Articles | Volume 15, issue 23
https://doi.org/10.5194/acp-15-13599-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-15-13599-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
09 Dec 2015
Research article |
| 09 Dec 2015
Viscous organic aerosol particles in the upper troposphere: diffusivity-controlled water uptake and ice nucleation?
D. M. Lienhard
Institute for Atmospheric and Climate Science, ETH Zürich, 8092 Zürich, Switzerland
present address: Department of Chemistry, University of Cambridge, Cambridge, UK
A. J. Huisman
Institute for Atmospheric and Climate Science, ETH Zürich, 8092 Zürich, Switzerland
present address: Chemistry Department, Union College, Schenectady, NY, USA
U. K. Krieger
Institute for Atmospheric and Climate Science, ETH Zürich, 8092 Zürich, Switzerland
Y. Rudich
Department of Environmental Sciences, Weizmann Institute, Rehovot 76100, Israel
C. Marcolli
Institute for Atmospheric and Climate Science, ETH Zürich, 8092 Zürich, Switzerland
Marcolli Chemistry and Physics Consulting GmbH, 8092 Zürich, Switzerland
B. P. Luo
Institute for Atmospheric and Climate Science, ETH Zürich, 8092 Zürich, Switzerland
Physikalisch-Meteorologisches Observatorium Davos and World Radiation Center PMOD/WRC, 7260 Davos, Switzerland
D. L. Bones
School of Chemistry, University of Bristol, BS8 1TS Bristol, UK
present address: School of Chemistry, University of Leeds, Leeds, UK
J. P. Reid
School of Chemistry, University of Bristol, BS8 1TS Bristol, UK
A. T. Lambe
Chemistry Department, Boston College, Chestnut Hill, MA 02467, USA
Aerodyne Research Inc., Billerica, MA 01821, USA
M. R. Canagaratna
Aerodyne Research Inc., Billerica, MA 01821, USA
P. Davidovits
Chemistry Department, Boston College, Chestnut Hill, MA 02467, USA
T. B. Onasch
Chemistry Department, Boston College, Chestnut Hill, MA 02467, USA
Aerodyne Research Inc., Billerica, MA 01821, USA
D. R. Worsnop
Aerodyne Research Inc., Billerica, MA 01821, USA
S. S. Steimer
Institute for Atmospheric and Climate Science, ETH Zürich, 8092 Zürich, Switzerland
Laboratory of Radiochemistry and Environmental Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland
Faculty of Chemistry, Bielefeld University, 33615 Bielefeld, Germany
T. Peter
Institute for Atmospheric and Climate Science, ETH Zürich, 8092 Zürich, Switzerland
Related authors
No articles found.
Nadia Shardt, Florin N. Isenrich, Julia Nette, Christopher Dreimol, Ning Ma, Zamin A. Kanji, Andrew J. deMello, and Claudia Marcolli
Atmos. Chem. Phys., 25, 17997–18014, https://doi.org/10.5194/acp-25-17997-2025, https://doi.org/10.5194/acp-25-17997-2025, 2025
Short summary
Short summary
In the atmosphere, minerals suspended in cloud droplets promote the formation of ice. We investigated ice formation in the presence of pure and binary mixtures of common minerals using a microfluidic device. The mineral with the best ability to initiate ice formation alone (that is, at the highest temperature) typically determined when ice formed in the binary mixture.
Cynthia Antossian, Marcel Müller, and Ulrich K. Krieger
EGUsphere, https://doi.org/10.5194/egusphere-2025-5928, https://doi.org/10.5194/egusphere-2025-5928, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
Short summary
Short summary
Organic aerosols undergo changes when exposed to oxidants like ozone or UV light. This study looks at how both aging processes affect particle properties, using trans-aconitic acid as a proxy for secondary organic aerosols. We found that exposure to UV light and ozone causes mass loss and changes viscosity significantly, up to 4 orders of magnitude. This suggests that aged particles may take much longer than untreated particles to equilibrate under dry conditions.
Andre F. Schaum, Kelvin H. Bates, Kyung-Eun Min, Faith Myers, Emmaline R. Longnecker, Manjula R. Canagaratna, Mitchell W. Alton, and Paul J. Ziemann
Aerosol Research, 3, 557–568, https://doi.org/10.5194/ar-3-557-2025, https://doi.org/10.5194/ar-3-557-2025, 2025
Short summary
Short summary
Organic aerosols consist of complex chemical mixtures that are challenging to characterize using chemical ionization mass spectrometry alone. This study presents a method for coupling liquid chromatography and chemical ionization mass spectrometry for the offline analysis of organic aerosols. The evaluation of the method using standards and laboratory-generated and field-collected organic aerosols showed that it can provide detailed characterization of environmentally relevant mixtures.
Barbara Ervens, Ken S. Carslaw, Thomas Koop, and Ulrich Pöschl
Atmos. Chem. Phys., 25, 13903–13952, https://doi.org/10.5194/acp-25-13903-2025, https://doi.org/10.5194/acp-25-13903-2025, 2025
Short summary
Short summary
Over 25 years, the European Geosciences Union (EGU) has demonstrated the success, viability and benefits of interactive open-access (OA) publishing with public peer review in its journals, its publishing platform EGUsphere and virtual compilations. The article summarizes the evolution of the EGU/Copernicus publications and of OA publishing with interactive public peer review at large by placing the EGU/Copernicus publications in the context of current and future global open science.
Dandan Zhang, Randall V. Martin, Xuan Liu, Aaron van Donkelaar, Christopher R. Oxford, Yanshun Li, Jun Meng, Danny M. Leung, Jasper F. Kok, Longlei Li, Haihui Zhu, Jay R. Turner, Yu Yan, Michael Brauer, Yinon Rudich, and Eli Windwer
Geosci. Model Dev., 18, 6767–6803, https://doi.org/10.5194/gmd-18-6767-2025, https://doi.org/10.5194/gmd-18-6767-2025, 2025
Short summary
Short summary
This study develops the fine mineral dust simulation in GEOS-Chem by: 1) implementing a new dust emission scheme with further refinements; 2) revisiting the size distribution of emitted dust; 3) explicitly tracking fine dust for emission, transport and deposition in 4 size bins; 4) updating the parametrization for below-cloud scavenging. All revisions significantly reduce the overestimation of surface fine dust from 94 % to 35 % while retaining comparable skill in representing columnar abundance.
Marcel Müller, Marcel Reichmuth, and Ulrich K. Krieger
Atmos. Chem. Phys., 25, 11441–11451, https://doi.org/10.5194/acp-25-11441-2025, https://doi.org/10.5194/acp-25-11441-2025, 2025
Short summary
Short summary
The initiation of autoxidation by ozonolysis was investigated on levitated linoleic acid droplets using electrodynamic balance–mass spectrometry. Exposing the droplets to ozone for 1 h before switching the gas phase to air without ozone led to a shortening of the autoxidation initiation phase in comparison to experiments without ozone exposure. Results were compared to a bulk reaction model to investigate the synergistic effects of ozonolysis and autoxidation.
Andrin Jörimann, Timofei Sukhodolov, Beiping Luo, Gabriel Chiodo, Graham Mann, and Thomas Peter
Geosci. Model Dev., 18, 6023–6041, https://doi.org/10.5194/gmd-18-6023-2025, https://doi.org/10.5194/gmd-18-6023-2025, 2025
Short summary
Short summary
Aerosol particles in the stratosphere affect our climate. Climate models therefore need an accurate description of their properties and evolution. Satellites measure how strongly aerosol particles extinguish light passing through the stratosphere. We describe a method to use such aerosol extinction data to retrieve the number and sizes of the aerosol particles and calculate their optical effects. The resulting data sets for models are validated against ground-based and balloon observations.
Yu Wang, Beiping Luo, Judith Kleinheins, Gang I. Chen, Liine Heikkinen, and Claudia Marcolli
EGUsphere, https://doi.org/10.5194/egusphere-2025-4319, https://doi.org/10.5194/egusphere-2025-4319, 2025
Short summary
Short summary
Ubiquitous semi-volatile compounds can co-condense on aerosol particles with water vapour when relative humidity increases. Simulations of cloud formation at a boreal forest site with a cloud parcel model that accounts for non-ideal organic–inorganic interactions yield an enhancement of cloud droplet number concentration from co-condensing NH3, HNO3, and organics up to 39–52 %, with strong sensitivities to volatility distributions, aerosol size distribution, and updraft velocity.
Ying Zhang, Yuwei Wang, Chuang Li, Yueyang Li, Sijia Yin, Megan S. Claflin, Brian M. Lerner, Douglas Worsnop, and Lin Wang
Atmos. Meas. Tech., 18, 3547–3568, https://doi.org/10.5194/amt-18-3547-2025, https://doi.org/10.5194/amt-18-3547-2025, 2025
Short summary
Short summary
This study provides insight into how individual ions measured by proton-transfer-reaction (PTR) mass spectrometry are produced by multiple volatile organic compounds (VOCs). A reference table is provided for attributing the PTR signal to contributing VOC species. The signals are grouped according to the complexity of their potential identities. We find that a number of signal ions such as C6H7+ for benzene and C5H9+ for isoprene merely give an upper limit of their corresponding concentrations.
Neil M. Donahue, Victoria Hofbauer, Henning Finkenzeller, Dominik Stolzenburg, Paulus S. Bauer, Randall Chiu, Lubna Dada, Jonathan Duplissy, Xu-Cheng He, Martin Heinritzi, Christopher R. Hoyle, Andreas Kürten, Aleksandr Kvashnin, Katrianne Lehtipalo, Naser Mahfouz, Vladimir Makhmutov, Roy L. Mauldin III, Ugo Molteni, Lauriane L. J. Quéléver, Matti Rissanen, Siegfried Schobesberger, Mario Simon, Andrea C. Wagner, Mingyi Wang, Chao Yan, Penglin Ye, Ilona Riipinen, Hamish Gordon, Joachim Curtius, Armin Hansel, Imad El Haddad, Markku Kulmala, Douglas R. Worsnop, Rainer Volkamer, Paul M. Winkler, Jasper Kirkby, and Richard Flagan
EGUsphere, https://doi.org/10.5194/egusphere-2025-2412, https://doi.org/10.5194/egusphere-2025-2412, 2025
This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
Short summary
Short summary
We describe accurate measurement of particle formation and growth in the CERN CLOUD chamber, using a suite of gas- and particle-phase instruments. The interconnected measurements establish high accuracy in key particle properties and critically important gas-phase sulfuric acid. This is a template for accurate calibration of similar experiments and thus accurate determination of aerosol nucleation and growth rates, which are an important source of uncertainty in climate science.
Dongwook Kim, Pedro Campuzano-Jost, Hongyu Guo, Douglas A. Day, Da Yang, Suresh Dhaniyala, Leah Williams, Philip Croteau, John Jayne, Douglas Worsnop, Rainer Volkamer, and Jose L. Jimenez
Aerosol Research, 3, 371–404, https://doi.org/10.5194/ar-3-371-2025, https://doi.org/10.5194/ar-3-371-2025, 2025
Short summary
Short summary
Quantitative real-time aerosol sampling on board aircraft platforms is challenging, especially at higher altitudes. Herein, we present comprehensive analyses of a new aircraft inlet system and tools for aerosol beam diagnostics for aerosol mass spectrometers (AMSs). The beam focusing of aerodynamic lenses and the thermal decomposition on the vaporizer were investigated. The new inlet system can be operated at higher altitudes while sampling aerosols over a broader size range than previous versions.
Qianying Liu, Dan Dan Huang, Andrew T. Lambe, Shengrong Lou, Lulu Zeng, Yuhang Wu, Congyan Huang, Shikang Tao, Xi Cheng, Qi Chen, Ka In Hoi, Hongli Wang, Kai Meng Mok, Cheng Huang, and Yong Jie Li
Atmos. Meas. Tech., 18, 2509–2521, https://doi.org/10.5194/amt-18-2509-2025, https://doi.org/10.5194/amt-18-2509-2025, 2025
Short summary
Short summary
We evaluate the applicability of empirical equations to estimate OH exposure (OHexp) in an oxidative flow reactor (OFR). The fitting parameters obtained within a narrow range of conditions can generally be extended to estimate the OHexp for wide ranges of conditions in the OFR, except for external OH reactivity, which requires new fitting. At least 20–30 data points from SO2 or CO decay with varying conditions are required to fit a set of empirical parameters that can accurately estimate OHexp.
Yann Poltera, Beiping Luo, Frank G. Wienhold, and Thomas Peter
EGUsphere, https://doi.org/10.5194/egusphere-2025-2003, https://doi.org/10.5194/egusphere-2025-2003, 2025
Short summary
Short summary
Frost point hygrometers are the most reliable instruments for measuring water vapor in the upper troposphere and lower stratosphere. Their greatest source of uncertainty arises from controller instabilities, which have been poorly investigated to date. The “Golden Points” and nonequilibrium correction is a new chilled mirror processing technique that enables existing instruments to measure the water vapor mixing ratio from the ground to the middle stratosphere with an unprecedented 4 % accuracy.
Anna J. Miller, Christopher Fuchs, Fabiola Ramelli, Huiying Zhang, Nadja Omanovic, Robert Spirig, Claudia Marcolli, Zamin A. Kanji, Ulrike Lohmann, and Jan Henneberger
Atmos. Chem. Phys., 25, 5387–5407, https://doi.org/10.5194/acp-25-5387-2025, https://doi.org/10.5194/acp-25-5387-2025, 2025
Short summary
Short summary
We analyzed the ability of silver iodide particles (a commonly used cloud-seeding agent) to form ice crystals in naturally occurring liquid clouds at −5 to −8 °C and found that only ≈ 0.1 %−1 % of particles nucleate ice, with a negative dependence on temperature. By contextualizing our results with previous laboratory studies, we help to bridge the gap between laboratory and field experiments, which also helps to inform future cloud-seeding projects.
Benjamin C. Sapper, Sean Youn, Daven K. Henze, Manjula Canagaratna, Harald Stark, and Jose L. Jimenez
Geosci. Model Dev., 18, 2891–2919, https://doi.org/10.5194/gmd-18-2891-2025, https://doi.org/10.5194/gmd-18-2891-2025, 2025
Short summary
Short summary
Positive matrix factorization (PMF) has been used by atmospheric scientists to extract underlying factors present in large datasets. This paper presents a new technique for error-weighted PMF that drastically reduces the computational costs of previously developed algorithms. We use this technique to deliver interpretable factors and solution diagnostics from an atmospheric chemistry dataset.
