Coherent interactions in femtosecond transient grating.

Abstract

Transient grating of a dye in liquid has been measured as a function of the electronic coherence period. A diffractive beam splitter and a pair of wedge prisms are implemented to achieve precise spatial phase overlap and interferometrically accurate control of the time delay between the pump pulses. As the electronic coherence period is varied, coherent interactions lead to an enhancement or loss of the sharp feature in the transient grating signal near time zero, which is usually called coherent spike. Sensitivity of the transient grating signal to the solvation process also changes by the coherence time delay. All the features can be accounted for by invoking third-order nonlinear response functions. Numerical simulations have been performed to corroborate our description. This work identifies a major source of the coherent spike in the transient grating and transient absorption experiments. In addition, it allows us to propose a method that measures the solvation function more efficiently than conventional transient grating technique does.