Articles | Volume 21, issue 12
https://doi.org/10.5194/acp-21-9705-2021
© Author(s) 2021. 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-21-9705-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
29 Jun 2021
Research article |
| 29 Jun 2021
| 29 Jun 2021
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
Shuaishuai Ma
The Institute of Chemical Physics, School of Chemistry and Chemical
Engineering, Beijing Institute of Technology, Beijing 100081, China
Zhe Chen
The Institute of Chemical Physics, School of Chemistry and Chemical
Engineering, Beijing Institute of Technology, Beijing 100081, China
The Institute of Chemical Physics, School of Chemistry and Chemical
Engineering, Beijing Institute of Technology, Beijing 100081, China
Yunhong Zhang
CORRESPONDING AUTHOR
The Institute of Chemical Physics, School of Chemistry and Chemical
Engineering, Beijing Institute of Technology, Beijing 100081, China
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Shuaishuai Ma, Qiong Li, and Yunhong Zhang
Atmos. Chem. Phys., 22, 10955–10970, https://doi.org/10.5194/acp-22-10955-2022, https://doi.org/10.5194/acp-22-10955-2022, 2022
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The nitrate phase state can play a critical role in determining the occurrence and extent of nitrate depletion in internally mixed NaNO3–DCA particles, which may be instructive for relevant aerosol reaction systems. Besides, organic acids have a potential to deplete nitrate based on the comprehensive consideration of acidity, particle-phase state, droplet water activity, and HNO3 gas-phase diffusion.
Bo Jing, Zhen Wang, Fang Tan, Yucong Guo, Shengrui Tong, Weigang Wang, Yunhong Zhang, and Maofa Ge
Atmos. Chem. Phys., 18, 5115–5127, https://doi.org/10.5194/acp-18-5115-2018, https://doi.org/10.5194/acp-18-5115-2018, 2018
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The nitrate/organic acid mixed aerosols exhibit varying phase behavior and hygroscopic growth depending upon the type of components in the particles. Our results reveal that the coexisting organic acid has considerable impacts on the phase and morphology of nitrate particles in the low and medium RH range, which thus result in obvious enhancement or suppression of water uptake with increasing RH. This new information provided here has important implications for atmospheric chemistry.
Xiaowei Wang, Bo Jing, Fang Tan, Jiabi Ma, Yunhong Zhang, and Maofa Ge
Atmos. Chem. Phys., 17, 12797–12812, https://doi.org/10.5194/acp-17-12797-2017, https://doi.org/10.5194/acp-17-12797-2017, 2017
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Our results reveal the formation of NH4HC2O4 and NH4HSO4 from the reaction of oxalic acid (OA) with ammonium sulfate within aerosols during the slow dehydration compared to the rapid dehydration process. The hygroscopic growth of mixed particles at high RH upon hydration is substantially lower than that of the corresponding dehydration process due to the significant formation of low hygroscopic NH4HC2O4 and residual OA. These findings have important implications for atmospheric chemistry.
Bo Jing, Shengrui Tong, Qifan Liu, Kun Li, Weigang Wang, Yunhong Zhang, and Maofa Ge
Atmos. Chem. Phys., 16, 4101–4118, https://doi.org/10.5194/acp-16-4101-2016, https://doi.org/10.5194/acp-16-4101-2016, 2016
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Water-soluble organic compounds (WSOCs) play an important role in the hygroscopicity of aerosols. The coexisting hygroscopic species such as levoglucosan, malonic acid, and phthalic acid have a strong influence on hygroscopic growth and phase behavior of oxalic acid, even suppressing its crystallization completely. The hygroscopic species such as levoglucosan in the mixed particles may significantly influence the hygroscopic behavior of ammonium sulfate by changing phase state of oxalic acid.
