Dipole-tunable interfacial engineering strategy for high-performance all-inorganic red quantum-dot light-emitting diodes

All-inorganic quantum dot (QD) light-emitting diodes (AI-QLEDs) with excellent stability received enormous interest in the past few years. Nevertheless, the vast energy offset and the high trap density at the NiOX/QDs interface limit hole injection leading to fluorescence quenching and hampering the performance. Here, we present self-assembled monolayers (SAMs) with phosphonic acid (PA) anchoring groups modifying NiOX hole transport layer (HTL) to tune energy level and passivate trap states. This strategy facilitates hole injection owning to the well-aligned energy level by interface dipole, downshifting the vacuum level, reducing the hole injection barrier from 0.94 eV to 0.28 eV. Meanwhile, it mitigates the interfacial recombination by passivating surface hydroxyl group (-OH) and oxygen vacancy (VO) traps in NiOX. The electron leakage from QDs toward NiOX HTL is significantly suppressed. The all-inorganic R-QLEDs exhibit one of the highest maximum luminance, external quantum efficiency and operational lifetime of 88980 cd m−2, 10.3% and 335045 h (T50@100 cd m−2), respectively. The as-proposed interface engineering provides an effective design principle for high-performance AI-QLEDs for future outdoor and optical projection-type display applications

Impacts of MAPbBr3 Additive on Crystallization Kinetics of FAPbI3 Perovskite for High Performance Solar Cells

Blending perovskite with different cations has been successful in improving performance of perovskite solar cells, but the complex pathway of perovskite crystal formation remains a mystery, hindering its further development. In this paper, the detailed crystallization process of formamidinium lead iodide (FAPbI3) perovskite films doped by methylammonium lead bromide (MAPbBr3) additive was investigated by in situ grazing incident wide-angle X-ray scattering measurements during both spin coating and annealing. During spin-coating, it was found that the FAPbI3 perovskite precursor easily formed a mixture of black perovskite phase (α phase) and non-perovskite yellow phase (δ phase) after the addition of MAPbBr3, whereas only δ phase formed without MAPbBr3. The δ phase gradually converted to α phase during annealing and there was only α phase left in both films with and without MAPbBr3. However, the doped films presented high film quality without PbI2 residue in contrast to the undoped films. These findings imply that the MAPbBr3 additive can effectively suppress the formation of the unfavorable δ phase and trigger the formation of the optically active α phase even during spin-coating, which enhances the film quality possibly by removing the energy barriers from δ phase to α phase at room temperature. Finally, PSCs based on MAPbBr3-doped FAPbI3 were fabricated with a champion efficiency as high as 19.4% from 14.2% for the PSCs based on undoped FAPbI3

Chemical interaction dictated energy level alignment at the N,N'-dipentyl-3,4,9,10-perylenedicarboximide/CH3NH3PbI3 interface

Here, we report the electronic structures at the N, N′-dipentyl-3,4,9,10-perylenedicarboximide (PTCDI-C5)/CH3NH3PbI3 interface identified in-situ by X-ray photoemission spectroscopy and ultraviolet photoemission spectroscopy. Strong chemical reactions are found to occur upon the deposition of PTCDI-C5 molecules on CH3NH3PbI3. Electron donation from PTCDI-C5 molecules to CH3NH3PbI3 leads to the filling of surface states and the emergence of an interfacial gap state with its onset tailed to the Fermi level. As a consequence, the downward surface band bending resulting from surface states acting as donor states at the pristine perovskite surface is reduced by 0.2 eV. After the energy level alignment at the interface is established, the perovskite conduction band minimum is found to be in line with the lowest unoccupied molecular orbital favoring the electron extraction with a moderate valence band maximum-highest occupied molecular orbital offset of ∼0.7 eV. The present results demonstrate that interfacial chemical reactions can dictate energetics at organic/perovskite interfaces. Understanding the chemical interaction and resultant electronic structures at those interfaces is crucial for efficient and long-term stable perovskite-based devices when passivation of chemical active sites and matched energy level could be readily reached

Charge carrier regulation for efficient blue quantum-dot light-emitting diodes via a high-mobility coplanar cyclopentane[b]thiopyran derivative

The performance of blue quantum dot light-emitting diodes (QLEDs) is limited by unbalanced charge injection, resulting from insufficient holes caused by low mobility or significant energy barriers. Here, we introduce an angular-shaped heteroarene based on cyclopentane[b]thiopyran (C8–SS) to modify the hole transport layer poly-N-vinylcarbazole (PVK), in blue QLEDs. C8–SS exhibits high hole mobility and conductivity due to the π···π and S···π interactions. Introducing C8–SS to PVK significantly enhanced hole mobility, increasing it by 2 orders of magnitude from 2.44 × 10–6 to 1.73 × 10–4 cm2 V–1 s–1. Benefiting from high mobility and conductivity, PVK:C8–SS-based QLEDs exhibit a low turn-on voltage (Von) of 3.2 V. More importantly, the optimized QLEDs achieve a high peak power efficiency (PE) of 7.13 lm/W, which is 2.65 times that of the control QLEDs. The as-proposed interface engineering provides a novel and effective strategy for achieving high-performance blue QLEDs in low-energy consumption lighting applications

