Orthorhombic (o) is crystallized when sputter deposited hafnia-titania nanolaminates with ultrathin layers and bilayer composition are annealed between 573 and 1173 K. However, demixes after annealing at 1273 K, a result not predicted from bulk thermodynamics. X-ray diffraction and Raman microscopy are used here to study structural changes as demixes upon long-term annealing at 1273 K into Ti-doped monoclinic and Hf-doped rutile . We conclude that crystallized at low temperature is intrinsically metastable. A space group symmetry analysis shows that demixing can be accomplished by a continuous phase transition chain.
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