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中国物理学会期刊

二维半导体材料β-TeO2的点缺陷:结构稳定性和电学性能

Point defects in the semiconducting β-TeO2 monolayer : Structural stability and electronic properties

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  • 最近新型二维半导体材料β-TeO2在实验上成功制备,并且呈现出优异的光电性质,受到学界的广泛关注。我们采用第一性原理方法系统地研究了单层β-TeO2中本征点缺陷(空位、间隙及反位缺陷)和替代缺陷的结构稳定性、电子性质和磁性。贫氧条件下最易出现的空位、间隙、反位和替代缺陷分别是VO1、Oi、TeO2和FO,而富氧条件下是VO1、Oi、TeO2和SbTe。引入空位缺陷(VO1、VO2和VTe),间隙缺陷(Tei)和反位缺陷(OTe,TeO1和TeO2)后,β-TeO2单层不会产生磁性且仍保持半导体特性,但其带隙中会引入丰富的自旋双重简并缺陷态,从而导致体系的带隙显著减小。相比之下,间隙缺陷(Oi)的引入既不诱导磁性也未在带隙中引入缺陷态,体系保持为半导体且带隙基本不变。然而,所有的替代缺陷(FO1、FO2、NO1、NO2、ITe、SbTe)均会给单层β-TeO2引入磁性,并在带隙中形成自旋极化的缺陷态,使体系转变为磁性半导体。此外,我们还详细分析了缺陷态和磁矩的来源和机制。我们的研究有助于理解二维β-TeO2的缺陷性质,并为其在电学和自旋电子学器件方面的应用提供理论基础。

    Recently, the novel two-dimensional semiconductor material β-TeO2 has been successfully synthesized in experiments and has demonstrated excellent optoelectronic properties, attracting growing attention and research interest. Using first-principles calculations based on density functional theory, we systematically investigate the structural stability, electronic properties, and magnetism of the monolayer β-TeO2 containing intrinsic point defects (vacancies, interstitials, and antisite defects) and substitutional defects. A number of physical quantities, such as the defect formation energy, electronic band structure, projected density of states, partial charge density, and magnetic moments, are calculated. It is found that, under oxygen-poor conditions, the most readily formed vacancy, interstitial, antisite, and substitutional defects are VO1, Oi, TeO2, and FO, respectively. Under oxygen-rich conditions, the corresponding defects are VO1, Oi, TeO2 and SbTe. The introduction of vacancy defects (VO1, VO2, and VTe), interstitial defects (Tei), and antisite defects (OTe, TeO1, and TeO2) does not induce magnetism in monolayer β-TeO2, and its semiconducting characteristics are still preserved. However, these defects introduce multiple spin-degenerate defect states within the bandgap, resulting in a notable decrease in the bandgap size. In contrast, the interstitial oxygen defects (Oi) do not induce magnetism and in-gap defect states in monolayer β-TeO2, the system preserve its semiconducting character and an essentially unchanged bandgap. Conversely, all substitutional defects (FO1, FO2, NO1, NO2, ITe, and SbTe) induce magnetism in monolayer β-TeO2 and generate spin-polarized defect states within the bandgap, transforming the system into a magnetic semiconductor. The corresponding magnetic moments are 0.66μB, 0.59μB, 0.67μB, 0.74μB, 0.77μB and 0.75μB, respectively. Furthermore, we present a detailed analysis of the origin and mechanism of the defect states and magnetic moments. Our study advances the understanding of defect properties in two-dimensional β-TeO2 and offers a theoretical foundation for its applications in electronic and spintronic devices.

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