Deep Learning Prediction of Triplet-Triplet Annihilation Parameters in Blue Fluorescent Organic Light-Emitting Diodes.

The triplet-triplet annihilation (TTA) ratio and the rate coefficient (kTT) of TTA are key factors in estimating the contribution of triplet excitons to radiative singlet excitons in fluorescent TTA organic light-emitting diodes. In this study, deep learning models are implemented to predict key factors from transient electroluminescence (trEL) data using new numerical equations. A new TTA model is developed that considers both polaron and exciton dynamics, enabling the distinction between prompt and delayed singlet decays with a fundamental understanding of the mechanism. In addition, deep learning models for predicting the kinetic coefficients and TTA ratio are established. After comprehensive optimization inspired by photophysics, determination coefficient values of 0.992 and 0.999 are achieved in the prediction of kTT and TTA ratio, respectively, indicating a nearly perfect prediction. The contribution of each kinetic parameter of polaron and exciton dynamics to the trEL curve is discussed using various deep-learning models.

Hybridization of short-range and long-range charge transfer excited states in multiple resonance emitter.

Multiple resonance (MR) thermally activated delayed fluorescence emitters have been actively studied as pure blue dopants for organic light-emitting diodes (OLEDs) because of excellent color purity and high efficiency. However, the reported MR emitter, 2,5,13,16-tetra-tert-butylindolo[3,2,1-jk]indolo[1',2',3':1,7]indolo[2,3-b]carbazole (tDIDCz) based on bis-fused indolocarbazole framework could not demonstrate efficient triplet-to-singlet spin crossover. In this work, we report two isomeric MR emitters designed to promote triplet exciton harvesting by reconstructing the electronic structure of tDIDCz. To manage excited states, strong electron donors were introduced at the 2,5-/1,6-position of tDIDCz. As a result, 2,5-positions managed tDIDCz shows long-range charge transfer characteristics while preserving the MR nature. Quantum chemical calculation demonstrates direct spin-orbit coupling by long-range charge transfer and spin-vibronic coupling assisted reverse intersystem crossing by short-range charge transfer simultaneously contribute to triplet-to-singlet spin crossover. Consequently, high performance blue OLED recorded a high external quantum efficiency of 30.8% at a color coordinate of (0.13, 0.13).

Color Stable Deep Blue Multi-Resonance Organic Emitters with Narrow Emission and High Efficiency.

The development of highly efficient and deep blue emitters satisfying the color specification of the commercial products has been a challenging hurdle in the organic light-emitting diodes (OLEDs). Here, deep blue OLEDs with a narrow emission spectrum with good color stability and spin-vibronic coupling assisted thermally activated delayed fluorescence are reported using a novel multi-resonance (MR) emitter built on a pure organic-based molecular platform of fused indolo[3,2,1-jk]carbazole structure. Two emitters derived from 2,5,11,14-tetrakis(1,1-dimethylethyl)indolo[3,2,1-jk]indolo[1',2',3':1,7]indolo[3,2-b]carbazole (tBisICz) core are synthesized as the MR type thermally activated delayed fluorescence emitters realizing a very narrow emission spectrum with a full-width-at-half-maximum (FWHM) of 16 nm with suppressed broadening at high doping concentration. The tBisICz core is substituted with a diphenylamine or 9-phenylcarbazole blocking group to manage the intermolecular interaction for high efficiency and narrow emission. The deep blue OLEDs achieve high external quantum efficiency (EQE) of 24.9%, small FWHM of 19 nm, and deep blue color coordinate of (0.16, 0.04) with good color stability with increase in doping concentration. To the authors' knowledge, the EQE in this work is one of the highest values reported for the deep blue OLEDs that achieve the BT.2020 standard.

Enhancing Horizontal Ratio of Transition Dipole Moment in Homoleptic Ir Complexes for High Outcoupling Efficiency of Organic Light-Emitting Diodes.

