Bright and stable perovskite light-emitting diodes in the near-infrared range.

Perovskite light-emitting diodes (LEDs) have attracted broad attention due to their rapidly increasing external quantum efficiencies (EQEs)1-15. However, most high EQEs of perovskite LEDs are reported at low current densities (<1 mA cm-2) and low brightness. Decrease in efficiency and rapid degradation at high brightness inhibit their practical applications. Here, we demonstrate perovskite LEDs with exceptional performance at high brightness, achieved by the introduction of a multifunctional molecule that simultaneously removes non-radiative regions in the perovskite films and suppresses luminescence quenching of perovskites at the interface with charge-transport layers. The resulting LEDs emit near-infrared light at 800 nm, show a peak EQE of 23.8% at 33 mA cm-2 and retain EQEs more than 10% at high current densities of up to 1,000 mA cm-2. In pulsed operation, they retain EQE of 16% at an ultrahigh current density of 4,000 mA cm-2, along with a high radiance of more than 3,200 W s-1 m-2. Notably, an operational half-lifetime of 32 h at an initial radiance of 107 W s-1 m-2 has been achieved, representing the best stability for perovskite LEDs having EQEs exceeding 20% at high brightness levels. The demonstration of efficient and stable perovskite LEDs at high brightness is an important step towards commercialization and opens up new opportunities beyond conventional LED technologies, such as perovskite electrically pumped lasers.

Hydrogen Bonding Regulated Flexibility and Disorder in Hydrazone-Linked Covalent Organic Frameworks.

Covalent organic framework (COF) chemistry is experiencing unprecedented development in recent decades. The current studies on COF chemistry are mainly focused on the discovery of novel covalent linkages, new topological structures, synthetic methodologies, and potential applications. However, despite the fact that noncovalent interactions are ubiquitous in COF chemistry, relatively little attention has been given to the role of noncovalent bonds on COF structures and their properties. In this work, a series of hydrazone-linked COFs involving noncovalent hydrogen bonds have been constructed, where the hydrogen-bonding interaction plays critical roles in the COF crystallinity and structures. The regulation of structural flexibility, the reversible transition between order and disorder, and the variety of host-guest interactions have been demonstrated in succession for the first time in COFs. The results obtained by the hydrogen-bonding-regulated strategy may also be extendable to other noncovalent interactions, such as π-π interactions, metal coordination interactions, Lewis acid-base interactions, etc. These findings will inspire future developments in the design, synthesis, structural regulation, and applications of COFs by manipulating noncovalent interactions.

Dielectric control of reverse intersystem crossing in thermally activated delayed fluorescence emitters.

Thermally activated delayed fluorescence enables organic semiconductors with charge transfer-type excitons to convert dark triplet states into bright singlets via reverse intersystem crossing. However, thus far, the contribution from the dielectric environment has received insufficient attention. Here we study the role of the dielectric environment in a range of thermally activated delayed fluorescence materials with varying changes in dipole moment upon optical excitation. In dipolar emitters, we observe how environmental reorganization after excitation triggers the full charge transfer exciton formation, minimizing the singlet-triplet energy gap, with the emergence of two (reactant-inactive) modes acting as a vibrational fingerprint of the charge transfer product. In contrast, the dielectric environment plays a smaller role in less dipolar materials. The analysis of energy-time trajectories and their free-energy functions reveals that the dielectric environment substantially reduces the activation energy for reverse intersystem crossing in dipolar thermally activated delayed fluorescence emitters, increasing the reverse intersystem crossing rate by three orders of magnitude versus the isolated molecule.

Highly efficient luminescence from space-confined charge-transfer emitters.

Charge-transfer (CT) complexes, formed by electron transfer from a donor to an acceptor, play a crucial role in organic semiconductors. Excited-state CT complexes, termed exciplexes, harness both singlet and triplet excitons for light emission, and are thus useful for organic light-emitting diodes (OLEDs). However, present exciplex emitters often suffer from low photoluminescence quantum efficiencies (PLQEs), due to limited control over the relative orientation, electronic coupling and non-radiative recombination channels of the donor and acceptor subunits. Here, we use a rigid linker to control the spacing and relative orientation of the donor and acceptor subunits, as demonstrated with a series of intramolecular exciplex emitters based on 10-phenyl-9,10-dihydroacridine and 2,4,6-triphenyl-1,3,5-triazine. Sky-blue OLEDs employing one of these emitters achieve an external quantum efficiency (EQE) of 27.4% at 67 cd m-2 with only minor efficiency roll-off (EQE = 24.4%) at a higher luminous intensity of 1,000 cd m-2. As a control experiment, devices using chemically and structurally related but less rigid emitters reach substantially lower EQEs. These design rules are transferrable to other donor/acceptor combinations, which will allow further tuning of emission colour and other key optoelectronic properties.

Controlling Singlet-Triplet Energy Splitting for Deep-Blue Thermally Activated Delayed Fluorescence Emitters.

The development of efficient metal-free organic emitters with thermally activated delayed fluorescence (TADF) properties for deep-blue emission is still challenging. A new family of deep-blue TADF emitters based on a donor-acceptor architecture has been developed. The electronic interaction between donor and acceptor plays a key role in the TADF mechanism. Deep-blue OLEDs fabricated with these TADF emitters achieved high external quantum efficiencies over 19.2 % with CIE coordinates of (0.148, 0.098).

Donor-σ-Acceptor Motifs: Thermally Activated Delayed Fluorescence Emitters with Dual Upconversion.