T. Lei, A. Zuend, W. G. Wang, Y. H. Zhang, and M. F. Ge
Atmos. Chem. Phys., 14, 11165–11183, https://doi.org/10.5194/acp-14-11165-2014, https://doi.org/10.5194/acp-14-11165-2014, 2014
Related subject area
Subject: Aerosols | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Physics (physical properties and processes)
Size-dependent hygroscopicity of levoglucosan and D-glucose aerosol nanoparticles
Technical note: Sublimation of frozen CsCl solutions in an environmental scanning electron microscope (ESEM) – determining the number and size of salt particles relevant to sea salt aerosols
Microphysics of liquid water in sub-10 nm ultrafine aerosol particles
Influence of the previous North Atlantic Oscillation (NAO) on the spring dust aerosols over North China
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
HUB: A method to model and extract the distribution of ice nucleation temperatures from drop-freezing experiments
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
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
Ting Lei, Hang Su, Nan Ma, Ulrich Pöschl, Alfred Wiedensohler, and Yafang Cheng
Atmos. Chem. Phys., 23, 4763–4774, https://doi.org/10.5194/acp-23-4763-2023, https://doi.org/10.5194/acp-23-4763-2023, 2023
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We investigate the hygroscopic behavior of levoglucosan and D-glucose nanoparticles using a nano-HTDMA. There is a weak size dependence of the hygroscopic growth factor of levoglucosan and D-glucose with diameters down to 20 nm, while a strong size dependence of the hygroscopic growth factor of D-glucose has been clearly observed in the size range 6 to 20 nm. The use of the DKA method leads to good agreement with the hygroscopic growth factor of glucose nanoparticles with diameters down to 6 nm.
Lubica Vetráková, Vilém Neděla, Kamila Závacká, Xin Yang, and Dominik Heger
Atmos. Chem. Phys., 23, 4463–4488, https://doi.org/10.5194/acp-23-4463-2023, https://doi.org/10.5194/acp-23-4463-2023, 2023
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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 understand polar spring ozone depletion and bromine explosion events.
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.
Yan Li, Falei Xu, Juan Feng, Mengying Du, Wenjun Song, Chao Li, and Wenjing Zhao
EGUsphere, https://doi.org/10.5194/egusphere-2023-52, https://doi.org/10.5194/egusphere-2023-52, 2023
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There is a significantly negative relationship between boreal winter North Atlantic Oscillation (NAO) and the dust aerosols (DAs) in the eastern part of China (30–40° N, 105–120° E), which is not a DAs source area but severely affected by the DEs. Under effect of the NAO negative phase, main atmospheric circulation during the dust events (DEs) is characterized due to variation of the transient eddy flux. The work is of reference value to the prediction of DEs and the understanding of their causes.
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.
Ingrid de Almeida Ribeiro, Konrad Meister, and Valeria Molinero
EGUsphere, https://doi.org/10.26434/chemrxiv-2022-ddzv8, https://doi.org/10.26434/chemrxiv-2022-ddzv8, 2022
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Ice formation is a key atmospheric process facilitated by a wide range of aerosols. We present a method to model and interpret of ice nucleation experiments and extract the distribution of potency of nucleation sites. We use the method to optimize conditions of laboratory sampling and extract distribution of ice nucleation temperatures from bacteria, fungi and pollen. These reveal unforeseen subpopulations of nuclei in these systems and how they respond to changes in their environment.
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.
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.
Cited articles
Ahn, K.-H., Kim, S.-M., Jung, H.-J., Lee, M.-J., Eom, H.-J., Maskey, S.,
and Ro, C.-U.: Combined use of optical and electron microscopic techniques
for the measurement of hygroscopic property, chemical composition, and
morphology of individual aerosol particles, Anal. Chem., 82, 7999–8009,
https://doi.org/10.1021/ac101432y, 2010.
Badger, C. L., Griffiths, P. T., George, I., Abbatt, J. P., and Cox, R. A.:
Reactive uptake of N2O5 by aerosol particles containing mixtures
of humic acid and ammonium sulfate, J. Phys. Chem. A, 110, 6986–6994,
https://doi.org/10.1021/jp0562678, 2006.
Bertram, A. K., Martin, S. T., Hanna, S. J., Smith, M. L., Bodsworth, A.,
Chen, Q., Kuwata, M., Liu, A., You, Y., and Zorn, S. R.: Predicting the
relative humidities of liquid-liquid phase separation, efflorescence, and
deliquescence of mixed particles of ammonium sulfate, organic material, and
water using the organic-to-sulfate mass ratio of the particle and the
oxygen-to-carbon elemental ratio of the organic component, Atmos. Chem.
