Open Access
Images reveal that atmospheric particles can undergo liquid-liquid phase separations
Allan K. Bertram,Yuan You,Lindsay Renbaum-Wolff,Marc Carreras-Sospedra,Naruki Hiranuma,M. L. Smith,Xiaolu Zhang,Rodney J. Weber,John E. Shilling,Donald Dabdub,Scot T. Martin +10 more
- Vol. 2012
TLDR
Using optical and fluorescence microscopy, images are presented that show the coexistence of two noncrystalline phases for real-world samples collected on multiple days in Atlanta, GA as well as for laboratory-generated samples under simulated atmospheric conditions that reveal that atmospheric particles can undergo liquid–liquid phase separations.Abstract:
A large fraction of submicron atmospheric aerosol particles contains both organic material and inorganic salts. As the relative humidity cycles in the atmosphere and the water content of the particles correspondingly changes, these mixed particles can undergo a range of phase transitions, possibly including liquid–liquid phase separation. If liquid–liquid phase separation occurs, the gas-particle partitioning of atmospheric semivolatile organic compounds, the scattering and absorption of solar radiation, and the reactive uptake of gas species on atmospheric particles may be affected, with important implications for climate predictions. The actual occurrence of liquid–liquid phase separation within individual atmospheric particles has been considered uncertain, in large part because of the absence of observations for real-world samples. Here, using optical and fluorescence microscopy, we present images that show the coexistence of two noncrystalline phases for real-world samples collected on multiple days in Atlanta, GA as well as for laboratory-generated samples under simulated atmospheric conditions. These results reveal that atmospheric particles can undergo liquid–liquid phase separations. To explore the implications of these findings, we carried out simulations of the Atlanta urban environment and found that liquid–liquid phase separation can result in increased concentrations of gas-phase NO3 and N2O5 due to decreased particle uptake of N2O5.read more
Citations
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Hygroscopicity of organic surrogate compounds from biomass burning and their effect on the efflorescence of ammonium sulfate in mixed aerosol particles
Ting Lei,Ting Lei,Andreas Zuend,Yafang Cheng,Yafang Cheng,Hang Su,Hang Su,Weigang Wang,Maofa Ge +8 more
TL;DR: In this article, the authors used a tandem differential mobility analyzer (HTDMA) to measure the hygroscopicity of mixed organic-inorganic aerosol particles in the presence of ammonium sulfate.
Journal ArticleDOI
Liquid-liquid phase separation reduces radiative absorption by aged black carbon aerosols
Jian Zhang,Yuanyuan Wang,Xiaomi Teng,Lei Liu,Yisheng Xu,Lihong Ren,Zongbo Shi,Yue Zhang,Jingkun Jiang,Dantong Liu,Min Hu,Longyi Shao,Jianmin Chen,Scot T. Martin,Xiaoye Zhang,Weijun Li +15 more
TL;DR: In this paper , the authors combine field observations, laboratory experiments, and transmission electron microscopy to demonstrate that liquid-liquid phase separation redistributes black carbon from inorganic particle cores to organic coatings under a wide range of relative humidity.
Journal ArticleDOI
Morphology and Viscosity Changes after Reactive Uptake of Isoprene Epoxydiols in Submicrometer Phase Separated Particles with Secondary Organic Aerosol Formed from Different Volatile Organic Compounds
Ziying Lei,Nicole E. Olson,Yue-Ning Zhang,Yuzhi Chen,Andrew T. Lambe,Jing Zhang,Natalie J. White,Joanna M. Atkin,Mark M. Banaszak Holl,Zhen‐Fa Zhang,Avram Gold,Jason D. Surratt,Andrew P. Ault +12 more
TL;DR: This paper showed that the viscosity and morphology of initially core-shell (inorganic-organic) particles changed substantially after acid-catalyzed reactive uptake of isoprene epoxydiols (IEPOX), and that differences were highly dependent on VOC precursor.
Sea salt aerosols as a reactive surface for inorganic and organic acidic gases in the arctic troposphere
TL;DR: In this paper, transmission electron microscopy with energy-dispersive X-ray spectrometry was used to analyze morphology, composition, size, and mixing state of individual sea salt aerosols at Ny-Alesund, Svalbard, in summertime.
