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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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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author Hio-Ieng Un
Kamil Iwanowski
Jordi Ferrer Orri
Ian E. Jacobs
Naoya Fukui
David Cornil
David Beljonne
Michele Simoncelli
Hiroshi Nishihara
Henning Sirringhaus
author_facet Hio-Ieng Un
Kamil Iwanowski
Jordi Ferrer Orri
Ian E. Jacobs
Naoya Fukui
David Cornil
David Beljonne
Michele Simoncelli
Hiroshi Nishihara
Henning Sirringhaus
author_sort Hio-Ieng Un
collection DOAJ
description 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.
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issn 2041-1723
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publishDate 2025-07-01
publisher Nature Portfolio
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series Nature Communications
spelling doaj-art-5c8d3982177846d3b15ea03cc158bde22025-08-20T03:05:14ZengNature PortfolioNature Communications2041-17232025-07-0116111310.1038/s41467-025-61920-wDefect-tolerant electron and defect-sensitive phonon transport in quasi-2D conjugated coordination polymersHio-Ieng Un0Kamil Iwanowski1Jordi Ferrer Orri2Ian E. Jacobs3Naoya Fukui4David Cornil5David Beljonne6Michele Simoncelli7Hiroshi Nishihara8Henning Sirringhaus9Optoelectronics Group, Cavendish Laboratory, University of CambridgeDepartment of Applied Physics and Applied Mathematics, Columbia UniversityOptoelectronics Group, Cavendish Laboratory, University of CambridgeOptoelectronics Group, Cavendish Laboratory, University of CambridgeResearch Institute for Science and Technology, Tokyo University of ScienceLaboratory for Chemistry of Novel Materials, University of MonsLaboratory for Chemistry of Novel Materials, University of MonsDepartment of Applied Physics and Applied Mathematics, Columbia UniversityResearch Institute for Science and Technology, Tokyo University of ScienceOptoelectronics Group, Cavendish Laboratory, University of CambridgeAbstract 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.https://doi.org/10.1038/s41467-025-61920-w
spellingShingle Hio-Ieng Un
Kamil Iwanowski
Jordi Ferrer Orri
Ian E. Jacobs
Naoya Fukui
David Cornil
David Beljonne
Michele Simoncelli
Hiroshi Nishihara
Henning Sirringhaus
Defect-tolerant electron and defect-sensitive phonon transport in quasi-2D conjugated coordination polymers
Nature Communications
title Defect-tolerant electron and defect-sensitive phonon transport in quasi-2D conjugated coordination polymers
title_full Defect-tolerant electron and defect-sensitive phonon transport in quasi-2D conjugated coordination polymers
title_fullStr Defect-tolerant electron and defect-sensitive phonon transport in quasi-2D conjugated coordination polymers
title_full_unstemmed Defect-tolerant electron and defect-sensitive phonon transport in quasi-2D conjugated coordination polymers
title_short Defect-tolerant electron and defect-sensitive phonon transport in quasi-2D conjugated coordination polymers
title_sort defect tolerant electron and defect sensitive phonon transport in quasi 2d conjugated coordination polymers
url https://doi.org/10.1038/s41467-025-61920-w
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