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1. The impact of ammonia on particle formation in the Asian Tropopause Aerosol Layer

Author

Christos Xenofontos, Matthias Kohl, Samuel Ruhl, João Almeida, Hannah M. Beckmann, Lucía Caudillo-Plath, Sebastian Ehrhart, Kristina Höhler, Milin Kaniyodical Sebastian, Weimeng Kong, Felix Kunkler, Antti Onnela, Pedro Rato, Douglas M. Russell, Mario Simon, Leander Stark, Nsikanabasi Silas Umo, Gabriela R. Unfer, Boxing Yang, Wenjuan Yu, Marcel Zauner-Wieczorek, Imad Zgheib, Zhensen Zheng, Joachim Curtius, Neil M. Donahue, Imad El Haddad, Richard C. Flagan, Hamish Gordon, Hartwig Harder, Xu-Cheng He, Jasper Kirkby, Markku Kulmala, Ottmar Möhler, Mira L. Pöhlker, Siegfried Schobesberger, Rainer Volkamer, Mingyi Wang, Stephan Borrmann, Andrea Pozzer, Jos Lelieveld, and Theodoros Christoudias

Subjects
Environmental sciences, GE1-350, Meteorology. Climatology, QC851-999
Abstract

Abstract During summer, ammonia emissions in Southeast Asia influence air pollution and cloud formation. Convective transport by the South Asian monsoon carries these pollutant air masses into the upper troposphere and lower stratosphere (UTLS), where they accumulate under anticyclonic flow conditions. This air mass accumulation is thought to contribute to particle formation and the development of the Asian Tropopause Aerosol Layer (ATAL). Despite the known influence of ammonia and particulate ammonium on air pollution, a comprehensive understanding of the ATAL is lacking. In this modelling study, the influence of ammonia on particle formation is assessed with emphasis on the ATAL. We use the EMAC chemistry-climate model, incorporating new particle formation parameterisations derived from experiments at the CERN CLOUD chamber. Our diurnal cycle analysis confirms that new particle formation mainly occurs during daylight, with a 10-fold enhancement in rate. This increase is prominent in the South Asian monsoon UTLS, where deep convection introduces high ammonia levels from the boundary layer, compared to a baseline scenario without ammonia. Our model simulations reveal that this ammonia-driven particle formation and growth contributes to an increase of up to 80% in cloud condensation nuclei (CCN) concentrations at cloud-forming heights in the South Asian monsoon region. We find that ammonia profoundly influences the aerosol mass and composition in the ATAL through particle growth, as indicated by an order of magnitude increase in nitrate levels linked to ammonia emissions. However, the effect of ammonia-driven new particle formation on aerosol mass in the ATAL is relatively small. Ammonia emissions enhance the regional aerosol optical depth (AOD) for shortwave solar radiation by up to 70%. We conclude that ammonia has a pronounced effect on the ATAL development, composition, the regional AOD, and CCN concentrations.

Published
2024
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2. Survival of newly formed particles in haze conditions

Author

Ruby Marten, Mao Xiao, Birte Rörup, Mingyi Wang, Weimeng Kong, Xu-Cheng He, Dominik Stolzenburg, Joschka Pfeifer, Guillaume Marie, Dongyu S. Wang, Wiebke Scholz, Andrea Baccarini, Chuan Ping Lee, Antonio Amorim, Rima Baalbaki, David M. Bell, Barbara Bertozzi, Lucía Caudillo, Biwu Chu, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Loïc Gonzalez Carracedo, Manuel Granzin, Armin Hansel, Martin Heinritzi, Victoria Hofbauer, Deniz Kemppainen, Andreas Kürten, Markus Lampimäki, Katrianne Lehtipalo, Vladimir Makhmutov, Hanna E. Manninen, Bernhard Mentler, Tuukka Petäjä, Maxim Philippov, Jiali Shen, Mario Simon, Yuri Stozhkov, António Tomé, Andrea C. Wagner, Yonghong Wang, Stefan K. Weber, Yusheng Wu, Marcel Zauner-Wieczorek, Joachim Curtius, Markku Kulmala, Ottmar Möhler, Rainer Volkamer, Paul M. Winkler, Douglas R. Worsnop, Josef Dommen, Richard C. Flagan, Jasper Kirkby, Neil M. Donahue, Houssni Lamkaddam, Urs Baltensperger, and Imad El Haddad

Published
2022
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3. Molecular Understanding of the Enhancement in Organic Aerosol Mass at High Relative Humidity

Author

Mihnea Surdu, Houssni Lamkaddam, Dongyu S. Wang, David M. Bell, Mao Xiao, Chuan Ping Lee, Dandan Li, Lucía Caudillo, Guillaume Marie, Wiebke Scholz, Mingyi Wang, Brandon Lopez, Ana A. Piedehierro, Farnoush Ataei, Rima Baalbaki, Barbara Bertozzi, Pia Bogert, Zoé Brasseur, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Xu-Cheng He, Kristina Höhler, Kimmo Korhonen, Jordan E. Krechmer, Katrianne Lehtipalo, Naser G. A. Mahfouz, Hanna E. Manninen, Ruby Marten, Dario Massabò, Roy Mauldin, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Birte Rörup, Mario Simon, Jiali Shen, Nsikanabasi Silas Umo, Franziska Vogel, Stefan K. Weber, Marcel Zauner-Wieczorek, Rainer Volkamer, Harald Saathoff, Ottmar Möhler, Jasper Kirkby, Douglas R. Worsnop, Markku Kulmala, Frank Stratmann, Armin Hansel, Joachim Curtius, André Welti, Matthieu Riva, Neil M. Donahue, Urs Baltensperger, and Imad El Haddad

Subjects
Environmental Chemistry, General Chemistry
Published
2023
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4. High Gas-Phase Methanesulfonic Acid Production in the OH-Initiated Oxidation of Dimethyl Sulfide at Low Temperatures

