Modified t-butyl in tetradentate platinum (II) complexes enables exceptional lifetime for blue-phosphorescent organic light-emitting diodes.

In blue phosphorescent dopants, the tetradentate platinum(II) complex is a promising material showing high efficiency and stability in devices. However, metal-metal-to-ligand charge transfer (MMLCT) formation leads to low photo-luminescence quantum yields (PLQYs), wide spectra, and intermolecular interaction. To suppress MMLCT, PtON-tb-TTB and PtON-tb-DTB are designed using theoretical simulation by modifying t-butyl in PtON-TBBI. Both materials effectively suppress MMLCT and exhibit high PLQYs of 99% and 78% in 5 wt% doped film, respectively. The PtON-tb-TTB and PtON-tb-DTB devices have maximum external quantum efficiencies of 26.3% and 20.9%, respectively. Additionally, the PtON-tb-DTB device has an extended lifetime of 169.3 h with an initial luminescence of 1200 nit, which is 8.5 times greater than the PtON-TBBI device. Extended lifetime because of suppressed MMLCT and smaller displacement between the lowest triplet and triplet metal-centered states compared to other dopants. The study provides an effective approach to designing platinum(II) complexes for long device lifetimes.

Structural Optimization of BODIPY Derivatives: Achieving Stable and Long-Lived Green Emission in Hyperfluorescent OLEDs.

Boron dipyrromethene (BODIPY) derivatives are widely studied as terminal emitters in organic light-emitting diodes (OLED) due to their narrow emission and high photoluminescence quantum yield (PLQY). However, the strategy for precisely tuning their emission toward a high color purity is still challenging. Herein, we developed a new design strategy to regulate the emission of BODIPY derivatives by modifying the electronic and steric dominance using functionalities, such as nitrile, pentafluorophenyl, diethyl, and monobenzyl. These rational modifications yielded a series of four novel green BODIPY emitters, namely, tPN-BODIPY, tPPP-BODIPY, tPBn-BODIPY, and tPEN-BODIPY, each benefited with a tuned emissions range of 517 to 542 nm with a narrow fwhm of 25 nm and high photoluminescence quantum yield up to 96%. Among these synthesized BODIPYs, an unsymmetrical tPBn-BODIPY was chosen as a final dopant (FD) to explore its application in OLED devices. The fabricated TADF sensitized fluorescence-OLED (TSF-OLED) exhibits a narrow band pure green emission at 531 nm with corresponding CIE coordinates of (x, y) = (0.27, 0.68) and a maximum external quantum efficiency (EQE) of 20%. Furthermore, the TSF-OLED displayed an exceptionally prolonged device operational lifetime (LT90) of 210 h at an initial luminescence of 3000 cd m-2.

High light extraction performance using evanescent waves for top emission OLED applications with thin film encapsulation.

We report high light extraction from the top emission OLED (TEOLED) device structure by improving mainly the waveguide mode loss in the atomic layer deposition processed thin film encapsulation (TFE) layer. A novel structure incorporating the light extraction concept using evanescent waves and the hermetic encapsulation of a TEOLED device is presented here. When the TEOLED device is fabricated using the TFE layer, a substantial amount of generated light is trapped inside the device due to the difference in refractive index (RI) between the capping layer (CPL) and the aluminum oxide (Al2O3) layer. By inserting a low RI layer at the interface between the CPL and Al2O3, the direction of the internal reflected light is changed by the evanescent waves. The high light extraction with the low RI layer is attributed to the presence of evanescent waves and an electric field in the low RI layer. The novel fabricated TFE structure, CPL/ low RI layer/ Al2O3/ polymer/ Al2O3, is reported here. The current efficiency of the fabricated blue TEOLED device using this low RI layer is improved by about 23% and the blue index value is enhanced by about 26%. This new approach for light extraction will be applicable to future encapsulation technology for flexible optoelectronic devices.

Forthcoming hyperfluorescence display technology: relevant factors to achieve high-performance stable organic light emitting diodes.

