Double-ended passivator enables dark-current-suppressed colloidal quantum dot photodiodes for CMOS-integrated infrared imagers

Lead sulfide(PbS)colloidal quantum dot(CQD)photodiodes integrated with silicon-based readout integrated circuits(ROICs)offer a promising solution for the next-generation short-wave infrared(SWIR)imaging technology.Despite their potential,large-size CQD photodiodes pose a challenge due to high dark currents resulting from surface states on nonpassivated(100)facets and trap states generated by CQD fusion.In this work,we present a novel approach to address this issue by introducing double-ended ligands that supplementally passivate(100)facets of halidecapped large-size CQDs,leading to suppressed bandtail states and reduced defect concentration.Our results demonstrate that the dark current density is highly suppressed by about an order of magnitude to 9.6 nA cm^(2) at -10 mV,which is among the lowest reported for PbS CQD photodiodes.Furthermore,the performance of the photodiodes is exemplary,yielding an external quantum efficiency of 50.8%(which corresponds to a responsivity of 0.532 A W^(-1))and a specific detectivity of 2.5×10^(12) Jones at 1300 nm.By integrating CQD photodiodes with CMOS ROICs,the CQD imager provides high-resolution(640×512)SWIR imaging for infrared penetration and material discrimination.

用于PPG信号测试的大面积柔性胶体量子点红外光电二极管

以铟镓砷、碲镉汞等外延生长的单晶材料作为吸光层的光电二极管是红外探测技术的主流方案.然而,它们的刚性结构、极高成本以及有限尺寸使其无法满足诸如人体内外环境监测,便携式医疗等智能穿戴应用的需求.基于低温液相工艺的胶体量子点(CQDs)红外光电二极管是实现大面积柔性红外光电探测器极具竞争力的候选方案,但由于其发展年限较短,仍存在暗电流密度大、均匀性差以及工作稳定性差等问题.本文通过在CQDs墨水中引入聚酰亚胺来制备CQDs光电二极管.这种聚合物配体既实现了对CQDs表面缺陷态的钝化,又能够保持胶体墨水的单分散性和持久性.这两点使得光电探测器的吸光层形貌得以改善,同时暗电流密度显著降低,极大地优化了CQDs光电二极管的均匀性和工作稳定性.采用该方案制备的大面积柔性CQDs光电二极管能够实现高于10^(13)Jones的比探测率,可在环境光下实现可穿戴式光电体积描记(PPG)心率信号监测,极大地降低了成本和功耗.

Heterogeneous system synthesis of high quality PbS quantum dots for efficient infrared solar cells

As promising optoelectronic materials,lead sulfide quantum dots(PbS QDs)have attracted great attention.However,their applications are substantially limited by the QD quality and/or complicated synthesis.Herein,a facile new synthesis is developed for highly monodisperse and halide passivated PbS QDs.The new synthesis is based on a heterogeneous system containing a PbCl_(2)-Pb(OA)_(2)solid-liquid precursor solution.The solid PbCl_(2)inhibits the diffusion of monomers and maintains a high oversaturation condition for the growth of PbS QDs,resulting in high monodispersities.In addition,the PbCl_(2)gives rise to halide passivation on the PbS QDs,showing excellent stability in air.The high monodispersity and good passivation endow these PbS QDs with outstanding optoelectronic properties,demonstrated by a 9.43%power conversion efficiency of PbS QD solar cells with a bandgap of~0.95 eV(1,300 nm).We believe that this heterogeneous strategy opens up a new avenue optimizing for the synthesis and applications of QDs.

Efficient quantum dot infrared solar cells with enhanced lowenergy photon conversion via optical engineering

Infrared(IR)solar cells are promising devices for improving the power conversion efficiency(PCE)of conventional solar cells by expanding the utilization region of the sunlight spectrum to near-infrared range.IR solar cells based on colloidal quantum dots(QDs)have attracted extensive attention due to the widely tunable absorption spectrum controlled by dot size and the unique solution processibility.However,the trade-off in QD solar cells between light absorption and photo-generated carrier collection has limited the further improvement of PCE.Here,we present high-performance PbS QD IR solar cells resulting from the combination of boosted light absorption and optimized carrier extraction.By constructing an optical resonance cavity,the light absorption is significantly enhanced in the range of 1,150–1,300 nm at a relatively thin photoactive layer.Meanwhile,the thin photoactive layer facilitates efficient carrier extraction.Consequently,the PbS QD IR solar cells exhibit a highly efficient photoelectric conversion in the IR region,resulting in a high IR PCE of 1.3%which is comparable to the highest value of solution-processed IR solar cells based on PbSe QDs.These results demonstrate that constructing an optical resonance cavity is a reasonable strategy for effective conversion of photons in the devices aiming at light in a relatively narrow wavelength range,such as IR solar cells and narrow band photodetectors.