Probing nanoscale oxygen ion motion in memristive systems

Ion transport is an essential process for various applications including energy storage, sensing, display, memory and so on, however direct visualization of oxygen ion motion has been a challenging task, which lies in the fact that the normally used electron microscopy imaging mainly focuses on the mass attribute of ions. The lack of appropriate understandings and analytic approaches on oxygen ion motion has caused significant difficulties in disclosing the mechanism of oxides-based memristors. Here we show evidence of oxygen ion migration and accumulation in HfO2 by in situ measurements of electrostatic force gradient between the probe and the sample, as systematically verified by the charge duration, oxygen gas eruption and controlled studies utilizing different electrolytes, field directions and environments. At higher voltages, oxygen-deficient nano-filaments are formed, as directly identified employing a CS-corrected transmission electron microscope. This study could provide a generalized approach for probing ion motions at the nanoscale.