Battist Utinger, Alexandre Barth, Andreas Paul, Arya Mukherjee, Steven John Campbell, Christa-Maria Müller, Mika Ihalainen, Pasi Yli-Pirilä, Miika Kortelainen, Zheng Fang, Patrick Martens, Markus Somero, Juho Louhisalmi, Thorsten Hohaus, Hendryk Czech, Olli Sippula, Yinon Rudich, Ralf Zimmermann, and Markus Kalberer
Aerosol Research, 3, 205–218, https://doi.org/10.5194/ar-3-205-2025, https://doi.org/10.5194/ar-3-205-2025, 2025
Short summary
Short summary
The oxidative potential (OP) of air pollution particles might be a metric explaining particle toxicity. This study quantifies the OP of fresh and aged car and wood burning emission particles and explores how the OP changes over time, using novel high-temporal-resolution instruments. We show that emissions from wood burning are more toxic than car exhaust per unit particle mass, especially as they age in the atmosphere. We also calculate emission factors for the OP, which could help to improve air pollution policies.
Valter Mickwitz, Otso Peräkylä, Frans Graeffe, Douglas Worsnop, and Mikael Ehn
Atmos. Meas. Tech., 18, 1537–1559, https://doi.org/10.5194/amt-18-1537-2025, https://doi.org/10.5194/amt-18-1537-2025, 2025
Short summary
Short summary
This work presents and evaluates an algorithm that automatically conducts the steps of fitting peaks and identifying formulas – necessary but time-consuming steps for most applications of mass spectrometry in atmospheric science. The aim of the algorithm is to save researchers working on these tasks significant amounts of time and allow them to proceed with their analysis. The work demonstrates that this algorithm can achieve the goal of speeding up analysis and provide accurate formulas.
Judith Kleinheins, Nadia Shardt, Ulrike Lohmann, and Claudia Marcolli
Atmos. Chem. Phys., 25, 881–903, https://doi.org/10.5194/acp-25-881-2025, https://doi.org/10.5194/acp-25-881-2025, 2025
Short summary
Short summary
We model the cloud condensation nuclei (CCN) activation of sea spray aerosol particles with classical Köhler theory and with a new model approach that takes surface tension lowering into account. We categorize organic compounds into weak, intermediate, and strong surfactants, and we outline for which composition surface tension lowering is important. The results suggest that surface tension lowering allows sea spray aerosol particles in the Aitken mode to be a source of CCN in marine updraughts.
Diego Aliaga, Victoria A. Sinclair, Radovan Krejci, Marcos Andrade, Paulo Artaxo, Luis Blacutt, Runlong Cai, Samara Carbone, Yvette Gramlich, Liine Heikkinen, Dominic Heslin-Rees, Wei Huang, Veli-Matti Kerminen, Alkuin Maximilian Koenig, Markku Kulmala, Paolo Laj, Valeria Mardoñez-Balderrama, Claudia Mohr, Isabel Moreno, Pauli Paasonen, Wiebke Scholz, Karine Sellegri, Laura Ticona, Gaëlle Uzu, Fernando Velarde, Alfred Wiedensohler, Doug Worsnop, Cheng Wu, Chen Xuemeng, Qiaozhi Zha, and Federico Bianchi
Aerosol Research, 3, 15–44, https://doi.org/10.5194/ar-3-15-2025, https://doi.org/10.5194/ar-3-15-2025, 2025
Short summary
Short summary
This study examines new particle formation (NPF) in the Bolivian Andes at Chacaltaya mountain (CHC) and the urban El Alto–La Paz area (EAC). Days are clustered into four categories based on NPF intensity. Differences in particle size, precursor gases, and pollution levels are found. High NPF intensities increased Aitken mode particle concentrations at both sites, while volcanic influence selectively diminished NPF intensity at CHC but not EAC. This study highlights NPF dynamics in the Andes.
Pamela A. Dominutti, Jean-Luc Jaffrezo, Anouk Marsal, Takoua Mhadhbi, Rhabira Elazzouzi, Camille Rak, Fabrizia Cavalli, Jean-Philippe Putaud, Aikaterini Bougiatioti, Nikolaos Mihalopoulos, Despina Paraskevopoulou, Ian Mudway, Athanasios Nenes, Kaspar R. Daellenbach, Catherine Banach, Steven J. Campbell, Hana Cigánková, Daniele Contini, Greg Evans, Maria Georgopoulou, Manuella Ghanem, Drew A. Glencross, Maria Rachele Guascito, Hartmut Herrmann, Saima Iram, Maja Jovanović, Milena Jovašević-Stojanović, Markus Kalberer, Ingeborg M. Kooter, Suzanne E. Paulson, Anil Patel, Esperanza Perdrix, Maria Chiara Pietrogrande, Pavel Mikuška, Jean-Jacques Sauvain, Katerina Seitanidi, Pourya Shahpoury, Eduardo J. d. S. Souza, Sarah Steimer, Svetlana Stevanovic, Guillaume Suarez, P. S. Ganesh Subramanian, Battist Utinger, Marloes F. van Os, Vishal Verma, Xing Wang, Rodney J. Weber, Yuhan Yang, Xavier Querol, Gerard Hoek, Roy M. Harrison, and Gaëlle Uzu
Atmos. Meas. Tech., 18, 177–195, https://doi.org/10.5194/amt-18-177-2025, https://doi.org/10.5194/amt-18-177-2025, 2025
Short summary
Short summary
In this work, 20 labs worldwide collaborated to evaluate the measurement of air pollution's oxidative potential (OP), a key indicator of its harmful effects. The study aimed to identify disparities in the widely used OP dithiothreitol assay and assess the consistency of OP among labs using the same protocol. The results showed that half of the labs achieved acceptable results. However, variability was also found, highlighting the need for standardisation in OP procedures.
Zhaojin An, Rujing Yin, Xinyan Zhao, Xiaoxiao Li, Yuyang Li, Yi Yuan, Junchen Guo, Yiqi Zhao, Xue Li, Dandan Li, Yaowei Li, Dongbin Wang, Chao Yan, Kebin He, Douglas R. Worsnop, Frank N. Keutsch, and Jingkun Jiang
Atmos. Chem. Phys., 24, 13793–13810, https://doi.org/10.5194/acp-24-13793-2024, https://doi.org/10.5194/acp-24-13793-2024, 2024
Short summary
Short summary
Online Vocus-PTR measurements show the compositions and seasonal variations in organic vapors in urban Beijing. With enhanced sensitivity and mass resolution, various species at a level of sub-parts per trillion (ppt) and organics with multiple oxygens (≥ 3) were observed. The fast photooxidation process in summer leads to an increase in both concentration and proportion of organics with multiple oxygens, while, in other seasons, the variations in them could be influenced by mixed sources.
Liviana K. Klein, Allan K. Bertram, Andreas Zuend, Florence Gregson, and Ulrich K. Krieger
Atmos. Chem. Phys., 24, 13341–13359, https://doi.org/10.5194/acp-24-13341-2024, https://doi.org/10.5194/acp-24-13341-2024, 2024
Short summary
Short summary
The viscosity of ammonium nitrate–sucrose–H2O was quantified with three methods ranging from liquid to solid state depending on the relative humidity. Moreover, the corresponding estimated internal aerosol mixing times remained below 1 h for most tropospheric conditions, making equilibrium partitioning a reasonable assumption.
Sandro Vattioni, Rahel Weber, Aryeh Feinberg, Andrea Stenke, John A. Dykema, Beiping Luo, Georgios A. Kelesidis, Christian A. Bruun, Timofei Sukhodolov, Frank N. Keutsch, Thomas Peter, and Gabriel Chiodo
Geosci. Model Dev., 17, 7767–7793, https://doi.org/10.5194/gmd-17-7767-2024, https://doi.org/10.5194/gmd-17-7767-2024, 2024
Short summary
Short summary
We quantified impacts and efficiency of stratospheric solar climate intervention via solid particle injection. Microphysical interactions of solid particles with the sulfur cycle were interactively coupled to the heterogeneous chemistry scheme and the radiative transfer code of an aerosol–chemistry–climate model. Compared to injection of SO2 we only find a stronger cooling efficiency for solid particles when normalizing to the aerosol load but not when normalizing to the injection rate.
Tianle Pan, Andrew T. Lambe, Weiwei Hu, Yicong He, Minghao Hu, Huaishan Zhou, Xinming Wang, Qingqing Hu, Hui Chen, Yue Zhao, Yuanlong Huang, Doug R. Worsnop, Zhe Peng, Melissa A. Morris, Douglas A. Day, Pedro Campuzano-Jost, Jose-Luis Jimenez, and Shantanu H. Jathar
Atmos. Meas. Tech., 17, 4915–4939, https://doi.org/10.5194/amt-17-4915-2024, https://doi.org/10.5194/amt-17-4915-2024, 2024
Short summary
Short summary
This study systematically characterizes the temperature enhancement in the lamp-enclosed oxidation flow reactor (OFR). The enhancement varied multiple dimensional factors, emphasizing the complexity of temperature inside of OFR. The effects of temperature on the flow field and gas- or particle-phase reaction inside OFR were also evaluated with experiments and model simulations. Finally, multiple mitigation strategies were demonstrated to minimize this temperature increase.
Zijun Zhang, Weiqi Xu, Yi Zhang, Wei Zhou, Xiangyu Xu, Aodong Du, Yinzhou Zhang, Hongqin Qiao, Ye Kuang, Xiaole Pan, Zifa Wang, Xueling Cheng, Lanzhong Liu, Qingyan Fu, Douglas R. Worsnop, Jie Li, and Yele Sun
Atmos. Chem. Phys., 24, 8473–8488, https://doi.org/10.5194/acp-24-8473-2024, https://doi.org/10.5194/acp-24-8473-2024, 2024
Short summary
Short summary
We investigated aerosol composition and sources and the interaction between secondary organic aerosol (SOA) and clouds at a regional mountain site in southeastern China. Clouds efficiently scavenge more oxidized SOA; however, cloud evaporation leads to the production of less oxidized SOA. The unexpectedly high presence of nitrate in aerosol particles indicates that nitrate formed in polluted areas has undergone interactions with clouds, significantly influencing the regional background site.
Muhammed Irfan, Thomas Kühn, Taina Yli-Juuti, Anton Laakso, Eemeli Holopainen, Douglas R. Worsnop, Annele Virtanen, and Harri Kokkola
Atmos. Chem. Phys., 24, 8489–8506, https://doi.org/10.5194/acp-24-8489-2024, https://doi.org/10.5194/acp-24-8489-2024, 2024
Short summary
Short summary
The study examines how the volatility of semi-volatile organic compounds affects secondary organic aerosol (SOA) formation and climate. Our simulations show that uncertainties in these volatilities influence aerosol mass and climate impacts. Accurate representation of these compounds in climate models is crucial for predicting global climate patterns.
Mark D. Tarn, Bethany V. Wyld, Naama Reicher, Matan Alayof, Daniella Gat, Alberto Sanchez-Marroquin, Sebastien N. F. Sikora, Alexander D. Harrison, Yinon Rudich, and Benjamin J. Murray
Aerosol Research, 2, 161–182, https://doi.org/10.5194/ar-2-161-2024, https://doi.org/10.5194/ar-2-161-2024, 2024
Short summary
Short summary
Ambient ice-nucleating particle (INP) concentrations were measured in Israel, which experiences air masses from a variety of sources. We found that the INP activity is typically dominated by K-feldspar mineral dust but that air masses passing over regions of fertile soils correlated with high INP concentrations and indicators of biological activity. This suggests that these fertile regions could be sporadic sources of warm-temperature biogenic INPs and warrants further study of these areas.
Chenjie Yu, Edouard Pangui, Kevin Tu, Mathieu Cazaunau, Maxime Feingesicht, Landsheere Xavier, Thierry Bourrianne, Vincent Michoud, Christopher Cantrell, Timothy B. Onasch, Andrew Freedman, and Paola Formenti
Atmos. Meas. Tech., 17, 3419–3437, https://doi.org/10.5194/amt-17-3419-2024, https://doi.org/10.5194/amt-17-3419-2024, 2024
Short summary
Short summary
To meet the requirements for measuring aerosol optical properties on airborne platforms and conducting dual-wavelength measurements, we introduced A2S2, an airborne dual-wavelength cavity-attenuated phase-shift single monitor. This study reports the results in the laboratory and an aircraft campaign over Paris and its surrounding regions. The results demonstrate A2S2's reliability in measuring aerosol optical properties at both wavelengths and its suitability for future aircraft campaigns.
Sandro Vattioni, Andrea Stenke, Beiping Luo, Gabriel Chiodo, Timofei Sukhodolov, Elia Wunderlin, and Thomas Peter
Geosci. Model Dev., 17, 4181–4197, https://doi.org/10.5194/gmd-17-4181-2024, https://doi.org/10.5194/gmd-17-4181-2024, 2024
Short summary
Short summary
We investigate the sensitivity of aerosol size distributions in the presence of strong SO2 injections for climate interventions or after volcanic eruptions to the call sequence and frequency of the routines for nucleation and condensation in sectional aerosol models with operator splitting. Using the aerosol–chemistry–climate model SOCOL-AERv2, we show that the radiative and chemical outputs are sensitive to these settings at high H2SO4 supersaturations and how to obtain reliable results.
Christina V. Brodowsky, Timofei Sukhodolov, Gabriel Chiodo, Valentina Aquila, Slimane Bekki, Sandip S. Dhomse, Michael Höpfner, Anton Laakso, Graham W. Mann, Ulrike Niemeier, Giovanni Pitari, Ilaria Quaglia, Eugene Rozanov, Anja Schmidt, Takashi Sekiya, Simone Tilmes, Claudia Timmreck, Sandro Vattioni, Daniele Visioni, Pengfei Yu, Yunqian Zhu, and Thomas Peter
Atmos. Chem. Phys., 24, 5513–5548, https://doi.org/10.5194/acp-24-5513-2024, https://doi.org/10.5194/acp-24-5513-2024, 2024
Short summary
Short summary
The aerosol layer is an essential part of the climate system. We characterize the sulfur budget in a volcanically quiescent (background) setting, with a special focus on the sulfate aerosol layer using, for the first time, a multi-model approach. The aim is to identify weak points in the representation of the atmospheric sulfur budget in an intercomparison of nine state-of-the-art coupled global circulation models.
Fangbing Li, Dan Dan Huang, Linhui Tian, Bin Yuan, Wen Tan, Liang Zhu, Penglin Ye, Douglas Worsnop, Ka In Hoi, Kai Meng Mok, and Yong Jie Li
Atmos. Meas. Tech., 17, 2415–2427, https://doi.org/10.5194/amt-17-2415-2024, https://doi.org/10.5194/amt-17-2415-2024, 2024
Short summary
Short summary
The responses of protonated, adduct, and fragmented ions of 21 volatile organic compounds (VOCs) were investigated with varying instrument settings and relative humidity (RH) in a Vocus proton-transfer-reaction mass spectrometer (PTR-MS). The protonated ions of most VOCs studied show < 15 % variation in sensitivity, except for some long-chain aldehydes. The relationship between sensitivity and PTR rate constant is complicated by the influences from ion transmission and protonated ion fraction.