Phys., 11, 10995–11006, https://doi.org/10.5194/acp-11-10995-2011, 2011.
Brown, S. S., Ryerson, T. B., Wollny, A. G., Brock, C. A., Peltier, R.,
Sullivan, A. P., Weber, R. J., Dube, W. P., Trainer, M., Meagher, J. F.,
Fehsenfeld, F. C., and Ravishankara, A. R.: Variability in nocturnal
nitrogen oxide processing and its role in regional air quality, Science,
311, 67–70, https://doi.org/10.1126/science.1120120, 2006.
Ciobanu, V. G., Marcolli, C., Krieger, U. K., Weers, U., and Peter, T.:
Liquid-liquid phase separation in mixed organic/inorganic aerosol particles,
J. Phys. Chem. A, 113, 10966–10978, https://doi.org/10.1021/jp905054d, 2009.
Cosman, L. M., Knopf, D. A., and Bertram, A. K.: N2O5 reactive
uptake on aqueous sulfuric acid solutions coated with branched and
straight-chain insoluble organic surfactants, J. Phys. Chem. A, 112,
2386–2396, https://doi.org/10.1021/jp710685r, 2008.
Ebert, M., Inerle-Hof, M., and Weinbruch, S.: Environmental scanning
electron microscopy as a new technique to determine the hygroscopic
behaviour of individual aerosol particles, Atmos. Environ., 36, 5909–5916, https://doi.org/10.1016/S1352-2310(02)00774-4, 2002.
Erdakos, G. B. and Pankow, J. F.: Gas/particle partitioning of neutral and
ionizing compounds to single- and multi-phase aerosol particles, 2. Phase
separation in liquid particulate matter containing both polar and
low-polarity organic compounds, Atmos. Environ., 38, 1005–1013,
https://doi.org/10.1016/j.atmosenv.2003.10.038, 2004.
Fard, M. M., Krieger, U. K., and Peter, T.: Kinetic limitation to inorganic
ion diffusivity and to coalescence of inorganic inclusions in viscous
liquid-liquid phase-separated particles, J. Phys. Chem. A, 121, 9284–9296,
https://doi.org/10.1021/acs.jpca.7b05242, 2017.
Gao, Y., Chen, S. B., and Yu, L. E.: Efflorescence relative humidity for
ammonium sulfate particles, J. Phys. Chem. A, 110, 7602–7608,
https://doi.org/10.1021/jp057574g, 2006.
Gao, Y., Yu, L. E., and Chen, S. B.: Theoretical investigation of substrate
effect on deliquescence relative humidity of NaCl particles, J. Phys. Chem.
A, 111, 633–639, https://doi.org/10.1021/jp0654967, 2007.
Hämeri, K., Laaksonen, A., Väkevä, M., and Suni, T.: Hygroscopic
growth of ultrafine sodium chloride particles, J. Geophys. Res.-Atmos., 106,
20749–20757, https://doi.org/10.1029/2000jd000200, 2001.
Haywood, J. and Boucher, O.: Estimates of the direct and indirect radiative
forcing due to tropospheric aerosols: A review, Rev. Geophys., 38, 513–543,
https://doi.org/10.1029/1999RG000078, 2000.
Heald, C. L., Kroll, J. H., Jimenez, J. L., Docherty, K. S., Decarlo, P. F.,
Aiken, A. C., Chen, Q., Martin, S. T., Farmer, D. K., and Artaxo, P.: A
simplified description of the evolution of organic aerosol composition in
the atmosphere, Geophys. Res. Lett., 37, L08803,
https://doi.org/10.1029/2010GL042737, 2010.
Hodas, N., Zuend, A., Schilling, K., Berkemeier, T., Shiraiwa, M., Flagan,
R. C., and Seinfeld, J. H.: Discontinuities in hygroscopic growth below and
above water saturation for laboratory surrogates of oligomers in organic
atmospheric aerosols, Atmos. Chem. Phys., 16, 12767–12792,
https://doi.org/10.5194/acp-16-12767-2016, 2016.
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., Marcolli, C., and Reid, J. P.: Exploring the complexity of
aerosol particle properties and processes using single particle techniques,
Chem. Soc. Rev., 41, 6631–6662, https://doi.org/10.1039/c2cs35082c, 2012.
