Herein, we demonstrate that the strategic implementation of electron-accepting tricoordinate boron and electron-donating carbazole subunits into polycyclic aromatic hydrocarbons (PAHs) produces a family of attractive full-color luminophores that can emit narrowband and efficient thermally activated delayed fluorescence (TADF). A versatile modular design for these boron- and carbazole-embedded PAHs can facilitate the systematic modulation of their photophysical and optoelectronic properties. Organic light-emitting diodes that utilize these PAHs as TADF emitters demonstrate narrowband electroluminescence from blue to red, achieving high maximum external quantum efficiencies of 29.3%, 31.8%, and 22.0% for blue, green, and red, respectively.

Full-Color, Narrowband, and High-Efficiency Electroluminescence from Boron and Carbazole Embedded Polycyclic Heteroaromatics.

Simultaneously achieving both a high efficiency and long lifetime in deep-blue organic light-emitting diodes is challenging. Here we report thermally activated delayed fluorescence (TADF) organic light-emitting diodes that aim to meet this goal by combining a new design of blue TADF materials with a triplet-exciton recycling protocol. Two TADF materials, one distributing and one emitting, were doped into a host to form triplet-exciton-distributed TADF devices. The singlet excitons were transferred from the host to the emitter via the distributing TADF material by cascade energy transfer, whereas the triplet excitons were transferred to the emitter as singlet excitons by a triplet-exciton recycling process between the low-triplet-energy host and the distributing TADF material. The resulting triplet-exciton-distributed TADF devices achieved a high external quantum efficiency of 33.5 ± 0.1, a colour coordinate corrected current efficiency over 400 cd A–1, a lifetime of >5,000 h and a y colour coordinate below 0.10. Exciton energy cascade transfer and recycling bring improvements in the efficiency and lifetime of deep-blue organic light-emitting diodes.

High-efficiency, long-lifetime deep-blue organic light-emitting diodes

Efficient organic emitters in the deep-red region are rare due to the "energy gap law". Herein, multiple boron (B)- and nitrogen (N)-atoms embedded polycyclic heteroaromatics featuring hybridized π-bonding/ non-bonding molecular orbitals are constructed, providing a way to overcome the above luminescent boundary. The introduction of B-phenyl-B and N-phenyl-N structures enhances the electronic coupling of those para-positioned atoms, forming restricted π-bonds on the phenyl-core for delocalized excited states and thus a narrow energy gap. The mutually ortho-positioned B- and N-atoms also induce a multi-resonance effect on the peripheral skeleton for the non-bonding orbitals, creating shallow potential energy surfaces to eliminate the high-frequency vibrational quenching. The corresponding deep-red emitters with peaks at 662 and 692 nm exhibit narrow full-width at half-maximums of 38 nm, high radiative decay rates of ca. 108  s-1 , ≈100 % photo-luminescence quantum yields and record-high maximum external quantum efficiencies of ca. 28 % in a normal planar organic light-emitting diode structure, simultaneously.

Multi-Resonance Deep-Red Emitters with Shallow Potential-Energy Surfaces to Surpass Energy-Gap Law**

Multiresonance thermally activated delayed fluorescence (MR-TADF) emitters manifest great potential for organic light-emitting diodes (OLEDs) due to their high exciton-utilization efficiency and narrowband emission. Nonetheless, their tendency toward self-quenching caused by strong interchromophore interactions would induce doping sensitivity and deteriorate the device performances, and effective strategy to construct quenching-resistant emitters without sacrifycing color purity is still to be developed. By segregating the planar MR-TADF skeleton using two bulky carbazolyl units, herein a highly emissive molecule with enhanced quenching resistance is reported. The steric effect largely removes the formation of detrimental excimers/aggregates, and boosts the performance of the corresponding devices with a maximum external quantum efficiency (EQEmax ) up to 40.0% and full width at half maximum (FWHM) of 25 nm, representative of the only example of single OLED that can concurrently achieve narrow bandwidth and high EL efficiency surpassing 40% to date. Even at doping ratio of 30 wt%, the EQEmax is retained to be 33.3% with nearly unchanged emission spectrum. This work provides a viable approach to realize doping-insensitive MR-TADF devices with extreme EL efficiency and color purity for high-end OLED displays.

Quenching-Resistant Multiresonance TADF Emitter Realizes 40% External Quantum Efficiency in Narrowband Electroluminescence at High Doping Level.

Organic light emitters based on multiresonance-induced thermally activated delayed fluorescent materials have great potential for realizing efficient, narrowband organic light-emitting diodes (OLEDs). However, at high brightness operation, efficiency roll-off attributed to the slow reverse intersystem crossing (RISC) process hinders the use of multiresonance-induced thermally activated delayed fluorescent materials in practical applications. Here we report a heavy-atom incorporating emitter, BNSeSe, which is based on a selenium-integrated boron–nitrogen skeleton and exhibits 100% photoluminescence quantum yield and a high RISC rate (kRISC) of 2.0 × 106 s−1. The corresponding green OLEDs exhibit excellent external quantum efficiencies of up to 36.8% and ultra-low roll-off character at high brightnesses (with very small roll-off values of 2.8% and 14.9% at 1,000 cd m−2 and 10,000 cd m−2, respectively). Furthermore, the outstanding capability to harvest triplet excitons also enables BNSeSe to be a superior sensitizer for a hyperfluorescence OLED, which shows state-of-the-art performance with a high excellent external quantum efficiency of 40.5%, power efficiency beyond 200 lm W−1, and luminance close to 20,0000 cd m−2. Green OLEDs based on BNSeSe offer high operational efficiency and reduced efficiency roll-off. 

/pdf/efficient-selenium-integrated-tadf-oleds-with-reduced-roll-1qxa4rnx.pdf

Efficient selenium-integrated TADF OLEDs with reduced roll-off

Multiple donor-acceptor-type carbazole-benzonitrile derivatives that exhibit thermally activated delayed fluorescence (TADF) are the state of the art in efficiency and stability in sky-blue organic light-emitting diodes. However, such a motif still suffers from low reverse intersystem crossing rates (kRISC ) with emission peaks 60 h at an initial luminance of 1000 cd m-2 .

Efficient and Stable Deep-Blue Fluorescent Organic Light-Emitting Diodes Employing a Sensitizer with Fast Triplet Upconversion.

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Efficient and Stable Deep-Blue Fluorescent Organic Light-Emitting Diodes Employing a Sensitizer with Fast Triplet Upconversion.