Measurement of third order coherence by in situ autocorrelation for determining three-photon cross-sections

We show theoretically that the third order coherence at zero delay can be obtained by measuring the second and third order autocorrelation traces of a pulsed laser. Our theory enables the measurement of a fluorophore’s three-photon cross-section without prior knowledge of the temporal profile of the excitation pulse by using the same fluorescent medium for both the measurement of the third order coherence at zero delay as well as the cross-section. Such an in situ measurement needs no assumptions about the pulse shape nor group delay dispersion of the optical system. To verify the theory experimentally, we measure the three-photon action cross-section of Alexa Fluor 350 and show that the measured value of the three-photon cross-section remains approximately constant despite varied amounts of chirp on the excitation pulses.