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钾掺杂对二维 Kagome 有机框架在 Ag(111) 表面的影响。

Impact of Potassium Doping on a Two-Dimensional Kagome Organic Framework on Ag(111).

作者信息

Wang Xingyue, Qin Tianchen, Ma Tian, You Sifan, Wang Jia, Hu Lei, Liang Baiyao, Hu Jun, Guo Dezhou, Pan Minghu, Zhu Junfa, Chi Lifeng

机构信息

School of Physics and Information Technology, Shaanxi Normal University, Xi'an 710119, P. R. China.

National Synchrotron Radiation Laboratory, Key Laboratory of Precision and Intelligent Chemistry, Department of Chemical Physics, and Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, University of Science and Technology of China, Hefei, Anhui 230029, P. R. China.

出版信息

J Phys Chem Lett. 2025 Jan 9;16(1):209-214. doi: 10.1021/acs.jpclett.4c03344. Epub 2024 Dec 23.

Abstract

Alkali element doping has significant physical implications for two-dimensional materials, primarily by tuning the electronic structure and carrier concentration. It can enhance interface electronic interactions, providing opportunities for effective charge transfer at metal-organic interfaces. In this work, we investigated the effects of gradually increasing the level of K doping on the lattice structure and electronic properties of an organometallic coordinated Kagome lattice on a Ag(111) surface. With the introduction of K dopants into the 4-fold N-Ag coordinated Kagome lattice, the highly periodic Kagome lattice gradually tends to become discrete. Combining synchrotron radiation photoemission spectroscopy, scanning tunneling microscopy/spectroscopy, and density functional theory calculations, we revealed the mechanism of structural transformation of the lattice, i.e., the change in thermodynamically favored structures caused by competition of electron donors. As an electron donor with a lower ionization energy, K adatoms tend to replace the Ag adatoms and form a more thermodynamically stable N-K coordination structure. Moreover, enhanced charge transfer from K to the Kagome lattice induced a rigid shift of the Fermi level. Our investigation provides new insights for the study of alkali-doped organometallic nanostructures.

摘要

碱金属元素掺杂对二维材料具有重要的物理影响,主要是通过调节电子结构和载流子浓度来实现。它可以增强界面电子相互作用,为金属 - 有机界面的有效电荷转移提供机会。在这项工作中,我们研究了逐渐增加K掺杂水平对Ag(111)表面上有机金属配位的 Kagome 晶格的晶格结构和电子性质的影响。随着K掺杂剂引入到四重N - Ag配位的Kagome晶格中,高度周期性的Kagome晶格逐渐趋于离散。结合同步辐射光电子能谱、扫描隧道显微镜/能谱以及密度泛函理论计算,我们揭示了晶格结构转变的机制,即由电子供体竞争导致的热力学上更有利结构的变化。作为具有较低电离能的电子供体,K吸附原子倾向于取代Ag吸附原子并形成热力学上更稳定的N - K配位结构。此外,从K到Kagome晶格的增强电荷转移导致费米能级的刚性移动。我们的研究为碱掺杂有机金属纳米结构的研究提供了新的见解。

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