Polymer morphology and interfacial charge transfer dominate over energy-dependent scattering in organic-inorganic thermoelectrics

TL;DR

This study reveals that in organic-inorganic hybrid thermoelectrics, polymer morphology and interfacial charge transfer are more influential on performance than energy-dependent scattering, challenging previous assumptions.

Contribution

It demonstrates that thermoelectric performance in hybrids is primarily governed by morphology and charge transfer, not energy-dependent scattering, using combined experiments and modeling.

Findings

Polymer morphology dominates thermoelectric performance.

Energy-dependent scattering remains unchanged in hybrids.

The Kang-Snyder model effectively explains hybrid thermoelectric behavior.

Abstract

Hybrid (organic-inorganic) materials have emerged as a promising class of thermoelectric materials, achieving power factors exceeding those of either constituent. The mechanism of this enhancement is still under debate, and pinpointing the underlying physics has proven difficult. In this work, we combine transport measurements with theoretical simulations and first principles calculations on a prototypical PEDOT:PSS-Te(Cux) nanowire hybrid material system to understand the effect of templating and charge redistribution on the thermoelectric performance. Further, we apply the recently developed Kang-Snyder charge transport model to show that scattering of holes in the hybrid system, defined by the energy-dependent scattering parameter, remains the same as in the host polymer matrix; performance is instead dictated by polymer morphology manifested in an energy-independent transport coefficient. We build upon this language to explain thermoelectric behavior in a variety of PEDOT and P3HT based hybrids acting as a guide for future work in multiphase materials.