Remote sensing of atmospheric aerosols is of great importance to public and environmental health. This research promotes a simple way of detecting an aerosol cloud using a passive Open Path FTIR (OP-FTIR) system, without utilizing radiative transfer models and without relying on an artificial light source. Meteorological measurements (temperature, relative humidity and solar irradiance), and chemometric methods (multiple linear regression and artificial neural networks) together with previous cloud-free OP-FTIR measurements were used to estimate the ambient spectrum in real time. The cloud detection process included a statistical comparison between the estimated cloud-free signal and the measured OP-FTIR signal. During the study we were able to successfully detect several aerosol clouds (water spray) in controlled conditions as well as during agricultural pesticide spraying in an orchard.