Mahen Konwar, Benjamin Werden, Edward C. Fortner, Sudarsan Bera, Mercy Varghese, Subharthi Chowdhuri, Kurt Hibert, Philip Croteau, John Jayne, Manjula Canagaratna, Neelam Malap, Sandeep Jayakumar, Shivsai A. Dixit, Palani Murugavel, Duncan Axisa, Darrel Baumgardner, Peter F. DeCarlo, Doug R. Worsnop, and Thara Prabhakaran
Atmos. Meas. Tech., 17, 2387–2400, https://doi.org/10.5194/amt-17-2387-2024, https://doi.org/10.5194/amt-17-2387-2024, 2024
Short summary
Short summary
In a warm cloud seeding experiment hygroscopic particles are released to alter cloud processes to induce early raindrops. During the Cloud–Aerosol Interaction and Precipitation Enhancement Experiment, airborne mini aerosol mass spectrometers analyse the particles on which clouds form. The seeded clouds showed higher concentrations of chlorine and potassium, the oxidizing agents of flares. Small cloud droplet concentrations increased, and seeding particles were detected in deep cloud depths.
Markku Kulmala, Diego Aliaga, Santeri Tuovinen, Runlong Cai, Heikki Junninen, Chao Yan, Federico Bianchi, Yafang Cheng, Aijun Ding, Douglas R. Worsnop, Tuukka Petäjä, Katrianne Lehtipalo, Pauli Paasonen, and Veli-Matti Kerminen
Aerosol Research, 2, 49–58, https://doi.org/10.5194/ar-2-49-2024, https://doi.org/10.5194/ar-2-49-2024, 2024
Short summary
Short summary
Atmospheric new particle formation (NPF), together with secondary production of particulate matter in the atmosphere, dominates aerosol particle number concentrations and submicron particle mass loads in many environments globally. In this opinion paper, we describe the paradigm shift to understand NPF in a continuous way instead of using traditional binary event–non-event analysis.
Jian Zhao, Valter Mickwitz, Yuanyuan Luo, Ella Häkkinen, Frans Graeffe, Jiangyi Zhang, Hilkka Timonen, Manjula Canagaratna, Jordan E. Krechmer, Qi Zhang, Markku Kulmala, Juha Kangasluoma, Douglas Worsnop, and Mikael Ehn
Atmos. Meas. Tech., 17, 1527–1543, https://doi.org/10.5194/amt-17-1527-2024, https://doi.org/10.5194/amt-17-1527-2024, 2024
Short summary
Short summary
Organic aerosol constitutes a significant portion of atmospheric fine particles but is less characterized due to its vast number of constituents. Recently, we developed a system for online measurements of particle-phase highly oxygenated organic molecules (HOMs). In this work, we systematically characterized the system, developed a new unit to enhance its performance, and demonstrated the essential role of thermograms in inferring volatility and quantifying HOMs in organic aerosols.
Jiangyi Zhang, Jian Zhao, Yuanyuan Luo, Valter Mickwitz, Douglas Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 24, 2885–2911, https://doi.org/10.5194/acp-24-2885-2024, https://doi.org/10.5194/acp-24-2885-2024, 2024
Short summary
Short summary
Due to the intrinsic connection between the formation pathways of O3 and HOMs, the ratio of HOM dimers or non-nitrate monomers to HOM organic nitrates could be used to determine O3 formation regimes. Owing to the fast formation and short lifetimes of HOMs, HOM-based indicating ratios can describe O3 formation in real time. Despite the success of our approach in this simple laboratory system, applicability to the much more complex atmosphere remains to be determined.
Matthew M. Coggon, Chelsea E. Stockwell, Megan S. Claflin, Eva Y. Pfannerstill, Lu Xu, Jessica B. Gilman, Julia Marcantonio, Cong Cao, Kelvin Bates, Georgios I. Gkatzelis, Aaron Lamplugh, Erin F. Katz, Caleb Arata, Eric C. Apel, Rebecca S. Hornbrook, Felix Piel, Francesca Majluf, Donald R. Blake, Armin Wisthaler, Manjula Canagaratna, Brian M. Lerner, Allen H. Goldstein, John E. Mak, and Carsten Warneke
Atmos. Meas. Tech., 17, 801–825, https://doi.org/10.5194/amt-17-801-2024, https://doi.org/10.5194/amt-17-801-2024, 2024
Short summary
Short summary
Mass spectrometry is a tool commonly used to measure air pollutants. This study evaluates measurement artifacts produced in the proton-transfer-reaction mass spectrometer. We provide methods to correct these biases and better measure compounds that degrade air quality.
Jan Clemens, Bärbel Vogel, Lars Hoffmann, Sabine Griessbach, Nicole Thomas, Suvarna Fadnavis, Rolf Müller, Thomas Peter, and Felix Ploeger
Atmos. Chem. Phys., 24, 763–787, https://doi.org/10.5194/acp-24-763-2024, https://doi.org/10.5194/acp-24-763-2024, 2024
Short summary
Short summary
The source regions of the Asian tropopause aerosol layer (ATAL) are debated. We use balloon-borne measurements of the layer above Nainital (India) in August 2016 and atmospheric transport models to find ATAL source regions. Most air originated from the Tibetan plateau. However, the measured ATAL was stronger when more air originated from the Indo-Gangetic Plain and weaker when more air originated from the Pacific. Hence, the results indicate important anthropogenic contributions to the ATAL.
Diego Aliaga, Santeri Tuovinen, Tinghan Zhang, Janne Lampilahti, Xinyang Li, Lauri Ahonen, Tom Kokkonen, Tuomo Nieminen, Simo Hakala, Pauli Paasonen, Federico Bianchi, Doug Worsnop, Veli-Matti Kerminen, and Markku Kulmala
Aerosol Research, 1, 81–92, https://doi.org/10.5194/ar-1-81-2023, https://doi.org/10.5194/ar-1-81-2023, 2023
Short summary
Short summary
We introduce a novel method for evaluating days when small particles are formed in the atmosphere. Instead of the traditional binary division between event and non-event days, our method, known as "nano ranking analysis", provides a continuous, non-categorical metric for each day. By utilizing data from Hyytiälä, Finland, we show that our approach effectively quantifies these events. This innovative method paves the way for a deeper understanding of the factors influencing particle formation.
Rolf Müller, Ulrich Pöschl, Thomas Koop, Thomas Peter, and Ken Carslaw
Atmos. Chem. Phys., 23, 15445–15453, https://doi.org/10.5194/acp-23-15445-2023, https://doi.org/10.5194/acp-23-15445-2023, 2023
Short summary
Short summary
Paul J. Crutzen was a pioneer in atmospheric sciences and a kind-hearted, humorous person with empathy for the private lives of his colleagues and students. He made fundamental scientific contributions to a wide range of scientific topics in all parts of the atmosphere. Paul was among the founders of the journal Atmospheric Chemistry and Physics. His work will continue to be a guide for generations of scientists and environmental policymakers to come.
Abd El Rahman El Mais, Barbara D'Anna, Luka Drinovec, Andrew T. Lambe, Zhe Peng, Jean-Eudes Petit, Olivier Favez, Selim Aït-Aïssa, and Alexandre Albinet
Atmos. Chem. Phys., 23, 15077–15096, https://doi.org/10.5194/acp-23-15077-2023, https://doi.org/10.5194/acp-23-15077-2023, 2023
Short summary
Short summary
Polycyclic aromatic hydrocarbons (PAHS) and furans are key precursors of secondary organic aerosols (SOAs) related to biomass burning emissions. We evaluated and compared the formation yields, and the physical and light absorption properties, of laboratory-generated SOAs from the oxidation of such compounds for both, day- and nighttime reactivities. The results illustrate that PAHs are large SOA precursors and may contribute significantly to the biomass burning brown carbon in the atmosphere.
Ryan N. Farley, Sonya Collier, Christopher D. Cappa, Leah R. Williams, Timothy B. Onasch, Lynn M. Russell, Hwajin Kim, and Qi Zhang
Atmos. Chem. Phys., 23, 15039–15056, https://doi.org/10.5194/acp-23-15039-2023, https://doi.org/10.5194/acp-23-15039-2023, 2023
Short summary
Short summary
Soot particles, also known as black carbon (BC), have important implications for global climate and regional air quality. After the particles are emitted, BC can be coated with other material, impacting the aerosol properties. We selectively measured the composition of particles containing BC to explore their sources and chemical transformations in the atmosphere. We focus on a persistent, multiday fog event in order to study the effects of chemical reactions occurring within liquid droplets.
Andrew T. Lambe, Bin Bai, Masayuki Takeuchi, Nicole Orwat, Paul M. Zimmerman, Mitchell W. Alton, Nga L. Ng, Andrew Freedman, Megan S. Claflin, Drew R. Gentner, Douglas R. Worsnop, and Pengfei Liu
Atmos. Chem. Phys., 23, 13869–13882, https://doi.org/10.5194/acp-23-13869-2023, https://doi.org/10.5194/acp-23-13869-2023, 2023
Short summary
Short summary
We developed a new method to generate nitrate radicals (NO3) for atmospheric chemistry applications that works by irradiating mixtures containing ceric ammonium nitrate with a UV light at room temperature. It has several advantages over traditional NO3 sources. We characterized its performance over a range of mixture and reactor conditions as well as other irradiation products. Proof of concept was demonstrated by generating and characterizing oxidation products of the β-pinene + NO3 reaction.
Franziska Zilker, Timofei Sukhodolov, Gabriel Chiodo, Marina Friedel, Tatiana Egorova, Eugene Rozanov, Jan Sedlacek, Svenja Seeber, and Thomas Peter
Atmos. Chem. Phys., 23, 13387–13411, https://doi.org/10.5194/acp-23-13387-2023, https://doi.org/10.5194/acp-23-13387-2023, 2023
Short summary
Short summary
The Montreal Protocol (MP) has successfully reduced the Antarctic ozone hole by banning chlorofluorocarbons (CFCs) that destroy the ozone layer. Moreover, CFCs are strong greenhouse gases (GHGs) that would have strengthened global warming. In this study, we investigate the surface weather and climate in a world without the MP at the end of the 21st century, disentangling ozone-mediated and GHG impacts of CFCs. Overall, we avoided 1.7 K global surface warming and a poleward shift in storm tracks.
Xu-Cheng He, Jiali Shen, Siddharth Iyer, Paxton Juuti, Jiangyi Zhang, Mrisha Koirala, Mikko M. Kytökari, Douglas R. Worsnop, Matti Rissanen, Markku Kulmala, Norbert M. Maier, Jyri Mikkilä, Mikko Sipilä, and Juha Kangasluoma
Atmos. Meas. Tech., 16, 4461–4487, https://doi.org/10.5194/amt-16-4461-2023, https://doi.org/10.5194/amt-16-4461-2023, 2023
Short summary
Short summary
In this study, the upgraded multi-scheme chemical ionisation inlet 2 is presented. Sulfuric acid, hypoiodous acid, iodine, sulfur dioxide, and hydroperoxyl radicals are calibrated, and the improved ion optics allow us to detect sulfuric acid and iodine-containing molecules at as low as a few parts per quadrillion by volume. Additionally, we confirm the reliable detection of iodic acid using both the nitrate and bromide chemical ionisation methods under atmospherically relevant conditions.
Marina Friedel, Gabriel Chiodo, Timofei Sukhodolov, James Keeble, Thomas Peter, Svenja Seeber, Andrea Stenke, Hideharu Akiyoshi, Eugene Rozanov, David Plummer, Patrick Jöckel, Guang Zeng, Olaf Morgenstern, and Béatrice Josse
Atmos. Chem. Phys., 23, 10235–10254, https://doi.org/10.5194/acp-23-10235-2023, https://doi.org/10.5194/acp-23-10235-2023, 2023
Short summary
Short summary
Previously, it has been suggested that springtime Arctic ozone depletion might worsen in the coming decades due to climate change, which might counteract the effect of reduced ozone-depleting substances. Here, we show with different chemistry–climate models that springtime Arctic ozone depletion will likely decrease in the future. Further, we explain why models show a large spread in the projected development of Arctic ozone depletion and use the model spread to constrain future projections.
Anita M. Avery, Mariam Fawaz, Leah R. Williams, Tami Bond, and Timothy B. Onasch
Atmos. Chem. Phys., 23, 8837–8854, https://doi.org/10.5194/acp-23-8837-2023, https://doi.org/10.5194/acp-23-8837-2023, 2023
Short summary
Short summary
Pyrolysis is the thermal decomposition of fuels like wood which occurs during combustion or as an isolated process. During combustion, some pyrolysis products are emitted directly, while others are oxidized in the combustion process. This work describes the chemical composition of particle-phase pyrolysis products in order to investigate both the uncombusted emissions from wildfires and the fuel that participates in combustion.
Mitchell W. Alton, Harald J. Stark, Manjula R. Canagaratna, and Eleanor C. Browne
Atmos. Meas. Tech., 16, 3273–3282, https://doi.org/10.5194/amt-16-3273-2023, https://doi.org/10.5194/amt-16-3273-2023, 2023
Short summary
Short summary
Mass spectrometric measurements of atmospheric composition routinely detect hundreds of different ions of varying chemical composition, creating challenges for visualization and data interpretation. We present a new analysis technique to facilitate visualization, while providing greater chemical insight. Additionally, it can aid in identifying the chemical composition of ions. A graphical user interface for performing the analysis is introduced and freely available, enabling broad applications.
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
Atmos. Chem. Phys., 23, 6613–6631, https://doi.org/10.5194/acp-23-6613-2023, https://doi.org/10.5194/acp-23-6613-2023, 2023
Short summary
Short summary
In this study, we present an intercomparison of four different techniques for measuring the chemical composition of nanoparticles. The intercomparison was performed based on the observed chemical composition, calculated volatility, and analysis of 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.
Daniel John Katz, Aroob Abdelhamid, Harald Stark, Manjula R. Canagaratna, Douglas R. Worsnop, and Eleanor C. Browne
Atmos. Chem. Phys., 23, 5567–5585, https://doi.org/10.5194/acp-23-5567-2023, https://doi.org/10.5194/acp-23-5567-2023, 2023
Short summary
Short summary
Ambient ion chemical composition measurements provide insight into trace gases that are precursors for the formation and growth of new aerosol particles. We use a new data analysis approach to increase the chemical information from these measurements. We analyze results from an agricultural region, a little studied land use type that is ~41 % of global land use, and find that the composition of gases important for aerosol formation and growth differs significantly from that in other ecosystems.
