General Approach to the Evolution of Singlet Nanoparticles from a Rapidly Quenched Point Source

Among the numerous point vapor sources, microsecond-pulsed spark ablation at atmospheric pressure is a versatile and environmentally friendly method for producing ultrapure inorganic nanoparticles ranging from singlets having sizes smaller than 1 nm to larger agglomerated structures. Due to its fast quenching and extremely high supersaturation, coagulational growth already begins at the atomic scale at room temperature. On the basis of this knowledge, we develop a simple semiempirical yet versatile model for predicting the size distribution of singlet particles as a function of the process conditions. The model assumes that a plume of a turbulent aerosol flow flares out from a concentrated point source, eventually reaching the walls of the confinement where a fraction of the particles is deposited. Despite the complexity of the entire process, the concentration and size evolution of particles can be adequately described by a first-order differential equation accounting for coagulation, turbulent dilution, and diffusional deposition to the walls. The model provides a simple and practical tool that can generally be used to design and control point vapor source reactors for the synthesis of singlets with tunable sizes starting from that of single atoms.