Articles | Volume 19, issue 14
https://doi.org/10.5194/acp-19-9333-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-19-9333-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
22 Jul 2019
Research article |
| 22 Jul 2019
Optimization of process models for determining volatility distribution and viscosity of organic aerosols from isothermal particle evaporation data
Department of Applied Physics, University of Eastern Finland, Kuopio, Finland
Väinö Hämäläinen
Department of Applied Physics, University of Eastern Finland, Kuopio, Finland
Grazia Rovelli
School of Chemistry, University of Bristol, Bristol, BS8 1TS, UK
Antti Lipponen
Atmospheric Research Centre of Eastern Finland, Finnish Meteorological Institute, Kuopio, Finland
Manabu Shiraiwa
Department of Chemistry, University of California, Irvine, CA, USA
Jonathan P. Reid
School of Chemistry, University of Bristol, Bristol, BS8 1TS, UK
Kari E. J. Lehtinen
Department of Applied Physics, University of Eastern Finland, Kuopio, Finland
Atmospheric Research Centre of Eastern Finland, Finnish Meteorological Institute, Kuopio, Finland
Taina Yli-Juuti
Department of Applied Physics, University of Eastern Finland, Kuopio, Finland
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This paper proposes a novel and accurate method for estimating and reconstructing aerosol optical depth from sunshine duration measurements under cloud-free conditions at any place and time since the late 19th century. The method performs very well when compared to AErosol RObotic NETwork measurements and operates an efficient detection of signals from massive volcanic eruptions. Reconstructed long-term aerosol optical depths are in agreement with the dimming/brightening phenomenon.
Arttu Ylisirniö, Angela Buchholz, Claudia Mohr, Zijun Li, Luis Barreira, Andrew Lambe, Celia Faiola, Eetu Kari, Taina Yli-Juuti, Sergey A. Nizkorodov, Douglas R. Worsnop, Annele Virtanen, and Siegfried Schobesberger
Atmos. Chem. Phys., 20, 5629–5644, https://doi.org/10.5194/acp-20-5629-2020, https://doi.org/10.5194/acp-20-5629-2020, 2020
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We studied the chemical composition and volatility of secondary organic aerosol (SOA) particles formed from emissions of Scots pines and compared those results to SOA formed from α-pinene and from a sesquiterpene mixture. We found that SOA formed from single precursors cannot capture the properties of SOA formed from real plant emissions.
Thomas Kühn, Kaarle Kupiainen, Tuuli Miinalainen, Harri Kokkola, Ville-Veikko Paunu, Anton Laakso, Juha Tonttila, Rita Van Dingenen, Kati Kulovesi, Niko Karvosenoja, and Kari E. J. Lehtinen
Atmos. Chem. Phys., 20, 5527–5546, https://doi.org/10.5194/acp-20-5527-2020, https://doi.org/10.5194/acp-20-5527-2020, 2020
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We investigate the effects of black carbon (BC) mitigation on Arctic climate and human health, accounting for the concurrent reduction of other aerosol species. While BC is attributed a net warming effect on climate, most other aerosol species cool the planet. We find that the direct radiative effect of mitigating BC induces cooling, while aerosol–cloud effects offset this cooling and introduce large uncertainties. Furthermore, the reduced aerosol emissions reduce human mortality considerably.
Kimmo Korhonen, Thomas Bjerring Kristensen, John Falk, Robert Lindgren, Christina Andersen, Ricardo Luis Carvalho, Vilhelm Malmborg, Axel Eriksson, Christoffer Boman, Joakim Pagels, Birgitta Svenningsson, Mika Komppula, Kari E. J. Lehtinen, and Annele Virtanen
Atmos. Chem. Phys., 20, 4951–4968, https://doi.org/10.5194/acp-20-4951-2020, https://doi.org/10.5194/acp-20-4951-2020, 2020
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Ice-nucleating abilities of particulate emissions from solid-fuel-burning cookstoves were studied using a portable ice nuclei counter in an extensive laboratory experiment campaign. We found that even small changes in combustion conditions may affect the ice-nucleating ability of the emissions significantly. Also six different physico-chemical properties of the emissions were studied, but no clear correlation to their ice-nucleating ability was found.
Andrew M. Sayer, Yves Govaerts, Pekka Kolmonen, Antti Lipponen, Marta Luffarelli, Tero Mielonen, Falguni Patadia, Thomas Popp, Adam C. Povey, Kerstin Stebel, and Marcin L. Witek
Atmos. Meas. Tech., 13, 373–404, https://doi.org/10.5194/amt-13-373-2020, https://doi.org/10.5194/amt-13-373-2020, 2020
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Satellite measurements of the Earth are routinely processed to estimate useful quantities; one example is the amount of atmospheric aerosols (which are particles such as mineral dust, smoke, volcanic ash, or sea spray). As with all measurements and inferred quantities, there is some degree of uncertainty in this process.
There are various methods to estimate these uncertainties. A related question is the following: how reliable are these estimates? This paper presents a method to assess them.
Santtu Mikkonen, Mikko R. A. Pitkänen, Tuomo Nieminen, Antti Lipponen, Sini Isokääntä, Antti Arola, and Kari E. J. Lehtinen
Atmos. Chem. Phys., 19, 12531–12543, https://doi.org/10.5194/acp-19-12531-2019, https://doi.org/10.5194/acp-19-12531-2019, 2019
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Atmospheric measurement data never come without measurement error. Too often, these errors are neglected when researchers make inferences from their data. We applied multiple line-fitting methods to simulated data mimicking two central variables in aerosol research. Our results show that an ordinary least squares fit, typically used to describe relationships, underestimates the slope of the fit and that methods taking the measurement uncertainty into account performed significantly better.
Mijung Song, Adrian M. Maclean, Yuanzhou Huang, Natalie R. Smith, Sandra L. Blair, Julia Laskin, Alexander Laskin, Wing-Sy Wong DeRieux, Ying Li, Manabu Shiraiwa, Sergey A. Nizkorodov, and Allan K. Bertram
Atmos. Chem. Phys., 19, 12515–12529, https://doi.org/10.5194/acp-19-12515-2019, https://doi.org/10.5194/acp-19-12515-2019, 2019
Kelly L. Pereira, Grazia Rovelli, Young C. Song, Alfred W. Mayhew, Jonathan P. Reid, and Jacqueline F. Hamilton
Atmos. Meas. Tech., 12, 4519–4541, https://doi.org/10.5194/amt-12-4519-2019, https://doi.org/10.5194/amt-12-4519-2019, 2019
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We present the design and operation of a newly built continuous-flow reactor (CFR), which can be used as a tool to gain considerable insights into the composition and physical state of secondary organic aerosol (SOA). The CFR was used to generate large quantities of SOA mass, allowing the use of highly accurate techniques that are not usually accessible. We demonstrate how this unique approach can be used to investigate the relationship between SOA formation and physiochemical properties.
Erin Evoy, Adrian M. Maclean, Grazia Rovelli, Ying Li, Alexandra P. Tsimpidi, Vlassis A. Karydis, Saeid Kamal, Jos Lelieveld, Manabu Shiraiwa, Jonathan P. Reid, and Allan K. Bertram
Atmos. Chem. Phys., 19, 10073–10085, https://doi.org/10.5194/acp-19-10073-2019, https://doi.org/10.5194/acp-19-10073-2019, 2019
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We measured the diffusion rates of organic molecules in a number of proxies for secondary organic aerosol (SOA) and compared measured diffusion with predictions from two relations: the Stokes–Einstein relation and a fractional Stokes–Einstein relation. The fractional relation does a better job of predicting diffusion rates in this case. Output from an atmospheric model shows that mixing times predicted using the two relations differ by up to 1 order of magnitude at an altitude of ~ 3 km.
Ying Li and Manabu Shiraiwa
Atmos. Chem. Phys., 19, 5959–5971, https://doi.org/10.5194/acp-19-5959-2019, https://doi.org/10.5194/acp-19-5959-2019, 2019
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Timescales for secondary organic aerosols (SOA) to reach equilibrium were estimated under various temperatures and relative humidities. Equilibration timescales in free troposphere can be longer than hours or days, even at moderate or relatively high relative humidities. These results provide critical insights into thermodynamic or kinetic treatments of SOA partitioning for accurate predictions of gas- and particle-phase concentrations of semi-volatile compounds in chemical transport models.
Angela Buchholz, Andrew T. Lambe, Arttu Ylisirniö, Zijun Li, Olli-Pekka Tikkanen, Celia Faiola, Eetu Kari, Liqing Hao, Olli Luoma, Wei Huang, Claudia Mohr, Douglas R. Worsnop, Sergey A. Nizkorodov, Taina Yli-Juuti, Siegfried Schobesberger, and Annele Virtanen
Atmos. Chem. Phys., 19, 4061–4073, https://doi.org/10.5194/acp-19-4061-2019, https://doi.org/10.5194/acp-19-4061-2019, 2019
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We studied the evaporation of α-pinene secondary organic aerosol particles in clean air to derive their volatility from the observed size changes. We found that the particles became more resilient to evaporation with increased oxidative age, possibly increasing their lifetime in the atmosphere. Also, increased relative humidity increased the particle evaporation. Mass spectrometry measurements of the particles at different stages of evaporation revealed some water-induced composition changes.
Thomas J. Bannan, Michael Le Breton, Michael Priestley, Stephen D. Worrall, Asan Bacak, Nicholas A. Marsden, Archit Mehra, Julia Hammes, Mattias Hallquist, M. Rami Alfarra, Ulrich K. Krieger, Jonathan P. Reid, John Jayne, Wade Robinson, Gordon McFiggans, Hugh Coe, Carl J. Percival, and Dave Topping
Atmos. Meas. Tech., 12, 1429–1439, https://doi.org/10.5194/amt-12-1429-2019, https://doi.org/10.5194/amt-12-1429-2019, 2019
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The Filter Inlet for Gases and AEROsols (FIGAERO) is an inlet designed to be coupled with a high-resolution time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS) and provides simultaneous molecular information relating to both the gas- and particle-phase samples. This method has been used to extract vapour pressures of compounds whilst giving quantitative concentrations in the particle phase. Here we detail an ideal set of benchmark compounds for characterization of the FIGAERO.
Liqing Hao, Olga Garmash, Mikael Ehn, Pasi Miettinen, Paola Massoli, Santtu Mikkonen, Tuija Jokinen, Pontus Roldin, Pasi Aalto, Taina Yli-Juuti, Jorma Joutsensaari, Tuukka Petäjä, Markku Kulmala, Kari E. J. Lehtinen, Douglas R. Worsnop, and Annele Virtanen
Atmos. Chem. Phys., 18, 17705–17716, https://doi.org/10.5194/acp-18-17705-2018, https://doi.org/10.5194/acp-18-17705-2018, 2018
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An aerosol mass spectrometer was used to characterize aerosol chemical composition during new particle formation periods. The time profiles of mass concentrations and chemical composition of observed aerosol particles are subjected to joint effects of boundary layer dilution, atmospheric chemistry and aerosol mixing in different boundary layers. During the nighttime, the increase in organic aerosol mass correlated well with the increase in condensed highly oxygenated organic molecules' mass.
Harri Kokkola, Thomas Kühn, Anton Laakso, Tommi Bergman, Kari E. J. Lehtinen, Tero Mielonen, Antti Arola, Scarlet Stadtler, Hannele Korhonen, Sylvaine Ferrachat, Ulrike Lohmann, David Neubauer, Ina Tegen, Colombe Siegenthaler-Le Drian, Martin G. Schultz, Isabelle Bey, Philip Stier, Nikos Daskalakis, Colette L. Heald, and Sami Romakkaniemi
Geosci. Model Dev., 11, 3833–3863, https://doi.org/10.5194/gmd-11-3833-2018, https://doi.org/10.5194/gmd-11-3833-2018, 2018
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In this paper we present a global aerosol–chemistry–climate model with the focus on its representation for atmospheric aerosol particles. In the model, aerosols are simulated using the aerosol module SALSA2.0, which in this paper is compared to satellite, ground, and aircraft-based observations of the properties of atmospheric aerosol. Based on this study, the model simulated aerosol properties compare well with the observations.
Yangxi Chu, Erin Evoy, Saeid Kamal, Young Chul Song, Jonathan P. Reid, Chak K. Chan, and Allan K. Bertram
Atmos. Meas. Tech., 11, 4809–4822, https://doi.org/10.5194/amt-11-4809-2018, https://doi.org/10.5194/amt-11-4809-2018, 2018
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The viscosity of erythritol, a tetrol found in aerosol particles, is highly uncertain. To help resolve this uncertainty, we measured the viscosities of
erythritol–water particles using rectangular-area fluorescence recovery after photobleaching and aerosol optical tweezers techniques. These results
should help improve the understanding of the viscosity of secondary organic aerosol particles. In addition, we present an intercomparison of techniques
for measuring the viscosity of particles.
