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We report a theoretical description and experimental implementation of anovel two-dimensional coherent excitation spectroscopy based onquasi-steady-state photoinduced absorption measurement of a long-livednonlinear population. We have studied asemiconductor-polymer:fullerene-derivative distributed heterostructure bymeasuring the 2D excitation spectrum by means of photoluminescence,photocurrent and photoinduced absorption from metastable polaronic products. Weconclude that the photoinduced absorption probe is a viable and valuable probein this family of 2D coherent spectroscopies.

Probing polaron excitation spectra in organic semiconductors by photoinduced-absorption-detected two-dimensional coherent spectroscopy