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Hydrogen-Bonded Two-Component Ionic Crystals Showing Enhanced Long-Lived Room-Temperature Phosphorescence via TADF-Assisted F?rster Resonance Energy Transfer
摘要： Molecular room-temperature phosphorescent (RTP) materials with long-lived excited states have attracted widespread attention in the fields of optical imaging, displays, and sensors. However, accessing ultralong RTP systems remains challenging and examples are still limited to date. Herein, a thermally activated delayed fluorescence (TADF)-assisted energy transfer route for the enhancement of persistent luminescence with an RTP lifetime as high as 2 s, which is higher than that of most state-of-the-art RTP materials, is proposed. The energy transfer donor and acceptor species are based on the TADF and RTP molecules, which can be self-assembled into two-component ionic salts via hydrogen-bonding interactions. Both theoretical and experimental studies illustrate the occurrence of effective F?rster resonance energy transfer (FRET) between donor and acceptor molecules with an energy transfer efficiency as high as 76%. Moreover, the potential for application of the donor–acceptor cocrystallized materials toward information security and personal identification systems is demonstrated, benefitting from their varied afterglow lifetimes and easy recognition in the darkness. Therefore, the work described in this study not only provides a TADF-assisted FRET strategy toward the construction of ultralong RTP, but also yields hydrogen-bonding-assembled two-component molecular crystals for potential encryption and anti-counterfeiting applications.
关键词： thermally activated delayed fluorescence,energy transfer,cocrystallization,hydrogen bonding self-assembly,room-temperature phosphorescence
更新于2025-09-10 09:29:36
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Recent Advances in Conjugated TADF Polymer Featuring in Backbone-Donor/Pendant-Acceptor Structure: Material and Device Perspectives
摘要： Along with the persistent research interest in organic light-emitting diode (OLED) display and lighting technology, a new studying topic is now focused on developing thermally activated delayed fluorescence (TADF) polymer emitters, with the purpose to achieve high-performance cost-effective, solution-processed OLEDs (s-OLEDs) purely from fluorescent-type materials. However, research in this topic is in its infancy about the designing rules of polymer structures, photophysical mechanisms and the correlated devices. In this Personal Account, mainly from our personal experience we will shortly introduce the historical developments, status and perspectives about one representative kinds of TADF polymers, i. e. the conjugated TADF polymers featuring in backbone-donor/pendant-acceptor (BDPA) structure scaffold, which shows very promising electroluminescent (EL) performance even using simple s-OLED structure. Special attention is focused on illustrate the molecular designing & synthesis motivation, chemistry & device tactics towards solving the limiting factors about the quantum yields and aggregation-quenching tendency in solid states. Further challenges and strategies towards optimizing their overall EL performance, e. g. simultaneous achieving extremely high external quantum efficiency, power efficiency and low roll-off rate, are also discussed.
关键词： thermally activated delayed fluorescence,exciplex,solution-processed,polymer,organic light-emitting diodes
更新于2025-09-10 09:29:36
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Highly efficient thermally activated delayed fluorescence with slow reverse intersystem crossing
摘要： We report an efficient luminescent molecule exhibiting thermally activated delayed fluorescence with a long-delayed fluorescence lifetime of 0.8 ms. Although the reverse intersystem crossing rate constant is small at 2.1 × 103 s?1, the molecule shows a high photoluminescence quantum yield of 89±2%, indicating the suppression of nonradiative decay from the triplet state.
关键词： Long triplet lifetime,Thermally activated delayed fluorescence (TADF),Reverse intersystem crossing (RISC)
更新于2025-09-10 09:29:36
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Kinetic Modelling of Transient Photoluminescence from Thermally Activated Delayed Fluorescence
摘要： A simplified state model and associated rate equations are used to extract the reverse intersystem crossing and other key rate constants from transient photoluminescence measurements of two high performance thermally activated delayed fluorescence materials. The values of the reverse intersystem crossing rate constant are in close agreement with established methods, but do not require a priori assumption of exponential decay kinetics, nor any additional steady state measurements. The model is also applied to measurements at different temperatures and found to reproduce previously reported thermal activation energies for the thermally activated delayed fluorescence process. Transient absorption measurements provide independent confirmation that triplet decay channels (neglected here) have no adverse effect on the fitting.