Jorma Joutsensaari, Matthew Ozon, Tuomo Nieminen, Santtu Mikkonen, Timo Lähivaara, Stefano Decesari, M. Cristina Facchini, Ari Laaksonen, and Kari E. J. Lehtinen
Atmos. Chem. Phys., 18, 9597–9615, https://doi.org/10.5194/acp-18-9597-2018, https://doi.org/10.5194/acp-18-9597-2018, 2018
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New particle formation (NPF) in the atmosphere is globally an important source of aerosol particles. NPF events are typically identified and analyzed manually by researchers from particle size distribution data day by day, which is time consuming and might be inconsistent. We have developed an automatic analysis method based on deep learning for NPF event identification. The developed method can be easily utilized to analyze any long-term datasets more accurately and consistently.
Wing-Sy Wong DeRieux, Ying Li, Peng Lin, Julia Laskin, Alexander Laskin, Allan K. Bertram, Sergey A. Nizkorodov, and Manabu Shiraiwa
Atmos. Chem. Phys., 18, 6331–6351, https://doi.org/10.5194/acp-18-6331-2018, https://doi.org/10.5194/acp-18-6331-2018, 2018
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The phase transition of organic particles between glassy and semi-solid states occurs at the glass transition temperature. We developed a method to predict glass transition temperatures and the viscosity of secondary organic aerosols using molecular composition, with consistent results with viscosity measurements. The viscosity of biomass burning particles was also estimated using the chemical composition measured by high-resolution mass spectrometry with two different ionization techniques.
Antti Lipponen, Tero Mielonen, Mikko R. A. Pitkänen, Robert C. Levy, Virginia R. Sawyer, Sami Romakkaniemi, Ville Kolehmainen, and Antti Arola
Atmos. Meas. Tech., 11, 1529–1547, https://doi.org/10.5194/amt-11-1529-2018, https://doi.org/10.5194/amt-11-1529-2018, 2018
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Atmospheric aerosols are small solid or liquid particles suspended in the atmosphere and they have a significant effect on the climate. Satellite data are used to get global estimates of atmospheric aerosols. In this work, a statistics-based Bayesian aerosol retrieval algorithm was developed to improve the accuracy and quantify the uncertainties related to the aerosol estimates. The algorithm is tested with NASA's Moderate Resolution Imaging Spectroradiometer (MODIS) satellite data.
Ekaterina Ezhova, Veli-Matti Kerminen, Kari E. J. Lehtinen, and Markku Kulmala
Atmos. Chem. Phys., 18, 2431–2442, https://doi.org/10.5194/acp-18-2431-2018, https://doi.org/10.5194/acp-18-2431-2018, 2018
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A condensation sink (CS) quantifies the rate of uptake of condensing vapours by pre-existing aerosol and can be used as well to quantify losses of monomers/clusters. An analytical solution of the condensation equation valid in a wide range of particle diameters is presented. We describe the dynamics of atmospheric CS, test the formulas against field observations and further use them to develop a simplified model of the coupled dynamics of aerosol and condensing vapours in the atmosphere.
Mallory L. Hinks, Julia Montoya-Aguilera, Lucas Ellison, Peng Lin, Alexander Laskin, Julia Laskin, Manabu Shiraiwa, Donald Dabdub, and Sergey A. Nizkorodov
Atmos. Chem. Phys., 18, 1643–1652, https://doi.org/10.5194/acp-18-1643-2018, https://doi.org/10.5194/acp-18-1643-2018, 2018
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We have observed a strong effect of relative humidity on the composition of particulate matter produced from the oxidation of toluene in clean air. At higher relative humidity, there was a significant reduction in the fraction of high-molecular-weight compounds present in the particles. The amount of particulate matter also decreased at higher relative humidity. The main implication of this study is that water vapor participates in the photooxidation of toluene in a complicated way.
Lukas Pichelstorfer, Dominik Stolzenburg, John Ortega, Thomas Karl, Harri Kokkola, Anton Laakso, Kari E. J. Lehtinen, James N. Smith, Peter H. McMurry, and Paul M. Winkler
Atmos. Chem. Phys., 18, 1307–1323, https://doi.org/10.5194/acp-18-1307-2018, https://doi.org/10.5194/acp-18-1307-2018, 2018
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Quantification of new particle formation as a source of atmospheric aerosol is clearly of importance for climate and health aspects. In our new study we developed two analysis methods that allow retrieval of nanoparticle growth dynamics at much higher precision than it was possible so far. Our results clearly demonstrate that growth rates show much more variation than is currently known and suggest that the Kelvin effect governs growth in the sub-10 nm size range.
Ulrich K. Krieger, Franziska Siegrist, Claudia Marcolli, Eva U. Emanuelsson, Freya M. Gøbel, Merete Bilde, Aleksandra Marsh, Jonathan P. Reid, Andrew J. Huisman, Ilona Riipinen, Noora Hyttinen, Nanna Myllys, Theo Kurtén, Thomas Bannan, Carl J. Percival, and David Topping
Atmos. Meas. Tech., 11, 49–63, https://doi.org/10.5194/amt-11-49-2018, https://doi.org/10.5194/amt-11-49-2018, 2018
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Vapor pressures of low-volatility organic molecules at atmospheric temperatures reported in the literature often differ by several orders of magnitude between measurement techniques. These discrepancies exceed the stated uncertainty of each technique, which is generally reported to be smaller than a factor of 2. We determined saturation vapor pressures for the homologous series of polyethylene glycols ranging in vapor pressure at 298 K from 1E−7 Pa to 5E−2 Pa as a reference set.
Man Mei Chim, Chiu Tung Cheng, James F. Davies, Thomas Berkemeier, Manabu Shiraiwa, Andreas Zuend, and Man Nin Chan
Atmos. Chem. Phys., 17, 14415–14431, https://doi.org/10.5194/acp-17-14415-2017, https://doi.org/10.5194/acp-17-14415-2017, 2017
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In this work, we report that methyl-substituted succinic acid present at or near the surface of aqueous organic droplets can be efficiently oxidized by gas-phase OH radicals. The alkoxy radical chemistry appears to be an important reaction pathway. In addition, our model simulations reveal the relative importance of functionalization and fragmentation processes, alongside volatilization, in the evolution of the particle-phase reaction, which is largely dependent on the extent of oxidation.
Elham Baranizadeh, Tuomo Nieminen, Taina Yli-Juuti, Markku Kulmala, Tuukka Petäjä, Ari Leskinen, Mika Komppula, Ari Laaksonen, and Kari E. J. Lehtinen
Atmos. Chem. Phys., 17, 13361–13371, https://doi.org/10.5194/acp-17-13361-2017, https://doi.org/10.5194/acp-17-13361-2017, 2017
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Extrapolation of the particle formation rates from one measured larger size (e.g., 7 nm) to smaller sizes (e.g., 3 nm) based on simplified growth-scavenging dynamics works fairly well to estimate mean daily formation rates, but it fails to predict the time evolution of the particle population. This points to the challenges in predicting atmospheric nucleation rates for locations where the particle growth and loss rates are size- and time-dependent.
Qing Mu, Gerhard Lammel, Christian N. Gencarelli, Ian M. Hedgecock, Ying Chen, Petra Přibylová, Monique Teich, Yuxuan Zhang, Guangjie Zheng, Dominik van Pinxteren, Qiang Zhang, Hartmut Herrmann, Manabu Shiraiwa, Peter Spichtinger, Hang Su, Ulrich Pöschl, and Yafang Cheng
Atmos. Chem. Phys., 17, 12253–12267, https://doi.org/10.5194/acp-17-12253-2017, https://doi.org/10.5194/acp-17-12253-2017, 2017
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Polycyclic aromatic hydrocarbons (PAHs) are hazardous pollutants with the largest emissions in East Asia. The regional WRF-Chem-PAH model has been developed to reflect the state-of-the-art understanding of current PAHs studies with several new or updated features. It is able to reasonably well simulate the concentration levels and particulate mass fractions of PAHs near the sources and at a remote outflow region of East Asia, in high spatial and temporal resolutions.
Michael I. Cotterell, Rose E. Willoughby, Bryan R. Bzdek, Andrew J. Orr-Ewing, and Jonathan P. Reid
Atmos. Chem. Phys., 17, 9837–9851, https://doi.org/10.5194/acp-17-9837-2017, https://doi.org/10.5194/acp-17-9837-2017, 2017
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The optical properties of aerosols are required to analyse measurements of aerosol properties, estimate radiative forcing and interpret remote sensing retrievals. We provide comprehensive data sets of the refractive indices of the most important inorganic aerosol constituents, reporting parameterisations for the wavelength and relative humidity dependencies for each system. We assess the accuracy of this study, made on single trapped particles, against previous less comprehensive data sets.
Thomas Berkemeier, Markus Ammann, Ulrich K. Krieger, Thomas Peter, Peter Spichtinger, Ulrich Pöschl, Manabu Shiraiwa, and Andrew J. Huisman
Atmos. Chem. Phys., 17, 8021–8029, https://doi.org/10.5194/acp-17-8021-2017, https://doi.org/10.5194/acp-17-8021-2017, 2017
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Kinetic process models are efficient tools used to unravel the mechanisms governing chemical and physical transformation in multiphase atmospheric chemistry. However, determination of kinetic parameters such as reaction rate or diffusion coefficients from multiple data sets is often difficult or ambiguous. This study presents a novel optimization algorithm and framework to determine these parameters in an automated fashion and to gain information about parameter uncertainty and uniqueness.
Aleksandra Marsh, Rachael E. H. Miles, Grazia Rovelli, Alexander G. Cowling, Lucy Nandy, Cari S. Dutcher, and Jonathan P. Reid
Atmos. Chem. Phys., 17, 5583–5599, https://doi.org/10.5194/acp-17-5583-2017, https://doi.org/10.5194/acp-17-5583-2017, 2017
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The response of aerosol particles to changes in relative humidity (RH) is dependent on the hygroscopicity of the constituent chemical components. We present accurate measurements of the hygroscopic response of aerosols over a wide range in RH, extending up to the saturation RH. The chemical compounds studied include dicarboxylic acids, amino acids, sugars and polyols. These data provide a comprehensive source of data to help improve functional group activity models of aerosol hygroscopicity.
Grazia Rovelli, Rachael E. H. Miles, Jonathan P. Reid, and Simon L. Clegg
Atmos. Chem. Phys., 17, 4369–4385, https://doi.org/10.5194/acp-17-4369-2017, https://doi.org/10.5194/acp-17-4369-2017, 2017
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The response of airborne particles to relative humidity (RH) in the atmosphere, referred to as their hygroscopicity, is a key property that determines their water content. The hygroscopicity depends on the chemical species that make up the particle. Here, we investigate the growth in particle size and composition that occurs with increasing RH for particles containing a series of amine compounds and sulfuric acid, typical atmospheric components, providing a comprehensive and accurate data set.
Petri Tiitta, Ari Leskinen, Liqing Hao, Pasi Yli-Pirilä, Miika Kortelainen, Julija Grigonyte, Jarkko Tissari, Heikki Lamberg, Anni Hartikainen, Kari Kuuspalo, Aki-Matti Kortelainen, Annele Virtanen, Kari E. J. Lehtinen, Mika Komppula, Simone Pieber, André S. H. Prévôt, Timothy B. Onasch, Douglas R. Worsnop, Hendryk Czech, Ralf Zimmermann, Jorma Jokiniemi, and Olli Sippula
Atmos. Chem. Phys., 16, 13251–13269, https://doi.org/10.5194/acp-16-13251-2016, https://doi.org/10.5194/acp-16-13251-2016, 2016
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Real-time measurements of OA aging and SOA formation from logwood combustion were conducted under dark and UV oxidation. Substantial SOA formation was observed in all experiments, leading to twice the initial OA mass emphasizing the importance of the burning conditions for the aging processes. The results prove that emissions are subject to intensive chemical processing in the atmosphere; e.g. the most of the POA was found to become oxidized after the ozone addition, forming aged POA.
Andrea M. Arangio, Haijie Tong, Joanna Socorro, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 16, 13105–13119, https://doi.org/10.5194/acp-16-13105-2016, https://doi.org/10.5194/acp-16-13105-2016, 2016
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We have quantified environmentally persistent free radicals and reactive oxygen species (ROS) in size-segregated atmospheric aerosol particles. We suggest that ROS were formed by decomposition of secondary organic aerosols interacting with transition metal ions and quinones contained in humic-like substances. The results have significant implications for aqueous-phase and cloud processing of organic aerosols as well as adverse health effects upon respiratory deposition of aerosol particles.
