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arXiv 1806.07280cond-mat.str-el
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Ruddlesden-Popper铱酸盐光学性质的相对论性$GW$ + BSE研究

Relativistic $GW$+BSE study of the optical properties of Ruddlesden-Popper iridates

Peitao Liu, Bongjae Kim, Xing-Qiu Chen, D. D. Sarma, Georg Kresse, Cesare Franchini

摘要:

通过求解Bethe-Salpeter方程(BSE)研究了Ruddlesden-Popper系列铱酸盐Sr $_{n+1}$ Ir $_n$ O $_{3n+1}$($n$ =1,2和$\infty$)的光学性质,其中准粒子(QP)能量和屏蔽相互作用$W$由包含自旋轨道耦合的$GW$近似得到.计算的光学电导率谱显示出很强的激子效应,并很好地再现了实验观察到的双峰结构,特别是自旋轨道莫特绝缘体Sr $_2$ IrO $_4$和Sr $_3$ Ir $_2$ O $_7$。然而,$GW$不能很好地解释SrIrO $_3$的相关金属态,这是由于太小的能带重整化,这影响了光学电导率的整体质量。我们的分析很好地描述了作为维数($n$)的函数的主要光学峰的渐进红移,这与电子相关性(由约束随机相位近似量化)向金属$n=\infty$极限的逐渐降低相关。我们还评估了一种计算成本更低的BSE方法的质量,该方法基于模型介电函数并在DFT+ $U$单电子能量之上进行。不幸的是,该模型BSE方法不能准确地再现完整的$GW$ +BSE方法的结果,并导致测量光谱的较大偏差。

英文摘要:

We study the optical properties of the Ruddlesden-Popper series of iridates Sr$_{n+1}$Ir$_n$O$_{3n+1}$ ($n$=1, 2 and $\infty$) by solving the Bethe-Salpeter equation (BSE), where the quasiparticle (QP) energies and screened interactions $W$ are obtained by the $GW$ approximation including spin-orbit coupling. The computed optical conductivity spectra show strong excitonic effects and reproduce very well the experimentally observed double-peak structure, in particular for the spin-orbital Mott insulators Sr$_2$IrO$_4$ and Sr$_3$Ir$_2$O$_7$. However, $GW$ does not account well for the correlated metallic state of SrIrO$_3$ owing to a much too small band renormalization, and this affects the overall quality of the optical conductivity. Our analysis describes well the progressive redshift of the main optical peaks as a function of dimensionality ($n$), which is correlated with the gradual decrease of the electronic correlation (quantified by the constrained random phase approximation) towards the metallic $n=\infty$ limit. We have also assessed the quality of a computationally cheaper BSE approach that is based on a model dielectric function and conducted on top of DFT+$U$ one-electron energies. Unfortunately, this model BSE approach does not accurately reproduce the outcome of the full $GW$+BSE method and leads to larger deviations to the measured spectra.

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