Time-delayed four-wave mixing using incoherent light for observation of ultrafast population relaxation

Abstract

Time-delayed four-wave mixing using incoherent light has been proposed as a new method to measure the ultrafast population relaxation time T₁. Assuming three input beams of incoherent light with much longer duration than T1, the theoretical calculation has shown that the decay curve by T₁ appears in the signal profile and that the time resolution is determined by the correlation time of the light. The decay time to be observed is twice that of the transient four-wave mixing with short pulses. We have experimentally confirmed the prediction by observing picosecond population relaxations of organic dye solutions, using nanosecond pulses from a normal broadband dye laser. An advantage of the present method over the pump-probe method using incoherent light is also discussed.