Pascale S. J. Lakey, Thomas Berkemeier, Manuel Krapf, Josef Dommen, Sarah S. Steimer, Lisa K. Whalley, Trevor Ingham, Maria T. Baeza-Romero, Ulrich Pöschl, Manabu Shiraiwa, Markus Ammann, and Dwayne E. Heard
Atmos. Chem. Phys., 16, 13035–13047, https://doi.org/10.5194/acp-16-13035-2016, https://doi.org/10.5194/acp-16-13035-2016, 2016
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Chemical oxidation in the atmosphere removes pollutants and greenhouse gases but generates undesirable products such as secondary organic aerosol. Radicals are key intermediates in oxidation, but how they interact with aerosols is still not well understood. Here we use a laser to measure the loss of radicals onto oxidised aerosols generated in a smog chamber. The loss of radicals was controlled by the thickness or viscosity of the aerosols, confirmed by using sugar aerosols of known thickness.
Natasha Hodas, Andreas Zuend, Katherine Schilling, Thomas Berkemeier, Manabu Shiraiwa, Richard C. Flagan, and John H. Seinfeld
Atmos. Chem. Phys., 16, 12767–12792, https://doi.org/10.5194/acp-16-12767-2016, https://doi.org/10.5194/acp-16-12767-2016, 2016
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Discontinuities in apparent hygroscopicity below and above water saturation have been observed for organic and mixed organic-inorganic aerosol particles in both laboratory studies and in the ambient atmosphere. This work explores the extent to which such discontinuities are influenced by organic component molecular mass and viscosity, non-ideal thermodynamic interactions between aerosol components, and the combination of these factors.
Elham Baranizadeh, Benjamin N. Murphy, Jan Julin, Saeed Falahat, Carly L. Reddington, Antti Arola, Lars Ahlm, Santtu Mikkonen, Christos Fountoukis, David Patoulias, Andreas Minikin, Thomas Hamburger, Ari Laaksonen, Spyros N. Pandis, Hanna Vehkamäki, Kari E. J. Lehtinen, and Ilona Riipinen
Geosci. Model Dev., 9, 2741–2754, https://doi.org/10.5194/gmd-9-2741-2016, https://doi.org/10.5194/gmd-9-2741-2016, 2016
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The molecular mechanisms through which new ultrafine (< 100 nm) aerosol particles are formed in the atmosphere have puzzled the scientific community for decades. In the past few years, however, significant progress has been made in unraveling these processes through laboratory studies and computational efforts. In this work we have implemented these new developments to an air quality model and study the implications of anthropogenically driven particle formation for European air quality.
Olli Väisänen, Antti Ruuskanen, Arttu Ylisirniö, Pasi Miettinen, Harri Portin, Liqing Hao, Ari Leskinen, Mika Komppula, Sami Romakkaniemi, Kari E. J. Lehtinen, and Annele Virtanen
Atmos. Chem. Phys., 16, 10385–10398, https://doi.org/10.5194/acp-16-10385-2016, https://doi.org/10.5194/acp-16-10385-2016, 2016
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In-cloud measurements of aerosol hygroscopicity and cloud droplet activation were conducted in Kuopio, Finland. According to the observations, the less hygroscopic accumulation mode particles were present in the non-activated aerosol, whereas the more hygroscopic particles were scavenged into cloud droplets. The results illustrate the sensitivity of cloud droplet formation to varying chemical composition and highlight the need for proper treatment of anthropogenic aerosols in CCN predictions.
Anna L. Hodshire, Michael J. Lawler, Jun Zhao, John Ortega, Coty Jen, Taina Yli-Juuti, Jared F. Brewer, Jack K. Kodros, Kelley C. Barsanti, Dave R. Hanson, Peter H. McMurry, James N. Smith, and Jeffery R. Pierce
Atmos. Chem. Phys., 16, 9321–9348, https://doi.org/10.5194/acp-16-9321-2016, https://doi.org/10.5194/acp-16-9321-2016, 2016
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Processes that control the growth of newly formed particles are not well understood and limit predictions of aerosol climate impacts. We combine state-of-the-art measurements at a central-US site with a particle-growth model to investigate the species and processes contributing to growth. Observed growth was dominated by organics, sulfate salts, or a mixture of these two. The model qualitatively captures the variability between different days.
Riikka Väänänen, Radovan Krejci, Hanna E. Manninen, Antti Manninen, Janne Lampilahti, Stephany Buenrostro Mazon, Tuomo Nieminen, Taina Yli-Juuti, Jenni Kontkanen, Ari Asmi, Pasi P. Aalto, Petri Keronen, Toivo Pohja, Ewan O'Connor, Veli-Matti Kerminen, Tuukka Petäjä, and Markku Kulmala
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2016-556, https://doi.org/10.5194/acp-2016-556, 2016
Revised manuscript has not been submitted
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A light aircraft was used as a platform to explore the horizontal and vertical variability of the aerosol particles over a boreal forest in Central Finland. This information is needed when data measured at ground level station is extrapolated and parameterized to represent the
conditions of the larger scale. The measurements showed that despite local fluctuations there was a good agreement between the on-ground and airborne measurements inside the planetary boundary layer.
Tero Mielonen, Anca Hienola, Thomas Kühn, Joonas Merikanto, Antti Lipponen, Tommi Bergman, Hannele Korhonen, Pekka Kolmonen, Larisa Sogacheva, Darren Ghent, Antti Arola, Gerrit de Leeuw, and Harri Kokkola
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2016-625, https://doi.org/10.5194/acp-2016-625, 2016
Revised manuscript not accepted
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We studied the temperature dependence of AOD and its radiative effects over the southeastern US. We used spaceborne observations of AOD, LST and tropospheric NO2 with simulations of ECHAM-HAMMOZ. The level of AOD in this region is governed by anthropogenic emissions but the temperature dependency is most likely caused by BVOC emissions. According to the observations and simulations, the regional clear-sky DRE for biogenic aerosols is −0.43 ± 0.88 W/m2/K and −0.86 ± 0.06 W/m2/K, respectively.
Jani Huttunen, Harri Kokkola, Tero Mielonen, Mika Esa Juhani Mononen, Antti Lipponen, Juha Reunanen, Anders Vilhelm Lindfors, Santtu Mikkonen, Kari Erkki Juhani Lehtinen, Natalia Kouremeti, Alkiviadis Bais, Harri Niska, and Antti Arola
Atmos. Chem. Phys., 16, 8181–8191, https://doi.org/10.5194/acp-16-8181-2016, https://doi.org/10.5194/acp-16-8181-2016, 2016
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For a good estimate of the current forcing by anthropogenic aerosols, knowledge in past is needed. One option to lengthen time series is to retrieve aerosol optical depth from solar radiation measurements. We have evaluated several methods for this task. Most of the methods produce aerosol optical depth estimates with a good accuracy. However, machine learning methods seem to be the most applicable not to produce any systematic biases, since they do not need constrain the aerosol properties.
Jenni Kontkanen, Tinja Olenius, Katrianne Lehtipalo, Hanna Vehkamäki, Markku Kulmala, and Kari E. J. Lehtinen
Atmos. Chem. Phys., 16, 5545–5560, https://doi.org/10.5194/acp-16-5545-2016, https://doi.org/10.5194/acp-16-5545-2016, 2016
Ying Li, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 16, 3327–3344, https://doi.org/10.5194/acp-16-3327-2016, https://doi.org/10.5194/acp-16-3327-2016, 2016
Haijie Tong, Andrea M. Arangio, Pascale S. J. Lakey, Thomas Berkemeier, Fobang Liu, Christopher J. Kampf, William H. Brune, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 16, 1761–1771, https://doi.org/10.5194/acp-16-1761-2016, https://doi.org/10.5194/acp-16-1761-2016, 2016
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We provide experimental evidence that terpene and isoprene SOA form substantial amounts of OH radicals upon interaction with liquid water and iron. Our measurements and model results imply that the chemical reactivity of SOA in the atmosphere, particularly in clouds, can be faster than previously thought. Inhalation and deposition of SOA particles in the human respiratory tract may lead to a substantial release of OH radicals in vivo, causing oxidative stress and adverse aerosol health effects.
J. Kim, L. Ahlm, T. Yli-Juuti, M. Lawler, H. Keskinen, J. Tröstl, S. Schobesberger, J. Duplissy, A. Amorim, F. Bianchi, N. M. Donahue, R. C. Flagan, J. Hakala, M. Heinritzi, T. Jokinen, A. Kürten, A. Laaksonen, K. Lehtipalo, P. Miettinen, T. Petäjä, M. P. Rissanen, L. Rondo, K. Sengupta, M. Simon, A. Tomé, C. Williamson, D. Wimmer, P. M. Winkler, S. Ehrhart, P. Ye, J. Kirkby, J. Curtius, U. Baltensperger, M. Kulmala, K. E. J. Lehtinen, J. N. Smith, I. Riipinen, and A. Virtanen
Atmos. Chem. Phys., 16, 293–304, https://doi.org/10.5194/acp-16-293-2016, https://doi.org/10.5194/acp-16-293-2016, 2016
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The hygroscopicity of nucleated nanoparticles was measured in the presence of sulfuric acid, sulfuric acid-dimethylamine, and sulfuric acid-organics derived from α-pinene oxidation during CLOUD7 at CERN in 2012. The hygroscopicity parameter κ decreased with increasing particle size, indicating decreasing acidity of particles.
D. M. Lienhard, A. J. Huisman, U. K. Krieger, Y. Rudich, C. Marcolli, B. P. Luo, D. L. Bones, J. P. Reid, A. T. Lambe, M. R. Canagaratna, P. Davidovits, T. B. Onasch, D. R. Worsnop, S. S. Steimer, T. Koop, and T. Peter
Atmos. Chem. Phys., 15, 13599–13613, https://doi.org/10.5194/acp-15-13599-2015, https://doi.org/10.5194/acp-15-13599-2015, 2015
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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.
T. Nieminen, T. Yli-Juuti, H. E. Manninen, T. Petäjä, V.-M. Kerminen, and M. Kulmala
Atmos. Chem. Phys., 15, 12385–12396, https://doi.org/10.5194/acp-15-12385-2015, https://doi.org/10.5194/acp-15-12385-2015, 2015
E. F. Mikhailov, G. N. Mironov, C. Pöhlker, X. Chi, M. L. Krüger, M. Shiraiwa, J.-D. Förster, U. Pöschl, S. S. Vlasenko, T. I. Ryshkevich, M. Weigand, A. L. D. Kilcoyne, and M. O. Andreae
Atmos. Chem. Phys., 15, 8847–8869, https://doi.org/10.5194/acp-15-8847-2015, https://doi.org/10.5194/acp-15-8847-2015, 2015
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Our manuscript describes the hygroscopic properties of accumulation- and coarse-mode aerosol particles sampled at the ZOTTO in central Siberia (61º N, 89º E). The hygroscopic growth measurements were supplemented with chemical analyses of the samples. In addition, the microstructure and chemical composition of aerosol particles were analyzed by x-ray micro-spectroscopy (STXM-NEXAFS) and transmission electron microscopy (TEM).
A. Leskinen, P. Yli-Pirilä, K. Kuuspalo, O. Sippula, P. Jalava, M.-R. Hirvonen, J. Jokiniemi, A. Virtanen, M. Komppula, and K. E. J. Lehtinen
Atmos. Meas. Tech., 8, 2267–2278, https://doi.org/10.5194/amt-8-2267-2015, https://doi.org/10.5194/amt-8-2267-2015, 2015
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A 29 m3 Teflon chamber was characterized and tested with oxidation experiments of toluene. Secondary organic aerosol yields of 12-42 % were obtained. These yields are comparable to those obtained in other laboratories.
M. J. Tang, M. Shiraiwa, U. Pöschl, R. A. Cox, and M. Kalberer
Atmos. Chem. Phys., 15, 5585–5598, https://doi.org/10.5194/acp-15-5585-2015, https://doi.org/10.5194/acp-15-5585-2015, 2015
E. Giannakaki, A. Pfüller, K. Korhonen, T. Mielonen, L. Laakso, V. Vakkari, H. Baars, R. Engelmann, J. P. Beukes, P. G. Van Zyl, M. Josipovic, P. Tiitta, K. Chiloane, S. Piketh, H. Lihavainen, K. E. J. Lehtinen, and M. Komppula
Atmos. Chem. Phys., 15, 5429–5442, https://doi.org/10.5194/acp-15-5429-2015, https://doi.org/10.5194/acp-15-5429-2015, 2015
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In this study we summarize 1 year of Raman lidar observations over South Africa. The analyses of lidar measurements presented here could assist in bridging existing gaps in the knowledge of vertical distribution of aerosols above South Africa, since limited long-term data of this type are available for this region. For the first time, we have been able to cover the full seasonal cycle on geometrical characteristics and optical properties of free tropospheric aerosol layers in the region.