A family of organic emitters with a donor-σ-acceptor (D-σ-A) motif is presented. Owing to the weakly coupled D-σ-A intramolecular charge-transfer state, a transition from the localized excited triplet state (3 LE) and charge-transfer triplet state (3 CT) to the charge-transfer singlet state (1 CT) occurred with a small activation energy and high photoluminescence quantum efficiency. Two thermally activated delayed fluorescence (TADF) components were identified, one of which has a very short lifetime of 200-400 ns and the other a longer TADF lifetime of the order of microseconds. In particular, the two D-σ-A materials presented strong blue emission with TADF properties in toluene. These results will shed light on the molecular design of new TADF emitters with short delayed lifetimes.

The Control of Conjugation Lengths and Steric Hindrance to Modulate Aggregation-Induced Emission with High Electroluminescence Properties and Interesting Optical Properties.

A series of novel AIE-active (aggregation-induced emission) molecules, named SAF-2-TriPE, SAF-3-TriPE, and SAF-4-TriPE, were designed and synthesized through facile reaction procedures. We found that incorporation of the spiro-acridine-fluorene (SAF) group, which is famous for its excellent hole-transporting ability and rigid structure, at different substitution positions on the phenyl ring affected the conjugation lengths of these compounds. Consequently, we have obtained molecules with different emission colors and properties without sacrificing good EL (electroluminescence) characteristics. Accordingly, a device that was based on compound SAF-2-TriPE displayed superior EL characteristics: it emitted green light with ηc, max =10.5 cd A(-1) and ηext, max =4.22 %, whereas a device that was based on compound SAF-3-TriPE emitted blue-green light with ηc, max =3.9 cd A(-1) and ηext, max = 1.71 %. These compounds also displayed different AIE performances: when the fraction of water in the THF solutions of these compounds was increased, we observed a significant improvement in the ΦF of compounds SAF-2-TriPE and SAF-3-TriPE; in contrast, compound SAF-4-TriPE showed an abnormal phenomenon, in that it emitted a strong fluorescence in both pure THF solution and in the aggregated state without a significant change in ΦF . Overall, this systematic study confirmed a relationship between the regioisomerism of the luminophore structure and its AIE activity and the resulting electroluminescent performance in non-doped devices.

Benzimidazobenzothiazole-Based Bipolar Hosts to Harvest Nearly All of the Excitons from Blue Delayed Fluorescence and Phosphorescent Organic Light-Emitting Diodes.

Much effort has been devoted to developing highly efficient organic light-emitting diodes (OLEDs) that function through phosphorescence or thermally activated delayed fluorescence (TADF). However, efficient host materials for blue TADF and phosphorescent guest emitters are limited because of their requirement of high triplet energy levels. Herein, we report the rigid acceptor unit benzimidazobenzothiazole (BID-BT), which is suitable for use in bipolar hosts in blue OLEDs. The designed host materials, based on BID-BT, possess high triplet energy and bipolar carrier transport ability. Both blue TADF and phosphorescent OLEDs containing BID-BT-based derivatives exhibit external quantum efficiencies as high as 20 %, indicating that these hosts allow efficient triplet exciton confinement appropriate for blue TADF and phosphorescent guest emitters.

Excited-State Engineering Enables Efficient Deep-Blue Light-Emitting Diodes Exhibiting BT.2020 Color Gamut.

Organic luminescent materials that exhibit thermally activated delayed fluorescence (TADF) can convert non-emissive triplet excitons into emissive singlet states through a reverse intersystem crossing (RISC) process. Therefore, they have tremendous potential for applications in organic light-emitting diodes (OLEDs). However, with the development of ultra-high definition 4K/8K display technologies, designing efficient deep-blue TADF materials to achieve the Commission Internationale de l'Éclairage (CIE) coordinates fulfilling BT.2020 remains a significant challenge. Here, an effective approach is proposed to design deep-blue TADF molecules based on hybrid long- and short-range charge-transfer by incorporation of multiple donor moieties into organoboron multiple resonance acceptors. The resulting TADF molecule exhibits deep-blue emission at 414 nm with a full width at half maximum (FWHM) of 29 nm, together with a thousand-fold increase in RISC rate. OLEDs based on the champion material achieve a record maximum external quantum efficiency (EQE) of 22.8% with CIE coordinates of (0.163, 0.046), approaching the coordinates of the BT.2020 blue standard. Moreover, TADF-assisted fluorescence devices employing the designed material as a sensitizer exhibit an exceptional EQE of 33.1%. This work thus provides a blueprint for future development of efficient deep-blue TADF emitters, representing an important milestone towards meeting the blue color gamut standard of BT.2020.

Silicon-based material with spiro-annulated fluorene/triphenylamine as host and exciton-blocking layer for blue electrophosphorescent devices.

A novel silicon-based compound, 10-phenyl-2'-(triphenylsilyl)-10H-spiro[acridine-9,9'-fluorene] (SSTF), with spiro structure has been designed, synthesized, and characterized. Its thermal, electronic absorption, and photoluminescence properties were studied. Its energy levels make it suitable as a host material or exciton-blocking material in blue phosphorescent organic light-emitting diodes (PhOLEDs). Accordingly, blue-emitting devices with iridium(III) bis[(4,6-difluorophenyl)-pyridinato-N,C(2)']picolinate (FIrpic) as phosphorescent dopant have been fabricated and show high efficiency with low roll-off. In particular, 44.0 cd A(-1) (41.3 lm W(-1)) at 100 cd m(-2) and 41.9 cd A(-1) (32.9 lm W(-1)) at 1000 cd m(-2) were achieved when SSTF was used as host material; 28.1 lm W(-1) at 100 cd m(-2) and 20.6 lm W(-1) at 1000 cd m(-2) were achieved when SSTF was used as exciton-blocking layer. All of the results are superior to those of the reference devices and show the potential applicability and versatility of SSTF in blue PhOLEDs.