Interplay of Quantum Dynamics and Decoherence.
Light absorption, electronic energy transfer (EET) and charge dissociation are important for both organic photovoltaic (OPV) devices and natural photosynthesis. The constitutive processes for an organic solar cell are analogous to those responsible for light harvesting in photosynthesis. In both cases, photons are captured in special chromophores whereby electronic excitations (excitons) are created; the excitation energy diffuses through a network of molecular structures until the electron-hole (e-h) pairs reach the photosynthetic reaction center (RC) or the donor/acceptor (D-A) junction. At the RC, or the D-A interface, electron-hole pairs are dissociated. Geminate recombination of e-h pairs is a major loss effect during the energy transfer and charge dissociation processes. The electrochemical energy produced is used to drive biochemical reactions in plants, algae and bacteria, or to power electric devices.
We developed a coarse-grained molecular envelope function method (MEF) to study the charge photogeneration dynamics in large scale systems taking into account the underlying quantum nature of the process. We focus on the interplay of quantum dynamics, quantum decoherence and recombination effects to describe the overall charge and energy transfer processes. ( J. Phys. Chem. C, 2017, 121 (42), pp 23276)