L. Q. Hao, A. Kortelainen, S. Romakkaniemi, H. Portin, A. Jaatinen, A. Leskinen, M. Komppula, P. Miettinen, D. Sueper, A. Pajunoja, J. N. Smith, K. E. J. Lehtinen, D. R. Worsnop, A. Laaksonen, and A. Virtanen
Atmos. Chem. Phys., 14, 13483–13495, https://doi.org/10.5194/acp-14-13483-2014, https://doi.org/10.5194/acp-14-13483-2014, 2014
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Positive matrix factorization (PMF) was applied to the unified high-resolution mass spectra organic species with NO+ and NO2+ ions from the measurement in a mixed region between the boreal forestland and the urban area. The PMF analysis succeeded in separating the mixed spectra into three distinct organic factors and one inorganic factor. The particulate organic nitrate was distinguished by PMF for the first time, with a contribution of one-third of the total nitrate mass.
T. Berkemeier, M. Shiraiwa, U. Pöschl, and T. Koop
Atmos. Chem. Phys., 14, 12513–12531, https://doi.org/10.5194/acp-14-12513-2014, https://doi.org/10.5194/acp-14-12513-2014, 2014
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Glassy organic particles can serve as ice nuclei at low temperatures. We provide a rationale for these findings using a numerical aerosol diffusion model that describes particle phase state and its kinetics during simulated atmospheric updrafts dependent upon composition, size, updraft velocity, temperature and humidity. Our simulations suggest that aerosols from anthropogenic aromatic organics can be particularly relevant for ice cloud formation.
M. Shiraiwa, T. Berkemeier, K. A. Schilling-Fahnestock, J. H. Seinfeld, and U. Pöschl
Atmos. Chem. Phys., 14, 8323–8341, https://doi.org/10.5194/acp-14-8323-2014, https://doi.org/10.5194/acp-14-8323-2014, 2014
C. L. Loza, J. S. Craven, L. D. Yee, M. M. Coggon, R. H. Schwantes, M. Shiraiwa, X. Zhang, K. A. Schilling, N. L. Ng, M. R. Canagaratna, P. J. Ziemann, R. C. Flagan, and J. H. Seinfeld
Atmos. Chem. Phys., 14, 1423–1439, https://doi.org/10.5194/acp-14-1423-2014, https://doi.org/10.5194/acp-14-1423-2014, 2014
T. Yli-Juuti, K. Barsanti, L. Hildebrandt Ruiz, A.-J. Kieloaho, U. Makkonen, T. Petäjä, T. Ruuskanen, M. Kulmala, and I. Riipinen
Atmos. Chem. Phys., 13, 12507–12524, https://doi.org/10.5194/acp-13-12507-2013, https://doi.org/10.5194/acp-13-12507-2013, 2013
S. A. K. Häkkinen, H. E. Manninen, T. Yli-Juuti, J. Merikanto, M. K. Kajos, T. Nieminen, S. D. D'Andrea, A. Asmi, J. R. Pierce, M. Kulmala, and I. Riipinen
Atmos. Chem. Phys., 13, 7665–7682, https://doi.org/10.5194/acp-13-7665-2013, https://doi.org/10.5194/acp-13-7665-2013, 2013
H. Keskinen, A. Virtanen, J. Joutsensaari, G. Tsagkogeorgas, J. Duplissy, S. Schobesberger, M. Gysel, F. Riccobono, J. G. Slowik, F. Bianchi, T. Yli-Juuti, K. Lehtipalo, L. Rondo, M. Breitenlechner, A. Kupc, J. Almeida, A. Amorim, E. M. Dunne, A. J. Downard, S. Ehrhart, A. Franchin, M.K. Kajos, J. Kirkby, A. Kürten, T. Nieminen, V. Makhmutov, S. Mathot, P. Miettinen, A. Onnela, T. Petäjä, A. Praplan, F. D. Santos, S. Schallhart, M. Sipilä, Y. Stozhkov, A. Tomé, P. Vaattovaara, D. Wimmer, A. Prevot, J. Dommen, N. M. Donahue, R.C. Flagan, E. Weingartner, Y. Viisanen, I. Riipinen, A. Hansel, J. Curtius, M. Kulmala, D. R. Worsnop, U. Baltensperger, H. Wex, F. Stratmann, and A. Laaksonen
Atmos. Chem. Phys., 13, 5587–5600, https://doi.org/10.5194/acp-13-5587-2013, https://doi.org/10.5194/acp-13-5587-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Physics (physical properties and processes)
Microphysics of liquid water in sub-10 nm ultrafine aerosol particles
Comparing the ice nucleation properties of the kaolin minerals kaolinite and halloysite
Physicochemical properties of charcoal aerosols derived from biomass pyrolysis affect their ice-nucleating abilities at cirrus and mixed-phase cloud conditions
Reconsideration of surface tension and phase state effects on cloud condensation nuclei activity based on the atomic force microscopy measurement
Technical note: Sublimation of frozen CsCl solutions in ESEM: determining the number and size of salt particles relevant to sea-salt aerosols
Hygroscopicity and CCN potential of DMS-derived aerosol particles
Hybrid water adsorption and solubility partitioning for aerosol hygroscopicity and droplet growth
Experimental development of a lake spray source function and its model implementation for Great Lakes surface emissions
The effectiveness of the coagulation sink of 3–10 nm atmospheric particles
What caused the interdecadal shift in the El Niño–Southern Oscillation (ENSO) impact on dust mass concentration over northwestern South Asia?
Measurement report: An exploratory study of fluorescence and cloud condensation nuclei activity of urban aerosols in San Juan, Puerto Rico
Viscosity and physical state of sucrose mixed with ammonium sulfate droplets
Distribution and stable carbon isotopic composition of dicarboxylic acids, ketocarboxylic acids and α-dicarbonyls in fresh and aged biomass burning aerosols
Time dependence of heterogeneous ice nucleation by ambient aerosols: laboratory observations and a formulation for models
Laboratory studies of ice nucleation onto bare and internally mixed soot–sulfuric acid particles
Enhanced soot particle ice nucleation ability induced by aggregate compaction and densification
Opinion: Insights into updating Ambient Air Quality Directive 2008/50/EC
On the evolution of sub- and super-saturated water uptake of secondary organic aerosol in chamber experiments from mixed precursors
Hygroscopicity of organic compounds as a function of organic functionality, water solubility, molecular weight, and oxidation level
Particle emissions from a modern heavy-duty diesel engine as ice nuclei in immersion freezing mode: a laboratory study on fossil and renewable fuels
Comparison of saturation vapor pressures of α-pinene + O3 oxidation products derived from COSMO-RS computations and thermal desorption experiments
Physical and chemical properties of black carbon and organic matter from different combustion and photochemical sources using aerodynamic aerosol classification
Technical note: Pyrolysis principles explain time-resolved organic aerosol release from biomass burning
The effect of (NH4)2SO4 on the freezing properties of non-mineral dust ice-nucleating substances of atmospheric relevance
Heterogeneous ice nucleation ability of aerosol particles generated from Arctic sea surface microlayer and surface seawater samples at cirrus temperatures
Aerosol formation and growth rates from chamber experiments using Kalman smoothing
Phase state of secondary organic aerosol in chamber photo-oxidation of mixed precursors
Ice nucleation on surrogates of boreal forest SOA particles: effect of water content and oxidative age
Viscosity and phase state of aerosol particles consisting of sucrose mixed with inorganic salts
Observations on hygroscopic growth and phase transitions of mixed 1, 2, 6-hexanetriol ∕ (NH4)2SO4 particles: investigation of the liquid–liquid phase separation (LLPS) dynamic process and mechanism and secondary LLPS during the dehumidification
Boundary layer structure characteristics under objective classification of persistent pollution weather types in the Beijing area
Properties and emission factors of cloud condensation nuclei from biomass cookstoves – observations of a strong dependency on potassium content in the fuel
Measurement report: Effects of NOx and seed aerosol on highly oxygenated organic molecules (HOMs) from cyclohexene ozonolysis
Interactions of organosulfates with water vapor under sub- and supersaturated conditions
Laboratory study of the collection efficiency of submicron aerosol particles by cloud droplets – Part I: Influence of relative humidity
Size-resolved atmospheric ice-nucleating particles during East Asian dust events
Aqueous-phase behavior of glyoxal and methylglyoxal observed with carbon and oxygen K-edge X-ray absorption spectroscopy
Brown carbon's emission factors and optical characteristics in household biomass burning: developing a novel algorithm for estimating the contribution of brown carbon
Effect of mixing structure on the water uptake of mixtures of ammonium sulfate and phthalic acid particles
Toward closure between predicted and observed particle viscosity over a wide range of temperatures and relative humidity
The effects of morphology, mobility size, and secondary organic aerosol (SOA) material coating on the ice nucleation activity of black carbon in the cirrus regime
The ice-nucleating activity of Arctic sea surface microlayer samples and marine algal cultures
Comparing secondary organic aerosol (SOA) volatility distributions derived from isothermal SOA particle evaporation data and FIGAERO–CIMS measurements
Laboratory studies of fresh and aged biomass burning aerosol emitted from east African biomass fuels – Part 1: Optical properties
Enhanced growth rate of atmospheric particles from sulfuric acid
Composition and volatility of secondary organic aerosol (SOA) formed from oxidation of real tree emissions compared to simplified volatile organic compound (VOC) systems
Effects of SO2 on optical properties of secondary organic aerosol generated from photooxidation of toluene under different relative humidity conditions
Influence of the dry aerosol particle size distribution and morphology on the cloud condensation nuclei activation. An experimental and theoretical investigation
Experimental investigation into the volatilities of highly oxygenated organic molecules (HOMs)
Detection of tar brown carbon with a single particle soot photometer (SP2)
Xiaohan Li and Ian C. Bourg
Atmos. Chem. Phys., 23, 2525–2556, https://doi.org/10.5194/acp-23-2525-2023, https://doi.org/10.5194/acp-23-2525-2023, 2023
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Aerosol particles with sizes smaller than 50 nm impact cloud formation and precipitation. Representation of this effect is hindered by limited understanding of the properties of liquid water in these particles. Our simulations of aerosol particles containing salt or organic compounds reveal that water enters a less cohesive phase at droplet sizes below 4 nm. This effect causes important deviations from theoretical predictions of aerosol properties, including phase state and hygroscopic growth.
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
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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.
Fabian Mahrt, Carolin Rösch, Kunfeng Gao, Christopher H. Dreimol, Maria A. Zawadowicz, and Zamin A. Kanji
Atmos. Chem. Phys., 23, 1285–1308, https://doi.org/10.5194/acp-23-1285-2023, https://doi.org/10.5194/acp-23-1285-2023, 2023
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Major aerosol types emitted by biomass burning include soot, ash, and charcoal particles. Here, we investigated the ice nucleation activity of 400 nm size-selected particles of two different pyrolyis-derived charcoal types in the mixed phase and cirrus cloud regime. We find that ice nucleation is constrained to cirrus cloud conditions, takes place via pore condensation and freezing, and is largely governed by the particle porosity and mineral content.
Chun Xiong, Xueyan Chen, Xiaolei Ding, Binyu Kuang, Xiangyu Pei, Zhengning Xu, Shikuan Yang, Huan Hu, and Zhibin Wang
Atmos. Chem. Phys., 22, 16123–16135, https://doi.org/10.5194/acp-22-16123-2022, https://doi.org/10.5194/acp-22-16123-2022, 2022
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Water surface tension is applied widely in current aerosol–cloud models but could be inappropriate in the presence of atmospheric surfactants. With cloud condensation nuclei (CCN) activity and atomic force microscopy (AFM) measurement results of mixed inorganic salt and dicarboxylic acid particles, we concluded that surface tension reduction and phase state should be carefully considered in aerosol–cloud interactions. Our results could help to decease uncertainties in climate models.
Ľubica Vetráková, Vilém Neděla, Kamila Závacká, Xin Yang, and Dominik Heger
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-684, https://doi.org/10.5194/acp-2022-684, 2022
Revised manuscript accepted for ACP
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Salt aerosols are important to polar atmospheric chemistry and global climate. Therefore, we utilized a unique electron microscope to identify the most suitable conditions for formation of the small salt (CsCl) particles, proxies of the aerosols, from sublimating salty snow. Very low sublimation temperature and low salt concentration are needed for formation of such particles. These observations may help us to better understood polar spring ozone depletion and bromine explosion events.
