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Clean and efficient energy storage technologies are essential to establishing a renewable energy infrastructure. Lithium-ion batteries are already dominant in personal electronic devices, and are promising candidates for reliable grid-level storage and electric vehicles. However, further development is needed to improve their charging rates and usable lifetimes. To aid the development of such faster-charging and longer-lasting batteries, scientists need to be able to understand the processes occurring inside an operating battery, to identify the limitations to battery performance.