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Enhancing lithium-ion battery technology in terms of specific capacity and charging time is key for the advancement of the electrification of transportation. Particularly for fast charging, inhomogeneous deposition of metallic lithium, for example on commercial graphite or metallic lithium anodes, leads to cell degradation and safety issues. To understand the underlying mechanisms and develop counter-measures, non-invasive online detection techniques providing satisfactory time resolution are crucial. Here, we demonstrate  in operando  pulse electron paramagnetic resonance to observe transient processes during pulsed fast charging in cells with metallic lithium anodes. Sampling timescales of 100 ms enable real-time monitoring of the formation and evolution of porous lithium during and after charging pulses. It was observed that the generated morphology continued to evolve after the end of a charging pulse, whereby surface features were fusing with a time constant that was slower than their formation.

Transient morphology of lithium anodes in batteries monitored by in operando pulse electron paramagnetic resonance