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Low-temperature epitaxial growth of refractory transition-metal nitride thin films by means of physical vapor deposition has been a recurring theme in advanced thin-film technology for several years. In the present study, 150-nm-thick epitaxial HfN layers are grown on MgO(001) by reactive high-power impulse magnetron sputtering (HiPIMS) with no external substrate heating. Maximum film-growth temperatures T-s due to plasma heating range from 70 to 150 degrees C, corresponding to T-s/T-m = 0.10-0.12 (in which T-m is the HfN melting point in K). During HiPIMS, gas and sputtered metal-ion fluxes incident at the growing film surface are separated in time due to strong gas rarefaction and the transition to a metal-ion-dominated plasma. In the present experiments, a negative bias of 100 V is applied to the substrate, either continuously during the entire deposition or synchronized with the metal-rich portion of the ion flux. Two different sputtering-gas mixtures, Ar/N-2 and Kr/N-2, are employed in order to probe effects associated with the noble-gas mass and ionization potential. The combination of x-ray diffraction, high-resolution reciprocal-lattice maps, and high-resolution cross-sectional transmission electron microscopy analyses establishes that all HfN films have a cube-on-cube orientational relationship with the substrate, i.e., [001](HfN)parallel to[001](MgO) and (100)(HfN)parallel to(100)(MgO). Layers grown with a continuous substrate bias, in either Ar/N-2 or Kr/N-2, exhibit a relatively high mosaicity and a high concentration of trapped inert gas. In distinct contrast, layers grown in Kr/N-2 with the substrate bias synchronized to the metal-ion-rich portion of HiPIMS pulses have much lower mosaicity, no measurable inert-gas incorporation, and a hardness of 25.7 GPa, in good agreement with the results for epitaxial HfN(001) layers grown at T-s = 650 degrees C (T-s/T-m = 0.26). The room-temperature film resistivity is 70 mu Omega cm, which is 3.2-10 times lower than reported values for polycrystalline-HfN layers grown at T-s = 400 degrees C. (c) 2018 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/). Funding Agencies|Swedish Research Council [VR 621-2014-4882]; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University (Faculty Grant SFO-Mat-LiU) [2009-00971] |