Anand Kumar, Kristian Klumpp, Chen Barak, Giora Rytwo, Michael Plötze, Thomas Peter, and Claudia Marcolli
Atmos. Chem. Phys., 23, 4881–4902, https://doi.org/10.5194/acp-23-4881-2023, https://doi.org/10.5194/acp-23-4881-2023, 2023
Short summary
Short summary
Smectites are a major class of clay minerals that are ice nucleation (IN) active. They form platelets that swell or even delaminate in water by intercalation of water between their layers. We hypothesize that at least three smectite layers need to be stacked together to host a critical ice embryo on clay mineral edges and that the larger the surface edge area is, the higher the freezing temperature. Edge sites on such clay particles play a crucial role in imparting IN ability to such particles.
Arseniy Karagodin-Doyennel, Eugene Rozanov, Timofei Sukhodolov, Tatiana Egorova, Jan Sedlacek, and Thomas Peter
Atmos. Chem. Phys., 23, 4801–4817, https://doi.org/10.5194/acp-23-4801-2023, https://doi.org/10.5194/acp-23-4801-2023, 2023
Short summary
Short summary
The future ozone evolution in SOCOLv4 simulations under SSP2-4.5 and SSP5-8.5 scenarios has been assessed for the period 2015–2099 and subperiods using the DLM approach. The SOCOLv4 projects a decline in tropospheric ozone in the 2030s in SSP2-4.5 and in the 2060s in SSP5-8.5. The stratospheric ozone increase is ~3 times higher in SSP5-8.5, confirming the important role of GHGs in ozone evolution. We also showed that tropospheric ozone strongly impacts the total column in the tropics.
Thomas Berkemeier, Matteo Krüger, Aryeh Feinberg, Marcel Müller, Ulrich Pöschl, and Ulrich K. Krieger
Geosci. Model Dev., 16, 2037–2054, https://doi.org/10.5194/gmd-16-2037-2023, https://doi.org/10.5194/gmd-16-2037-2023, 2023
Short summary
Short summary
Kinetic multi-layer models (KMs) successfully describe heterogeneous and multiphase atmospheric chemistry. In applications requiring repeated execution, however, these models can be too expensive. We trained machine learning surrogate models on output of the model KM-SUB and achieved high correlations. The surrogate models run orders of magnitude faster, which suggests potential applicability in global optimization tasks and as sub-modules in large-scale atmospheric models.
Qiaozhi Zha, Wei Huang, Diego Aliaga, Otso Peräkylä, Liine Heikkinen, Alkuin Maximilian Koenig, Cheng Wu, Joonas Enroth, Yvette Gramlich, Jing Cai, Samara Carbone, Armin Hansel, Tuukka Petäjä, Markku Kulmala, Douglas Worsnop, Victoria Sinclair, Radovan Krejci, Marcos Andrade, Claudia Mohr, and Federico Bianchi
Atmos. Chem. Phys., 23, 4559–4576, https://doi.org/10.5194/acp-23-4559-2023, https://doi.org/10.5194/acp-23-4559-2023, 2023
Short summary
Short summary
We investigate the chemical composition of atmospheric cluster ions from January to May 2018 at the high-altitude research station Chacaltaya (5240 m a.s.l.) in the Bolivian Andes. With state-of-the-art mass spectrometers and air mass history analysis, the measured cluster ions exhibited distinct diurnal and seasonal patterns, some of which contributed to new particle formation. Our study will improve the understanding of atmospheric ions and their role in high-altitude new particle formation.
Ella Häkkinen, Jian Zhao, Frans Graeffe, Nicolas Fauré, Jordan E. Krechmer, Douglas Worsnop, Hilkka Timonen, Mikael Ehn, and Juha Kangasluoma
Atmos. Meas. Tech., 16, 1705–1721, https://doi.org/10.5194/amt-16-1705-2023, https://doi.org/10.5194/amt-16-1705-2023, 2023
Short summary
Short summary
Highly oxygenated compounds contribute to the formation and growth of atmospheric organic aerosol and thus impact the global climate. Knowledge of their transformations and fate after condensing into the particle phase has been limited by the lack of suitable detection techniques. Here, we present an online method for measuring highly oxygenated compounds from organic aerosol. We evaluate the performance of the method and demonstrate that the method is applicable to different organic species.
Jian Zhao, Ella Häkkinen, Frans Graeffe, Jordan E. Krechmer, Manjula R. Canagaratna, Douglas R. Worsnop, Juha Kangasluoma, and Mikael Ehn
Atmos. Chem. Phys., 23, 3707–3730, https://doi.org/10.5194/acp-23-3707-2023, https://doi.org/10.5194/acp-23-3707-2023, 2023
Short summary
Short summary
Based on the combined measurements of gas- and particle-phase highly oxygenated organic molecules (HOMs) from α-pinene ozonolysis, enhancement of dimers in particles was observed. We conducted experiments wherein the dimer to monomer (D / M) ratios of HOMs in the gas phase were modified (adding CO / NO) to investigate the effects of the corresponding D / M ratios in the particles. These results are important for a better understanding of secondary organic aerosol formation in the atmosphere.
Kristian Klumpp, Claudia Marcolli, Ana Alonso-Hellweg, Christopher H. Dreimol, and Thomas Peter
Atmos. Chem. Phys., 23, 1579–1598, https://doi.org/10.5194/acp-23-1579-2023, https://doi.org/10.5194/acp-23-1579-2023, 2023
Short summary
Short summary
The prerequisites of a particle surface for efficient ice nucleation are still poorly understood. This study compares the ice nucleation activity of two chemically identical but morphologically different minerals (kaolinite and halloysite). We observe, on average, not only higher ice nucleation activities for halloysite than kaolinite but also higher diversity between individual samples. We identify the particle edges as being the most likely site for ice nucleation.
Lukas Eickhoff, Maddalena Bayer-Giraldi, Naama Reicher, Yinon Rudich, and Thomas Koop
Biogeosciences, 20, 1–14, https://doi.org/10.5194/bg-20-1-2023, https://doi.org/10.5194/bg-20-1-2023, 2023
Short summary
Short summary
The formation of ice is an important process in Earth’s atmosphere, biosphere, and cryosphere, in particular in polar regions. Our research focuses on the influence of the sea ice diatom Fragilariopsis cylindrus and of molecules produced by it upon heterogenous ice nucleation. For that purpose, we studied the freezing of tiny droplets containing the diatoms in a microfluidic device. Together with previous studies, our results suggest a common freezing behaviour of various sea ice diatoms.
Qing Ye, Matthew B. Goss, Jordan E. Krechmer, Francesca Majluf, Alexander Zaytsev, Yaowei Li, Joseph R. Roscioli, Manjula Canagaratna, Frank N. Keutsch, Colette L. Heald, and Jesse H. Kroll
Atmos. Chem. Phys., 22, 16003–16015, https://doi.org/10.5194/acp-22-16003-2022, https://doi.org/10.5194/acp-22-16003-2022, 2022
Short summary
Short summary
The atmospheric oxidation of dimethyl sulfide (DMS) is a major natural source of sulfate particles in the atmosphere. However, its mechanism is poorly constrained. In our work, laboratory measurements and mechanistic modeling were conducted to comprehensively investigate DMS oxidation products and key reaction rates. We find that the peroxy radical (RO2) has a controlling effect on product distribution and aerosol yield, with the isomerization of RO2 leading to the suppression of aerosol yield.
Arseniy Karagodin-Doyennel, Eugene Rozanov, Timofei Sukhodolov, Tatiana Egorova, Jan Sedlacek, William Ball, and Thomas Peter
Atmos. Chem. Phys., 22, 15333–15350, https://doi.org/10.5194/acp-22-15333-2022, https://doi.org/10.5194/acp-22-15333-2022, 2022
Short summary
Short summary
Applying the dynamic linear model, we confirm near-global ozone recovery (55°N–55°S) in the mesosphere, upper and middle stratosphere, and a steady increase in the troposphere. We also show that modern chemistry–climate models (CCMs) like SOCOLv4 may reproduce the observed trend distribution of lower stratospheric ozone, despite exhibiting a lower magnitude and statistical significance. The obtained ozone trend pattern in SOCOLv4 is generally consistent with observations and reanalysis datasets.
Nikou Hamzehpour, Claudia Marcolli, Sara Pashai, Kristian Klumpp, and Thomas Peter
Atmos. Chem. Phys., 22, 14905–14930, https://doi.org/10.5194/acp-22-14905-2022, https://doi.org/10.5194/acp-22-14905-2022, 2022
Short summary
Short summary
Playa surfaces in Iran that emerged through Lake Urmia (LU) desiccation have become a relevant dust source of regional relevance. Here, we identify highly erodible LU playa surfaces and determine their physicochemical properties and mineralogical composition and perform emulsion-freezing experiments with them. We find high ice nucleation activities (up to 250 K) that correlate positively with organic matter and clay content and negatively with pH, salinity, K-feldspars, and quartz.
Nikou Hamzehpour, Claudia Marcolli, Kristian Klumpp, Debora Thöny, and Thomas Peter
Atmos. Chem. Phys., 22, 14931–14956, https://doi.org/10.5194/acp-22-14931-2022, https://doi.org/10.5194/acp-22-14931-2022, 2022
Short summary
Short summary
Dust aerosols from dried lakebeds contain mineral particles, as well as soluble salts and (bio-)organic compounds. Here, we investigate ice nucleation (IN) activity of dust samples from Lake Urmia playa, Iran. We find high IN activity of the untreated samples that decreases after organic matter removal but increases after removing soluble salts and carbonates, evidencing inhibiting effects of soluble salts and carbonates on the IN activity of organic matter and minerals, especially microcline.
Caroline C. Womack, Steven S. Brown, Steven J. Ciciora, Ru-Shan Gao, Richard J. McLaughlin, Michael A. Robinson, Yinon Rudich, and Rebecca A. Washenfelder
Atmos. Meas. Tech., 15, 6643–6652, https://doi.org/10.5194/amt-15-6643-2022, https://doi.org/10.5194/amt-15-6643-2022, 2022
Short summary
Short summary
We present a new miniature instrument to measure nitrogen dioxide (NO2) using cavity-enhanced spectroscopy. NO2 contributes to the formation of pollutants such as ozone and particulate matter, and its concentration can vary widely near sources. We developed this lightweight (3.05 kg) low-power (<35 W) instrument to measure NO2 on uncrewed aircraft vehicles (UAVs) and demonstrate that it has the accuracy and precision needed for atmospheric field measurements.
Paul A. Barrett, Steven J. Abel, Hugh Coe, Ian Crawford, Amie Dobracki, James Haywood, Steve Howell, Anthony Jones, Justin Langridge, Greg M. McFarquhar, Graeme J. Nott, Hannah Price, Jens Redemann, Yohei Shinozuka, Kate Szpek, Jonathan W. Taylor, Robert Wood, Huihui Wu, Paquita Zuidema, Stéphane Bauguitte, Ryan Bennett, Keith Bower, Hong Chen, Sabrina Cochrane, Michael Cotterell, Nicholas Davies, David Delene, Connor Flynn, Andrew Freedman, Steffen Freitag, Siddhant Gupta, David Noone, Timothy B. Onasch, James Podolske, Michael R. Poellot, Sebastian Schmidt, Stephen Springston, Arthur J. Sedlacek III, Jamie Trembath, Alan Vance, Maria A. Zawadowicz, and Jianhao Zhang
Atmos. Meas. Tech., 15, 6329–6371, https://doi.org/10.5194/amt-15-6329-2022, https://doi.org/10.5194/amt-15-6329-2022, 2022
Short summary
Short summary
To better understand weather and climate, it is vital to go into the field and collect observations. Often measurements take place in isolation, but here we compared data from two aircraft and one ground-based site. This was done in order to understand how well measurements made on one platform compared to those made on another. Whilst this is easy to do in a controlled laboratory setting, it is more challenging in the real world, and so these comparisons are as valuable as they are rare.
Marina Friedel, Gabriel Chiodo, Andrea Stenke, Daniela I. V. Domeisen, and Thomas Peter
Atmos. Chem. Phys., 22, 13997–14017, https://doi.org/10.5194/acp-22-13997-2022, https://doi.org/10.5194/acp-22-13997-2022, 2022
Short summary
Short summary
In spring, winds the Arctic stratosphere change direction – an event called final stratospheric warming (FSW). Here, we examine whether the interannual variability in Arctic stratospheric ozone impacts the timing of the FSW. We find that Arctic ozone shifts the FSW to earlier and later dates in years with high and low ozone via the absorption of UV light. The modulation of the FSW by ozone has consequences for surface climate in ozone-rich years, which may result in better seasonal predictions.
Florin N. Isenrich, Nadia Shardt, Michael Rösch, Julia Nette, Stavros Stavrakis, Claudia Marcolli, Zamin A. Kanji, Andrew J. deMello, and Ulrike Lohmann
Atmos. Meas. Tech., 15, 5367–5381, https://doi.org/10.5194/amt-15-5367-2022, https://doi.org/10.5194/amt-15-5367-2022, 2022
Short summary
Short summary
Ice nucleation in the atmosphere influences cloud properties and lifetimes. Microfluidic instruments have recently been used to investigate ice nucleation, but these instruments are typically made out of a polymer that contributes to droplet instability over extended timescales and relatively high temperature uncertainty. To address these drawbacks, we develop and validate a new microfluidic instrument that uses fluoropolymer tubing to extend droplet stability and improve temperature accuracy.
Chao Yan, Yicheng Shen, Dominik Stolzenburg, Lubna Dada, Ximeng Qi, Simo Hakala, Anu-Maija Sundström, Yishuo Guo, Antti Lipponen, Tom V. Kokkonen, Jenni Kontkanen, Runlong Cai, Jing Cai, Tommy Chan, Liangduo Chen, Biwu Chu, Chenjuan Deng, Wei Du, Xiaolong Fan, Xu-Cheng He, Juha Kangasluoma, Joni Kujansuu, Mona Kurppa, Chang Li, Yiran Li, Zhuohui Lin, Yiliang Liu, Yuliang Liu, Yiqun Lu, Wei Nie, Jouni Pulliainen, Xiaohui Qiao, Yonghong Wang, Yifan Wen, Ye Wu, Gan Yang, Lei Yao, Rujing Yin, Gen Zhang, Shaojun Zhang, Feixue Zheng, Ying Zhou, Antti Arola, Johanna Tamminen, Pauli Paasonen, Yele Sun, Lin Wang, Neil M. Donahue, Yongchun Liu, Federico Bianchi, Kaspar R. Daellenbach, Douglas R. Worsnop, Veli-Matti Kerminen, Tuukka Petäjä, Aijun Ding, Jingkun Jiang, and Markku Kulmala
Atmos. Chem. Phys., 22, 12207–12220, https://doi.org/10.5194/acp-22-12207-2022, https://doi.org/10.5194/acp-22-12207-2022, 2022
Short summary
Short summary
Atmospheric new particle formation (NPF) is a dominant source of atmospheric ultrafine particles. In urban environments, traffic emissions are a major source of primary pollutants, but their contribution to NPF remains under debate. During the COVID-19 lockdown, traffic emissions were significantly reduced, providing a unique chance to examine their relevance to NPF. Based on our comprehensive measurements, we demonstrate that traffic emissions alone are not able to explain the NPF in Beijing.
