High Quantum Efficiency Research Articles

Enabling robust near-infrared afterglow polymers through cascade energy transfer

Near-infrared afterglow materials, which can significantly reduce background fluorescence and improve penetration in living organisms, are vital for precision imaging. However, the practicability of near-infrared afterglow materials has been hindered by their short lifetime and low luminescence quantum efficiency. Herein, we propose an effective strategy for doping water-soluble afterglow polymer host materials with fluorescent dyes, leveraging the step-by-step Förster energy transfer principle to realize near-infrared afterglow. Benefiting from the ultralong lifetime of 4.2 s and high quantum efficiency of 20.1 % for the blue host PAMCz as well as efficient cascade energy transfer efficiency of 83.3 %, the developed NIR afterglow exhibits luminescence peaked at 750 nm, a lifetime of 1.4 s, and a quantum efficiency of 17.1 %. A successful demonstration of near-infrared afterglow biological imaging with a penetration depth of 3.4 mm and signal-to-background ratio of 48.3, has been established. These advancements expand the scope of near-infrared afterglow materials by combining an ultralong lifetime with high quantum efficiency, providing a roadmap for designing robust near-infrared materials.

Enhancing Spin-Orbit Coupling in an Indolocarbazole Multiresonance Emitter by a Sulfur-Containing Peripheral Substituent for a Fast Reverse Intersystem Crossing.

A fast reverse intersystem crossing (RISC) remains an ongoing pursuit for multiresonance (MR) emitters but faces formidable challenges, particularly for indolocarbazole (ICz) derived ones. Here, heavy-atom effect is introduced first to construct ICz-MR emitter using a sulfur-containing substitute, simultaneously enhancing both spin-orbit and spin-vibronic coupling to afford a fast RISC with a rate of 1.2×105s-1, nearly one order of magnitude higher than previous maximum values. The emitter also exhibits an extremely narrow deep-blue emission peaking at 456nm with full-width at half-maxima of merely 12nm and a photoluminescence quantum yield of 92%. Benefiting from its efficient triplet upconversion capability, this emitter achieves not only a high maximum external quantum efficiency (EQE) of 31.1% in organic light-emitting diodes but also greatly alleviates efficiency roll-off, affording record-high EQEs of 29.9% at 1000cdm-2 and 18.7% at 5000cdm-2 among devices with ICz-MR emitters.

High EQE of 43.76% in solution-processed OLEDs operating at a wavelength of 626 nm

Simultaneously achieving high-efficiency, deep-red emission, and solution-processed organic light-emitting diodes (OLEDs) remains a huge challenge. In this work, a thermally activated delayed fluorescent (TADF) material of CzPXZ that exhibits aggregation-induced emission property and a deep-red phosphorescent emitter of Ir(dmppy)(piq)2(od) are developed to build effective energy transfer pathways by dissolving them in a non-polar organic solvent. The electroluminescent emission peaks of CzPXZ:Ir(III)-based OLEDs are located at deep-red 626 nm, demonstrating efficient energy transfer from CzPXZ to the Ir(III) complex. Furthermore, an optimized DPEPO hole-blocking layer is utilized in such Ir(III)-doped OLEDs to enhance the radiative recombination. Therefore, a high external quantum efficiency of 43.76% is achieved for CzPXZ:Ir(III)-based OLEDs. This work sheds light on the great potential of energy transfer from AIE-TADF to red phosphorescent emitters for high-efficiency, solution-processed, deep-red OLEDs.

In Situ Growth of MoS2 Onto Co-Based MOF Derivatives Toward High-Efficiency Quantum Dot-Sensitized Solar Cells.

Quantum dot sensitized solar cells (QDSCs) represent a promising third-generation photovoltaic technology, boasting a high theoretical efficiency of 44% and cost efficiency. However, their practical efficiency is constrained by reduced photovoltage (Voc) and fill factor (FF). One primary reason is the inefficient charge transfer and elevated recombination rates at the counter electrode (CE). In this work, a novel CE composed of a titanium mesh loaded with Co,N─C@MoS2 is introduced for the assembly of QDSCs. The incorporation of nanosized MoS2 enhances the density of catalytic sites, while the Co,N─C component ensures high conductivity and provides a substantial active surface area. Additionally, the titanium mesh's 3D structure serves as an effective electrical conduit, facilitating rapid electron transfer from the external circuit to the composite. These improvements in catalytic activity, charge transfer rate, and stability of the CE significantly enhance the photovoltaic performance of QDSCs. The optimized cells achieve a groundbreaking power conversion efficiency (PCE) of 16.39%, accompanied by a short-circuit current density (Jsc) of 27.26mA cm-2, Voc of 0.818V, and FF of 0.735. These results not only offer a new strategy for designing electrodes with high catalytic activity but also underscore the promising application of the Co,N─C@MoS2 composite in enhancing QDSC technology.

