Title

Electronic structure of the SiNx/TiN interface: A model system for superhard nanocomposites

Document Type

Article

Publication Date

3-31-2011

Abstract

Nanostructured materials such as nanocomposites and nanolaminates-subjects of intense interest in modern materials research-are defined by internal interfaces, the nature of which is generally unknown. Nevertheless, the interfaces often determine the bulk properties. An example of this is superhard nanocomposites with hardness approaching that of diamond. TiN/Si 3N4 nanocomposites (TiN nanocrystals encapsulated in a fully percolated SiNx tissue phase) and nanolaminates, in particular, have attracted much attention as model systems for the synthesis of such superhard materials. Here, we use in situ angle-resolved x-ray photoelectron spectroscopy to probe the electronic structure of Si3N 4/TiN(001), Si/TiN(001), and Ti/TiN(001) bilayer interfaces, in which 4-ML-thick overlayers are grown in an ultrahigh vacuum system by reactive magnetron sputter deposition onto epitaxial TiN layers on MgO(001). The thickness of the Si3N4, Si, and Ti overlayers is chosen to be thin enough to insure sufficient electron transparency to probe the interfaces, while being close to values reported in typical nanocomposites and nanolaminates. The results show that these overlayer/TiN(001) interfaces have distinctly different bonding characteristics. Si3N4 exhibits interface polarization through the formation of an interlayer, in which the N concentration is enhanced at higher substrate bias values during Si 3N4 deposition. The increased number of Ti-N bonds at the interface, together with the resulting polarization, strengthens interfacial bonding. In contrast, overlayers of Si and, even more so, metallic Ti weaken the interface by minimizing the valence band energy difference between the two phases. A model is proposed that provides a semiquantitative explanation of the interfacial bond strength in nitrogen-saturated and nitrogen-deficient Ti-Si-N nanocomposites. © 2011 American Physical Society.

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