Abstract:In this work we report the optimisation of the solution processable TADF exciplex emitter in OLED devices formed by the small molecules 9-[2,8]-9-carbazole-[dibenzothiophene-S,S-dioxide]-carbazole (DCz-DBTO2) and 4,4′-cyclohexylidenebis[N,N-bis(4-methylphenyl)benzenamine] (TAPC). This exciplex, previously reported by Jankus et al. [1], has gave vacuum deposited devices having respectively current efficiency, power efficiency and EQE of 32.3 cd/A, 26.7 lm/W and 10.3 % obtained for with DCz-DBTO2:TAPC wt% ratio … Show more
“…Future investigations of the TADF mechanism may reveal the role of other vibrational modes by mechanically dampening them in similar ways as explored here. These alternative or lowamplitude vibrational motions may be a driving factor in non-D−A TADF emitters, such as exciplexes 56,57 and multiresonance boron−nitrogen materials, where large-amplitude modes for vibronic coupling like D−A dihedral angle rocking are not obvious. 58 The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.chemmater.0c03783.…”
We investigate a series of D−A molecules consisting of spiro[acridan-9,9′-fluorene] as the donor and 2-phenylenepyrimidine as the acceptor. In two of the materials, a spiro center effectively electronically isolates the D unit from (consequently) optically innocent yet structurally influential adamantyl side groups. In a third material, adamantyl groups attached directly to the acceptor strongly influence the electronic properties. Steady-state and time-resolved photophysical studies in solution, Zeonex polymer matrix, and neat films reveal that the substituents impact the efficiency of vibronic coupling between singlet and triplet states relevant to reverse intersystem crossing (rISC) and thermally activated delayed fluorescence (TADF), without significantly changing the singlet−triplet gap in the materials. The adamantyl groups serve to raise the segmental mass and inertia, thereby damping intramolecular motions (both vibrational and rotational). This substitution pattern reveals the role of large-amplitude (primarily D−A dihedral angle rocking) motions on reverse intersystem crossing (rISC), as well as smaller contributions from lowamplitude or dampened vibrations in solid state. We demonstrate that rISC still occurs when the high-amplitude motions are suppressed in Zeonex and discuss various vibronic coupling scenarios that point to an underappreciated role of intersegmental motions that persist in rigid solids. Our results underline the complexity of vibronic couplings in the mediation of rISC and provide a synthetic tool to enable future investigations of vibronic coupling through selective mechanical dampening with no impact on electronic systems.
“…Future investigations of the TADF mechanism may reveal the role of other vibrational modes by mechanically dampening them in similar ways as explored here. These alternative or lowamplitude vibrational motions may be a driving factor in non-D−A TADF emitters, such as exciplexes 56,57 and multiresonance boron−nitrogen materials, where large-amplitude modes for vibronic coupling like D−A dihedral angle rocking are not obvious. 58 The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.chemmater.0c03783.…”
We investigate a series of D−A molecules consisting of spiro[acridan-9,9′-fluorene] as the donor and 2-phenylenepyrimidine as the acceptor. In two of the materials, a spiro center effectively electronically isolates the D unit from (consequently) optically innocent yet structurally influential adamantyl side groups. In a third material, adamantyl groups attached directly to the acceptor strongly influence the electronic properties. Steady-state and time-resolved photophysical studies in solution, Zeonex polymer matrix, and neat films reveal that the substituents impact the efficiency of vibronic coupling between singlet and triplet states relevant to reverse intersystem crossing (rISC) and thermally activated delayed fluorescence (TADF), without significantly changing the singlet−triplet gap in the materials. The adamantyl groups serve to raise the segmental mass and inertia, thereby damping intramolecular motions (both vibrational and rotational). This substitution pattern reveals the role of large-amplitude (primarily D−A dihedral angle rocking) motions on reverse intersystem crossing (rISC), as well as smaller contributions from lowamplitude or dampened vibrations in solid state. We demonstrate that rISC still occurs when the high-amplitude motions are suppressed in Zeonex and discuss various vibronic coupling scenarios that point to an underappreciated role of intersegmental motions that persist in rigid solids. Our results underline the complexity of vibronic couplings in the mediation of rISC and provide a synthetic tool to enable future investigations of vibronic coupling through selective mechanical dampening with no impact on electronic systems.