Over the decade, there have been developments in purely organic thermally activated delayed fluorescent (TADF) materials for organic light-emitting diodes (OLEDs). However, achieving narrow full width at half maximum (FWHM) and high external quantum efficiency (EQE) is crucial for real display industries. To overcome these hurdles, hyperfluorescence (HF) technology was proposed for next-generation OLEDs. In this technology, the TADF material was considered a sensitizing host, the so-called TADF sensitized host (TSH), for use of triplet excitons via the reverse intersystem crossing (RISC) pathway. Since most of the TADF materials show bipolar characteristics, electrically generated singlet and triplet exciton energies can be transported to the final fluorescent emitter (FE) through Förster resonance energy transfer (FRET) rather than Dexter energy transfer (DET). This mechanism is possible from the S1 state of the TSH to the S1 state of the final fluorescent dopant (FD) as a long-range energy transfer. Considering this, some reports are available based on hyperfluorescence OLEDs, but the detailed analysis for highly efficient and stable devices for commercialization was unclear. So herein, we reviewed the relevant factors based on recent advancements to build a highly efficient and stable hyperfluorescence system. The factors include an energy transfer mechanism based on spectral overlapping, TSH requirements, electroluminescence study based on exciplex and polarity system, shielding effect, DET suppression, and FD orientation. Furthermore, the outlook and future positives with new directions were discussed to build high-performance OLEDs.

Tailoring Extremely Narrow FWHM in Hypsochromic and Bathochromic Shift of Polycyclo-Heteraborin MR-TADF Materials for High-Performance OLEDs.

Developing double boron-based emitters with extremely narrow band spectrum and high efficiency in organic light-emitting diodes (OLEDs) is crucial and challenging. Herein, we report two materials, NO-DBMR and Cz-DBMR, hinge on polycyclic heteraborin skeletons based on role-play of the highest occupied molecular orbital (HOMO) energy levels. The NO-DBMR contains an oxygen atom, whereas the Cz-DBMR has a carbazole core in the double boron-embedded ν-DABNA structure. The synthesized materials resulted in an unsymmetrical pattern for NO-DBMR and surprisingly a symmetrical pattern for Cz-DBMR. Consequently, both materials showed extremely narrow full width at half maximum (FWHM) of 14 nm in hypsochromic (pure blue) and bathochromic (Bluish green) shifted emission without losing their high color fidelity. Furthermore, both materials show high photoluminescence quantum yield (PLQY) of over 82 %, and an extremely small singlet-triplet energy gap (ΔEST ) of 0.04 eV, resulting in high reverse intersystem crossing process (kRISC ) of 105  s-1 . Due to the efficient thermally activated delayed fluorescence (TADF) characteristics, the fabricated OLEDs based on these heteraborins manifested maximum external quantum efficiency (EQEmax ) of 33.7 and 29.8 % for NO-DBMR and Cz-DBMR, respectively. This is the first work reported with this type of strategy for achieving an extremely narrow emission spectrum in hypsochromic and bathochromic shifted emissions with a similar molecular skeleton.

Multiresonant TADF materials: triggering the reverse intersystem crossing to alleviate the efficiency roll-off in OLEDs.

The hunt for narrow-band emissive pure organic molecules capable of harvesting both singlet and triplet excitons for light emission has garnered enormous attention to promote the advancement of organic light-emitting diodes (OLEDs). Over the past decade, organic thermally activated delayed fluorescence (TADF) materials based on donor (D)/acceptor (A) combinations have been researched for OLEDs in wide color gamut (RGB) regions. However, due to the strong intramolecular charge-transfer (CT) state, they exhibit broad emission with full-width-at-half maximum (FWHM) > 70 nm, which deviates from being detrimental to achieving high color purity for future high-end display electronics such as high-definition TVs and ultra-high-definition TVs (UHDTVs). Recently, the new development in the sub-class of TADF emitters called multi-resonant TADF (MR-TADF) emitters based on boron/nitrogen atoms has attracted much interest in ultra-high definition OLEDs. Consequently, MR-TADF emitters are appeal to their potentiality as promising candidates in fabricating the high-efficient OLEDs due to their numerous advantages such as high photoluminescence quantum yield (PLQY), unprecedented color purity, and narrow bandwidth (FWHM ≤ 40 nm). Until now many MR-TADF materials have been developed for ultra-gamut regions with different design concepts. However, most MR-TADF-OLEDs showed ruthless external quantum efficiency (EQE) roll-off characteristics at high brightness. Such EQE roll-off characteristics were derived mainly from the low reverse intersystem crossing (kRISC) rate values. This feature article primarily focuses on the design strategies to improve kRISC for MR-TADF materials with some supportive strategies including extending charge delocalization, heavy atom introduction, multi-donor/acceptor utilization, and a hyperfluorescence system approach. Furthermore, the outlook and prospects for future developments in MR-TADF skeletons are described.

