Photosynthesis-inspired device architectures for organic photovoltaics

Organic semiconductor photovoltaics offer a promising route to low-cost, scalable, emissions-free electricity generation. However, achieving higher power conversion efficiencies is critical before these devices can play a larger role in our future energy generation landscape. Organic photovoltaic devices are currently limited by two primary challenges: (1) a trade-off between light absorption and exciton diffusion and (2) low open-circuit voltage due to charge recombination at the donor-acceptor interface. In this work, we demonstrate two new device architectures inspired by photosynthesis that aim to overcome these two challenges. First, we overcome the trade-off between light absorption and exciton diffusion by introducing an external light absorbing antenna layer. We model energy transfer from the antenna to the charge generating layers via surface plasmon polariton modes in the interfacial thin silver contact and via radiation into waveguide modes. We experimentally demonstrate devices with both single layer antennas and strongly absorbing resonant cavity antennas. We measure energy transfer efficiency from the antenna layer to the PV active layers as high as 51±10%. We discuss structural design criteria and describe ideal antenna material characteristics. Second, we reduce charge transfer state recombination in organic photovoltaics by inserting a thin interfacial layer at the donor-acceptor interface. The thin interfacial layer creates a cascade energy structure that destabilizes the Coulombically bound charge transfer state formed immediately following exciton dissociation. We find the optimal interfacial layer thickness to be approximately 1.5 nm. In CuPc/C60 devices, under simulated solar illumination the short-circuit current increased 34%, the opencircuit voltage increased 33%, and the power conversion efficiency increased 49%. Thin interfacial layers can also be used to study the physics of exciton separation. Thesis Supervisor: Marc A. Baldo Title: Associate Professor