“…[ 23–25 ] Generally, exciplex could be formed in bulk phase by mixing donor and acceptor together (denoted as bulk exciplex) or at the interface of donor and acceptor layers (named interfacial exciplex). [ 26 ] Although a series of vacuum‐deposited exciplex hosts have been developed and achieved very perfect device performance, [ 8,20–22 ] exciplex‐type hosts used for vacuum‐deposited OLEDs might not suitable for solution‐processed OLEDs, because of the very limited solubility and strong intermolecular interaction, [ 27 ] which may induce phase separation or serious intermolecular π‐π stacking. In addition, compared with vacuum‐deposited counterparts with multilayer structures, solution‐processed exciplex‐based OLEDs usually use a simple device structure, because of the dissolved problem between organic layers.…”
Two kinds of interfacial exciplex hosts formed between a dendritic oligocarbazole donor (H2) and two pyridine‐containing isomeric acceptors (B4PyMPM and B3PyMPM) are developed for solution‐processed thermally activated delayed fluorescent (TADF) organic light‐emitting diodes (OLEDs). The exciplex hosts exhibit small singlet−triplet energy splitting (90–110 meV) and distinct TADF effect which can convert triplet excitons into singlet ones and thus are beneficial for alleviating the triplet annihilation process. Notably, it is found that a small structural variation of acceptor from B4PyMPM (para‐linked pyridyl units) to B3PyMPM (meta‐linked pyridyl units) has a significant effect on enhancing carrier balance between donor and acceptor layers of interfacial exciplex, leading to greatly improved electroluminescent efficiency for the resultant devices. Solution‐processed TADF‐OLEDs based on H2/B3PyMPM interfacial exciplex host achieve the maximum power efficiency (PE) of 95.0 lm W−1 (85.5 cd A−1, 26.4 %), which is much better than that of H2/B4PyMPM devices (69.9 lm W−1) and represents the record PE for solution‐processed TADF‐OLEDs.
“…TADF emitters for solution-processed OLEDs are challenging to synthesize; they have a high molecular weight and their synthesis/production can be expensive. 41 Research in this area is at the beginning stage because of the lack of standardization for the fabrication protocol and performance evaluation of these devices. Unlike phosphorescent emitters-based OLEDs, generally, high efficiency in solution-processed TADF OLEDs is achieved in a complex multilayer architecture.…”
Section: Introductionmentioning
confidence: 99%
“…However, in this context, the role of some important device structural parameters, for instance, the thicknesses of the HTL and the emissive layer (EML) have been the highlight. All these specifications are the heart of the solution-processed fabrication because of the influence on electrical properties; , therefore, it should be considered as an essential component when understanding the charge carriers’ transport, which is not yet described to evaluate the effect on device stability and efficiency. TADF emitters for solution-processed OLEDs are challenging to synthesize; they have a high molecular weight and their synthesis/production can be expensive .…”
Section: Introductionmentioning
confidence: 99%
“…All these specifications are the heart of the solution-processed fabrication because of the influence on electrical properties; , therefore, it should be considered as an essential component when understanding the charge carriers’ transport, which is not yet described to evaluate the effect on device stability and efficiency. TADF emitters for solution-processed OLEDs are challenging to synthesize; they have a high molecular weight and their synthesis/production can be expensive . Research in this area is at the beginning stage because of the lack of standardization for the fabrication protocol and performance evaluation of these devices.…”
Simple
solution-processed structures of organic light-emitting
diodes (OLEDs) based on thermally activated delayed fluorescence (TADF)
have been demonstrated, but their efficiency and roll-off are still
problematic, mainly due to the difficulty in optimizing such device
structures. For the first time, solution-processed fabrication of
efficient TADF green OLEDs with a simple structure is demonstrated.
The emitter 2PXZ-OXD (2,5-bis(4-(10H-phenoxazin-10-yl)phenyl)-1,3,4-oxadiazole)
was dispersed in a poly(N-vinylcarbazole)/1,3-bis[2-(4-tert-butylphenyl)-1,3,4-oxadiazo-5-yl]benzene (OXD-7) host
matrix. Different emitter concentrations (1–10% wt) and different
layer thicknesses were applied. Photophysical analysis supports the
device structure configuration. The results show a balanced electrical
carrier transport, a low turn-on voltage (5 V), an external quantum
efficiency (EQE) of 7.5%, and a current efficiency of 16.2 cd/A with
a brightness of 7240 cd/m2. The device exhibited a suppressed
roll-off at 1000 cd/m2 (EQE: 7.15%). Simulations of charge
transport properties allowed to explain the results and to optimize,
opening interesting frameworks for simple solution-deposited large-area
OLEDs.
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