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We present an incisive spectroscopic technique for directly probing redoxorbitals based on bulk electron momentum density measurements viahigh-resolution x-ray Compton scattering. Application of our method to spinelLixMn2O4, a lithium ion battery cathode material, is discussed. The orbitalinvolved in the lithium insertion and extraction process is shown to mainly bethe oxygen 2p orbital. Moreover, the manganese 3d states are shown toexperience spatial delocalization involving 0.16 electrons per Mn site duringthe battery operation. Our analysis provides a clear understanding of thefundamental redox process involved in the working of a lithium ion battery.

Extracting the Redox Orbitals in Li Battery Materials with High-Resolution X-Ray Compton Scattering Spectroscopy