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In recent years, pure organic room‐temperature phosphorescence (RTP) with highly efficient and long‐persistent afterglow has drawn substantial awareness. Commonly, spin‐orbit coupling can be improved by introducing heavy atoms into pure‐organic molecules. However, this strategy will simultaneously increase the radiative and non‐radiative transition rate, further resulting in dramatic decreases in the excited state lifetime and afterglow duration. Here in this work, a highly symmetric bird‐like structure tetraphenylene (TeP), and its three symmetrical halogenated derivatives (TeP−F, TeP−Cl and TeP−Br) are synthesized, while their RTP properties and mechanisms are systematically investigated by both theoretical and experimental approaches. As the results, the rigid, highly twisted conformation of TeP restricts the non‐radiative processes of RTP and gives rise to the enhancement of electron‐exchange, which can contribute to the RTP radiation process. Despite the faint RTP of the bromine and chlorine‐substituted ones (TeP−Br, TeP−Cl), the fluoro‐substituted TeP−F exhibited a long phosphorescent lifetime up to 890 ms, corresponding to an extremely long RTP afterglow over 8 s, which could be incorporated into the best series of non‐heavy‐atom RTP materials reported in previous literature. [ABSTRACT FROM AUTHOR]

Organic materials with excitation wavelength‐dependent (Ex‐de) emission are highly attractive for anticounterfeiting, optoelectronics and bioassay applications; however, the realization of Ex‐de fluorescence, independent of aggregation states, remains a challenge. We herein report a photoinduced electron transfer (PeT) strategy to design Ex‐de fluorescence materials by manipulating the relaxation pathways of multiple excited states. As expected, the o‐carborane dyad presents a clear Ex‐de fluorescence colour in the aggregated states, resulting from the tunable relative intensity of the dual‐fluorescence spectra. Taking TP[1]B as an example, the amorphous powders emitted bright blue‐violet, white and yellow colours under 390 nm, 365 nm and 254 nm UV illumination, respectively. Importantly, multicolour, flexible and transparent films as well as an anticounterfeiting application using this o‐carborane dyad are demonstrated. [ABSTRACT FROM AUTHOR]

[Display omitted] • Deep-red emissive material TPANZPPICN with AIEE property is synthesized. • The "hot-exciton" mechanism is clearly revealed with MEL experiment. • Doped OLED of TPANZPPICN shows high EQE of 8.0 % at 660 nm. Organic deep-red fluorescent materials have a wide range of applications in organic light-emitting diodes (OLEDs), biological imaging, night-vision equipment, and other fields. Here, we designed and synthesized a new deep-red emissive donor–acceptor (D-A) compound TPANZPPICN , whose non-doped OLED achieves stable pure deep-red electroluminescence (EL) at 692 nm with a maximum external quantum efficiency (EQE) of 2.67 % in non-doped OLED and a maximum EQE of 7.96 % at 660 nm in doped OLED. Magneto-electroluminescence (MEL) measurements reveal a negative response in the doped OLED, which is a significant character of reversed intersystem crossing (RISC) on high-lying excited states. Both theoretical calculations and experimental results confirm that the hot-exciton mechanism is responsible for the high efficiency EL of doped OLED, which proves to be a novel approach to realize the efficient deep-red organic fluorescent OLEDs. [ABSTRACT FROM AUTHOR]

Rational regulation on the hybrid local and charge-transfer (HLCT) excited state is crucial for the optimization of light color, especially those of the blue-emissive materials. In this work, two rigid, orthogonal donor-acceptor (D-A) materials are designed and synthesized using the tripenylamine-phenanthroimidazole backbone donor and triphenyltriazine as the acceptor, with different distance between the donor and acceptor units. The shorter distanced DRZ-TPM forms a typical CT excited state, and its organic light emitting diode (OLED) produced green electroluminescence with maximum external quantum efficiency (EQE max) of 5.0%. To regulate the light color, we inserted a phenyl ring to increase the donor-acceptor distance for a reduced CT component. The new material TRZ-TPM achieves sky-blue electroluminescence at 452 nm with EQE max of 2.5% in doped OLED. Furthermore, TRZ-TPM showed obvious excimer emission in the aggregated state, and the non-doped OLED performed reduced opening-voltage comparing to the doped OLED, owing to the better formation of intermolecular charge-transfer state. Two orthogonal donor-acceptor (D-A) materials are designed and synthesized to investigate both intramolecular and intermolecular effect on the hybrid-local and charge-transfer (HLCT) excited state. The extended D-A distance gives rise to the optimized blue-purity and the dimerization can help lowering the turn-on voltage in organic light emitting diode (OLED). [Display omitted] • Rigidly, orthogonally linked donor-acceptor structured, hybrid local and charge-transfer (HLCT) materials are synthesized. • Extended donor-acceptor distance weakens the charge-transfer and realizes better blue purity and electrofluorescence. • A special excimer emission phenomenon with its formation mechanism is discovered and explored. [ABSTRACT FROM AUTHOR]

In this work, two novel D-π-A compounds (PXZ-FR-DRZ and CZ-FR-DRZ) are designed and synthesized, aiming at the excited-state regulation from thermally-activated delayed fluorescence (TADF) to hybridized local and charge-transfer (HLCT) emission. This change of excited-state nature can be ascribed to the weakened electron-donating ability of carbazole relative to phenoxazine, together with the decreased twisting angle between carbazole and fluorine units. As a result of twisted charge-transfer (CT) excited state, the doped organic light-emitting diode (OLED) of PXZ-FR-DRZ demonstrates a blue-green TADF electroluminescence (EL) with a maximum external quantum efficiency (EQE max) of 11.5%, while its non-doped device shows a much lower EQE max. Due to HLCT state of CZ-FR-DRZ , both its doped and non-doped OLEDs achieve the deep-blue non-delayed EL with the satisfied external quantum efficiency (EQE), especially for the excellent efficiency roll-off. Overall, this excited-state transformation between TADF and HLCT allows us to harvest the better comprehensive performance of OLED emitters for the practical applications, which provides a feasible solution for the development of OLED industry. Two different donors (phenoxazine and carbazole) are designed to match the same acceptor of 2,4-diphenyl-1,3,5-triazine (DRZ) through a π-bridged linkage of 9,9-dimethyl-9H-fluorene (FR), resulting in two novel D-π-A molecules of PXZ-FR-DRZ and CZ-FR-DRZ , respectively. The PXZ-FR-DRZ realizes a blue-green thermally-activated delayed fluorescence (TADF) with high external quantum efficiency (EQE) in the doped organic light-emitting diodes (OLEDs) due to the twisted charge-transfer (CT) excited state, whereas the CZ-FR-DRZ achieves a deep-blue non-doped OLED with the better comprehensive performance as a result of the hybridized local and charge-transfer (HLCT) state. [Display omitted] • Two D-π-A materials CZ-FR-DRZ and PXZ-FR-DRZ are synthesized with HLCT and TADF properties respectively. • The TADF PXZ-FR-DRZ exhibits higher EQE than CZ-FR-DRZ. • As an HLCT material, CZ-FR-DRZ displays high performance in non-doped OLED. • The conversion between HLCT and TADF is investigated by changing different donors. [ABSTRACT FROM AUTHOR]