Dataset for Universal In Situ Isotope Exchange Raman Spectroscopy (IERS) Methodology for Measuring Oxygen Surface Exchange Dynamics Using a Probe Layer

We have developed a novel ubiquitous methodology which we report for the first time in our manuscript entitled “Universal in situ isotope exchange Raman spectroscopy (IERS) methodology for measuring oxygen surface exchange dynamics using a probe layer”. (DOI: 10.1002/adfm.202514047) The conventional IERS method, based upon the Raman frequency shift due to the changes in isotope concentration, has recently proved to be a powerful technique to study the oxygen diffusion and surface exchange kinetics in situ. Its ground-breaking advantages have been evidenced by the previous work ([1] A. Stangl, M. Buriel et al., Advanced Materials, 10.1002/adma.202303259, 2023; [2] A. Stangl, M. Buriel et al., Small Structures, 10.1002/sstr.202400237, 2024). However, the existence of at least one active oxygen vibrational Raman mode is the prerequisite to apply conventional IERS to characterize oxygen transport of a given material. This confines its applicability to a limited range of compositions. To address this limitation, we demonstrate here that by using an innovative methodology, it is possible to extend the use of the IERS technique to study the oxygen surface exchange dynamics independently of the vibrational properties of the functional material of interest. A multilayer thin film configuration has been designed, comprising the following main elements: i) the functional layer, i.e., a dense and thin layer consisting of the material under study, ii) the probe layer; and iii) the blocking layer. This bespoke sample configuration overcomes the material dependency of conventional IERS, standing out as an alternative approach to the traditional Isotope exchange depth profiling combined with secondary ion mass spectrometry (IEDP-SIMS) method to study the oxygen mass transport dynamics in nano thin films. Compared to IEDP-SIMS, this universal IERS methodology is more efficient, non-destructive and provides additional structural information and time resolution. Additionally, the IERS method can be further extended to various isotopic elements (such as Li+ or H+) enabling mechanism studies on ion transport dynamics under realistic conditions. This methodology is expected to rapidly establish itself as a standardized in situ technique for studying ion transport, with a significant and wide-reaching impact due to its versatile applications.