Calzolari Arrigo, Oses Corey, Toher Cormac, Esters Marco, Campilongo Xiomara, Stepanoff Sergei P, Wolfe Douglas E, Curtarolo Stefano
CNR-NANO Research Center S3, Modena, Italy.
Department of Mechanical Engineering and Materials Science, Duke University, Durham, NC, USA.
Nat Commun. 2022 Oct 11;13(1):5993. doi: 10.1038/s41467-022-33497-1.
Discovering multifunctional materials with tunable plasmonic properties, capable of surviving harsh environments is critical for advanced optical and telecommunication applications. We chose high-entropy transition-metal carbides because of their exceptional thermal, chemical stability, and mechanical properties. By integrating computational thermodynamic disorder modeling and time-dependent density functional theory characterization, we discovered a crossover energy in the infrared and visible range, corresponding to a metal-to-dielectric transition, exploitable for plasmonics. It was also found that the optical response of high-entropy carbides can be largely tuned from the near-IR to visible when changing the transition metal components and their concentration. By monitoring the electronic structures, we suggest rules for optimizing optical properties and designing tailored high-entropy ceramics. Experiments performed on the archetype carbide HfTaC yielded plasmonic properties from room temperature to 1500K. Here we propose plasmonic transition-metal high-entropy carbides as a class of multifunctional materials. Their combination of plasmonic activity, high-hardness, and extraordinary thermal stability will result in yet unexplored applications.
发现具有可调谐等离子体特性且能够在恶劣环境中生存的多功能材料，对于先进的光学和电信应用至关重要。由于其卓越的热、化学稳定性和机械性能，我们选择了高熵过渡金属碳化物。通过整合计算热力学无序建模和含时密度泛函理论表征，我们发现了红外和可见光范围内的一个交叉能量，对应于金属到电介质的转变，可用于等离子体学。还发现，当改变过渡金属成分及其浓度时，高熵碳化物的光学响应可以从近红外到可见光进行很大程度的调谐。通过监测电子结构，我们提出了优化光学性能和设计定制高熵陶瓷的规则。对原型碳化物HfTaC进行的实验在室温至1500K范围内产生了等离子体特性。在此，我们提出等离子体过渡金属高熵碳化物作为一类多功能材料。它们的等离子体活性、高硬度和非凡的热稳定性相结合，将带来尚未探索的应用。