Overcoming the EQE × Li-Fi Frequency Constraint by Modulating the PbS CQDs Distribution in Perovskite Film.

Advanced photodetectors are crucial for high-fidelity optical communication. However, the tradeoff between high external quantum efficiency (EQE) and high light fidelity (Li-Fi) frequency often limits data transmission accuracy and timeliness. Here, we report a photodetector consisting of lead sulfide (PbS) colloidal quantum dots (CQDs) with near-infrared responsiveness and perovskite frameworks responsible for the charge transport to overcome the EQE × Li-Fi constraint. Optimizing the PbS CQDs distribution and trap depth in the perovskite layer enhances charge injection, achieving a device gain of 11892% for 1200 nm photons and a response frequency of 24 kHz at -2 V. The device exhibits a record EQE × Li-Fi frequency product of 106 Hz. We have applied the detector to near-infrared optical communications at a data transfer rate of 2000 bits per second (2 kbps) to demonstrate the advances in high fidelity, the device retains over 98% of the original waveform information in its output.

Fe3+-doped broadband near-infrared phosphor with high quantum efficiency toward multifunctional pc-LEDs applications

A broadband near-infrared (NIR) luminescence that is comparable to chromium ions activated materials is fulfilled in Li3Sc2(PO4)3:Fe3+ phosphor, which is highly desired for environmental and biomedical applications due to the non-toxicity of Fe3+ ions. Structural and spectral analysis reveal that the broadband NIR emission peaked at 805 nm with a full width at half-maximum of 130 nm is derived from the non-selective two-site occupation of Fe3+ in the Sc3+ sites. A high internal/external quantum efficiency of 53 %/38.7 % is achieved via relaxing the selection rule for the forbidden 4T1(4G) → 6A1(6S) transitions of Fe3+ by larger lattice distortion. The influence of Fe3+ concentration and environment temperature on the broadband NIR luminescence properties of the as-prepared phosphors are also investigated. Finally, a NIR pc-LED prototype is fabricated and its electro-optical performance has guaranteed the applications in non-destructive detection and night vision. All the results have validated Li3Sc2(PO4)3 as a novel matrix system for access to highly efficient broadband NIR Fe3+-doping phosphor materials.

Pure-Phase Perovskite Quantum Well for Green Light-Emitting Diodes.

Perovskite multiple quantum wells (MQWs) have shown great potential in the field of light-emitting diodes (LEDs). However, the random formation of QWs with varying well widths (n numbers) often leads to suboptimal interface defects and charge transport issues. Here, we reveal that the crystallization sequence of bromide-based perovskite MQWs is large-n QWs preceding small-n QWs. With this insight, we prevent the crystallization of subsequent small-n QWs by reducing the crystallization rate, ultimately resulting in the crystallization of only n = 5 QWs. This reduction in the crystallization rate is achieved through the chemical interaction of dual additives with perovskite constituents. Additionally, the chemical interaction effectively passivates the uncoordinated lead ions defects. Consequently, pure-phase perovskite QWs with a high photoluminescence quantum efficiency of 75% are achieved. The resulting green LEDs achieve a peak external quantum efficiency of 17.1% and a maximum luminance of 29,480 cd m-2, which is attractive for full-color display applications of perovskites.

Spin-Valley-Locked Electroluminescence for High-Performance Circularly Polarized Organic Light-Emitting Diodes.

