N-Type Organic Thermoelectrics: Improved Power Factor by Tailoring Host–Dopant Miscibility

In this contribution, for the first time, the polarity of fullerene derivatives is tailored to enhance the miscibility between the host and dopant molecules. A fullerene derivative with a hydrophilic triethylene glycol type side chain (PTEG-1) is used as the host and (4-(1,3-dimethyl-2,3-dihydro-1H-benzoimidazol-2-yl)phenyl)dimethylamine n-DMBI) as the dopant. Thereby, the doping efficiency can be greatly improved to around 18% (<1% for a nonpolar reference sample) with optimized electrical conductivity of 2.05 S cm⁻¹, which represents the best result for solution-processed fullerene derivatives. An in-depth microstructural study indicates that the PTEG-1 molecules readily form layered structures parallel to the substrate after solution processing. The fullerene cage plane is alternated by the triethylene glycol side chain plane; the n-DMBI dopants are mainly incorporated in the side chain plane without disturbing the π–π packing of PTEG-1. This new microstructure, which is rarely observed for codeposited thin films from solution, formed by PTEG-1 and n-DMBI molecules explains the increased miscibility of the host/dopant system at a nanoscale level and the high electrical conductivity. Finally, a power factor of 16.7 µW m⁻¹ K⁻² is achieved at 40% dopant concentration. This work introduces a new strategy for improving the conductivity of solution-processed n-type organic thermoelectrics.

An efficient n-type doping system by tailoring host–dopant miscibility is demonstrated in this organic thermoelectric study. A record conductivity of 2.05 S cm⁻¹ for solution-processed fullerene derivative films is realized by enhancing the doping efficiency. The optimized system shows a power factor of 16.7 µW m⁻¹ K⁻² with a Seebeck coefficient of -284 µV K⁻¹, representing one of the best results for solution-processed n-type organic thermoelectrics.

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