Clustered and integrated fluorescence spectra from single atmospheric aerosol particles excited by a 263- and 351-nm laser at New Haven, CT, and Adelphi, MD

Fluorescence spectra from individual micron-sized atmospheric aerosol particles were measured by a Dual-wavelength-excitation Particle Fluorescence Spectrometer (DPFS). Particles were drawn into our laboratory at Adelphi, MD, an urban site in the Washington, DC, metroplex and within the Yale University campus at New Haven, CT. Two fluorescence spectra were obtained for every individual particle as it was moving through the DPFS system and excited sequentially by single laser pulses at 263 and 351 nm. There were around ten to a few hundred particles detected per second and up to a few million per day within the 1-10 μm particle size range. The majority of the particles have weak fluorescence, but 10-50% of the particles have fluorescence signals above the noise level at both sites at different time period. For the first time, these Ultra Violet laser-induced-fluorescence (UV-LIF) spectra from individual particles were integrated every 10 min, which forms a group of about a few thousand to a few tens of thousand particles, to provide the averaged background atmospheric fluorescence spectral profiles which may be helpful in the development of bioaerosol detection systems, particularly those systems based on integrated fluorescence from a group of aerosol particles, such as Light Detection And Rangeing (LIDAR) remotor biosensor and the point sensor based on collected particles on substrate. These integrated spectral profiles had small variations from time to time and were distinguishable from that of the bacterial simulant B. subtilis. Also for the first time, the individual spectra excited by a 351 nm laser were grouped using unstructured hierarchical cluster analysis, with parameters chosen so that spectra clustered into 8 main categories. They showed less spectral variations than that excited by a 263-nm laser. Over 98% of the spectra were able to be grouped into 8 clusters, and over 90% of the fluorescent particles were in clusters 3-5 with a fluorescence emission peak around 420-470 nm; these were mostly from biological and organic carbon-containing compounds. Integrated fluorescence spectral profiles and averaged spectra for each cluster show high similarity between New Haven, CT and Adelphi, MD.

► Fluorescence spectra from atmospheric aerosol particles excited by 263 nm and 351 nm laser pulses. ► Time integrated fluorescence spectra from individual micron-sized atmospheric aerosol particles. ► Unstructured hierarchical cluster analysis of single atmospheric particle fluorescence spectra. ► Spectra by 351 nm excitation show less variation than that by 263 nm excitation. ► Integrated fluorescence spectral profiles show similarity in New Haven, CT and Adelphi, MD.