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  1. Abstract Modern electronic systems rely on components with nanometer-scale feature sizes in which failure can be initiated by atomic-scale electronic defects. These defects can precipitate dramatic structural changes at much larger length scales, entirely obscuring the origin of such an event. The transmission electron microscope (TEM) is among the few imaging systems for which atomic-resolution imaging is easily accessible, making it a workhorse tool for performing failure analysis on nanoscale systems. When equipped with spectroscopic attachments TEM excels at determining a sample’s structure and composition, but the physical manifestation of defects can often be extremely subtle compared to their effect on electronic structure. Scanning TEM electron beam-induced current (STEM EBIC) imaging generates contrast directly related to electronic structure as a complement the physical information provided by standard TEM techniques. Recent STEM EBIC advances have enabled access to a variety of new types of electronic and thermal contrast at high resolution, including conductivity mapping. Here we discuss the STEM EBIC conductivity contrast mechanism and demonstrate its ability to map electronic transport in both failed and pristine devices. 
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  2. Abstract 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. 
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  3. The lithium-ion battery is currently the preferred power source for applications ranging from smart phones to electric vehicles. Imaging the chemical reactions governing its function as they happen, with nanoscale spatial resolution and chemical specificity, is a long-standing open problem. Here, we demonstrate operando spectrum imaging of a Li-ion battery anode over multiple charge-discharge cycles using electron energy-loss spectroscopy (EELS) in a scanning transmission electron microscope (STEM). Using ultrathin Li-ion cells, we acquire reference EELS spectra for the various constituents of the solid-electrolyte interphase (SEI) layer and then apply these “chemical fingerprints” to high-resolution, real-space mapping of the corresponding physical structures. We observe the growth of Li and LiH dendrites in the SEI and fingerprint the SEI itself. High spatial- and spectral-resolution operando imaging of the air-sensitive liquid chemistries of the Li-ion cell opens a direct route to understanding the complex, dynamic mechanisms that affect battery safety, capacity, and lifetime. 
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