The role of low-volatility organic compounds in initial particle growth in the atmosphere
Jasmin Tröstl,Wayne Chuang,Hamish Gordon,Martin Heinritzi,Chao Yan,Ugo Molteni,Lars Ahlm,Carla Frege,F. Bianchi,F. Bianchi,F. Bianchi,Robert Wagner,Mario Simon,Katrianne Lehtipalo,Katrianne Lehtipalo,Christina Williamson,Christina Williamson,Christina Williamson,J. S. Craven,Jonathan Duplissy,Jonathan Duplissy,Alexey Adamov,Joao Almeida,Anne-Kathrin Bernhammer,Martin Breitenlechner,Sophia Brilke,Antonio Dias,Sebastian Ehrhart,Richard C. Flagan,Alessandro Franchin,Claudia Fuchs,Roberto Guida,Martin Gysel,Armin Hansel,Christopher R. Hoyle,Tuija Jokinen,Heikki Junninen,Juha Kangasluoma,Helmi Keskinen,Helmi Keskinen,Helmi Keskinen,Jaeseok Kim,Jaeseok Kim,Manuel Krapf,Andreas Kürten,Ari Laaksonen,Ari Laaksonen,Michael J. Lawler,Michael J. Lawler,Markus Leiminger,Serge Mathot,Ottmar Möhler,Tuomo Nieminen,Tuomo Nieminen,Antti Onnela,Tuukka Petäjä,Felix Piel,Pasi Miettinen,Matti P. Rissanen,Linda Rondo,Nina Sarnela,Siegfried Schobesberger,Siegfried Schobesberger,Kamalika Sengupta,Mikko Sipilä,James N. Smith,James N. Smith,Gerhard Steiner,Gerhard Steiner,Gerhard Steiner,António Tomé,Annele Virtanen,Andrea Christine Wagner,Ernest Weingartner,Ernest Weingartner,Daniela Wimmer,Daniela Wimmer,Paul M. Winkler,Penglin Ye,Kenneth S. Carslaw,Joachim Curtius,Josef Dommen,Jasper Kirkby,Jasper Kirkby,Markku Kulmala,Ilona Riipinen,Douglas R. Worsnop,Douglas R. Worsnop,Neil M. Donahue,Neil M. Donahue,Urs Baltensperger +90 more
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TLDR
It is shown that organic vapours alone can drive nucleation, and a particle growth model is presented that quantitatively reproduces the measurements and implements a parameterization of the first steps of growth in a global aerosol model that can change substantially in response to concentrations of atmospheric cloud concentration nuclei.Abstract:
About half of present-day cloud condensation nuclei originate from atmospheric nucleation, frequently appearing as a burst of new particles near midday. Atmospheric observations show that the growth rate of new particles often accelerates when the diameter of the particles is between one and ten nanometres. In this critical size range, new particles are most likely to be lost by coagulation with pre-existing particles, thereby failing to form new cloud condensation nuclei that are typically 50 to 100 nanometres across. Sulfuric acid vapour is often involved in nucleation but is too scarce to explain most subsequent growth, leaving organic vapours as the most plausible alternative, at least in the planetary boundary layer. Although recent studies predict that low-volatility organic vapours contribute during initial growth, direct evidence has been lacking. The accelerating growth may result from increased photolytic production of condensable organic species in the afternoon, and the presence of a possible Kelvin (curvature) effect, which inhibits organic vapour condensation on the smallest particles (the nano-Kohler theory), has so far remained ambiguous. Here we present experiments performed in a large chamber under atmospheric conditions that investigate the role of organic vapours in the initial growth of nucleated organic particles in the absence of inorganic acids and bases such as sulfuric acid or ammonia and amines, respectively. Using data from the same set of experiments, it has been shown that organic vapours alone can drive nucleation. We focus on the growth of nucleated particles and find that the organic vapours that drive initial growth have extremely low volatilities (saturation concentration less than 10(-4.5) micrograms per cubic metre). As the particles increase in size and the Kelvin barrier falls, subsequent growth is primarily due to more abundant organic vapours of slightly higher volatility (saturation concentrations of 10(-4.5) to 10(-0.5) micrograms per cubic metre). We present a particle growth model that quantitatively reproduces our measurements. Furthermore, we implement a parameterization of the first steps of growth in a global aerosol model and find that concentrations of atmospheric cloud concentration nuclei can change substantially in response, that is, by up to 50 per cent in comparison with previously assumed growth rate parameterizations.read more
Citations
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Journal ArticleDOI
Ion-induced nucleation of pure biogenic particles
Jasper Kirkby,Jasper Kirkby,Jonathan Duplissy,Jonathan Duplissy,Kamalika Sengupta,Carla Frege,Hamish Gordon,Christina Williamson,Christina Williamson,Martin Heinritzi,Martin Heinritzi,Mario Simon,Chao Yan,Joao Almeida,Joao Almeida,Jasmin Tröstl,Tuomo Nieminen,Tuomo Nieminen,Ismael K. Ortega,Robert Wagner,Alexey Adamov,António Amorim,Anne-Kathrin Bernhammer,F. Bianchi,F. Bianchi,Martin Breitenlechner,Sophia Brilke,Xuemeng Chen,J. S. Craven,Antonio Dias,Sebastian Ehrhart,Sebastian Ehrhart,Richard C. Flagan,Alessandro Franchin,Claudia Fuchs,Roberto Guida,Jani Hakala,Christopher R. Hoyle,Tuija Jokinen,Heikki Junninen,Juha Kangasluoma,Jaeseok Kim,Jaeseok Kim,Manuel Krapf,Andreas Kürten,Ari Laaksonen,Ari Laaksonen,Katrianne Lehtipalo,Katrianne Lehtipalo,Vladimir Makhmutov,Serge Mathot,Ugo Molteni,Antti Onnela,Otso Peräkylä,Felix Piel,Tuukka Petäjä,Arnaud P. Praplan,Kirsty J. Pringle,Alexandru Rap,N. A. D. Richards,Ilona Riipinen,Matti P. Rissanen,Linda Rondo,Nina Sarnela,Siegfried Schobesberger,Siegfried Schobesberger,Catherine E. Scott,John H. Seinfeld,Mikko Sipilä,Mikko Sipilä,Gerhard Steiner,Gerhard Steiner,Gerhard Steiner,Yuri Stozhkov,Frank Stratmann,António Tomé,Annele Virtanen,Alexander L. Vogel,Andrea Christine Wagner,Paul E. Wagner,Ernest Weingartner,Daniela Wimmer,Daniela Wimmer,Paul M. Winkler,Penglin Ye,Xuan Zhang,Armin Hansel,Josef Dommen,Neil M. Donahue,Douglas R. Worsnop,Douglas R. Worsnop,Urs Baltensperger,Markku Kulmala,Markku Kulmala,Kenneth S. Carslaw,Joachim Curtius +95 more
TL;DR: Ion-induced nucleation of pure organic particles constitutes a potentially widespread source of aerosol particles in terrestrial environments with low sulfuric acid pollution.
