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Thermally activated delayed fluorescence (TADF) was achieved when electron-rich triphenylene (Tpl) donors (D) were confined to a cage-based porous MOF host (NKU-111) composed of electron-deficient 2,4,6-tri(pyridin-4-yl)-1,3,5-triazine (Tpt) acceptor (A) as the ligand. The spatially-separated D and A molecules in a face-to-face stacking pattern generated strong through-space charge transfer (CT) interactions with a small singlet-triplet excited states energy splitting (∼0.1 eV), which enabled TADF. The resulting Tpl@NKU-111 exhibited an uncommon enhanced emission intensity as the temperature increased. Extensive steady-state and time-resolved spectroscopic measurements and first-principles simulations revealed the chemical and electronic structure of this compound in both the ground and low-lying excited states. A double-channel (T1, T2) intersystem crossing mechanism with S1 was found and explained as single-directional CT from the degenerate HOMO-1/HOMO of the guest donor to the LUMO + 1 of one of the nearest acceptors. The rigid skeleton of the compound and effective through-space CT enhanced the photoluminescence quantum yield (PLQY). A maximum PLQY of 57.36% was achieved by optimizing the Tpl loading ratio in the host framework. These results indicate the potential of the MOFs for the targeted construction and optimization of TADF materials.

Manipulating spatial alignment of donor and acceptor in host–guest MOF for TADF