Breaking the Size Limitation of Directly-Synthesized PbS Quantum Dot Inks Toward Efficient Short-wavelength Infrared Optoelectronic Applications.

PbS quantum dots (QDs) are promising building blocks for solution-processed short-wavelength infrared (SWIR) devices. The recently developed direct synthesis of semi-conductive PbS QD inks has substantially simplified the preparation processing and reduced the material cost, while facing the challenge to synthesize large-size QDs with absorption covering the SWIR region. Herein, we for the first time realize a low-cost, scalable synthesis of SWIR PbS QD inks after an extensive investigation of the reaction kinetics. Finally, based on these PbS SWIR QD inks, the solar cell demonstrates a record-high power conversion efficiency (PCE) of 1.44 % through an 1100 nm cutoff silicon filter and the photodetector device shows a low dark current density of 2×10-6  A cm-2 at -0.8 V reverse bias with a high external quantum efficiency (EQE) of 70 % at ≈1300 nm. Our results realize the direct synthesis of low-cost and scalable SWIR QD inks and may accelerate the industrialization of consumer SWIR technologies.

Open-Shell Diradical-Sensitized Electron Transport Layer for High-Performance Colloidal Quantum Dot Solar Cells.

The zinc oxide (ZnO) nanoparticles (NPs) are well-documented as an excellent electron transport layer (ETL) in optoelectronic devices. However, the intrinsic surface flaw of the ZnO NPs can easily result in serious surface recombination of carriers. Exploring effective passivation methods of ZnO NPs is essential to maximize the device's performance. Herein, a hybrid strategy is explored for the first time to improve the quality of ZnO ETL by incorporating stable organic open-shell donor-acceptor type diradicaloids. The high electron-donating feature of the diradical molecules can efficiently passivate the deep-level trap states and improve the conductivity of ZnO NP film. The unique advantage of the radical strategy is that its passivation effectiveness is highly correlated with the electron-donating ability of radical molecules, which can be precisely controlled by the rational design of molecular chemical structures. The well-passivated ZnO ETL is applied in lead sulfide (PbS) colloidal quantum dot solar cells, delivering a power conversion efficiency of 13.54%. More importantly, as a proof-of-concept study, this work will inspire the exploration of general strategies using radical molecules to construct high-efficiency solution-processed optoelectronic devices.