Unraveling Ultrafast Li-Ion Dynamics in the Solid Electrolyte LiTi2(PS4)3 by NMR Down to Cryogenic Temperatures

Publikation: Beitrag in FachzeitschriftArtikelForschungPeer-Review

Autorschaft

  • Denise Tapler
  • Bernhard Gadermaier
  • Jonas Spychala
  • Florian Stainer
  • Annika Marko
  • Jana Königsreiter
  • Katharina Hogrefe
  • Paul Heitjans
  • H. Martin R. Wilkening

Externe Organisationen

  • Technische Universität Graz
Forschungs-netzwerk anzeigen

Details

OriginalspracheEnglisch
Seiten (von - bis)20023-20032
Seitenumfang10
FachzeitschriftJournal of the American Chemical Society
Jahrgang147
Ausgabenummer23
Frühes Online-Datum2 Juni 2025
PublikationsstatusVeröffentlicht - 11 Juni 2025

Abstract

Self-diffusion processes of small atoms or ions play a crucial role in many areas of research. The unique crystal structure of LiTi 2(PS 4) 3 (LTPS) presents a variety of energetically inequivalent diffusion pathways for small Li + charge carriers and has resulted in one of the highest Li + diffusion coefficients. Investigating these pathways individually at the atomic scale poses significant challenges, especially for probing jump processes. In this study, we utilized nuclear spin relaxation techniques down to cryogenic temperatures (10 K) to reveal unprecedented details about both long-range and short-range Li + dynamics. The temperature-dependent 7Li NMR spin-lattice relaxation (SLR) rate exhibits a series of diffusion-induced peaks, allowing the extraction of activation energies and jump rates. Due to the exceptionally fast localized Li + exchange processes in LTPS, temperatures as low as 50 K are required to freeze Li + dynamics, on the SLR time scale, entirely within the ring-like cages of the LTPS structure.

ASJC Scopus Sachgebiete

Zitieren

Unraveling Ultrafast Li-Ion Dynamics in the Solid Electrolyte LiTi2(PS4)3 by NMR Down to Cryogenic Temperatures. / Tapler, Denise ; Gadermaier, Bernhard ; Spychala, Jonas et al.
in: Journal of the American Chemical Society, Jahrgang 147, Nr. 23, 11.06.2025, S. 20023-20032.

Publikation: Beitrag in FachzeitschriftArtikelForschungPeer-Review

Tapler, D, Gadermaier, B, Spychala, J, Stainer, F, Marko, A, Königsreiter, J, Hogrefe, K, Heitjans, P & Wilkening, HMR 2025, 'Unraveling Ultrafast Li-Ion Dynamics in the Solid Electrolyte LiTi2(PS4)3 by NMR Down to Cryogenic Temperatures', Journal of the American Chemical Society, Jg. 147, Nr. 23, S. 20023-20032. https://doi.org/10.1021/jacs.5c05253
Tapler, D., Gadermaier, B., Spychala, J., Stainer, F., Marko, A., Königsreiter, J., Hogrefe, K., Heitjans, P., & Wilkening, H. M. R. (2025). Unraveling Ultrafast Li-Ion Dynamics in the Solid Electrolyte LiTi2(PS4)3 by NMR Down to Cryogenic Temperatures. Journal of the American Chemical Society, 147(23), 20023-20032. https://doi.org/10.1021/jacs.5c05253
Tapler D, Gadermaier B, Spychala J, Stainer F, Marko A, Königsreiter J et al. Unraveling Ultrafast Li-Ion Dynamics in the Solid Electrolyte LiTi2(PS4)3 by NMR Down to Cryogenic Temperatures. Journal of the American Chemical Society. 2025 Jun 11;147(23):20023-20032. Epub 2025 Jun 2. doi: 10.1021/jacs.5c05253
Tapler, Denise ; Gadermaier, Bernhard ; Spychala, Jonas et al. / Unraveling Ultrafast Li-Ion Dynamics in the Solid Electrolyte LiTi2(PS4)3 by NMR Down to Cryogenic Temperatures. in: Journal of the American Chemical Society. 2025 ; Jahrgang 147, Nr. 23. S. 20023-20032.
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abstract = "Self-diffusion processes of small atoms or ions play a crucial role in many areas of research. The unique crystal structure of LiTi 2(PS 4) 3 (LTPS) presents a variety of energetically inequivalent diffusion pathways for small Li + charge carriers and has resulted in one of the highest Li + diffusion coefficients. Investigating these pathways individually at the atomic scale poses significant challenges, especially for probing jump processes. In this study, we utilized nuclear spin relaxation techniques down to cryogenic temperatures (10 K) to reveal unprecedented details about both long-range and short-range Li + dynamics. The temperature-dependent 7Li NMR spin-lattice relaxation (SLR) rate exhibits a series of diffusion-induced peaks, allowing the extraction of activation energies and jump rates. Due to the exceptionally fast localized Li + exchange processes in LTPS, temperatures as low as 50 K are required to freeze Li + dynamics, on the SLR time scale, entirely within the ring-like cages of the LTPS structure.",
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AU - Gadermaier, Bernhard

AU - Spychala, Jonas

AU - Stainer, Florian

AU - Marko, Annika

AU - Königsreiter, Jana

AU - Hogrefe, Katharina

AU - Heitjans, Paul

AU - Wilkening, H. Martin R.

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