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hard ceramic electrolytes at high current density.32 Ostensibly, this seems to defy physics; however, there must be an explanation. Understanding the underlying mechanisms that allow this unusual phenomenon to occur could guide future efforts to mitigate it. Second, intrinsic to their design, solid-state batteries require a chemical and physical union between the cathode, which is typically a ceramic, and the solid electrolyte. Because the approach to construct a rechargeable, bulk-scale, solid-state battery is unknown territory, it is important to understand how the transport of ions and electrons occurs across these solid interfaces, and how mechanical stresses are generated when the electrode changes volume during cycling while the solid electrolyte does not. Lastly, the development of new in situ characterization techniques tailored for the analysis of advanced solid- solid interfaces could facilitate understanding by observing phenomena in real time and without the artifacts frequently created by postmortem analyses, especially with air-sensitive materials. Acquiring a fundamental understanding related to these aspects will accelerate the development of solid-state batteries. In summary, the key scientific challenges for enabling solid electrolyte/solid electrode interfaces are: understand what limits the stability and kinetics of the alkali-metal/solid electrolyte interface, understand charge transport and the mechanical stability of the ceramic cathode/solid electrolyte interface, and develop in situ techniques to analyze solid-solid interfaces. Alkali Metal Solid-Electrolyte Interface: One of the most promising approaches to enable a step increase in battery energy density is to stabilize the alkali-metal/solid-electrolyte interface.61,62 Solid inorganic, polymeric, or ceramic/polymeric composite electrolytes could act as a physical barrier to block the formation of dendrites, thereby stabilizing the alkali metal electrode surface during cycling.1,32,53,63 Additionally, the solid electrolyte must be compatible with the alkali metal while possessing high ionic conductivity and mechanical and electrochemical stability.37-39,43,64 Of particular importance is achieving facile and stable charge transport across the alkali-metal/ solid-electrolyte interface at meaningful current densities.53,65 Though there are some hypotheses and models that analyze the alkali-metal/solid-electrolyte interface, none has been validated.66,67 Similarly, there are limited experimental studies that precisely determine what governs the maximum current density of the alkali-metal/ solid-electrolyte interface.53,68 Currently, for example, it is believed that Li penetrates grain boundaries in polycrystalline LLZO electrolyte (see Figure 2.3.5 in Chapter 2) at current densities above a few tenths of a mA/cm2.32,69 Why this occurs is currently not understood. Thus, the need to understand the underlying mechanisms that govern the stability of the alkali-metal/solid-electrolyte interface is clear (Figure 3.5.5). In-Situ and Operando Characterization of the Solid-Electrolyte Interface: Though computation can predict electrochemical stability, solid-electrolyte interphases often form between a metal electrode and solid electrolyte.37,70 The effects of the alkali-metal/solid-electrolyte interface can be benign, detrimental, or beneficial.64,71 Nevertheless, because the alkali-metal/solid-electrolyte interface can affect interface kinetics, stability, and durability, efforts are needed to better understand all solid electrolyte-electrode interactions at the atomic, molecular, and microstructural level (Figure 3.5.6).71,72 Our knowledge of heterogeneous ionic interfaces, however, is very limited, mainly because of the complexity of interfacial structure and chemistry in real materials systems, where not only chemical inter-diffusion, lattice strain, defects, and chemical reactions can occur, but space charge effects may also complicate analysis .73-77 As these phenomena are correlated, all associated microscopic factors (i.e., lattice, electrons, polarons, and ions) must be simultaneously considered when studying the effects of spatial, temporal, and space charge. Analyzing these effects requires atomic-scale resolution, which creates the need for the fabrication of a precise model for all solid interfaces. Because crystallographic orientation could affect charge transport, fabrication of bicrystals78 with control over atomic plane alignment and composition at interfaces will be necessary. New characterization techniques, which could analyze all these factors simultaneously under relevant and simulated operating environments, are therefore needed. In summary, the discovery of numerous viable solid electrolytes could allow for a paradigm shift in battery technology. However, little is known about their integration with electrodes and into solid-state batteries. Myriad barriers related to the all-solid interface remain but may be overcome through a galvanizing and holistic effort bringing together the fields of materials science, solid-state electrochemistry, mechanical engineering, computation, physics, and materials characterization. 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