Author

Jiali Shen, Wiebke Scholz, Xu-Cheng He, Putian Zhou, Guillaume Marie, Mingyi Wang, Ruby Marten, Mihnea Surdu, Birte Rörup, Rima Baalbaki, Antonio Amorim, Farnoush Ataei, David M. Bell, Barbara Bertozzi, Zoé Brasseur, Lucía Caudillo, Dexian Chen, Biwu Chu, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Manuel Granzin, Roberto Guida, Martin Heinritzi, Victoria Hofbauer, Siddharth Iyer, Deniz Kemppainen, Weimeng Kong, Jordan E. Krechmer, Andreas Kürten, Houssni Lamkaddam, Chuan Ping Lee, Brandon Lopez, Naser G. A. Mahfouz, Hanna E. Manninen, Dario Massabò, Roy L. Mauldin, Bernhard Mentler, Tatjana Müller, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Pontus Roldin, Siegfried Schobesberger, Mario Simon, Dominik Stolzenburg, Yee Jun Tham, António Tomé, Nsikanabasi Silas Umo, Dongyu Wang, Yonghong Wang, Stefan K. Weber, André Welti, Robin Wollesen de Jonge, Yusheng Wu, Marcel Zauner-Wieczorek, Felix Zust, Urs Baltensperger, Joachim Curtius, Richard C. Flagan, Armin Hansel, Ottmar Möhler, Tuukka Petäjä, Rainer Volkamer, Markku Kulmala, Katrianne Lehtipalo, Matti Rissanen, Jasper Kirkby, Imad El-Haddad, Federico Bianchi, Mikko Sipilä, Neil M. Donahue, Douglas R. Worsnop, Institute for Atmospheric and Earth System Research (INAR), Polar and arctic atmospheric research (PANDA), INAR Physics, Helsinki Institute of Physics, Tampere University, and Physics

Subjects
Astrophysics and Astronomy, OH-initiated oxidation, methanesulfinic acid (CH3S(O)OH, MSIA), Low temperatures, Environmental Chemistry, General Chemistry, methanesulfonic acid (MSA), dimethyl sulfide (DMS), 114 Physical sciences
Abstract

Dimethyl sulfide (DMS) influences climate via cloud condensation nuclei (CCN) formation resulting from its oxidation products (mainly methanesulfonic acid, MSA, and sulfuric acid, H2SO4). Despite their importance, accurate prediction of MSA and H2SO4from DMS oxidation remains challenging. With comprehensive experiments carried out in the Cosmics Leaving Outdoor Droplets (CLOUD) chamber at CERN, we show that decreasing the temperature from +25 to -10 °C enhances the gas-phase MSA production by an order of magnitude from OH-initiated DMS oxidation, while H2SO4production is modestly affected. This leads to a gas-phase H2SO4-to-MSA ratio (H2SO4/MSA) smaller than one at low temperatures, consistent with field observations in polar regions. With an updated DMS oxidation mechanism, we find that methanesulfinic acid, CH3S(O)OH, MSIA, forms large amounts of MSA. Overall, our results reveal that MSA yields are a factor of 2-10 higher than those predicted by the widely used Master Chemical Mechanism (MCMv3.3.1), and the NOxeffect is less significant than that of temperature. Our updated mechanism explains the high MSA production rates observed in field observations, especially at low temperatures, thus, substantiating the greater importance of MSA in the natural sulfur cycle and natural CCN formation. Our mechanism will improve the interpretation of present-day and historical gas-phase H2SO4/MSA measurements. publishedVersion

Published
2022
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5. Nitrate radicals suppress biogenic new particle formation from monoterpene oxidation

Author

Dandan Li, Wei Huang, Dongyu Wang, Mingyi Wang, Joel Thornton, Lucía Caudillo, Birte Rörup, Ruby Marten, Wiebke Scholz, Henning Finkenzeller, Guillaume Marie, David Bell, Zoé Brasseur, Joachim Curtius, Lubna Dada, Jonathan Duplissy, Xianda Gong, Armin Hansel, Xu-cheng He, Victoria Hofbauer, Heikki Junninen, Jordan E. Krechmer, Andreas Kurten, Houssni Lamkaddam, Katrianne LEHTIPALO, Brandon Lopez, Yingge Ma, Naser Mahfouz, Hanna E. Manninen, Bernhard Mentler, Sebastien Perrier, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Meredith Schervish, Siegfried Schobesberger, Jiali Shen, Mihnea Surdu, Sophie Tomaz, Rainer Volkamer, Xinke Wang, Stefan Weber, André Welti, Douglas Worsnop, yusheng wu, Chao Yan, Marcel Zauner-Wieczorek, Markku Kulmala, Jasper Kirkby, Neil Donahue, Christian George, Imad El-Haddad, Federico Bianchi, and Matthieu Riva

Abstract

Highly oxygenated organic molecules (HOMs) are a major source of new particles affecting Earth’s climate1,2. HOM production from the oxidation of volatile organic compounds (VOCs) occurs during both day and night, and can lead to new particle formation (NPF)3,4. However, NPF involving organic vapors has been reported much more often during daytime3-6 than during nighttime7,8. Here, we show that the nitrate radicals (NO3) - which arise predominantly at night – inhibit NPF during the oxidation of monoterpenes based on three lines of observational evidence: NPF experiments in the CLOUD chamber at CERN; radical chemistry experiments using an oxidation flow reactor; and field observations in a wetland that occasionally exhibits nocturnal NPF. Nitrooxy-peroxy radicals formed from NO3 chemistry suppress the production of ultra-low volatility organic compounds (ULVOCs) responsible for biogenic NPF, which are covalently bound RO2 dimer association products. The ULVOC yield of α-pinene in the presence of NO3 is one-fifth of that resulting from ozone chemistry alone. Even trace amounts of NO3 radicals, at sub parts per trillion level, suppress the NPF rate by a factor of 4. Ambient observations further confirm that when NO3 chemistry is involved, monoterpene NPF is completely turned off. Our results explain the frequent absence of nocturnal biogenic NPF in monoterpene-rich environments.

