A new fluorescence-based methodology for studying bioaerosol scavenging processes using a hyperspectral LIF-LIDAR...

This paper presents a novel experimental approach to in-situ study of atmospheric phenomena such as nucleation scavenging by biological seeds, bio-droplet dehydration, and bioaerosol's particle scavenging by raindrops. Our methodology is based on the analysis of the dynamical changes of fluorescence signal. We use a remote sensing system based on a homebuilt hyperspectral laser induced fluorescence (LIF) Lidar to measure the transient back-fluorescence and backscattering signals. The spectral line shape of the transient fluorescence associated with an aerosolized tryptophan solution was first analyzed in the laboratory. It then used to study bioaerosol phase transitions between wet and dry conditions. The experiments were first conducted in a dynamic aerosol cell where we repetitively create and monitor the droplets containing bioaerosol cloud starting from its early formation till its total evaporation. The LIF-Lidar was used to simultaneously measure back-fluorescence, scattering and transmission. These measurements were synchronized with the generation of droplets containing bioaerosol and with the monitoring of aerosol's size distribution and ambient conditions. A novel optical receiver design was used to simultaneously detect both back-fluorescence polarization components. Results showed that along with droplet's evaporation process, bioaerosol's fluorescence spectrum exhibit a blue shift, known as the dynamic Stokes-shifts, of ∼2000 cm^-1 and an increase in its fluorescence anisotropy. To the best of our knowledge, this is the first report of fluorescence Stokes-shifts and anisotropy within microdroplets containing a biological solution due to wet-dry phase transitions. This method was also used to quantify scavenging of biological particle by raindrops from 100 m. It shows that valuable information can be derived from analyzing the fluorescence spectrum of bioaerosol within a cloud and demonstrate the potential of a LIF-LIDAR remote system to perform in-situ studies of scavenging processes.