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Title: Novel strategy for low-temperature, high-rate growth of dense, hard, and stress-free refractory ceramic thin films

Growth of fully dense refractory thin films by means of physical vapor deposition (PVD) requires elevated temperatures T{sub s} to ensure sufficient adatom mobilities. Films grown with no external heating are underdense, as demonstrated by the open voids visible in cross-sectional transmission electron microscopy images and by x-ray reflectivity results; thus, the layers exhibit low nanoindentation hardness and elastic modulus values. Ion bombardment of the growing film surface is often used to enhance densification; however, the required ion energies typically extract a steep price in the form of residual rare-gas-ion-induced compressive stress. Here, the authors propose a PVD strategy for the growth of dense, hard, and stress-free refractory thin films at low temperatures; that is, with no external heating. The authors use TiN as a model ceramic materials system and employ hybrid high-power pulsed and dc magnetron co-sputtering (HIPIMS and DCMS) in Ar/N{sub 2} mixtures to grow dilute Ti{sub 1−x}Ta{sub x}N alloys on Si(001) substrates. The Ta target driven by HIPIMS serves as a pulsed source of energetic Ta{sup +}/Ta{sup 2+} metal–ions, characterized by in-situ mass and energy spectroscopy, while the Ti target operates in DCMS mode (Ta-HIPIMS/Ti-DCMS) providing a continuous flux of metal atoms to sustain a high depositionmore » rate. Substrate bias V{sub s} is applied in synchronous with the Ta-ion portion of each HIPIMS pulse in order to provide film densification by heavy-ion irradiation (m{sub Ta} = 180.95 amu versus m{sub Ti} = 47.88 amu) while minimizing Ar{sup +} bombardment and subsequent trapping in interstitial sites. Since Ta is a film constituent, primarily residing on cation sublattice sites, film stress remains low. Dense Ti{sub 0.92}Ta{sub 0.08}N alloy films, 1.8 μm thick, grown with T{sub s} ≤ 120 °C (due to plasma heating) and synchronized bias, V{sub s} = 160 V, exhibit nanoindentation hardness H = 25.9 GPa and elastic modulus E = 497 GPa compared to 13.8 and 318 GPa for underdense Ti-HIPIMS/Ti-DCMS TiN reference layers (T{sub s} < 120 °C) grown with the same V{sub s}, and 7.8 and 248 GPa for DCMS TiN films grown with no applied bias (T{sub s} < 120 °C). Ti{sub 0.92}Ta{sub 0.08}N residual stress is low, σ = −0.7 GPa, and essentially equal to that of Ti-HIPIMS/Ti-DCMS TiN films grown with the same substrate bias.« less
Authors:
; ;  [1] ; ; ; ;  [2] ; ;  [3]
  1. Department of Physics (IFM), Linköping University, SE-581 83 Linköping (Sweden)
  2. CemeCon AG, Adenauerstr. 20 A4, D-52146 Wűrselen (Germany)
  3. Department of Physics (IFM), Linköping University, SE-581 83 Linköping, Sweden and Department of Materials Science, Physics, and the Frederick Seitz Materials Research Laboratory, University of Illinois, Urbana, Illinois 61801 (United States)
Publication Date:
OSTI Identifier:
22318054
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Vacuum Science and Technology. A, Vacuum, Surfaces and Films; Journal Volume: 32; Journal Issue: 4; Other Information: (c) 2014 American Vacuum Society; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; HEAVY IONS; PHYSICAL VAPOR DEPOSITION; PRESSURE RANGE GIGA PA; RESIDUAL STRESSES; TANTALUM IONS; THIN FILMS; TITANIUM NITRIDES; TRANSMISSION ELECTRON MICROSCOPY