Thickness-variation-insensitive near-infrared quantum dot LEDs.

In terms of tunable luminescence and high quantum efficiency, colloidal quantum dots (CQDs) are promising semiconductors for constructing near-infrared light-emitting diodes (NIR-LEDs). However, currently available NIR-LEDs are susceptible to variations in the emission layer thickness (EMLT), the highest external quantum efficiency (EQE) decreases to below 50% (relative to peak EQE) when the EMLT varies out of a narrow range of (±30 nm). This is due to the thickness-dependent carrier recombination rate and current density variation, resulting in batch-to-batch EQE fluctuations that limit LED reproducibility. Here we report efficient NIR-LEDs that exhibit EQE variations of less than 15% (relative to the champion EQE) over an EMLT range of 40-220 nm; the highest achievable EQE of ∼11.5% was obtained by encapsulating a 212 nm-thick CQD within a type-I inorganic shell to enhance the radiative recombination in the dots, resulting in a high photoluminescence quantum yield of 80%, and by post-treating the films with a bifunctional linking agent to improve and balance the hole and electron mobilities in the entire film (electron mobility: 8.23 × 10-3 cm2 V-1 s-1; hole mobility: 7.0 × 10-3 cm2 V-1 s-1). This work presents the first NIR-LEDs that exhibit EMLT-invariant EQE over an EMLT range of 40-220 nm, which represents the highest EQE among reported CQD NIR-LEDs with a QD thickness exceeding 100 nm.

Ion-Dipole Interaction Enabling Highly Efficient CsPbI3 Perovskite Indoor Photovoltaics.

Metal halide perovskites are ideal candidates for indoor photovoltaics (IPVs) because of their easy-to-adjust bandgaps, which can be designed to cover the spectrum of any artificial light source. However, the serious non-radiative carrier recombination under low light illumination restrains the application of perovskite-based IPVs (PIPVs). Herein, polar molecules of amino naphthalene sulfonates are employed to functionalize the TiO2 substrate, anchoring the CsPbI3 perovskite crystal grains with a strong ion-dipole interaction between the molecule-level polar interlayer and the ionic perovskite film. The resulting high-quality CsPbI3 films with the merit of defect-immunity and large shunt resistance under low light conditions enable the corresponding PIPVs with an indoor power conversion efficiency of up to 41.2% (Pin : 334.11 µW cm-2 , Pout : 137.66 µW cm-2 ) under illumination from a commonly used indoor light-emitting diode light source (2956 K, 1062 lux). Furthermore, the device also achieves efficiencies of 29.45% (Pout : 9.80 µW cm-2 ) and 32.54% (Pout : 54.34 µW cm-2 ) at 106 (Pin : 33.84 µW cm-2 ) and 522 lux (Pin : 168.21 µW cm-2 ), respectively.

Efficient Near-Infrared Electroluminescence from Lanthanide-Doped Perovskite Quantum Cutters.

Perovskite nanocrystals (PeNCs) deliver size- and composition-tunable luminescence of high efficiency and color purity in the visible range. However, attaining efficient electroluminescence (EL) in the near-infrared (NIR) region from PeNCs is challenging, limiting their potential applications. Here we demonstrate a highly efficient NIR light-emitting diode (LED) by doping ytterbium ions into a PeNCs host (Yb3+ : PeNCs), extending the EL wavelengths toward 1000 nm, which is achieved through a direct sensitization of Yb3+ ions by the PeNC host. Efficient quantum-cutting processes enable high photoluminescence quantum yields (PLQYs) of up to 126 % from the Yb3+ : PeNCs. Through halide-composition engineering and surface passivation to improve both PLQY and charge-transport balance, we demonstrate an efficient NIR LED with a peak external quantum efficiency of 7.7 % at a central wavelength of 990 nm, representing the most efficient perovskite-based LEDs with emission wavelengths beyond 850 nm.

Robust Laminated Anode with an Ultrathin Titanium Nitride Layer for High-Efficiency Top-Emitting Organic Light-Emitting Diodes.

The effective reflective anode remains a highly desirable component for the fabrication of reliable top-emitting organic light-emitting diodes (TE-OLEDs) which have the potential to be integrated with complementary metal-oxide-semiconductor (CMOS) circuits for microdisplays. This work demonstrates a novel laminated anode consisting of a Cr/Al/Cr multilayer stack. Furthermore, we implement an ultra-thin titanium nitride (TiN) layer as a protective layer on the top of the Cr/Al/Cr composite anode, which creates a considerably reflective surface in the visible range, and meanwhile improves the chemical stability of the electrode against the atmosphere or alkali environment. Based on [2-(2-pyridinyl-N)phenyl-C](acetylacetonate)iridium(III) as green emitter and Mg/Ag as transparent cathode, our TE-OLED using the TiN-coated anode achieves the maximum current efficiency of 71.2 cd/A and the maximum power efficiency of 66.7 lm/W, which are 81% and 90% higher than those of the reference device without TiN, respectively. The good device performance shows that the Cr/Al/Cr/TiN could function as a promising reflective anode for the high-resolution microdisplays on CMOS circuits.

