Exploring the role of phase modulation on photoluminescence yield

Abstract

We report an investigation to elucidate the mechanisms of control in phase-sensitive experiments in two molecular systems. A first inspection of optimization procedures yields the same experimental result: increase in the emission efficiency upon excitation by a phase modulated pulse in a two-photon transition. More detailed studies, which include power dependence, spectral response, one and two color pump–probe and pump–pump experiments show that while for one chromophore phase modulation leads to spectral matching between the two-photon cross section and the second order power spectrum for the other it provides a tool to manipulate the wavepacket dynamics in the excited state.