ABSTRACT

Coherent optical techniques contrast with those based on incoherent pro­ cesses, such as laser-induced fluorescence or spontaneous Raman scattering, by emitting a signal in a laserlike beam of radiation. For combustion diag­ nostics this presents obvious advantages for efficient collection of the signal and discrimination against background noise from scattered light or lumi­ nescence from the target gas. However, coherent emission requires that the emitting species be excited in a phased array or that some process ensures phase coherence in the signal direction. This is usually achieved in practice by a nonlinear optical process that couples energy from incident laser fields to the signal via the medium response. In gas-phase media symmetry con­ siderations dictate that the third-order susceptibility x(3) is the lowest order that can be employed. Thus the induced nonlinear polarization will be described by a term of the form

P f K ~r) = «2> "3. <*>4)E/(ft>i, ‘^ )E /(ft>3, ~T) (3.1)

where Em(con, ~r) are complex field amplitudes. This polarization radiates the signal wave E(&>4) in the general process known as four-wave mixing. (For a detailed treatment of the background physics of nonlinear optics see the excellent text by Boyd [1].)

In this chapter we describe four different processes which belong to this general class of nonlinearity: (i) degenerate four-wave mixing (DFWM), (ii) laser-induced thermal grating spectroscopy (LITGS), (iii) coherent antiStokes Raman scattering (CARS), and (iv) polarization spectroscopy (PS). Figure 3.1 shows the basic interactions involved in these processes.