Bernadette Rosati, Sini Isokääntä, Sigurd Christiansen, Mads Mørk Jensen, Shamjad P. Moosakutty, Robin Wollesen de Jonge, Andreas Massling, Marianne Glasius, Jonas Elm, Annele Virtanen, and Merete Bilde
Atmos. Chem. Phys., 22, 13449–13466, https://doi.org/10.5194/acp-22-13449-2022, https://doi.org/10.5194/acp-22-13449-2022, 2022
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Sulfate aerosols have a strong influence on climate. Due to the reduction in sulfur-based fossil fuels, natural sulfur emissions play an increasingly important role. Studies investigating the climate relevance of natural sulfur aerosols are scarce. We study the water uptake of such particles in the laboratory, demonstrating a high potential to take up water and form cloud droplets. During atmospheric transit, chemical processing affects the particles’ composition and thus their water uptake.
Kanishk Gohil, Chun-Ning Mao, Dewansh Rastogi, Chao Peng, Mingjin Tang, and Akua Asa-Awuku
Atmos. Chem. Phys., 22, 12769–12787, https://doi.org/10.5194/acp-22-12769-2022, https://doi.org/10.5194/acp-22-12769-2022, 2022
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The Hybrid Activity Model (HAM) is a promising new droplet growth model that can be potentially used for the analysis of any type of atmospheric compound. HAM may potentially improve the representation of hygroscopicity of organic aerosols in large-scale global climate models (GCMs), hence reducing the uncertainties in the climate forcing due to the aerosol indirect effect.
Charbel Harb and Hosein Foroutan
Atmos. Chem. Phys., 22, 11759–11779, https://doi.org/10.5194/acp-22-11759-2022, https://doi.org/10.5194/acp-22-11759-2022, 2022
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A model representation of lake spray aerosol (LSA) ejection from freshwater breaking waves is crucial for understanding their climatic and public health impacts. We develop an LSA emission parameterization and implement it in an atmospheric model to investigate Great Lakes surface emissions. We find that the same breaking wave is likely to produce fewer aerosols in freshwater than in saltwater and that Great Lakes emissions influence the regional aerosol burden and can reach the cloud layer.
Runlong Cai, Ella Häkkinen, Chao Yan, Jingkun Jiang, Markku Kulmala, and Juha Kangasluoma
Atmos. Chem. Phys., 22, 11529–11541, https://doi.org/10.5194/acp-22-11529-2022, https://doi.org/10.5194/acp-22-11529-2022, 2022
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The influences of new particle formation on the climate and air quality are governed by particle survival, which has been under debate due to uncertainties in the coagulation sink. Here we measure the coagulation coefficient of sub-10 nm particles and demonstrate that collisions between the freshly nucleated and background particles can effectively lead to coagulation. We further show that the effective coagulation sink is consistent with the new particle formation measured in urban Beijing.
Lamei Shi, Jiahua Zhang, Da Zhang, Jingwen Wang, Xianglei Meng, Yuqin Liu, and Fengmei Yao
Atmos. Chem. Phys., 22, 11255–11274, https://doi.org/10.5194/acp-22-11255-2022, https://doi.org/10.5194/acp-22-11255-2022, 2022
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Dust impacts climate and human life. Analyzing the interdecadal change in dust activity and its influence factors is crucial for disaster mitigation. Based on a linear regression method, this study revealed the interdecadal variability of relationships between ENSO and dust over northwestern South Asia from 1982 to 2014 and analyzed the effects of atmospheric factors on this interdecadal variability. The result sheds new light on numerical simulation involving the interdecadal variation of dust.
Bighnaraj Sarangi, Darrel Baumgardner, Benjamin Bolaños-Rosero, and Olga L. Mayol-Bracero
Atmos. Chem. Phys., 22, 9647–9661, https://doi.org/10.5194/acp-22-9647-2022, https://doi.org/10.5194/acp-22-9647-2022, 2022
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Here, the fluorescent characteristics and cloud-forming efficiency of aerosols at an urban site in Puerto Rico are discussed. The results from this pilot study highlight the capabilities of ultraviolet-induced fluorescence (UV-IF) measurements for characterizing the properties of fluorescing aerosol particles, as they relate to the daily evolution of primary biological aerosol particles. This work has established a database of measurements on which future, longer-term studies will be initiated.
Rani Jeong, Joseph Lilek, Andreas Zuend, Rongshuang Xu, Man Nin Chan, Dohyun Kim, Hi Gyu Moon, and Mijung Song
Atmos. Chem. Phys., 22, 8805–8817, https://doi.org/10.5194/acp-22-8805-2022, https://doi.org/10.5194/acp-22-8805-2022, 2022
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In this study, the viscosities of particles of sucrose–H2O, AS–H2O, and sucrose–AS–H2O for OIRs of 4:1, 1:1, and 1:4 for decreasing RH, were quantified by poke-and-flow and bead-mobility techniques at 293 ± 1 K. Based on the viscosity results, the particles of binary and ternary systems ranged from liquid to semisolid, and even the solid state depending on the RH. Moreover, we compared the measured viscosities of ternary systems to the predicted viscosities with excellent agreement.
Minxia Shen, Kin Fai Ho, Wenting Dai, Suixin Liu, Ting Zhang, Qiyuan Wang, Jingjing Meng, Judith C. Chow, John G. Watson, Junji Cao, and Jianjun Li
Atmos. Chem. Phys., 22, 7489–7504, https://doi.org/10.5194/acp-22-7489-2022, https://doi.org/10.5194/acp-22-7489-2022, 2022
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Looking at characteristics and δ13C compositions of dicarboxylic acids and related compounds in BB aerosols, we used a combined combustion and aging system to generate fresh and aged aerosols from burning straw. The results showed the emission factors (EFaged) of total diacids of aging experiments were around an order of magnitude higher than EFfresh. This meant that dicarboxylic acids are involved with secondary photochemical processes in the atmosphere rather than primary emissions from BB.
Jonas K. F. Jakobsson, Deepak B. Waman, Vaughan T. J. Phillips, and Thomas Bjerring Kristensen
Atmos. Chem. Phys., 22, 6717–6748, https://doi.org/10.5194/acp-22-6717-2022, https://doi.org/10.5194/acp-22-6717-2022, 2022
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Long-lived cold-layer clouds at subzero temperatures are observed to be remarkably persistent in their generation of ice particles and snow precipitation. There is uncertainty about why this is so. This motivates the present lab study to observe the long-term ice-nucleating ability of aerosol samples from the real troposphere. Time dependence of their ice nucleation is observed to be weak in lab experiments exposing the samples to isothermal conditions for up to about 10 h.
Kunfeng Gao, Chong-Wen Zhou, Eszter J. Barthazy Meier, and Zamin A. Kanji
Atmos. Chem. Phys., 22, 5331–5364, https://doi.org/10.5194/acp-22-5331-2022, https://doi.org/10.5194/acp-22-5331-2022, 2022
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Incomplete combustion of fossil fuel produces carbonaceous particles called soot. These particles can affect cloud formation by acting as centres for droplet or ice formation. The atmospheric residence time of soot particles is of the order of days to weeks, which can result in them becoming coated by various trace species in the atmosphere such as acids. In this study, we quantify the cirrus cloud-forming ability of soot particles coated with the atmospherically ubiquitous sulfuric acid.
Kunfeng Gao, Franz Friebel, Chong-Wen Zhou, and Zamin A. Kanji
Atmos. Chem. Phys., 22, 4985–5016, https://doi.org/10.5194/acp-22-4985-2022, https://doi.org/10.5194/acp-22-4985-2022, 2022
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Soot particles impact cloud formation and radiative properties in the upper atmosphere where aircraft emit carbonaceous particles. We use cloud chambers to mimic the upper atmosphere temperature and humidity to test the influence of the morphology of the soot particles on ice cloud formation. For particles larger than 200 nm, the compacted (densified) samples have a higher affinity for ice crystal formation in the cirrus regime than the fluffy (un-compacted) soot particles of the same sample.
Joel Kuula, Hilkka Timonen, Jarkko V. Niemi, Hanna E. Manninen, Topi Rönkkö, Tareq Hussein, Pak Lun Fung, Sasu Tarkoma, Mikko Laakso, Erkka Saukko, Aino Ovaska, Markku Kulmala, Ari Karppinen, Lasse Johansson, and Tuukka Petäjä
Atmos. Chem. Phys., 22, 4801–4808, https://doi.org/10.5194/acp-22-4801-2022, https://doi.org/10.5194/acp-22-4801-2022, 2022
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Modern and up-to-date policies and air quality management strategies are instrumental in tackling global air pollution. As the European Union is preparing to revise Ambient Air Quality Directive 2008/50/EC, this paper initiates discussion on selected features of the directive that we believe would benefit from a reassessment. The scientific community has the most recent and deepest understanding of air pollution; thus, its contribution is essential.
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
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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.
Shuang Han, Juan Hong, Qingwei Luo, Hanbing Xu, Haobo Tan, Qiaoqiao Wang, Jiangchuan Tao, Yaqing Zhou, Long Peng, Yao He, Jingnan Shi, Nan Ma, Yafang Cheng, and Hang Su
Atmos. Chem. Phys., 22, 3985–4004, https://doi.org/10.5194/acp-22-3985-2022, https://doi.org/10.5194/acp-22-3985-2022, 2022
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We present the hygroscopicity of 23 organic species with different physicochemical properties using a hygroscopicity tandem differential mobility analyzer (HTDMA) and compare the results with previous studies. Based on the hygroscopicity parameter κ, the influence of different physicochemical properties that potentially drive hygroscopicity, such as the functionality, water solubility, molar volume, and O : C ratio of organics, are examined separately.
Kimmo Korhonen, Thomas Bjerring Kristensen, John Falk, Vilhelm B. Malmborg, Axel Eriksson, Louise Gren, Maja Novakovic, Sam Shamun, Panu Karjalainen, Lassi Markkula, Joakim Pagels, Birgitta Svenningsson, Martin Tunér, Mika Komppula, Ari Laaksonen, and Annele Virtanen
Atmos. Chem. Phys., 22, 1615–1631, https://doi.org/10.5194/acp-22-1615-2022, https://doi.org/10.5194/acp-22-1615-2022, 2022
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We investigated the ice-nucleating abilities of particulate emissions from a modern diesel engine using the portable ice-nuclei counter SPIN, a continuous-flow diffusion chamber instrument. Three different fuels were studied without blending, including fossil diesel and two renewable fuels, testing different emission aftertreatment systems and photochemical aging. We found that the diesel emissions were inefficient ice nuclei, and aging had no or little effect on their ice-nucleating abilities.
Noora Hyttinen, Iida Pullinen, Aki Nissinen, Siegfried Schobesberger, Annele Virtanen, and Taina Yli-Juuti
Atmos. Chem. Phys., 22, 1195–1208, https://doi.org/10.5194/acp-22-1195-2022, https://doi.org/10.5194/acp-22-1195-2022, 2022
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Accurate saturation vapor pressure estimates of atmospherically relevant organic compounds are critical for modeling secondary organic aerosol (SOA) formation. We investigated vapor pressures of highly oxygenated SOA constituents using state-of-the-art computational and experimental methods. We found a good agreement between low and extremely low vapor pressures estimated using the two methods, and the smallest molecules detected in our experiment were likely products of thermal decomposition.
Dawei Hu, M. Rami Alfarra, Kate Szpek, Justin M. Langridge, Michael I. Cotterell, Claire Belcher, Ian Rule, Zixia Liu, Chenjie Yu, Yunqi Shao, Aristeidis Voliotis, Mao Du, Brett Smith, Greg Smallwood, Prem Lobo, Dantong Liu, Jim M. Haywood, Hugh Coe, and James D. Allan
Atmos. Chem. Phys., 21, 16161–16182, https://doi.org/10.5194/acp-21-16161-2021, https://doi.org/10.5194/acp-21-16161-2021, 2021
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Here, we developed new techniques for investigating these properties in the laboratory and applied these to BC and BrC from different sources, including diesel exhaust, inverted propane flame and wood combustion. These have allowed us to quantify the changes in shape and chemical composition of different soots according to source and variables such as the moisture content of wood.
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
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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.
Soleil E. Worthy, Anand Kumar, Yu Xi, Jingwei Yun, Jessie Chen, Cuishan Xu, Victoria E. Irish, Pierre Amato, and Allan K. Bertram
Atmos. Chem. Phys., 21, 14631–14648, https://doi.org/10.5194/acp-21-14631-2021, https://doi.org/10.5194/acp-21-14631-2021, 2021
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We studied the effect of (NH4)2SO4 on the immersion freezing of non-mineral dust ice-nucleating substances (INSs) and mineral dusts. (NH4)2SO4 had no effect on the median freezing temperature of 9 of the 10 tested non-mineral dust INSs, slightly decreased that of the other, and increased that of all the mineral dusts. The difference in the response of mineral dust and non-mineral dust INSs to (NH4)2SO4 suggests that they nucleate ice and/or interact with (NH4)2SO4 via different mechanisms.
