Mj. Kleeman et al., MODELING THE AIRBORNE PARTICLE COMPLEX AS A SOURCE-ORIENTED EXTERNAL MIXTURE, JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 102(D17), 1997, pp. 21355-21372
A Lagrangian air quality model is developed which represents the airbo
rne particle complex as a source-oriented external mixture. In a sourc
e-oriented external mixture, particles of the same size can evolve to
display different chemical compositions that depend on the chemical an
d hygroscopic properties of the primary seed particles initially emitt
ed from different sources. In contrast, previous models initialize the
airborne particles as an internal mixture in which all particles of t
he same size are assumed to have the same chemical composition. Test c
ases show that representation of the aerosol as an internal mixture ca
n distort the predicted particle composition and concentration in the
HNO3/NH3/HCl/H2SO4/aerosol Cl-/SO4=/NO3-/NH4+/Na+ system when Na+ and
SO4= exist in separate particles, as may occur when sea spray coexists
with long-distance transport of anthropogenic sulfates. Tests also in
dicate that the external mixture model can predict the evolution of a
nearly monodisperse aerosol into a bimodally distributed aerosol as re
lative humidity increases, qualitatively matching observations. The so
urce-oriented external mixture model is applied to predict the size an
d composition distribution of airborne particles observed at Claremont
, California, on August 28, 1987. Calculations produce an aerosol mass
distribution that is distinctly bimodal in the size range from 0.1 mu
m to 1.0 mu m particle diameter, matching field observations. Externa
l mixture calculations also predict specific differences in compositio
n between particles of the same diameter. The external mixture model i
s expected to have applications including exploration of the cause of
the particle-to-particle differences seen by time-of-flight mass spect
rometers that measure single exist in separate particles.