A tetradentate bis(pyridylpyrazolate) chelate, L, is assembled by connecting two bidentate 3-(trifluoromethyl)-5-(2-pyridyl)pyrazole chelates at the 6 position of the pyridyl fragment with a phenylamido appendage. This chelate was then utilized in the synthesis of three osmium(II) complexes, namely, [Os(L)(CO)2] (4), [Os(L)(PPh2Me)2] (5), and [Os(L)(PPhMe2)2] (6). Single-crystal X-ray structural analyses were executed on 4 and 5 to reveal the bonding arrangement of the L chelate. Phosphine-substituted derivatives 5 and 6 are highly emissive in both solution and the solid state, and their photophysical properties were measured and discussed on the basis of computational approaches. For application, fabrication and analysis of organic light-emitting diodes (OLEDs) were also carried out. The OLEDs using 5 and 6 as dopants exhibit saturated red emission with maximum external quantum efficiencies of 9.8% and 9.4%, respectively, which are higher than that of the device using [Ir(piq)3] as a red-emitting reference sample. Moreover, for documentation, 5 and 6 also achieve a maximum brightness of 19540 cd·m(-2) at 800 mA·cm(-2) (11.6 V) and 12900 cd·m(-2) at 500 mA·cm(-2) (10.5 V), respectively.
It is a well-known issue that the application of time-dependent density functional theory (TD-DFT) on charge transfer excitations often leads to a severe underestimation if the non-local exchange energy is not properly included. Here we perform a careful first-principles investigation on a specific molecular system that is known to exhibit thermally activated delayed fluorescence (TADF) phenomenon, using three different functions, B3LYP, CAM-B3LYP, and M06-2X. We find that even in functionals with more adequately described or fitted long-range exchange part, the triplet excitation energy levels may still show a large variation, indicating that the performance of a specific functional cannot solely be based on the comparison with the absorption or emission spectra. An inclusion of the solvent effect adds to further complexity. Since the efficiency of TADF is directly related to the energy gaps between low-lying singlet and triplet excited states, the proposed underlying mechanism to illustrate photophysical processes would be intimately associated to the chosen functional and the treatment of the polar medium.
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