Heterodyne coincidence spectroscopy

A new type of light-scattering experiment, which should measure directly the triple static structure factor S ⁽³⁾ (k, q) of a fluid, is proposed. S ⁽³⁾(k, q) is the full spatial Fourier transform of the equilibrium triplet distribution function g ⁽³⁾(r ₁, r ₂, r ₃). The experiment may also be used to study dynamic correlation functions of the form <a_k (t)a_q (t′)a_k_q(t″)> (where a_k () is the kth spatial Fourier component of the density), thereby giving new information on mode-mode coupling. The method obtains its information from triple correlations in the arrival of scattered photons at three detectors. The detectors must be operated in the heterodyne mode (i.e. with a local oscillator); the scattering volume must be much larger than the volume over which molecular positions are correlated. Comparison is made with previous analyses of other multi-detector experiments.