Robert Wagner, Luisa Ickes, Allan K. Bertram, Nora Els, Elena Gorokhova, Ottmar Möhler, Benjamin J. Murray, Nsikanabasi Silas Umo, and Matthew E. Salter
Atmos. Chem. Phys., 21, 13903–13930, https://doi.org/10.5194/acp-21-13903-2021, https://doi.org/10.5194/acp-21-13903-2021, 2021
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Sea spray aerosol particles are a mixture of inorganic salts and organic matter from phytoplankton organisms. At low temperatures in the upper troposphere, both inorganic and organic constituents can induce the formation of ice crystals and thereby impact cloud properties and climate. In this study, we performed experiments in a cloud simulation chamber with particles produced from Arctic seawater samples to quantify the relative contribution of inorganic and organic species in ice formation.
Matthew Ozon, Dominik Stolzenburg, Lubna Dada, Aku Seppänen, and Kari E. J. Lehtinen
Atmos. Chem. Phys., 21, 12595–12611, https://doi.org/10.5194/acp-21-12595-2021, https://doi.org/10.5194/acp-21-12595-2021, 2021
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Measuring the rate at which aerosol particles are formed is of importance for understanding climate change. We present an analysis method based on Kalman smoothing, which retrieves new particle formation and growth rates from size-distribution measurements. We apply it to atmospheric simulation chamber experiments and show that it agrees well with traditional methods. In addition, it provides reliable uncertainty estimates, and we suggest instrument design optimisation for signal processing.
Yu Wang, Aristeidis Voliotis, Yunqi Shao, Taomou Zong, Xiangxinyue Meng, Mao Du, Dawei Hu, Ying Chen, Zhijun Wu, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 21, 11303–11316, https://doi.org/10.5194/acp-21-11303-2021, https://doi.org/10.5194/acp-21-11303-2021, 2021
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Aerosol phase behaviour plays a profound role in atmospheric physicochemical processes. We designed dedicated chamber experiments to study the phase state of secondary organic aerosol from biogenic and anthropogenic mixed precursors. Our results highlight the key role of the organic–inorganic ratio and relative humidity in phase state, but the sources and organic composition are less important. The result provides solid laboratory evidence for understanding aerosol phase in a complex atmosphere.
Ana A. Piedehierro, André Welti, Angela Buchholz, Kimmo Korhonen, Iida Pullinen, Ilkka Summanen, Annele Virtanen, and Ari Laaksonen
Atmos. Chem. Phys., 21, 11069–11078, https://doi.org/10.5194/acp-21-11069-2021, https://doi.org/10.5194/acp-21-11069-2021, 2021
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Ice crystals in cirrus clouds contain particles that start ice formation. We study whether particles forming above boreal forests can help in the making of cirrus clouds and if the water content in the particles affects this property. In the laboratory, we made boreal-forest-like particles and cooled and humidified them to measure whether an ice crystal develops. We found that only when dry can these particles form an ice crystal but no better than solution droplets.
Young-Chul Song, Joseph Lilek, Jae Bong Lee, Man Nin Chan, Zhijun Wu, Andreas Zuend, and Mijung Song
Atmos. Chem. Phys., 21, 10215–10228, https://doi.org/10.5194/acp-21-10215-2021, https://doi.org/10.5194/acp-21-10215-2021, 2021
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We report viscosity of binary mixtures of organic material / H2O and inorganic salts / H2O, as well as ternary mixtures of organic material / inorganic salts/ H2O, over the atmospheric relative humidity (RH) range. The viscosity measurements indicate that the studied mixed organic–inorganic particles range in phase state from liquid to semi-solid or even solid across the atmospheric RH range at a temperature of 293 K.
Shuaishuai Ma, Zhe Chen, Shufeng Pang, and Yunhong Zhang
Atmos. Chem. Phys., 21, 9705–9717, https://doi.org/10.5194/acp-21-9705-2021, https://doi.org/10.5194/acp-21-9705-2021, 2021
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LLPS, efflorescence and deliquescence of aerosol particles can be observed visually and determined quantitatively. Different LLPS mechanisms may dominate successively in mixed organic–inorganic particles. The formation of more concentrated inorganic inclusions may cause secondary LLPS. Furthermore, high inorganic factions may result in an inorganic salt crust enclosing the separated organic phases.
Zhaobin Sun, Xiujuan Zhao, Ziming Li, Guiqian Tang, and Shiguang Miao
Atmos. Chem. Phys., 21, 8863–8882, https://doi.org/10.5194/acp-21-8863-2021, https://doi.org/10.5194/acp-21-8863-2021, 2021
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Different weather types will shape significantly different structures of the pollution boundary layer. The findings of this study allow us to understand the inherent difference among heavy pollution boundary layers; in addition, they reveal the formation mechanism of haze pollution from an integrated synoptic-scale and boundary layer structure perspective.
Thomas Bjerring Kristensen, John Falk, Robert Lindgren, Christina Andersen, Vilhelm B. Malmborg, Axel C. Eriksson, Kimmo Korhonen, Ricardo Luis Carvalho, Christoffer Boman, Joakim Pagels, and Birgitta Svenningsson
Atmos. Chem. Phys., 21, 8023–8044, https://doi.org/10.5194/acp-21-8023-2021, https://doi.org/10.5194/acp-21-8023-2021, 2021
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Residential biomass combustion is a major anthropogenic source of aerosol particles on regional and global scales. Nevertheless, little is known about those aerosol particles' ability to act as cloud condensation nuclei (CCN) and thus influence cloud properties and climate. Our study shows a strong link between the potassium content in the fuel and emissions of CCN for different stove technologies. Previous studies may have underestimated the anthropogenic climate impact of these emissions.
Meri Räty, Otso Peräkylä, Matthieu Riva, Lauriane Quéléver, Olga Garmash, Matti Rissanen, and Mikael Ehn
Atmos. Chem. Phys., 21, 7357–7372, https://doi.org/10.5194/acp-21-7357-2021, https://doi.org/10.5194/acp-21-7357-2021, 2021
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Cyclohexene resembles certain relatively complex compounds in the atmosphere that through oxidation produce vapours that take part in aerosol formation. We studied the highly oxygenated organic molecules (HOMs) formed in cyclohexene ozonolysis, the relationship between their chemical composition and their tendency to condense onto seed aerosol, as well as the effect of NOx pollutants on their signals. Two existing models were also tested for their ability to predict the volatility of the HOMs.
Chao Peng, Patricia N. Razafindrambinina, Kotiba A. Malek, Lanxiadi Chen, Weigang Wang, Ru-Jin Huang, Yuqing Zhang, Xiang Ding, Maofa Ge, Xinming Wang, Akua A. Asa-Awuku, and Mingjin Tang
Atmos. Chem. Phys., 21, 7135–7148, https://doi.org/10.5194/acp-21-7135-2021, https://doi.org/10.5194/acp-21-7135-2021, 2021
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Organosulfates are important constituents in tropospheric aerosol particles, but their hygroscopic properties and cloud condensation nuclei activities are not well understood. In our work, three complementary techniques were employed to investigate the interactions of 11 organosulfates with water vapor under sub- and supersaturated conditions.
Alexis Dépée, Pascal Lemaitre, Thomas Gelain, Marie Monier, and Andrea Flossmann
Atmos. Chem. Phys., 21, 6945–6962, https://doi.org/10.5194/acp-21-6945-2021, https://doi.org/10.5194/acp-21-6945-2021, 2021
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Present article describe a new In-Cloud Aerosol Scavenging Experiment (In-CASE) that has been conceived to measure the collection efficiency of submicron aerosol particles by cloud droplets. The present article focuses on the influence of phoretic effects on the collection efficiency.
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
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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.
Georgia Michailoudi, Jack J. Lin, Hayato Yuzawa, Masanari Nagasaka, Marko Huttula, Nobuhiro Kosugi, Theo Kurtén, Minna Patanen, and Nønne L. Prisle
Atmos. Chem. Phys., 21, 2881–2894, https://doi.org/10.5194/acp-21-2881-2021, https://doi.org/10.5194/acp-21-2881-2021, 2021
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This study provides insight into hydration of two significant atmospheric compounds, glyoxal and methylglyoxal. Using synchrotron radiation excited X-ray absorption spectroscopy, we confirm that glyoxal is fully hydrated in water, and for the first time, we experimentally detect enol structures in aqueous methylglyoxal. Our results support the contribution of these compounds to secondary organic aerosol formation, known to have a large uncertainty in atmospheric models and climate predictions.
Jianzhong Sun, Yuzhe Zhang, Guorui Zhi, Regina Hitzenberger, Wenjing Jin, Yingjun Chen, Lei Wang, Chongguo Tian, Zhengying Li, Rong Chen, Wen Xiao, Yuan Cheng, Wei Yang, Liying Yao, Yang Cao, Duo Huang, Yueyuan Qiu, Jiali Xu, Xiaofei Xia, Xin Yang, Xi Zhang, Zheng Zong, Yuchun Song, and Changdong Wu
Atmos. Chem. Phys., 21, 2329–2341, https://doi.org/10.5194/acp-21-2329-2021, https://doi.org/10.5194/acp-21-2329-2021, 2021
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Brown carbon (BrC) emission factors from household biomass fuels were measured with an integrating sphere optics approach supported by iterative calculations. A novel algorithm to directly estimate the absorption contribution of BrC relative to that of BrC + black carbon (FBrC) was proposed based purely on the absorption exponent (AAE)
(FBrC = 0.5519 lnAAE + 0.0067). The FBrC for household biomass fuels was as high as 50.8 % across the strongest solar spectral range of 350−850 nm.
Weigang Wang, Ting Lei, Andreas Zuend, Hang Su, Yafang Cheng, Yajun Shi, Maofa Ge, and Mingyuan Liu
Atmos. Chem. Phys., 21, 2179–2190, https://doi.org/10.5194/acp-21-2179-2021, https://doi.org/10.5194/acp-21-2179-2021, 2021
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Aerosol mixing state regulates the interactions between water molecules and particles and thus controls aerosol activation and hygroscopic growth, which thereby influences visibility degradation, cloud formation, and its radiative forcing. However, there are few studies attempting to investigate their interactions with water molecules. Here, we investigated the effect of organic coatings on the hygroscopic behavior of the inorganic core.
Sabin Kasparoglu, Ying Li, Manabu Shiraiwa, and Markus D. Petters
Atmos. Chem. Phys., 21, 1127–1141, https://doi.org/10.5194/acp-21-1127-2021, https://doi.org/10.5194/acp-21-1127-2021, 2021
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Viscosity is important because it determines the lifetime, impact, and fate of particulate matter. We collected new data to rigorously test a framework that is used to constrain the phase state in global simulations. We find that the framework is accurate as long as appropriate compound specific inputs are available.
Cuiqi Zhang, Yue Zhang, Martin J. Wolf, Leonid Nichman, Chuanyang Shen, Timothy B. Onasch, Longfei Chen, and Daniel J. Cziczo
Atmos. Chem. Phys., 20, 13957–13984, https://doi.org/10.5194/acp-20-13957-2020, https://doi.org/10.5194/acp-20-13957-2020, 2020
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Black carbon (BC) is considered the second most important global warming agent. However, the role of BC aerosol–cloud–climate interactions in the cirrus formation remains uncertain. Our study of selected BC types and sizes suggests that increases in diameter, compactness, and/or surface oxidation of BC particles lead to more efficient ice nucleation (IN) via pore condensation freezing (PCF) pathways，and that coatings of common secondary organic aerosol (SOA) materials can inhibit ice formation.
Luisa Ickes, Grace C. E. Porter, Robert Wagner, Michael P. Adams, Sascha Bierbauer, Allan K. Bertram, Merete Bilde, Sigurd Christiansen, Annica M. L. Ekman, Elena Gorokhova, Kristina Höhler, Alexei A. Kiselev, Caroline Leck, Ottmar Möhler, Benjamin J. Murray, Thea Schiebel, Romy Ullrich, and Matthew E. Salter
Atmos. Chem. Phys., 20, 11089–11117, https://doi.org/10.5194/acp-20-11089-2020, https://doi.org/10.5194/acp-20-11089-2020, 2020
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The Arctic is a region where aerosols are scarce. Sea spray might be a potential source of aerosols acting as ice-nucleating particles. We investigate two common phytoplankton species (Melosira arctica and Skeletonema marinoi) and present their ice nucleation activity in comparison with Arctic seawater microlayer samples from different field campaigns. We also aim to understand the aerosolization process of marine biological samples and the potential effect on the ice nucleation activity.
Olli-Pekka Tikkanen, Angela Buchholz, Arttu Ylisirniö, Siegfried Schobesberger, Annele Virtanen, and Taina Yli-Juuti
Atmos. Chem. Phys., 20, 10441–10458, https://doi.org/10.5194/acp-20-10441-2020, https://doi.org/10.5194/acp-20-10441-2020, 2020
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We compared the volatility distributions of secondary organic aerosol (SOA) constituents estimated from isothermal evaporation experiments from either particle size change data, by process modelling and global optimization, or from mass spectrometer data with positive matrix factorization analysis. Our results show that, despite the two very different estimation methods, the volatility distributions are comparable if uncertainties are taken into account.