Clare E. Singer, Benjamin W. Clouser, Sergey M. Khaykin, Martina Krämer, Francesco Cairo, Thomas Peter, Alexey Lykov, Christian Rolf, Nicole Spelten, Armin Afchine, Simone Brunamonti, and Elisabeth J. Moyer
Atmos. Meas. Tech., 15, 4767–4783, https://doi.org/10.5194/amt-15-4767-2022, https://doi.org/10.5194/amt-15-4767-2022, 2022
Short summary
Short summary
In situ measurements of water vapor in the upper troposphere are necessary to study cloud formation and hydration of the stratosphere but challenging due to cold–dry conditions. We compare measurements from three water vapor instruments from the StratoClim campaign in 2017. In clear sky (clouds), point-by-point differences were <1.5±8 % (<1±8 %). This excellent agreement allows detection of fine-scale structures required to understand the impact of convection on stratospheric water vapor.
Lisa J. Beck, Siegfried Schobesberger, Heikki Junninen, Janne Lampilahti, Antti Manninen, Lubna Dada, Katri Leino, Xu-Cheng He, Iida Pullinen, Lauriane L. J. Quéléver, Anna Franck, Pyry Poutanen, Daniela Wimmer, Frans Korhonen, Mikko Sipilä, Mikael Ehn, Douglas R. Worsnop, Veli-Matti Kerminen, Tuukka Petäjä, Markku Kulmala, and Jonathan Duplissy
Atmos. Chem. Phys., 22, 8547–8577, https://doi.org/10.5194/acp-22-8547-2022, https://doi.org/10.5194/acp-22-8547-2022, 2022
Short summary
Short summary
The presented article introduces an overview of atmospheric ions and their composition above the boreal forest. We provide the results of an extensive airborne measurement campaign with an air ion mass spectrometer and particle measurements, showing their diurnal evolution within the boundary layer and free troposphere. In addition, we compare the airborne dataset with the co-located data from the ground at SMEAR II station, Finland.
Lauriane L. J. Quéléver, Lubna Dada, Eija Asmi, Janne Lampilahti, Tommy Chan, Jonathan E. Ferrara, Gustavo E. Copes, German Pérez-Fogwill, Luis Barreira, Minna Aurela, Douglas R. Worsnop, Tuija Jokinen, and Mikko Sipilä
Atmos. Chem. Phys., 22, 8417–8437, https://doi.org/10.5194/acp-22-8417-2022, https://doi.org/10.5194/acp-22-8417-2022, 2022
Short summary
Short summary
Understanding how aerosols form is crucial for correctly modeling the climate and improving future predictions. This work provides extensive analysis of aerosol particles and their precursors at Marambio Station, Antarctic Peninsula. We show that sulfuric acid, ammonia, and dimethylamine are key contributors to the frequent new particle formation events observed at the site. We discuss nucleation mechanisms and highlight the need for targeted measurement to fully understand these processes.
Patrick Weber, Andreas Petzold, Oliver F. Bischof, Benedikt Fischer, Marcel Berg, Andrew Freedman, Timothy B. Onasch, and Ulrich Bundke
Atmos. Meas. Tech., 15, 3279–3296, https://doi.org/10.5194/amt-15-3279-2022, https://doi.org/10.5194/amt-15-3279-2022, 2022
Short summary
Short summary
In our laboratory closure study, we measured the full set of aerosol optical properties for different light-absorbing aerosols using a set of instruments.
Our key finding is that the extensive and intensive aerosol optical properties obtained agree with data from reference instruments, except the absorption Ångström exponent of externally mixed aerosols. The reported uncertainty in the single-scattering albedo fulfils the defined goals for Global Climate Observing System applications of 10 %.
Yu Wang, Aristeidis Voliotis, Dawei Hu, Yunqi Shao, Mao Du, Ying Chen, Judith Kleinheins, Claudia Marcolli, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 22, 4149–4166, https://doi.org/10.5194/acp-22-4149-2022, https://doi.org/10.5194/acp-22-4149-2022, 2022
Short summary
Short summary
Aerosol water uptake plays a key role in atmospheric physicochemical processes. We designed chamber experiments on aerosol water uptake of secondary organic aerosol (SOA) from mixed biogenic and anthropogenic precursors with inorganic seed. Our results highlight this chemical composition influences the reconciliation of the sub- and super-saturated water uptake, providing laboratory evidence for understanding the chemical controls of water uptake of the multi-component aerosol.
Kristian Klumpp, Claudia Marcolli, and Thomas Peter
Atmos. Chem. Phys., 22, 3655–3673, https://doi.org/10.5194/acp-22-3655-2022, https://doi.org/10.5194/acp-22-3655-2022, 2022
Short summary
Short summary
Surface interactions with solutes can significantly alter the ice nucleation activity of mineral dust. Past studies revealed the sensitivity of microcline, one of the most ice-active types of dust in the atmosphere, to inorganic solutes. This study focuses on the interaction of microcline with bio-organic substances and the resulting effects on its ice nucleation activity. We observe strongly hampered ice nucleation activity due to the presence of carboxylic and amino acids but not for polyols.
Debra K. Weisenstein, Daniele Visioni, Henning Franke, Ulrike Niemeier, Sandro Vattioni, Gabriel Chiodo, Thomas Peter, and David W. Keith
Atmos. Chem. Phys., 22, 2955–2973, https://doi.org/10.5194/acp-22-2955-2022, https://doi.org/10.5194/acp-22-2955-2022, 2022
Short summary
Short summary
This paper explores a potential method of geoengineering that could be used to slow the rate of change of climate over decadal scales. We use three climate models to explore how injections of accumulation-mode sulfuric acid aerosol change the large-scale stratospheric particle size distribution and radiative forcing response for the chosen scenarios. Radiative forcing per unit sulfur injected and relative to the change in aerosol burden is larger with particulate than with SO2 injections.
Zhi-Hui Zhang, Elena Hartner, Battist Utinger, Benjamin Gfeller, Andreas Paul, Martin Sklorz, Hendryk Czech, Bin Xia Yang, Xin Yi Su, Gert Jakobi, Jürgen Orasche, Jürgen Schnelle-Kreis, Seongho Jeong, Thomas Gröger, Michal Pardo, Thorsten Hohaus, Thomas Adam, Astrid Kiendler-Scharr, Yinon Rudich, Ralf Zimmermann, and Markus Kalberer
Atmos. Chem. Phys., 22, 1793–1809, https://doi.org/10.5194/acp-22-1793-2022, https://doi.org/10.5194/acp-22-1793-2022, 2022
Short summary
Short summary
Using a novel setup, we comprehensively characterized the formation of particle-bound reactive oxygen species (ROS) in anthropogenic and biogenic secondary organic aerosols (SOAs). We found that more than 90 % of all ROS components in both SOA types have a short lifetime. Our results also show that photochemical aging promotes particle-bound ROS production and enhances the oxidative potential of the aerosols. We found consistent results between chemical-based and biological-based ROS analyses.
Hang Yin, Jing Dou, Liviana Klein, Ulrich K. Krieger, Alison Bain, Brandon J. Wallace, Thomas C. Preston, and Andreas Zuend
Atmos. Chem. Phys., 22, 973–1013, https://doi.org/10.5194/acp-22-973-2022, https://doi.org/10.5194/acp-22-973-2022, 2022
Short summary
Short summary
Iodine and carbonate species are important components in marine and dust aerosols, respectively. We introduce an extended version of the AIOMFAC thermodynamic mixing model, which includes the ions I−, IO3−, HCO3−, CO32−, OH−, and CO2(aq) as new species, and we discuss two methods for solving the carbonate dissociation equilibria numerically. We also present new experimental water activity data for aqueous iodide and iodate systems.
Mikko Sipilä, Nina Sarnela, Kimmo Neitola, Totti Laitinen, Deniz Kemppainen, Lisa Beck, Ella-Maria Duplissy, Salla Kuittinen, Tuuli Lehmusjärvi, Janne Lampilahti, Veli-Matti Kerminen, Katrianne Lehtipalo, Pasi P. Aalto, Petri Keronen, Erkki Siivola, Pekka A. Rantala, Douglas R. Worsnop, Markku Kulmala, Tuija Jokinen, and Tuukka Petäjä
Atmos. Chem. Phys., 21, 17559–17576, https://doi.org/10.5194/acp-21-17559-2021, https://doi.org/10.5194/acp-21-17559-2021, 2021
Short summary
Short summary
Metallurgical industry in Kola peninsula is a large source of air pollution in the (sub-)Arctic domain. Sulfur dioxide emissions from the ore smelters are transported across large areas. We investigated sulfur dioxide and its transformation to sulfuric acid aerosol particles during winter months in Finnish Lapland, close to Kola industrial areas. We observed intense formation of new aerosol particles despite the low solar radiation intensity, often required for new particle formation elsewhere.
Dongyu S. Wang, Chuan Ping Lee, Jordan E. Krechmer, Francesca Majluf, Yandong Tong, Manjula R. Canagaratna, Julia Schmale, André S. H. Prévôt, Urs Baltensperger, Josef Dommen, Imad El Haddad, Jay G. Slowik, and David M. Bell
Atmos. Meas. Tech., 14, 6955–6972, https://doi.org/10.5194/amt-14-6955-2021, https://doi.org/10.5194/amt-14-6955-2021, 2021
Short summary
Short summary
To understand the sources and fate of particulate matter in the atmosphere, the ability to quantitatively describe its chemical composition is essential. In this work, we developed a calibration method for a state-of-the-art measurement technique without the need for chemical standards. Statistical analyses identified the driving factors behind instrument sensitivity variability towards individual components of particulate matter.
Arseniy Karagodin-Doyennel, Eugene Rozanov, Timofei Sukhodolov, Tatiana Egorova, Alfonso Saiz-Lopez, Carlos A. Cuevas, Rafael P. Fernandez, Tomás Sherwen, Rainer Volkamer, Theodore K. Koenig, Tanguy Giroud, and Thomas Peter
Geosci. Model Dev., 14, 6623–6645, https://doi.org/10.5194/gmd-14-6623-2021, https://doi.org/10.5194/gmd-14-6623-2021, 2021
Short summary
Short summary
Here, we present the iodine chemistry module in the SOCOL-AERv2 model. The obtained iodine distribution demonstrated a good agreement when validated against other simulations and available observations. We also estimated the iodine influence on ozone in the case of present-day iodine emissions, the sensitivity of ozone to doubled iodine emissions, and when considering only organic or inorganic iodine sources. The new model can be used as a tool for further studies of iodine effects on ozone.
Chenyang Bi, Jordan E. Krechmer, Graham O. Frazier, Wen Xu, Andrew T. Lambe, Megan S. Claflin, Brian M. Lerner, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 14, 6835–6850, https://doi.org/10.5194/amt-14-6835-2021, https://doi.org/10.5194/amt-14-6835-2021, 2021
Short summary
Short summary
Iodide-adduct chemical ionization mass spectrometry (I-CIMS) has been widely used to analyze airborne organics. In this study, I-CIMS sensitivities of isomers within a formula are found to generally vary by 1 and up to 2 orders of magnitude. Comparisons between measured and predicted moles, obtained using a voltage-scanning calibration approach, show that predictions for individual compounds or formulas might carry high uncertainty, yet the summed moles of analytes agree reasonably well.
Mariam Fawaz, Anita Avery, Timothy B. Onasch, Leah R. Williams, and Tami C. Bond
Atmos. Chem. Phys., 21, 15605–15618, https://doi.org/10.5194/acp-21-15605-2021, https://doi.org/10.5194/acp-21-15605-2021, 2021
Short summary
Short summary
Biomass burning is responsible for 90 % of the emissions of primary organic aerosols to the atmosphere. Emissions from biomass burning sources are considered chaotic. In this work, we developed a controlled experimental approach to understand the controlling factors in emission. Our results showed that emissions are repeatable and deterministic and that emissions from wood can be constrained.
Bernd Kärcher and Claudia Marcolli
Atmos. Chem. Phys., 21, 15213–15220, https://doi.org/10.5194/acp-21-15213-2021, https://doi.org/10.5194/acp-21-15213-2021, 2021
Short summary
Short summary
Aerosol–cloud interactions play an important role in climate change. Simulations of the competition between homogeneous solution droplet freezing and heterogeneous ice nucleation can be compromised by the misapplication of ice-active particle fractions frequently derived from laboratory measurements or parametrizations. Our study frames the problem and establishes a solution that is easy to implement in cloud models.
Chenyang Bi, Jordan E. Krechmer, Manjula R. Canagaratna, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 14, 6551–6560, https://doi.org/10.5194/amt-14-6551-2021, https://doi.org/10.5194/amt-14-6551-2021, 2021
Short summary
Short summary
Calibration techniques have been recently developed to log-linearly correlate analyte sensitivity with CIMS operating conditions particularly for compounds without authentic standards. In this work, we examine the previously ignored bias in the log-linear-based calibration method and estimate an average bias of 30 %, with 1 order of magnitude for less sensitive compounds in some circumstances. A step-by-step guide was provided to reduce and even remove the bias.
Quanfu He, Zheng Fang, Ofir Shoshanim, Steven S. Brown, and Yinon Rudich
Atmos. Chem. Phys., 21, 14927–14940, https://doi.org/10.5194/acp-21-14927-2021, https://doi.org/10.5194/acp-21-14927-2021, 2021
Short summary
Short summary
Rayleigh scattering and absorption cross sections for CO2, N2O, SF6, O2, and CH4 were measured between 307 and 725 nm. New dispersion relations for N2O, SF6, and CH4 in the UV–vis range were derived. This study provides refractive index dispersion relations, scattering, and absorption cross sections which are highly needed for accurate instrument calibration and for improved accuracy of Rayleigh scattering parameterizations for major greenhouse gases in Earth's atmosphere.
Yuliang Liu, Wei Nie, Yuanyuan Li, Dafeng Ge, Chong Liu, Zhengning Xu, Liangduo Chen, Tianyi Wang, Lei Wang, Peng Sun, Ximeng Qi, Jiaping Wang, Zheng Xu, Jian Yuan, Chao Yan, Yanjun Zhang, Dandan Huang, Zhe Wang, Neil M. Donahue, Douglas Worsnop, Xuguang Chi, Mikael Ehn, and Aijun Ding
Atmos. Chem. Phys., 21, 14789–14814, https://doi.org/10.5194/acp-21-14789-2021, https://doi.org/10.5194/acp-21-14789-2021, 2021
Short summary
Short summary
Oxygenated organic molecules (OOMs) are crucial intermediates linking volatile organic compounds to secondary organic aerosols. Using nitrate time-of-flight chemical ionization mass spectrometry in eastern China, we performed positive matrix factorization (PMF) on binned OOM mass spectra. We reconstructed over 1000 molecules from 14 derived PMF factors and identified about 72 % of the observed OOMs as organic nitrates, highlighting the decisive role of NOx in OOM formation in populated areas.
