Combinatorial Reactive Sputtering with Auger Parameter Analysis Enables Synthesis of Wurtzite Zn2TaN3

TL;DR

This study demonstrates a combinatorial high-throughput approach combined with Auger parameter analysis to synthesize and confirm the formation of a novel wurtzite Zn2TaN3 phase, addressing challenges in materials screening.

Contribution

It introduces a workflow integrating chemical state analysis with phase screening to reliably identify new ternary nitride materials.

Findings

Successful synthesis of single-phase WZ-Zn2TaN3.

Identification of a clear discontinuity in Ta binding environment indicating new phase formation.

Mapping of functional properties of ZnxTa1-xN and reporting of chemical states for Zn3N2, TaN, and Zn2TaN3.

Abstract

The discovery of new functional materials is one of the key challenges in materials science. Combinatorial high-throughput approaches using reactive sputtering are commonly employed to screen unexplored phase spaces. During reactive combinatorial deposition the process conditions are rarely optimized, which can lead to poor crystallinity of the thin films. In addition, sputtering at shallow deposition angles can lead to off-axis preferential orientation of the grains. This can make the results from a conventional structural phase screening ambiguous. Here we perform a combinatorial screening of the Zn-Ta-N phase space with the aim to synthesize the novel semiconductor Zn2TaN3. While the results of the XRD phase screening are inconclusive, including chemical state analysis mapping in our workflow allows us to see a very clear discontinuity in the evolution of the Ta binding environment. This is indicative of the formation of a new ternary phase. In additional experiments, we isolate the material and perform a detailed characterization confirming the formation of single phase WZ-Zn2TaN3. Besides the formation of the new ternary nitride, we map the functional properties of ZnxTa1-xN and report previously unreported clean chemical state analysis for Zn3N2, TaN and Zn2TaN3. Overall, the results of this study showcase common challenges in high-throughput materials screening and highlight the merit of employing characterization techniques sensitive towards changes in the materials' short-range order and chemical state.