Efficient pure blue hyperfluorescence devices utilizing quadrupolar donor-acceptor-donor type of thermally activated delayed fluorescence sensitizers.

The hyperfluorescence (HF) system has drawn great attention in display technology. However, the energy loss mechanism by low reverse intersystem crossing rate (kRISC) and the Dexter energy transfer (DET) channel is still challenging. Here, we demonstrate that this can be mitigated by the quadrupolar donor-acceptor-donor (D-A-D) type of thermally activated delayed fluorescence (TADF) sensitizer materials, DBA-DmICz and DBA-DTMCz. Further, the HF device with DBA-DTMCz and ν-DABNA exhibited 43.9% of high maximum external quantum efficiency (EQEmax) with the Commission Internationale de l'Éclairage coordinates of (0.12, 0.16). The efficiency values recorded for the device are among the highest reported for HF devices. Such high efficiency is assisted by hindered DET process through i) high kRISC, and ii) shielded lowest unoccupied molecular orbital with the presence of two donors in D-A-D type of skeleton. Our current study provides an effective way of designing TADF sensitizer for future HF technology.

Stable ZnS Electron Transport Layer for High-Performance Inverted Cadmium-Free Quantum Dot Light-Emitting Diodes.

We report high-efficiency and long-lifetime inverted green cadmium-free (InP-based) quantum dot light-emitting diodes (QLEDs) using a stable ZnO/ZnS cascaded electron transport layer (ETL). We have successfully developed a strategy to spin-coat stable ZnS ETLs with a relatively higher conduction band minimum (CBM) and lower electron mobility than that of ZnO, which leads to balanced carrier injection and an improved device lifetime. Analysis shows that by using the ZnO/ZnS cascaded ETL, electron injection is reduced, resulting in an improved charge balance in the QD layer and suppressed exciton quenching, which preserves the emission properties of QDs. Optimized devices with ZnO/ZnS cascaded ETLs show a maximum external quantum efficiency of 10.8% and a maximum current efficiency of 37.5 cd/A; these efficiency values are an almost 2.2-fold improvement compared to those of reference devices without ZnS. The QLED devices also showed a remarkably long lifetime (LT70) of 265 h at an initial luminance of 1000 cd/m2. The predicted half-lifetime (LT50) at 100 cd/m2 is 60,255 h, which, to our knowledge, is currently the longest lifetime yet reported for InP-based green QLEDs.

An efficient organic and inorganic hybrid interlayer for high performance inverted red cadmium-free quantum dot light-emitting diodes.

The efficiency and device lifetime of quantum dot light-emitting diode (QLED) devices suffer from the charge imbalance issue resulting from excess electron injection from the ZnO electron transport layer (ETL) to the quantum dot (QD) emissive layer (EML). Herein we report 1,3-bis(9-phenyl-1,10-phenanthrolin-2-yl)benzene (BPPB) small molecule ETL blended ZnO as an interlayer in inverted red indium phosphide (InP) based QLEDs to slow down the ZnO ETL mobility. The device with ZnO : BPPB (15 wt%) shows 16.7% external quantum efficiency and 595 h lifetime (T 50) at 1000 cd m-2. Insertion of a thin hybrid interlayer reduces the electron injection to match the charge balance in the QD layer and also suppresses the interfacial exciton quenching between the ZnO ETL and QD EML.

Manipulating Spectral Width and Emission Wavelength towards Highly Efficient Blue Asymmetric Carbazole Fused Multi-Resonance Emitters.

