Precise Donor-Acceptor Engineering for High-Mobility Ambipolar Emissive Polymer Semiconductors

Abstract

Conjugated polymers are promising platforms for integrated optoelectronics, yet in most reported high mobility diketopyrrolopyrrole (DPP)-based semiconductors, strong intermolecular aggregation and narrow bandgaps suppress luminescence, limiting their applicability in multifunctional devices. The concurrent realization of efficient charge transport and strong thin film emission therefore remains a fundamental challenge. Here, we report two novel DPP-derived polymers, PTFBVDPP-V and PTFBVDPP-TVT, synthesized via Stille coupling through precise donor-acceptor (D-A) engineering. Both polymers possess highly coplanar backbones, forming continuous fiber networks and ordered crystalline films with close intermolecular π-π stacking. Polymer PTFBVDPP-V functions as a unipolar n-type semiconductor with an electron mobility (μ_e) of 2.61 cm²·V⁻¹·s⁻¹ but negligible emission. In contrast, precise D–A modulation in PTFBVDPP-TVT enables balanced ambipolar transport with a hole mobility of 1.52 cm²·V⁻¹·s⁻¹ and an electron mobility of 1.15 cm²·V⁻¹·s⁻¹, while retaining a thin-film photoluminescence quantum yield (Φ) of 6.5%. This combination delivers a maximum Φ·μ_e exceeding 10⁻² cm²·V⁻¹·s⁻¹, establishing a record performance among high-mobility ambipolar emissive polymer semiconductors and breaking the long-standing trade-off between charge transport and luminescence in conventional high-mobility DPP-based systems.

Keywords

Diketopyrrolopyrrole / Molecular design / High mobility / Ambipolar / Intense luminescence / Polymer semiconductors / Organic field-effect transistors / Organic light-emitting transistors

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