AbstractThe performance of a narrow‐angle and a wide‐angle, forward scattering laser aerosol spectrometer has been studied as a function of particle size and refractive index. The results have been compared with theoretical calculations based on light scattering theory. The results indicate that for the narrow‐angle instrument, the scattered‐light intensity is not a monotonic function of particle size for transparent particles (a monotonic relationship is required for unambiguous particle size measurement) above 0.7 μm. The instrument is therefore limited in its useful range to size distribution measurement between 0.2 μm – its lower particle size limit – and 0.7 μm for transparent particles. In the case of the wide‐angle instrument, the instrument output is a monotonic function of particle size for transparent particles, but the output is severely attenuated for light absorbing particles above 0.3 μm. The instrument, therefore, cannot be used for accurate size measurements above 0.3 μm for light a