Sample introduction to inductively coupled plasma atomic emission using thermospray nebulization is studied at a fundamental level. Optimum signals and signal-to-noise ratios result from thermospray operation at temperatures which coincide with highest analyte transport (>20%). High transport levels are maintained at sample flow rates of up to 3 mL/min. On the basis of comparison with analyte transport measurements for a pneumatic nebulizer (1.5%), signal increases are less than anticipated. Measurement of primary thermospray aerosols, using Fraunhofer diffraction, indicates that the enhanced transport results from decreased particle sizes for thermospray aerosols compared with pneumatic aerosols. Solvent is more rapidly vaporized from hot thermospray aerosols, further increasing the disparity in particle sizes. On the basis of aerosol particle size data, a conceptual model for aerosol generation, which is similar to pneumatic processes, is developed for thermospray. Trends for further improvements in thermospray aerosol production are predicted.
In order to develop a consistent nucleation theory, the main assumptions of the theory should be revised. One of the questionable problems is the role of the carrier gas in nucleation and the surface tension for the critical embryo as a function of cluster size. Using a flow diffusion chamber, the vapor nucleation rates were measured with high precision and phase transitions in critical embryos containing two and more dozen molecules were detected. Phase transitions in critical embryos were used as markers to detect that the new phase critical embryos contain two components. Phase transitions of the first order related with critical point second-order phase transitions in the pure CO2 carrier-gas were used as markers to demonstrate the presence of CO2 in critical embryos of condensate. Results of this research, in our opinion, very clearly demonstrate that vapor nucleation in a gaseous atmosphere is a binary process and must be interpreted from the point of view of nucleation theory within a binary system. “Supercritical” nucleation is a virtual term born by interpretation of binary vapor–gas nucleation by using the nucleation model of a single component. A critical condition for the binary system could be a higher level for the single component critical pressure and/or temperature, which can produce the illusion of supercritical nucleation. One component interpretation can be used far from the critical condition. On the other hand, the Laplace pressure practically always is able to approach the nucleation condition to the critical pressure. This level of detail is a problem for future studies. The traditional application of classical nucleation theory for vapor–gas nucleation should be modified to consider the nucleation conditions in pressure-temperature-composition space.
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