Recent scientific findings and legislations have clearly highlighted the need for comprehensive approaches and methods to evaluate natural dust contributions to an urban atmosphere. The evaluation of chemical compositions of airborne aerosols is of these methods that may employ several advanced analytical techniques and processes. In this paper, an episodic appearance of Saharan dust incursion over a megacity (Istanbul, Turkey) was investigated using size segregated particulate matter (PM) samples in fine and coarse fractions collected between February 27 and March 8, 2009. The Saharan impact was investigated using satellite observations, backward air trajectory statistics, and chemical analyses of the collected samples. In the chemical analyses, Fourier transform infrared coupled with attenuated total reflectance (ATR-FTIR) spectroscopic method was used to determine the functional groups, namely, alcohols, ammonium, aliphatic carbons, carbonyls, organonitrates, nitrate, silicate, silica, kaolinite, and calcium carbonate. Among all the measured functional groups, it was clearly seen that the intensities of IR peaks related to silicate, silica, kaolinite, and calcium carbonate were associated with the increased mass concentrations during the impact period. The observed IR peaks at 1,030 and 800 cm⁻¹for silicate ions in the samples can be used as an indicator of the large dust incursion into the atmosphere (e.g., Saharan dust episodes observed in Istanbul). This study showed that the ATR-FTIR spectroscopic method is a fast and convenient method to identify these peaks and the IR method in general is useful for identifying a large dust incursion into the atmosphere.