论文标题

空缺缺陷诱导了通过光谱椭圆法和第一原理计算研究的NIO的电子和光学特性的变化

Vacancy defects induced changes in the electronic and optical properties of NiO studied by spectroscopic ellipsometry and first-principles calculations

论文作者

Egbo, Kingsley O., Liu, Chao Ping, Ekuma, Chinedu E., Yu, Kin Man

论文摘要

半导体中的天然缺陷在其光电特性中起重要作用。镍氧化物(NIO)是少数几个宽间隙P型氧化物半导体之一,其电导率被认为主要由Ni-Vacancy受体控制。在本文中,我们提出了一项系统研究,该研究比较了化学计量计NiO,富含氧气的NIO与NI空缺(NiO:VNI)和富含Ni-Nio的NiO(Nio:nio:vo)的光学特性。通过光谱椭圆法获得了光学特性,而价带光谱是通过高分辨率X射线光电子光谱探测的。实验结果被直接与第一原理密度功能理论 + U计算进行比较。计算结果证实,两个NIO系统中存在差距状态。 NIO中的差距状态:VO主要是Ni 3D状态,而Nio:VNI中的差异是由Ni 3D和O 2p状态组成的。与NIO和NIO:VO样品相比,NIO:VNI样品的吸收光谱显示出明显的缺陷诱导的特征。 NIO:VNI中亚间隙吸收的增加可以归因于在态的电子密度中观察到的间隙状态。证明了天然空置缺陷与电子和光学特性之间的关系,表明在相似的空位浓度下,NiO:VNI的光学常数与Nio:vo。我们的实验和计算结果表明,尽管VNI是NIO的有效受体,但它们也降低了材料的可见透明度。因此,对于透明的光电设备应用,需要优化具有外部掺杂的天然VNI缺陷以同时提高P型电导率和透明度。

Native defects in semiconductors play an important role in their optoelectronic properties. Nickel oxide (NiO) is one of the few wide-gap p-type oxide semiconductors and its conductivity is believed to be controlled primarily by Ni-vacancy acceptors. Herein, we present a systematic study comparing the optoelectronic properties of stoichiometric NiO, oxygen-rich NiO with Ni vacancies (NiO:VNi), and Ni-rich NiO with O vacancies (NiO:VO). The optical properties were obtained by spectroscopic ellipsometry, while valence band spectra were probed by high-resolution x-ray photoelectron spectroscopy. The experimental results are directly compared to first-principles density functional theory + U calculations. Computational results confirm that gap states are present in both NiO systems with vacancies. Gap states in NiO:Vo are predominantly Ni 3d states, while those in NiO:VNi are composed of both Ni 3d and O 2p states. The absorption spectra of the NiO:VNi sample show significant defect-induced features below 3.0 eV compared to NiO and NiO:VO samples. The increase in sub-gap absorptions in NiO:VNi can be attributed to gap states observed in the electronic density of states. The relation between native vacancy defects and electronic and optical properties of NiO are demonstrated, showing that at similar vacancy concentration, the optical constants of NiO:VNi deviate significantly from those of NiO:VO. Our experimental and computational results reveal that although VNi are effective acceptors in NiO, they also degrade the visible transparency of the material. Hence, for transparent optoelectronic device applications, an optimization of native VNi defects with extrinsic doping is required to simultaneously enhance p-type conductivity and transparency.

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