Circularly polarized (CP) organic light-emitting diodes (OLEDs) have attracted attention in potential applications, including novel display and photonic technologies. However, conventional approaches cannot meet the requirements of device performance, such as high dissymmetry factor, high directionality, narrowband emission, simplified device structure, and low costs. Here, we demonstrate spin-valley-locked CP-OLEDs without chiral emitters but based on photonic spin-orbit coupling, where photons with opposite CP characteristics are emitted from different optical valleys. These spin-valley-locked OLEDs exhibit a narrowband emission of 16 nm, a high external quantum efficiency of 3.65%, a maximum luminance of near 98,000 cd/m2, and a gEL of up to 1.80, which are among the best performances of active single-crystal CP-OLEDs, achieved with a simple device structure. This strategy opens an avenue for practical applications toward three-dimensional displays and on-chip CP-OLEDs.

Enhancing Specific Detectivity and Device Stability in Vacuum-Deposited Organic Photodetectors Utilizing Nonfullerene Acceptors.

Organic photodetector (OPD) studies have undergone a revolutionary transformation by introducing nonfullerene acceptors (NFAs), which provide substantial benefits such as tunable band gaps and enhanced absorption in the visible spectrum. Vacuum-processed small-molecule-based OPD devices are presented in this study by utilizing a blend of boron subphthalocyanine (SubPc) and chlorinated subphthalocyanine (Cl6SubPc) as the active layer. Four different active layer thicknesses are further investigated to understand the intrinsic phenomena, unveiling the suppression of dark current density while maintaining photoexcitation and charge separation efficiency. Experimental results reveal that, at an applied bias of -3 V, the 50-nm-thick active layer achieves a remarkably low dark current density of 1.002 nA cm-2 alongside a high external quantum efficiency (EQE) of 52.932% and a responsivity of 0.226 A W-1. These impressive performance metrics lead to a specific detectivity of 1.263 × 1013 Jones. Furthermore, the findings offer new insights into intrinsic phenomena within the bulk heterojunction (BHJ), such as thermally generated current and exciton quenching. This integration is potentially well-heeled to revolutionize display technology by combining high-sensitivity photodetection, offering new possibilities for novel display panels with sensing applications.

High efficiency in blue TADF OLED using favorable horizontal oriented host

An appropriate host featuring a wide band gap (Eg) and high triplet energy (T1) is crucial for facilitating highly efficient blue-light emitting devices. In this study, 4Ac26CzBz, a new host comprising acridan and carbazole moieties linked to a benzimidazole core, has been synthesized and characterized. Notedly, 4Ac26CzBz exhibits a wide optical gap (Eg) and high triplet energy (T1) of 3.3 and 3.0 eV, respectively, and has been proven a suitable host for blue thermally activated delayed fluorescence (TADF) OLED. By adopting 4TCzBN as a blue-light dopant, a remarkably high device external quantum efficiency of 35.8 % (59.8 cd/A and 62.8 lm/W) and a low turn-on voltage (<3 eV) have been demonstrated, with significant suppression of the efficiency roll-off, maintaining a high efficiency of 29.7 % as luminance at 1000 cd/m2. This excellent performance is deduced from the host’s ambipolar carrier transporting properties, which refer to its ability to transport both electrons and holes effectively, high photoluminescence quantum yield (PLQY) of 98.6 %, and highly horizontal orientation of transition dipole, as determined through diverse analytical measurements. The good material properties of 4Ac26CzBz and the high OLED performance reveal its potential for the next generation’s advanced display and lighting applications.

Clar's Aromatic π-Sextet Rule for the Construction of Red Multiple Resonance Emitter.

Despite the proliferation of multiple resonance (MR) materials in the blue to green spectral ranges, red MR emitters remain scarce in the literature, an area that certainly warrants attention for future applications. Here, through a clever application of classic Clar's aromatic π-sextet rule, we triumphantly constructed the first red MR emitter by substituting the conventional benzene ring core with anthracene (fewer π-sextets). Theoretical studies indicate that the quantity of π-sextets ultimately determines the optical bandgap of a molecule, rather than the number of fused benzene rings. Benefiting from the high photoluminescence quantum yield of ~94% and horizontal dipole ratio of ~90%, the corresponding narrowband red (luminescence wavelength: 608 nm) organic light-emitting diode shows a high external quantum efficiency of 27.3%, with only a slight decrease of 3.7% at an elevated luminance level of 100,000 cd/m2.

Efficient Deep-Blue Organic Light-Emitting Diodes Employing Doublet Sensitization.

