The global transition from fossil fuels to green energy
underpins
the need for efficient and reliable energy storage systems. Advanced
analysis and characterization of battery materials is not only important
to understand fundamental battery properties but also crucial for
their continued development. A deep understanding of these systems
is often difficult to obtain through only pre- and/or post-mortem
analyses, with the full complexity of a battery being hidden in its
operational state. Thus, we have developed anoperandomethodology to analyze solid-state batteries (SSBs) structurally
as well as chemically before, during, and after cycling. The approach
is based on a specially designed sample holder, which enables a variety
of electrochemical experiments. Since the entire workflow is performed
within a single focused ion beam scanning electron microscope equipped
with an in-house developed magnetic sector secondary ion mass spectrometer,
we are able to pause the cycling at any time, perform analysis, and
then continue cycling. Microstructural analysis is performed via secondary
electron imaging, and the chemical mapping is performed using the
secondary ion mass spectrometer. In this proof-of-concept study, we
were able to identify dendrites in a short-circuited symmetric cell
and to chemically map dendritic structures. While this methodology
focuses on SSBs, the approach can directly be adapted to different
battery systems and beyond. Our technique clearly has an advantage
over many alternatives for battery analysis as no transfer of samples
between instruments is needed and a correlation between the microstructure,
chemical composition, and electrochemical performance is obtained
directly.