Oxidation products of biogenic emissions contribute to nucleation of atmospheric particles.
Atmospheric new-particle formation affects climate and is one of the least understood atmospheric aerosol processes. The complexity and variability of the atmosphere has hindered elucidation of the fundamental mechanism of new-particle formation from gaseous precursors. We show, in experiments performed with the CLOUD (Cosmics Leaving Outdoor Droplets) chamber at CERN, that sulfuric acid and oxidized organic vapors at atmospheric concentrations reproduce particle nucleation rates observed in the lower atmosphere. The experiments reveal a nucleation mechanism involving the formation of clusters containing sulfuric acid and oxidized organic molecules from the very first step. Inclusion of this mechanism in a global aerosol model yields a photochemically and biologically driven seasonal cycle of particle concentrations in the continental boundary layer, in good agreement with observations.
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, Switzerland.
Francesco
F
Riccobono
Department of Physics, University of Helsinki, Helsinki, Finland.
Siegfried
S
Schobesberger
School of Earth and Environment, University of Leeds, Leeds, UK.
Catherine E
CE
Scott
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, Switzerland.
Josef
J
Dommen
Department of Physics, University of Helsinki, Helsinki, Finland.
Ismael K
IK
Ortega
Institute for Atmospheric and Environmental Sciences, Goethe University of Frankfurt, Frankfurt am Main, Germany.
Linda
L
Rondo
Institute for Atmospheric and Environmental Sciences, Goethe University of Frankfurt, Frankfurt am Main, Germany.
João
J
Almeida
Laboratory for Systems, Instrumentation, and Modeling in Science and Technology for Space and the Environment (SIM), University of Lisbon and University of Beira Interior, Lisbon, Portugal.
Antonio
A
Amorim
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, Switzerland.
Federico
F
Bianchi
Ionicon Analytik GmbH and University of Innsbruck, Institute for Ion and Applied Physics, Innsbruck, Austria.
Martin
M
Breitenlechner
CERN (European Organization for Nuclear Research), Geneva, Switzerland.
André
A
David
Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA 91125, USA.
Andrew
A
Downard
School of Earth and Environment, University of Leeds, Leeds, UK.
Eimear M
EM
Dunne
Department of Physics, University of Helsinki, Helsinki, Finland. Helsinki Institute of Physics, University of Helsinki, Helsinki, Finland.
Jonathan
J
Duplissy
Institute for Atmospheric and Environmental Sciences, Goethe University of Frankfurt, Frankfurt am Main, Germany.
Sebastian
S
Ehrhart
Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA 91125, USA.
Richard C
RC
Flagan
Department of Physics, University of Helsinki, Helsinki, Finland.
Alessandro
A
Franchin
Ionicon Analytik GmbH and University of Innsbruck, Institute for Ion and Applied Physics, Innsbruck, Austria.
Armin
A
Hansel
Department of Physics, University of Helsinki, Helsinki, Finland.
Heikki
H
Junninen
Department of Physics, University of Helsinki, Helsinki, Finland.
Maija
M
Kajos
University of Eastern Finland, Kuopio, Finland.
Helmi
H
Keskinen
Faculty of Physics, University of Vienna, Vienna, Austria.
Agnieszka
A
Kupc
Institute for Atmospheric and Environmental Sciences, Goethe University of Frankfurt, Frankfurt am Main, Germany.
Andreas
A
Kürten
Solar and Cosmic Ray Research Laboratory, Lebedev Physical Institute, Moscow, Russia.
Alexander N
AN
Kvashin
University of Eastern Finland, Kuopio, Finland.
Ari
A
Laaksonen
Department of Physics, University of Helsinki, Helsinki, Finland.
Katrianne
K
Lehtipalo
Solar and Cosmic Ray Research Laboratory, Lebedev Physical Institute, Moscow, Russia.
Vladimir
V
Makhmutov
CERN (European Organization for Nuclear Research), Geneva, Switzerland.
