Defect-tolerant electron and defect-sensitive phonon transport in quasi-2D conjugated coordination polymers

Abstract Thermoelectric materials, enabling direct waste-heat to electricity conversion, need to be highly electrically conducting while simultaneously thermally insulating. This is fundamentally challenging since electrical and thermal conduction usually change in tandem. In quasi-two-dimensional c...

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Bibliographic Details
Main Authors: Hio-Ieng Un, Kamil Iwanowski, Jordi Ferrer Orri, Ian E. Jacobs, Naoya Fukui, David Cornil, David Beljonne, Michele Simoncelli, Hiroshi Nishihara, Henning Sirringhaus
Format: Article
Language:English
Published: Nature Portfolio 2025-07-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-025-61920-w
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Summary:Abstract Thermoelectric materials, enabling direct waste-heat to electricity conversion, need to be highly electrically conducting while simultaneously thermally insulating. This is fundamentally challenging since electrical and thermal conduction usually change in tandem. In quasi-two-dimensional conjugated coordination polymer films we discover an advantageous thermoelectric transport regime, in which charge transport is defect-tolerant but heat propagation is defect-sensitive; it imparts the ideal mix of antithetical properties—temperature-activated, exceptionally low lattice thermal conductivities of 0.2 W m−1 K−1 below Kittel’s limit originating from small-amplitude, quasi-harmonic lattice dynamics with disorder-limited lifetimes and vibrational scattering length on the order of interatomic spacing, and high electrical conductivities up to 2000 S cm−1 with metallic temperature dependence, notably in poorly crystalline structures with paracrystallinity >10%. These materials offer attractive properties, such as ease of processing and defect tolerance, for applications, that require fast charge, but slow heat transport.
ISSN:2041-1723