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The solid-electrolyte interphase (SEI) plays crucial roles for the reversible operation of lithium metal batteries. However, fundamental understanding of the mechanisms of SEI formation and evolution is still limited. Herein, we develop a depth-sensitive plasmon-enhanced Raman spectroscopy (DS-PERS) method to enable in-situ and nondestructive characterization of the nanostructure and chemistry of SEI, based on synergistic enhancements of localized surface plasmons from nanostructured Cu, shell-isolated Au nanoparticles and Li deposits at different depths. We monitor the sequential formation of SEI in both ether-based and carbonate-based dual-salt electrolytes on a Cu current collector and then on freshly deposited Li, with dramatic chemical reconstruction. The molecular-level insights from the DS-PERS study unravel the profound influences of Li in modifying SEI formation and in turn the roles of SEI in regulating the Li-ion desolvation and the subsequent Li deposition at SEI-coupled interfaces. Last, we develop a cycling protocol that promotes a favorable direct SEI formation route, which significantly enhances the performance of anode-free Li metal batteries. The solid-electrolyte interphase is crucial for most batteries, but its characterization is challenging. Here, authors develop a depth-sensitive plasmon-enhanced Raman spectroscopy method to enable in-situ and nondestructive resolving of its structure and chemistry as well as formation mechanisms. [ABSTRACT FROM AUTHOR]

As a nondestructive and ultrasensitive technique, surface-enhanced Raman spectroscopy (SERS) has captivated the attention of the global scientific community for over 50 years. Among the various spectroscopic techniques derived from SERS, shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS) stands as a cutting-edge advancement. The innovative and versatile core-shell nanoparticle structures used in SHINERS have emerged as an ideal platform for interfacial research, offering high sensitivity and broad applicability across diverse materials and single-crystal surfaces. Consequently, SHINERS has seen widespread adoption in pivotal fields, such as interface chemistry, electrocatalysis, biomedicine, materials, and food safety. In this Perspective, we outline the evolutionary journey of SHINERS, delve deep into its applications in fundamental research for interface characterization and catalysis, and explore its practical utility in critical areas of food safety and biomedicine analysis. Additionally, we map out the prospective trajectory and future milestones that await SHINERS as it continues to revolutionize the landscape of scientific exploration.