Publication date: 15th December 2025
Phase-selective doping is an effective approach to enhance the thermoelectric performance of conjugated polymers (CPs), but how to translate this effect to other doping systems is unclear. Here, we employ a strategy based on a solvent affinity calculated by the Hansen Solubility Parameter (HSP) to control the phase-selective doping in the new n-type polymer 2PyDPP-2CNTVT with tetrabutylammonium fluoride (TBAF). Optical, electrical, and structural analysis reveal that a solvent with strong affinity for the polymer leads to an amorphous phase and distribute dopant both amorphous and crystalline domains, resulting in low electrical conductivity. In contrast, a solvent with partial affinity for both polymer and dopant lead to a bimodal phase, localizing dopant in the amorphous domain while preserving the crystalline domain. This partial affinity solvent can maintain a higher crystallinity at elevated doping concentration in a doped film, resulting in electrical conductivity nearly an order of magnitude higher than that produced with high-affinity solvents at similar doping concentrations. Grazing incidence wide-angle X-ray scattering (GIWAXS) confirms that dopant exclusion from crystalline domains preserves p-p stacking, favouring efficient charge transport. This work demonstrates a solvent-centric and phase-selective doping strategy to optimize solid-state ordering and fine-tune the electrical properties for various polymer and dopant systems.
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