Abstract
Summary The presence of a van der Waals gap within layered materials enables the intercalation of guest species, which can be used for tuning properties. The introduction of intercalant species may also lead to structural transformations across a range of temperatures and use conditions, but we have a limited understanding of the high-temperature evolution of intercalated layered materials. Here, we use in situ transmission electron microscopy to investigate temperature-dependent structural evolution of Bi2Te3, a layered material with well-known application as a thermoelectric, which contains intercalated Cu. As temperature is increased, the initially disordered Cu undergoes local ordering within the van der Waals gap, along with anisotropic sublimation behavior of the crystals. As the temperature is raised further, layered Cu2Te crystals nucleate and grow with a crystallographic relationship to the Bi2Te3 lattice. Notably, the presence of Cu decreases the thermal stability of the Bi2Te3 and substantially alters the transformation pathways during heating.
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