixed SA-AM-DMA clusters more efficiently for freshly nucleated particles compared to the pure SA-AM and SA-DMA systems.
Jonas Elm, Aladár Czitrovszky, Andreas Held, Annele Virtanen, Astrid Kiendler-Scharr, Benjamin J. Murray, Daniel McCluskey, Daniele Contini, David Broday, Eirini Goudeli, Hilkka Timonen, Joan Rosell-Llompart, Jose L. Castillo, Evangelia Diapouli, Mar Viana, Maria E. Messing, Markku Kulmala, Naděžda Zíková, and Sebastian H. Schmitt
Aerosol Research, 1, 13–16, https://doi.org/10.5194/ar-1-13-2023, https://doi.org/10.5194/ar-1-13-2023, 2023
Bernadette Rosati, Sini Isokääntä, Sigurd Christiansen, Mads Mørk Jensen, Shamjad P. Moosakutty, Robin Wollesen de Jonge, Andreas Massling, Marianne Glasius, Jonas Elm, Annele Virtanen, and Merete Bilde
Atmos. Chem. Phys., 22, 13449–13466, https://doi.org/10.5194/acp-22-13449-2022, https://doi.org/10.5194/acp-22-13449-2022, 2022
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Sulfate aerosols have a strong influence on climate. Due to the reduction in sulfur-based fossil fuels, natural sulfur emissions play an increasingly important role. Studies investigating the climate relevance of natural sulfur aerosols are scarce. We study the water uptake of such particles in the laboratory, demonstrating a high potential to take up water and form cloud droplets. During atmospheric transit, chemical processing affects the particles’ composition and thus their water uptake.
Jingwen Xue, Fangfang Ma, Jonas Elm, Jingwen Chen, and Hong-Bin Xie
Atmos. Chem. Phys., 22, 11543–11555, https://doi.org/10.5194/acp-22-11543-2022, https://doi.org/10.5194/acp-22-11543-2022, 2022
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·OH/·Cl initiated indole reactions mainly form organonitrates, alkoxy radicals and hydroperoxide products, showing a varying mechanism from previously reported amines reactions. This study reveals carcinogenic nitrosamines cannot be formed in indole oxidation reactions despite radicals formed from -NH- H abstraction. The results are important to understand the atmospheric impact of indole oxidation and extend current understanding on the atmospheric chemistry of organic nitrogen compounds.
Rongjie Zhang, Jiewen Shen, Hong-Bin Xie, Jingwen Chen, and Jonas Elm
Atmos. Chem. Phys., 22, 2639–2650, https://doi.org/10.5194/acp-22-2639-2022, https://doi.org/10.5194/acp-22-2639-2022, 2022
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Formic acid is screened out as the species that can effectively catalyze the new particle formation (NPF) of the methanesulfonic acid (MSA)–methylamine system, indicating organic acids might be required to facilitate MSA-driven NPF in the atmosphere. The results are significant to comprehensively understand the MSA-driven NPF and expand current knowledge of the contribution of OAs to NPF.
Robin Wollesen de Jonge, Jonas Elm, Bernadette Rosati, Sigurd Christiansen, Noora Hyttinen, Dana Lüdemann, Merete Bilde, and Pontus Roldin
Atmos. Chem. Phys., 21, 9955–9976, https://doi.org/10.5194/acp-21-9955-2021, https://doi.org/10.5194/acp-21-9955-2021, 2021
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This study presents a detailed analysis of the OH-initiated oxidation of dimethyl sulfide (DMS) based on experiments performed in the Aarhus University Research on Aerosol (AURA) smog chamber and the gas- and particle-phase chemistry kinetic multilayer model (ADCHAM). We capture the formation, growth and chemical composition of aerosols in the chamber setup by an improved multiphase oxidation mechanism and utilize our results to reproduce the important role of DMS in the marine boundary layer.
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
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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.
