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            Abstract Ferroelectrics are being increasingly called upon for electronic devices in extreme environments. Device performance and energy efficiency is highly correlated to clock frequency, operational voltage, and resistive loss. To increase performance it is common to engineer ferroelectric domain structure with highly‐correlated electrical and elastic coupling that elicit fast and efficient collective switching. Designing domain structures with advantageous properties is difficult because the mechanisms involved in collective switching are poorly understood and difficult to investigate. Collective switching is a hierarchical process where the nano‐ and mesoscale responses control the macroscopic properties. Using chemical solution synthesis, epitaxially nearly‐relaxed (100) BaTiO3films are synthesized. Thermal strain induces a strongly‐correlated domain structure with alternating domains of polarization along the [010] and [001] in‐plane axes and 90° domain walls along the [011] or [01] directions. Simultaneous capacitance–voltage measurements and band‐excitation piezoresponse force microscopy revealed strong collective switching behavior. Using a deep convolutional autoencoder, hierarchical switching is automatically tracked and the switching pathway is identified. The collective switching velocities are calculated to be ≈500 cm s−1at 5 V (7 kV cm−1), orders‐of‐magnitude faster than expected. These combinations of properties are promising for high‐speed tunable dielectrics and low‐voltage ferroelectric memories and logic.more » « less
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            Abstract Carbon‐supported nitrogen‐coordinated single‐metal site catalysts (i.e., M−N−C, M: Fe, Co, or Ni) are active for the electrochemical CO2reduction reaction (CO2RR) to CO. Further improving their intrinsic activity and selectivity by tuning their N−M bond structures and coordination is limited. Herein, we expand the coordination environments of M−N−C catalysts by designing dual‐metal active sites. The Ni‐Fe catalyst exhibited the most efficient CO2RR activity and promising stability compared to other combinations. Advanced structural characterization and theoretical prediction suggest that the most active N‐coordinated dual‐metal site configurations are 2N‐bridged (Fe‐Ni)N6, in which FeN4and NiN4moieties are shared with two N atoms. Two metals (i.e., Fe and Ni) in the dual‐metal site likely generate a synergy to enable more optimal *COOH adsorption and *CO desorption than single‐metal sites (FeN4or NiN4) with improved intrinsic catalytic activity and selectivity.more » « less
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            Abstract While lithium ion batteries with electrodes based on intercalation compounds have dominated the portable energy storage market for decades, the energy density of these materials is fundamentally limited. Today, rapidly growing demand for this type of energy storage is driving research into materials that utilize alternative reaction mechanisms to enable higher energy densities. Transition metal compounds are one such class of materials, with storage enabled by “conversion” reactions, where the material is converted to new compound upon lithiation. MoS2is one example of this type of material that has generated a large amount of interest recently due to its high theoretical lithium storage capacity compared to graphite. Here, cryogenic scanning transmission electron microscopy techniques are used to reveal the atomic‐scale processes that occur during reaction of a model monolayer MoS2system by enabling the unaltered atomic structure to be determined at various levels of lithiation. It is revealed that monolayer MoS2can undergo a conversion reaction even with no substrate, and that the resulting particles are smaller than those that form in bulk MoS2, likely due to the more limited 2D diffusion. Additionally, while bilayer MoS2undergoes intercalation with a corresponding phase transition before conversion, monolayer MoS2does not.more » « less
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