Published
2023
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6. An intercomparison study of four different techniques for measuring the chemical composition of nanoparticles

Author

Lucía Caudillo, Mihnea Surdu, Brandon Lopez, Mingyi Wang, Markus Thoma, Steffen Bräkling, Angela Buchholz, Mario Simon, Andrea C. Wagner, Tatjana Müller, Manuel Granzin, Martin Heinritzi, Antonio Amorim, David M. Bell, Zoé Brasseur, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Xu-Cheng He, Houssni Lamkaddam, Naser G. A. Mahfouz, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Roy L. Mauldin, Bernhard Mentler, Antti Onnela, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Birte Rörup, Wiebke Scholz, Jiali Shen, Dominik Stolzenburg, Christian Tauber, Ping Tian, António Tomé, Nsikanabasi Silas Umo, Dongyu S. Wang, Yonghong Wang, Stefan K. Weber, André Welti, Marcel Zauner-Wieczorek, Urs Baltensperger, Richard C. Flagan, Armin Hansel, Jasper Kirkby, Markku Kulmala, Katrianne Lehtipalo, Douglas R. Worsnop, Imad El Haddad, Neil M. Donahue, Alexander L. Vogel, Andreas Kürten, and Joachim Curtius

Subjects
Earth sciences, ddc:550
Abstract

Currently, the complete chemical characterization of nanoparticles (< 100 nm) represents an analytical challenge, since these particles are abundant in number but have negligible mass. Several methods for particle-phase characterization have been recently developed to better detect and infer more accurately the sources and fates of sub-100 nm particles, but a detailed comparison of different approaches is missing. Here we report on the chemical composition of secondary organic aerosol (SOA) nanoparticles from experimental studies of α-pinene ozonolysis at −50, −30, and −10 ∘C and intercompare the results measured by different techniques. The experiments were performed at the Cosmics Leaving OUtdoor Droplets (CLOUD) chamber at the European Organization for Nuclear Research (CERN). The chemical composition was measured simultaneously by four different techniques: (1) thermal desorption–differential mobility analyzer (TD–DMA) coupled to a NO3- chemical ionization–atmospheric-pressure-interface–time-of-flight (CI–APi–TOF) mass spectrometer, (2) filter inlet for gases and aerosols (FIGAERO) coupled to an I− high-resolution time-of-flight chemical ionization mass spectrometer (HRToF-CIMS), (3) extractive electrospray Na+ ionization time-of-flight mass spectrometer (EESI-TOF), and (4) offline analysis of filters (FILTER) using ultra-high-performance liquid chromatography (UHPLC) and heated electrospray ionization (HESI) coupled to an Orbitrap high-resolution mass spectrometer (HRMS). Intercomparison was performed by contrasting the observed chemical composition as a function of oxidation state and carbon number, by estimating the volatility and comparing the fraction of volatility classes, and by comparing the thermal desorption behavior (for the thermal desorption techniques: TD–DMA and FIGAERO) and performing positive matrix factorization (PMF) analysis for the thermograms. We found that the methods generally agree on the most important compounds that are found in the nanoparticles. However, they do see different parts of the organic spectrum. We suggest potential explanations for these differences: thermal decomposition, aging, sampling artifacts, etc. We applied PMF analysis and found insights of thermal decomposition in the TD–DMA and the FIGAERO.

Published
2023
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7. Supplementary material to 'Measurement of the rate coefficients between atmospheric ions and multiply charged aerosol particles in the CERN CLOUD chamber'

Author

Joschka Pfeifer, Naser G. Mahfouz, Ben Schulze, Serge Mathot, Dominik Stolzenburg, Rima Baalbaki, Zoé Brasseur, Lucia Caudillo, Lubna Dada, Manuel Granzin, Xu-Cheng He, Houssni Lamkaddam, Brandon Lopez, Vladimir Makhmutov, Ruby Marten, Bernhard Mentler, Tatjana Müller, Antti Onnela, Maxim Philippov, Ana A. Piedehierro, Birte Rörup, Meredith Schervish, Ping Tian, Nsikanabasi S. Umo, Dongyu S. Wang, Mingyi Wang, Stefan K. Weber, André Welti, Yusheng Wu, Marcel Zauner-Wieczorek, Antonio Amorim, Imad El Haddad, Markku Kulmala, Katrianne Lehtipalo, Tuukka Petäjä, António Tomé, Sander Mirme, Hanna E. Manninen, Neil M. Donahue, Richard C. Flagan, Andreas Kürten, Joachim Curtius, and Jasper Kirkby

Published
2022
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8. The gas-phase formation mechanism of iodic acid as an atmospheric aerosol source

Author

Henning Finkenzeller, Siddharth Iyer, Xu-Cheng He, Mario Simon, Theodore K. Koenig, Christopher F. Lee, Rashid Valiev, Victoria Hofbauer, Antonio Amorim, Rima Baalbaki, Andrea Baccarini, Lisa Beck, David M. Bell, Lucía Caudillo, Dexian Chen, Randall Chiu, Biwu Chu, Lubna Dada, Jonathan Duplissy, Martin Heinritzi, Deniz Kemppainen, Changhyuk Kim, Jordan Krechmer, Andreas Kürten, Alexandr Kvashnin, Houssni Lamkaddam, Chuan Ping Lee, Katrianne Lehtipalo, Zijun Li, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Roy L. Mauldin, Bernhard Mentler, Tatjana Müller, Tuukka Petäjä, Maxim Philippov, Ananth Ranjithkumar, Birte Rörup, Jiali Shen, Dominik Stolzenburg, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Dongyu S. Wang, Mingyi Wang, Yonghong Wang, Stefan K. Weber, Wei Nie, Yusheng Wu, Mao Xiao, Qing Ye, Marcel Zauner-Wieczorek, Armin Hansel, Urs Baltensperger, Jérome Brioude, Joachim Curtius, Neil M. Donahue, Imad El Haddad, Richard C. Flagan, Markku Kulmala, Jasper Kirkby, Mikko Sipilä, Douglas R. Worsnop, Theo Kurten, Matti Rissanen, Rainer Volkamer, Tampere University, Physics, Department of Chemistry, INAR Physical Chemistry, Institute for Atmospheric and Earth System Research (INAR), Polar and arctic atmospheric research (PANDA), INAR Physics, Air quality research group, and Helsinki Institute of Physics

Subjects
particle formation, General Chemical Engineering, nucleation, 116 Chemical sciences, emissions, General Chemistry, chemistry, ammonia, 114 Physical sciences, sulfuric-acid, in-situ, methanesulfonic-acid, impacts, Chemical Physics and Chemistry, sea-surface
Abstract

Iodine is a reactive trace element in atmospheric chemistry that destroys ozone and nucleates particles. Iodine emissions have tripled since 1950 and are projected to keep increasing with rising O3 surface concentrations. Although iodic acid (HIO3) is widespread and forms particles more efficiently than sulfuric acid, its gas-phase formation mechanism remains unresolved. Here, in CLOUD atmospheric simulation chamber experiments that generate iodine radicals at atmospherically relevant rates, we show that iodooxy hypoiodite, IOIO, is efficiently converted into HIO3 via reactions (R1) IOIO + O3 → IOIO4 and (R2) IOIO4 + H2O → HIO3 + HOI + (1)O2. The laboratory-derived reaction rate coefficients are corroborated by theory and shown to explain field observations of daytime HIO3 in the remote lower free troposphere. The mechanism provides a missing link between iodine sources and particle formation. Because particulate iodate is readily reduced, recycling iodine back into the gas phase, our results suggest a catalytic role of iodine in aerosol formation.

