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Author(s)
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Stolzenburg, Dominik (Vienna U. ; Helsinki U.) ; Simon, Mario (Frankfurt U.) ; Ranjithkumar, Ananth (Leeds U.) ; Kürten, Andreas (Frankfurt U.) ; Lehtipalo, Katrianne (Helsinki U. ; Finnish Meteorological Inst.) ; Gordon, Hamish (Leeds U.) ; Ehrhart, Sebastian (Mainz, Max Planck Inst.) ; Finkenzeller, Henning (U. Colorado, Boulder) ; Pichelstorfer, Lukas (Helsinki U.) ; Nieminen, Tuomo (Helsinki U.) ; He, Xu-Cheng (Helsinki U.) ; Brilke, Sophia (Vienna U.) ; Xiao, Mao (PSI, Villigen) ; Amorim, António (Lisbon U.) ; Baalbaki, Rima (Helsinki U.) ; Baccarini, Andrea (PSI, Villigen) ; Beck, Lisa (Helsinki U.) ; Bräkling, Steffen (Unlisted, CH) ; Caudillo Murillo, Lucía (Frankfurt U.) ; Chen, Dexian (Carnegie Mellon U.) ; Chu, Biwu (Helsinki U.) ; Dada, Lubna (Helsinki U.) ; Dias, António (Lisbon U.) ; Dommen, Josef (PSI, Villigen) ; Duplissy, Jonathan (Helsinki U.) ; El Haddad, Imad (PSI, Villigen) ; Fischer, Lukas (Innsbruck U.) ; Gonzalez Carracedo, Loic (Vienna U.) ; Heinritzi, Martin (Frankfurt U.) ; Kim, Changhyuk (Caltech ; Pusan Natl. U.) ; Koenig, Theodore K (U. Colorado, Boulder) ; Kong, Weimeng (Caltech) ; Lamkaddam, Houssni (PSI, Villigen) ; Lee, Chuan Ping (PSI, Villigen) ; Leiminger, Markus (Innsbruck U.) ; Li, Zijun (UEF, Kuopio) ; Makhmutov, Vladimir (Lebedev Inst.) ; Manninen, Hanna E (CERN) ; Marie, Guillaume (Frankfurt U.) ; Marten, Ruby (PSI, Villigen) ; Müller, Tatjana (Frankfurt U.) ; Nie, Wei (Nanjing U.) ; Partoll, Eva (Innsbruck U.) ; Petäjä, Tuukka (Helsinki U.) ; Pfeifer, Joschka (CERN) ; Philippov, Maxim (Lebedev Inst.) ; Rissanen, Matti P (Helsinki U. ; Tampere U. of Tech.) ; Rörup, Birte (Helsinki U.) ; Schobesberger, Siegfried (UEF, Kuopio) ; Schuchmann, Simone (CERN) ; Shen, Jiali (Helsinki U.) ; Sipilä, Mikko (Helsinki U.) ; Steiner, Gerhard (Innsbruck U.) ; Stozhkov, Yuri (Lebedev Inst.) ; Tauber, Christian (Vienna U.) ; Tham, Yee Jun (Helsinki U.) ; Tomé, António (Beira Interior U., Covilha) ; Vazquez-Pufleau, Miguel (Vienna U.) ; Wagner, Andrea C (Frankfurt U. ; U. Colorado, Boulder) ; Wang, Mingyi (Carnegie Mellon U.) ; Wang, Yonghong (Carnegie Mellon U.) ; Weber, Stefan K (CERN) ; Wimmer, Daniela (Vienna U. ; Helsinki U.) ; Wlasits, Peter J (Vienna U.) ; Wu, Yusheng (Helsinki U.) ; Ye, Qing (Carnegie Mellon U.) ; Zauner-Wieczorek, Marcel (Frankfurt U.) ; Baltensperger, Urs (PSI, Villigen) ; Carslaw, Kenneth S (Leeds U.) ; Curtius, Joachim (Frankfurt U.) ; Donahue, Neil M (Carnegie Mellon U.) ; Flagan, Richard C (Caltech) ; Hansel, Armin (Innsbruck U.) ; Kulmala, Markku (Helsinki U.) ; Lelieveld, Jos (Mainz, Max Planck Inst.) ; Volkamer, Rainer (U. Colorado, Boulder) ; Kirkby, Jasper (Frankfurt U. ; CERN) ; Winkler, Paul M (Vienna U.) |
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Abstract
| In the present-day atmosphere, sulfuric acid is the
most important vapour for aerosol particle formation and initial growth. However, the growth rates of nanoparticles ( <
10 nm) from sulfuric acid remain poorly measured. Therefore, the effect of stabilizing bases, the contribution of ions
and the impact of attractive forces on molecular collisions are
under debate. Here, we present precise growth rate measurements of uncharged sulfuric acid particles from 1.8 to 10 nm,
performed under atmospheric conditions in the CERN (European Organization for Nuclear Research) CLOUD chamber.
Our results show that the evaporation of sulfuric acid particles above 2 nm is negligible, and growth proceeds kinetically even at low ammonia concentrations. The experimental
growth rates exceed the hard-sphere kinetic limit for the condensation of sulfuric acid. We demonstrate that this results
from van der Waals forces between the vapour molecules and
particles and disentangle it from charge–dipole interactions.
The magnitude of the enhancement depends on the assumed
particle hydration and collision kinetics but is increasingly
important at smaller sizes, resulting in a steep rise in the observed growth rates with decreasing size. Including the experimental results in a global model, we find that the enhanced growth rate of sulfuric acid particles increases the
predicted particle number concentrations in the upper free
troposphere by more than 50 %. |