The novel carbazole-based multiresonance types of thermally activated delayed fluorescence (MR-TADF) emitters of mICz-DABNA and BFCz-DABNA are reported, and their spectroscopic properties are investigated with the inductive effect on the central nitrogen atom for pure and deep blue emission. With the introduction of electron-donating/-withdrawing properties of substituents, emitters exhibited the bathochromic/hypsochromic shifted emission, respectively, compared to simple carbazole-based MR-TADF. Moreover, their spectral bandwidths became narrower. Theoretical calculation indicated that the meta-positioned bulky moiety restricts the molecular geometry discrepancy and reduces the Huang-Rhys factors. Particularly, the organic light-emitting diode (OLED) with 3% BFCz-DABNA exhibited the maximum external quantum efficiency of 28.0% with the Commission International de l'Éclairage (CIE) of (0.13, 0.09), which is the best record value among single-boron MR-TADF devices of CIE y < 0.10.

Synthesis of fluorescent organic nano-dots and their application as efficient color conversion layers.

Efficient conversion of light from short wavelengths to longer wavelengths using color conversion layers (CCLs) underpins the successful operation of numerous contemporary display and lighting technologies. Inorganic quantum dots, based on CdSe or InP, for example, have received much attention in this context, however, suffer from instability and toxic cadmium or phosphine chemistry. Organic nanoparticles (NPs), though less often studied, are capable of very competitive performance, including outstanding stability and water-processability. Surfactants, which are critical in stabilizing many types of nano-structures, have not yet been used extensively in organic NPs. Here we show the utility of surfactants in the synthesis and processing of organic NPs by thoroughly characterizing the effect of ionic and non-ionic surfactants on the properties of fluorescent organic NPs. Using this information, we identify surfactant processing conditions that result in nearly 100 % conversion of organic fluorophores into sub-micrometer particles, or nano-dots, with outstanding performance as CCLs. Such water dispersions are environmentally benign and efficiently convert light. They can be used for a range of fluorophores covering a full spectral gamut, with excellent color purity, including full-width at half-maximum (FWHM) values as low as 21 nm. Compared to inorganic (InP) reference CCLs, the organic nano-dot based CCLs show superior color conversion efficiency and substantially improved long-term stability.

Color-Tunable All-Fluorescent White Organic Light-Emitting Diodes with a High External Quantum Efficiency Over 30% and Extended Device Lifetime.

White organic light-emitting diodes (WOLEDs) with high efficiencies and tunable colors attracts considerable interest from the industry and academia. Thermally activated delayed-fluorescence (TADF) emitters can revolutionize such WOLED devices; however, they still suffer from poor performances. In this study, an advanced double-emissive-layer device architecture capable of hole-trapping TADF-sensitized emissions is proposed to not only achieve a recombination zone shift for the tunable colors but also accelerate exciton emission dynamics for high efficiency and alleviated roll-off. The proof-of-concept WOLEDs exhibit significant shifts in their Commission Internationale de l'Eclairage (CIE) coordinates and correlated color temperatures from (0.40, 0.47) and 4088 K at 100 cd m-2 to (0.27, 0.33) and 9269 K at 5000 cd m-2 . Additionally, the maximum external quantum efficiency (EQE) reaches 30.7% and remains >25% over a wide luminance range of 500-5000 cd m-2 , along with an extended LT80 of over 20 000 h at an initial luminance of 100 cd m-2 . This is the first time that all-fluorescent WOLEDs have been used to realize an EQE exceeding 30%, thereby establishing a new benchmark in this field.

Double boron-embedded multiresonant thermally activated delayed fluorescent materials for organic light-emitting diodes.

The subclass of multi resonant thermally activated delayed fluorescent emitters (MR-TADF) containing boron atoms has garnered significant attention in the field of organic light emitting diode (OLED) research. Among boron-based MR-TADF emitters, double boron-embedded MR-TADF (DB-MR-TADF) emitters show excellent electroluminescence performances with high photoluminescence quantum yields, narrow band emission, and beneficially small singlet-triplet energy levels in all the full-color gamut regions. This article reviews recent progress in DB-MR-TADF emitters, with particular attention to molecular design concepts, synthetic routes, optoelectronic properties, and OLED performance, giving future prospects for real-world applications.

