To date, there has been much research into the size distribution of ambient atmospheric aerosols, particularly either the total aerosol population or water-soluble ionic species such as sulfate or nitrate. Meanwhile, there have been virtually no size-resolved measurements of water-insoluble aerosols (WIA). This has been due to a lack of practical measurement technology rather than a reflection of the importance of WIA to climate and health. Particle solubility influences the planetary radiation balance both directly and indirectly: solubility influences both the amount of hygroscopic growth (and thus light scattering) that occurs as a function of relative humidity and the ability of particles to serve as cloud condensation nuclei (and thus the lifetime and albedo of clouds). Also, recent information suggests that WIA may be harmful to human health. To address these concerns, a new real-time technique has been developed to measure the size-resolved concentration of WIA. This technique involves the entrainment of particles into a liquid stream and measurement of the WIA size distribution using a liquid optical particle counter. The time resolution of this instrumentation is approximately 4 min (depending on flow rate) and is capable of sizing and counting insoluble particles with diameters of 0.25-2.0 microm at atmospheric concentrations as low as 0.1 cm(-3). Laboratory characterization using polystyrene latex spheres shows agreement within +/-5% of the liquid stream and air stream particle concentrations when adjusted for flow rate. The instrumentation was field-tested at a rural site on the edge of the metro-Atlanta urban area. During this test, the WIA concentration averaged 5% of the total particle concentration between 0.25 and 2.0 microm but reached as high as 35%.