关键词： Thermally Activated Delayed Fluorescence,Transient Photoluminescence,Reverse Intersystem Crossing,Kinetic Modelling
更新于2025-09-10 09:29:36
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Heteroleptic Copper(I) Complexes Prepared from Phenanthroline and Bis-Phosphine Ligands: Rationalization of the Photophysical and Electrochemical Properties
摘要： The electronic and structural properties of ten heteroleptic [Cu(NN)(PP)]+ complexes have been investigated. NN indicates 1,10-phenanthroline (phen) or 4,7-diphenyl-1,10-phenanthroline (Bphen); each of these ligands is combined with five PP bis-phosphine chelators, i.e., bis(diphenylphosphino)methane (dppm), 1,2-bis(diphenylphosphino)ethane (dppe), 1,3-bis(diphenylphosphino)propane (dppp), 1,2-bis(diphenylphosphino)benzene (dppb), and bis[(2-diphenylphosphino)phenyl] ether (POP). All complexes are mononuclear, apart from those based on dppm, which are dinuclear. Experimental data—also taken from the literature and including electrochemical properties, X-ray crystal structures, UV?vis absorption spectra in CH2Cl2, luminescence spectra and lifetimes in solution, in PMMA, and as powders—have been rationalized with the support of density functional theory calculations. Temperature dependent studies (78?358 K) have been performed for selected complexes to assess thermally activated delayed fluorescence. The main findings are (i) dependence of the ground-state geometry on the crystallization conditions, with the same complex often yielding different crystal structures; (ii) simple model compounds with imposed C2v symmetry ([Cu(phen)(PX3)2]+; X = H or CH3) are capable of modeling structural parameters as a function of the P?Cu?P bite angle, which plays a key role in dictating the overall structure of [Cu(NN)(PP)]+ complexes; (iii) as the P?Cu?P angle increases, the energy of the metal-to-ligand charge transfer absorption bands linearly increases; (iv) the former correlation does not hold for emission spectra, which are red-shifted for the weaker luminophores; (v) the larger the number of intramolecular π-interactions within the complex in the ground state, the higher the luminescence quantum yield, underpinning a geometry locking effect that limits the structural flattening of the excited state. This work provides a general framework to rationalize the structure?property relationships of [Cu(NN)(PP)]+, a class of compounds of increasing relevance for electroluminescent devices, photoredox catalysis, and solar-to-fuels conversion, which so far have been investigated in an unsystematic fashion, eluding a comprehensive understanding.
关键词： electrochemical properties,bis-phosphine ligands,photophysical properties,phenanthroline,thermally activated delayed fluorescence,density functional theory,heteroleptic copper(I) complexes
更新于2025-09-09 09:28:46
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Photo-Physical Properties of Thermally Activated Delayed Fluorescent Materials upon Distortion of Central Axis of Donor Moiety
摘要： In this study, we showed the distortion of central axis of donor moiety can switch critically the rate of reverse intersystem crossing (kRISC) process, which is the trigger point to modulate the lifetime of delayed fluorescence. To achieve kRISC what we desired (105 to 106 s-1) in a series of donor-acceptor-donor (D-A-D) type thermally activated delayed fluorescence (TADF) materials, the donor groups (phenoxazine and phenothiazine) was selectively introduced. Maintaining the near orthogonality between donor and acceptor (benzonitrile) moiety, the occurrence of the distortion of central axis of donor moiety could make the effect of locally excited triplet state (3LE). In other words, the interaction between 3LE and the charge transfer counterparts (i.e., 1CT and 3CT) contributes an opposite propensity of kRISC for each target TADF materials when those are dissolved in solution and condensed in solid-state. Herein, we have theoretically and experimentally shown the photo-physical behavior of common D-A-D type TADF upon the different system.
关键词： Reverse Intersystem Crossing,Thermally Activated Delayed Fluorescence,Benzonitrile,Phenoxazine,Donor-Acceptor-Donor,Phenothiazine
更新于2025-09-09 09:28:46
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Production and Characterization of Vacuum Deposited Organic Light Emitting Diodes
摘要： A method for producing simple and efficient thermally-activated delayed fluorescence organic light-emitting diodes (OLEDs) based on guest-host or exciplex donor-acceptor emitters is presented. With a step-by-step procedure, readers will be able to repeat and produce OLED devices based on simple organic emitters. A patterning procedure allowing the creation of personalized indium tin oxide (ITO) shape is shown. This is followed by the evaporation of all layers, encapsulation and characterization of each individual device. The end goal is to present a procedure that will give the opportunity to repeat the information presented in cited publication but also using different compounds and structures in order to prepare efficient OLEDs.