Over 800 nm Emission via Harvesting of Triplet Excitons in Exciplex Organic Light-Emitting Diodes.

Triplet excitons can be utilized upon introduction of phosphors into exciplexes, and such a scenario has been studied in the development of high-performance near-infrared (NIR) organic light-emitting diodes (OLEDs). To generate exciplexes in an emitting layer (EML) in the device, commercially available phosphors bis(2-phenylpyridinato-N,C2')iridium(acetylacetonate) [Ir(ppy)2acac] and iridium(III) bis(4-phenylthieno[3,2-c]pyridinato-N,C2')acetylacetonate (PO-01) were selected as donor components; in addition, a new designed fluorescent molecule, 3-([1,1':3',1″-terphenyl]-5'-yl)acenaphtho[1,2-b]quinoxaline-9,10-dicarbonitrile (AQDC-tPh), and recently reported 3-([1,1':3',1″-terphenyl]-5'-yl)acenaphtho[1,2-b]pyrazine-8,9-dicarbonitrile (APDC-tPh) were selected as acceptor components. An OLED with PO-01:AQDC-tPh blends as the EML has realized NIR emission at 750 nm and a maximum external quantum efficiency (EQE) of >0.23%. Furthermore, an OLED containing a PO-01:APDC-tPh blend realizes a maximum EQE of 0.16% at 824 nm. The high performance of these devices underlying phosphor-based exciplexes proves the potential and feasibility of our strategy for the construction of efficient NIR OLEDs.

Multi-Layer π-Stacked Molecules as Efficient Thermally Activated Delayed Fluorescence Emitters.

Multi-layer π-stacked emitters based on spatially confined donor/acceptor/donor (D/A/D) patterns have been developed to achieve high-efficiency thermally activated delayed fluorescence (TADF). In this case, dual donor moieties and a single acceptor moiety are introduced to form two three-dimensional (3D) emitters, DM-BD1 and DM-BD2, which rely on spatial charge transfer (CT). Owing to the enforced face-to-face D/A/D pattern, effective CT interactions are realized, which lead to high photoluminescence quantum yields (PLQYs) of 94.2 % and 92.8 % for the two molecules, respectively. The resulting emitters exhibit small singlet-triplet energy splitting (ΔEST ) and fast reverse intersystem crossing (RISC) processes. Maximum external quantum efficiencies (EQEs) of 28.0 % and 26.6 % were realized for devices based on DM-BD1 and DM-BD2, respectively, which are higher than those of their D/A-type analogues.

Sky-Blue Thermally Activated Delayed Fluorescence with Intramolecular Spatial Charge Transfer Based on a Dibenzothiophene Sulfone Emitter.

Intramolecular spatial charge transfer (ISCT) plays a critical role in determining the optical and charge transport properties of thermally activated delayed fluorescence (TADF) materials. Herein, a new donor/acceptor-type TADF compound based on rigid dibenzothiophene sulfone (DBTS) moiety, STF-DBTS, was designed and synthesized. Fluorene unit was used as a rigid linker to position the rigid acceptor and donor subunit in close vicinity with control over their spacing and molecular structure and to achieve high photoluminescence quantum yield (∼53%) and TADF property. For comparison purposes, we constructed the more flexible STF-DPS with a less rotationally constrained diphenylsulphone (DPS) acceptor instead of the rigid DBTS units, and STF-DPS showed no TADF properties and lower PLQY (16.0%). Organic light-emitting diodes (OLEDs) based on STF-DBTS achieve an external quantum efficiency (EQE) of 10.3% at 488 nm, which is a fivefold improvement in EQE with respect to STF-DPS.

Optimization of Low-Dimensional Components of Quasi-2D Perovskite Films for Deep-Blue Light-Emitting Diodes.

Compared to efficient green and near-infrared light-emitting diodes (LEDs), less progress has been made on deep-blue perovskite LEDs. They suffer from inefficient domain [various number of PbX6 - layers (n)] control, resulting in a series of unfavorable issues such as unstable color, multipeak profile, and poor fluorescence yield. Here, a strategy involving a delicate spacer modulation for quasi-2D perovskite films via an introduction of aromatic polyamine molecules into the perovskite precursor is reported. With low-dimensional component engineering, the n1 domain, which shows nonradiative recombination and retarded exciton transfer, is significantly suppressed. Also, the n3 domain, which represents the population of emission species, is remarkably increased. The optimized quasi-2D perovskite film presents blue emission from the n3 domain (peak at 465 nm) with a photoluminescence quantum yield (PLQY) as high as 77%. It enables the corresponding perovskite LEDs to deliver stable deep-blue emission (CIE (0.145, 0.05)) with an external quantum efficiency (EQE) of 2.6%. The findings in this work provide further understanding on the structural and emission properties of quasi-2D perovskites, which pave a new route to design deep-blue-emissive perovskite materials.