Kasper Kristensen, Louise N. Jensen, Lauriane L. J. Quéléver, Sigurd Christiansen, Bernadette Rosati, Jonas Elm, Ricky Teiwes, Henrik B. Pedersen, Marianne Glasius, Mikael Ehn, and Merete Bilde
Atmos. Chem. Phys., 20, 12549–12567, https://doi.org/10.5194/acp-20-12549-2020, https://doi.org/10.5194/acp-20-12549-2020, 2020
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Atmospheric particles are important in relation to human health and the global climate. As the global temperature changes, so may the atmospheric chemistry controlling the formation of particles from reactions of naturally emitted volatile organic compounds (VOCs). In the current work, we show how temperatures influence the formation and chemical composition of atmospheric particles from α-pinene: a biogenic VOC largely emitted in high-latitude environments such as the boreal forests.
Noora Hyttinen, Jonas Elm, Jussi Malila, Silvia M. Calderón, and Nønne L. Prisle
Atmos. Chem. Phys., 20, 5679–5696, https://doi.org/10.5194/acp-20-5679-2020, https://doi.org/10.5194/acp-20-5679-2020, 2020
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Organosulfates have been identified in atmospheric secondary organic aerosol (SOA). The thermodynamic properties of SOA constituents, such as organosulfates, affect the stability and atmospheric impact of the SOA. Here we present estimated solubility, activity, pKa, saturation vapor pressure and Henry's law solubility values for several atmospherically relevant monoterpene- and isoprene-derived organosulfate compounds. These properties can be used, for example, in aerosol process modeling.
Related subject area
Fundamental Aerosol Research (FAR)
Cluster-to-particle transition in atmospheric nanoclusters
Vertical concentrations gradients and transport of airborne microplastics in wind tunnel experiments
Photocatalytic chloride-to-chlorine conversion by ionic iron in aqueous aerosols: a combined experimental, quantum chemical, and chemical equilibrium model study
Haide Wu, Yosef Knattrup, Andreas Buchgraitz Jensen, and Jonas Elm
Aerosol Research, 2, 303–314, https://doi.org/10.5194/ar-2-303-2024, https://doi.org/10.5194/ar-2-303-2024, 2024
Short summary
Short summary
The exact point at which a given assembly of molecules represents an atmospheric molecular cluster or a particle remains ambiguous. Using quantum chemical methods, here we explore a cluster-to-particle transition point. Based on our results, we deduce a property-based criterion for defining freshly nucleated particles (FNPs) that act as a boundary between discrete cluster configurations and bulk particles.
Eike Maximilian Esders, Christoph Georgi, Wolfgang Babel, Andreas Held, and Christoph Karl Thomas
Aerosol Research, 2, 235–243, https://doi.org/10.5194/ar-2-235-2024, https://doi.org/10.5194/ar-2-235-2024, 2024
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Our study explores how tiny plastic particles, known as microplastics (MPs), move through the air. We focus on their journey in a wind tunnel to mimic atmospheric transport. Depending on the air speed and the height of their release, they move downwards or upwards. These results suggest that MPs behave like mineral particles and that we can expect MPs to accumulate where natural dust also accumulates in the environment, offering insights for predicting the spread and impacts of MPs.
Marie K. Mikkelsen, Jesper B. Liisberg, Maarten M. J. W. van Herpen, Kurt V. Mikkelsen, and Matthew S. Johnson
Aerosol Research, 2, 31–47, https://doi.org/10.5194/ar-2-31-2024, https://doi.org/10.5194/ar-2-31-2024, 2024
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We analyze the mechanism whereby sunlight and iron catalyze the production of chlorine from chloride in sea spray aerosol. This process occurs naturally over the North Atlantic and is the single most important source of chlorine. We investigate the mechanism using quantum chemistry, laboratory experiments, and aqueous chemistry modelling. The process will change depending on competing ions, light distribution, acidity, and chloride concentration.
