Radlatlon generated by stlmulated Raman scatterlng (SRS) in H, at llquld N, temperatures was evaluated as a tunable, sharpline, ultravblet lasef source for the excltath of atomlc fluorescence of those elements, such as As, Se, Te, and Zn, whose resonance excited states are usually more than 40 000 cm-' above the ground state. To populate these states requires primary radlatlon of wavelengths that are shorter than can be provided by laser-frequency doubHng techniques.These wavelengths are within the range that can be reached through stimulated Raman scattering of dye-laser primary radlatlon. In the stwlles described, a YAG pumped, dye-laser source provided the primary radlatlon that was scattered In the SRS cell Into Stokes and anti-Stokes components. Data on the analytkai flgures of merit are presented and compared with those obtalned by conventlonal Inductively coupled plasma atomlc emlsslon spectroscopy and hollow-cathode lamp excited atomlc fluorescence spectroscopy.I t is logical that the analytical potential of atomic fluorescence spectroscopy (AFS) systems based on the use of tunable, dye-laser excitation of free atoms in inductively coupled plasma (ICP) atomization cells should attract attention, which it has (1-9). An indicator of the progress made to date in laser-excited (LE) atomic fluorescence generated in ICP atomization cells can be developed by comparing reported powers of detection for LE-ICP-AFS with those observed in the conventional atomic emission mode (ICP-AES). Such a comparison leads to an obvious general conclusion, namely, that useful LE-AFS detection limits have not been reported for those elements, e.g., As, Sb, Se, and Zn, whose resonance excited states are more than 40 000 cm-' above the ground state. To populate these levels, exciting radiation at wavelengths less than 250 nm is required. Conventional laser-frequency doubling techniques have to date not been able to provide adequate radiant fluxes at these short wavelengths to produce analytically useful atomic fluorescence intensities. In addition, no wavelengths below 217 nm have been produced with conventional laser-frequency doubling techniques.Several attractive avenues of exploration remain for attaining analytically useful detection limits for the elements under consideration. Among these are the use of (a) pulsed Nd:YAG laser pumped, dye laser system combined with stimulated Raman scattering to produce and/or increase the radiant flux of exciting radiation at wavelengths less than 250 nm, and (b) ultrasonic generation of aerosol combined with aerosol desolvation to increase the analyte mass loading of the ICP atomization cell (10-12).Stimulated Raman Scattering (SRS). This process, which was first demonstrated by Woodbury and Ng (13) and Eckhardt et al. (14) in 1962, has the potential advantage of not only shifting sharply tuned, ultraviolet dye laser radiation to lower wavelengths but also being able to provide greater radiation fluxes at the shorter wavelengths (Le., less than 220 nm) than has been available by other me...