A two-step ligand-exchange strategy is developed, in which the long-carbon- chain ligands on all-inorganic perovskite (CsPbX , X = Br, Cl) quantum dots (QDs) are replaced with halide-ion-pair ligands. Green and blue light-emitting diodes made from the halide-ion-pair-capped quantum dots exhibit high external quantum efficiencies compared with the untreated QDs.
We demonstrate ultra-air- and photostable CsPbBr3 quantum dots (QDs) by using an inorganic-organic hybrid ion pair as the capping ligand. This passivation approach to perovskite QDs yields high photoluminescence quantum yield with unprecedented operational stability in ambient conditions (60 ± 5% lab humidity) and high pump fluences, thus overcoming one of the greatest challenges impeding the development of perovskite-based applications. Due to the robustness of passivated perovskite QDs, we were able to induce ultrastable amplified spontaneous emission (ASE) in solution processed QD films not only through one photon but also through two-photon absorption processes. The latter has not been observed before in the family of perovskite materials. More importantly, passivated perovskite QD films showed remarkable photostability under continuous pulsed laser excitation in ambient conditions for at least 34 h (corresponds to 1.2 × 10(8) laser shots), substantially exceeding the stability of other colloidal QD systems in which ASE has been observed.
Defect passivation and surface modification of hybrid perovskite films are essential to achieving high power conversion efficiency (PCE) and stable perovskite photovoltaics. Here, we demonstrate a facile strategy that combines high PCE with high stability in CH 3 NH 3 PbI 3 (MAPbI 3 ) solar cells. The strategy utilizes inorganic perovskite quantum dots (QDs) to distribute elemental dopants uniformly across the MAPbI 3 film and attach ligands to the film's surface. Compared with pristine MAPbI 3 films, MAPbI 3 films processed with QDs show a reduction in tail states, smaller trap-state density, and an increase in carrier recombination lifetime. This strategy results in reduced voltage losses and an improvement in PCE from 18.3% to 21.5%, which is among the highest efficiencies for MAPbI 3 devices. Ligands introduced with the aid of the QDs render the perovskite film's surface hydrophobic-inhibiting moisture penetration. The devices maintain 80% of their initial PCE under 1-sun continuous illumination for 500 h and show improved thermal stability.
Molecular doping has recently been shown to improve the operating characteristics of organic photovoltaics (OPVs). Here, we prepare neutral Diquat (DQ) and use it as n-dopant to improve the performance of state-of-the-art OPVs. Adding DQ in ternary bulk-heterojunction (BHJ) cells based of PM6:Y6:PC 71 BM is found to consistently increase their power conversion efficiency (PCE) from 16.7 to 17.4%. Analyses of materials and devices reveal that DQ acts as n-type dopant and morphology modifier for the BHJ leading to observable changes in its surface topography. The resulting n-doped BHJs exhibit higher optical absorption coefficients, balanced ambipolar transport, longer carrier lifetimes and suppressed bimolecular recombination, which are ultimately responsible for the increased PCE. The use of DQ was successfully extended to OPVs based on PM6:BTP-eC9:PC 71 BM for which a maximum PCE of 18.3% (uncertified) was achieved. Our study highlights DQ as a promising dopant for application in next generation organic solar cells.
The rapid development of halide perovskite synthesis offers the opportunity to fabricate high-quality perovskite nanocrystals (NCs), whose structural uniformity can lead to assembled supra-structures with improved device performance and novel collective properties. Light is known to significantly affect the structure and properties of halide perovskites and plays a crucial role in the growth and assembly of their crystals. Nevertheless, the light-induced growth mechanisms of perovskite NCs are not yet clearly understood. In this work, we performed a systematic study of the visible-light-induced template-free synthesis of CsPbBr 3 nanowires (NWs) generated through self-assembly of cubic (in phase and close to cubic morphology) NCs. Using atomicresolution electron microscopy, we visualized the cubic-toorthorhombic phase transition in NCs and the interface between coalesced NCs. Remarkably, the images of the interface revealed the coexistence of CsBr and PbBr 2 surface terminations in halide perovskites. Our results shed light on the mechanism underlying the observed anisotropic assembly of halide perovskites and elucidate the vital role of light illumination during this process. More importantly, as an elegant and promising green-chemistry approach, light-induced self-assembly represents a rational method for designing perovskites.
The all‐inorganic nature of CsPbI3 perovskites allows to enhance stability in perovskite devices. Research efforts have led to improved stability of the black phase in CsPbI3 films; however, these strategies—including strain and doping—are based on organic‐ligand‐capped perovskites, which prevent perovskites from forming the close‐packed quantum dot (QD) solids necessary to achieve high charge and thermal transport. We developed an inorganic ligand exchange that leads to CsPbI3 QD films with superior phase stability and increased thermal transport. The atomic‐ligand‐exchanged QD films, once mechanically coupled, exhibit improved phase stability, and we link this to distributing strain across the film. Operando measurements of the temperature of the LEDs indicate that KI‐exchanged QD films exhibit increased thermal transport compared to controls that rely on organic ligands. The LEDs exhibit a maximum EQE of 23 % with an electroluminescence emission centered at 640 nm (FWHM: ≈31 nm). These red LEDs provide an operating half‐lifetime of 10 h (luminance of 200 cd m−2) and an operating stability that is 6× higher than that of control devices.
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