Cited articles
Ayoubi, D., Knattrup, Y., and Elm, J.: Clusteromics V: Organic Enhanced Atmospheric Cluster Formation, ACS Omega, 8, 9621–9629, 2023. a
Baccarini, A., Karlsson, L., Dommen, J., Duplessis, P., Vüllers, J., Brooks, I. M., Saiz-Lopez, A., Salter, M., Tjernström, M., Baltensperger, U., Zieger, P., and Schmale, J.: Frequent New Particle Formation Over the High Arctic Pack Ice by Enhanced Iodine Emissions, Nat. Commun., 11, 4924, https://doi.org/10.1038/s41467-020-18551-0, 2020. a
Bannwarth, C., Caldeweyher, E., Ehlert, S., Hansen, A., Pracht, P., Seibert, J., Spicher, S., and Grimme, S.: Extended Tight-binding Quantum Chemistry Methods, WIREs Comput. Mol. Sci., 11, e1493, https://doi.org/10.1002/wcms.1493, 2021. a
Beck, L. J., Sarnela, N., Junninen, H., Hoppe, C. J. M., Garmash, O., Bianchi, F., Riva, M., Rose, C., Peräkylä, O., Wimmer, D., et al.: Differing Mechanisms of New Particle Formation at Two Arctic Sites, Geophys. Res. Lett., 48, e2020GL091334, https://doi.org/10.1029/2020GL091334, 2021. a
Canadell, J. G., Monteiro, P. M. S., Costa, M. H., Cotrim da Cunha, L., Cox, P. M., Eliseev, A. V., Henson, S., Ishii, M., Jaccard, S., Koven, C., Lohila, A., Patra, P. K., Piao, S., Rogelj, J., Syampungani, S., Zaehle, S., and Zickfeld, K.: Global Carbon and other Biogeochemical Cycles and Feedbacks, in: Climate Change 2021, The Physical Science Basis. Contribution of Working Group I to the Sixth Assessment Report of the Intergovernmental Panel on Climate Change, edited by: Masson-Delmotte, V., Zhai, P., Pirani, A., Connors, S. L., Péan, C., Berger, S., Caud, N., Chen, Y., Goldfarb, L., Gomis, M. I., Huang, M., Leitzell, Lonnoy, K., E., Matthews, J. B. R., Maycock, T. K., Waterfield, T., Yelekçi, O., Yu, R., and Zhou, B., 673–816 pp., Cambridge University Press, Cambridge, United Kingdom and New York, NY, USA, https://doi.org/10.1017/9781009157896.007, 2021. a
Chai, J. and Martin, H.: Long-Range Corrected Hybrid Density Functionals with Damped Atom-Atom Dispersion Corrections, Phys. Chem. Chem. Phys., 10, 6615–6620, 2008. a
Dada, L., Stolzenburg, D., Simon, M., et al.: Role of Sesquiterpenes in Biogenic New Particle Formation, Sci. Adv., 9, eadi5297, https://doi.org/10.1126/sciadv.adi5297, 2023. a, b
Dal Maso, M., Hyvrinen, A., Komppula, M., Tunved, P., Kerminen, V.-M., Lihavainen, H., Viisanen, Y., Hansson, H.-C., and Kulmala, M.: Annual and Interannual Variation in Boreal Forest Aerosol Particle Number and Volume Concentration and their Connection to Particle Formation, Tellus B, 60, 495–508, 2008. a
Dunne, E. M., Gordon, H., Kürten, A., et al.: Global Atmospheric Particle Formation from CERN CLOUD Measurements, Science, 354, 1119–1124, 2016. a
Ehn, M., Thornton, J. A., Kleist, E., et al.: A Large Source of Low-Volatility Secondary Organic Aerosol, Nature, 506, 476–479, 2014. a
Elm, J.: Elucidating the Limiting Steps in Sulfuric Acid - Base New Particle Formation, J. Phys. Chem. A, 121, 8288–8295, 2017. a
Elm, J.: An Atmospheric Cluster Database Consisting of Sulfuric Acid, Bases, Organics, and Water, ACS Omega, 4, 10965–10974, 2019a. a
