Localization and Orientation of Dye Molecules at the Surface of a Levitated Microdroplet in Air Revealed by Whispering Gallery Mode Resonances

Microdroplets offer unique environments that accelerate chemical reactions; however, the mechanisms behind these processes remain debated. The localization and orientation of solute molecules near the droplet surface have been proposed as factors for this acceleration. Since significant reaction acceleration has been observed for electrospray- and sonic-spray-generated aerosol droplets, the analysis of microdroplets in air has become essential. Here, we utilized whispering gallery mode (WGM) resonances to investigate the localization and orientation of dissolved rhodamine B (RhB) in a levitated microdroplet (∼3 μm in diameter) in air. Fluorescence enhancement upon resonance with the WGMs revealed the localization and orientation of RhB near the droplet surface. Numerical modeling using Mie theory quantified the RhB orientation at 68° to the surface normal, with a small fraction randomly oriented inside the droplet. Additionally, low RhB concentrations increased surface localization. These results support the significance of surface reactions in the acceleration of microdroplet reactions.