Low Efficiency Roll-off Research Articles

High-Performance perovskite quantum dots light-emitting diodes with hole transport layer engineering and synergetic outcoupling enhancement

Perovskite quantum dot light-emitting diodes (PeQLEDs) are frequently considered as the most promising alternatives to organic light-emitting diodes (OLEDs). However, the efficiency of PeQLEDs remains inferior to OLEDs due to suboptimal charge carrier transport and intrinsic light outcoupling efficiency (ηout). Herein, a combination of hole transport layer (HTL) engineering and substrate engineering is demonstrated to improve the charge injection and ηout of PeQLEDs. To replace the conventional PEDOT:PSS, a novel HTL bilayer based on modified PEDOT:PSS and PVK with a lower refractive index and fewer trap densities at the HTL-QDs interface is developed. Additionally, this study identifies the ideal thickness of ITO for achieving optimal ηout of PeQLEDs through optical simulations and experimental validation. Based on the synergistic use of HTL bilayer and 70-nm-thick ITO, the PeQLEDs achieved an optimal external quantum efficiency of 17.96 % at a luminance of 1763 cd/m2 and 15.19 % at 8300 cd/m2 without using any external outcoupling structure, indicating a low efficiency roll-off.

Lattice reconstruction for mixed-halide blue perovskite light-emitting diodes with high brightness, outstanding color stability and low efficiency roll-off

We report a simple, effective, and universal lattice reconstruction approach to improve the quality of perovskite films by using nonpolar solvents with high Gutmann donor numbers (DNs). We find that high-DN nonpolar solvents, for instance, ethyl acetate, can interact with perovskite precursors. Such a solvent can make the perovskite lattice more ordered and “harder” and promote the formation of heterostructures with low-dimensional perovskite impurities and residual solvent molecules. As a result, the lattice-reconstructed perovskite films exhibit reduced defect densities and suppressed ion migration. The resultant mixed-halide blue perovskite light-emitting diodes (PeLEDs) show greatly enhanced tolerance to high driving current densities and voltages, demonstrating high brightness, outstanding color stability and low efficiency roll-off. Our work provides a deep understanding of the interactions between nonpolar solvents and perovskites and offers useful guidelines for further development of high-power PeLEDs.

Molecular Engineering Towards Efficient Aggregation-Induced Delayed Fluorescence Luminogens as Emitters and Sensitizers for High-Performance Organic Light-Emitting Diodes.

Exploring efficient thermally-activated delayed fluorescence materials having maximum external quantum efficiencies (ηext,maxs) exceeding 30 % for organic light-emitting diodes (OLEDs) still remains challenging because it generally requires efficient reverse intersystem crossing (RISC), high photoluminescence quantum yield (ΦPL), and large optical out-coupling efficiency (Φout) simultaneously. Herein, two green aggregation-induced delayed fluorescence (AIDF) luminogens, named XTCz-2 and XTCz-3, are designed and constructed by using xanthone (XT) as electron acceptor and phenylcarbazole-substituted carbazole as donors. XTCz-2 and XTCz-3 exhibit distinguished advantages of high thermal stability (439-560 °C), excellent ΦPLs (84-88 %) and fast RISC rates (1.9×105-4.2×105 s-1), and prefer horizontal dipole orientation and thus have high Φouts. Consequently, they can achieve the state-of-the-art electroluminescence (EL) performances with ηext,maxs of up to 35.0 %. Moreover, XTCz-3 is selected as a sensitizer for sky-blue multi-resonance delayed fluorescence emitter in hyperfluorescence OLEDs, providing narrow EL spectra and excellent ηext,maxs of up to 33.8 % with low efficiency roll-offs. The splendid comprehensive performances demonstrate the significant application potential of these AIDF luminogens as both light-emitting materials and sensitizers for OLEDs.