Alleviating Efficiency Roll-Off of Hybrid Single-Emitting Layer WOLED Utilizing Bipolar TADF Material as Host and Emitter.

Hybrid single-emitting layer (SEML) white organic light-emitting diodes (WOLEDs) incorporating blue thermally activated delayed fluorescent (TADF) or fluorescent materials and yellow phosphors have been widely utilized for solid-state lighting. Nonetheless, developing appropriate host materials to reduce the large efficiency roll-off at high luminance is still an unsolved issue. Here, two TADF materials denoted as TRZ-CF and TRZ-CzF were synthesized, with electroluminescent emission peaking at 476 and 460 nm, respectively. In particular, TRZ-CF, using 7,7-dimethyl-5,7-dihydroindeno[2,1- b]carbazole (CF) as donor moiety, maintained both highly efficient blue emission (EQEmax = 20.0%) and excellent charge transport abilities. The WOLED utilizing TRZ-CF as host material, doped by 0.8 wt % iridium(III) bis(4-phenylthieno[3,2- c]pyridinato- N, C2') (PO-01), has EQEmax of 20.3%, realizing the lowest roll-off to date of less than 2% at a luminance of 10 000 cd/m2. The efficiency roll-off is alleviated through the reduction the exciton quenching and triplet-triplet annihilation (TTA) within the light-emitting layer, benefited from the TADF effect and bipolar property. The hybrid SEML WOLED exhibits Commission Internationale de L'Eclairage (CIE) coordinates of (0.38, 0.45), providing a practical way to simplify the production complexity and to reduce efficiency roll-off for solid-state lighting.

High-Performance White Organic Light-Emitting Diodes with Simplified Structure Incorporating Novel Exciplex-Forming Host.

It is a challenge to engineer white organic light-emitting diodes (WOLEDs) with high efficiency, low operating voltage, good color quality, and low efficiency roll-off, simultaneously. Herein, we employ a novel exciplex to solve this problem, which mixes a bipolar host material 2,6-bis(3-(carbazol-9-yl)phenyl)pyridine (26DCzPPy) with a common electron-transporting material 4,6-bis[3,5-(dipyrid-4-yl)phenyl]-2-methylpyrimidine (B4PyMPM) to form the host for a blue emitter iridium(III)bis(4,6-(difluorophenyl)-pyridinato- N,C2') picolinate (FIrpic). The blue OLED with maximum power efficiency (PE) over 48 lm W-1 and Commission International de I'Eclairage chromaticity diagram (0.17, 0.36) was achieved. To obtain white light emission, a complementary orange emission layer is used, which consists of the bis(4-phenylth-ieno[3,2- c]pyridine)(acetylacetonate)iridium(III) (PO-01) doped into the single host of 26DCzPPy adjacent to the blue emission layer. Benefiting from the exciplex and effective utilization of the excitons by using the optimized multifunctional device structure, the WOLEDs remarkably exhibit maximum external quantum efficiency, PE, and current efficiency of 28.5%, 95.5 lm W-1, and 82.0 cd A-1, respectively. At the luminance of 100 cd m-2, it maintains the values of 27.2%, 90.2 lm W-1, and 78.4 cd A-1, respectively. Furthermore, the WOLEDs have a low threshold voltage of about 2.6 V and remain around 4.0 V at 10 000 cd m-2. These results indicate that the exciplex-forming co-host 26DCzPPy:B4PyMPM can provide an effective strategy to fabricate high-efficiency WOLEDs for potential applications.

Self-Assembled High Quality CsPbBr3 Quantum Dot Films toward Highly Efficient Light-Emitting Diodes.

Full inorganic cesium lead halide perovskites (IOPs) are regarded as attractive candidates for light-emitting diodes (LEDs) by their excellent luminescent conversion. However, unsatisfactory efficiency and stability are still the main drawbacks that hinder the commercialization progress of perovskite LEDs (PeLEDs). Here, we report an extremely uniform and flat CsPbBr3 film composing of self-assembly core-shell structured quantum dots (SCQDs) based on one-step precursor coating. The QDs size in the CsPbBr3 film is around 4.5 nm (smaller than the Bohr radius), which significantly confines injected carriers and leads to a ultrahigh exciton binding energy ( Eb) of 198 meV. In addition, unfavorable surfacial defects are dramatically passivated by a thin surfacial-capping layer composed of long-chain ammonium groups (phenylalanine bromide, PPABr), resulting in an ultralow nonradiative recombination rate. Consequently, the CsPbBr3 SCQDs film presents a high photoluminescence quantum yield (PLQY) of 85%. It enables the resulting green PeLEDs to deliver a recorded external quantum efficiency (EQE) over 15% with ideal operational stability. Furthermore, the developed CsPbBr3 SCQDs film also demonstrates promising potential in multifunctional lighting sources such as flexible and smart devices.