Serge
S
Mathot
Department of Physics, University of Helsinki, Helsinki, Finland. Helsinki Institute of Physics, University of Helsinki, Helsinki, Finland.
Tuomo
T
Nieminen
CERN (European Organization for Nuclear Research), Geneva, Switzerland.
Antti
A
Onnela
Department of Physics, University of Helsinki, Helsinki, Finland.
Tuukka
T
Petäjä
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, Switzerland.
Arnaud P
AP
Praplan
Laboratory for Systems, Instrumentation, and Modeling in Science and Technology for Space and the Environment (SIM), University of Lisbon and University of Beira Interior, Lisbon, Portugal.
Filipe D
FD
Santos
Department of Physics, University of Helsinki, Helsinki, Finland.
Simon
S
Schallhart
Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA 91125, USA.
John H
JH
Seinfeld
Department of Physics, University of Helsinki, Helsinki, Finland. Helsinki Institute of Physics, University of Helsinki, Helsinki, Finland.
Mikko
M
Sipilä
School of Earth and Environment, University of Leeds, Leeds, UK.
Dominick V
DV
Spracklen
Solar and Cosmic Ray Research Laboratory, Lebedev Physical Institute, Moscow, Russia.
Yuri
Y
Stozhkov
Leibniz Institute for Tropospheric Research, Leipzig, Germany.
Frank
F
Stratmann
Laboratory for Systems, Instrumentation, and Modeling in Science and Technology for Space and the Environment (SIM), University of Lisbon and University of Beira Interior, Lisbon, Portugal.
Antonio
A
Tomé
Leibniz Institute for Tropospheric Research, Leipzig, Germany.
Georgios
G
Tsagkogeorgas
University of Eastern Finland, Kuopio, Finland.
Petri
P
Vaattovaara
Finnish Meteorological Institute, Helsinki, Finland.
Yrjö
Y
Viisanen
Faculty of Physics, University of Vienna, Vienna, Austria.
Aron
A
Vrtala
Faculty of Physics, University of Vienna, Vienna, Austria.
Paul E
PE
Wagner
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, Switzerland.
Ernest
E
Weingartner
Leibniz Institute for Tropospheric Research, Leipzig, Germany.
Heike
H
Wex
Institute for Atmospheric and Environmental Sciences, Goethe University of Frankfurt, Frankfurt am Main, Germany.
Daniela
D
Wimmer
School of Earth and Environment, University of Leeds, Leeds, UK.
Kenneth S
KS
Carslaw
Institute for Atmospheric and Environmental Sciences, Goethe University of Frankfurt, Frankfurt am Main, Germany.
Joachim
J
Curtius
Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA 15213, USA.
Neil M
NM
Donahue
Institute for Atmospheric and Environmental Sciences, Goethe University of Frankfurt, Frankfurt am Main, Germany. CERN (European Organization for Nuclear Research), Geneva, Switzerland.
Jasper
J
Kirkby
Department of Physics, University of Helsinki, Helsinki, Finland. Helsinki Institute of Physics, University of Helsinki, Helsinki, Finland.
Markku
M
Kulmala
Department of Physics, University of Helsinki, Helsinki, Finland. Aerodyne Research Incorporated, Billerica, MA 01821, USA.
Douglas R
DR
Worsnop
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, Switzerland. urs.baltensperger@psi.ch.
Urs
U
Baltensperger
D000336:Aerosols / Q000737:chemistry*; D001272:Atmosphere / Q000737:chemistry*; D057231:Climate Change; D003198:Computer Simulation; D008956:Models, Chemical; D009930:Organic Chemicals / Q000737:chemistry*; D010084:Oxidation-Reduction; D055668:Photochemical Processes; D012621:Seasons; D013464:Sulfuric Acids / Q000737:chemistry*; D014835:Volatilization
D000336:Aerosols; D009930:Organic Chemicals; D013464:Sulfuric Acids; C033158:sulfuric acid