Crafting host materials for narrowband blue OLEDs with low efficiency roll-off by the medium-ring strategy

Crafting host materials for narrowband blue OLEDs with low efficiency roll-off by the medium-ring strategy

Conformational Isomerization Promotes Balanced Ambipolar Transport for Efficient Narrowband Near-Ultraviolet Fluorophore and Non-doped Device with Low Efficiency Roll-Off

Conformational Isomerization Promotes Balanced Ambipolar Transport for Efficient Narrowband Near-Ultraviolet Fluorophore and Non-doped Device with Low Efficiency Roll-Off

Novel bipolar host materials based on benzimidazole-hybridized phenanthridine for efficient red PhOLEDs

In this work, two innovative bipolar host materials, TPA-BIP and Cz-BIP, were designed and synthesized based on benzimidazole-hybridized phenanthridine (BIP) moiety as the electron transport unit. Compared to the widely used electronic transport unit benzimidazole, the BIP unit possesses a large planar rigid structure that can effectively enhance the thermal stability and the electron transfer capability of materials. Both materials exhibit good thermal stability respectively with Tg of 113 °C and 141 °C, proper HOMO/LUMO energy levels, and balance carrier transport capabilities. The red phosphorescent organic light-emitting diode prepared based on both materials achieve relatively high luminescence efficiency and relatively low efficiency roll-off. In particular, the EQEmax of the R1 device using TPA-BIP as the host material reaches 21.5 %, which is more superior than that of the conventional host material CBP (EQEmax of 9.84 %). Even at 1000 cd/m2, the device still achieves an EQE of 21.3 % with virtually no decrease. In conclusion, the results demonstrate the broad development potential of these BIP-based host materials for red PhOLEDs applications.

Application of carbazole derivatives as a multifunctional material for organic light-emitting devices

The object of research is newly synthesized carbazole-derived compounds and organic light-emitting structures based on them. The problem lies in the complex solution of scientific and technical problems of improving the characteristics and stability of organic light-emitting diodes (OLEDs), namely improving the brightness and energy-efficient parameters. Organic light-emitting structures of blue, blue, and green radiation with color coordinates were formed by the thermovacuum sputtering method and the solution deposition method. The turn-on voltage of the white OLED is 6 V, the maximum brightness of the light-emitting structures was 10,000 cd/m2. The devices demonstrated a sufficiently high external quantum efficiency of 5 % to 7 %. This paper reports the multifunctional application of a simple donor-acceptor organic compound, as active and host material in the emission layer of organic light emitting devices. Em1 has been used as active components in OLEDs, where Em1 is the guest emitter (Device A), the acceptor part of the excited emitter (Device B) and the host matrix of the CdSeS/ZnS alloy quantum dot. At least four different OLEDs have been designed and characterized where Em1 plays the role of the guest emitter (Device C). The external quantum efficiencies of devices A–C are characterized by values common to pure fluorescent OLEDs (up to 5 % of the theoretical limit), but these devices sustain low-efficiency roll-off of electroluminescence over a wide range of current densities. Organic light-emitting diodes based on carbazole-derived compounds, due to their color characteristics, are promising candidates for use in the latest lighting systems. A separate advantage of the data light-emitting structures is a multifunctional application of one compound for different types of light-emitting structures. In addition, organic LEDs on based on carbazole-derived compounds have low energy consumption and are environmentally friendly due to the absence of toxic substances in their architecture, which creates prerequisites for saving energy resources and reducing the industrial burden on the environment.

Effective donor and acceptor modifications of carbazole-benzonitrile thermally activated delayed fluorescence molecules enabling high-performance OLEDs

