Spontaneous and nonphotochemical laser-induced nucleation in levitated supersaturated microdroplets

Research of nucleation in levitated supersaturated microdroplets was conducted in this dissertation. An unconventional crystallization system, levitated microdroplets, was utilized in this research. The microdroplet was levitated by an electrodynamic balance (EDB) constructed inside a vacuum chamber. EDB has the advantage of creating a containerless environment for the crystallization system. Spontaneous nucleation in levitated microdroplets was investigated. Spontaneous nucleation of aqueous microdroplets was caused by reducing the ambient relative humidity (RH) surrounding the solution droplets. Different polymorphs of glutaric acid and malonic acid are nucleated in levitated microdroplets when injected into a chamber maintained at different initial RH values. Effect of surfactant as additive is also investigated. A site-dependent evaporation-driven crystallization theory is established to explain the spontaneous nucleation phenomena in levitated aqueous microdroplets. Levitated microdroplets containing a solute and an organic solvent were also investigated. The crystallization behavior of glutaric acid methanol solutions and ethanol solutions was observed. ROY, a deca-polymorphic compound, was also studied from its DMSO solution microdroplets. Non-photochemical laser induced nucleation (NPLIN) was observed in levitated microdroplets of supersaturated potassium chloride (KCl) aqueous solution. A focused green (532 nm) pulsed laser with 1 ns pulse width was used to induce nucleation. Nucleation of levitated KCl microdroplet with high supersaturation was observed upon laser irradiation. A laser-induced charge loss phenomenon was also observed. A hypothesis of laser-induced electrostriction and corona discharge is discussed. Analysis with classical nucleation theory suggests that the NPLIN results in levitated microdroplets are consistent with previously published data on bulk samples.