Basic properties mapping of anodic oxides in the hafnium-niobium-tantalum ternary system

Sci Technol Adv Mater. 2018 Aug 13;19(1):554-568. doi: 10.1080/14686996.2018.1498703. eCollection 2018.

Abstract

A thin film combinatorial library deposited by co-sputtering of Hf, Nb and Ta was employed to characterise fundamental properties of the Hf-Nb-Ta system. Compositional mappings of microstructure and crystallography revealed similarities in alloy evolution. Distinct lattice distortion was observed upon addition of hexagonal Hf, leading to amorphisation of alloys containing more than 32 at.% Hf and less than 27 and 41 at.% Nb and Ta, respectively. Volta potential and open circuit potential mappings indicated minimal values for the highest Hf concentration. Localised anodisation of the library by scanning droplet cell microscopy revealed valve metal behaviour. Oxide formation factors above 2 nm V-1 were identified in compositional zones with high amounts of Nb and Ta. Fitting of electrochemical impedance spectroscopy data allowed electrical permittivity and resistivity of mixed oxides to be mapped. Their compositional behaviours were attributed to characteristics of the parent metal alloys and particularities of the pure oxides. Mott-Schottky analysis suggested n-type semiconductor properties for all Hf-Nb-Ta oxides studied. Donor density and flat-band potential were mapped compositionally, and their variations were found to be related mainly to the Nb amount. Synergetic effects were identified in mappings of Hf-Nb-Ta parent metals and their anodic oxides.

Keywords: 202 Dielectrics / Piezoelectrics / Insulators; 306 Thin film / Coatings, Anodic oxides; 40 Optical, magnetic and electronic device materials; Combinatorial libraries; anodic oxide films; high-throughput experimentation; scanning droplet cell microscopy; valve metals.

Grants and funding

This work was supported by the Christian Doppler Forschungsgesellschaft [COMBOX]; Österreichische Forschungsförderungsgesellschaft mbH [CEST-UPPER].