Carbazole-benzonitrile derivatives (CzBNs) have great potential to enable thermally activated delayed fluorescence (TADF) molecules with both high efficiency and good stability simultaneously. However, the device performances of most CzBN-based organic light-emitting diodes (OLEDs) still lag behind other types of TADF molecules. In this work, we proposed a design strategy to construct efficient CzBN-TADF molecules through acceptor and donor modifications. The cyano-modified acceptor enables the extension of the lowest unoccupied molecular orbital while mostly preserving the overlapped area with the highest occupied molecular orbital. The optimized distributions of frontier molecular orbitals contribute to tiny singlet-triplet energy gaps while maintaining a high radiative decay rate. The incorporation of tert-butyl units in the donor groups further enhances the TADF property of resulted tPCNBN molecule due to suppressed non-radiative decay and reduced exciton self-quenching. Accordingly, OLEDs based on tPCNBN present the best device performances, such as a maximum external quantum efficiency of 33.1 % at 400 cd m−2, which is still as high as 26.3 % at a high luminance of 4000 cd m−2, demonstrating relatively low efficiency roll-off. These results confirm the effectiveness of the proposed design strategy in developing efficient and stable CzBN-TADF materials and devices.

Application of the Heavy-Atom Effect for (Sub)microsecond Thermally Activated Delayed Fluorescence and an All-Organic Light-Emitting Device with Low-Efficiency Roll-off.

The feature of abundant and environmentally friendly heavy atoms (HAs) like bromine to accelerate spin-forbidden transitions in organic molecules has been known for years. In combination with the easiness of incorporation, bromine derivatives of organic emitters showing thermally activated delayed fluorescence (TADF) emerge as a cheap and efficient solution for the slow reverse intersystem crossing (rISC) problem in such emitters and strong efficiency roll-off of all-organic light-emitting diodes (OLEDs). Here, we present a comprehensive photophysical study of a tri-PXZ-TRZ emitter reported previously and its hexabromo derivative showing a remarkable enhancement of rISC of up to 9 times and a short lifetime of delayed fluorescence of 2 μs. Analysis of the key molecular vibrations and TADF mechanism indicates almost compete blockage of the spin-flip transition between the charge-transfer states of different multiplicity 3CT → 1CT. In such a case, rISC as well as its enhancement by the HA is realized via the 3LE → 1CT transition, where 3LE is the triplet state localized on the same brominated phenoxazine donor involved in the formation of the 1CT state. Interestingly, the spin-orbit coupling (SOC) with two other 3LE states is negligible because they are localized on different donors and not involved in 1CT. We consider this as an example of an additional "localization" criterion that completes the well-known El Sayed rule on the different nature of states for nonzero SOC. The applicative potential of such a hexabromo emitter is tested in a "hyperfluorescent" system containing a red fluorescent dopant (tetraphenyldibenzoperiflanthene, DBP) as an acceptor of Förster resonance energy transfer, affording a narrow-band red-emitting system, with most of the emission in the submicrosecond domain. In fact, the fabricated red OLED devices show remarkable improvement of efficiency roll-off from 2-4 times depending on the luminance, mostly because of the increase of the rISC constant rate and the decrease of the overall delayed fluorescence lifetime thanks to the HA effect.

High-Efficiency Asymmetric TADF Dendrimers via Promoting Mixing of Multiple Excited States toward Solution-Processed OLEDs with Low Efficiency Rolloff

High-Efficiency Asymmetric TADF Dendrimers via Promoting Mixing of Multiple Excited States toward Solution-Processed OLEDs with Low Efficiency Rolloff

Homogeneous mono-layer mixed-halide perovskite quantum dots towards blue light-emitting diodes with stable spectra under continuous driving

Mixed-halide perovskite quantum dots (QDs) light-emitting diodes (QLEDs) with blue emission still suffer from low efficiency due to surface defects and halide migration. The issue of halide migration in the mixed-halide perovskite QLEDs under increasing biases have been basically solved. However, under continuous driving, the QLEDs still face the problem of halide migration or electroluminescence (EL) peak shift. In this work, we found that when ligand passivation effects on mixed-halide perovskite QDs are similar, the homogeneity of a mono-layer QDs film plays a decisive role in suppressing halide migration and improving the EL spectral stability of the QLEDs under continuous driving. Moreover, 4 and 64 mm2 QLEDs with emission peaks from pure-blue to deep-blue and low efficiency roll-off were fabricated and the analysis results show that factors, such as chlorine content or defects in the QDs, driving bias, operation time at the driving bias and current density, also matter in the EL spectral stability of the QLEDs. In addition, we found that the devices exhibit similar performance after being stored for a year, demonstrating high stability of the devices with homogeneous mono-layer QDs structure. Our work provides a timely and systematic guide on achieving spectrally stable and efficient blue QLEDs with high color purity based on mixed-halide perovskite QDs.

