Toward highly efficient deep-blue OLEDs: Tailoring the multiresonance-induced TADF molecules for suppressed excimer formation and near-unity horizontal dipole ratio.

Boron-based compounds exhibiting a multiresonance thermally activated delayed fluorescence are regarded promising as a narrowband blue emitter desired for efficient displays with wide color gamut. However, their planar nature makes them prone to concentration-induced excimer formation that broadens the emission spectrum, making it hard to increase the emitter concentration without raising CIE y coordinate. To overcome this bottleneck, we here propose o-Tol-ν-DABNA-Me, wherein sterically hindered peripheral phenyl groups are introduced to reduce intermolecular interactions, leading to excimer formation and thus making the pure narrowband emission character far less sensitive to concentration. With this approach, we demonstrate deep-blue OLEDs with y of 0.12 and full width at half maximum of 18 nm, with maximum external quantum efficiency (EQE) of ca. 33%. Adopting a hyperfluorescent architecture, the OLED performance is further enhanced to EQE of 35.4%, with mitigated efficiency roll-off, illustrating the immense potential of the proposed method for energy-efficient deep-blue OLEDs.

Dense Local Triplet States and Steric Shielding of a Multi-Resonance TADF Emitter Enable High-Performance Deep-Blue OLEDs.

Multi-resonance thermally activated delayed fluorescence (MR-TADF) molecules based on boron and nitrogen atoms are emerging as next-generation blue emitters for organic light-emitting diodes (OLEDs) due to their narrow emission spectra and triplet harvesting properties. However, intermolecular aggregation stemming from the planar structure of typical MR-TADF molecules that leads to concentration quenching and broadened spectra limits the utilization of the full potential of MR-TADF emitters. Herein, a deep-blue MR-TADF emitter, pBP-DABNA-Me, is developed to suppress intermolecular interactions effectively. Furthermore, photophysical investigation and theoretical calculations reveal that adding biphenyl moieties to the core body creates dense local triplet states in the vicinity of S1 and T1 energetically, letting the emitter harvest excitons efficiently. OLEDs based on pBP-DABNA-Me show a high external quantum efficiency (EQE) of 23.4% and a pure-blue emission with a Commission Internationale de L'Eclairage (CIE) coordinate of (0.132, 0.092), which are maintained even at a high doping concentration of 100 wt%. Furthermore, by incorporating a conventional TADF sensitizer, deep-blue OLEDs with a CIE value of (0.133, 0.109) and an extremely high EQE of 30.1% are realized. These findings provide insight into design strategies for developing efficient deep-blue MR-TADF emitters with fast triplet upconversion and suppressed self-aggregation.

Boron-Based Multi-Resonance TADF Emitter with Suppressed Intermolecular Interaction and Isomer Formation for Efficient Pure Blue OLEDs.

Multi-resonance (MR) thermally activated delayed fluorescent (TADF) emitters are highly attractive due to their superior color purity as well as efficient light-harvesting ability from singlets and triplets. However, boron and nitrogen-based MR-TADF emitters suffer from their strong π-π interaction owing to their rigid flat cores. Herein, a boron-based multi-resonance blue TADF emitter with suppressed intermolecular interaction and isomer formation is developed through a simple synthetic process by introducing meta-xylene and meta-phenyphenyl groups to the core. The MR-TADF emitter, mBP-DABNA-Me, shows a narrowband blue emission with a peak at 467 nm, along with full width at half maximum of 28 nm, and photoluminescence quantum yield of 97%. Notably, highly efficient pure blue organic light-emitting diode (OLED) is realized using mBP-DABNA-Me, showing a maximum external quantum efficiency of 24.3% and a stable blue emission with a Commission Internationale de L'Eclairage coordinate of (0.124, 0.140). The color purity of the OLED is maintained at a high doping concentration of over 20%, attributed to the suppressed intermolecular interaction between the MR emitters.

A Tuned Alternating D-A Copolymer Hole-Transport Layer Enables Colloidal Quantum Dot Solar Cells with Superior Fill Factor and Efficiency.

