A strategy for achieving high-performance single layer polymer photodetectors through dark current reduction using PMMA additives

Suppressing dark current density is crucial for optimizing the performance of organic photodetectors (PDs), particularly in terms of detectivity (D∗) and linear dynamic range (LDR). Organic PDs often utilize the bulk heterojunction structure of organic solar cells to significantly increase photocurrent. However, unlike solar cells, which are unaffected by dark current, photodetectors' performance is substantially limited by it. The interconnected network of bulk heterojunctions leads to a noticeable increase in dark current, thus degrading device performance. Typically, reducing dark current involves adding a modification layer or using multilayer planar heterojunctions, which effectively reduce dark current but often delay response speed and complicate manufacturing. This study presents an alternative approach by incorporating a small concentration of PMMA into single-layer polymer photodetectors, significantly reducing dark current without affecting photocurrent. For this single-layer polymer PD, an ultra-low dark current density of 1.25 × 10⁻⁸ A/cm², a high D_sh∗ of 2.74 × 10¹² Jones, an LDR of 120.5 dB, and a fast response time with 1.6 μs were achieved. The capacitance-voltage (C-V), electrochemical impedance spectroscopy (EIS), scanning electron microscopy (SEM), and atomic force microscopy (AFM) measurements revealed that the PMMA additive reduces internal defects, increases bulk resistance, optimizes phase separation, and enhances carrier transport efficiency. The improved device performances are attributed to a more efficient vertical arrangement of the donor-acceptor interface and carrier channels, thus reducing carrier recombination loss. These findings offer a new direction for fabricating high-performance single-layer photodetectors.