Comment on "Bipolar Resistive Switching in Lanthanum Titanium Oxide and an Increased On/Off Ratio Using an Oxygen-Deficient ZnO Interlayer"

The Mott-based resistive switching random access memory (RRAM) has been considered as a promising candidate for next-generation nonvolatile mass storage. Its performance relies on the oxygen migration process. In ACS Appl. Mater. Interfaces 2022, 14, 17682-17690, Wang et al. demonstrated that inserting a ZnO layer between the top tungsten electrode and the lanthanum titanium oxide (LTO) layer can improve the ON/OFF current ratio of the RRAM. This improvement was attributed to the increased oxygen vacancies in the ZnO layer. We argue their interpretation with the role, significance, and statistics of the oxygen vacancy in the samples. Our experimental evidence contradicts their claim, and we propose that hydroxy groups should be the responsible candidate for their claimed oxygen vacancy peak at around 531-532 eV in the O 1s photoelectron spectroscopy observed in their samples. We thus propose an alternative mechanism for the ON/OFF ratio enhancement with the ZnO interlayer: the ZnO layer prevents the LTO oxygen and hydroxy groups migration and from reacting with the multivalent tungsten electrode.