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Dryad

Data from: Probing lithium mobility at a solid electrolyte surface

Citation

Zuerch, Michael (2023), Data from: Probing lithium mobility at a solid electrolyte surface, Dryad, Dataset, https://doi.org/10.6078/D1N41X

Abstract

Solid-state electrolytes overcome many challenges of present lithium-ion batteries such as safety hazards and dendrite formation. However, detailed understanding of the involved lithium dynamics is missing due to a lack of in operando measurements with chemical and interfacial specificities. Here, we investigate a prototypical solid-state electrolyte using linear and nonlinear absorption spectroscopies. Leveraging the surface sensitivity of extreme-ultraviolet second-harmonic generation spectroscopy (XUV-SHG), we obtained a direct spectral signature of surface lithium ions, showing a distinct blue-shift relative to the bulk absorption spectra. First-principles simulations attributed the shift to transitions from the lithium 1s state into hybridized Li-s/Ti-d orbitals at the surface. Our calculations further suggest a reduction in lithium interfacial mobility due to suppressed low-frequency rattling modes, which is the fundamental origin of the large interfacial resistance in this material. Our findings pave the way for new optimization strategies for these electrochemical devices via interfacial engineering of lithium ions.

Methods

See associated manuscript.

Funding

U.S. Department of Energy, Award: DE-SC0004993

U.S. Department of Energy, Award: DE-SC-0023355

U.S. Department of Energy, Award: DE-AC02-05CH11231

National Science Foundation, Award: ACI-1548562

National Science Foundation, Award: 1852537

National Science Foundation, Award: DMR-1720139

National Science Foundation, Award: ECCS-2025633

Laboratory Directed Research and Development Program at Berkeley Lab , Award: 107573

National Science Foundation, Award: CBET-309147

U.S. Department of Energy, Award: DE-SC0023503

National Science Foundation, Award: DMR-2011924

Office of the President, University of California, Award: M21PL3263

Office of the President, University of California, Award: M23PR5931