High-Performance All-Inorganic Architecture Perovskite Light-Emitting Diodes Based on Tens-of-Nanometers-Sized CsPbBr3 Emitters in a Carrier-Confined Heterostructure.

Developing green perovskite light-emitting diodes (PeLEDs) with a high external quantum efficiency (EQE) and low efficiency roll-off at high brightness remains a critical challenge. Nanostructured emitter-based devices have shown high efficiency but restricted ascending luminance at high current densities, while devices based on large-sized crystals exhibit low efficiency roll-off but face great challenges to high efficiency. Herein, we develop an all-inorganic device architecture combined with utilizing tens-of-nanometers-sized CsPbBr3 (TNS-CsPbBr3) emitters in a carrier-confined heterostructure to realize green PeLEDs that exhibit high EQEs and low efficiency roll-off. A typical type-I heterojunction containing TNS-CsPbBr3 crystals and wide-bandgap Cs4PbBr6 within a grain is formed by carefully controlling the precursor ratio. These heterostructured TNS-CsPbBr3 emitters simultaneously enhance carrier confinement and retain low Auger recombination under a large injected carrier density. Benefiting from a simple device architecture consisting of an emissive layer and an oxide electron-transporting layer, the PeLEDs exhibit a sub-bandgap turn-on voltage of 2.0 V and steeply rising luminance. In consequence, we achieved green PeLEDs demonstrating a peak EQE of 17.0% at the brightness of 36,000 cd m-2, and the EQE remained at 15.7% and 12.6% at the brightness of 100,000 and 200,000 cd m-2, respectively. In addition, our results underscore the role of interface degradation during device operation as a factor in device failure.

Enhancing Reverse Intersystem Crossing in Triptycene-TADF Emitters: Theoretical Insights into Reorganization Energy and Heavy Atom Effects.

Thermally activated delayed fluorescence (TADF) emitters based on the triptycene skeleton demonstrate exceptional performance, superior stability, and low efficiency roll-off. Understanding the interplay between the luminescent properties of triptycene-TADF molecules and their assembly environments, along with their excited-state characteristics, necessitates a comprehensive theoretical exploration. Herein, we predict the photophysical properties of triptycene-TADF molecules in a thin film environment using the quantum mechanics/molecular mechanics method and quantify their substantial dependency on the heavy atom effects and reorganization energies using the Marcus-Levich theory. Our calculated photophysical properties for two recently reported molecules closely align with experimental values. We design three novel triptycene-TADF molecules by incorporating chalcogen elements (O, S, and Se) to modify the acceptor units. These newly designed molecules exhibit reduced reorganization energies and enhanced reverse intersystem crossing (RISC) rates. The heavy atom effect amplifies spin-orbit coupling, thereby facilitating the RISC process, particularly at a remarkably high rate of ∼109 s-1.

Spirobifluorene-fused strategy enables pure-green multiple resonance emitters with low efficiency roll-off.

Herein, we present a molecular design strategy centered on the spiroannulation of the MR-core skeleton to fabricate green MR-emitters and reduce device efficiency roll-off. Fusing 9,9'-spirobifluorene into the central framework of MR-emitters facilitates the distribution of the highest occupied molecular orbital (HOMO) across the spiro units, leading to a red-shifted emission and giving rise to a pure-green MR-emitter (DPhCz-SFBN) with the Commission Internationale de l'Eclairage (CIE) coordinates of [0.16, 0.74] in toluene solution, closely matching the BT.2020 standard for green. Additionally, the resultant highly twisted hetero[6]helicene conformation and a nearly perpendicular conformation of spirocycle structure effectively minimize close π-π stacking interactions among the MR-emitting cores, thereby reducing exciton quenching. Consequently, organic light-emitting diodes (OLEDs) based on DPhCz-SFBN exhibit a high maximum quantum efficiency (EQEmax) of 32.8% with low efficiency roll-off, maintaining an EQE of 23.2% at a practical luminance level of 5000 cd m-2.

