High-performance nondoped organic light-emitting diodes(OLEDs)are promising technologies for future commercial applications.Herein,we synthesized two new thermally activated delayed fluorescence(TADF)emitters that ena...High-performance nondoped organic light-emitting diodes(OLEDs)are promising technologies for future commercial applications.Herein,we synthesized two new thermally activated delayed fluorescence(TADF)emitters that enable us,for the first time,to combine three effective approaches for enhancing the efficiency of nondoped OLEDs.First,the two emitters are designed to have high steric hindrances such that their emitting cores will be suitably isolated from those of their neighbors to minimize concentration quenching.On the other hand,each of the two emitters has two stable conformations in solid films.In their neat films,molecules with the minority conformation behave effectively as dopants in the matrix composing of the majority conformation.One hundred percent exciton harvesting is thus theoretically feasible in this unique architecture of“self-doped”neat films.Furthermore,both emitters have relatively high aspect ratios in terms of their molecular shapes.This leads to films with preferred molecular orientations enabling high populations of horizontal dipoles beneficial for optical outcoupling.With these three factors,OLEDs with nondoped emitting layers of the respective emitters both achieve nearly 100%exciton utilization and deliver over 30%external quantum efficiencies and ultralow efficiency roll-off at high brightness,which have not been observed in reported nondoped OLEDs.展开更多
Thermally activated delayed fluorescence(TADF)materials with aggregationinduced emission(AIE)features can overcome aggregation-caused quenching(ACQ)and emit intensely in aggregate states and thus have attracted enormo...Thermally activated delayed fluorescence(TADF)materials with aggregationinduced emission(AIE)features can overcome aggregation-caused quenching(ACQ)and emit intensely in aggregate states and thus have attracted enormous attention in the fields of high-efficiency organic light-emitting diodes,bioimaging,photodynamic therapy,photocatalysis,etc.However,their corresponding exact working mechanisms at the microscopic level are still far from clear.Herein,by carefully investigating the physical properties of our newly designed TADF material 6-(10H-spiro[acridine-9,9′-fluoren]-10-yl)nicotinonitrile in various states,we concluded that conformational isomerization plays an important role in realizing high photoluminescence quantum yields in its amorphous neat film state,in which the high-lying quasi-axial conformations with non-TADF features and low-lying quasiequal conformations with TADF characteristics serve as the host matrix and dopant,respectively,thus suppressing ACQ in disordered aggregate states.Our work not only offers a new possible microscopic mechanism by using conformational isomerization for the AIE-TADF phenomenon but also provides a novel method for designing high-efficiency AIE-TADF emitters.展开更多
基金National Natural Science Foundation of China,Grant/Award Numbers:51821002,52003185,52003186,52130304National Key Research&Development Program of China,Grant/Award Numbers:2020YFA0714601,2020YFA0714604+2 种基金Suzhou Key Laboratory of Functional Nano&Soft MaterialsCollaborative Innovation Center of Suzhou Nano Science&Technologythe 111 Project。
文摘High-performance nondoped organic light-emitting diodes(OLEDs)are promising technologies for future commercial applications.Herein,we synthesized two new thermally activated delayed fluorescence(TADF)emitters that enable us,for the first time,to combine three effective approaches for enhancing the efficiency of nondoped OLEDs.First,the two emitters are designed to have high steric hindrances such that their emitting cores will be suitably isolated from those of their neighbors to minimize concentration quenching.On the other hand,each of the two emitters has two stable conformations in solid films.In their neat films,molecules with the minority conformation behave effectively as dopants in the matrix composing of the majority conformation.One hundred percent exciton harvesting is thus theoretically feasible in this unique architecture of“self-doped”neat films.Furthermore,both emitters have relatively high aspect ratios in terms of their molecular shapes.This leads to films with preferred molecular orientations enabling high populations of horizontal dipoles beneficial for optical outcoupling.With these three factors,OLEDs with nondoped emitting layers of the respective emitters both achieve nearly 100%exciton utilization and deliver over 30%external quantum efficiencies and ultralow efficiency roll-off at high brightness,which have not been observed in reported nondoped OLEDs.
基金National Natural Science Foundation of China,Grant/Award Numbers:52130304,51821002,52003185,52003186National Key Research&Development Program of China,Grant/Award Numbers:2020YFA0714601,2020YFA0714604+3 种基金Suzhou Key Laboratory of Functional Nano&Soft MaterialsCollaborative Innovation Center of Suzhou Nano Science&Technologythe 111 ProjectJoint International Research Laboratory of Carbon-Based Functional Materials and Devices。
文摘Thermally activated delayed fluorescence(TADF)materials with aggregationinduced emission(AIE)features can overcome aggregation-caused quenching(ACQ)and emit intensely in aggregate states and thus have attracted enormous attention in the fields of high-efficiency organic light-emitting diodes,bioimaging,photodynamic therapy,photocatalysis,etc.However,their corresponding exact working mechanisms at the microscopic level are still far from clear.Herein,by carefully investigating the physical properties of our newly designed TADF material 6-(10H-spiro[acridine-9,9′-fluoren]-10-yl)nicotinonitrile in various states,we concluded that conformational isomerization plays an important role in realizing high photoluminescence quantum yields in its amorphous neat film state,in which the high-lying quasi-axial conformations with non-TADF features and low-lying quasiequal conformations with TADF characteristics serve as the host matrix and dopant,respectively,thus suppressing ACQ in disordered aggregate states.Our work not only offers a new possible microscopic mechanism by using conformational isomerization for the AIE-TADF phenomenon but also provides a novel method for designing high-efficiency AIE-TADF emitters.
基金supported by the National Natural Science Foundation of China (51773029, 51533005 and 51373190)the National Key Research & Development Program of China (2016YFB0401002)+1 种基金Collaborative Innovation Center of Suzhou Nano Science & Technology, the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)the 111 Project and Qing Lan Project, China
基金supported by the National Natural Science Foundation of China(51773029,52073040,51533005 and 51821002)the Fundamental Research Funds for the Central Universities(ZYGX2016Z010)the International Cooperation and Exchange Project of Science and Technology Department of Sichuan Province(2019YFH0057 and 2019YFH0059)。