Elm, J.: Clusteromics II: Methanesulfonic Acid-Base Cluster Formation, ACS Omega, 7, 17035–17044, 2021b. a
Elm, J.: Clusteromics III: Acid Synergy in Sulfuric Acid-Methanesulfonic Acid-Base Cluster Formation, ACS Omega, 6, 15206–15214, 2022. a
Elm, J. and Kristensen, K.: Basis Set Convergence of the Binding Energies of Strongly Hydrogen-Bonded Atmospheric Clusters, Phys. Chem. Chem. Phys, 19, 1122–1133, 2017. a
Elm, J. and Kubecka, J.: Atmospheric Cluster Database (ACDB) (v2.0), Zenodo [data set], https://doi.org/10.5281/zenodo.11422835, 2024. a
Elm, J. and Mikkelsen, K. V.: Computational Approaches for Efficiently Modelling of Small Atmospheric Clusters, Chem. Phys. Lett., 615, 26–29, 2014. a
Elm, J., Myllys, N., Olenius, T., Halonen, R., Kurtén, T., and Vehkamäki, H.: Formation of Atmospheric Molecular Clusters Consisting of Sulfuric Acid and C8H12O6 Tricarboxylic Acid, Phys. Chem. Chem. Phys., 19, 4877–4886, 2017b. a
Elm, J., Ayoubi, D., Engsvang, M., Jensen, A. B., Knattrup, Y., Kubečka, J., Bready, C. J., Fowler, V. R., Harold, S. E., Longsworth, O. M., and Shields, G. C.: Quantum Chemical Modeling of Organic Enhanced Atmospheric Nucleation: A Critical Review, WIREs Comput. Mol. Sci., 13, e1662, https://doi.org/10.1002/wcms.1662, 2023. a, b, c
Gaussian, A., Frisch, M. J., Trucks, G. W., et al.: Gaussian, Inc., Wallingford CT, 2016. a
Grimme, S.: Supramolecular Binding Thermodynamics by Dispersion-Corrected Density Functional Theory, Chem. Eur. J., 18, 9955–9964, 2012. a
Grimme, S., Bannwarth, C., and Shushkov, P.: A Robust and Accurate Tight-Binding Quantum Chemical Method for Structures, Vibrational Frequencies, and Noncovalent Interactions of Large Molecular Systems Parametrized for All spd-Block Elements (Z=1–86), J. Chem. Theory Comput., 13, 1989–2009, 2017. a
He, X.-C., Tham, Y. J., Dada, L., et al.: Role of Iodine Oxoacids in Atmospheric Aerosol Nucleation, Science, 371, 589–595, 2021. a
He, X.-C., Simon, M., Iyer, S., Xie, H.-B., Rörup, B., Shen, J., Finkenzeller, H., Stolzenburg, D., Zhang, R., and Baccarini, A.: Iodine Oxoacids Enhance Nucleation of Sulfuric Acid Particles in the Atmosphere, Science, 382, 1308–1314, 2023. a
Jaoui, M., Corse, E., Kleindienst, T. E., Offenberg, J. H., Lewandowski, M., and Edney, E. O.: Analysis of Secondary Organic Aerosol Compounds from the Photooxidation of d-Limonene in the Presence of NOX and their Detection in Ambient PM2.5, Environ. Sci. Technol, 40, 3819–3828, 2006. a
Jensen, A. B., Kubečka, J., Schmitz, G., Christiansen, O., and Elm, J.: Massive Assessment of the Binding Energies of Atmospheric Molecular Clusters, J. Chem. Theory Comput., 18, 7373–7383, 2022. a
Jimenez, J. L., Canagaratna, M. R., Donahue, N. M., et al.: Evolution of Organic Aerosols in the Atmosphere, Science, 326, 1525–1529, 2009. a
Jokinen, T., Sipilä, M., Junninen, H., Ehn, M., Lönn, G., Hakala, J., Petäjä, T., Mauldin III, R. L., Kulmala, M., and Worsnop, D. R.: Atmospheric sulphuric acid and neutral cluster measurements using CI-APi-TOF, Atmos. Chem. Phys., 12, 4117–4125, https://doi.org/10.5194/acp-12-4117-2012, 2012. a