Published
2022

9. Supplementary material to 'An intercomparison study of four different techniques for measuring the chemical composition of nanoparticles'

Author

Lucía Caudillo, Mihnea Surdu, Brandon Lopez, Mingyi Wang, Markus Thoma, Steffen Bräkling, Angela Buchholz, Mario Simon, Andrea C. Wagner, Tatjana Müller, Manuel Granzin, Martin Heinritzi, Antonio Amorim, David M. Bell, Zoé Brasseur, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Xu-Cheng He, Houssni Lamkaddam, Naser G. A. Mahfouz, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Roy L. Mauldin, Bernhard Mentler, Antti Onnela, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Birte Rörup, Wiebke Scholz, Jiali Shen, Dominik Stolzenburg, Christian Tauber, Ping Tian, António Tomé, Nsikanabasi Silas Umo, Dongyu S. Wang, Yonghong Wang, Stefan K. Weber, André Welti, Marcel Zauner-Wieczorek, Urs Baltensperger, Richard C. Flagan, Armin Hansel, Jasper Kirkby, Markku Kulmala, Katrianne Lehtipalo, Douglas R. Worsnop, Imad El Haddad, Neil M. Donahue, Alexander L. Vogel, Andreas Kürten, and Joachim Curtius

Published
2022
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11. Rapid growth of new atmospheric particles by nitric acid and ammonia condensation

Author

Armin Hansel, Dominik Stolzenburg, António Tomé, Jonathan Duplissy, Rainer Volkamer, Richard C. Flagan, Jasper Kirkby, Jordan E. Krechmer, Dongyu S. Wang, Jenni Kontkanen, Yusheng Wu, Stavros Amanatidis, Roberto Guida, Wiebke Scholz, Stefan K. Weber, Mikko Sipilä, Houssni Lamkaddam, Douglas R. Worsnop, Chuan Ping Lee, Steffen Bräkling, Andrea C. Wagner, Barbara Bertozzi, Arto Heitto, Taina Yli-Juuti, Lucía Caudillo Murillo, Mario Simon, Andrea Baccarini, Bernhard Mentler, Peter Josef Wlasits, Xueqin Zhou, Neil M. Donahue, Imad El-Haddad, Gerhard Steiner, Joschka Pfeifer, Joachim Curtius, Ilona Riipinen, Andreas Kürten, Paul M. Winkler, Markku Kulmala, Randall Chiu, T. Müller, Qing Ye, Mao Xiao, Jiali Shen, Guillaume Marie, Antti Onnela, Birte Rörup, Eva Partoll, António Amorim, Ruby Marten, Hanna E. Manninen, John H. Seinfeld, Ananth Ranjithkumar, Louis Philippe De Menezes, Serge Mathot, Marcel Zauner-Wieczorek, Roy L. Mauldin, Weimeng Kong, Markus Lampimäki, Loic Gonzalez Carracedo, Urs Baltensperger, Biwu Chu, Mingyi Wang, Yonghong Wang, Josef Dommen, Dexian Chen, Matti P. Rissanen, Sophia Brilke, Victoria Hofbauer, Rima Baalbaki, Vladimir Makhmutov, Katrianne Lehtipalo, Henning Finkenzeller, Xu-Cheng He, Lubna Dada, Veronika Pospisilova, Yee Jun Tham, Manuel Granzin, Tuukka Petäjä, David M. Bell, M. V. Philippov, Tampere University, Physics, INAR Physics, Air quality research group, Institute for Atmospheric and Earth System Research (INAR), Helsinki Institute of Physics, Polar and arctic atmospheric research (PANDA), Staff Services, and Department of Physics

Subjects
010504 meteorology & atmospheric sciences, Nucleation, 010501 environmental sciences, 01 natural sciences, 114 Physical sciences, Article, chemistry.chemical_compound, Ammonia, Nitric acid, medicine, ddc:550, Atmospheric science, Climate change, Scavenging, 0105 earth and related environmental sciences, Range (particle radiation), Multidisciplinary, Condensation, Sulfuric acid, medicine.disease, Earth sciences, chemistry, Chemical engineering, 13. Climate action, Vapours
Abstract

A list of authors and their affiliations appears at the end of the paper New-particle formation is a major contributor to urban smog1,2, but how it occurs in cities is often puzzling3. If the growth rates of urban particles are similar to those found in cleaner environments (1–10 nanometres per hour), then existing understanding suggests that new urban particles should be rapidly scavenged by the high concentration of pre-existing particles. Here we show, through experiments performed under atmospheric conditions in the CLOUD chamber at CERN, that below about +5 degrees Celsius, nitric acid and ammonia vapours can condense onto freshly nucleated particles as small as a few nanometres in diameter. Moreover, when it is cold enough (below −15 degrees Celsius), nitric acid and ammonia can nucleate directly through an acid–base stabilization mechanism to form ammonium nitrate particles. Given that these vapours are often one thousand times more abundant than sulfuric acid, the resulting particle growth rates can be extremely high, reaching well above 100 nanometres per hour. However, these high growth rates require the gas-particle ammonium nitrate system to be out of equilibrium in order to sustain gas-phase supersaturations. In view of the strong temperature dependence that we measure for the gas-phase supersaturations, we expect such transient conditions to occur in inhomogeneous urban settings, especially in wintertime, driven by vertical mixing and by strong local sources such as traffic. Even though rapid growth from nitric acid and ammonia condensation may last for only a few minutes, it is nonetheless fast enough to shepherd freshly nucleated particles through the smallest size range where they are most vulnerable to scavenging loss, thus greatly increasing their survival probability. We also expect nitric acid and ammonia nucleation and rapid growth to be important in the relatively clean and cold upper free troposphere, where ammonia can be convected from the continental boundary layer and nitric acid is abundant from electrical storms4,5., Measurements in the CLOUD chamber at CERN show that the rapid condensation of ammonia and nitric acid vapours could be important for the formation and survival of new particles in wintertime urban conditions, contributing to urban smog.