The need for optoelectronic and chemical compatibility between the layers in colloidal quantum dot (CQD) photovoltaic devices remains a bottleneck in further increasing performance. Conjugated polymers are promising candidates as new hole-transport layer (HTL) materials in CQD solar cells (CQD-SCs) owing to the highly tunable optoelectronic properties and compatible chemistries. A diketopyrrolopyrrole-based polymer with benzothiadiazole derivatives (PD2FCT-29DPP) as an HTL in these devices is reported. The energy level, molecular orientation, and hole mobility of this HTL are manipulated through molecular engineering. By levering the polymer's optical absorption spectrum complementary to that of the CQD active layer, EQE across the visible and near-infrared regions is maximized. As a result, a PD2FCT-29DPP-based device exhibits a fill factor of 70% and approximately 35% efficiency enhancement compared to a PTB7-based device.

Highly Efficient Deep-Blue OLEDs using a TADF Emitter with a Narrow Emission Spectrum and High Horizontal Emitting Dipole Ratio.

New blue (DBA-SAB) and deep-blue (TDBA-SAF) thermally activated delayed fluorescence (TADF) emitters are synthesized for blue-emitting organic-light emitting diodes (OLEDs) by incorporating spiro-biacridine and spiro-acridine fluorene donor units with an oxygen-bridged boron acceptor unit, respectively. The molecules show blue and deep-blue emission because of the deep highest occupied molecular energy levels of the donor units. Besides, both emitters exhibit narrow emission spectra with the full-width at half maximum (FWHM) of less than 65 nm due to the rigid donor and acceptor units. In addition, the long molecular structure along the transition dipole moment direction results in a high horizontal emitting dipole ratio over 80%. By combining the effects, the OLED utilizing DBA-SAB as the emitter exhibits a maximum external quantum efficiency (EQE) of 25.7% and 1931 Commission Internationale de l'éclairage (CIE) coordinates of (0.144, 0.212). Even a higher efficiency deep blue TADF OLED with a maximum EQE of 28.2% and CIE coordinates of (0.142, 0.090) is realized using TDBA-SAF as the emitter.

Enhanced Triplet-Triplet Annihilation of Blue Fluorescent Organic Light-Emitting Diodes by Generating Excitons in Trapped Charge-Free Regions.

Three new anthracene-cored molecules, 3,3'-(5-(10-(naphthalen-1-yl)anthracen-9-yl)-1,3-phenylene)dipyridine (AP3Py-Na), 3,3'-(5-(10-(naphthalen-2-yl)anthracen-9-yl)-1,3-phenylene)dipyridine (AP3Py-2Na), and 9,10-bis(3,5-di(pyridin-3-yl)phenyl)anthracene (ADP3Py), were synthesized to be used as an efficiency-enhancement layer (EEL) in blue fluorescent organic light-emitting diodes. Insertion of a very thin EEL (3 nm) between the deep blue emitting layer (EML) and the electron transport layer enhanced the external quantum efficiency (EQE) of the blue device by 44% compared to the device without the EEL, resulting in an EQE of 7.9% and a current efficiency of 9.0 cd A-1 at 1000 cd m-2; the CIE coordinates of the emitting color were (0.13, 0.14). The transient electroluminescence showed that the efficiency enhancement originates from the triplet-triplet annihilation (TTA) process in the EEL, followed by energy transfer to the emitting dye in the EML.

Molecular Engineering of a Donor-Acceptor Polymer To Realize Single Band Absorption toward a Red-Selective Thin-Film Organic Photodiode.

Herein, we explore the strategy of realizing a red-selective thin-film organic photodiode (OPD) by synthesizing a new copolymer with a highly selective red-absorption feature. PCZ-Th-DPP, with phenanthrocarbazole (PCZ) and diketopyrrolopyrrole (DPP) as donor and acceptor units, respectively, was strategically designed/synthesized based on a time-dependent density functional theory calculation, which predicted the significant suppression of the band II absorption of PCZ-Th-DPP due to the extremely efficient intramolecular charge transfer. We demonstrate that the synthesized PCZ-Th-DPP exhibits not only a high absorption coefficient within the red-selective band I region, as theoretically predicted, but also a preferential face-on intermolecular structure in the thin-film state, which is beneficial for vertical charge extraction as an outcome of a glancing incidence X-ray diffraction study. By employing PCZ-Th-DPP as a photoactive layer of Schottky OPD, to fully match its absorption characteristic to the spectral response of the red-selective OPD, we demonstrate a genuine red-selective specific detectivity in the order of 1012 Jones while maintaining a thin active layer thickness of ∼300 nm. This work demonstrates the possibility of realizing a full color image sensor with a synthetic approach to the constituting active layers without optical manipulation.