Acceptor-Donor-Acceptor-Type Orange-Red Thermally Activated Delayed Fluorescence Materials Realizing External Quantum Efficiency Over 30% with Low Efficiency Roll-Off.

Two new orange-red thermally activated delayed fluorescence (TADF) materials, PzTDBA and PzDBA, are reported. These materials are designed based on the acceptor-donor-acceptor (A-D-A) configuration, containing rigid boron acceptors and dihydrophenazine donor moieties. These materials exhibit a small ΔEST of 0.05-0.06 eV, photoluminescence quantum yield (PLQY) as high as near unity, and short delayed exciton lifetime (τd ) of less than 2.63 µs in 5 wt% doped film. Further, these materials show a high reverse intersystem crossing rate (krisc ) on the order of 106 s-1 . The TADF devices fabricated with 5 wt% PzTDBA and PzDBA as emitting dopants show maximum EQE of 30.3% and 21.8% with extremely low roll-off of 3.6% and 3.2% at 1000 cd m-2 and electroluminescence (EL) maxima at 576 nm and 595 nm, respectively. The low roll-off character of these materials is analyzed by using a roll-off model and the exciton annihilation quenching rates are found to be suppressed by the fast krisc and short delayed exciton lifetime. These devices show operating device lifetimes (LT50 ) of 159 and 193 h at 1000 cd m-2 for PzTDBA and PzDBA, respectively. The high efficiency and low roll-off of these materials are attributed to the good electronic properties originatng from the A-D-A molecular configuration.

A New BODIPY Material for Pure Color and Long Lifetime Red Hyperfluorescence Organic Light-Emitting Diode.

A red fluorescent material, 1,3,7,9-tetrakis(4-(tert-butyl)phenyl)-5,5-difluoro-10-(2-methoxyphenyl)-5H-4l4,5l4-dipyrrolo[1,2-c:2',1'-f][1,3,2]diazaborinine (4tBuMB), as an emitting dopant in a thermally activated delayed fluorescence (TADF) sensitized hyperfluorescence organic light-emitting diode (HFOLED) is reported. The 4tBuMB shows a high photoluminescence quantum yield (PLQY) of 99% with an emission maximum at 620 nm and a full width at half-maximum (fwhm) of 31 nm in solution. Further, it shows a deep lowest unoccupied molecular orbital (LUMO) of 3.83 eV. Thus, two TADF materials, 4CzIPN and 4CzTPN, as sensitizing hosts, are selected on the basis of a suitable LUMO level and spectrum overlap with 4tBuMB. The fabricated HFOLED device with 4CzTPN as a sensitizing host and 4tBuMB as an emitting dopant shows a maximum external quantum efficiency (EQE), an emission maximum, an fwhm, and CIE coordinates of 19.4%, 617 nm, 44 nm, and (0.64, 0.36), respectively. The electroluminance performances of the 4CzTPN sensitized device are higher than those of the 4CzIPN-based device, which is attributed to a higher Förster resonance energy transfer (FRET) rate and reduced intersystem crossing/reverse intersystem crossing (ISC/RISC) cycles of the former. Also, the 4CzTPN-based HF device shows a longer device lifetime (LT90) of 954 h than the 4CzIPN-baed device (LT90 of 57 h) at 3000 cd m-2. The higher device stability is due to the higher bond dissociation energies (BDEs) of 4CzTPN and 4tBuMB than that of 4CzIPN.

Asymmetric Host Molecule Bearing Pyridine Core for Highly Efficient Blue Thermally Activated Delayed Fluorescence OLEDs.

