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Dual-pulse LIBS has been previously investigated to a large extent on solid and liquid phase analytes, where it has been demonstrated to significantly enhance atomic emission signal intensity, and more importantly, to enhance the analyte peak-to-base and signal-to-noise ratios. This study focuses on the effects of an orthogonal dual-pulse laser configuration on the atomic emission response for both purely gaseous and calcium-based aerosol samples. The gaseous sample consisted of purified (i.e. aerosol free) air, from which nitrogen and oxygen spectral emission lines were analyzed. Measurements for the gaseous system resulted in no notable improvements with the dual-pulse configuration as compared to the single-pulse LIBS. Experiments were also conducted in purified air seeded with calcium-rich particles, which revealed a marked improvement in calcium atomic emission peak-to-base (∼ 2-fold …