An investigation of the factors influencing the detection sensitivity of cavity enhanced Raman scattering for probing aqueous binary aerosol droplets.

Stimulated Raman scattering (SRS) from single aerosol droplets can be observed at extremely low laser threshold intensities at wavelengths commensurate with whispering gallery modes. Although droplet size can routinely be determined from the ensuing cavity enhanced Raman scattering (CERS) fingerprint, determining droplet composition is a considerably more challenging measurement. We present here an examination of the factors that influence and limit the detection sensitivity of CERS in quantifying the concentrations of sulfate and nitrate in water droplets, 20-50 microm in radius. In particular, we consider the variation in nitrate and sulfate SRS signal with variation in species concentration, probe laser intensity and droplet size. We illustrate that the band contour of the OH stretching band can be used as a relative measure of the internal light intensity circulating within the droplet and experimentally investigate how the threshold condition for SRS is achieved.

Heterogeneous atmospheric aerosol chemistry: laboratory studies of chemistry on water droplets.

Heterogeneous chemical reactions on aerosol particles play a pivotal role in atmospheric chemistry. In this review, the fundamental concepts underlying the chemical dynamics of liquid aerosol droplets are discussed, with particular emphasis on the properties of the aqueous-air interface and the reaction mechanisms of key chemical processes. Recent laboratory studies of heterogeneous chemistry on aqueous aerosol particles are reviewed, with techniques that probe the gas phase, liquid phase and the interface directly, discussed in turn.

Chemistry in the clouds: the role of aerosols in atmospheric chemistry.

Ever since the discovery of the ozone hole over the Antarctic and the recognition of the damaging effects of acid rain, the role of atmospheric aerosol particles in determining the chemical balance of the atmosphere has received much attention. Aerosol particles produced in combustion can also have a deleterious effect on human health. In this article we review the chemistry that can occur on aerosol particles, particularly on aqueous based aerosols in the troposphere. The sources, transformation and loss mechanisms of atmospheric aerosol will be discussed. In particular, we will focus on the role of chemical transformation on aerosol particles in promoting reactions that would otherwise be too slow in the homogeneous atmospheric gas phase. Heterogeneous reaction mechanisms of some key chemical reactions will be described. Recent observations of a high organic content of tropospheric aerosol particles will be described and a model of organic coated aerosols will be reviewed.