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Morphology and crystallization kinetics in HfO2 thin films grown by atomic layer deposition

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13 Author(s)
Ho, M.-Y. ; Department of Materials Science, National University of Singapore, 119260, Singapore ; Gong, H. ; Wilk, G.D. ; Busch, B.W.
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We report the effects of annealing on the morphology and crystallization kinetics for the high-κ gate dielectric replacement candidate hafnium oxide (HfO2). HfO2 films were grown by atomic layer deposition (ALD) on thermal and chemical SiO2 underlayers. High-sensitivity x-ray diffractometry shows that the as-deposited ALD HfO2 films on thermal oxide are polycrystalline, containing both monoclinic and either tetragonal or orthorhombic phases with an average grain size of ∼8.0 nm. Transmission electron microscopy shows a columnar grain structure. The monoclinic phase predominates as the annealing temperature and time increase, with the grain size reaching ∼11.0 nm after annealing at 900 °C for 24 h. The crystallized fraction of the film has a strong dependence on annealing temperature but not annealing time, indicating thermally activated grain growth. As-deposited ALD HfO2 films on chemical oxide underlayers are amorphous, but show strong signatures of ordering at a subnanometer level in Z-contrast scanning transmission electron microscopy and fluctuation electron microscopy. These films show the same crystallization kinetics as the films on thermal oxide upon annealing. © 2003 American Institute of Physics.

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Journal of Applied Physics  (Volume:93 ,  Issue: 3 )