Coherent Charge Transfer Reveals a Different Theoretical Limit of Power Conversion Efficiency in Organic Solar Cells

The hopping charge transfer (CT) theory is used to explain the dynamics of traditional donor-acceptor (D-A) devices in organic solar cells (OSCs). But it is not applicable to the unconventional OSCs inspired by photosynthesis, referred to as Z-devices. In this study, we establish a universal heterojunction CT model in OSCs, based on the reported coherent CT in photosynthesis. Compared to the trade-off between energy loss and charge generation efficiency in the D-A device, we analyze its change in the Z-device. We introduce the "avalanche-like" CT of the Z-device induced by many-body Coulomb interaction and relevant experimental support. Combining with the Shockley-Queisser theory, we evaluate the theory limit power conversion efficiency of a D-A device and a Z-device. The Z-device has the potential to surpass the Shockley-Queisser limit of 33%.