Correction: A disorder-free conformation boosts phonon and charge transfer in an electron-deficient-core-based non-fullerene acceptor (vol 8, pg 8566, 2020)

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Anchoring charge selective self-assembled monolayers for tin-lead perovskite solar cells

Self-assembled monolayers (SAMs) have displayed great potential for improving efficiency and stability in p-i-n perovskite solar cells (PSCs). The anchoring of SAMs at the conductiv metal oxide substrates and their interaction with perovskite materials must be rationally tailored to ensure efficient charge carrier extraction and improved quality of the perovskite films. Herein, SAMs molecules with different anchoring groups and spacers to control the interaction with perovskite in the p-i-n mixed Sn-Pb PSCs are selected. It is found that the monolayer with the carboxylate group exhibits appropriate interaction and has a more favorable orientation and arrangement than that of the phosphate group. This results in reduced nonradiative recombination and enhanced crystallinity. In addition, the short chain length leads to an improved energy level alignment of SAMs with perovskite, improving hole extraction. As a result, the narrow bandgap (≈1.25 eV) Sn-Pb PSCs show efficiencies of up to 23.1% with an open-circuit voltage of up to 0.89 V. Unencapsulated devices retain 93% of their initial efficiency after storage in N2 atmosphere for over 2500 h. Overall, this work highlights the underexplored potential of SAMs for perovskite photovoltaics and provides essential findings on the influence of their structural modification

Defects controlled doping and electrical transport in TiS2 single crystals

TiS2 has been intensively studied as an electrode material and a thermoelectric material for energy storage and conversion applications due to its high electrical conductivity. Understanding the influence of defects on electrical transport is of importance not only to resolve the long-standing question concerning the nature of TiS2, but also for the rational design of TiS2 based devices for energy scavenging applications. In this study, we integrate photoemission spectroscopy, Raman spectroscopy, and electrical transport measurements to determine the chemical compositions dominated by defects and their influence on the doping and electrical properties. Our results demonstrate that TiS2 is a heavily self-doped semiconductor with the Fermi level close to the conduction band, which serves as the conclusive experimental evidence regarding the semiconducting nature of TiS2. The doping effect is sensitive to the (subtle) changes in the chemical composition. The electron donation from the Ti interstitials (Tii) to the TiS2 host explains the high carrier concentration. The Ti Frenkel pair (TiF) acting as the acceptor is responsible for the decrease in the electron carrier concentration and electrical conductivity. High conductivity maintains upon partial oxidization, indicating the oxidization-tolerance in terms of the electronic structure. Our results provide valuable insight into the evolution of electronic properties modulated by defects that reveal unambiguously the self-doped semiconducting nature of TiS2 and chemical- and environment-tolerance of TiS2 as an advanced energy scavenging material.</p

Top-Down Exfoliation Process Constructing 2D/3D Heterojunction toward Ultrapure Blue Perovskite Light-Emitting Diodes

3D perovskites with low energy disorder and high ambipolar charge mobility represent a promising solution for efficient and bright light-emitting diodes. However, the challenges of regulating the nanocrystal size to trigger the quantum confinement effect and control the surface trap states to reduce charge loss hinder the applications of 3D perovskites in blue perovskite light-emitting diodes (PeLEDs). In this study, we present a top-down exfoliation method to obtain blue 3D perovskite films with clipped nanocrystals and tunable bandgaps by employing methyl cyanide (MeCN) for post-treatment. In this method, the MeCN solvent exfoliates the surface components of the 3D perovskite grains through a partial dissolution process. Moreover, the dissolved precursor can be further utilized to construct an ingenious 2D/3D heterostructure by incorporating an organic spacer into the MeCN solvent, contributing to efficient defect passivation and improved energy transfer. Consequently, efficient PeLEDs featuring ultrapure blue emission at 478 nm achieve a record external quantum efficiency of 12.3% among their 3D counterparts. This work emphasizes the significance of inducing the quantum confinement effect in 3D perovskites for efficient blue PeLEDs and provides a viable scheme for the in situ regulation of perovskite crystals

Suppressed Energy Transfer Loss of Dion–Jacobson Perovskite Enabled by DMSO Vapor Treatment for Efficient Sky-Blue Light-Emitting Diodes

The formation of a middle-n phase is obstructed by a high formation energy for the Dion–Jacobson perovskites, leading to an energy transfer gap between the small-n phases and the light emission phase, which thus largely decreases the efficiencies of the related perovskite light-emitting diodes (PeLEDs). Herein, we report that the phase distribution is effectively modulated by the treatment of DMSO vapor, largely increasing the efficiencies of the relating PeLEDs to 13.7% and 15.5% with emission peaks at 489 and 494 nm, respectively. The rearranged phase distribution with matched energy landscape and phase content shows efficient energy transfer with an effectively eliminated energy transfer gap and significantly suppressed energy losses. This work puts forward an effective way of DMSO vapor treatment to modulate the phase crystallization and highlights the importance of reducing the energy losses in the energy transfer process, for the efficient light emission of Dion–Jacobson perovskites