There has been a tremendous amount of interest in developing highefficiency light-emitting diodes (LEDs) based on colloidal nanocrystals (NCs) of hybrid lead halide perovskites. Here, we systematically investigate the ligand effects on EL characteristics by tuning the hydrophobicity of primary alkylamine ligands used in NC synthesis. By increasing the ligand hydrophobicity, we find (i) a reduced NC size that induces a higher degree of quantum confinement, (ii) a shortened exciton lifetime that increases the photoluminescence quantum yield, (iii) a lowering of refractive index that increases the light outcoupling efficiency, and (iv) an increased thin-film resistivity. Accordingly, ligand engineering allows us to demonstrate high-performance green LEDs exhibiting a maximum external quantum efficiency up to 16.2%. The device operational lifetime, defined by the time lasted when the device luminance reduces to 85% of its initial value, LT85, reaches 243 min at an initial luminance of 516 cd m −2 .

Quantum dot (QD) light-emitting diodes (LEDs) are emerging as one of the most promising candidates for next-generation displays. However, their intrinsic light outcoupling efficiency remains considerably lower than the organic counterpart, because it is not yet possible to control the transition-dipole-moment (TDM) orientation in QD solids at device level. Here, using the colloidal lead halide perovskite anisotropic nanocrystals (ANCs) as a model system, we report a directed self-assembly approach to form the anisotropic nanocrystal superlattices (ANSLs). Emission polarization in individual ANCs rescales the radiation from horizontal and vertical transition dipoles, effectively resulting in preferentially horizontal TDM orientation. Based on the emissive thin films comprised of ANSLs, we demonstrate an enhanced ratio of horizontal dipole up to 0.75, enhancing the theoretical light outcoupling efficiency of greater than 30%. Our optimized single-junction QD LEDs showed peak external quantum efficiency of up to 24.96%, comparable to state-of-the-art organic LEDs.

We report efficient perovskite nanocrystal LEDs based on a new electron transport material, BBIA, possessing high electron mobility of 4.17 × 10−4 cm2 V−1 s−1. BBIA-based devices exhibit a nearly two-fold enhancement than TPBi counterpart.

It is well known that by horizontally aligning the transition dipole moments of exciton dipoles in the emitter films of organic light‐emitting diodes (OLEDs), a larger fraction of the radiative power can escape from the OLED stack, increasing the light outcoupling efficiency by up to 50 % compared to the isotropic counterparts. In this account, we review recent advances in understanding this phenomenon, with a special focus on the practical strategies to control the molecular orientation in vacuum‐deposited films of thermally activated delayed fluorescent (TADF) dyes. The role of molecular orientation in efficient OLED design is discussed, which has been experimentally proven to increase the external quantum efficiency exceeding 30 %. We outline the future challenges and perspectives in this field, including the potential to extend the concept to the solution‐processed films. Finally, the development of multiscale computer simulations is reviewed to assess their potential as a complementary approach to systematically screening OLED molecules in silico.

Quantum dot (QD) light-emitting diodes (LEDs) are emerging as one of the most promising candidates for next-generation displays. However, their intrinsic light outcoupling efficiency remains considerably lower than the organic counterpart, because it is not yet possible to control the transition-dipole-moment (TDM) orientation in QD solids at device level. Here, using the colloidal lead halide perovskite nanoplatelets (NPLs) as a model system, we report a directed self-assembly approach to form the two-dimensional superlattices (2DSLs) with the out-of-plane vector perpendicular to the substrate plane. The ligand and substrate engineering yields close-packed planar arrays with the side faces linked to each other. Emission polarization in individual NPLs rescales the radiation from horizontal and vertical transition dipoles, effectively resulting in preferentially horizontal TDM orientation. Based on the emissive thin films comprised of stacks of 2D superlattices, we demonstrate an enhanced ratio of horizontal dipole as revealed by 2D k-space spectroscopy. Our optimized single-junction QD LEDs showed peak external quantum efficiency of up to 24% and power efficiency exceeding 110 lm W-1, comparable to state-of-the-art organic LEDs.

Tuning the transition dipole moment (TDM) orientation in low-dimensional semiconductors is of fundamental and practical interest, as it enables high-efficiency nanophotonics and light-emitting diodes. However, despite recent progress in nanomaterials physics and chemistry, material systems that allow continuous tuning of the TDM orientation remain rare. Here, combining k-space photoluminescence spectroscopy and multiscale modeling, we demonstrate that the TDM orientation in lead halide perovskite (LHP) nanoplatelet (NPL) solids is largely confinement-tunable through the NPL geometry that regulates the anisotropy of Bloch states, dielectric confinement, and exciton fine structure. We further quantified the role of uniaxial ordering during NPL assembly in modifying the macroscopic emission directionality of thin films, which is especially important in actual optoelectronic devices. Our theoretical framework successfully corroborates the previous prediction of exciton bright level order reversal with experimental evidence of a counterintuitive reduction of in-plane dipole ratio in ultrathin (one-and two-monolayer-thick) NPLs, even at room temperature. More interestingly, the NPLs retain their TDM orientation in binary blends irrespective of interparticle energy transfer, owing to the phase segregation and NPL−NPL decoupling, enabling the design of films whose fluorescence exhibits an intrinsic angle-dependent color gradient.

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