Theory of laser-induced amplitude and phase gratings including photoselection, orientational relaxation and population kinetics

Abstract

The generation of amplitude and phase gratings in an absorbing medium is discussed, including the effects of light polarization, population kinetics and orientational relaxation. A theory is given which describes light diffraction by a combination of an amplitude and a phase grating. It is shown that the coherent coupling effect in transient absorption measurements is solely due to the amplitude grating. Weak absorption and a low triplet yield favour diffraction of the probing beam by the phase grating in triple-beam experiments. Phase grating experiments can be performed with highly soluble absorber dyes, the absorption maximum of which is far away from the laser wavelength. Due to photoselection, diffraction by an amplitude grating depends on the polarization of the probing beam while phase grating diffraction is insensitive to this. Perpendicular polarization of the two exciting pulses prevents the buildup of a phase grating and results in light diffracted by the amplitude grating that is proportional to the transient dichroism signal as known from the common absorption relaxation.