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

By M.-Y. Ho, H. Gong, G. D. Wilk, B. W. Busch, M. L. Green, P. M. Voyles, D. A. Muller, M. Bude, W. H. Lin, A. See, M. E. Loomans, S. K. Lahiri and Petri I. Raisanen


We report the effects of annealing on the morphology and crystallization kinetics for the high-k 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

Topics: fluctuation electron microscopy, gate dielectric, HfO2
Year: 2003
DOI identifier: 10.1063/1.1534381
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