AbstractIn a novel modification of transient differential transmission spectroscopy, the first excited state S1 is reexcited via a second laser pulse towards a higher lying state Sn. The dynamics of the relaxation of this state Sn as well as the states created from Sn are revealed by a broad-band probe pulse.We find that the charge carrier generation efficiency from Sn is higher compared to S1. The push and probe durations below 20 fs enable the temporal resolution of the ultrafast relaxation of the Sn state and enables us to identify the two main contributions to enhanced charge generation from Sn, energy migration towards sites of high dissociation probability, and exciton dissociation during vibrational relaxation.
