Ionically Gated Small-Molecule OPV: Interfacial Doping of Charge Collector and Transport Layer

We demonstrate an improvement in the performance of organic photovoltaic (OPV) systems based on small molecules by ionic gating via controlled reversible n-doping of multi-wall carbon nanotubes (MWCNTs) coated on fullerene electron transport layers (ETLs): C₆₀ and C₇₀. Such electric double-layer charging (EDLC) doping, achieved by ionic liquid (IL) charging, allows tuning of the electronic concentration in MWCNTs and the fullerene planar acceptor layers, increasing it by orders of magnitude. This leads to the decrease of the series and increase of the shunt resistances of OPVs and allows use of thick (up to 200 nm) ETLs, increasing the durability of OPVs. Two stages of OPV enhancement are described upon the increase of gating bias V_g: at small (or even zero) V_g, the extended interface of ILs and porous transparent MWCNTs is charged by gating, and the fullerene charge collector is significantly improved, becoming an ohmic contact. This changes the S-shaped J-V curve via improving the electron collection by an n-doped MWCNT cathode with an ohmic interfacial contact. The J-V curves further improve at higher gating bias V_g due to the increase of the Fermi level and decrease of the MWCNT work function. At the next qualitative stage, the acceptor fullerene layer becomes n-doped by electron injection from MWCNTs while ions of ILs penetrate into the fullerene. At this step, the internal built-in field is created within OPV, which helps in exciton dissociation and charge separation/transport, increasing further the J_sc and the fill factor. The ionic gating concept demonstrated here for most simple classical planar small-molecule OPV cells can be potentially applied to more complex highly efficient hybrid devices, such as perovskite photovoltaic with an ETL or a hole transport layer, providing a new way to tune their properties via controllable and reversible interfacial doping of charge collectors and transport layers.