Chiral TADF-Active Polymers for High-Efficiency Circularly Polarized Organic Light-Emitting Diodes.

A strategy of chiral donor-acceptor copolymerization is proposed to develop chiral nonconjugated polymers with thermally activated delayed fluorescence (TADF). Based on this strategy, two pairs of chiral polymers (R,R)-/(S,S)-pTpAcDPS and (R,R)-/(S,S)-pTpAcBP were synthesized. The alternating copolymerization of the chiral donors and acceptors could effectively separate the frontier molecular orbitals, which made the polymers show small ΔEST of 0.01-0.03 eV and efficient TADF properties. Moreover, the polymers also showed the quantum yield of up to 92 % and the circularly polarized luminescence. The solution-processed circularly polarized organic light-emitting diodes showed circularly polarized electroluminescence signals with high external quantum efficiencies of up to 22.1 % and maximum luminance of up to 34350 cd m-2 . This is the first report of CP-OLEDs based on chiral TADF polymer, which provides a useful and valuable guidance for the development of high-efficiency CPEL polymers.

Chiral Conjugated Thermally Activated Delayed Fluorescent Polymers for Highly Efficient Circularly Polarized Polymer Light-Emitting Diodes.

Two novel chiral conjugated polymers R-P and S-P designed and synthesized from a pair of circularly polarized thermally activated delayed fluorescence (CP-TADF) enantiomers are presented in this work. The two polymers exhibited excellent TADF properties with small singlet-triplet energy gaps (ΔEST) of 0.045 and 0.061 eV and relatively high photoluminescence quantum yields (PLQYs) of 72 and 76%, respectively. Besides, intense mirror-image circularly polarized luminescence signals were detected from R-P and S-P in both solution and film states with dissymmetry factors (|glum|) of up to 1.9 × 10-3. Furthermore, solution-processed circularly polarized polymer light-emitting diodes (CP-PLEDs) fabricated with R-P and S-P achieved high maximum external quantum efficiencies of 14.9 and 15.8% and high maximum brightness (Lmax) of 8940 and 12,180 cd/m2 with yellowish-green emission peaks at 546 and 544 nm, respectively. Moreover, intense circularly polarized electroluminescence signals with electroluminescence dissymmetry factors (gEL) of -1.5 × 10-3 and +1.6 × 10-3 were detected from the CP-PLED devices fabricated with R-P and S-P, respectively.

D-π*-A type planar chiral TADF materials for efficient circularly polarized electroluminescence.

Planar chiral organic fluorescent materials that exhibit high chiral stability, high efficiency and circularly polarized luminescence (CPL) currently remain an unresolved issue despite their promising applications in optical encryption and 3D-display. Herein, a pair of new donor-chiral π-acceptor (D-π*-A) type planar chiral thermally activated delayed fluorescence (TADF) enantiomers, namely R/S-PXZ-PT, are developed. Such a D-π*-A type structure completely suppresses the racemisation of the planar chirality, making it possible to prepare circularly polarized organic light-emitting diodes (CP-OLEDs) by vacuum deposition processing. Moreover, this design perfectly integrates the chiral unit into the luminescent unit to achieve intense CPL activity with luminescence asymmetry factors (glum) of ±1.9 × 10-3. Notably, the enantiomer-based devices exhibit a yellow coloured emission with a maximum external quantum efficiency (EQE) of 20.1%, and mirror-image circularly polarized electroluminescence signals with electroluminescence dissymmetry factors (gEL) of +1.5 × 10-3/-1.3 × 10-3. This work not only enriches the diversity of chiral TADF molecular design, but also provides a new perspective for the development of highly-efficient CP-OLEDs with stable planar chiral TADF materials.