HR: 09:15h
AN: A41B-05 [PDF]
TI: The importance of the organic aerosol component for
the passivation of aqueous atmospheric particles
AU: * Kiendler-Scharr, A W
EM: a.kiendler-scharr@fz-juelich.de
AF: ICG-II: Troposph\"are, Forschungszentrum J\"ulich, J\"ulich, 52425
Germany
AU: Folkers, M
EM: m.folkers@fz-juelich.de
AF: ICG-II: Troposph\"are, Forschungszentrum J\"ulich, J\"ulich, 52425
Germany
AU: Mentel, T F
EM: t.mentel@fz-juelich.de
AF: ICG-II: Troposph\"are, Forschungszentrum J\"ulich, J\"ulich, 52425
Germany
AU: Wahner, A
EM: a.wahner@fz-juelich.de
AF: ICG-II: Troposph\"are, Forschungszentrum J\"ulich, J\"ulich, 52425
Germany
AB:
Secondary tropospheric particles are often mixtures of aqueous
electrolytes and soluble organic components or surfactants. The
uptake kinetics of e.g.~$\rm N_2O_5$ and the thermodynamics of
binary and higher mixtures of aqueous electrolytes are quite well
understood. In contrast, not much is known on a quantitative basis
about the modification of these properties by organic aerosol
components.
The hydrolysis of $\rm N_2O_5$ on aqueous aerosol surfaces of
mixed inorganic and organic aerosols was used to probe the surface
reactivity/water availability. The experiments were performed in
the large Aerosol Chamber at the FZ-J\"ulich at room temperature
and 60 - 70 % relative humidity.
The ozonolysis of $\alpha$-pinene, myrcene, limonene and isoprene
was utilized to condense organic components on $\rm NH_4HSO_4$
particles. The build up of the organic component was monitored by
Aerosol Mass Spectrometry (Aerodyne AMS). In the terpene
experiments the hydrolysis of $\rm N_2O_5$ on the particle surface
was diminished by factors of 2 to 30 compared to the pure
inorganic salt (reaction probability $\gamma_{N2O5}$ = 0.02). The
degree of passivation depends on the organic load and the specific
terpene. For purely organic particles from $\alpha$-pinene
ozonolysis, which are not hygroscopic, the reaction probabilty
$\gamma_{N2O5}$ is 0.00045.
In the isoprene experiment the main known ozonolysis products in
the particulate phase are water soluble $\alpha$-dicarbonyls.
Despite the low organic mass fraction of only 6% the hydrolysis
on this mixed organic/inorganic aerosol is significantly retarded
by a factor of 2 ( $\gamma_{N2O5}$ = 0.01). We were able to
identify mass fragments of methyl glyoxal and pyruvic acid in the
particles. Moreover, there is indication by the AMS that higher
molecular components are also present in the particles, possibly
formed in the particulate phase. Specific addition even of high
loads of the single component methyl glyoxal to $\rm (NH_4)_2SO_4$
particles did only show a smaller effect ($\gamma_{N2O5}$ = 0.014)
compared to the "real" and complex ozonolysis products of
isoprene.
Our findings demonstrate the importance of oxidized large biogenic
organics for passivation (reduced water availability at the
surface) of mixed particles. But also small molecules can
contribute to passivation if condensation reactions takes place
which form larger (ampholytic) molecules (M. Jang et al., Science,
298, 814-817, 2002)
The studies are part of the EC CASOMIO project.
DE: 0305 Aerosols and particles (0345, 4801)
DE: 0315 Biosphere/atmosphere interactions
DE: 0365 Troposphere--composition and chemistry
DE: 0394 Instruments and techniques
SC: Atmospheric Sciences [A]
MN: 2003 Fall Meeting