Damon M. Smith, Marc N. Fiddler, Rudra P. Pokhrel, and Solomon Bililign
Atmos. Chem. Phys., 20, 10149–10168, https://doi.org/10.5194/acp-20-10149-2020, https://doi.org/10.5194/acp-20-10149-2020, 2020
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Biomass burning aerosol can scatter and absorb light, contributing to the cooling or warming of the planet. The scattering and absorption properties (optical properties) change as aerosol ages and interacts with atmospheric gases. Optical properties also depend on burning conditions, fuel type, and morphology. Africa is a major source of biomass burning aerosols, but there are very few laboratory studies. This study focuses on the optical properties of aerosols from east African biomass fuels.
Dominik Stolzenburg, Mario Simon, Ananth Ranjithkumar, Andreas Kürten, Katrianne Lehtipalo, Hamish Gordon, Sebastian Ehrhart, Henning Finkenzeller, Lukas Pichelstorfer, Tuomo Nieminen, Xu-Cheng He, Sophia Brilke, Mao Xiao, António Amorim, Rima Baalbaki, Andrea Baccarini, Lisa Beck, Steffen Bräkling, Lucía Caudillo Murillo, Dexian Chen, Biwu Chu, Lubna Dada, António Dias, Josef Dommen, Jonathan Duplissy, Imad El Haddad, Lukas Fischer, Loic Gonzalez Carracedo, Martin Heinritzi, Changhyuk Kim, Theodore K. Koenig, Weimeng Kong, Houssni Lamkaddam, Chuan Ping Lee, Markus Leiminger, Zijun Li, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Tatjana Müller, Wei Nie, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Matti P. Rissanen, Birte Rörup, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Mingyi Wang, Yonghong Wang, Stefan K. Weber, Daniela Wimmer, Peter J. Wlasits, Yusheng Wu, Qing Ye, Marcel Zauner-Wieczorek, Urs Baltensperger, Kenneth S. Carslaw, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Armin Hansel, Markku Kulmala, Jos Lelieveld, Rainer Volkamer, Jasper Kirkby, and Paul M. Winkler
Atmos. Chem. Phys., 20, 7359–7372, https://doi.org/10.5194/acp-20-7359-2020, https://doi.org/10.5194/acp-20-7359-2020, 2020
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Sulfuric acid is a major atmospheric vapour for aerosol formation. If new particles grow fast enough, they can act as cloud droplet seeds or affect air quality. In a controlled laboratory set-up, we demonstrate that van der Waals forces enhance growth from sulfuric acid. We disentangle the effects of ammonia, ions and particle hydration, presenting a complete picture of sulfuric acid growth from molecular clusters onwards. In a climate model, we show its influence on the global aerosol budget.
Arttu Ylisirniö, Angela Buchholz, Claudia Mohr, Zijun Li, Luis Barreira, Andrew Lambe, Celia Faiola, Eetu Kari, Taina Yli-Juuti, Sergey A. Nizkorodov, Douglas R. Worsnop, Annele Virtanen, and Siegfried Schobesberger
Atmos. Chem. Phys., 20, 5629–5644, https://doi.org/10.5194/acp-20-5629-2020, https://doi.org/10.5194/acp-20-5629-2020, 2020
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We studied the chemical composition and volatility of secondary organic aerosol (SOA) particles formed from emissions of Scots pines and compared those results to SOA formed from α-pinene and from a sesquiterpene mixture. We found that SOA formed from single precursors cannot capture the properties of SOA formed from real plant emissions.
Wenyu Zhang, Weigang Wang, Junling Li, Chao Peng, Kun Li, Li Zhou, Bo Shi, Yan Chen, Mingyuan Liu, and Maofa Ge
Atmos. Chem. Phys., 20, 4477–4492, https://doi.org/10.5194/acp-20-4477-2020, https://doi.org/10.5194/acp-20-4477-2020, 2020
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We investigated the effect of SO2 under different humidities on optical properties of toluene-derived SOA under four conditions with CRDs and PAX at 532 and 375 nm, respectively. Our results showed that SO2 under different humidities can change the refractive complex index of toluene SOA by influencing the multiphase processes and altering the aerosol chemical compositions. Different atmospheric conditions could affect the properties of toluene SOA, as well as the global radiative balance.
Junteng Wu, Alessandro Faccinetto, Symphorien Grimonprez, Sébastien Batut, Jérôme Yon, Pascale Desgroux, and Denis Petitprez
Atmos. Chem. Phys., 20, 4209–4225, https://doi.org/10.5194/acp-20-4209-2020, https://doi.org/10.5194/acp-20-4209-2020, 2020
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Soot particles released during anthropogenic activities may lead to positive direct or negative indirect climate forcing depending on their aging in the atmosphere. The latter occurs whenever soot particles act as cloud condensation nuclei (CCN) and trigger the formation of persistent clouds. Herein, we investigate the impact of the size distribution and morphology of freshly emitted soot particles on their aging process and propose a model to quantitatively predict their efficiency as CCN.
Otso Peräkylä, Matthieu Riva, Liine Heikkinen, Lauriane Quéléver, Pontus Roldin, and Mikael Ehn
Atmos. Chem. Phys., 20, 649–669, https://doi.org/10.5194/acp-20-649-2020, https://doi.org/10.5194/acp-20-649-2020, 2020
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Highly oxygenated organic molecules have been suggested to form a large part of secondary organic aerosol. However, with their exotic structures, their volatilities are not well known, making their exact role in particle formation hard to assess. In laboratory experiments, we found the volatility of HOMs formed in the ozonolysis of the monoterpene alpha-pinene to be in the middle of earlier estimates. The volatilities of HOMs could be well explained in terms of their molecular formulae.
Joel C. Corbin and Martin Gysel-Beer
Atmos. Chem. Phys., 19, 15673–15690, https://doi.org/10.5194/acp-19-15673-2019, https://doi.org/10.5194/acp-19-15673-2019, 2019
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We review the literature to refine the definition of "tar balls" (or tar particles). Then, using a marine-engine data set, we show that a standard SP2 can identify tar particles in two ways, as evaporating and non-incandescing (30 % of tar particles by number) or incandescing particles which scatter more light than soot at incandescence (70 % of tar particles by number). To our knowledge, no other technique can provide in situ, real-time evidence for the presence of tar particles in an aerosol.
Cited articles
Abramson, E., Imre, D., Beránek, J., Wilson, J., and Zelenyuk, A.:
Experimental determination of chemical diffusion within secondary organic
aerosol particles, Phys. Chem. Chem. Phys., 15, 2983–2991,
https://doi.org/10.1039/C2CP44013J, 2013.
Arangio, A. M., Slade, J. H., Berkemeier, T., Pöschl, 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, https://doi.org/10.1021/jp510489z, 2015.
Bayes, T., Price, R., and Canton, J.: An essay towards solving a problem in the
doctrine of chances, Philos. T. Roy. Soc., https://doi.org/10.1098/rstl.1763.0053, 1763.
Berkemeier, T., Steimer, S. S., Krieger, K. U., Peter, T., Pöschl, U.,
Ammann, M., and Shiraiwa, M.: Ozone uptake on glassy, semi-solid and liquid
organic matter and the role of reactive oxygen intermediates in atmospheric
aerosol chemistry, Phys. Chem. Chem. Phys., 18, 12662–12674,
https://doi.org/10.1039/C6CP00634E, 2016.
Berkemeier, T., Ammann, M., Krieger, U. K., Peter, T., Spichtinger, P., Pöschl, U., Shiraiwa, M., and Huisman, A. J.: Technical note: Monte Carlo genetic algorithm (MCGA) for model analysis of multiphase chemical kinetics to determine transport and reaction rate coefficients using multiple experimental data sets, Atmos. Chem. Phys., 17, 8021–8029, https://doi.org/10.5194/acp-17-8021-2017, 2017.
Bilde, M., Barsanti, K., Booth, M., Cappa, C. D., Donahue, N. M.,
Emanuelsson, E. U., McFiggans, G., Krieger, U. K., Marcolli, C., Topping,
D., Ziemann, P., Barley, M., Clegg, S., Dennis-Smither, B., Hallquist, M.,
Hallquist, Åsa M, Khlystov, A., Kulmala, M., Mogensen, D.,
Percival, C. J., Pope, F., Reid, J. P., V Ribeiro da Silva, M. A.,
Rosenoern, T., Salo, K., Pia Soonsin, V., Yli-Juuti, T., Prisle, N. L.,
Pagels, J., Rarey, J., Zardini, A. A., and Riipinen, I.: Saturation Vapor
Pressures and Transition Enthalpies of Low- Volatility Organic Molecules of
Atmospheric Relevance: From Dicarboxylic Acids to Complex Mixtures, Chem.
Rev., 115, 4115–4156, https://doi.org/10.1021/cr5005502, 2015.
Carpenter, B., Gelman, A., Hoffman, M. D., Lee, D., Goodrich, B.,
Betancourt, M., Brubaker, M., Guo, J., Li, P., and Riddell, A.: Stan: A
probabilistic programming language, J. Stat. Softw., 76, 1–32, https://doi.org/10.18637/jss.v076.i01, 2017.
Davies, J. F., Haddrell, A. E., and Reid, J. P.: Time-Resolved Measurements
of the Evaporation of Volatile Components from Single Aerosol Droplets,
Aerosol Sci. Tech., 46, 666–677, https://doi.org/10.1080/02786826.2011.652750,
2012.
Davies, J. F., Haddrell, A. E., Rickards, A. M. J., and Reid, J. P.:
Simultaneous Analysis of the Equilibrium Hygroscopicity and Water Transport
Kinetics of Liquid Aerosol, Anal. Chem., 85, 5819–5826,
https://doi.org/10.1021/ac4005502, 2013.
Donahue, N. M., Robinson, A. L., Stanier, C. O., and Pandis, S. N.: Coupled
partitioning, dilution, and chemical aging of semivolatile organics,
Environ. Sci. Technol., 40, 2635–2643, https://doi.org/10.1021/es052297c, 2006.
Einstein, A.: Über die von der molekularkinetischen Theorie der
Wärme geforderte Bewegung von in ruhenden Flüssigkeiten
suspendierten Teilchen, Ann. Phys., 322, 549–560,
https://doi.org/10.1002/andp.19053220806, 1905.
Gelman, A., Stern, H. S., Carlin, J. B., Dunson, D. B., Vehtari, A., and
Rubin, D. B.: Bayesian data analysis, Chapman and Hall/CRC, Boca Raton, FL, USA, 2013.
Glantschnig, W. J. and Chen, S.-H.: Light scattering from water droplets in
the geometrical optics approximation, Appl. Optics, 20, 2499,
https://doi.org/10.1364/AO.20.002499, 1981.
Hallquist, M., Wenger, J. C., Baltensperger, U., Rudich, Y., Simpson, D., Claeys, M., Dommen, J., Donahue, N. M., George, C., Goldstein, A. H., Hamilton, J. F., Herrmann, H., Hoffmann, T., Iinuma, Y., Jang, M., Jenkin, M. E., Jimenez, J. L., Kiendler-Scharr, A., Maenhaut, W., McFiggans, G., Mentel, Th. F., Monod, A., Prévôt, A. S. H., Seinfeld, J. H., Surratt, J. D., Szmigielski, R., and Wildt, J.: The formation, properties and impact of secondary organic aerosol: current and emerging issues, Atmos. Chem. Phys., 9, 5155–5236, https://doi.org/10.5194/acp-9-5155-2009, 2009.
Haynes, W. M.: CRC handbook of chemistry and physics, 6th ed., CRC press, Boca Raton, FL, USA,
2009.
Hernández, W. P., Castello, D. A., Roitman, N., and Magluta, C.:
Thermorheologically simple materials: A bayesian framework for model
calibration and validation, J. Sound Vib., 402, 14–30,
https://doi.org/10.1016/j.jsv.2017.05.005, 2017.
Hoffman, M. D. and Gelman, A.: The No-U-turn sampler: adaptively setting
path lengths in Hamiltonian Monte Carlo., J. Mach. Learn. Res., 15,
1593–1623, 2014.
Jimenez, J. L., Canagaratna, M. R., Donahue, N. M., Prevot, A. S. H., Zhang,
Q., Kroll, J. H., DeCarlo, P. F., Allan, J. D., Coe, H., Ng, N. L., Aiken,
A. C., Docherty, K. S., Ulbrich, I. M., Grieshop, A. P., Robinson, A. L.,
Duplissy, J., Smith, J. D., Wilson, K. R., Lanz, V. A., Hueglin, C., Sun, Y.
