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Seebeck Effect in Molecular Wires Facilitating Long-Range Transport

Cite this: J. Am. Chem. Soc. 2024, 146, 7, 4922–4929
Publication Date (Web):February 7, 2024
https://doi.org/10.1021/jacs.3c14012
Copyright © 2024 American Chemical Society

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    Abstract

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    The study of molecular wires facilitating long-range charge transport is of fundamental interest for the development of various technologies in (bio)organic and molecular electronics. Defining the nature of long-range charge transport is challenging as electrical characterization does not offer the ability to distinguish a tunneling mechanism from the other. Here, we show that investigation of the Seebeck effect provides the ability. We examine the length dependence of the Seebeck coefficient in electrografted bis-terpyridine Ru(II) complex films. The Seebeck coefficient ranges from 307 to 1027 μV/K, with an increasing rate of 95.7 μV/(K nm) as the film thickness increases to 10 nm. Quantum-chemical calculations unveil that the nearly overlapped molecular-orbital energy level of the Ru complex with the Fermi level accounts for the giant thermopower. Landauer–Büttiker probe simulations indicate that the significant length dependence evinces the Seebeck effect dominated by coherent near-resonant tunneling rather than thermal hopping. This study enhances our comprehension of long-range charge transport, paving the way for efficient electronic and thermoelectric materials.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/jacs.3c14012.

    • Experimental details; details for calculations; additional data and figures including AFM topography image, XPS spectra, thermovoltage histograms, and current density histograms; and summarizing tables of literature survey and experimental details (PDF)

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