论文标题

关于在呈现原子依赖电荷顺序的材料中使用扫描隧道光谱准确测量LDOS图的重要性:相关的PB/SI(111)单个原子层

On the importance of measuring accurately LDOS maps using scanning tunneling spectroscopy in materials presenting atom-dependent charge order: the case of the correlated Pb/Si(111) single atomic layer

论文作者

Tresca, C., Bilgeri, T., Bilgeri, T., Menard, G., Cherkez, V., Federicci, R., Longo, D., Hervé, M., Debontridder, F., David, P., Roditchev, D., Profeta, G., Cren, T., Calandra, M., Brun, C.

论文摘要

我们展示了如何从扫描隧道显微镜/光谱(STM/STS)测量中正确提取二维材料中的局部电荷顺序。当电荷顺序在单位电池内的原子尺度上呈现空间变化并取决于能量时,应特别注意。在这种情况下,使用锁定技术的使用,同时在封闭的反馈循环中获得STM地形时,会导致系统不正确的DI/DV测量值,从而产生了错误的局部费用顺序。正确的方法是执行恒定的高度测量,或者使用偏置电压设定点在材料带宽之外进行DI/DV(V)光谱的完整网格,在该材料带宽之外,该材料带宽(LDOS)在空间上是同质的。我们以二维材料的范式示例为1/3单层PB/SI(111)。由于无法种植此阶段的大面积,因此该系统中的电荷排序无法获得角度分辨光发射或放牧X射线衍射。 STM/STS先前由{\ it i i i}密度函数理论(DFT)计算补充的研究得出的结论是,该材料经历了一个相过渡到低温$ 3 \ times 3 $ 3 $重建,其中一个PB原子移动,两个剩下的Pb原子移动下降。 Adler {\ it等人} [PRL 123,086401(2019)]进行的第三次STM/STS研究得出了相反的结论,即两个Pb原子在上升,而一个PB原子向下移动。后一个错误的结论来自滥用锁定技术。相比之下,使用DI/DV(V)光谱测量的完整网格,我们表明,依赖能量的LDOS映射与最先进的DFT计算非常吻合,从而确认了单个上升的两次收费顺序。在$ 3 \ times 3 $单位单元中,这种结构和电荷重新排序同样由电子 - 电子相互作用以及与基板耦合的驱动。

We show how to properly extract the local charge order in two-dimensional materials from scanning tunneling microscopy/spectroscopy (STM/STS) measurements. When the charge order presents spatial variations at the atomic scale inside the unit cell and is energy dependent, particular care should be taken. In such cases the use of the lock-in technique, while acquiring an STM topography in closed feedback loop, leads to systematically incorrect dI/dV measurements giving a false local charge order. A correct method is either to perform a constant height measurement or to perform a full grid of dI/dV(V) spectroscopies, using a bias voltage setpoint outside the material bandwidth where the local density-of-states (LDOS) is spatially homogeneous. We take as a paradigmatic example of two-dimensional material the 1/3 single-layer Pb/Si(111). As large areas of this phase cannot be grown, charge ordering in this system is not accessible to angular resolved photoemission or grazing x-ray diffraction. Previous investigations by STM/STS supplemented by {\it ab initio} Density Functional Theory (DFT) calculations concluded that this material undergoes a phase transition to a low-temperature $3\times 3$ reconstruction where one Pb atom moves up, the two remaining Pb atoms shifting down. A third STM/STS study by Adler {\it et al.} [PRL 123, 086401 (2019)] came to the opposite conclusion, i.e. that two Pb atoms move up, while one Pb atom shifts down. This latter erroneous conclusion comes from a misuse of the lock-in technique. In contrast, using a full grid of dI/dV(V) spectroscopy measurements, we show that the energy-dependent LDOS maps agree very well with state-of-the-art DFT calculations confirming the one-up two-down charge ordering. This structural and charge re-ordering in the $3\times 3$ unit cell is equally driven by electron-electron interactions and the coupling to the substrate.

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