Spirobifluorene-based hole-transporting materials for RGB OLEDs with high efficiency and low efficiency roll-off.

In this work, we designed and synthesized three spirobifluorene (SBF)-based hole-transporting materials (HTMs) by incorporating the di-4-tolylamino group at different positions of the SBF skeleton. These materials demonstrate excellent thermal stability with thermal decomposition temperatures (T d) up to 506 °C and outstanding morphological stability with a glass transition temperature (T g) exceeding 145 °C. The meta-linkage mode between the conjugated skeleton and functional groups in the molecular structure results in electronic decoupling, giving these 3,6-substituted SBFs higher triplet energies (E T) compared to 2,7-substituted SBFs. This makes the 3,6-substituted SBFs suitable as universal HTMs for red, green, and blue (RGB) organic light emitting diodes (OLEDs). Among the three HTMs, 3,3',6,6'-tetra(N,N-ditolylamino)-9,9'-spirobifluorene (3,3',6,6'-TDTA-SBF) exhibits the best device performance, achieving maximum external quantum efficiencies (EQEmax) of 26.1%, 26.4%, and 25.4% for RGB phosphorescent OLEDs, with extremely low efficiency roll-off in both green and blue devices. Utilizing 3,3',6,6'-TDTA-SBF as the HTM, we have also fabricated narrowband blue OLEDs based on the widely used multiple resonance emitter BCz-BN, which exhibits a EQEmax of 29.8% and low efficiency roll-off.

High-performance deep-blue electroluminescence from multi-resonance TADF emitters with a spirofluorene-fused double boron framework.

The development of multi-resonance thermally activated delayed fluorescence (MR-TADF) materials in the deep-blue region is highly desirable. A usual approach involves constructing an extended MR-TADF framework; however, it may also intensify aggregate-caused quenching issues and thereby reduce device efficiency. In this study, we develop a molecular design strategy that fuses the MR-TADF skeleton with 9,9'-spirobifluorene (SF) units to create advanced deep-blue emitters. The SF moiety facilitates high-yield one-shot bora-Friedel-Crafts reaction towards an extended skeleton and mitigates interchromophore interactions as a steric group. Our findings reveal that orbital interactions at the fusion site significantly influence the electronic structure, and optimizing the fusion mode allows for the development of emitters with extended conjugation length while maintaining non-bonding character. The proof-of-concept emitter exhibits narrowband emission in the deep-blue region, a near-unity photoluminescence quantum yield, and a fast k RISC of 2.4 × 105 s-1. These exceptional properties enable the corresponding sensitizer-free OLED to achieve a maximum external quantum efficiency (EQEmax) of 39.0% and Commission Internationale de l'Eclairage (CIE) coordinates of (0.13, 0.09). Furthermore, the hyperfluorescence device realizes an EQEmax of 40.4% with very low efficiency roll-off.

Utilizing Spiro-Type Backbone Donor to Develop Exciplex Emitter and Highly Efficient Phosphorescent OLEDs With Low Efficiency Roll-Off

Utilizing Spiro-Type Backbone Donor to Develop Exciplex Emitter and Highly Efficient Phosphorescent OLEDs With Low Efficiency Roll-Off

Intramolecular exciplex featuring a bis-sp3 C-locked acceptor-donor-acceptor sandwich.

