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We present a detailed investigation of ultrafast (subpicosecond) excitondynamics in the lattice model of a donor/acceptor heterojunction. Excitongeneration by means of a photoexcitation, exciton dissociation, and furthercharge separation are treated on equal footing. The experimentally observedpresence of space-separated charges at $\lesssim 100$ fs after thephotoexcitation is usually attributed to ultrafast transitions from excitons inthe donor to charge transfer and charge separated states. Here, we show,however, that the space-separated charges appearing on $\lesssim 100$-fs timescales are predominantly directly optically generated. Our theoretical insightsinto the ultrafast pump-probe spectroscopy challenge usual interpretations ofpump-probe spectra in terms of ultrafast population transfer from donorexcitons to space-separated charges.

Origin of space-separated charges in photoexcited organic heterojunctions on ultrafast time scales