Published
2020

12. Mass spectrometric measurements of ambient ions and estimation of gaseous sulfuric acid in the free troposphere and lowermost stratosphere during the CAFE-EU/BLUESKY campaign

Author

Marcel Zauner-Wieczorek, Martin Heinritzi, Manuel Granzin, Timo Keber, Andreas Kürten, Katharina Kaiser, Johannes Schneider, and Joachim Curtius

Abstract

Ambient ions play an important role in atmospheric processes such as ion-induced new particle formation. While there are several studies of ambient ions for different layers of the atmosphere, data coverage for the free troposphere and especially the upper troposphere and lower stratosphere (UTLS) region is scarce. Here, we present the first airborne measurements of ambient ions using a high-resolution atmospheric pressure interface time-of-flight mass spectrometer (HR-APi-TOF-MS) in the free troposphere and lower stratosphere above Europe on board the HALO aircraft during the CAFE-EU/BLUESKY campaign in May and June 2020. In negative measurement mode, we observed nitrate and hydrogen sulfate and their related ion clusters in an altitude range of 4.7 to 13.4 km. The horizontal profiles for those ions reveal an increasing count rate for NO3- and (HNO3)NO3- towards higher altitudes but no significant trend for HSO4−. From the count rates of the nitrate (NO3-) and hydrogen sulfate (HSO4-) core ions, we inferred the number concentration of gaseous sulfuric acid. The lowest average value was found to be 1.9×105 cm−3 at the maximum altitude bin, i.e. 13.4 km. The highest average value of 7.8×105 cm−3 was observed in the 8.7–9.2 km altitude bin. During the transit through a mixed-phase cloud, we observed an event of enhanced ion count rates and aerosol particle concentrations that can largely be assigned to nitrate ions and particles, respectively; this may have been caused by the shattering of liquid cloud droplets on the surface of the aircraft or the inlet. Furthermore, we report the proof of principle for the measurement of ambient cations and the identification of protonated pyridine.

Published
2022
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13. Chemical composition of nanoparticles from alpha-pinene nucleation and the influence of isoprene and relative humidity at low temperature

Author

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, Joachim Curtius, Institute for Atmospheric and Earth System Research (INAR), INAR Physics, Helsinki Institute of Physics, and Polar and arctic atmospheric research (PANDA)

Subjects
Earth sciences, 13. Climate action, ddc:550, 114 Physical sciences
Abstract

Biogenic organic precursors play an important role in atmospheric new particle formation (NPF). One of the major precursor species is α-pinene, which upon oxidation can form a suite of products covering a wide range of volatilities. Highly oxygenated organic molecules (HOMs) comprise a fraction of the oxidation products formed. While it is known that HOMs contribute to secondary organic aerosol (SOA) formation, including NPF, they have not been well studied in newly formed particles due to their very low mass concentrations. Here we present gas- and particle-phase chemical composition data from experimental studies of α-pinene oxidation, including in the presence of isoprene, at temperatures (−50 and −30 ∘C) and relative humidities (20 % and 60 %) relevant in the upper free troposphere. The measurements took place at the CERN Cosmics Leaving Outdoor Droplets (CLOUD) chamber. The particle chemical composition was analyzed by a thermal desorption differential mobility analyzer (TD-DMA) coupled to a nitrate chemical ionization–atmospheric pressure interface–time-of-flight (CI-APi-TOF) mass spectrometer. CI-APi-TOF was used for particle- and gas-phase measurements, applying the same ionization and detection scheme. Our measurements revealed the presence of C8−10 monomers and C18−20 dimers as the major compounds in the particles (diameter up to ∼ 100 nm). Particularly, for the system with isoprene added, C5 (C5H10O5−7) and C15 compounds (C15H24O5−10) were detected. This observation is consistent with the previously observed formation of such compounds in the gas phase. However, although the C5 and C15 compounds do not easily nucleate, our measurements indicate that they can still contribute to the particle growth at free tropospheric conditions. For the experiments reported here, most likely isoprene oxidation products enhance the growth of particles larger than 15 nm. Additionally, we report on the nucleation rates measured at 1.7 nm (J1.7 nm) and compared with previous studies, we found lower J1.7 nm values, very likely due to the higher α-pinene and ozone mixing ratios used in the present study.

Published
2021

14. The ion-ion recombination coefficient α: Comparison of temperature- and pressure-dependent parameterisations for the troposphere and lower stratosphere

Author

Andreas Kürten, Marcel Zauner-Wieczorek, and Joachim Curtius

Subjects
Atmosphere, Physics, Troposphere, Work (thermodynamics), Altitude, Field (physics), Stratosphere, Recombination, Ion, Computational physics
Abstract

Many different atmospheric, physical and chemical processes are affected by ions. An important sink for atmospheric ions is the reaction and mutual neutralisation of a positive and a negative ion, also called ion-ion recombination. While the value for the ion-ion recombination coefficient α is well known for standard conditions (namely 1.7 · 10–6 cm3 s–1), it needs to be calculated for deviating temperature and pressure conditions, especially for applications in higher altitudes of the atmosphere. In this work, we review the history of theories and parameterisations of the ion-ion recombination coefficient, focussing on the temperature and pressure dependencies and on the altitude range between 0 and 20 km. Starting from theories based on J. J. Thomson’s work, we describe important semi-empirical adjustments as well as field, model and laboratory data sets, followed by a short review of physical theories that take the microscopic processes during recombination into account, including a molecular dynamics approach. We present a comparison between all theories, parameterisations, field, model, and laboratory data sets to conclude on a favourable parameterisation. While many theories agree well with field data above approx. 10 km altitude, the nature of the recombination coefficient is still widely unknown between Earth’s surface and an altitude of 10 km. According to the current state of knowledge, it appears most reasonable to assume a constant value for the recombination coefficient for this region, while we recommend using a parameterisation for altitudes above 10 km. Overall, the parameterisation of Brasseur and Chatel (1983) shows the most convincing results. The need for future research, be it in the laboratory or by means of modelling, is identified.

