Fundamental picture of the conduction mechanism in solid-state polymer electrolytes revealed by terahertz spectroscopy

Fuente: arXiv
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Main Authors: Weidelt, Johanna, Nair, Jijeesh Ravi, Diddens, Diddo, Zhang, Wentao, Pfeiffer, Felix, Schneider, Tiago de Oliveira, Meinert, Markus, Hiraoka, Tomoki, Nesterov, Linda, Baghernejad, Masoud, Turchinovich, Dmitry, Hafez, Hassan A.
Format: Preprint
Published: 2026
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author Weidelt, Johanna
Nair, Jijeesh Ravi
Diddens, Diddo
Zhang, Wentao
Pfeiffer, Felix
Schneider, Tiago de Oliveira
Meinert, Markus
Hiraoka, Tomoki
Nesterov, Linda
Baghernejad, Masoud
Turchinovich, Dmitry
Hafez, Hassan A.
author_facet Weidelt, Johanna
Nair, Jijeesh Ravi
Diddens, Diddo
Zhang, Wentao
Pfeiffer, Felix
Schneider, Tiago de Oliveira
Meinert, Markus
Hiraoka, Tomoki
Nesterov, Linda
Baghernejad, Masoud
Turchinovich, Dmitry
Hafez, Hassan A.
contents Solid polymer electrolytes (SPEs) based on cross-linked poly(ethylene oxide) (PEO) encompassing lithium salts have gained significant attention as separators in solid-state lithium metal batteries. Here, we employ terahertz time-domain spectroscopy (THz-TDS), as a noninvasive contact-free technique, to investigate the conduction properties of these cross-linked SPEs and unravel their dependencies on the added lithium salt and the sample temperature. The obtained THz conductivity spectra are dominated by THz absorption bands, which we attribute to resonant vibrations within the polymer matrix of the electrolyte. By careful application of Lorentz model, the conductivity spectra have been analyzed, and the relevant polymer vibration modes have been quantitatively assessed. Calculations based on the density functional theory (DFT) were performed to elucidate the possible microscopic mechanisms of these resonant vibrations. This study sheds light on the relevance of polymer matrix vibrations validating the hopping transport of lithium ions in SPEs which ultimately leads to the technologically relevant ionic conduction in the solid-state polymer-based electrolytes.
format Preprint
id arxiv_https___arxiv_org_abs_2604_25497
institution arXiv
publishDate 2026
record_format arxiv
spellingShingle Fundamental picture of the conduction mechanism in solid-state polymer electrolytes revealed by terahertz spectroscopy
Weidelt, Johanna
Nair, Jijeesh Ravi
Diddens, Diddo
Zhang, Wentao
Pfeiffer, Felix
Schneider, Tiago de Oliveira
Meinert, Markus
Hiraoka, Tomoki
Nesterov, Linda
Baghernejad, Masoud
Turchinovich, Dmitry
Hafez, Hassan A.
Soft Condensed Matter
Materials Science
Solid polymer electrolytes (SPEs) based on cross-linked poly(ethylene oxide) (PEO) encompassing lithium salts have gained significant attention as separators in solid-state lithium metal batteries. Here, we employ terahertz time-domain spectroscopy (THz-TDS), as a noninvasive contact-free technique, to investigate the conduction properties of these cross-linked SPEs and unravel their dependencies on the added lithium salt and the sample temperature. The obtained THz conductivity spectra are dominated by THz absorption bands, which we attribute to resonant vibrations within the polymer matrix of the electrolyte. By careful application of Lorentz model, the conductivity spectra have been analyzed, and the relevant polymer vibration modes have been quantitatively assessed. Calculations based on the density functional theory (DFT) were performed to elucidate the possible microscopic mechanisms of these resonant vibrations. This study sheds light on the relevance of polymer matrix vibrations validating the hopping transport of lithium ions in SPEs which ultimately leads to the technologically relevant ionic conduction in the solid-state polymer-based electrolytes.
title Fundamental picture of the conduction mechanism in solid-state polymer electrolytes revealed by terahertz spectroscopy
topic Soft Condensed Matter
Materials Science
url https://arxiv.org/abs/2604.25497