From a gaseous mixture of butyl azide (BAz) and acrolein, sedimentary aerosol particles were produced under irradiation with N2 laser light, in addition to a film which deposited all over the side wall of the irradiation cell. The yield of the sedimentary aerosol particles, the main chemical component of which was polyacrolein, increased with increasing laser intensity and with increasing the partial pressure of BAz, indicating that BAz increased the efficiency of aerosol particle formation, although its light absorptivity at 337.1 nm is very small. To elucidate the nucleation process of the aerosol particles, monitor (He-Ne laser) light intensity scattered by the aerosol particles as formed from the gaseous mixture was measured under irradiation with N2 laser light. Characteristic behavior of the scattered light intensity indicated that nucleation proceeded only through the photochemical reaction of BAz at low laser intensity (1.5 mJ/pulse), but at higher laser intensity (z 1.9 mJ/pulse) nucleation due to photochemical reaction of acrolein followed the nucleation through photochemical reaction of BAz.