Spatially resolved measurement of the distribution of solid and liquid Si nanoparticles in plasma synthesis through line-of-sight extinction spectroscopy.

Abstract

In many high-temperature gas-phase nanoparticle synthesis processes, freshly nucleated particles are liquid and solidify during growth and cooling. This study presents an approach to determine the location of the liquid-to-solid phase transition and the volume fraction and number density of particles of both phases within a gas phase reactor. Spectrally-resolved line-of-sight attenuation (LOSA) measurements are applied to a silicon nanoparticle aerosol generated from monosilane in a microwave plasma reactor. A phantom-based analysis using particle number density, particle size, and temperature distribution from direct numerical simulation (DNS) of the reacting flow indicates that the contributions from the two particle phases can be decoupled under practical conditions, even with noisy data. The approach was applied to analyze spatially and spectrally resolved LOSA measurements from the hot gas flow downstream of the plasma zone where both solid and liquid silicon particles coexist. Extinction spectra were recorded along a line perpendicular to the flow direction by a spectrometer with an electron-multiplying charge-coupled device (EMCCD) camera, and two-dimensional projections were deconvolved to obtain radial extinction coefficient distributions of solid and liquid particles across the cross-section of the flow. Particle number densities of both particle phases were retrieved simultaneously based on the size-dependent extinction cross-sections of the nanoparticles. The particle-size distribution was determined via thermophoretic sampling at the same location with subsequent transmission electron microscopy (TEM) analysis. The particle temperature distribution was determined from the particle's thermal radiation based on line-of-sight emission (LOSE) measurements. The approach for phase-selective data analysis can be transferred to other materials aerosol systems as long as significant differences exist in extinction spectra for the related different particle classes.