Kildgaard, J., Mikkelsen, K., Bilde, M., and Elm, J.: Hydration of Atmospheric Molecular Clusters II: Organic Acid – Water Clusters, J. Phys. Chem. A, 122, 8549–8556, 2018a. a
Kildgaard, J. V., Mikkelsen, K. V., Bilde, M., and Elm, J.: Hydration of Atmospheric Molecular Clusters: A New Method for Systematic Configurational Sampling, J. Phys. Chem. A, 122, 5026–5036, 2018b. a
Kirkby, J., Curtius, J., Almeida, J., et al.: Role of Sulphuric Acid, Ammonia and Galactic Cosmic Rays in Atmospheric Aerosol Nucleation, Nature, 476, 429–433, 2011. a
Kirkby, J., Duplissy, J., Sengupta, K., et al.: Ion-induced Nucleation of Pure Biogenic Particles, Nature, 533, 521–525, 2016. a
Kirkby, J., Amorim, A., Baltensperger, U., Carslaw, K. S., Christoudias, T., Curtius, J., Donahue, N. M., El Haddad, I., Flagan, R. C., Gordon, H., Hansel, A., Harder, H., Junninen, H., Kulmala, M., Kürten, A., Laaksonen, A., Lehtipalo, K., Lelieveld, J., Möhler, O., Riipinen, I., Stratmann, F., Tomé, A., Virtanen, A., Volkamer, R., Winkler, P. M., and Worsnop, D. R.: Atmospheric New Particle Formation from the CERN CLOUD Experiment, Nat. Geosci., 16, 948–957, 2023. a, b
Knattrup, Y. and Elm, J.: Clusteromics IV: The Role of Nitric Acid in Atmospheric Cluster Formation, ACS Omega, 7, 31551–31560, 2022. a
Kontkanen, J., Lehtipalo, K., Ahonen, L., Kangasluoma, J., Manninen, H. E., Hakala, J., Rose, C., Sellegri, K., Xiao, S., Wang, L., Qi, X., Nie, W., Ding, A., Yu, H., Lee, S., Kerminen, V.-M., Petäjä, T., and Kulmala, M.: Measurements of sub-3 nm particles using a particle size magnifier in different environments: from clean mountain top to polluted megacities, Atmos. Chem. Phys., 17, 2163–2187, https://doi.org/10.5194/acp-17-2163-2017, 2017. a
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. a
Kubečka, J., Besel, V., Neefjes, I., Knattrup, Y., Kurtén, T., Vehkamäki, H., and Elm, J.: Computational Tools for Handling Molecular Clusters: Configurational Sampling, Storage, Analysis, and Machine Learning, ACS Omega, 8, 45115–45128, 2023. a
Kulmala, M., Kontkanen, J., Junninen, H., et al.: Direct Observations of Atmospheric Aerosol Nucleation, Science, 339, 943–946, 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
Liakos, D. G., Sparta, M., Kesharwani, M. K., Martin, J. M. L., and Neese, F.: Exploring the Accuracy Limits of Local Pair Natural Orbital Coupled-Cluster Theory, J. Chem. Theory Comput., 11, 1525–1539, 2015. a
McGrath, M. J., Olenius, T., Ortega, I. K., Loukonen, V., Paasonen, P., Kurtén, T., Kulmala, M., and Vehkamäki, H.: Atmospheric Cluster Dynamics Code: a flexible method for solution of the birth-death equations, Atmos. Chem. Phys., 12, 2345–2355, https://doi.org/10.5194/acp-12-2345-2012, 2012. a, b, c
Metzger, A., Verheggen, B., Dommen, J., Duplissy, J., Prevot, A. S. H., Weingartner, E., Riipinen, I., Kulmala, M., Spracklen, D. V., Carslaw, K. S., and Baltensperger, U.: Evidence for the Role of Organics in Aerosol Particle Formation under Atmospheric Conditions, P. Natl. Acad. Sci. USA, 107, 6646–6651, 2010. a
