Freeman, DME; Musser, AJ; Frost, JM; Stern, HL; Forster, AK; Fallon, KJ; Rapidis, AG; ... Bronstein, H; + view all Freeman, DME; Musser, AJ; Frost, JM; Stern, HL; Forster, AK; Fallon, KJ; Rapidis, AG; Cacialli, F; McCulloch, I; Clarke, TM; Friend, RH; Bronstein, H; - view fewer (2017) Synthesis and Exciton Dynamics of Donor-Orthogonal Acceptor Conjugated Polymers: Reducing the Singlet-Triplet Energy Gap. Journal of the American Chemical Society , 139 (32) pp. 11073-11080. 10.1021/jacs.7b03327.

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Abstract

The presence of energetically low-lying triplet states is a hallmark of organic semiconductors. Even though they present a wealth of interesting photophysical properties, these optically dark states significantly limit optoelectronic device performance. Recent advances in emissive charge-transfer molecules have pioneered routes to reduce the energy gap between triplets and "bright" singlets, allowing thermal population exchange between them and eliminating a significant loss channel in devices. In conjugated polymers, this gap has proved resistant to modification. Here, we introduce a general approach to reduce the singlet-triplet energy gap in fully conjugated polymers, using a donor-orthogonal acceptor motif to spatially separate electron and hole wave functions. This new generation of conjugated polymers allows for a greatly reduced exchange energy, enhancing triplet formation and enabling thermally activated delayed fluorescence. We find that the mechanisms of both processes are driven by excited-state mixing between π-π*and charge-transfer states, affording new insight into reverse intersystem crossing.

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