Sensitive Organic Photodetectors With Spectral Response up to 1.3 µm Using a Quinoidal Molecular Semiconductor

Abstract Detecting short‐wavelength infrared (SWIR) light has underpinned several emerging technologies. However, the development of highly sensitive organic photodetectors (OPDs) operating in the SWIR region is hindered by their poor external quantum efficiencies (EQEs) and high dark currents. Herein, the development of high‐sensitivity SWIR‐OPDs with an efficient photoelectric response extending up to 1.3 µm is reported. These OPDs utilize a new ultralow‐bandgap molecular semiconductor featuring a quinoidal tricyclic electron‐deficient central unit and multiple non‐covalent conformation locks. The SWIR‐OPD achieves an unprecedented EQE of 26% under zero bias and an even more impressive EQE of up to 41% under a –4 V bias at 1.10 µm, effectively pushing the detection limit of silicon photodetectors. Additionally, the low energetic disorder and trap density in the active layer lead to significant suppression of thermal‐generation carriers and dark current, resulting in excellent detectivity ( D sh * ) exceeding 10 13 Jones from 0.50 to 1.21 µm and surpassing 10 12 Jones even at 1.30 µm under zero bias, marking the highest achievements for OPDs beyond the silicon limit to date. Validation with photoplethysmography measurements, a spectrometer prototype in the 0.35–1.25 µm range, and image capture under 1.20 µm irradiation demonstrate the extensive applications of this SWIR‐OPD.