Müller, L., Reinnig, M.-C., Naumann, K. H., Saathoff, H., Mentel, T. F., Donahue, N. M., and Hoffmann, T.: Formation of 3-methyl-1,2,3-butanetricarboxylic acid via gas phase oxidation of pinonic acid – a mass spectrometric study of SOA aging, Atmos. Chem. Phys., 12, 1483–1496, https://doi.org/10.5194/acp-12-1483-2012, 2012. a
Myllys, N., Elm, J., and Kurtén, T.: Density Functional Theory Basis Set Convergence of Sulfuric Acid-Containing Molecular Clusters, Comp. Theor. Chem., 1098, 1–12, 2016. 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, 2017. a
Neese, F.: The ORCA Program System, Wiley Interdiscip. Rev.: Comput. Mol. Sci., 2, 73–78, 2012. a
Neese, F.: Software Update: The ORCA Program System, Version 4.0, Wiley Interdiscip. Rev.: Comput. Mol. Sci., 8, e1327, https://doi.org/10.1002/wcms.1327, 2018. a
Neese, F.: Software update: The ORCA program system—Version 5.0, WIREs Comput. Mol. Sci., 12, e1606, https://doi.org/10.1002/wcms.1606, 2022. a
Neese, F., Wennmohs, F., Becker, U., and Riplinger, C.: The ORCA Quantum Chemistry Program Package, J. Chem. Phys., 152, 224108, https://doi.org/10.1063/5.0004608, 2020. a
Odbadrakh, T. T., Gale, A. G., T., B. B., Temelso, B., and Shields, G. C.: Computation of Atmospheric Concentrations of Molecular Clusters from ab initio Thermochemistry, J. Vis. Exp., 8, e60964, https://doi.org/10.3791/60964, 2020. a
Olenius, T., Kupiainen-Määttä, O., Ortega, I. K., Kurtén, T., and Vehkamäki, H.: Free Energy Barrier in the Growth of Sulfuric Acid–Ammonia and Sulfuric Acid–Dimethylamine Clusters, J. Chem. Phys., 139, 084312, https://doi.org/10.1063/1.4819024, 2013. a, b
Ortega, I. K., Donahue, N. M., Kurtén, T., Kulmala, M., Focsa, C., and Vehkamäki, H.: Can Highly Oxidized Organics Contribute to Atmospheric New Particle Formation?, J. Phys. Chem. A, 120, 1452–1458, 2016. a
Pelucchi, C., Negri, E., Gallus, S., Boffetta, P., Tramacere, I., and La Vecchia, C.: Long-term Particulate Matter Exposure and Mortality: A Review of European Epidemiological Studies, BMC Public Health, 9, 453, https://doi.org/10.1186/1471-2458-9-453, 2009. a
Riccobono, F., Schobesberger, S., Scott, C. E., et al.: Oxidation Products of Biogenic Emissions Contribute to Nucleation of Atmospheric Particles, Science, 344, 717–721, 2014. a
Riplinger, C. and Neese, F.: An Efficient and Near Linear Scaling Pair Natural Orbital Based Local Coupled Cluster Method, J. Chem. Phys., 138, 034106, https://doi.org/10.1063/1.4773581, 2013. a
Riplinger, C., Sandhoefer, B., Hansen, A., and Neese, F.: Natural Triple Excitations in Local Coupled Cluster Calculations With Pair Natural Orbitals, J. Chem. Phys., 139, 134101, https://doi.org/10.1063/1.4821834, 2013. a
Roldin, P., Ehn, M., Kurtén, T., Olenius, T., Rissanen, M. P., Sarnela, N., Elm, J., Rantala, P., Hao, L., Hyttinen, N., Heikkinen, L., Worsnop, D. R., Pichelstorfer, L., Xavier, C., Clusius, P., Öström, E., Petäjä, T., Kulmala, M., Vehkamäki, H., Virtanen, A., Riipinen, I., and Boy, M.: The Role of Highly Oxygenated Organic Molecules in the Boreal Aerosol-cloud-climate System, Nat. Commun., 10, 4370, https://doi.org/10.1038/s41467-019-12338-8, 2019. a
