High-Performance Colloidal Quantum Dot Photodiodes via Suppressing Interface Defects

PbS colloidal quantum dot (CQD) infrared photodiodes have attracted wide attention due to the prospect of developing cost-effective infrared imaging technology. Presently, ZnO films are widely used as the electron transport layer (ETL) of PbS CQDs infrared photodiodes. However, ZnO-based devices still suffer from the problems of large dark current and low repeatability, which are caused by the low crystallinity and sensitive surface of ZnO films. Here, we effectively optimized the device performance of PbS CQDs infrared photodiode via diminishing the influence of adsorbed H₂O at the ZnO/PbS CQDs interface. The polar (002) ZnO crystal plane showed much higher adsorption energy of H₂O molecules compared with other nonpolar planes, which could reduce the interface defects induced by detrimentally adsorbed H₂O. Based on the sputtering method, we obtained the [002]-oriented and high-crystallinity ZnO ETL and effectively suppressed the adsorption of detrimental H₂O molecules. The prepared PbS CQDs infrared photodiode with the sputtered ZnO ETL demonstrated lower dark current density, higher external quantum efficiency, and faster photoresponse compared with the sol-gel ZnO device. Simulation results further unveiled the relationship between interface defects and device dark current. Finally, a high-performance sputtered ZnO/PbS CQDs device was obtained with a specific detectivity of 2.15 × 10¹² Jones at -3 dB bandwidth (94.6 kHz).