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Nucleation of HfO2 atomic layer deposition films on chemical oxide and H-terminated Si

J. Appl. Phys. 102, 034101 (2007); doi:10.1063/1.2764223

Published 2 August 2007

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Justin C. Hackley and Theodosia Gougousi
Department of Physics, University of Maryland Baltimore County (UMBC), Baltimore, Maryland 21250

J. Derek Demaree
Weapons & Materials Research Directorate, Army Research Laboratory, Aberdeen Proving Ground, Maryland 21005-5069
HfO2 thin films have been deposited by an atomic layer deposition (ALD) process using alternating pulses of tetrakis-ethylmethylamino hafnium and H2O precursors at 250 °C. The as-deposited films are mainly amorphous and nearly stoichiometric HfO2 (O/Hf ratio ~1.9) with low bonded carbon content (~3  at. %). A comparison of the nucleation stage of the films on OH- and H-terminated Si(100) surfaces has been performed using Rutherford backscattering spectrometry, x-ray photoelectron spectroscopy (XPS), and spectroscopic ellipsometry (SE). We find for the initial 5–7 process cycles that the film nucleates more efficiently on the OH-terminated surface. However, after the 7th cycle both surfaces exhibit similar surface coverage, which takes about 40 cycles to reach a steady growth rate per cycle. Angle resolved XPS measurements reveal the formation of a ~6  Å interfacial layer after four ALD cycles on the H-terminated surface and the thickness of the interfacial layer does not change substantially between the 4th and the 50th process cycles as shown by transmission electron microscopy. Although the surface coverage is comparable for both starting surfaces, film measurements performed by SE suggest that thick films deposited on H-terminated Si are ~5% thicker than similar films on the chemical oxide surface. Atomic force microscopy (AFM) measurements reveal higher surface roughness for the films deposited in the H-terminated surface. The SE and the AFM data are consistent with higher porosity for the films on H-terminated surfaces. ©2007 American Institute of Physics
History: Received 24 April 2007; accepted 13 June 2007; published 2 August 2007
Permalink: http://link.aip.org/link/?JAPIAU/102/034101/1
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KEYWORDS and PACS

Keywords
PACS
  • 77.55.+f
    Dielectric thin films
  • 68.55.Ac
    Thin film nucleation and growth: microscopic aspects
  • 81.15.Gh
    Chemical vapor deposition including plasma-enhanced CVD, MOCVD, etc
  • 81.15.Ef
    Vacuum deposition
  • 68.37.Ps
    Atomic force microscopy (AFM) of surfaces, interfaces and thin films
  • 79.60.Bm
    Photoelectron spectra of clean metal, semiconductor, and insulator surfaces
  • YEAR: 2007

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PUBLICATION DATA

ISSN:
0021-8979 (print)   1089-7550 (online)
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