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In Situ Solid Phase Crystallization of Functional Ceramics in the Transmission Electron Microscope

Many interesting and technologically relevant materials are not at their true thermodynamic free-energy minimum but instead are kinetically stabilized Some of these metastable structures may demonstrate unique, and potentially improved properties over their thermodynamically stable counterparts. However, accessing metastable reaction products and controlling formation pathways to target them presents a formidable challenge. This is especially true for systems such as complex oxides, which often display diverse polymorphism We present a route for the formation of potentially novel, layered complex oxide structures formed from a solid thin-film amorphous precursor through rapid heating and quenching, whereby solid-phase crystallization (SPC) of 30-nm thick La 0.8 Sr 0.2 MnO 3 (LSM82) pulsed-laser deposited (PLD) films is performed in situ in the transmission electron microscope (TEM). In contrast to solid-phase epitaxy (SPE) where the substrate imposes epitaxial constraints, LSM82 films are deposited on an amorphous Si x N y substrate such that the resulting phases are free of such constraints. This provides a very open phase space that affords plentiful opportunities to access unusual structures. Although the perovskite structure is the true equilibrium phase of bulk LSM82 under the processing the exceptionally high free-energy starting film of this non-glass-former generates a tendency to adopt metastable or transition states upon crystallization. In accordance with step rule, those phases that develop first are likely those closest in free-energy starting a