High-Detectivity Non-Fullerene Organic Photodetectors Enabled by a Cross-Linkable Electron Blocking Layer

The anode interlayer plays a critical role in the performance of organic photodetectors, which requires sufficient electron-blocking ability to simultaneously attain a high photocurrent and low dark current. Here, we developed two cross-linkable polymers, which can be deposited on the top of the widely used poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) and form a robust layer that can effectively suppress the electron injection from the anode under reverse bias. The optimized device with the resulting cross-linkable XP2 exhibited the lowest dark current density of 5.81 × 10^-9 A cm^-2 at -0.1 V, which is about 2 orders of magnitude lower than the control devices. A remarkable responsivity of 0.5 A W^-1 and a detectivity of >1 × 10¹³ Jones at a near-infrared wavelength of 800 nm were achieved. Of particular importance is that the resulting device exhibited a linear dynamic range of >135 dB associated with a high working frequency that is shorter than typical commercial digital imagers. The planar heterojunction devices demonstrate that the dark current is closely correlated to the charge generation, which relied on the highest occupied molecular orbital energy levels of the developed cross-linked interlays. The Mott-Schottky analysis revealed that the optimized cross-linked interlayer increased the depletion width of the devices.