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arXiv 1811.00569cond-mat.str-el
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Co(CO)n/Cu(001):理解近藤效应的化学控制

Co(CO)n/Cu(001): Towards understanding chemical control of the Kondo effect

Marc Philipp Bahlke, Peter Wahl, Lars Diekhöner, Carmen Herrmann

摘要:

近藤效应是一种多体效应,它可以用来研究金属表面自旋极化吸附物的电子和原子结构。它的化学控制是有趣的,因为它加深了这种洞察力,但其潜在的机制只有部分了解。我们研究了增加连接到铜(001)上的钴吸附原子的CO配体的数量的影响,其与实验上Kondo温度$T_K$的增加相关(P.Wahl等人,Phy. Rev. Lett. 95,166601(2005)),通过求解由密度泛函理论(DFT ++)参数化的Anderson杂质模型。我们的结果表明,负责近藤效应的轨道是$d_{x^2-y^2}$的四羰基,和它的组合$d_{z^2}$的二羰基。的分子结构在很大程度上取决于近似的交换-相关功能,这可能与已知的困难描述CO结合到金属表面。这些结构的变化强烈地影响近藤性能,这不仅是一个预测研究的关注,但也感兴趣的检测机械变形和理解的尖端-吸附物相互作用的影响,在扫描隧道显微镜。尽管如此,通过将四羰基限制为$C_{4v}$对称性,如实验数据所示,我们发现结构与$T_K$的实验趋势相容(采用BLYP-D3 + U)。这是不可能的三羰基,尽管扫描的计算参数的范围。对于四羰基和二羰基,增加的$T_K$与费米能级上更大的杂化功能相关,我们可以追溯到Co $3d$轨道与配体的相互作用增加。

英文摘要:

The Kondo effect is a many-body phenomenon allowing insight into the electronic and atomistic structure of spin-polarized adsorbates on metal surfaces. Its chemical control is intriguing because it deepens such insight, but the underlying mechanisms are only partly understood. We study the effect of increasing the number of CO ligands attached to a cobalt adatom on copper(001), which correlates with an increase in the Kondo temperature $T_K$ experimentally (P. Wahl et al, Phy. Rev. Lett. 95, 166601 (2005)), by solving an Anderson impurity model parametrized by density functional theory (DFT++). Our results suggest that the orbital responsible for the Kondo effect is $d_{x^2-y^2}$ for the tetracarbonyl, and its combination with $d_{z^2}$ for the dicarbonyl. The molecular structures depend considerably on the approximate exchange--correlation functional, which may be related to the known difficulty of describing CO binding to metal surfaces. These structural variations strongly affect the Kondo properties, which is not only a concern for predictive studies, but also of interest for detecting mechanical deformations and for understanding the effect of tip--adsorbate interactions in the scanning tunneling microscope. Still, by constraining the tetracarbonyl to $C_{4v}$ symmetry, as suggested by experimental data, we find structures compatible with the experimental trend for $T_K$ (employing BLYP-D3+U). This is not possible for the tricarbonyl despite the range of computational parameters scanned. For the tetra- and dicarbonyl, the increased $T_K$ correlates with a larger hybridization function at the Fermi level, which we trace back to an increased interaction of the Co $3d$ orbitals with the ligands.

机构、总结、中文摘要均由AI分析而来,可能存在错误,请以论文正文为准。

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