Recovering the Thermally Activated Delayed Fluorescence in Aggregation-Induced Emitters of Carborane.

The aggregation-induced emission (AIE) behaviors of carborane-based hybrid emitters have been extensively reported, while their combinations with the thermally activated delayed fluorescence (TADF) are still scarce. We designed and synthesized three Janus carboranes (the chemical structures resemble the double-faced god, Janus) Cb-1/2/3 with different carbazole moieties. All of the Janus carboranes exhibited quenched emission in solution with ΦPL (quantum efficiency of photoluminescence (PL)) lower than 0.01. The PL performance was improved by proceeding to the aggregates in THF/water (ΦPL 0.17-0.35) and further improved in the crystals or solid with ΦPL up to 0.99 for Cb-1, 0.85 for Cb-2, and 0.61 for Cb-3, which agreed with the AIE enhancement. Although the PL of solid Cb-1/2/3 showed non-TADF properties with lifetimes only at several nanoseconds, the crystallographic studies have shown a root cause of π···π stacking that quenched the TADF, and the theoretical calculations forecasted small singlet-triplet energy gaps (ΔES-T) therein. According to these findings, TADF was recovered in Cb-1/2/3 by doping into 1,3-bis(carbazol-9-yl)benzene (mCP). The 10 wt % doped films of Cb-1/2/3 have achieved a trade-off of ΦPL (0.84 in Cb-3 and 0.83 in Cb-1) and delayed lifetime (up to 8 µs). The doped devices of organic light-emitting diodes incorporating Cb-1/2/3 achieved the highest external quantum efficiency at 10.1% and the maximized luminance of 5920 cd/m2 at a driving voltage of 8 V.

Efficient Exciplex-based Green and Near-Infrared Organic Light-Emitting Diodes Employing a Novel Donor-Acceptor Type Donor.

Widely investigated thermally activated delayed fluorescence (TADF) can be achieved by intramolecular and intermolecular charge transfer between an electron donor and electron acceptor which corresponds to a TADF material and exciplex, respectively. However, the development of efficient organic light-emitting diodes (OLEDs) based on an exciplex lags far behind the development of those based on efficient TADF materials. In this work, a novel D-A type electron donor TPAFPO was designed and synthesized. TPAFPO:PO-T2T exhibits a small ΔEST of 79 meV and significant delayed emission, demonstrating TADF characteristics. OLEDs based on TPAFPO:PO-T2T exhibit a low turn-on voltage of 2.4 V and high an EQE value of 17.0%. Besides, NIR OLEDs utilizing TPAFPO:PO-T2T as host exhibit a turn-on voltage of 3.0 V and high EQE of 9.2% with a NIR emission peak at 690 nm. Furthermore, solution-processed exciplex and NIR devices also can maintain high efficiencies of 15.1% and 8.1%, respectively.

Imidazo[1,2-a]pyridine as an Electron Acceptor to Construct High-Performance Deep-Blue Organic Light-Emitting Diodes with Negligible Efficiency Roll-Off.

Two novel bipolar deep-blue fluorescent emitters, IP-PPI and IP-DPPI, featuring different lengths of the phenyl bridge, were designed and synthesized, in which imidazo[1,2-a]pyridine (IP) and phenanthroimidazole (PI) were proposed as an electron acceptor and an electron donor, respectively. Both of them exhibit outstanding thermal stability and high emission quantum yields. All the devices based on these two materials showed negligible efficiency roll-off with increasing current density. Impressively, non-doped organic light-emitting diodes (OLEDs) based on IP-PPI and IP-DPPI exhibited external quantum efficiencies (EQEs) of 4.85 % and 4.74 % with CIE coordinates of (0.153, 0.097) and (0.154, 0.114) at 10000 cd m-2 , respectively. In addition, the 40 wt % IP-PPI doped device maintained a high EQE of 5.23 % with CIE coordinates of (0.154, 0.077) at 10000 cd m-2 . The doped device based on 20 wt % IP-DPPI exhibited a higher deep-blue electroluminescence (EL) performance with a maximum EQE of up to 6.13 % at CIE of (0.153, 0.078) and maintained an EQE of 5.07 % at 10000 cd m-2 . To the best of our knowledge, these performances are among the state-of-the art devices with CIEy ≤0.08 at a high brightness of 10000 cd m-2 . Furthermore, by doping a red phosphorescent dye Ir(MDQ)2 (MDQ=2-methyldibenzo[f,h]quinoxaline) into the IP-PPI and IP-DPPI hosts, high-performance red phosphorescent OLEDs with EQEs of 20.8 % and 19.1 % were achieved, respectively. This work may provide a new approach for designing highly efficient deep-blue emitters with negligible roll-off for OLED applications.

Ternary Acceptor-Donor-Acceptor Asymmetrical Phenanthroimidazole Molecule for Highly Efficient Near-Ultraviolet Electroluminescence with External Quantum Efficiency (EQE) >4 .

A new ternary acceptor (A)-donor (D)-acceptor (A) asymmetrically twisted deep-blue emitting molecule, PPI-2BI, was synthesized by attaching two electrophilic benzimidazole (BI) units to the C2 and N1 positions of a phenanthroimidazole (PI) donor unit. Profiting from the enhanced D-A electronic coupling, the electron injecting and transporting abilities of the new triangle-shaped A-D-A molecule are considerably improved and the molecule shows high photoluminescence (PL) and electroluminescence (EL) efficiencies. By using PPI-2BI as a non-doped emitting layer (EML), the resulting organic light-emitting device exhibits emission with color coordinates of (0.158, 0.124) and a maximum external quantum efficiency (EQE), current efficiency (CE), and power efficiency (PE) of 4.63 %, 4.98 cd A-1 , and 4.82 lm W-1 , respectively. Additionally, a simple bilayer device using PPI-2BI as both the EML and the electron-transporting layer (ETL) also shows an EQE of 3.81 % with little changes to the color purity. Remarkably, a PPI-2BI-based doped device emits efficient near-ultraviolet EL with color coordinates of (0.154, 0.047) and an EQE of 4.12 %, which is comparable to that of the best reported near-UV emitting devices.

EQE Climbing Over 6% at High Brightness of 14350 cd/m2 in Deep-Blue OLEDs Based on Hybridized Local and Charge-Transfer Fluorescence.

Three deep-blue emitters PPi-Pid, PPi-Xid, and PPi-Mid based on a novel conjugated system phenantroimidazole-π-indolizine have been designed and synthesized. Here, indolizine with appropriate π-conjugation length was used as the acceptor profited from its high-photoluminescence quantum yield and good electron-withdrawing ability. Fluorescent organic light-emitting diodes (OLEDs) based on PPi-Pid, PPi-Xid, and PPi-Mid achieved deep-blue emissions with the Commission Internationale de L'Eclairage coordinates of (0.151, 0.076), (0.155, 0.052), and (0.153, 0.052); high brightness of 14350, 4377, and 4002 cd/m2; and high external quantum efficiencies (EQEs) of 6.01, 3.90, and 4.28%, respectively. Moreover, it is noticeable that all of the devices exhibited efficiencies increasing with brightness. In particular, the PPi-Pid-based device exhibited high EQE over 6% at a high brightness of 14350 cd/m2. Such high brightness along with high EQE is very rare whether in deep-blue fluorescent or thermally activated delayed fluorescent OLEDs.