Lee, S. H., Murphy, D. M., Thomson, D. S., and Middlebrook, A. M.: Chemical
components of single particles measured with Particle Analysis by Laser Mass
Spectrometry (PALMS) during the Atlanta SuperSite Project: Focus on
organic/sulfate, lead, soot, and mineral particles, J. Geophys. Res.-Atmos.,
107, 4003, https://doi.org/10.1029/2000JD000011, 2002.
Liu, P. F., Song, M., Zhao, T. N., Gunthe, S. S., Ham, S., He, Y. P., Qin,
Y. M., Gong, Z. H., Amorim, J. C., Bertram, A. K., and Martin, S. T.:
Resolving the mechanisms of hygroscopic growth and cloud condensation nuclei
activity for organic particulate matter, Nat. Commun., 9, 4076,
https://doi.org/10.1038/s41467-018-06622-2, 2018.
Lv, X. J., Chen, Z., Ma, J. B., and Zhang, Y. H.: Volatility measurements of
1, 2, 6-hexanetriol in levitated viscous aerosol particles, J. Aerosol Sci.,
138, 105449, https://doi.org/10.1016/j.jaerosci.2019.105449, 2019.
Ma, S. S., Yang, W., Zheng, C. M., Pang, S. F., and Zhang, Y. H.: Subsecond
measurements on aerosols: From hygroscopic growth factors to efflorescence
kinetics, Atmos. Environ., 210, 177–185,
https://doi.org/10.1016/j.atmosenv.2019.04.049, 2019.
Ma, S. S., Chen, Z., Pang, S. F., and Zhang, Y. H.: Data of “Observations on
hygroscopic growth and phase transitions of 1, 2,
6-hexanetriol/(NH4)2SO4 mixed particles: Investigation of
liquid-liquid phase separation (LLPS) dynamic process and mechanism and
secondary LLPS during the dehumidification”, Zenodo [Dataset], https://doi.org/10.5281/zenodo.4863581, 2021.
Marcolli, C., Luo, B. P., Peter, T., and Wienhold, F. G.: Internal mixing of
the organic aerosol by gas phase diffusion of semivolatile organic
compounds, Atmos. Chem. Phys., 4, 2593–2599,
https://doi.org/10.5194/acp-4-2593-2004, 2004.
Marcolli, C. and Krieger, U. K.: Phase changes during hygroscopic cycles of
mixed organic/inorganic model systems of tropospheric aerosols, J. Phys.
Chem. A, 110, 1881–1893, https://doi.org/10.1021/jp0556759, 2006.
Martin, S. T.: Phase transitions of aqueous atmospheric particles, Chem.
Rev., 100, 3403–3453, https://doi.org/10.1021/cr990034t, 2000.
Martin, S. T., Hung, H. M., Park, R. J., Jacob, D. J., Spurr, R. J. D.,
Chance, K. V., and Chin, M.: Effects of the physical state of tropospheric
ammonium-sulfate-nitrate particles on global aerosol direct radiative
forcing, Atmos. Chem. Phys., 4, 183–214,
https://doi.org/10.5194/acp-4-183-2004, 2004.
McNeill, V. F., Patterson, J., Wolfe, G. M., and Thornton, J. A.: The effect
of varying levels of surfactant on the reactive uptake of N2O5 to
aqueous aerosol, Atmos. Chem. Phys., 6, 1635–1644,
https://doi.org/10.5194/acp-6-1635-2006, 2006.
McNeill, V. F., Wolfe, G. M., and Thornton, J. A.: The oxidation of oleate
in submicron aqueous salt aerosols: Evidence of a surface process, J. Phys.
Chem. A, 111, 1073–1083, https://doi.org/10.1021/jp066233f, 2007.
Middlebrook, A. M., Murphy, D. M., and Thomson, D. S.: Observations of
organic material in individual marine particles at Cape Grim during the
First Aerosol Characterization Experiment (ACE 1), J. Geophys. Res.-Atmos.,
103, 16475, https://doi.org/10.1029/97JD03719, 1998.
