Efficient organic light-emitting diodes have been developed using emitters containing rare metals, such as platinum and iridium complexes. However, there is an urgent need to develop emitters composed of more abundant materials. Here we show a thermally activated delayed fluorescence material for organic light-emitting diodes, which realizes both approximately 100% photoluminescence quantum yield and approximately 100% up-conversion of the triplet to singlet excited state. The material contains electron-donating diphenylaminocarbazole and electron-accepting triphenyltriazine moieties. The typical trade-off between effective emission and triplet-to-singlet up-conversion is overcome by fine-tuning the highest occupied molecular orbital and lowest unoccupied molecular orbital distributions. The nearly zero singlet–triplet energy gap, smaller than the thermal energy at room temperature, results in an organic light-emitting diode with external quantum efficiency of 29.6%. An external quantum efficiency of 41.5% is obtained when using an out-coupling sheet. The external quantum efficiency is 30.7% even at a high luminance of 3,000 cd m−2.
Triarylboron compounds have attracted much attention, and found wide use as functional materials because of their electron-accepting properties arising from the vacant p orbitals on the boron atoms. In this study, we design and synthesize new donor-acceptor triarylboron emitters that show thermally activated delayed fluorescence. These emitters display sky-blue to green emission and high photoluminescence quantum yields of 87-100 % in host matrices. Organic light-emitting diodes using these emitting molecules as dopants exhibit high external quantum efficiencies of 14.0-22.8 %, which originate from efficient up-conversion from triplet to singlet states and subsequent efficient radiative decay from singlet to ground states.
Visible light driven hydrogen (H2) production from water is a promising strategy to convert and store solar energy as chemical energy. Covalent organic frameworks (COFs) are front runners among different classes of organic photocatalyst, owing to their tunable porosity, crystallinity, optical and electronic properties.Photocatalytic activity of COFs depends on numerous factors such as band gap, crystallinity, porosity, exciton migration, charge separation and transport, stability etc. However, it is challenging to fine tune all these factors simultaneously to enhance the photocatalytic activity. Hence, in this report, we have prioritized the key factors for efficient photocatalytic H2 production through structure-property-activity relationship combined with microwave spectroscopy and first-principles calculations. Careful molecular engineering allowed us to tune the light absorption (i.e. band gap), crystallinity, porosity, layer stacking and charge carrier generation and transport of a series of isoreticular COFs. We have assessed how these properties and the interplay between them impact photocatalytic activity of studied COFs. From the structure-property-activity relationship, we found that light absorption and charge carrier generation and transport are the prime factors, which influence the photocatalytic H2 production of COFs in much greater extent than other factors. File list (2)download file view on ChemRxiv Ghosh_etal_Manuscript.pdf (5.34 MiB) download file view on ChemRxiv Ghosh_etal_SI.pdf (4.80 MiB) Scheme 1. Chemical structures of the building blocks along with corresponding molecular lengths and torsional angles. Reaction scheme for the synthesis of COFs under different solvothermal conditions, condition A and condition B.
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