Isotope Exchange Raman Spectroscopy (IERS): A Novel Technique to Probe Physicochemical Processes In Situ.

A novel in situ methodology for the direct study of mass-transport properties in oxides with spatial and unprecedented time resolution, based on Raman spectroscopy coupled to isothermal isotope exchanges, is developed. Changes in the isotope concentration, resulting in a Raman frequency shift, can be followed in real time, which is not accessible by conventional methods, enabling complementary insights for the study of ion-transport properties of electrode and electrolyte materials for advanced solid-state electrochemical devices. The proof of concept and strengths of isotope exchange Raman spectroscopy (IERS) is demonstrated by studying the oxygen isotope back-exchange in gadolinium-doped ceria (CGO) thin films.