Murphy, D. M., Cziczo, D. J., Froyd, K. D., Hudson, P. K., Matthew, B. M.,
Middlebrook, A. M., Peltier, R. E., Sullivan, A., Thomson, D. S., and Weber,
R. J.: Single-particle mass spectrometry of tropospheric aerosol particles,
J. Geophys. Res.-Atmos., 111, D23S32, https://doi.org/10.1029/2006JD007340, 2006.
Ng, N. L., Canagaratna, M. R., Zhang, Q., Jimenez, J. L., Tian, J., Ulbrich,
I. M., Kroll, J. H., Docherty, K. S., Chhabra, P. S., and Bahreini, R.:
Organic aerosol components observed in Northern Hemispheric datasets from
Aerosol Mass Spectrometry, Atmos. Chem. Phys., 10, 4625–4641,
https://doi.org/10.5194/acp-10-4625-2010, 2010.
O'Brien, R. E., Wang, B. B., Kelly, S. T., Lundt, N., You, Y., Bertram, A.
K., Leone, S. R., Laskin, A., and Gilles, M. K.: Liquid-liquid phase
separation in aerosol particles: Imaging at the nanometer scale, Environ.
Sci. Technol., 49, 4995–5002, https://doi.org/10.1021/acs.est.5b00062, 2015.
Pant, A., Fok, A., Parsons, M. T., Mak, J., and Bertram, A. K.:
Deliquescence and crystallization of ammonium sulfate-glutaric acid and
sodium chloride-glutaric acid particles, Geophys. Res. Lett., 31, L12111,
https://doi.org/10.1029/2004gl020025, 2004.
Papon, P., Leblond, J., and Meijer, P. H. E.: The Physics of phase
transitions: Concepts and applications, Springer, Berlin, 1999.
Qiu, Y. Q. and Molinero, V.: Morphology of liquid-liquid phase separated
aerosols, J. Am. Chem. Soc., 137, 10642–10651,
https://doi.org/10.1021/jacs.5b05579, 2015.
Renbaum-Wolff, L., Song, M., Marcolli, C., Zhang, Y., Liu, P. F., Grayson,
J. W., Geiger, F. M., Martin, S. T., and Bertram, A. K.: Observations and
implications of liquid–liquid phase separation at high relative humidities
in secondary organic material produced by α-pinene ozonolysis
without inorganic salts, Atmos. Chem. Phys., 16, 7969–7979,
https://doi.org/10.5194/acp-16-7969-2016, 2016.
Robinson, C. B., Schill, G. P., Zarzana, K. J., and Tolbert, M. A.: Impact
of organic coating on optical growth of ammonium sulfate particles, Environ.
Sci. Technol., 47, 13339–13346, https://doi.org/10.1021/es4023128, 2013.
Russell, L. M. and Ming, Y.: Deliquescence of small particles, J. Chem.
Phys., 116, 311–321, https://doi.org/10.1063/1.1420727, 2002.
Shelby, J. E.: Introduction to glass science and technology, The Royal
Society of Chemistry, Cambridge, UK, 1997.
Shiraiwa, M., Zuend, A., Bertram, A. K., and Seinfeld, J. H.: Gas-particle
partitioning of atmospheric aerosols: interplay of physical state, non-ideal
mixing and morphology, Phys. Chem. Chem. Phys., 15, 11441–11453,
https://doi.org/10.1039/c3cp51595h, 2013.
Sjogren, S., Gysel, M., Weingartner, E., Baltensperger, U., Cubison, M. J.,
Coe, H., Zardini, A. A., Marcolli, C., Krieger, U. K., and Peter, T.:
Hygroscopic growth and water uptake kinetics of two-phase aerosol particles
consisting of ammonium sulfate, adipic and humic acid mixtures, J. Aerosol
Sci., 38, 157–171, https://doi.org/10.1016/j.jaerosci.2006.11.005, 2007.
Song, M., Marcolli, C., Krieger, U. K., Zuend, A., and Peter, T.:
Liquid-liquid phase separation in aerosol particles: Dependence on O:C,
organic functionalities, and compositional complexity, Geophys. Res. Lett.,
39, L19801, https://doi.org/10.1029/2012gl052807, 2012a.
