TY  - JOUR
A1  - Tröstl, Jasmin
A1  - Chuang, Wayne K.
A1  - Gordon, Hamish
A1  - Heinritzi, Martin
A1  - Yan, Chao
A1  - Molteni, Ugo
A1  - Ahlm, Lars
A1  - Frege, Carla
A1  - Bianchi, Federico
A1  - Wagner, Robert
A1  - Simon, Mario
A1  - Lehtipalo, Katrianne
A1  - Williamson, Christina
A1  - Craven, Jill
A1  - Duplissy, Jonathan
A1  - Adamov, Alexey
A1  - Almeida, Joao
A1  - Bernhammer, Anne-Kathrin
A1  - Breitenlechner, Martin
A1  - Brilke, Sophia
A1  - Dias, Antonio
A1  - Ehrhart, Sebastian
A1  - Flagan, Richard C.
A1  - Franchin, Alessandro
A1  - Fuchs, Claudia
A1  - Guida, Roberto
A1  - Gysel, Martin
A1  - Hansel, Armin
A1  - Hoyle, Christopher Robert
A1  - Jokinen, Tuija
A1  - Junninen, Heikki
A1  - Kangasluoma, Juha
A1  - Keskinen, Helmi
A1  - Kim, Jaeseok
A1  - Krapf, Manuel
A1  - Kürten, Christoph Andreas
A1  - Laaksonen, Ari
A1  - Lawler, Michael Joseph
A1  - Leiminger, Markus
A1  - Mathot, Serge
A1  - Möhler, Ottmar
A1  - Nieminen, Tuomo
A1  - Onnela, Antti
A1  - Petäjä, Tuukka
A1  - Piel, Felix
A1  - Miettinen, Pasi
A1  - Rissanen, Matti P.
A1  - Rondo, Linda
A1  - Sarnela, Nina
A1  - Schobesberger, Siegfried
A1  - Sengupta, Kamalika
A1  - Sipilä, Mikko
A1  - Smith, James N.
A1  - Steiner, Gerhard
A1  - Tomé, Antonio
A1  - Virtanen, Annele
A1  - Wagner, Andrea Christine
A1  - Weingartner, Ernest
A1  - Wimmer, Daniela
A1  - Winkler, Paul M.
A1  - Ye, Penglin
A1  - Carslaw, Kenneth S.
A1  - Curtius, Joachim
A1  - Dommen, Josef
A1  - Kirkby, Jasper
A1  - Kulmala, Markku
A1  - Riipinen, Ilona
A1  - Worsnop, Douglas R.
A1  - Donahue, Neil McPherson
A1  - Baltensperger, Urs
T1  - The role of low-volatility organic compounds in initial particle growth in the atmosphere
T2  - Nature
N2  - About half of present-day cloud condensation nuclei originate from atmospheric nucleation, frequently appearing as a burst of new particles near midday1. Atmospheric observations show that the growth rate of new particles often accelerates when the diameter of the particles is between one and ten nanometres2,3. In this critical size range, new particles are most likely to be lost by coagulation with pre-existing particles4, 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 growth5,6, leaving organic vapours as the most plausible alternative, at least in the planetary boundary layer7,8,9,10. Although recent studies11,12,13 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 afternoon2, and the presence of a possible Kelvin (curvature) effect, which inhibits organic vapour condensation on the smallest particles (the nano-Köhler theory)2,14, 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 shown15 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.
KW  - Atmospheric chemistry
KW  - Thermodynamics
Y1  - 2016
UR  - http://publikationen.ub.uni-frankfurt.de/frontdoor/index/index/docId/50569
UR  - https://nbn-resolving.org/urn:nbn:de:hebis:30:3-505694
SN  - 1476-4687
SN  - 0028-0836
N1  - This work is licensed under a Creative Commons Attribution 4.0 International (CC BY 4.0) licence. The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons licence, users will need to obtain permission from the licence holder to reproduce the material. To view a copy of this licence, visit http://creativecommons.org/licenses/by/4.0/.
VL  - 533
IS  - 7604
SP  - 527
EP  - 531
PB  - Nature Publ. Group
CY  - London [u. a.]
ER  -