The light-emitting dipole orientation (EDO) of a phosphorescent emitter is a key to improving the external quantum efficiency (EQE) of organic light-emitting diodes (OLEDs) without structural modification of the device. Here, four homoleptic Ir complexes as a phosphorescent emitter are systematically designed based on the molecular structure of tris(2-phenylpyridine)iridium(III) (Ir(ppy)3 ) to control the EDO. Trimethylsilane, methyl, 2-methylpropyl, and cyclopentylmethyl group substituted to pyridine ring of the ligand contribute to the improvement of the EDO from 76.5% for Ir(ppy)3 to 87.5%. A linear relationship between the EDO and the aspect ratio (geometric anisotropy factor) is founded, implying the importance of the effective area for the nonbonding force between host and dopant molecules. Also, it is investigated that the EDO enhancement mainly originates from the vertical alignment of the C3 axis of molecule in the substrate axis rather than the change in the direction of the transition dipole alignment in the molecular axis. The optical simulation reveals that the outcoupling efficiency of phosphorescent OLEDs adopting new dopants reaches 38.4%. The green OLEDs exhibiting 28.3% of EQE, 103.2 cd A-1 of current efficiency, and 98.2 lm W-1 of power efficiency are demonstrated, which is understood to have little electrical loss.

Understanding the charge dynamics in organic light-emitting diodes using convolutional neural network.

Knowledge about the charge dynamics in organic light-emitting diodes (OLEDs) is a critical clue to optimize device architecture for enhancing the power efficiency and driving voltage characteristics in addition to the external quantum efficiency. In this work, we demonstrated that the charge behavior according to the operation voltage of OLEDs could be understood by introducing the convolutional neural network (CNN) of the machine learning framework without additional analysis of the unipolar charge devices. The CNN model trained using a two-dimensional (2D) modulus fingerprint simultaneously predicted the mobilities of the charge transport and emitting layers, realizing a deep understanding of the complicated data that humans cannot interpret. The machine learning model successfully describes the electrical properties of the organic layers in the actual devices configurated by different electron-transporting materials and the composition of cohosts in the emitting layer. For the first time, it was revealed that 2D fingerprints extracted using frequency- and voltage-dependent modulus spectra were effective data to represent comprehensive charge dynamics of OLEDs. The interpretation and perspective of the machine learning approach in this work were also discussed.

Multiple-Resonance Extension and Spin-Vibronic-Coupling-Based Narrowband Blue Organic Fluorescence Emitters with Over 30% Quantum Efficiency.

Achieving narrow-bandwidth emission and high external quantum efficiency (EQE) simultaneously is a challenge for next-generation blue-emitting organic light-emitting diodes (OLEDs). In this study, novel multiple-resonance thermally activated delayed fluorescence (MR-TADF) emitters are developed by fusing an indolocarbazole unit with two carbazole skeletons using para-oriented nitrogen atoms. The resulting rigid and planar π-system without electron-accepting atoms exhibits pure blue photoluminescence at 470 nm, reaching a 100% quantum yield with a full-width-at-half-maximum (FWHM) of 25 nm. Higher-level quantum chemistry calculations confirm an MR effect within the extended π-conjugation and an enhanced triplet-to-singlet crossover (104 s-1 ) through a reduced energy gap (ΔEST ) coupled with large spin-vibronic coupling mediated by low-lying triplet excited states. An OLED fabricated using the MR-TADF emitter with CIE color coordinates of (0.12, 0.16) exhibits a record high EQE of 30.9% and a small FWHM of 23 nm. With further optimization of the device structure, a high EQE of 33.8% is achieved without additional outcoupling enhancements owing to the near-perfect horizontal alignment of the emitting dipoles.

High Efficiency of over 25% and Long Device Lifetime of over 500 h at 1000 nit in Blue Fluorescent Organic Light-Emitting Diodes.

In this study, a multiple resonance (MR) type blue emitter is synthesized, characterized, and evaluated for highly efficient and stable blue fluorescent organic light-emitting diodes (OLEDs). The MR blue fluorescent emitter has a di-tert-butyl benzene substituent in the MR core structure to minimize quenching mechanisms by intermolecular interaction. The emitter shows a high photoluminescence quantum yield and small full width at half maximum of 22 nm, which realize high external quantum efficiency (EQE) of 11.4% in the single unit OLED and device lifetime up to 95% of the initial luminance (LT95 ) of 208 h at 1000 cd m-2 and over 10 000 h at 100 cd m-2 . The optimized tandem device of the new blue emitter achieves high EQE over 25% and extremely long LT95 of over 500 h at 1000 cd m-2 and 30 000 h at 100 cd m-2 . The lifetime of this work is one of the best data of blue OLED lifetime reported in the literature.

