State-crossing from a Locally Excited to an Electron Transfer State(SLEET)Model Rationalizing the Aggregation-induced Emission Mechanism of(Bi)piperidylanthracenes

Luminogens with aggregation-induced emission(AIE)characteristics(or AIEgens)have been widely used in various applications due to their excellent luminescent properties in molecular aggregates and the solid state.A deep understanding of the AIE mechanism is critical for the rational development of AIEgens.In this work,the“state-crossing from a locally excited to an electron transfer state”(SLEET)model is employed to rationalize the AIE phenomenon of two(bi)piperidylanthracenes.According to the SLEET model,an electron transfer(ET)state is formed along with the rotation of the piperidyl group in the excited state of(bi)piperidylan-thracene monomers,leading to fluorescence quenching.In contrast,a bright state exists in the crystal and molecular aggregates of these compounds,as the intermolecular interactions restrict the formation of the dark ET state.This mechanistic understanding could inspire the deployment of the SLEET model in the rational designs of various functional AIEgens.

Photophysical Properties of 4t-（p-aminophenyl）-2,2＇：6＇,2″-terpyridine

Spectral and photophysical investigations of 4＇-（p-aminophenyl）-2,2＇：6＇,2″-terpyridine （APT） have been performed in various solvents with different polarity and hydrogen-bonding ability. The emission spectra of APT are found to exhibit dual fluorescence in polar solvents, which attributes to the local excited and intramolecular charge transfer states, respectively. The two-state model is proven out for APT in polar solvent by the time-correlated single photon counting emission decay measurement. Interestingly, the linear relationships of different emission maxima and solvent polarity parameter are found for APT in protic and aprotic solvents, because of the hydrogen bond formation between APT and alcohols at the amino nitrogen N25. Furthermore, the effects of the complexation of the metal ion with tpy group of APT and the hydrogen bond formation between APT with methanol at the terpyridine nitrogen N4-NS-N14 are also presented. The appearance of new long-wave absorption and fluorescence bands indicates that a new ground state of the complexes is formed.

Efficient and Fast X-Ray Luminescence in Organic Phosphors Through High-Level Triplet-Singlet Reverse Intersystem Crossing

Organic scintillators that efficiently generate bright triplet excitons are of critical importance for highperformance X-ray-excited luminescence in radiation detection.However,the nature of triplet-singlet spinforbidden transitions in these materials often result in long-lived phosphorescence,which is undesirable for ultrafast X-ray detection and imaging.Here we demonstrate that the effect of hybridized local and charge-transfer(HLCT)excited states enables organic scintillators to exhibit highly efficient and fast radioluminescence(RL)in response to X-ray irradiation.Our experimental and theoretical investigation shows that the oxidized 1,8-naphthalimide-phenothiazine dyad(OMNI-PTZ 2)with HLCT-excited states has an enhanced overlap integral of the highest occupied molecular orbital(HOMO)and lowest unoccupied molecular orbital(LUMO)on MNIπ-orbitals,and moderate donor–acceptor electron interactions.As a result,the RL of these crystals exhibits a 61-fold increase and its monoexponential decay lifetime is three orders of magnitude faster compared to its corresponding thermally activated delayed fluorescence(TADF)molecule MNI-PTZ 1.We further demonstrate the practical utility of the OMNI-PTZ 2(G)in high-performance X-ray detection and imaging,achieving an X-ray dose sensitivity of 97 nGy s−1 and an exceptional spatial resolution of 20 lp/mm.Our study provides a promising molecular design principle for utilizing triplet excitons to develop high-efficiency and fast X-ray scintillators for the development of next-generation flexible and stretchable X-ray imaging detectors.

Triplet fusion delayed fluorescence materials for OLEDs

The development of fluorescent materials capable of harvesting triplet excitons efficiently is of great importance in achieving high-performance low-cost organic light-emitting diodes（OLEDs）.Among the three mechanisms converting triplet to singlet excitons,triplet fusion delayed fluorescence（TFDF） plays a key role in the demonstration of highly efficient and reliable OLEDs,especially blue devices,for practice applications.This review focuses on the recent development of TFDF materials and their applications in OLEDs.Fundamental TFDF mechanism,molecular design principles,and the structure-property relationship of TFDF materials with a particular emphasis on their different excited state characters,are presented and discussed.Moreover,the future perspectives and ongoing challenges of TFDF materials are also highlighted.

Nearly 100% exciton utilization in highly efficient red OLEDs based on dibenzothioxanthone acceptor

Improving the utilization of excitons has always been an important topic for the development of electroluminescence devices.In this work,we designed and synthesized three red TADF emitters TPA-DBT12,TPA-DBT3 and DTPA-DBT by employing dibenzothioxanthone(DBT)acceptor framework to stabilize the locally excited triplet state to participate in the reverse intersystem crossing(RISC)process.The fast RISC process and singlet radiation decay process gave rise to evidently enhanced exciton utilization.All of the red OLEDs based on these materials showed maximum EQE over 11% and high exciton utilization close to 100%.This work not only extend the acceptor framework for red materials but also provide a new perspective for the design of highly efficient red TADF materials with 100% exciton utilization by managing locally excited triplet state.