In Operando Correlated Studies in Energy Materials via Combined AFM/ToF-SIMS Platform

The performance of energy storage and conversion devices, including batteries, fuel cells, and photovoltaics, is defined by the delicate interplay of electrical response and charge carrier migration at the nanoscale. Although physical behavior and macroscopic functional response is well established, intrinsic chemical phenomena associated with ionic motion or localized electrochemical reactions can dramatically alter behavior and restrict utility of these materials. Over the last decade, advancements in development of novel characterization tools such as atomic force microscopy (AFM) have revolutionized our understanding of the electrical and mechanical response of materials; however, <i>dynamic</i>electrochemical behavior and ion migration remain poorly understood. Recently time-of-flight secondary ion mass spectrometry (ToF-SIMS) has proven to be effective tool for characterization of static chemical states in energy materials. However, its application to study of dynamic electrochemical processes still requires development.<br/>Here we introduce approach based on combined AFM/ToF-SIMS platform for correlated studies of the dynamic chemical phenomena on the nanoscale in operando conditions. Being used for characterization of the perovskite materials it allowed direct observation of the ionic migration within the device in externally applied electric fields, which is important for fundamental understanding of the material functionality. Similarly, this approach allowed to study relaxation processes of the chemical phenomena in ferroelectric materials as a function of sample temperature. Altogether, developed approach enables direct characterization of interplay between chemical and functional response in energy materials and aids in the development and optimization of novel devices.<br/>This research was conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility and using instrumentation within ORNL's Materials Characterization Core provided by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy.