Quantum coherence controls the charge separation in a prototypical artificial light harvesting system

In artificial light harvesting systems the conversion of light into charges or chemical energy happens on the femtosecond time scale and is thought to involve the incoherent jump of an electron from the optical absorber to an electron acceptor. Here we investigate the primary process of electronic charge transfer dynamics in a carotene-porphyrin-fullerene triad, a prototypical elementary component for an artificial light harvesting system combining coherent femtosecond spectroscopy and first-principles quantum dynamics simulations. Our experimental and theoretical results provide strong evidence that the driving mechanism of the photoinduced current generation cycle is a quantum-correlated wavelike motion of electrons and nuclei on a timescale of few tens of femtoseconds. We furthermore highlight the fundamental role played by the interface between the light-absorbing chromophore and the charge acceptor in triggering the coherent wavelike electron-hole splitting. © 2013 IEEE