Fast and efficient exciton utilization is a crucial solution and highly desirable for achieving high-performance blue organic light-emitting diodes (OLEDs). However, the rate and efficiency of exciton utilization in traditional OLEDs, which employ fully closed-shell materials as emitters, are inevitably limited by spin statistical limitations and transition prohibition. Herein, a new sensitization strategy, namely doublet-sensitized fluorescence (DSF), is proposed to realize high-performance deep-blue electroluminescence. In the DSF-OLED, a doublet-emitting cerium(III) complex, Ce-2, is utilized as sensitizer for multi-resonance thermally activated delayed fluorescence emitter ν-DABNA. Experimental results reveal that holes and electrons predominantly recombine on Ce-2 to form doublet excitons, which subsequently transfer energy to the singlet state of ν-DABNA via exceptionally fast (over 108s-1) and efficient (≈100%) Förster resonance energy transfer for deep-blue emission. Due to the circumvention of spin-flip in the DSF mechanism, near-unit exciton utilization efficiency and remarkably short exciton residence time of 1.36µs are achieved in the proof-of-concept deep-blue DSF-OLED, which achieves a Commission Internationale de l'Eclairage coordinate of (0.13, 0.14), a high external quantum efficiency of 30.0%, and small efficiency roll-off of 14.7% at a luminance of 1000cdm-2. The DSF device exhibits significantly improved operational stability compared with unsensitized reference device.

Construction of Concentration Quenching‐Resistant Multi‐Resonance TADF Emitters via Positional Isomerization for OLEDs

AbstractMultiple resonance thermally activated delayed fluorescence (MR‐TADF) emitters are promising for high‐definition organic light‐emitting diodes (OLEDs) due to their high exciton utilization and color purity. However, strong interchromophore interactions cause most MR‐TADF emitters with planar structures to aggregate at high doping concentrations, leading to degraded efficiencies. Herein, using benzenesulfonyl‐functionalized dibenzothiophene sulfoximine with steric effects, three MR‐TADF emitters (2SBN, 3SBN, and 4SBN) are synthesized by coupling the classic DtBuCzB skeleton at different sites. Three emitters exhibit green or blue‐green emission with full width at half maximum (FWHM) values less than 29 nm and photoluminescence quantum yields exceeding 90%. OLEDs based on 2SBN, 3SBN, and 4SBN achieve high maximum external quantum efficiency (EQEmax) values of 30.1%, 27%, and 33.8%, respectively, at a 5 wt.% doping concentration. Notably, due to the distorted conformation of 4SBN and suppressed intermolecular interaction, the OLED remains high EQEmax of 28.9% at a doping concentration of 20 wt.%. These results demonstrate the feasibility of molecular design to modulate spatial conformations via positional isomerism to develop MR‐TADF emitters with reduced concentration quenching.

Room-temperature efficient and tunable interlayer exciton emissions in WS2/WSe2 heterobilayers at high generation rates.

Transition metal dichalcogenide (TMDC) heterobilayers (HBs) have been intensively investigated lately because they offer novel platforms for the exploration of interlayer excitons (IXs). However, the potentials of IXs in TMDC HBs have not been fully studied as efficient and tunable emitters for both photoluminescence (PL) and electroluminescence (EL) at room temperature (RT). Also, the efficiencies of the PL and EL of IXs have not been carefully quantified. In this work, we demonstrate that IX in WS2/WSe2 HBs could serve as promising emitters at high generation rates due to its immunity to efficiency roll-off. Furthermore, by applying gate voltages to balance the electron and hole concentrations and to reinforce the built-in electric fields, high PL quantum yield (QY) and EL external quantum efficiency (EQE) of ∼0.48% and ∼0.11% were achieved at RT, respectively, with generation rates exceeding 1021 cm-2·s-1, which confirms the capabilities of IXs as efficient NIR light emitters by surpassing most of the intralayer emissions from TMDCs.

