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1 nm, corresponding to a few atomic layers of Li. To identify the growth mechanism, the SPR reflectance spectra of various possible Li-metal deposition processes were simulated. Comparison of the simulated spectra with the experimental data found good agreement with the well-known nucleation and growth model for Li-metal deposition from PC-based electrolytes. The demonstrated operando electrochemical SPR measurement should be a valuable tool for basic research on the initial Li-metal deposition process.Data-driven strategies are gaining