Intramolecular exciplex systems featuring thermally activated delayed fluorescence (TADF) have garnered significant attention in the realm of organic light-emitting diodes (OLEDs). Nonetheless, the occurrence of organic sandwich intramolecular exciplexes remains rare due to structural limitations and synthetic challenges. Herein, we present a novel rigid acceptor-donor-acceptor (A-D-A) sandwich complex, dSFQP, characterized by two sp3 C-locking moieties. This compound exhibits TADF characteristics facilitated by a multiple through-space charge-transfer process. X-ray crystallographic analysis confirms the distinctive sandwich configuration. The parallel spatial arrangement and minimized A-D-A configuration enhance electronic interactions, resulting in a high photoluminescence quantum yield, rapid reverse intersystem crossing rate, and sluggish nonradiative decay rate. OLEDs employing dSFQP as the dopant achieve a maximum external quantum efficiency (EQE) of 28.5% with a low efficiency roll-off of merely 2.8% at 1000 cd m-2. Even at a high brightness of 10 000 cd m-2, the EQE remains notably high at 17.5%. Our current results provide an effective way to further innovate the design of new organic charge-transfer complexes.

A high-performance hyperfluorescent device through host optimization

The unsatisfied feature in the operating lifetime and efficiency has hindered the wide application of hyperfluorescent organic light emitting diodes (OLEDs). In order to achieve high efficiency and long lifetime, it is necessary to ensure the stability of the emitting layer (EML) while maintaining high exciton utilization. However, this faces enormous challenges. Our research reveals the impact of host characteristics on the efficiency and lifetime, in a typical hyperfluorescent system. The experimental results show that the carrier mobility and triplet states (T1) of host seriously affect device performance. Strategically adjusting exciton recombination through host selection, can help achieve an efficient and stable device. In addition, the stability of assistant layers adjacent to EML, also has influence on the lifetime of the devices. On this basis, a high-performance green hyperfluorecent device was fabricated, with a maximum efficiency of 227.7 cd A−1. The LT95 (brightness attenuation to 95%) lifetime of such device achieved to 410 h with an initial brightness of 31338 cd m−2, creating a new record. The performance of this hyperfluoresent OLED has reached the same level as the latest generation of commercial phosphorescent devices. More than that, the color of CIE-1931 (0.205, 0.757) of the device well meets the requirement of Adobe standard for green. In addition, a low efficiency roll-off of 1.07%, from maximum efficiency to efficiency at 10 mA cm−2, was observed, which helped to reduce the power consumption of OLED high gray display.The purposeful adjustment of the position and width of exciton recombination region by a well-chosen host, is considered the main reason for achieving such excellent performance. This study systematically reveals the influence of host on OLEDs based on thermally activated delayed fluorescence (TADF), and shows a great possibility of the technology in practical application.

Regulating excited states by varying different acceptors of D-π-A emitters for efficient non-doped blue electroluminescence with high luminance and low efficiency roll-off.

Chromophores with hybridized local and charge-transfer (HLCT) excited state are promising for the realization of high performance blue organic light-emitting diodes (OLEDs). The rational manipulation of HLCT excited state for efficient emitters remains challenging. Herein, we present three donor-π-acceptor (D-π-A) molecules (mPAN, mPANPH, and mPNAPH) with phenanthro[9,10-d]imidazole (PI) and pyridinyl as donor and π-bridge respectively. Changes in various kinds of polycyclic aromatic derivative acceptors (anthracene, 9-phenylanthracene, and 1-phenylnaphthalene) could manipulate the excited states and optoelectronic properties. Theoretical calculations reveal that the S1 state of mPNAPH exhibits HLCT nature while the other two molecules show local excited (LE) state dominated feature. The photophysical properties also demonstrate this characteristic. Therefore, compared with mPAN and mPANPH, mPNAPH has higher photoluminescence quantum yield (PLQY) whether in solutions or neat films.Ultimately, the non-doped devices based on these emitters show high luminance larger than 35000 cd m-2, and high maximum external quantum efficiencies (EQEmaxs) larger than 5% with low efficiency roll-off. In particular, the mPNAPH-based device displays an excellent performance of pure blue emission at 456 nm with Commission Internationale de L'Eclairage coordinate of (0.15, 0.16) and EQEmax of 6.13% that benefited from the HLCT state and high-lying reverse intersystem crossing process.