Data-driven prediction of higher-order structure in carbon nanotube films for high thermoelectric power factor

Abstract We optimized the higher-order structures and semiconducting purity of single-walled carbon nanotubes (SWCNTs) to enhance the thermoelectric power factor PF by combining the thermoelectric random stick network (TE-RSN) method and a genetic algorithm. The PF of the optimized films was increased approximately fivefold for initial random structures. In addition, while the random structures showed the maximum PF when the ratio of semiconducting to metallic SWCNTs R s exceeded 0.98, the optimized structures converged to an R s of approximately 0.9. The optimized structures exhibited an increased local density and the peak of alignment angle distribution, leading to an increase in both the electrical conductivity and the Seebeck coefficient. We interpreted the increase in the Seebeck coefficient using a serial model. The results indicated that the reduction in the number of contacts within the paths and the subsequent increase in temperature difference on semiconducting SWCNTs led to the increase in the Seebeck coefficient.