Mao Xiao, Christopher R. Hoyle, Lubna Dada, Dominik Stolzenburg, Andreas Kürten, Mingyi Wang, Houssni Lamkaddam, Olga Garmash, Bernhard Mentler, Ugo Molteni, Andrea Baccarini, Mario Simon, Xu-Cheng He, Katrianne Lehtipalo, Lauri R. Ahonen, Rima Baalbaki, Paulus S. Bauer, Lisa Beck, David Bell, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, António Dias, Jonathan Duplissy, Henning Finkenzeller, Hamish Gordon, Victoria Hofbauer, Changhyuk Kim, Theodore K. Koenig, Janne Lampilahti, Chuan Ping Lee, Zijun Li, Huajun Mai, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Serge Mathot, Roy L. Mauldin, Wei Nie, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti Rissanen, Siegfried Schobesberger, Simone Schuchmann, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Robert Wagner, Yonghong Wang, Lena Weitz, Daniela Wimmer, Yusheng Wu, Chao Yan, Penglin Ye, Qing Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Ken Carslaw, Joachim Curtius, Armin Hansel, Rainer Volkamer, Paul M. Winkler, Richard C. Flagan, Markku Kulmala, Douglas R. Worsnop, Jasper Kirkby, Neil M. Donahue, Urs Baltensperger, Imad El Haddad, and Josef Dommen
Atmos. Chem. Phys., 21, 14275–14291, https://doi.org/10.5194/acp-21-14275-2021, https://doi.org/10.5194/acp-21-14275-2021, 2021
Short summary
Short summary
Experiments at CLOUD show that in polluted environments new particle formation (NPF) is largely driven by the formation of sulfuric acid–base clusters, stabilized by amines, high ammonia concentrations or lower temperatures. While oxidation products of aromatics can nucleate, they play a minor role in urban NPF. Our experiments span 4 orders of magnitude variation of observed NPF rates in ambient conditions. We provide a framework based on NPF and growth rates to interpret ambient observations.
Timofei Sukhodolov, Tatiana Egorova, Andrea Stenke, William T. Ball, Christina Brodowsky, Gabriel Chiodo, Aryeh Feinberg, Marina Friedel, Arseniy Karagodin-Doyennel, Thomas Peter, Jan Sedlacek, Sandro Vattioni, and Eugene Rozanov
Geosci. Model Dev., 14, 5525–5560, https://doi.org/10.5194/gmd-14-5525-2021, https://doi.org/10.5194/gmd-14-5525-2021, 2021
Short summary
Short summary
This paper features the new atmosphere–ocean–aerosol–chemistry–climate model SOCOLv4.0 and its validation. The model performance is evaluated against reanalysis products and observations of atmospheric circulation and trace gas distribution, with a focus on stratospheric processes. Although we identified some problems to be addressed in further model upgrades, we demonstrated that SOCOLv4.0 is already well suited for studies related to chemistry–climate–aerosol interactions.
Benjamin Sumlin, Edward Fortner, Andrew Lambe, Nishit J. Shetty, Conner Daube, Pai Liu, Francesca Majluf, Scott Herndon, and Rajan K. Chakrabarty
Atmos. Chem. Phys., 21, 11843–11856, https://doi.org/10.5194/acp-21-11843-2021, https://doi.org/10.5194/acp-21-11843-2021, 2021
Short summary
Short summary
We present a comparison of the changes to light absorption behavior and chemical composition of wildfire smoke particles from day- and nighttime oxidation processes and discuss the results within the context of previous laboratory findings.
Ralf Weigel, Christoph Mahnke, Manuel Baumgartner, Antonis Dragoneas, Bärbel Vogel, Felix Ploeger, Silvia Viciani, Francesco D'Amato, Silvia Bucci, Bernard Legras, Beiping Luo, and Stephan Borrmann
Atmos. Chem. Phys., 21, 11689–11722, https://doi.org/10.5194/acp-21-11689-2021, https://doi.org/10.5194/acp-21-11689-2021, 2021
Short summary
Short summary
In July and August 2017, eight StratoClim mission flights of the Geophysica reached up to 20 km in the Asian monsoon anticyclone. New particle formation (NPF) was identified in situ by abundant nucleation-mode aerosols (6–15 nm in diameter) with mixing ratios of up to 50 000 mg−1. NPF occurred most frequently at 12–16 km with fractions of non-volatile residues of down to 15 %. Abundance and productivity of observed NPF indicate its ability to promote the Asian tropopause aerosol layer.
Louise N. Jensen, Manjula R. Canagaratna, Kasper Kristensen, Lauriane L. J. Quéléver, Bernadette Rosati, Ricky Teiwes, Marianne Glasius, Henrik B. Pedersen, Mikael Ehn, and Merete Bilde
Atmos. Chem. Phys., 21, 11545–11562, https://doi.org/10.5194/acp-21-11545-2021, https://doi.org/10.5194/acp-21-11545-2021, 2021
Short summary
Short summary
This work targets the chemical composition of α-pinene-derived secondary organic aerosol (SOA) formed in the temperature range from -15 to 20°C. Experiments were conducted in an atmospheric simulation chamber. Positive matrix factorization analysis of data obtained by a high-resolution time-of-flight aerosol mass spectrometer shows that the elemental aerosol composition is controlled by the initial α-pinene concentration and temperature during SOA 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.
Benjamin A. Nault, Duseong S. Jo, Brian C. McDonald, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Jason C. Schroder, James Allan, Donald R. Blake, Manjula R. Canagaratna, Hugh Coe, Matthew M. Coggon, Peter F. DeCarlo, Glenn S. Diskin, Rachel Dunmore, Frank Flocke, Alan Fried, Jessica B. Gilman, Georgios Gkatzelis, Jacqui F. Hamilton, Thomas F. Hanisco, Patrick L. Hayes, Daven K. Henze, Alma Hodzic, James Hopkins, Min Hu, L. Greggory Huey, B. Thomas Jobson, William C. Kuster, Alastair Lewis, Meng Li, Jin Liao, M. Omar Nawaz, Ilana B. Pollack, Jeffrey Peischl, Bernhard Rappenglück, Claire E. Reeves, Dirk Richter, James M. Roberts, Thomas B. Ryerson, Min Shao, Jacob M. Sommers, James Walega, Carsten Warneke, Petter Weibring, Glenn M. Wolfe, Dominique E. Young, Bin Yuan, Qiang Zhang, Joost A. de Gouw, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 11201–11224, https://doi.org/10.5194/acp-21-11201-2021, https://doi.org/10.5194/acp-21-11201-2021, 2021
Short summary
Short summary
Secondary organic aerosol (SOA) is an important aspect of poor air quality for urban regions around the world, where a large fraction of the population lives. However, there is still large uncertainty in predicting SOA in urban regions. Here, we used data from 11 urban campaigns and show that the variability in SOA production in these regions is predictable and is explained by key emissions. These results are used to estimate the premature mortality associated with SOA in urban regions.
Liine Heikkinen, Mikko Äijälä, Kaspar R. Daellenbach, Gang Chen, Olga Garmash, Diego Aliaga, Frans Graeffe, Meri Räty, Krista Luoma, Pasi Aalto, Markku Kulmala, Tuukka Petäjä, Douglas Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 21, 10081–10109, https://doi.org/10.5194/acp-21-10081-2021, https://doi.org/10.5194/acp-21-10081-2021, 2021
Short summary
Short summary
In many locations worldwide aerosol particles have been shown to be made up of organic aerosol (OA). The boreal forest is a region where aerosol particles possess a high OA mass fraction. Here, we studied OA composition using the longest time series of OA composition ever obtained from a boreal environment. For this purpose, we tested a new analysis framework and discovered that most of the OA was highly oxidized, with strong seasonal behaviour reflecting different sources in summer and winter.
Michael Weimer, Jennifer Buchmüller, Lars Hoffmann, Ole Kirner, Beiping Luo, Roland Ruhnke, Michael Steiner, Ines Tritscher, and Peter Braesicke
Atmos. Chem. Phys., 21, 9515–9543, https://doi.org/10.5194/acp-21-9515-2021, https://doi.org/10.5194/acp-21-9515-2021, 2021
Short summary
Short summary
We show that we are able to directly simulate polar stratospheric clouds formed locally in a mountain wave and represent their effect on the ozone chemistry with the global atmospheric chemistry model ICON-ART. Thus, we show the first simulations that close the gap between directly resolved mountain-wave-induced polar stratospheric clouds and their representation at coarse global resolutions.
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.
Chenshuo Ye, Bin Yuan, Yi Lin, Zelong Wang, Weiwei Hu, Tiange Li, Wei Chen, Caihong Wu, Chaomin Wang, Shan Huang, Jipeng Qi, Baolin Wang, Chen Wang, Wei Song, Xinming Wang, E Zheng, Jordan E. Krechmer, Penglin Ye, Zhanyi Zhang, Xuemei Wang, Douglas R. Worsnop, and Min Shao
Atmos. Chem. Phys., 21, 8455–8478, https://doi.org/10.5194/acp-21-8455-2021, https://doi.org/10.5194/acp-21-8455-2021, 2021
Short summary
Short summary
We performed measurements of gaseous and particulate organic compounds using a state-of-the-art online mass spectrometer in urban air. Using the dataset, we provide a holistic chemical characterization of oxygenated organic compounds in the polluted urban atmosphere, which can serve as a reference for the future field measurements of organic compounds in cities.
Chenyang Bi, Jordan E. Krechmer, Graham O. Frazier, Wen Xu, Andrew T. Lambe, Megan S. Claflin, Brian M. Lerner, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 14, 3895–3907, https://doi.org/10.5194/amt-14-3895-2021, https://doi.org/10.5194/amt-14-3895-2021, 2021
Short summary
Short summary
Measurement techniques that can achieve molecular characterizations are necessary to understand the differences of fate and transport within isomers produced in the atmospheric oxidation process. In this work, we develop an instrument to conduct isomer-resolved measurements of particle-phase organics. We assess the number of isomers per chemical formula in atmospherically relevant samples and examine the feasibility of extending the use of an existing instrument to a broader range of analytes.
Claudia Marcolli, Fabian Mahrt, and Bernd Kärcher
Atmos. Chem. Phys., 21, 7791–7843, https://doi.org/10.5194/acp-21-7791-2021, https://doi.org/10.5194/acp-21-7791-2021, 2021
Short summary
Short summary
Pores are aerosol particle features that trigger ice nucleation, as they take up water by capillary condensation below water saturation that freezes at low temperatures. The pore ice can then grow into macroscopic ice crystals making up cirrus clouds. Here, we investigate the pores in soot aggregates responsible for pore condensation and freezing (PCF). Moreover, we present a framework to parameterize soot PCF that is able to predict the ice nucleation activity based on soot properties.
Weiqi Xu, Masayuki Takeuchi, Chun Chen, Yanmei Qiu, Conghui Xie, Wanyun Xu, Nan Ma, Douglas R. Worsnop, Nga Lee Ng, and Yele Sun
Atmos. Meas. Tech., 14, 3693–3705, https://doi.org/10.5194/amt-14-3693-2021, https://doi.org/10.5194/amt-14-3693-2021, 2021
Short summary
Short summary
Here we developed a method for estimation of particulate organic nitrates (pON) from the measurements of a high-resolution aerosol mass spectrometer coupled with a thermodenuder based on the volatility differences between inorganic nitrate and pON. The results generally had improvements in reducing negative values due to the influences of a high concentration of inorganic nitrate and a constant ratio of NO+ to NO2+ of organic nitrates (RON).
Anna L. Hodshire, Emily Ramnarine, Ali Akherati, Matthew L. Alvarado, Delphine K. Farmer, Shantanu H. Jathar, Sonia M. Kreidenweis, Chantelle R. Lonsdale, Timothy B. Onasch, Stephen R. Springston, Jian Wang, Yang Wang, Lawrence I. Kleinman, Arthur J. Sedlacek III, and Jeffrey R. Pierce
Atmos. Chem. Phys., 21, 6839–6855, https://doi.org/10.5194/acp-21-6839-2021, https://doi.org/10.5194/acp-21-6839-2021, 2021
Short summary
Short summary
Biomass burning emits particles and vapors that can impact both health and climate. Here, we investigate the role of dilution in the evolution of aerosol size and composition in observed US wildfire smoke plumes. Centers of plumes dilute more slowly than edges. We see differences in concentrations and composition between the centers and edges both in the first measurement and in subsequent measurements. Our findings support the hypothesis that plume dilution influences smoke aging.
Mutian Ma, Laura-Hélèna Rivellini, YuXi Cui, Megan D. Willis, Rio Wilkie, Jonathan P. D. Abbatt, Manjula R. Canagaratna, Junfeng Wang, Xinlei Ge, and Alex K. Y. Lee
Atmos. Meas. Tech., 14, 2799–2812, https://doi.org/10.5194/amt-14-2799-2021, https://doi.org/10.5194/amt-14-2799-2021, 2021
Short summary
Short summary
Chemical characterization of organic coatings is important to advance our understanding of the physio-chemical properties and atmospheric processing of black carbon (BC) particles. This work develops two approaches to improve the elemental analysis of oxygenated organic coatings using a soot-particle aerosol mass spectrometer. Analyzing ambient data with the new approaches indicated that secondary organics that coated on BC were likely less oxygenated compared to those externally mixed with BC.
Steven J. Campbell, Kate Wolfer, Battist Utinger, Joe Westwood, Zhi-Hui Zhang, Nicolas Bukowiecki, Sarah S. Steimer, Tuan V. Vu, Jingsha Xu, Nicholas Straw, Steven Thomson, Atallah Elzein, Yele Sun, Di Liu, Linjie Li, Pingqing Fu, Alastair C. Lewis, Roy M. Harrison, William J. Bloss, Miranda Loh, Mark R. Miller, Zongbo Shi, and Markus Kalberer
Atmos. Chem. Phys., 21, 5549–5573, https://doi.org/10.5194/acp-21-5549-2021, https://doi.org/10.5194/acp-21-5549-2021, 2021
Short summary
Short summary
In this study, we quantify PM2.5 oxidative potential (OP), a metric widely suggested as a potential measure of particle toxicity, in Beijing in summer and winter using four acellular assays. We correlate PM2.5 OP with a comprehensive range of atmospheric and particle composition measurements, demonstrating inter-assay differences and seasonal variation of PM2.5 OP. Using multivariate statistical analysis, we highlight specific particle chemical components and sources that influence OP.
