Pb(Zr0.52Ti0.48)O3 (PZT) thin films were crystallized on SrTiO3 (100) and MgO (100) substrates by a sol‐gel process using nonhydrolyzed metal methoxyethoxide precursors, spin coating, and rapid thermal annealing. Solid phase epitaxial growth of PZT on SrTiO3 was observed directly from the amorphous phase even at 425 °C. The PZT had a single (001) orientation and rocking curve full width at half maximum (FWHM) less than 0.1°. High‐temperature annealing of MgO substrates improved orientation of PZT thin films. Epitaxial crystallization of PZT with a single (001) orientation on the annealed MgO was observed at temperature above 550 °C after the formation of the pyrochlore phase.

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