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            Abstract The dynamic behavior of the interface between the lithium metal electrode and a solid-state electrolyte plays a critical role in all-solid-state battery performance. The evolution of this interface throughout cycling involves multiscale mechanical and chemical heterogeneity at the micro- and nano-scale. These features are dependent on operating conditions such as current density and stack pressure. Here we report the coupling of operando acoustic transmission measurements with nuclear magnetic resonance spectroscopy and magnetic resonance imaging to correlate changes in interfacial mechanics (such as contact loss and crack formation) with the growth of lithium microstructures during cell cycling. Together, the techniques reveal the chemo-mechanical behavior that governs lithium metal and Li 7 La 3 Zr 2 O 12 interfacial dynamics at various stack pressure regimes and with voltage polarization.more » « less
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            null (Ed.)In this work we build upon acoustic–electrochemical correlations to investigate the relationships between sound wave structure and chemo-mechanical properties of a pouch cell battery. Cell thickness imaging and wave detection during pouch cell cycling are conducted in parallel. Improved acoustic hardware and signal processing are used to validate the direct measurement of material stiffness, which is an intrinsic physical property. Measurement of cell thickness to micron resolution and wave transmit time to nanosecond resolution in a temperature and pressure controlled acoustic rig allows for estimation of the effective stiffness. We further explore the effects of material type and cell layering on the acoustic signal, demonstrating that the operando acoustic method can accurately measure the changes in physical state properties of a battery with high dynamic temporal and spatial range.more » « less
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