Published
2021

15. Synergistic HNO

Author

Mingyi, Wang, Mao, Xiao, Barbara, Bertozzi, Guillaume, Marie, Birte, Rörup, Benjamin, Schulze, Roman, Bardakov, Xu-Cheng, He, Jiali, Shen, Wiebke, Scholz, Ruby, Marten, Lubna, Dada, Rima, Baalbaki, Brandon, Lopez, Houssni, Lamkaddam, Hanna E, Manninen, António, Amorim, Farnoush, Ataei, Pia, Bogert, Zoé, Brasseur, Lucía, Caudillo, Louis-Philippe, De Menezes, Jonathan, Duplissy, Annica M L, Ekman, Henning, Finkenzeller, Loïc Gonzalez, Carracedo, Manuel, Granzin, Roberto, Guida, Martin, Heinritzi, Victoria, Hofbauer, Kristina, Höhler, Kimmo, Korhonen, Jordan E, Krechmer, Andreas, Kürten, Katrianne, Lehtipalo, Naser G A, Mahfouz, Vladimir, Makhmutov, Dario, Massabò, Serge, Mathot, Roy L, Mauldin, Bernhard, Mentler, Tatjana, Müller, Antti, Onnela, Tuukka, Petäjä, Maxim, Philippov, Ana A, Piedehierro, Andrea, Pozzer, Ananth, Ranjithkumar, Meredith, Schervish, Siegfried, Schobesberger, Mario, Simon, Yuri, Stozhkov, António, Tomé, Nsikanabasi Silas, Umo, Franziska, Vogel, Robert, Wagner, Dongyu S, Wang, Stefan K, Weber, André, Welti, Yusheng, Wu, Marcel, Zauner-Wieczorek, Mikko, Sipilä, Paul M, Winkler, Armin, Hansel, Urs, Baltensperger, Markku, Kulmala, Richard C, Flagan, Joachim, Curtius, Ilona, Riipinen, Hamish, Gordon, Jos, Lelieveld, Imad, El-Haddad, Rainer, Volkamer, Douglas R, Worsnop, Theodoros, Christoudias, Jasper, Kirkby, Ottmar, Möhler, and Neil M, Donahue

Abstract

New particle formation in the upper free troposphere is a major global source of cloud condensation nuclei (CCN)

Published
2021

16. Supplementary material to 'Chemical composition of nanoparticles from α-pinene nucleation and the influence of isoprene and relative humidity at low temperature'

Author

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

Published
2021
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17. Molecular understanding of new-particle formation from alpha-pinene between −50 °C and 25 °C

Author

Mario Simon, Lubna Dada, Martin Heinritzi, Wiebke Scholz, Dominik Stolzenburg, Lukas Fischer, Andrea C. Wagner, Andreas Kürten, Birte Rörup, Xu-Cheng He, João Almeida, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Lisa Beck, Anton Bergen, Federico Bianchi, Steffen Bräkling, Sophia Brilke, Lucia Caudillo, Dexian Chen, Biwu Chu, António Dias, Danielle C. Draper, Jonathan Duplissy, Imad El Haddad, Henning Finkenzeller, Carla Frege, Loic Gonzalez-Carracedo, Hamish Gordon, Manuel Granzin, Jani Hakala, Victoria Hofbauer, Christopher R. Hoyle, Changhyuk Kim, Weimeng Kong, Houssni Lamkaddam, Chuan P. Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Bernhard Mentler, Ugo Molteni, Leonid Nichman, Wei Nie, Andrea Ojdanic, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Lauriane L. J. Quéléver, Ananth Ranjithkumar, Matti Rissanen, Simon Schallhart, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee J. Tham, António R. Tomé, Miguel Vazquez-Pufleau, Alexander Vogel, Robert Wagner, Mingyi Wang, Dongyu S. Wang, Yonghong Wang, Stefan K. Weber, Yusheng Wu, Mao Xiao, Chao Yan, Penglin Ye, Qing Ye, Marcel Zauner-Wieczorek, Xueqin Zhou, Urs Baltensperger, Josef Dommen, Rick C. Flagan, Armin Hansel, Markku Kulmala, Rainer Volkamer, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius

Subjects
0301 basic medicine, 03 medical and health sciences, 030104 developmental biology, 13. Climate action
Abstract

Highly-oxygenated organic molecules (HOMs) contribute substantially to the formation and growth of atmospheric aerosol particles, which affect air quality, human health and Earth's climate. HOMs are formed by rapid, gas-phase autoxidation of volatile organic compounds (VOCs) such as α-pinene, the most abundant monoterpene in the atmosphere. Due to their abundance and low volatility, HOMs can play an important role for new-particle formation (NPF) and the early growth of atmospheric aerosols, even without any further assistance of other low-volatility compounds such as sulfuric acid. Both the autoxidation reaction forming HOMs and their new-particle formation rates are expected to be strongly dependent on temperature. However, experimental data on both effects are limited. Dedicated experiments were performed at the CLOUD (Cosmics Leaving OUtdoor Droplets) chamber at CERN to address this question. In this study, we show that a decrease in temperature (from +25 to −50 °C) results in a reduced HOM yield and reduced oxidation state of the products, whereas the new-particle formation rates (J1.7 nm) increase substantially. Measurements with two different chemical ionization mass spectrometers (using nitrate and protonated water as reagent ion, respectively) provide the molecular composition of the gaseous oxidation products and a 2-dimensional volatility basis set model (2D-VBS) provides their volatility distribution. The HOM yield decreases with temperature from 6.2 % at 25 °C to 0.7 % at −50 °C. However, there is a strong reduction of the saturation vapor pressure of each oxidation state as the temperature is reduced. Overall, the reduction in volatility with temperature leads to an increase in the nucleation rates by up to three orders of magnitude at −50 °C compared with 25 °C. In addition, the enhancement of the nucleation rates by ions decreases with decreasing temperature, since the neutral molecular clusters have increased stability against evaporation. The resulting data quantify how the interplay between the temperature-dependent oxidation pathways and the associated vapor pressures affect biogenic new-particle formation at the molecular level. Our measurements therefore improve our understanding of pure biogenic new-particle formation for a wide range of tropospheric temperatures and precursor concentrations.

