论文标题
钻石中的指纹缺陷:分区振动光谱
Fingerprinting defects in diamond: Partitioning the vibrational spectrum
论文作者
论文摘要
在这项工作中,我们提出了一种计算方案,用于隔离固体中缺陷的振动光谱。通过量化原子投影的振动光谱的缺陷特征,可以确定贡献原子并确定其贡献的强度。该方法可用于系统地改善声子碎片计算。更有趣的是,直接使用缺陷原子的原子预测的振动光谱,可以以较低的计算成本获得良好的缺陷光谱,这也结合了宿主晶格相互作用。使用钻石作为宿主材料,考虑了四个测试案例缺陷,每种缺陷都呈现出明显不同的振动行为:一个重型替代掺杂剂(EU),两个固有缺陷(中性空位和间隙分裂)以及带负电荷的N V剂中心。重型掺杂剂和间隙分别以低频和高频的局部模式,几乎没有与宿主光谱重叠。相比之下,中性空缺和N视口中心对宿主光谱的上部光谱范围有广泛的贡献,使它们具有挑战性。独立于振动行为,可以清楚地识别出导致缺陷谱的主要原子。其原子射光光谱的重组导致孤立的缺陷光谱。
In this work, we present a computational scheme for isolating the vibrational spectrum of a defect in a solid. By quantifying the defect character of the atom-projected vibrational spectra, the contributing atoms are identified and the strength of their contribution determined. This method could be used to systematically improve phonon fragment calculations. More interestingly, using the atom-projected vibrational spectra of the defect atoms directly, it is possible to obtain a well-converged defect spectrum at lower computational cost, which also incorporates the host-lattice interactions. Using diamond as the host material, four test case defects, each presenting a distinctly different vibrational behaviour, are considered: a heavy substitutional dopant (Eu), two intrinsic defects (neutral vacancy and split interstitial), and the negatively charged N-vacancy center. The heavy dopant and split interstitial present localized modes at low and high frequencies, respectively, showing little overlap with the host spectrum. In contrast, the neutral vacancy and the N-vacancy center show a broad contribution to the upper spectral range of the host spectrum, making them challenging to extract. Independent of the vibrational behaviour, the main atoms contributing to the defect spectrum can be clearly identified. Recombination of their atom-projected spectra results in the isolated defect spectrum.