Construction of rigid TADF compounds allows us to minimize the conformational disorder and obtain single-exponential DF in solid hosts with an exceptional RISC rate of nearly 6 × 106 s−1 and high emission yield.
Time-resolved emission
spectra of thermally activated delayed fluorescence
(TADF) compounds in solid hosts demonstrate significant temporal shifts.
To explain the shifts, two possible mechanisms were suggested, namely,
slow solid-state solvation and conformational disorder. Here we employ
solid hosts with controllable polarity for analysis of the temporal
dynamics of TADF. We show that temporal fluorescence shifts are independent
of the dielectric constant of the solid film; however, these shifts
evidently depend on the structural parameters of both the host and
the TADF dopant. A ≤50% smaller emission peak shift was observed
in more rigid polymer host polystyrene than in poly(methyl methacrylate).
The obtained results imply that both the host and the dopant should
be as rigid as possible to minimize fluorescence instability.
The interest in organic materials exhibiting thermally activated delayed fluorescence (TADF) significantly increased in recent years owing to their potential application as emitters in highly efficient organic light emitting diodes (OLEDs). Simple modification of the molecular structure of TADF compounds through the selection of different electron-donating or accepting fragments opens great possibilities to tune the emission properties and rates. Here we present the synthesis of a series of novel pyrimidine–carbazole emitters and their photophysical characterization in view of effects of substituents in the pyrimidine ring on their TADF properties. We demonstrate that electron-withdrawing substituents directly connected to the pyrimidine unit have greater impact on the lowering of the energy gap between singlet and triplet states (ΔEST) for efficient TADF as compared to those attached through a phenylene bridge. A modification of the pyrimidine unit with CN, SCH3, and SO2CH3 functional groups at position 2 is shown to enhance the emission yield up to 0.5 with pronounced TADF activity.
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