Weiqi Xu, Chun Chen, Yanmei Qiu, Ying Li, Zhiqiang Zhang, Eleni Karnezi, Spyros N. Pandis, Conghui Xie, Zhijie Li, Jiaxing Sun, Nan Ma, Wanyun Xu, Pingqing Fu, Zifa Wang, Jiang Zhu, Douglas R. Worsnop, Nga Lee Ng, and Yele Sun
Atmos. Chem. Phys., 21, 5463–5476, https://doi.org/10.5194/acp-21-5463-2021, https://doi.org/10.5194/acp-21-5463-2021, 2021
Short summary
Short summary
Here aerosol volatility and viscosity at a rural site (Gucheng) and an urban site (Beijing) in the North China Plain (NCP) were investigated in summer and winter. Our results showed that organic aerosol (OA) in winter in the NCP is more volatile than that in summer due to enhanced primary emissions from coal combustion and biomass burning. We also found that OA existed mainly as a solid in winter in Beijing but as semisolids in Beijing in summer and Gucheng in winter.
Haiyan Li, Manjula R. Canagaratna, Matthieu Riva, Pekka Rantala, Yanjun Zhang, Steven Thomas, Liine Heikkinen, Pierre-Marie Flaud, Eric Villenave, Emilie Perraudin, Douglas Worsnop, Markku Kulmala, Mikael Ehn, and Federico Bianchi
Atmos. Chem. Phys., 21, 4123–4147, https://doi.org/10.5194/acp-21-4123-2021, https://doi.org/10.5194/acp-21-4123-2021, 2021
Short summary
Short summary
For the first time, we performed binPMF analysis on the complex mass spectra acquired with the Vocus PTR-TOF in two European pine forests and identified various primary emission sources and secondary oxidation processes of atmospheric organic vapors, i.e., terpenes and their oxidation products, with varying oxidation degrees. Further insights were gained regarding monoterpene and sesquiterpene reactions based on the interpretation results.
Jingchuan Chen, Zhijun Wu, Jie Chen, Naama Reicher, Xin Fang, Yinon Rudich, and Min Hu
Atmos. Chem. Phys., 21, 3491–3506, https://doi.org/10.5194/acp-21-3491-2021, https://doi.org/10.5194/acp-21-3491-2021, 2021
Short summary
Short summary
Asian mineral dust is a crucial contributor to global ice-nucleating particles (INPs), while its size-resolved information on freezing activity is extremely rare. Here we conducted the first known INP measurements of size-resolved airborne East Asian dust particles. An explicit size dependence of both INP concentration and surface
ice-active-site density was observed. The new parameterizations can be widely applied in models to better characterize and predict ice nucleation activities of dust.
Julia Perim de Faria, Ulrich Bundke, Andrew Freedman, Timothy B. Onasch, and Andreas Petzold
Atmos. Meas. Tech., 14, 1635–1653, https://doi.org/10.5194/amt-14-1635-2021, https://doi.org/10.5194/amt-14-1635-2021, 2021
Short summary
Short summary
An evaluation of the performance and accuracy of a Cavity Attenuated Phase-Shift Single Scattering Albedo Monitor (CAPS PMSSA; Aerodyne Research, Inc.) was conducted in an optical-closure study with proven technologies for aerosol particle optical-property measurements. This study demonstrates that the CAPS PMSSA is a robust and reliable instrument for the direct measurement of the particle scattering and extinction coefficients and thus single-scattering albedo.
Manuel Graf, Philipp Scheidegger, André Kupferschmid, Herbert Looser, Thomas Peter, Ruud Dirksen, Lukas Emmenegger, and Béla Tuzson
Atmos. Meas. Tech., 14, 1365–1378, https://doi.org/10.5194/amt-14-1365-2021, https://doi.org/10.5194/amt-14-1365-2021, 2021
Short summary
Short summary
Water vapor is the most important natural greenhouse gas. The accurate and frequent measurement of its abundance, especially in the upper troposphere and lower stratosphere (UTLS), is technically challenging. We developed and characterized a mid-IR absorption spectrometer for highly accurate water vapor measurements in the UTLS. The instrument is sufficiently small and lightweight (3.9 kg) to be carried by meteorological balloons, which enables frequent and cost-effective soundings.
Runlong Cai, Chao Yan, Dongsen Yang, Rujing Yin, Yiqun Lu, Chenjuan Deng, Yueyun Fu, Jiaxin Ruan, Xiaoxiao Li, Jenni Kontkanen, Qiang Zhang, Juha Kangasluoma, Yan Ma, Jiming Hao, Douglas R. Worsnop, Federico Bianchi, Pauli Paasonen, Veli-Matti Kerminen, Yongchun Liu, Lin Wang, Jun Zheng, Markku Kulmala, and Jingkun Jiang
Atmos. Chem. Phys., 21, 2457–2468, https://doi.org/10.5194/acp-21-2457-2021, https://doi.org/10.5194/acp-21-2457-2021, 2021
Short summary
Short summary
Based on long-term measurements, we discovered that the collision of H2SO4–amine clusters is the governing mechanism that initializes fast new particle formation in the polluted atmospheric environment of urban Beijing. The mechanism and the governing factors for H2SO4–amine nucleation in the polluted atmosphere are quantitatively investigated in this study.
Michael Steiner, Beiping Luo, Thomas Peter, Michael C. Pitts, and Andrea Stenke
Geosci. Model Dev., 14, 935–959, https://doi.org/10.5194/gmd-14-935-2021, https://doi.org/10.5194/gmd-14-935-2021, 2021
Short summary
Short summary
We evaluate polar stratospheric clouds (PSCs) as simulated by the chemistry–climate model (CCM) SOCOLv3.1 in comparison with measurements by the CALIPSO satellite. A cold bias results in an overestimated PSC area and mountain-wave ice is underestimated, but we find overall good temporal and spatial agreement of PSC occurrence and composition. This work confirms previous studies indicating that simplified PSC schemes may also achieve good approximations of the fundamental properties of PSCs.
Arttu Ylisirniö, Luis M. F. Barreira, Iida Pullinen, Angela Buchholz, John Jayne, Jordan E. Krechmer, Douglas R. Worsnop, Annele Virtanen, and Siegfried Schobesberger
Atmos. Meas. Tech., 14, 355–367, https://doi.org/10.5194/amt-14-355-2021, https://doi.org/10.5194/amt-14-355-2021, 2021
Short summary
Short summary
FIGAERO-ToF-CIMS enables online volatility measurements of chemical compounds in ambient aerosols. Previously published volatility calibration results however differ from each other significantly. In this study we investigate the reason for this discrepancy. We found a major source of error in the widely used syringe deposition method and propose a new method for volatility calibration by using atomized calibration compounds.
Teresa Jorge, Simone Brunamonti, Yann Poltera, Frank G. Wienhold, Bei P. Luo, Peter Oelsner, Sreeharsha Hanumanthu, Bhupendra B. Singh, Susanne Körner, Ruud Dirksen, Manish Naja, Suvarna Fadnavis, and Thomas Peter
Atmos. Meas. Tech., 14, 239–268, https://doi.org/10.5194/amt-14-239-2021, https://doi.org/10.5194/amt-14-239-2021, 2021
Short summary
Short summary
Balloon-borne frost point hygrometers are crucial for the monitoring of water vapour in the upper troposphere and lower stratosphere. We found that when traversing a mixed-phase cloud with big supercooled droplets, the intake tube of the instrument collects on its inner surface a high percentage of these droplets. The newly formed ice layer will sublimate at higher levels and contaminate the measurement. The balloon is also a source of contamination, but only at higher levels during the ascent.
Jing Dou, Peter A. Alpert, Pablo Corral Arroyo, Beiping Luo, Frederic Schneider, Jacinta Xto, Thomas Huthwelker, Camelia N. Borca, Katja D. Henzler, Jörg Raabe, Benjamin Watts, Hartmut Herrmann, Thomas Peter, Markus Ammann, and Ulrich K. Krieger
Atmos. Chem. Phys., 21, 315–338, https://doi.org/10.5194/acp-21-315-2021, https://doi.org/10.5194/acp-21-315-2021, 2021
Short summary
Short summary
Photochemistry of iron(III) complexes plays an important role in aerosol aging, especially in the lower troposphere. Ensuing radical chemistry leads to decarboxylation, and the production of peroxides, and oxygenated volatile compounds, resulting in particle mass loss due to release of the volatile products to the gas phase. We investigated kinetic transport limitations due to high particle viscosity under low relative humidity conditions. For quantification a numerical model was developed.
Arseniy Karagodin-Doyennel, Eugene Rozanov, Ales Kuchar, William Ball, Pavle Arsenovic, Ellis Remsberg, Patrick Jöckel, Markus Kunze, David A. Plummer, Andrea Stenke, Daniel Marsh, Doug Kinnison, and Thomas Peter
Atmos. Chem. Phys., 21, 201–216, https://doi.org/10.5194/acp-21-201-2021, https://doi.org/10.5194/acp-21-201-2021, 2021
Short summary
Short summary
The solar signal in the mesospheric H2O and CO was extracted from the CCMI-1 model simulations and satellite observations using multiple linear regression (MLR) analysis. MLR analysis shows a pronounced and statistically robust solar signal in both H2O and CO. The model results show a general agreement with observations reproducing a negative/positive solar signal in H2O/CO. The pattern of the solar signal varies among the considered models, reflecting some differences in the model setup.
Megan S. Claflin, Demetrios Pagonis, Zachary Finewax, Anne V. Handschy, Douglas A. Day, Wyatt L. Brown, John T. Jayne, Douglas R. Worsnop, Jose L. Jimenez, Paul J. Ziemann, Joost de Gouw, and Brian M. Lerner
Atmos. Meas. Tech., 14, 133–152, https://doi.org/10.5194/amt-14-133-2021, https://doi.org/10.5194/amt-14-133-2021, 2021
Short summary
Short summary
We have developed a field-deployable gas chromatograph with thermal desorption preconcentration and detector switching between two high-resolution mass spectrometers for in situ measurements of volatile organic compounds (VOCs). This system combines chromatography with both proton transfer and electron ionization to offer fast time response and continuous molecular speciation. This technique was applied during the 2018 ATHLETIC campaign to characterize VOC emissions in an indoor environment.
Cited articles
Abramson, E., Imre, D., Beranek, J., Wilson, J., and Zelenyuk, A.: Experimental determination of chemical diffusion within secondary organic aerosol particles, Phys. Chem. Chem. Phys., 15, 2983–2991, 2013.
Arangio, A. M., Slade, J. H., Berkemeier, T., Poeschl, U., Knopf, D. A., and Shiraiwa, M.: Multiphase chemical kinetics of OH radical uptake by molecular organic markers of biomass burning aerosols: humidity and temperature dependence, surface reaction, and bulk diffusion, J. Phys. Chem. A, 119, 4533–4544, 2015.
Bateman, A. P., Bertram, A. K., and Martin, S. T.: Hygroscopic influence on the semisolid-to-liquid transition of secondary organic materials, J. Phys. Chem. A, 119, 4386–4395, 2015.
Berkemeier, T., Shiraiwa, M., Pöschl, U., and Koop, T.: Competition between water uptake and ice nucleation by glassy organic aerosol particles, Atmos. Chem. Phys., 14, 12513–12531, https://doi.org/10.5194/acp-14-12513-2014, 2014.
Bones, D. L., Reid, J. P., Lienhard, D. M., and Krieger, U. K.: Comparing the mechanism of water condensation and evaporation in glassy aerosol, P. Natl. Acad. Sci. USA, 109, 11613–11618, https://doi.org/10.1073/pnas.1200691109, 2012.
Booth, A. M., Murphy, B., Riipinen, I., Percival, C. J., and Topping, D. O.: Connecting bulk viscosity measurements to kinetic limitations on attaining equilibrium for a model aerosol composition, Environ. Sci. Technol., 48, 9298–9305, 2014.
Cai, W. D., Ramesh, N., Tihminlioglu, F., Danner, R. P., Duda, J. L., and de Haan, A.: Phase equilibrium and diffusion of solvents in polybutadiene: a capillary-column inverse gas chromatography study, J. Polym. Sci. Pol. Phys., 40, 1046–1055, 2002.
Cohen, M. H. and Grest, G. S.: Liquid-glass transition, a free-volume approach, Phys. Rev. B, 20, 1077–1098, 1979.
Corti, H. R., Frank, G. A., and Marconi, M. C.: Diffusion-viscosity decoupling in supercooled aqueous trehalose solutions, J. Phys. Chem. B, 112, 12899–12906, https://doi.org/10.1021/jp802806p, 2008.
Debenedetti, P. G.: Metastable Liquids: Concepts and Principles, Princeton University Press, Princeton, NJ, USA, 1996.
Debenedetti, P. G. and Stillinger, F. H.: Supercooled liquids and the glass transition, Nature, 410, 259–267, 2001.
Demertzis, P. G. and Kontominas, M. G.: Thermodynamic study of water sorption and water vapor diffusion in poly(vinylidene chloride) copolymers, in: Inverse Gas Chromatography, edited by: Lloyd, D. R., Ward, T. C., Schreiber, H. P., and Pizana, C. C., chap. 7, American Chemical Society, Washington, D.C., USA, 77–86, 1989.
Dette, H. P., Qi, M., Schroeder, D. C., Godt, A., and Koop, T.: Glass-forming properties of 3-methylbutane-1,2,3-tricarboxylic acid and its mixtures with water and pinonic acid, J. Phys. Chem. A, 118, 7024–7033, 2014.
Duda, J. L.: Molecular diffusion in polymeric systems, Pure Appl. Chem., 57, 1681–1690, 1985.
Ekdawi-Sever, N., de Pablo, J. J., Feick, E., and von Meerwall, E.: Diffusion of sucrose and alpha,alpha-trehalose in aqueous solutions, J. Phys. Chem. A, 107, 936–943, 2003.
Faldi, A., Tirrell, M., Lodge, T. P., and von Meerwall, E.: Monomer diffusion and the kinetics of methyl methacrylate radical polymerization at intermediate to high converstion, Macromolecules, 27, 4184–4192, 1994.
Gillen, K. T., Douglass, D. C., and Hoch, J. R.: Self-diffusion in liquid water to −31 degrees C, J. Chem. Phys., 57, 5117–5119, https://doi.org/10.1063/1.1678198, 1972.
Gordon, J. M. and Taylor, J. S.: Ideal copolymers and the 2nd-order transitions of synthetic rubbers. 1. Non-crystalline copolymers, J. Appl. Chem., 2, 493–500, 1952.
Hagiwara, T., Sakiyama, T., and Watanabe, H.: Estimation of water diffusion coefficients in freeze-concentrated matrices of sugar solutions using molecular dynamics: correlation between estimated diffusion coefficients and measured ice-crystal recrystallization rates, Food Biophys., 4, 340–346, 2009.
