|
Read Full Article (file size: 2387130 bytes) Cited by
JOURNAL OF GEOPHYSICAL RESEARCH,
VOL. 113,
D12209,
doi:10.1029/2007JD009327,
2008
How biogenic terpenes govern the correlation between sulfuric acid concentrations and new particle formation
B. Bonn
Department of Physical Sciences, Helsinki University, Helsinki, Finland
M. Kulmala
Department of Physical Sciences, Helsinki University, Helsinki, Finland
I. Riipinen
Department of Physical Sciences, Helsinki University, Helsinki, Finland
S.-L. Sihto
Department of Physical Sciences, Helsinki University, Helsinki, Finland
T. M. Ruuskanen
Department of Physical Sciences, Helsinki University, Helsinki, Finland
Abstract
New particle formation has been observed to take place all around the world. However, because of the inability to determine
the chemical composition of the smallest clusters or particles, indirect tools such as the correlation between nucleation
rate and measured sulfuric acid concentrations have been used to infer the nucleation mechanism. In this study we describe
the observed correlation with gaseous sulfuric acid concentrations by interactions of sesquiterpene oxidation products with
sulfuric acid. Two formation pathways of nucleation initiating molecules are considered. The interaction of sulfuric acid
with organic sulfates, which are formed from stabilized Criegee intermediates (sCIs, formed from sesquiterpenes), can be used
to explain the observed squared relationship between particle formation rate and ambient sulfuric acid concentrations. The
corresponding linear dependence is explained with the participation of secondary ozonides, which are formed from sCIs and
aldehydes. Both pathways are negatively affected by increasing water vapor concentration as observed in recent studies. In
order to check the assumptions made we apply the derived nucleation coefficients to measurements of the BACCI/QUEST IV campaign
made during spring 2005 in Hyytiälä, Finland. A reasonable agreement between the measurement data and the predicted nucleation
rates is found, giving support for the presented nucleation description.
Received 28
August
2007;
accepted 2
April
2008;
published 25
June
2008.
Keywords: nucleation rate;
sulphuric acid;
terpenes.
Index Terms: 0305 Atmospheric Composition and Structure: Aerosols and particles (0345, 4801, 4906); 0315 Atmospheric Composition and Structure: Biosphere/atmosphere interactions (0426, 1610); 0317 Atmospheric Composition and Structure: Chemical kinetic and photochemical properties.
Read Full Article (file size: 2387130 bytes) Cited by
Citation: Bonn, B., M. Kulmala, I. Riipinen, S.-L. Sihto, and T. M. Ruuskanen
(2008),
How biogenic terpenes govern the correlation between sulfuric acid concentrations and new particle formation,
J. Geophys. Res.,
113,
D12209,
doi:10.1029/2007JD009327.
Copyright 2008 by the American Geophysical Union.
|