In this study, two host materials, pCzBzbCz and pCzPybCz, are synthesized to achieve a high efficiency and long lifetime of blue thermally activated delayed fluorescence organic light-emitting diodes (TADF-OLEDs). The molecular design strategy involves the introduction of a pyridine group into the core structure of pCzPybCz as an electron-withdrawing unit, and an electron-donating phenyl group into the structure of pCzBzbCz. These host materials demonstrate good thermal stability and high triplet energy (T1 =3.07 eV for pCzBzbCz and 3.06 eV for pCzPybCz) for the fabrication of blue TADF-OLEDs. In particular, pCzPybCz-based OLED devices demonstrate an external quantum efficiency (EQE) of 22.7 % and an operational lifetime of 24 h (LT90 , time to attain 90 % of initial luminance) at an initial luminance of 1000 cd m-2 . This superior lifetime could be explained by the C-N bond dissociation energy (BDE) in the host molecular structure. Furthermore, a mixed-host system using the electron-deficient 2,4-bis(dibenzo[b,d]furan-2-yl)-6-phenyl-1,3,5-triazine (DDBFT) is proposed to inhibit the formation of the anion state of our host materials. In short, the device operational lifetime is further improved by applying DDBFT. The carbazole-based asymmetric host molecule containing a pyridine core realizes a high-efficiency blue TADF-OLED showing a positive effect on the operating lifetime, and can provide useful strategies for designing new host materials.

Recent Advancement in Boron-Based Efficient and Pure Blue Thermally Activated Delayed Fluorescence Materials for Organic Light-Emitting Diodes.

In the last few years, electron-deficient materials have been actively researched for application in organic light-emitting diode (OLED) as dopant and electron-transporting materials. The boron-containing materials are interesting as they give good emissive properties in solid state with an electron-accepting character. Recently, many boron-containing materials are used as emissive materials for thermally activated delayed fluorescence (TADF) OLED applications. In this review, boron acceptor-based push-pull small molecules used for application in blue TADF OLEDs are reviewed, covering their different types of acceptor, molecular design, structure-property relation, material properties, and device properties. Also, the importance of boron acceptors to address the key issue of blue TADF OLEDs is discussed.

External Quantum Efficiency Exceeding 24% with CIEy Value of 0.08 using a Novel Carbene-Based Iridium Complex in Deep-Blue Phosphorescent Organic Light-Emitting Diodes.

Deep-blue triplet emitters remain far inferior to standard red and green triplet emitters in terms of exhibiting high-color-purity Commission International de l'Éclairage (CIE) y values of ≤0.1, external quantum efficiencies (EQEs), and high electroluminescent brightnesses in phosphorescent organic light-emitting diodes. In fact, no deep-blue triplet emitter with color purity and high device performance has previously been reported. In this study, a deep-blue triplet emitter, mer-tris(N-phenyl, N-benzyl-pyridoimidazol-2-yl)iridium(III) (mer-Ir1) is developed, which meets the requirements of the National Television System Committee (NTSC) CIE(x, y) coordinates of (0.149, 0.085) with an extremely high EQE of 24.8% and maximum brightness (Lmax ) of 6453 cd m-2 , by a device with a 40 vol% doping ratio. Moreover, another device demonstrates an EQEmax of 21.3%, an Lmax of 5247 cd m-2 , and CIE(x, y) coordinates of (0.151, 0.086) at a 30 vol% doping ratio. This is the first report of a high-performance, deep-blue phosphor, carbene-based Ir(III) complex device with outstanding CIE(x, y) color coordinates and a high EQE. The results of this study indicate that the novel dopant mer-Ir1 is a promising candidate for reducing power consumption in display applications.

Efficient Cadmium-Free Inverted Red Quantum Dot Light-Emitting Diodes.

Here, we report an efficient inverted red indium phosphide (InP) comprising QD (InP/ZnSe/ZnS, core/shell structure) light-emitting diode (QLED) by modulating an interfacial contact between the electron transport layer and emissive InP-QDs and applying self-aging approach. The red InP-QLED with optimized interfacial contact exhibits a significant improvement in maximum external quantum efficiency and current efficiency from 4.42 to 10.2% and 4.70 to 10.8 cd/A, respectively, after 69 days of self-aging, which is an almost 2.3-fold improvement compared to the fresh device. The analysis indicates the consecutive reduction in electron injection and accumulation in the emissive QD due to changes in the conduction band minimum of ZnMgO (0.1 eV after 10 days of storage) through a downward vacuum-level shift according to the aging times. During the device aging periods, the oxygen vacancy of ZnMgO reduces, which leads to lower the conductivity of ZnMgO. As a result, charge balance of the device is improved with the suppression of exciton quenching at the interface of ZnMgO and InP-QD.