Journal ArticleDOI
Recent advances in understanding secondary organic aerosol: Implications for global climate forcing
Manish Shrivastava,Christopher D. Cappa,Jiwen Fan,Allen H. Goldstein,Alex Guenther,Jose L. Jimenez,Chongai Kuang,Alexander Laskin,Scot T. Martin,Nga L. Ng,Tuukka Petäjä,Jeffrey R. Pierce,Philip J. Rasch,Pontus Roldin,John H. Seinfeld,John E. Shilling,James N. Smith,Joel A. Thornton,Rainer Volkamer,Jian Wang,Douglas R. Worsnop,Rahul A. Zaveri,Alla Zelenyuk,Qi Zhang +23 more
TL;DR: In this paper, a review summarizes some of the important developments during the past decade in understanding secondary organic aerosol (SOA) formation, including formation of extremely low volatility organics in the gas phase, acid-catalyzed multiphase chemistry of isoprene epoxydiols, particle-phase oligomerization, and physical properties such as volatility and viscosity.
Journal ArticleDOI
Highly Oxygenated Organic Molecules (HOM) from Gas-Phase Autoxidation Involving Peroxy Radicals: A Key Contributor to Atmospheric Aerosol
F. Bianchi,Theo Kurtén,Matthieu Riva,Claudia Mohr,Matti P. Rissanen,Pontus Roldin,Torsten Berndt,John D. Crounse,Paul O. Wennberg,Thomas F. Mentel,Jürgen Wildt,Heikki Junninen,Heikki Junninen,Tuija Jokinen,Markku Kulmala,Douglas R. Worsnop,Joel A. Thornton,Neil M. Donahue,Henrik G. Kjaergaard,Mikael Ehn +19 more
TL;DR: This Review defines HOM and describes the currently available techniques for their identification/quantification, followed by a summary of the current knowledge on their formation mechanisms and physicochemical properties.
Journal ArticleDOI
Atmospheric new particle formation from sulfuric acid and amines in a Chinese megacity
Lei Yao,Olga Garmash,F. Bianchi,F. Bianchi,Jun Zheng,Chao Yan,Jenni Kontkanen,Jenni Kontkanen,Heikki Junninen,Stephany Buenrostro Mazon,Mikael Ehn,Pauli Paasonen,Mikko Sipilä,Mingyi Wang,Xinke Wang,Shan Xiao,Hangfei Chen,Yiqun Lu,Bowen Zhang,Dongfang Wang,Qingyan Fu,Fuhai Geng,Li Li,Hongli Wang,Liping Qiao,Xin Yang,Xin Yang,Jianmin Chen,Jianmin Chen,Veli-Matti Kerminen,Tuukka Petäjä,Douglas R. Worsnop,Markku Kulmala,Markku Kulmala,Lin Wang +34 more
TL;DR: Investigation of new particle formation in Shanghai found that the observed concentration of sulfuric acid was high enough to explain the particle growth to ~3 nanometers under the very high condensation sink, whereas the subsequent higher growth rate beyond this size is believed to result from the added contribution of condensing organic species.
Journal ArticleDOI
Aerosol Health Effects from Molecular to Global Scales
Manabu Shiraiwa,Kayo Ueda,Andrea Pozzer,Gerhard Lammel,Christopher J. Kampf,Akihiro Fushimi,Shinichi Enami,Andrea M. Arangio,Janine Fröhlich-Nowoisky,Yuji Fujitani,Akiko Furuyama,Pascale S. J. Lakey,Jos Lelieveld,Kurt Lucas,Yu Morino,Ulrich Pöschl,Satoshi Takahama,Akinori Takami,Haijie Tong,Bettina Weber,Ayako Yoshino,Kei Sato +21 more
TL;DR: The role of distinct PM components in health impacts and mortality needs to be clarified by integrated research on various spatiotemporal scales for better evaluation and mitigation of aerosol effects on public health in the Anthropocene.
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