Forward-scattering degenerate four-wave mixing as a simple sub-attomole-sensitive nonlinear laser analytical spectrometric method.

Optical phase conjugation by "forward-scattering" degenerate four-wave mixing in an absorbing liquid analyte solution is reported as a sensitive and simple nonlinear laser spectroscopic method. Since only two input laser beams are used in this nonlinear four-wave mixing setup, it offers important advantages including ease of optical alignment, efficient use of input photon density, low laser power requirements, and high wave-mixing efficiency. In addition, since the phase-conjugate signal is a laser beam, optical signal detection is very efficient and the signal-to-noise is excellent. Important characteristics of this novel nonlinear laser technique, including signal dependence on analyte concentration, individual input beam power, and modulation frequencies, are examined. Excellent detection sensitivity, small detection volume, and convenient sample introduction promise many applications for this nonlinear laser spectroscopic method. Preliminary detection limits of 0.7 amol of eosin B and 45 amol of iodine inside a probe volume of 98 pL are reported using a forward-scattering degenerate four-wave mixing setup.