Dual‐Core Engineering for Efficient Deep‐Blue Multiple Resonance Thermally Activated Delayed Fluorescent Materials

AbstractDeveloping narrowband blue multiple resonance (MR) organic emitters with Commission Internationale de L'Eclairage (CIE) y coordinates &lt;0.1 is essential for advanced display technologies. This study proposes a deep‐blue thermally activated delayed fluorescence (TADF) emitter, named 2BNO, which integrates two independent MR cores. Unlike many TADF materials with single‐bonded dual emitting cores, 2BNO utilizes a steric hindrance‐assisted fluorene bridge to achieve an orthorhombic molecular structure. The dual‐core MR‐TADF emitter shows enhanced light absorption and a high photoluminescence quantum yield. Notably, the emission of 2BNO is not significantly redshifted compared to single‐core compounds and maintains a narrow full width at half‐maximum (FWHM) of 24 nm with CIE coordinates of (0.147, 0.041) in 2Me‐THF solution, nearing the BT.2020 blue standard. Organic light‐emitting diodes (OLEDs) incorporating 2BNO as the emitter exhibit deep‐blue emission at 460 nm with a narrow FWHM of 29 nm and CIE coordinates of (0.14, 0.09). The dual emitting core design significantly improves device efficiency, achieving a high external quantum efficiency (EQE) of 19.8%. The dual‐core molecular design strategy in this work is demonstrated to be effective in promoting the efficiency of the TADF emitters while preserving deep‐blue color purity.

Efficient and Near-Zero Thermal Quenching Cr3+-Doped Garnet-Type Phosphor for High-Performance Near-Infrared Light-Emitting Diode Applications.

In recent years, near-infrared (NIR) phosphors have attracted great research interest due to their unique physical properties and broad application prospects. However, obtaining NIR phosphors with both high quantum efficiency and excellent thermal stability remains a great challenge. In this study, novel NIR Ca3Mg2ZrGe3O12:Cr3+ phosphors were successfully prepared using a high-temperature solid-phase method, and the structure and luminescent properties of the material were systematically investigated. Ca3Mg2ZrGe3O12:0.01Cr3+ emits NIR light in the range of 600 to 900 nm with a peak at 758 nm and a half-height width of 89 nm under the excitation of 457 nm blue light. NIR luminescence shows considerable quantum efficiency, and the internal quantum efficiency of the optimized sample is up to 68.7%. Remarkably, the Ca3Mg2ZrGe3O12:0.01Cr3+ phosphor exhibits a near-zero thermal quenching behavior, and the luminescence intensity of the sample at 250 °C maintains 92% of its intensity at room temperature. The mechanism of high thermal stability has been elucidated by calculating the Huang Kun factor and activation energy. Finally, NIR pc-LED devices prepared from Ca3Mg2ZrGe3O12:0.01Cr3+ phosphor with commercial blue LED chips have good performance, proving that this Ca3Mg2ZrGe3O12:0.01Cr3+ NIR phosphor has potential applications in night vision and biomedical imaging.

Multiple Enol-Keto Isomerization and Excited-State Unidirectional Intramolecular Proton Transfer Generate Intense, Narrowband Red OLEDs.

A novel series of excited-state intramolecular proton transfer (ESIPT) emitters, namely, DPNA, DPNA-F, and DPNA-tBu, endowed with dual intramolecular hydrogen bonds, were designed and synthesized. In the condensed phase, DPNAs exhibit unmatched absorption and emission spectral features, where the minor 0-0 absorption peak becomes a major one in the emission. Detailed spectroscopic and dynamic approaches conclude fast ground-state equilibrium among enol-enol (EE), enol-keto (EK), and keto-keto (KK) isomers. The equilibrium ratio can be fine-tuned by varying the substitutions in DPNAs. Independent of isomers and excitation wavelength, ultrafast ESIPT takes place for all DPNAs, giving solely KK tautomer emission maximized at >650 nm. The spectral temporal evolution of ESIPT was resolved by a state-of-the-art technique, namely, the transient grating photoluminescence (TGPL), where the rate of EK* → KK* is measured to be (157 fs)-1 for DPNA-tBu, while a stepwise process is resolved for EE* → EK* → KK*, with a rate of EE* → EK* of (72 fs)-1. For all DPNAs, the KK tautomer emission shows a narrowband emission with high photoluminescence quantum yields (PLQY, ∼62% for DPNA in toluene) in the red, offering advantages to fabricate deep-red organic light-emitting diodes (OLED). The resulting OLEDs give high external quantum efficiency with a spectral full width at half-maximum (FWHM) as narrow as ∼40 nm centered at 666-670 nm for DPNAs, fully satisfying the BT. 2020 standard. The unique ESIPT properties and highly intense tautomer emission with a small fwhm thus establish a benchmark for reaching red narrowband organic electroluminescence.

