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We have investigated the surface of lithium metal using x-ray photoemission spectroscopy and optical spectroscopic ellipsometry. Even if we prepare the surface of lithium metal rigorously by chemical cleaning and mechanical polishing inside a glovebox, both spectroscopic investigations show the existence of a few tens of nanometer-thick surface layers, consisting of lithium oxides and lithium carbonates. When lithium metal is exposed to room air (∼50% moisture), in situ real-time monitoring of optical spectra indicates that the surface layer grows at a rate of approximately 24 nm/min, presumably driven by an interface-controlled process. Our results hint that surface-layer-free lithium metals are formidable to achieve by a simple cleaning/polishing method, suggesting that the initial interface between lithium metal electrodes and solid-state electrolytes in fabricated lithium metal batteries can differ from an ideal lithium/electrolyte contact. 

Chiral phonons and their strong coupling to spins reveal unconventional interlayer exchange interaction and resultant spin state. 

Abstract Engineering of phonons, that is, collective lattice vibrations in crystals, is essential for manipulating physical properties of materials such as thermal transport, electron‐phonon interaction, confinement of lattice vibration, and optical polarization. Most approaches to phonon‐engineering have been largely limited to the high‐quality heterostructures of III–V compound semiconductors. Yet, artificial engineering of phonons in a variety of materials with functional properties, such as complex oxides, will yield unprecedented applications of coherent tunable phonons in future quantum acoustic devices. In this study, artificial engineering of phonons in the atomic‐scale SrRuO₃/SrTiO₃superlattices is demonstrated, wherein tunable phonon modes are observed via confocal Raman spectroscopy. In particular, the coherent superlattices led to the backfolding of acoustic phonon dispersion, resulting in zone‐folded acoustic phonons in the THz frequency domain. The frequencies can be largely tuned from 1 to 2 THz via atomic‐scale precision thickness control. In addition, a polar optical phonon originating from the local inversion symmetry breaking in the artificial oxide superlattices is observed, exhibiting emergent functionality. The approach of atomic‐scale heterostructuring of complex oxides will vastly expand material systems for quantum acoustic devices, especially with the viability of functionality integration.