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Developing protocols for making thin sheet FeGa (Galfenol) with abnormally grown Goss or Cube grains, which provide maximum magnetostriction, is challenging because the mechanisms that regulate grain boundary mobility and texture development in these alloys are not yet understood. Grain boundary energy models do not account for forces caused by the control of surface energy from atmospheric annealing conditions. By characterizing the surface energy of specific Galfenol grains, we can develop a more accurate thermodynamic framework for modeling abnormal grain growth and texture development. To non‐destructively measure surface energy of specific crystal orientations and overcome passivation layer difficulties in previous studies, a two‐liquid‐phase contact angle method is utilized. A single‐crystal (1 0 0) Fe₈₂Ga₁₈is used as a proof of concept for its isotropic surface crystal orientation. The resultant contact angle data shows a high dependence on the use of Ar‐plasma surface preparation to remove native oxides exposing a true interaction between a sessile drop and the Galfenol surface. Experimentally measured surface energy values are in agreement with density functional theory simulations. Surface texture and composition are confirmed using EBSD and XPS measurements. This non‐destructive technique paves the way towards studying surface energies of bare metal surfaces.

The electrical double layer is known to spontaneously form at the electrode‐electrolyte interface, impacting many important chemical and physical processes as well as applications including electrocatalysis, electroorganic synthesis, nanomaterial preparation, energy storage, and even emulsion stabilization. However, it has been challenging to study this fundamental phenomenon at the molecular level because the electrical double layer is deeply “buried” by the bulk electrolyte solution. Here, we report a quantitative probing of the electrical double layer of ionic liquids from the solid side of a photoelectron‐transparent graphene‐carbon nanotube hybrid membrane electrode using X‐ray photoelectron spectroscopy. The membrane window is ultrathin (1‐1.5 nm), large (~1 cm²), and robust, enabling a tight seal of the electrolyte and quantitative measurement with excellent photoelectron signals. Byoperandomonitoring the population changes of cations and anions in response to the applied electrical potentials, we experimentally resolve the chemical structure and dynamics of the electrical double layer, which corroborate results from molecular dynamics simulations.

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Organic electrode materials are promising for green and sustainable lithium‐ion batteries. However, the high solubility of organic materials in the liquid electrolyte results in the shuttle reaction and fast capacity decay. Herein, azo compounds are firstly applied in all‐solid‐state lithium batteries (ASSLB) to suppress the dissolution challenge. Due to the high compatibility of azobenzene (AB) based compounds to Li₃PS₄(LPS) solid electrolyte, the LPS solid electrolyte is used to prevent the dissolution and shuttle reaction of AB. To maintain the low interface resistance during the large volume change upon cycling, a carboxylate group is added into AB to provide 4‐(phenylazo) benzoic acid lithium salt (PBALS), which could bond with LPS solid electrolyte via the ionic bonding between oxygen in PBALS and lithium ion in LPS. The ionic bonding between the active material and solid electrolyte stabilizes the contact interface and enables the stable cycle life of PBALS in ASSLB.