Hydrogen passivation of acceptor defects in delafossite CuMO2 (M = Al, Ga, In): Insights for enhanced p-type conductivity

Aroon Ananchuensook, Intuon Chatratin, Anderson Janotti, T. Watcharatharapong, J. T‐Thienprasert, Adisak Boonchun, S. Jungthawan, P. Reunchan
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Abstract

Transparent conducting oxides with p-type conductivity hold immense potential for various electronic applications. The role of native point defects in delafossite CuMO2 (M = Al, Ga, In) as the source of p-type conductivity has been widely acknowledged. However, understanding the primary defects governing the electrical properties and devising strategies for improvement remains a critical challenge. In this study, we employ range-separated hybrid density functional calculations to elucidate the impact of acceptor defects and their interactions with hydrogen on electrical conductivity. Our findings demonstrate that hydrogen plays a pivotal role in controlling p-type conductivity in these oxides. Our investigation reveals that the interactions between hydrogen interstitial Hi and copper vacancy VCu lead to the formation of stable complexes that are electrically inactive. Considerable binding energies are observed for Hi–VCu complexes, indicating that they are highly bound complexes with low formation energy and, thus, high concentrations under both O-rich and O-poor conditions. A second hydrogen can be bound to VCu to form 2Hi–VCu complexes, which are thermodynamically stable and function as a single donor. Furthermore, hydrogen can bind with the antisite acceptor defects, CuM, forming Hi–CuM complexes. However, the lower binding energies associated with these complexes suggest likely dissociation into isolated Hi and CuM at relatively low temperatures. By shedding light on the strong influence of hydrogen passivation of acceptor defects, this study offers valuable insights into p-type conductivity in delafossite CuMO2.
二化石 CuMO2(M = Al、Ga、In)中受体缺陷的氢钝化:增强 p 型导电性的启示
具有 p 型导电性的透明导电氧化物在各种电子应用中具有巨大的潜力。作为 p 型导电性的来源,delafossite CuMO2(M = Al、Ga、In)中的原生点缺陷的作用已得到广泛认可。然而,了解支配电性能的主要缺陷并制定改进策略仍然是一项严峻的挑战。在本研究中,我们采用范围分离混合密度泛函计算来阐明受体缺陷及其与氢的相互作用对导电性的影响。我们的研究结果表明,氢在控制这些氧化物的 p 型电导率方面起着关键作用。我们的研究发现,氢间隙 Hi 与铜空位 VCu 之间的相互作用导致形成了电性不活泼的稳定复合物。我们观察到氢-VCu 复合物具有相当大的结合能,这表明它们是高度结合的复合物,具有较低的形成能,因此在富氧和贫氧条件下都具有较高的浓度。第二个氢可以与 VCu 结合,形成 2Hi-VCu 复合物,这种复合物在热力学上是稳定的,可以作为单一供体发挥作用。此外,氢还能与反异位受体缺陷 CuM 结合,形成 Hi-CuM 复合物。然而,与这些复合物相关的较低结合能表明,在相对较低的温度下,它们很可能解离成孤立的 Hi 和 CuM。这项研究揭示了氢钝化对受体缺陷的强烈影响,从而为了解 delafossite CuMO2 的 p 型导电性提供了宝贵的见解。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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