Publication date: 10th April 2024
Ion transport is the foundation of electrochemical devices, underpinning the performance of intercalated electrodes and solid electrolytes for batteries and fuel cells. The typical model of ion transport describes a single ion hopping through a periodic lattice with an enthalpic energy barrier and hop attempt frequency. This model assumes a static energetic landscape, neglecting any contribution of phonons to the local structure and energy landscape within the ion hop. Recent work correlates strongly anharmonic phonon modes with superionic phase transformations in solid electrolytes through variable-temperature phonon measurements, as modes shift to lower frequency and broaden with increased temperature due to anharmonic effects. However, the mechanism of how phonons and strong anharmonicity contribute to the ion hop remains unclear.
We present a detailed study of the variable-temperature phonon behavior of Li7La3Zr2O12 (LLZO), a promising solid electrolyte for solid-state lithium-ion batteries which undergoes a superionic phase change from the tetragonal to the cubic phase. We investigate the phonon behavior through variable-temperature Raman spectroscopy and THz time-domain spectroscopy. Single crystal polarization-dependent Raman spectroscopy contributes to mode assignment to underlying structure in the cubic and tetragonal phases.
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