Enhancement of thermoelectric power factor by modulation doping of bulk polycrystalline SnS / thin film PEDOT:PSS bilayer

Abstract

Modulation doping occurs in a heterojunction where a charge carrier-rich material transfers charge to a carrier-deficient material. The modulation-doped material is intentionally selected to have higher charge carrier mobility than the modulation dopant material, so that the overall electrical conductivity can be boosted. Although this modulation doping strategy has proven effective in enhancing power factor in thermoelectrics, selection criteria for such semiconductor couples have not been explicitly clarified, resulting in only a few discovered semiconductor couples available for modulation doping-driven thermoelectric systems [1-4]. Here, we (i) report an electronic band structure-based guideline to actualize modulation doping, (ii) reveal that hole-rich PEDOT:PSS can modulation dope otherwise undoped tin monosulfide (SnS) in their bilayered structure, (iii) prove that modulation doping is responsible for thermoelectric power factor enhancement by comparing computational and experimental Seebeck coefficient and electrical conductivity values. The optimized PEDOT:PSS thin film / SnS pellet bilayered structure had a 134.7 fold improvement in electrical conductivity and a 93.6 fold power factor enhancement over those of undoped SnS, with only a ~ 20 % decrease in Seebeck coefficient. The modulation doping effect can result in further power factor improvement when SnS becomes a nanoscale thin film or nanoparticles in the future.