Colloidal PbS Quantum Dot Photodiode Imager with Suppressed Dark Current

Lead sulfide (PbS) colloidal quantum dots (CQDs) for photodetectors (PDs) have garnered great attention due to their potential use as low-cost, high-performance, and large-area infrared focal plane arrays. The prevailing device architecture employed for PbS CQD PDs is the p-i-n structure, where PbS CQD films treated with thiol molecules, such as 1,2-ethanedithiol (EDT), are widely used as p-type layers due to their favorable band alignment. However, PbS-EDT films face a critical challenge associated with low film quality, resulting in many defects that curtail the device performance. Herein, a controlled oxidization process is developed for better surface passivation of the PbS-EDT transport layer. The dark current density (J_d) of PbS CQD PDs based on optimized PbS-EDT layer shows a dramatic decrease by nearly 2 orders of magnitude. The increase of carrier lifetime and suppression of carrier recombination via controlled oxidation in PbS-EDT CQDs were confirmed by transient absorption spectra and electrochemical impedance spectra. The device based on the optimized PbS-EDT hole transport layer (HTL) exhibits a specific detectivity (D*) that is 3.4 times higher compared to the control device. Finally, the CQD PD employing oxidization PbS-EDT CQDs is integrated with a thin film transistor (TFT) readout circuit, which successfully accomplishes material discrimination imaging, material occlusion imaging, and smoke penetration imaging. The controlled oxidization strategy verifies the significance of surface management of CQD solids and is expected to help advance infrared optoelectronic applications based on CQDs.