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Dielectric breakdown (DB) controls the failure, and increasingly the function, of microelectronic devices. Standard imaging techniques, which generate contrast based on physical structure, struggle to visualize this electronic process. Here in situ scanning transmission electron microscopy (STEM) electron beam‐induced current (EBIC) imaging of DB in Pt/HfO2/Ti valence change memory devices is reported. STEM EBIC imaging directly visualizes the electronic signatures of DB, namely local changes in the conductivity and in the electric field, with high spatial resolution and good contrast. DB is observed to proceed through two distinct structures arranged in series: a volatile, "soft" filament created by electron injection; and a non‐volatile, "hard" filament created by oxygen‐vacancy aggregation. This picture makes a physical distinction between "soft" and "hard" DB, while at the same time accommodating "progressive" DB, where the relative lengths of the hard and soft filaments can change on a continuum. [ABSTRACT FROM AUTHOR]

Surface properties of electrode materials play a critical role in the function of batteries. Therefore, surface modifications, such as coatings, have been widely used to improve battery performance. Understanding how these coatings function to improve battery performance is crucial for both scientific research and applications. In this study the electrochemical performance of coated and uncoated LiNi0.5Mn1.5O4 (LNMO) electrodes is correlated with ensemble-averaged soft X-ray absorption spectroscopy (XAS) and spatially resolved scanning transmission electron microscopy-electron energy loss spectroscopy (STEM-EELS) to illustrate the mechanism of how ultrathin layer Al2O3 coatings improve the cycle life of LiNi0.5Mn1.5O4. Mn2+ evolution on the surface is clearly observed in the uncoated sample, which results from the reaction between the electrolytic solution and the surfaces of LiNi0.5Mn1.5O4 particles, and also possibly atomic structure reconstructions and oxygen loss from the surface region in LiNi0.5Mn1.5O4. The coating effectively suppresses Mn2+ evolution and improves the battery performance by decelerating the impedance buildup from the surface passivation. This study demonstrates the importance of combining ensemble-averaged techniques (e.g., XAS) with localized techniques (e.g., STEM-EELS), as the latter may yield unrepresentative information due to the limited number of studied particles, and sheds light on the design of future coating processes and materials. [ABSTRACT FROM AUTHOR]

Atomic layer deposition of Al2O3 is employed as ultrathin coating on LiNi0.5Mn1.5O4, a high voltage cathode in Li‐ion batteries. X‐ray absorption spectroscopy and scanning transmission electron microscopy electron energy loss spectroscopy show that the coating suppresses Mn2+ formation on the surface and decelerates impedance buildup. The detailed analysis by Chongwu Zhou and co‐workers is shown in article number 1602873. [ABSTRACT FROM AUTHOR]