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

Hio-Ieng Un (), Kamil Iwanowski, Jordi Ferrer Orri, Ian E. Jacobs, Naoya Fukui, David Cornil, David Beljonne, Michele Simoncelli (), Hiroshi Nishihara and Henning Sirringhaus ()
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Hio-Ieng Un: University of Cambridge
Kamil Iwanowski: Columbia University
Jordi Ferrer Orri: University of Cambridge
Ian E. Jacobs: University of Cambridge
Naoya Fukui: Tokyo University of Science
David Cornil: University of Mons
David Beljonne: University of Mons
Michele Simoncelli: Columbia University
Hiroshi Nishihara: Tokyo University of Science
Henning Sirringhaus: University of Cambridge

Nature Communications, 2025, vol. 16, issue 1, 1-13

Abstract: 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.

Date: 2025
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DOI: 10.1038/s41467-025-61920-w

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