title: Analysis of laser-produced aerosols by inductively coupled plasma mass spectrometry: transport phenomena and elemental fractionation.
abstract: The transport phenomena of laser-produced aerosols prior to analysis by inductively coupled plasma mass spectrometry (ICPMS) were examined. Aerosol particles were visualized over the cross section of a transport tube attached to the outlet of a conventional ablation cell by light scattering using a pulsed laser source. Experiments were carried out under laminar or turbulent in-cell flow conditions applying throughputs of up to 2.0 L/min and reveal the nature of aerosol transportation to strongly depend on both flow rate and carrier gas chosen. For instance, laser ablation (LA) using laminar in-cell flow and helium as aerosol carrier resulted in stationary but inhomogeneous dispersion patterns. In addition, aerosols appear to be separated into two coexisting phases consisting of (i) dispersed particles that accumulate at the boundary layer of several vortex channel flows randomly arranged along the tube axis and (ii) larger fragments moving inside. The occurrence of these fragments was found to affect the accuracy of Si-, Zn-, and Cd-specific ICPMS analyses of aerosols released by LA of silicate glass (SRM NIST610). Accuracy drifts of more than 10% were observed for helium flow rates of >1 L/min, most probably, due to preferential evaporation and diffusion losses of volatile constituents inside the ICP. The utilization of turbulent in-cell flow made the vortex channels collapse and resulted in an almost complete aerosol homogenization. In contrast, LA using argon as aerosol carrier generally yielded a higher degree of dispersion, which was nearly independent of the flow conditions applied. To illustrate the differences among laminar and turbulent in-cell flow, furthermore, the velocity field inside the ablation cell was simulated by computational fluid dynamics.
authors.affiliation: Laboratory of Inorganic Chemistry, Swiss Federal Institute of Technology, Wolfgang-Pauli-Strasse 10, ETH Zürich, Zürich, Switzerland. koch@inorg.chem.ethz.ch
authors.forename: J
authors.initials: J
authors.lastname: Koch
authors.forename: M
authors.initials: M
authors.lastname: Wälle
authors.forename: R
authors.initials: R
authors.lastname: Dietiker
authors.forename: D
authors.initials: D
authors.lastname: Günther