Journal ArticleDOI
Not all types of secondary organic aerosol mix: two phases observed when mixing different secondary organic aerosol types
Fabian Mahrt,Long Peng,Julia Zaks,Yuanzhou Huang,Paul E. Ohno,Natalie R. Smith,Florence K. A. Gregson,Yiming Qin,Celia Faiola,Scot T. Martin,Sergey A. Nizkorodov,Markus Ammann,Allan K. Bertram +12 more
TL;DR: In this paper , the number of phases in internal mixtures of different secondary organic aerosol (SOA) types was found to depend on the difference in the average O/C ratio between the two SOA types.
References
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Journal ArticleDOI
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Jose L. Jimenez,Manjula R. Canagaratna,Neil M. Donahue,André S. H. Prévôt,Qi Zhang,Jesse H. Kroll,Peter F. DeCarlo,James Allan,Hugh Coe,Nga L. Ng,Allison C. Aiken,Kenneth S. Docherty,Ingrid M. Ulbrich,Andrew P. Grieshop,Allen L. Robinson,Jonathan Duplissy,Jared D. Smith,Kevin R. Wilson,V. A. Lanz,Christoph Hueglin,Yele Sun,Yele Sun,Jian Tian,Ari Laaksonen,Tomi Raatikainen,Tomi Raatikainen,J. Rautiainen,Petri Vaattovaara,Mikael Ehn,Markku Kulmala,Markku Kulmala,Jason Tomlinson,Don R. Collins,Michael J. Cubison,Edward J. Dunlea,J. A. Huffman,Timothy B. Onasch,M. R. Alfarra,Paul I. Williams,Keith Bower,Yutaka Kondo,Johannes Schneider,Frank Drewnick,Stephan Borrmann,S. Weimer,Kenneth L. Demerjian,D. Salcedo,L. Cottrell,Robert J. Griffin,Akinori Takami,Takao Miyoshi,Shiro Hatakeyama,Akio Shimono,J. Y. Sun,Y. M. Zhang,Katja Dzepina,Joel R. Kimmel,Donna Sueper,J. T. Jayne,Scott C. Herndon,A. Trimborn,Leah R. Williams,Ezra C. Wood,Ann M. Middlebrook,Charles E. Kolb,Urs Baltensperger,Douglas R. Worsnop +66 more
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Book
Chemistry of the Upper and Lower Atmosphere: Theory, Experiments, and Applications
TL;DR: A detailed overview of the chemistry of Polluted and Remote Atmospheres can be found in this paper, where the OZIPR model is used to simulate the formation of gases and particles in the Troposphere.
Journal ArticleDOI
Field-Deployable, High-Resolution, Time-of-Flight Aerosol Mass Spectrometer
Peter F. DeCarlo,Joel R. Kimmel,A. Trimborn,M. J. Northway,John T. Jayne,Allison C. Aiken,Marc Gonin,Katrin Fuhrer,Thomas Horvath,Kenneth S. Docherty,Doug Worsnop,Jose L. Jimenez +11 more
TL;DR: The development of a new high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) is reported, which allows the direct separation of most ions from inorganic and organic species at the same nominal m/z, and the quantification of several types of organic fragments.
Journal ArticleDOI
O/C and OM/OC Ratios of Primary, Secondary, and Ambient Organic Aerosols with High-Resolution Time-of-Flight Aerosol Mass Spectrometry
Allison C. Aiken,Peter F. DeCarlo,Jesse H. Kroll,Douglas R. Worsnop,J. Alex Huffman,Kenneth S. Docherty,Ingrid M. Ulbrich,Claudia Mohr,Joel R. Kimmel,Donna Sueper,Yele Sun,Qi Zhang,A. Trimborn,M. J. Northway,Paul J. Ziemann,Manjula R. Canagaratna,Timothy B. Onasch,M. Rami Alfarra,André S. H. Prévôt,Josef Dommen,Jonathan Duplissy,A. Metzger,Urs Baltensperger,Jose L. Jimenez +23 more
TL;DR: A recently developed method to rapidly quantify the elemental composition of bulk organic aerosols (OA) using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) is improved and applied to ambient measurements.