Enhanced forward emission by backside mirror design in micron-sized LEDs.

Tiny InGaN micro-LEDs (μ-LEDs) play a pivotal role in emerging display technologies, particularly augmented reality (AR) applications. Achieving both high internal quantum efficiency (IQE) and efficient light extraction efficiency (LEE) is essential. While wet chemical etching can recover the IQE after dry etching, it alters the pixel shape, impacting optical properties and reducing the LEE. In this study, we overcome this issue by fabricating 1 μm thin-film-based μ-LED emitter arrays with a metallic backside mirror deposited on a patterned dielectric material around the μ-LED mesa. This concave mirror can be straightforwardly integrated into a thin-film LED process chain, and it redirects photons within the μ-LED structure, enhancing the LEE in the forward direction. Electro-optical measurements show a 2.1-fold improvement in light output within the ±15∘ emission cone compared to μ-LEDs with vertical sidewalls. These findings hold significant implications for μ-LED projection displays, where maximizing the overall efficiency and directionality is critical.

Thermally Activated Delayed Fluorescence and Beyond. Photophysics and Material Design Strategies.

This review focuses on thermally activated delayed fluorescence (TADF). Photophysical properties of Cu(I) complexes and unique organic molecules are addressed. Investigations, based on temperature‐dependent emission studies, micro‐ to femto‐second time‐resolved spectroscopy investigations, quantum mechanical considerations, state‐of‐art calculations, and organic light‐emitting diodes (OLED) device studies, address exciton harvesting mechanisms and photophysical impact of the energy gap ΔE(S1–T1) and spin‐orbit coupling (SOC). We disclose relationship between (i) ΔE(S1–T1) and transition rate k(S1–S0); (ii) SOC, phosphorescence, and intersystem crossing (ISC); (iii) internal/external rigidity, luminescence quantum yield, excitation self‐trapping, and concentration quenching; (iv) environment polarity and state energy tuning, as well as (v) SOC and combined ambient‐temperature TADF/phosphorescence, zero‐field splitting, and spin‐lattice relaxation (at T = 1.2 K). These studies guide us to milestone Cu(I) complexes. Moreover, we demonstrate that fast ISC in organic molecules requires state mixing with an additional, energetically close triplet state. Thus, a guide structure for unique organic TADF molecules with ultra‐fast ISC and reverse‐ISC rates (&gt;109 s−1) combined with ΔE(S1–T1)&lt;10 cm−1 (&lt;1 meV) is presented allowing for ultra‐fast singlet‐triplet equilibrated fluorescence with sub‐microsecond decay. First OLEDs fabricated show high external quantum efficiency of ≈19%. Based on this breakthrough material class, a new exciton harvesting mechanism, the direct singlet harvesting (DSH), is presented.

Efficient and Stable Red Perovskite Light-Emitting Diodes via Thermodynamic Crystallization Control.

Efficient and stable red perovskite light-emitting diodes (PeLEDs) demonstrate promising potential in high-definition displays and biomedical applications. Although significant progress has been made in device performance, meeting commercial demands remains a challenge in the aspects of long-term stability and high external quantum efficiency (EQE). Here, an in situ crystallization regulation strategy is developed for optimizing red perovskite films through ingenious vapor design. Mixed vapor containing dimethyl sulfoxide and carbon disulfide (CS2) is incorporated to conventional annealing, which contributes to thermodynamics dominated perovskite crystallization for well-aligned cascade phase arrangement. Additionally, the perovskite surface defect density is minimized by the CS2 molecule adsorption. Consequently, the target perovskite films exhibit smooth exciton energy transfer, reduced defect density, and blocked ion migration pathways. Leveraging these advantages, spectrally stable red PeLEDs are obtained featuring emission at 668, 656, and 648nm, which yield record peak EQEs of 30.08%, 32.14%, and 29.04%, along with prolonged half-lifetimes of 47.7, 60.0, and 43.7h at the initial luminances of 140, 250, and 270cd m-2, respectively. This work provides a universal strategy for optimizing perovskite crystallization and represents a significant stride toward the commercialization of red PeLEDs.