Our research seeks to elucidate the links between the structure and properties of electrochemical materials used, for instance, in rechargeable batteries. Our approach encompasses the synthesis and electrochemical testing of electrode/electrolyte materials, as well as the in-depth investigation of structural and electronic phenomena taking place during normal battery function. For this, we use and continue to develop state-of-the-art characterization tools, including high resolution solid-state nuclear magnetic resonance (NMR) spectroscopy, real-time or operando electron paramagnetic resonance (EPR) spectroscopy, operando magnetometry, and operando magnetic resonance imaging (MRI). We also conduct first principles calculations to facilitate the interpretation of the experimental data.