Song, M., Marcolli, C., Krieger, U. K., Zuend, A., and Peter, T.:
Liquid-liquid phase separation and morphology of internally mixed
dicarboxylic acids/ammonium sulfate/water particles, Atmos. Chem. Phys., 12,
2691–2712, https://doi.org/10.5194/acp-12-2691-2012, 2012b.
Song, M., Liu, P. F., Martin, S. T., and Bertram, A. K.: Liquid–liquid
phase separation in particles containing secondary organic material free of
inorganic salts, Atmos. Chem. Phys., 17, 11261–11271,
https://doi.org/10.5194/acp-17-11261-2017, 2017.
Thornton, J. A. and Abbatt, J. P. D.: N2O5 reaction on submicron
sea salt aerosol: kinetics, products, and the effect of surface active
organics, J. Phys. Chem. A, 109, 10004–10012,
https://doi.org/10.1021/jp054183t, 2005.
Wang, F., Zhang, Y. H., Li, S. H., Wang L.Y., and Zhao, L. J.: A strategy
for single supersaturated droplet analysis: Confocal Raman investigations on
the complicated hygroscopic properties of individual MgSO4 droplets on
the quartz substrate, Anal. Chem., 77, 7148–7155,
https://doi.org/10.1021/ac050938g, 2005.
Wang, X. W., Jing, B., Tan, F., Ma, J. B., Zhang, Y. H., and Ge, M. F.:
Hygroscopic behavior and chemical composition evolution of internally mixed
aerosols composed of oxalic acid and ammonium sulfate, Atmos. Chem. Phys.,
17, 12797–12812, https://doi.org/10.5194/acp-17-12797-2017, 2017.
Yu, H., Kaufman, Y. J., Chin, M., Feingold, G., Remer, L. A., Anderson, T.
L., Balkanski, Y., Bellouin, N., Boucher, O., and Christopher, S.: A review
of measurement-based assessments of the aerosol direct radiative effect and
forcing, Atmos. Chem. Phys., 6, 613–666,
https://doi.org/10.5194/acp-6-613-2006, 2005.
Zhang, Q., Jimenez, J. L., Canagaratna, M. R., Allan, J. D., Coe, H.,
Ulbrich, I., Alfarra, M. R., Takami, A., Middlebrook, A. M., Sun, Y. L.,
Dzepina, K., Dunlea, E., Docherty, K., DeCarlo, P. F., Salcedo, D., Onasch,
T., Jayne, J. T., Miyoshi, T., Shimono, A., Hatakeyama, S., Takegawa, N.,
Kondo, Y., Schneider, J., Drewnick, F., Borrmann, S., Weimer, S., Demerjian,
K., Williams, P., Bower, K., Bahreini, R., Cottrell, L., Griffin, R. J.,
Rautiainen, J., Sun, J. Y., Zhang, Y. M., and Worsnop, D. R.: Ubiquity and
dominance of oxygenated species in organic aerosols in
anthropogenically-influenced Northern Hemisphere midlatitudes, Geophys. Res.
Lett., 34, L13801, https://doi.org/10.1029/2007gl029979, 2007.
Zhou, Q., Pang, S. F., Wang, Y., Ma, J. B., and Zhang, Y. H.: Confocal raman
studies of the evolution of the physical state of mixed phthalic
acid/ammonium sulfate aerosol droplets and the effect of substrates, J.
Phys. Chem. B, 118, 6198–6205, https://doi.org/10.1021/jp5004598, 2014.
Zuend, A. and Seinfeld, J. H.: Modeling the gas-particle partitioning of
secondary organic aerosol: the importance of liquid-liquid phase separation,
Atmos. Chem. Phys., 12, 3857–3882, https://doi.org/10.5194/acp-12-3857-2012,
2012.
Zuend, A., Marcolli, C., Peter, T., and Seinfeld, J. H.: Computation of
liquid-liquid equilibria and phase stabilities: implications for
RH-dependent gas/particle partitioning of organic-inorganic aerosols, Atmos.
Chem. Phys., 10, 7795–7820, https://doi.org/10.5194/acp-10-7795-2010, 2010.
Short summary
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.
LLPS, efflorescence and deliquescence of aerosol particles can be observed visually and...
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