Hardy, G. F.: Solubility and diffusion of water in acetal polymers, J. Polym. Sci. A2, 5, 671–684, 1967.
Heaton, K. J., Sleighter, R. L., Hatcher, P. G., Hall, W. A., and Johnston, M. V.: Composition domains in monoterpene secondary organic aerosol, Environ. Sci. Technol., 43, 7797–7802, 2009.
Hong, S. U.: Prediction of polymer-solvent diffusion behaviour using free-volume theory, Ind. Eng. Chem. Res., 34, 2536–2544, 1995.
Hosny, N. A., Fitzgerald, C., Tong, C., Kalberer, M., Kuimova, M. K., and Pope, F. D.: Fluorescent lifetime imaging of atmospheric aerosols: a direct probe of aerosol viscosity, Faraday Discuss., 165, 343–356, 2013.
Karlsson, O. J., Stubbs, J. M., Karlsson, L. E., and Sundberg, D. C.: Estimating diffusion coefficients for small molecules in polymers and polymer solutions, Polymer, 42, 4915–4923, 2001.
Kokes, R. J. and Long, F. A.: Diffusion of organic vapors into polyvinyl acetate, J. Am. Chem. Soc., 75, 6142–6146, 1953.
Koop, T., Luo, B. P., Tsias, A., and Peter, T.: Water activity as the determinant for homogeneous ice nucleation in aqueous solutions, Nature, 406, 611–614, 2000.
Koop, T., Bookhold, J., Shiraiwa, M., and Pöschl, U.: Glass transition and phase state of organic compounds: dependency on molecular properties and implications for secondary organic aerosols in the atmosphere, Phys. Chem. Chem. Phys., 13, 19238–19255, 2011.
Kumins, C. A. and Roteman, J.: Diffusion of gases and vapors through polyvinyl chloride-polyvinyl acetate copolymer films. 1. Glass transition effect, J. Polym. Sci., 55, 683–698, 1961.
Kumins, C. A., Rolle, C. J., and Roteman, J.: Water vapor diffusion through vinyl chloride-vinyl acetate copolymer, J. Phys. Chem., 61, 1290–1296, 1957.
Lambe, A. T., Ahern, A. T., Williams, L. R., Slowik, J. G., Wong, J. P. S., Abbatt, J. P. D., Brune, W. H., Ng, N. L., Wright, J. P., Croasdale, D. R., Worsnop, D. R., Davidovits, P., and Onasch, T. B.: Characterization of aerosol photooxidation flow reactors: heterogeneous oxidation, secondary organic aerosol formation and cloud condensation nuclei activity measurements, Atmos. Meas. Tech., 4, 445–461, https://doi.org/10.5194/amt-4-445-2011, 2011.
Lambe, A. T., Cappa, C. D., Massoli, P., Onasch, T. B., Forestieri, S. D., Martin, A. T., Cummings, M. J., Croasdale, D. R., Brune, W. H., Worsnop, D. R., and Davidovits, P.: Relationship between oxidation level and optical properties of secondary organic aerosol, Environ. Sci. Technol., 47, 6349–6357, 2013.
Launay, A., Thominette, F., and Verdu, J.: Water sorption in amorphous poly(ethylene terephthalate), J. Appl. Polym. Sci., 73, 1131–1137, 1999.
Lienhard, D. M., Bones, D. L., Zuend, A., Krieger, U. K., Reid, J. P., and Peter, T.: Measurements of thermodynamic and optical properties of selected aqueous organic and organic-inorganic mixtures of atmospheric relevance, J. Phys. Chem. A, 116, 9954–9968, https://doi.org/10.1021/jp3055872, 2012a.
Lienhard, D. M., Zobrist, B., Zuend, A., Krieger, U. K., and Peter, T.: Experimental evidence for excess entropy discontinuities in glass-forming solutions, J. Chem. Phys., 136, 074515, https://doi.org/10.1063/1.3685902, 2012b.
Lienhard, D. M., Huisman, A. J., Bones, D. L., Te, Y.-F., Luo, B. P., Krieger, U. K., and Reid, J. P.: Retrieving the translational diffusion coefficient of water from experiments on single levitated aerosol droplets, Phys. Chem. Chem. Phys., 16, 16677–16683, 2014.
Long, F. A. and Thompson, L. J.: Diffusion of water vapor in polymers, J. Polym. Sci., 15, 413–426, 1955.
Mapes, M. K., Swallen, S. F., and Ediger, M. D.: Self-diffusion of supercooled o-terphenyl near the glass transition temperature, J. Phys. Chem. B, 110, 507–511, https://doi.org/10.1021/jp0555955, 2006.
McGlashan, M. L.: Deviations from Raoult's law, J. Chem. Educ., 40, 516–518, 1963.
Molinero, V. and Goddard, W. A.: Microscopic mechanism of water diffusion in glucose glasses, Phys. Rev. Lett., 95, 045701, https://doi.org/10.1103/PhysRevLett.95.045701, 2005.
Murphy, D. M. and Koop, T.: Review of the vapour pressures of ice and supercooled water for atmospheric applications, Q. J. Roy. Meteorol. Soc., 131, 1539–1565, 2005.
Murray, B. J., Wilson, T. W., Dobbie, S., Cui, Z., Al-Jumur, S. M. R. K., Möhler, O., Schnaiter, M., Wagner, R., Benz, S., Niemand, M., Saathoff, H., Ebert, V., Wagner, S., and Kärcher, B.: Heterogeneous nucleation of ice particles on glassy aerosols under cirrus conditions, Nat. Geosci., 3, 233–237, 2010.
Pajunoja, A., Lambe, A. T., Hakala, J., Rastak, N., Cummings, M. J., Brogan, J. F., Hao, L., Paramonov, M., Hong, J., Prisle, N. L., Malila, J., Romakkaniemi, S., Lehtinen, K. E. J., Laaksonen, A., Kulmala, M., Massoli, P., Onasch, T. B., Donahue, N. M., Riipinen, I., Davidovits, P., Worsnop, D. R., Petaja, T., and Virtanen, A.: Adsorptive uptake of water by semisolid secondary organic aerosols, Geophys. Res. Lett., 42, 3063–3068, 2015.
Park, G. S.: Transport principles – solution, diffusion and permeation in polymer membranes, in: Synthetic Membranes: Science, Engineering and Applications, edited by: Bungay, P. M., Lonsdale, H. K., and de Pinho, M. N., vol. 181, Reidel, Dordrecht, the Netherlands, 57–107, 1986.
Parker, R. and Ring, S. G.: Diffusion in maltose-water mixtures at temperatures close to the glass transition, Carbohydr. Res., 273, 147–155, https://doi.org/10.1016/0008-6215(95)00120-I, 1995.
Petters, M. D. and Kreidenweis, S. M.: A single parameter representation of hygroscopic growth and cloud condensation nucleus activity, Atmos. Chem. Phys., 7, 1961–1971, https://doi.org/10.5194/acp-7-1961-2007, 2007.
Power, R. M., Simpson, S. H., Reid, J. P., and Hudson, A. J.: The transition from liquid to solid-like behaviour in ultrahigh viscosity aerosol particles, Chem. Sci., 4, 2597–2604, https://doi.org/10.1039/c3sc50682g, 2013.
Price, H. C., Murray, B. J., Mattsson, J., O'Sullivan, D., Wilson, T. W., Baustian, K. J., and Benning, L. G.: Quantifying water diffusion in high-viscosity and glassy aqueous solutions using a Raman isotope tracer method, Atmos. Chem. Phys., 14, 3817–3830, https://doi.org/10.5194/acp-14-3817-2014, 2014.
Price, H. C., Mattsson, J., Zhang, Y., Bertram, A. K., Davies, J. F., Grayson, J. W., Martin, S. T., O'Sullivan, D., Reid, J. P., Rickards, A. M. J., and Murray, B. J.: Water diffusion in atmospherically relevant α-pinene secondary organic material, Chem. Sci., 6, 4876–4883, 2015.
Price, W. S., Ide, H., and Arata, Y.: Self-diffusion of supercooled water to 238 K using PGSE NMR diffusion measurements, J. Phys. Chem. A, 103, 448–450, 1999.
Pruppacher, H. R.: Self-diffusion coefficient of supercooled water, J. Chem. Phys., 56, 101–107, 1972.
Ramesh, N., Davis, P. K., Zielinski, J. M., Danner, R. P., and Duda, J. L.: Application of free-volume theory to self diffusion of solvents in polymers below the glass transition temperature: a review, J. Polym. Sci. Pol. Phys., 49, 1629–1644, 2011.
Renbaum-Wolff, L., Grayson, J. W., Bateman, A. P., Kuwata, M., Sellier, M., Murray, B. J., Shilling, J. E., Martin, S. T., and Bertram, A. K.: Viscosity of alpha-pinene secondary organic material and implications for particle growth and reactivity, P. Natl. Acad. Sci. USA, 110, 8014–8019, 2013.
Rickards, A. M. J., Miles, R. E. H., Davies, J. F., Marshall, F. H., and Reid, J. P.: Measurements of the sensitivity of aerosol hygroscopicity and the kappa parameter to the O / C ratio, J. Phys. Chem. A, 117, 14120–14131, 2013.
Schatzberg, P.: Diffusion of water through hydrocarbon liquids, J. Polym. Sci. C, 10PC, 87–92, 1965.
Seinfeld, J. H. and Pandis, S. N.: Atmospheric Chemistry and Physics, Wiley and Sons Inc., New York, 1998.
Shiraiwa, M., Ammann, M., Koop, T., and Pöschl, U.: Gas uptake and chemical aging of semisolid organic aerosol particles, P. Natl. Acad. Sci. USA, 108, 11003–11008, https://doi.org/10.1073/pnas.1103045108, 2011.
Shiraiwa, M., Zuend, A., Bertram, A. K., and Seinfeld, J. H.: Gas-particle partitioning of atmospheric aerosols: interplay of physical state, non-ideal mixing and morphology, Phys. Chem. Chem. Phys., 15, 11441–11453, 2013.
Smith, R. S. and Kay, B. D.: The existence of supercooled liquid water at 150 K, Nature, 398, 788–791, 1999.
Steimer, S. S., Krieger, U. K., Te, Y.-F., Lienhard, D. M., Huisman, A. J., Luo, B. P., Ammann, M., and Peter, T.: Electrodynamic balance measurements of thermodynamic, kinetic, and optical aerosol properties inaccessible to bulk methods, Atmos. Meas. Tech., 8, 2397–2408, https://doi.org/10.5194/amt-8-2397-2015, 2015.
Tong, H.-J., Reid, J. P., Bones, D. L., Luo, B. P., and Krieger, U. K.: Measurements of the timescales for the mass transfer of water in glassy aerosol at low relative humidity and ambient temperature, Atmos. Chem. Phys., 11, 4739–4754, https://doi.org/10.5194/acp-11-4739-2011, 2011.
Tonge, M. P. and Gilbert, R. G.: Testing models for penetrant diffusion in glassy polymers, Polymer, 42, 501–513, 2001.
Tonge, M. P., Stubbs, J. M., Sundberg, D. C., and Gilbert, R. G.: Penetrant diffusion in poly(methyl methacrylate) near T-g: dependence on temperature and polymer weight fraction, Polymer, 41, 3659–3670, 2000.
Tromp, R. H., Parker, R., and Ring, S. G.: Water diffusion in glasses of carbohydrates, Carbohyd. Res., 303, 199–205, 1997.
Vignes, A.: Diffusion in binary solutions. Variation of diffusion coefficient with composition, Ind. Eng. Chem. Fundam., 5, 189–199, 1966.
Virtanen, A., Joutsensaari, J., Koop, T., Kannosto, J., Yli-Pirila, P., Leskinen, J., Makela, J. M., Holopainen, J. K., Poeschl, U., Kulmala, M., Worsnop, D. R., and Laaksonen, A.: An amorphous solid state of biogenic secondary organic aerosol particles, Nature, 467, 824–827, https://doi.org/10.1038/nature09455, 2010.
Vrentas, J. S. and Vrentas, C. M.: Solvent self-diffusion in glassy polymer-solvent systems, Macromolecules, 27, 5570–5576, 1994.
Vrentas, J. S. and Vrentas, C. M.: Effect of glass transition on the concentration dependence of self-diffusion coefficients, J. Appl. Polym. Sci., 89, 1682–1684, 2003.
Vrentas, J. S., Duda, J. L., and Ling, H. C.: Influence of the glass transition on the solvent self-diffusion in amorphous polymers, J. Polym. Sci. Pol. Phys., 26, 1059–1065, 1988.
Wang, B. B., Lambe, A. T., Massoli, P., Onasch, T. B., Davidovits, P., Worsnop, D. R., and Knopf, D. A.: The deposition ice nucleation and immersion freezing potential of amorphous secondary organic aerosol: Pathways for ice and mixed-phase cloud formation, J. Geophys. Res., 117, D16209, https://doi.org/10.1029/2012JD018063, 2012.
Yasuda, H. and Stannett, V.: Permeation, solution, and diffusion of water in some high polymers, J. Polym. Sci., 57, 907–923, 1962.
Zardini, A. A., Krieger, U. K., and Marcolli, C.: White light Mie resonance spectroscopy used to measure very low vapor pressures of substances in aqueous solution aerosol particles, Opt. Express, 14, 6951–6962, 2006.
Zhang, Y., Sanchez, M. S., Douet, C., Wang, Y., Bateman, A. P., Gong, Z., Kuwata, M., Renbaum-Wolff, L., Sato, B. B., Liu, P. F., Bertram, A. K., Geiger, F. M., and Martin, S. T.: Changing shapes and implied viscosities of suspended submicron particles, Atmos. Chem. Phys., 15, 7819–7829, https://doi.org/10.5194/acp-15-7819-2015, 2015.
Zobrist, B., Marcolli, C., Pedernera, D. A., and Koop, T.: Do atmospheric aerosols form glasses?, Atmos. Chem. Phys., 8, 5221–5244, https://doi.org/10.5194/acp-8-5221-2008, 2008.
Zobrist, B., Soonsin, V., Luo, B. P., Krieger, U. K., Marcolli, C., Peter, T., and Koop, T.: Ultra-slow water diffusion in aqueous sucrose glasses, Phys. Chem. Chem. Phys., 13, 3514–3526, https://doi.org/10.1039/C0CP01273D, 2011.
Short summary
New data of water diffusivity in secondary organic aerosol (SOA) material and organic/inorganic model mixtures is presented over an extensive temperature range. Our data suggest that water diffusion in SOA is sufficiently fast so that it is unlikely to have significant consequences on the direct climatic effect under tropospheric conditions. Glass formation in SOA is unlikely to restrict homogeneous ice nucleation.
New data of water diffusivity in secondary organic aerosol (SOA) material and organic/inorganic...
Altmetrics
Final-revised paper
Preprint