Asymmetric Blue Multiresonance TADF Emitters with a Narrow Emission Band.

In this study, we synthesized and characterized multiple resonance (MR) type blue thermally activated delayed fluorescence (TADF) emitters. Unlike many boron-based MR-TADF materials, the blue TADF emitters of this work had an asymmetric molecular structure with one boron, one oxygen, and one nitrogen. The aromatic units linked to the nitrogen were changed into diphenylamine, carbazole, dimethylacridine, and diphenylacridine to manage the light emission properties of the emitters. The TADF emitters exhibited a blue emission due to the weak electron-donating oxygen atom and the emission color was controlled by the aromatic unit connected to the nitrogen. The simple diphenylamine unit was effective in achieving real deep-blue emission for the BT2020 standard with a high external quantum efficiency (EQE), while the electron-rich nitrogen-based dimethylacridine and diphenylacridine accelerated the reverse intersystem crossing for high EQE and small EQE roll-off. Among the emitters, a diphenylamine-substituted emitter, 7-(tert-butyl)-9-phenyl-9H-5-oxa-9-aza-13b-boranaphtho[3,2,1-de]anthracene (B-O-dpa), showed a maximum external quantum efficiency of 16.3%, a small full width at half-maximum of 32 nm, and a real deep-blue color coordinate of (0.15, 0.05).

Triplet Exciton Upconverting Blue Exciplex Host for Deep Blue Phosphors.

A thermally activated delayed fluorescence (TADF)-type exciplex host employing a novel electron-transport type (n-type) type host managing positive polarons and stabilizing excitons was developed to elongate the device lifetime of deep blue phosphorescent organic light-emitting diodes (PhOLEDs). The bipolar n-type host was designed to prevent hole leakage and secure hole stability while being stabilized under excitons by introducing a CN-modified carbazole moiety as a weak donor. The TADF-type exciplex host-based blue PhOLEDs showed high (above 20 %) quantum efficiency with a deep blue color coordinate of (0.14, 0.16) and elongated device lifetime. The device operational lifetime of the blue PhOLEDs bearing the TADF-type exciplex host was extended by more than twice compared to that of the exciplex-free unipolar host. This work suggested a design concept of the n-type host to develop the TADF-type exciplex host for deep blue phosphors to reach a long lifespan in the deep blue PhOLEDs.

Strategic Synchronization of 7,7-Dimethyl-5,7-dihydroindeno[2,1-b]carbazole for Narrow-Band, Pure Violet Organic Light-Emitting Diodes with an Efficiency of > 5% and a CIE y Coordinate of < 0.03.

A novel violet emitter, 1,3-bis[10,10-dimethyl-10H-indeno[2,1-b]]indolo[3,2,1-jk]indolo[1',2',3':1,7]indolo[3,2-b]carbazole (m-FLDID), was designed and synthesized by meta-oriented bis-fusion of two 7,7-dimethyl-5,7-dihydroindeno[2,1-b]carbazole (DMID) subunits for use in a pure violet organic light-emitting diode (OLED). Incorporation of the DMID subunits effectively reduced the nonradiative recombination rate, improving the photoluminescence quantum yield of the m-FLDID emitter. The meta-oriented bis-fusion of the two DMID subunits not only triggered an alternative distribution of the frontier orbitals but also effectively locked the π-conjugation chain, which ultimately resulted in a narrow-band, pure violet emission of the m-FLDID emitter. Doped m-FLDID devices possessed an external quantum efficiency (EQE) of > 5%, pure violet emission with a maximum at 407 nm, a narrow full width at half-maximum of 17 nm, and a Commission Internationale de l'éclairage y coordinate of less than 0.03. This is the first work reporting an EQE of > 5% and an extremely narrow emission spectrum for a pure violet emitter.