L., Tian, J., Laaksonen, A., Raatikainen, T., Rautiainen, J., Vaattovaara,
P., Ehn, M., Kulmala, M., Tomlinson, J. M., Collins, D. R., Cubison, M. J.,
Dunlea, E. J., Huffman, J. A., Onasch, T. B., Alfarra, M. R., Williams, P.
I., Bower, K., Kondo, Y., Schneider, J., Drewnick, F., Borrmann, S., Weimer,
S., Demerjian, K., Salcedo, D., Cottrell, L., Griffin, R., Takami, A.,
Miyoshi, T., Hatakeyama, S., Shimono, A., Sun, J. Y., Zhang, Y. M., Dzepina,
K., Kimmel, J. R., Sueper, D., Jayne, J. T., Herndon, S. C., Trimborn, A.
M., Williams, L. R., Wood, E. C., Middlebrook, A. M., Kolb, C. E.,
Baltensperger, U., Worsnop, D. R., and Worsnop, D. R.: Evolution of organic
aerosols in the atmosphere, Science, 326, 1525–1529,
https://doi.org/10.1126/science.1180353, 2009.
Kaipio, J. P., Kolehmainen, V., Somersalo, E., and Vauhkonen, M.: Statistical
inversion and Monte Carlo sampling methods in electrical impedance
tomography, Inverse Probl., 16, 1487, https://doi.org/10.1088/0266-5611/16/5/321,
2000.
Kanakidou, M., Seinfeld, J. H., Pandis, S. N., Barnes, I., Dentener, F. J., Facchini, M. C., Van Dingenen, R., Ervens, B., Nenes, A., Nielsen, C. J., Swietlicki, E., Putaud, J. P., Balkanski, Y., Fuzzi, S., Horth, J., Moortgat, G. K., Winterhalter, R., Myhre, C. E. L., Tsigaridis, K., Vignati, E., Stephanou, E. G., and Wilson, J.: Organic aerosol and global climate modelling: a review, Atmos. Chem. Phys., 5, 1053–1123, https://doi.org/10.5194/acp-5-1053-2005, 2005.
Krieger, U. K., Siegrist, F., Marcolli, C., Emanuelsson, E. U., Gøbel, F. M., Bilde, M., Marsh, A., Reid, J. P., Huisman, A. J., Riipinen, I., Hyttinen, N., Myllys, N., Kurtén, T., Bannan, T., Percival, C. J., and Topping, D.: A reference data set for validating vapor pressure measurement techniques: homologous series of polyethylene glycols, Atmos. Meas. Tech., 11, 49–63, https://doi.org/10.5194/amt-11-49-2018, 2018.
Kulmala, M., Vesala, T., and Wagner, P. E.: An analytical expression for the
rate of binary condensational particle growth, Proc. R. Soc. Lon. Ser.-A, 441,
589–605, https://doi.org/10.1098/rspa.1993.0081, 1993.
Kulmala, M., Vesala, T., Schwarz, J., and Smolik, J.: Mass transfer from a
drop – II. Theoretical analysis of temperature dependent mass flux
correlation, Int. J. Heat Mass Tran., 38, 1705–1708,
https://doi.org/10.1016/0017-9310(94)00302-C, 1995.
Lehtinen, K. E. J. and Kulmala, M.: A model for particle formation and growth in the atmosphere with molecular resolution in size, Atmos. Chem. Phys., 3, 251–257, https://doi.org/10.5194/acp-3-251-2003, 2003.
Liu, P., Li, Y. J., Wang, Y., Gilles, M. K., Zaveri, R. A., Bertram, A. K.,
and Martin, S. T.: Lability of secondary organic particulate matter, P.
Natl. Acad. Sci. USA, 113, 12643–12648,
https://doi.org/10.1073/pnas.1603138113, 2016.
Lowe, S., Partridge, D. G., Topping, D., and Stier, P.: Inverse modelling of Köhler theory – Part 1: A response surface analysis of CCN spectra with respect to surface-active organic species, Atmos. Chem. Phys., 16, 10941–10963, https://doi.org/10.5194/acp-16-10941-2016, 2016.
Marsh, A., Miles, R. E. H., Rovelli, G., Cowling, A. G., Nandy, L., Dutcher, C. S., and Reid, J. P.: Influence of organic compound functionality on aerosol hygroscopicity: dicarboxylic acids, alkyl-substituents, sugars and amino acids, Atmos. Chem. Phys., 17, 5583–5599, https://doi.org/10.5194/acp-17-5583-2017, 2017.
Metropolis, N., Rosenbluth, A. W., Rosenbluth, M. N., Teller, A. H., and
Teller, E.: Equation of State Calculations by Fast Computing Machines, J.
Chem. Phys., 21, 1087–1092, https://doi.org/10.1063/1.1699114, 1953.
O'Meara, S., Topping, D. O., and McFiggans, G.: The rate of equilibration of viscous aerosol particles, Atmos. Chem. Phys., 16, 5299–5313, https://doi.org/10.5194/acp-16-5299-2016, 2016.
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., Petäjä, T., and Virtanen, A.: Adsorptive uptake of water by
semisolid secondary organic aerosols, Geophys. Res. Lett., 42,
3063–3068, https://doi.org/10.1002/2015GL063142, 2015.
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, https://doi.org/10.1039/c3sc50682g, 2013.
Reid, J. P., Bertram, A. K., Topping, D. O., Laskin, A., Martin, S. T.,
Petters, M. D., Pope, F. D., and Rovelli, G.: The viscosity of
atmospherically relevant organic particles, Nat. Commun., 9, 956,
https://doi.org/10.1038/s41467-018-03027-z, 2018.
Reid, R. C., Prausnitz, J. M. and Poling, B. E.: The properties of gases and
liquids, 4th ed., McGraw Hill Book Co, New York, NY, USA, 1987.
Renbaum-Wolff, L., Grayson, J. W., Bateman, A. P., Kuwata, M., Sellier, M.,
Murray, B. J., Shilling, J. E., Martin, S. T., and Bertram, A. K.: Viscosity
of α-pinene secondary organic material and implications for particle
growth and reactivity, P. Natl. Acad. Sci. USA, 110, 8014–8019,
https://doi.org/10.1073/pnas.1219548110, 2013.
Rovelli, G., Miles, R. E. H., Reid, J. P., and Clegg, S. L.: Accurate
Measurements of Aerosol Hygroscopic Growth over a Wide Range in Relative
Humidity, J. Phys. Chem. A, 120, 4376–4388,
https://doi.org/10.1021/acs.jpca.6b04194, 2016.
Rumble, J., R., Lide, D., R., and Bruno, T., J.: CRC handbook of chemistry
and physics, 99th ed., CRC press, Taylor & Francis Group, Boca
Raton, FL., USA, 2018.
Shiraiwa, M., Pfrang, C., Koop, T., and Pöschl, U.: Kinetic multi-layer model of gas-particle interactions in aerosols and clouds (KM-GAP): linking condensation, evaporation and chemical reactions of organics, oxidants and water, Atmos. Chem. Phys., 12, 2777–2794, https://doi.org/10.5194/acp-12-2777-2012, 2012.
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,
https://doi.org/10.1039/c3cp51595h, 2013.
Shiraiwa, M., Li, Y., Tsimpidi, A. P., Karydis, V. A., Berkemeier, T.,
Pandis, S. N., Lelieveld, J., Koop, T., and Pöschl, U.: Global
distribution of particle phase state in atmospheric secondary organic
aerosols, Nat. Commun., 8, 15002, https://doi.org/10.1038/ncomms15002, 2017.
Song, Y. C., Haddrell, A. E., Bzdek, B. R., Reid, J. P., Bannan, T.,
Topping, D. O., Percival, C., and Cai, C.: Measurements and Predictions of
Binary Component Aerosol Particle Viscosity, J. Phys. Chem. A, 120,
8123–8137, https://doi.org/10.1021/acs.jpca.6b07835, 2016.
Tsigaridis, K., Daskalakis, N., Kanakidou, M., Adams, P. J., Artaxo, P., Bahadur, R., Balkanski, Y., Bauer, S. E., Bellouin, N., Benedetti, A., Bergman, T., Berntsen, T. K., Beukes, J. P., Bian, H., Carslaw, K. S., Chin, M., Curci, G., Diehl, T., Easter, R. C., Ghan, S. J., Gong, S. L., Hodzic, A., Hoyle, C. R., Iversen, T., Jathar, S., Jimenez, J. L., Kaiser, J. W., Kirkevåg, A., Koch, D., Kokkola, H., Lee, Y. H., Lin, G., Liu, X., Luo, G., Ma, X., Mann, G. W., Mihalopoulos, N., Morcrette, J.-J., Müller, J.-F., Myhre, G., Myriokefalitakis, S., Ng, N. L., O'Donnell, D., Penner, J. E., Pozzoli, L., Pringle, K. J., Russell, L. M., Schulz, M., Sciare, J., Seland, Ø., Shindell, D. T., Sillman, S., Skeie, R. B., Spracklen, D., Stavrakou, T., Steenrod, S. D., Takemura, T., Tiitta, P., Tilmes, S., Tost, H., van Noije, T., van Zyl, P. G., von Salzen, K., Yu, F., Wang, Z., Wang, Z., Zaveri, R. A., Zhang, H., Zhang, K., Zhang, Q., and Zhang, X.: The AeroCom evaluation and intercomparison of organic aerosol in global models, Atmos. Chem. Phys., 14, 10845–10895, https://doi.org/10.5194/acp-14-10845-2014, 2014.
Vaden, T. D., Imre, D., Beránek, J., Shrivastava, M., and Zelenyuk, A.:
Evaporation kinetics and phase of laboratory and ambient secondary
organic aerosol, P. Natl. Acad. Sci. USA, 108, 2190–2195,
https://doi.org/10.1073/pnas.1013391108, 2011.
Varvia, P., Rautiainen, M., and Seppänen, A.: Bayesian estimation of
seasonal course of canopy leaf area index from hyperspectral satellite data,
J. Quant. Spectrosc. Ra., 208, 19–28,
https://doi.org/10.1016/j.jqsrt.2018.01.008, 2018.
Vesala, T., Kulmala, M., Rudolf, R., Vrtala, A., and Wagner, P. E.: Models
for condensational growth and evaporation of binary aerosol particles, J.
Aerosol Sci., 28, 565–598, https://doi.org/10.1016/S0021-8502(96)00461-2, 1997.
Virtanen, A., Joutsensaari, J., Koop, T., Kannosto, J., Yli-Pirilä, P.,
Leskinen, J., Mäkelä, J. M., Holopainen, J. K., Pöschl, 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.
Wilson, J., Imre, D., Beraek, J., Shrivastava, M., and Zelenyuk, A.:
Evaporation Kinetics of Laboratory-Generated Secondary Organic Aerosols at
Elevated Relative Humidity, Environ. Sci. Technol., 49, 243–249, https://doi.org/10.1021/es505331d, 2015.
Yli-Juuti, T., Pajunoja, A., Tikkanen, O.-P., Buchholz, A., Faiola, C.,
Väisänen, O., Hao, L., Kari, E., Peräkylä, O., Garmash, O.,
Shiraiwa, M., Ehn, M., Lehtinen, K., and Virtanen, A.: Factors controlling
the evaporation of secondary organic aerosol from α-pinene
ozonolysis, Geophys. Res. Lett., 44, 2562–2570,
https://doi.org/10.1002/2016GL072364, 2017.
Zuend, A., Marcolli, C., Luo, B. P., and Peter, T.: A thermodynamic model of mixed organic-inorganic aerosols to predict activity coefficients, Atmos. Chem. Phys., 8, 4559–4593, https://doi.org/10.5194/acp-8-4559-2008, 2008.
Zuend, A., Marcolli, C., Booth, A. M., Lienhard, D. M., Soonsin, V., Krieger, U. K., Topping, D. O., McFiggans, G., Peter, T., and Seinfeld, J. H.: New and extended parameterization of the thermodynamic model AIOMFAC: calculation of activity coefficients for organic-inorganic mixtures containing carboxyl, hydroxyl, carbonyl, ether, ester, alkenyl, alkyl, and aromatic functional groups, Atmos. Chem. Phys., 11, 9155–9206, https://doi.org/10.5194/acp-11-9155-2011, 2011.
Short summary
We assessed how well the organic aerosol particle composition and viscosity can be captured by optimizing process models to match particle evaporation data. We performed the analysis for both artificial and real evaporation data and tested two optimization algorithms. Our findings show that the optimization method yields a good estimate for the studied properties. The timescale of the evaporation data and particle size was found to be important in identifying the volatility of organic compounds.
We assessed how well the organic aerosol particle composition and viscosity can be captured by...
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