关键词： ambipolar,Donor-Acceptor,Thermally Activated Delayed Fluorescence,exciplex,Organic Electronics,patterning,thermal evaporation,Issue 141,OLED,Engineering
更新于2025-09-09 09:28:46
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Importance of Chromophore Rigidity on the Efficiency of Blue Thermally Activated Delayed Fluorescence Emitters
摘要： Four new symmetrical donor?acceptor?donor (D?A?D)-type molecules are reported with diphenylamine (DPA) or 10,11-dihydro-5H-dibenz[b,f ]azepine (Az) as electron donors and 9,9-dimethylthioxanthene-S,S-dioxide (TXO2) as the electron acceptor. The donors are attached at different positions on the acceptor core: either para or meta to the sulfone unit. This series provides new insights into the effects of chromophore rigidity/flexibility on the efficiency of thermally activated delayed fluorescence (TADF). The molecules have been characterized by X-ray crystallography, by in-depth photophysical studies, and by theoretical calculations. The clear differences observed in the photophysical properties when using DPA or Az as a donor are shown to originate from different geometries of the donor unit which, in turn, influence the geometry of the nitrogen lone pair and the donating strength of the corresponding fragment. Thus, a para-substituted Az derivative demonstrated blue TADF in polar media, while the compounds with more flexible DPA units did not show delayed fluorescence. To obtain deep-blue emitters, weaker donating units are needed. A more flexible donor unit leads to increased local excited state (donor) LE emission and reduced TADF. However, a certain amount of flexibility has to be present to ensure deep-blue TADF.
关键词： chromophore rigidity,blue emitters,donor-acceptor-donor,photophysical properties,thermally activated delayed fluorescence
更新于2025-09-04 15:30:14
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Cell-Penetrating Peptides Transport Noncovalently Linked Thermally Activated Delayed Fluorescence Nanoparticles for Time-Resolved Luminescence Imaging
摘要： Luminescent probes and nanoparticles (NPs) with long excited state lifetimes are essential for time-resolved biological imaging. Generally, cell membranes are physiological barriers that could prevent the uptake of many unnatural compounds. It is still a big challenge to prepare biocompatible imaging agents with high cytomembrane permeability, especially for nonmetallic NPs with long-lived luminescence. Herein, an amphiphilic cell-penetrating peptide, F6G6(rR)3R2, was designed to transport hydrophobic fluorophores across cellular barriers. Three classical thermally activated delayed fluorescence (TADF) molecules, 4CzIPN, NAI-DPAC, and BTZ-DMAC, could self-assemble into well-dispersed NPs with F6G6(rR)3R2 in aqueous solution. These NPs showed low cytotoxicity and could penetrate membranes easily. Moreover, long-lived TADF enabled them to be used in time-resolved luminescence imaging in oxygenic environments. These findings greatly expanded the applications of cell-penetrating peptides for delivery of molecules and NPs by only noncovalent interactions, which were more flexible and easier than covalent modifications.
关键词： cell-penetrating peptide,Luminescent probes,time-resolved biological imaging,nanoparticles,noncovalent interactions,thermally activated delayed fluorescence
更新于2025-09-04 15:30:14
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High Performance Thermally Activated Delayed Fluorescence Sensitized Organic Light‐Emitting Diodes
摘要： Recently, organic light-emitting diodes (OLEDs) employing thermally activated delayed fluorescence (TADF) materials have aroused huge attention in both academia and industry. Compared with fluorescent and phosphorescent materials, TADF materials can theoretically capture 100 % excitons without incorporating noble metals, making them effective emitters and hosts for OLEDs simultaneously. Here, in this review, our recent works on mechanisms and materials of high performance TADF-sensitized phosphorescent (TSP) OLEDs, TADF-sensitized fluorescent (TSF) OLEDs and TADF-sensitized TADF (TST) OLEDs are summarized. Finally, we propose the outlook for the further development and application of TADF-sensitized OLEDs.
关键词： bipolar host,Dexter energy transfer,organic light-emitting diodes,F?rster energy transfer,thermally activated delayed fluorescence
更新于2025-09-04 15:30:14