Published
2020
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18. Supplementary material to 'Molecular understanding of new-particle formation from alpha-pinene between −50 °C and 25 °C'

Author

Mario Simon, Lubna Dada, Martin Heinritzi, Wiebke Scholz, Dominik Stolzenburg, Lukas Fischer, Andrea C. Wagner, Andreas Kürten, Birte Rörup, Xu-Cheng He, João Almeida, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Lisa Beck, Anton Bergen, Federico Bianchi, Steffen Bräkling, Sophia Brilke, Lucia Caudillo, Dexian Chen, Biwu Chu, António Dias, Danielle C. Draper, Jonathan Duplissy, Imad El Haddad, Henning Finkenzeller, Carla Frege, Loic Gonzalez-Carracedo, Hamish Gordon, Manuel Granzin, Jani Hakala, Victoria Hofbauer, Christopher R. Hoyle, Changhyuk Kim, Weimeng Kong, Houssni Lamkaddam, Chuan P. Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Bernhard Mentler, Ugo Molteni, Leonid Nichman, Wei Nie, Andrea Ojdanic, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Lauriane L. J. Quéléver, Ananth Ranjithkumar, Matti Rissanen, Simon Schallhart, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee J. Tham, António R. Tomé, Miguel Vazquez-Pufleau, Alexander Vogel, Robert Wagner, Mingyi Wang, Dongyu S. Wang, Yonghong Wang, Stefan K. Weber, Yusheng Wu, Mao Xiao, Chao Yan, Penglin Ye, Qing Ye, Marcel Zauner-Wieczorek, Xueqin Zhou, Urs Baltensperger, Josef Dommen, Rick C. Flagan, Armin Hansel, Markku Kulmala, Rainer Volkamer, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius

Published
2020
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19. Enhanced growth rate of atmospheric particles from sulfuric acid

Author

Dominik Stolzenburg, Mario Simon, Ananth Ranjithkumar, Andreas Kürten, Katrianne Lehtipalo, Hamish Gordon, Tuomo Nieminen, Lukas Pichelstorfer, Xu-Cheng He, Sophia Brilke, Mao Xiao, António Amorim, Rima Baalbaki, Andrea Baccarini, Lisa Beck, Steffen Bräkling, Lucía Caudillo Murillo, Dexian Chen, Biwu Chu, Lubna Dada, António Dias, Josef Dommen, Jonathan Duplissy, Imad El Haddad, Henning Finkenzeller, Lukas Fischer, Loic Gonzalez Carracedo, Martin Heinritzi, Changhyuk Kim, Theodore K. Koenig, Weimeng Kong, Houssni Lamkaddam, Chuan Ping Lee, Markus Leiminger, Zijun Li, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Tatjana Müller, Wei Nie, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Matti P. Rissanen, Birte Rörup, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Mingyi Wang, Yonghong Wang, Stefan K. Weber, Daniela Wimmer, Peter J. Wlasits, Yusheng Wu, Qing Ye, Marcel Zauner-Wieczorek, Urs Baltensperger, Kenneth S. Carslaw, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Armin Hansel, Markku Kulmala, Rainer Volkamer, Jasper Kirkby, and Paul M. Winkler

Subjects
inorganic chemicals, 010501 environmental sciences, 01 natural sciences, 0105 earth and related environmental sciences
Abstract

In the present-day atmosphere, sulfuric acid is the most important vapour for aerosol particle formation and initial growth. However, the growth rates of nanoparticles (

Published
2019
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20. Supplementary material to 'Enhanced growth rate of atmospheric particles from sulfuric acid'

Author

Dominik Stolzenburg, Mario Simon, Ananth Ranjithkumar, Andreas Kürten, Katrianne Lehtipalo, Hamish Gordon, Tuomo Nieminen, Lukas Pichelstorfer, Xu-Cheng He, Sophia Brilke, Mao Xiao, António Amorim, Rima Baalbaki, Andrea Baccarini, Lisa Beck, Steffen Bräkling, Lucía Caudillo Murillo, Dexian Chen, Biwu Chu, Lubna Dada, António Dias, Josef Dommen, Jonathan Duplissy, Imad El Haddad, Henning Finkenzeller, Lukas Fischer, Loic Gonzalez Carracedo, Martin Heinritzi, Changhyuk Kim, Theodore K. Koenig, Weimeng Kong, Houssni Lamkaddam, Chuan Ping Lee, Markus Leiminger, Zijun Li, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Tatjana Müller, Wei Nie, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Matti P. Rissanen, Birte Rörup, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Mingyi Wang, Yonghong Wang, Stefan K. Weber, Daniela Wimmer, Peter J. Wlasits, Yusheng Wu, Qing Ye, Marcel Zauner-Wieczorek, Urs Baltensperger, Kenneth S. Carslaw, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Armin Hansel, Markku Kulmala, Rainer Volkamer, Jasper Kirkby, and Paul M. Winkler

Published
2019
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21. Molecular understanding of new-particle formation from α-pinene between −50 and +25 °C

Author

Houssni Lamkaddam, Manuel Granzin, Jani Hakala, Dexian Chen, Xu-Cheng He, Siegfried Schobesberger, Danielle C. Draper, Qing Ye, Neil M. Donahue, Lubna Dada, Antonio Dias, Guillaume Marie, Victoria Hofbauer, Matti P. Rissanen, Ugo Molteni, Christian Tauber, Gerhard Steiner, Eva Partoll, Alexander L. Vogel, Markus Leiminger, Antti Onnela, Joachim Curtius, Robert Wagner, Sophia Brilke, Mikko Sipilä, Lisa Beck, Chuan P. Lee, Wei Nie, Armin Hansel, Ananth Ranjithkumar, Imad El-Haddad, Xueqin Zhou, Urs Baltensperger, Dominik Stolzenburg, Paul M. Winkler, Joao Almeida, Yusheng Wu, Chao Yan, Stefan K. Weber, Rima Baalbaki, Lauriane L. J. Quéléver, Biwu Chu, Markku Kulmala, Rainer Volkamer, Simone Schuchmann, Marcel Zauner-Wieczorek, Birte Rörup, Simon Schallhart, Paulus Salomon Bauer, António Tomé, Wiebke Scholz, Mingyi Wang, Steffen Bräkling, Christopher R. Hoyle, Yonghong Wang, Anton Bergen, Mario Simon, Martin Heinritzi, Jiali Shen, Huajun Mai, Andreas Kürten, Andrea Baccarini, Bernhard Mentler, Loic Gonzalez-Carracedo, Richard C. Flagan, Douglas R. Worsnop, Miguel Vazquez-Pufleau, Jonathan Duplissy, Penglin Ye, Joschka Pfeifer, Lukas Fischer, Josef Dommen, Jasper Kirkby, Ruby Marten, Dongyu S. Wang, Andrea C. Wagner, Lucía Caudillo, Hamish Gordon, Katrianne Lehtipalo, Henning Finkenzeller, Changhyuk Kim, Yuri Stozhkov, Yee J. Tham, Leonid Nichman, Weimeng Kong, Tuukka Petäjä, Carla Frege, Mao Xiao, Hanna E. Manninen, F. Bianchi, M. V. Philippov, and Andrea Ojdanic

