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

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...

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Bibliographic Details
Published in:Nature communications Vol. 16; no. 1; pp. 6628 - 13
Main Authors: Un, Hio-Ieng, Iwanowski, Kamil, Ferrer Orri, Jordi, Jacobs, Ian E., Fukui, Naoya, Cornil, David, Beljonne, David, Simoncelli, Michele, Nishihara, Hiroshi, Sirringhaus, Henning
Format: Journal Article
Language:English
Published: London Nature Publishing Group UK 18.07.2025
Nature Publishing Group
Nature Portfolio
Subjects:
140/146
639/301/299/2736
639/638/455/954
639/766/119/995
Charge transport
Conduction
Conductivity
Coordination polymers
Crystal defects
Defects
Diffraction
Dimensional tolerances
Electrons
Grain boundaries
Heat
Heat conductivity
Heat transmission
Heat transport
Humanities and Social Sciences
multidisciplinary
Polymer films
Polymers
Ratios
Science
Science (multidisciplinary)
Spectrum analysis
Temperature dependence
Thermoelectric materials
ISSN:2041-1723, 2041-1723
Online Access:Get full text
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Summary: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. Thermoelectric materials are required to be electrically conducting while thermally insulating, which can be challenging to achieve. Here, the authors report a thermoelectric transport regime with defect tolerant charge transport but defect intolerant heat propagation in two-dimensional coordination polymer films.
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ISSN:2041-1723
2041-1723
DOI:10.1038/s41467-025-61920-w