Rose, C., Zha, Q., Dada, L., Yan, C., Lehtipalo, K., Junninen, H., Mazon, S. B., Jokinen, T., Sarnela, N., and Sipilä, M.: Observations of Biogenic Ion-induced Cluster Formation in the Atmosphere, Sci. Adv., 4, eaar5218, https://doi.org/10.1126/sciadv.aar5218, 2018. a
Schmitz, G. and Elm, J.: Assessment of the DLPNO Binding Energies of Strongly Non-covalent Bonded Atmospheric Molecular Clusters, ACS Omega, 5, 7601–7612, 2020. a
Schobesberger, S., Junninen, H., Bianchi, F., et al.: Molecular Understanding of Atmospheric Particle Formation from Sulfuric Acid and Large Oxidized Organic Molecules, P. Natl. Acad. Sci. USA, 110, 17223–17228, 2013. a
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. 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, 2010. a
Tan, S., Chen, X., and Yin, S.: Comparison Results of Eight Oxygenated Organic Molecules: Unexpected Contribution to New Particle Formation in the Atmosphere, Atmos. Environ., 268, 118817, https://doi.org/10.1016/j.atmosenv.2021.118817, 2022. a
Temelso, B., Mabey, J. M., Kubota, T., Appiah-Padi, N., and Shields, G. C.: ArbAlign: A Tool for Optimal Alignment of Arbitrarily Ordered Isomers Using the Kuhn–Munkres Algorithm, J. Chem. Inf. Model., 57, 1045–1054, 2017. a
Temelso, B., Morrison, E. F., Speer, D. L., Cao, B. C., Appiah-Padi, N., Kim, G., and Shields, G. C.: Effect of Mixing Ammonia and Alkylamines on Sulfate Aerosol Formation, J. Phys. Chem. A, 122, 1612–1622, 2018. a
Vander Auwera, J., Didriche, K., Perrin, A., and Keller, F.: Absolute Line Intensities for Formic Acid and Dissociation Constant of the Dimer, J. Chem. Phys, 126, 124311, https://doi.org/10.1063/1.2712439, 2007. a
Yasmeen, F., Szmigielski, R., Vermeylen, R., Gómez-González, Y., Surratt, J. D., Chan, A. W. H., Seinfeld, J. H., Maenhaut, W., and Claeys, M.: Mass Spectrometric Characterization of Isomeric Terpenoic Acids From the Oxidation of α-pinene, β-pinene, d-limonene, and Δ3-carene in Fine Forest Aerosol, J. Mass Spectrom., 46, 425–442, 2011. a
Zhang, J. and Dolg, M.: ABCluster: The Artificial Bee Colony Algorithm for Cluster Global Optimization, Phys. Chem. Chem. Phys., 17, 24173–24181, 2015. a
Zhang, J. and Dolg, M.: Global Optimization of Clusters of Rigid Molecules Using the Artificial Bee Colony Algorithm, Phys. Chem. Chem. Phys., 18, 3003–3010, 2016. a
Zhang, R., Suh, I., Zhao, J., Zhang, D., Fortner, E. C., Tie, X., Molina, L. T., and Molina, M. J.: Atmospheric New Particle Formation Enhanced by Organic Acids, Science, 304, 1487–1490, 2004. a
Short summary
Aerosol formation is an important process for our global climate. While inorganic species have been shown to be important for aerosol formation, there remains a large gap in our knowledge about the exact involvement of organics. We present a new quantum chemical procedure for screening relevant organics that for the first time allows us to obtain direct molecular-level insight into the organics involved in aerosol formation.
Aerosol formation is an important process for our global climate. While inorganic species have...
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