Subjects
Atmospheric Science, Chemical ionization, 010504 meteorology & atmospheric sciences, Autoxidation, Vapor pressure, Analytical chemistry, Nucleation, Sulfuric acid, 010402 general chemistry, 01 natural sciences, 0104 chemical sciences, 3. Good health, Aerosol, chemistry.chemical_compound, chemistry, 13. Climate action, Oxidation state, Volatility (chemistry), 0105 earth and related environmental sciences
Abstract

Highly oxygenated organic molecules (HOMs) contribute substantially to the formation and growth of atmospheric aerosol particles, which affect air quality, human health and Earth's climate. HOMs are formed by rapid, gas-phase autoxidation of volatile organic compounds (VOCs) such as α-pinene, the most abundant monoterpene in the atmosphere. Due to their abundance and low volatility, HOMs can play an important role in new-particle formation (NPF) and the early growth of atmospheric aerosols, even without any further assistance of other low-volatility compounds such as sulfuric acid. Both the autoxidation reaction forming HOMs and their NPF rates are expected to be strongly dependent on temperature. However, experimental data on both effects are limited. Dedicated experiments were performed at the CLOUD (Cosmics Leaving OUtdoor Droplets) chamber at CERN to address this question. In this study, we show that a decrease in temperature (from +25 to −50 ∘C) results in a reduced HOM yield and reduced oxidation state of the products, whereas the NPF rates (J1.7 nm) increase substantially. Measurements with two different chemical ionization mass spectrometers (using nitrate and protonated water as reagent ion, respectively) provide the molecular composition of the gaseous oxidation products, and a two-dimensional volatility basis set (2D VBS) model provides their volatility distribution. The HOM yield decreases with temperature from 6.2 % at 25 ∘C to 0.7 % at −50 ∘C. However, there is a strong reduction of the saturation vapor pressure of each oxidation state as the temperature is reduced. Overall, the reduction in volatility with temperature leads to an increase in the nucleation rates by up to 3 orders of magnitude at −50 ∘C compared with 25 ∘C. In addition, the enhancement of the nucleation rates by ions decreases with decreasing temperature, since the neutral molecular clusters have increased stability against evaporation. The resulting data quantify how the interplay between the temperature-dependent oxidation pathways and the associated vapor pressures affect biogenic NPF at the molecular level. Our measurements, therefore, improve our understanding of pure biogenic NPF for a wide range of tropospheric temperatures and precursor concentrations.

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22. Synergistic HNO3–H2SO4–NH3 upper tropospheric particle formation

Author

Mingyi Wang, Mao Xiao, Barbara Bertozzi, Guillaume Marie, Birte Rörup, Benjamin Schulze, Roman Bardakov, Xu-Cheng He, Jiali Shen, Wiebke Scholz, Ruby Marten, Lubna Dada, Rima Baalbaki, Brandon Lopez, Houssni Lamkaddam, Hanna E. Manninen, António Amorim, Farnoush Ataei, Pia Bogert, Zoé Brasseur, Lucía Caudillo, Louis-Philippe De Menezes, Jonathan Duplissy, Annica M. L. Ekman, Henning Finkenzeller, Loïc Gonzalez Carracedo, Manuel Granzin, Roberto Guida, Martin Heinritzi, Victoria Hofbauer, Kristina Höhler, Kimmo Korhonen, Jordan E. Krechmer, Andreas Kürten, Katrianne Lehtipalo, Naser G. A. Mahfouz, Vladimir Makhmutov, Dario Massabò, Serge Mathot, Roy L. Mauldin, Bernhard Mentler, Tatjana Müller, Antti Onnela, Tuukka Petäjä, Maxim Philippov, Ana A. Piedehierro, Andrea Pozzer, Ananth Ranjithkumar, Meredith Schervish, Siegfried Schobesberger, Mario Simon, Yuri Stozhkov, António Tomé, Nsikanabasi Silas Umo, Franziska Vogel, Robert Wagner, Dongyu S. Wang, Stefan K. Weber, André Welti, Yusheng Wu, Marcel Zauner-Wieczorek, Mikko Sipilä, Paul M. Winkler, Armin Hansel, Urs Baltensperger, Markku Kulmala, Richard C. Flagan, Joachim Curtius, Ilona Riipinen, Hamish Gordon, Jos Lelieveld, Imad El-Haddad, Rainer Volkamer, Douglas R. Worsnop, Theodoros Christoudias, Jasper Kirkby, Ottmar Möhler, Neil M. Donahue, Institute for Atmospheric and Earth System Research (INAR), Polar and arctic atmospheric research (PANDA), Air quality research group, Helsinki Institute of Physics, and Department of Physics

Subjects
Ammonia, Gases, Nitric Acid, Atmosphere, Ice, Earth sciences, Multidisciplinary, Meteorology and Atmospheric Sciences, Meteorologi och atmosfärforskning, ddc:550, 114 Physical sciences
Abstract

New particle formation in the upper free troposphere is a major global source of cloud condensation nuclei (CCN)1–4. However, the precursor vapours that drive the process are not well understood. With experiments performed under upper tropospheric conditions in the CERN CLOUD chamber, we show that nitric acid, sulfuric acid and ammonia form particles synergistically, at rates that are orders of magnitude faster than those from any two of the three components. The importance of this mechanism depends on the availability of ammonia, which was previously thought to be efficiently scavenged by cloud droplets during convection. However, surprisingly high concentrations of ammonia and ammonium nitrate have recently been observed in the upper troposphere over the Asian monsoon region5,6. Once particles have formed, co-condensation of ammonia and abundant nitric acid alone is sufficient to drive rapid growth to CCN sizes with only trace sulfate. Moreover, our measurements show that these CCN are also highly efficient ice nucleating particles—comparable to desert dust. Our model simulations confirm that ammonia is efficiently convected aloft during the Asian monsoon, driving rapid, multi-acid HNO3–H2SO4–NH3nucleation in the upper troposphere and producing ice nucleating particles that spread across the mid-latitude Northern Hemisphere.

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