Kondo temperature of magnetic impurities at surfaces

Based on the experimental observation that only the close vicinity of a magnetic impurity at metal surfaces determines its Kondo behavior, we introduce a simple model which explains the Kondo temperatures observed for cobalt adatoms at the (111) and (100) surfaces of Cu, Ag, and Au. Excellent agreement between the model and scanning tunneling spectroscopy experiments is demonstrated. The Kondo temperature is shown to depend on the occupation of the d level determined by the hybridization between the adatom and the substrate with a minimum around single occupancy.     

Manipulation of the Kondo effect via two-dimensional molecular assembly

We report the manipulation of a Kondo resonance originating from the spin-electron interactions between a two-dimensional molecular assembly of TBrPP-Co molecules and a Cu(111) surface at 4.6 K. By manipulating nearest-neighbor molecules with a scanning tunneling microscope tip we are able to tune the spin-electron coupling of the center molecule inside a hexagonal molecular assembly in a controlled step-by-step manner. The Kondo temperature increases from 105 to 170 K with decreasing the number of nearest neighbor molecules from six to zero. The scattering of surface electrons by the molecules located at edges of the molecular layer reduces the spin-electron coupling strength for the molecules inside the layer. Investigations of different molecular arrangements indicate that the observed Kondo resonance is independent on the molecular lattice.     

Mapping itinerant electrons around Kondo impurities

We investigate single Fe and Co atoms buried below a Cu(100) surface using low temperature scanning tunneling spectroscopy. By mapping the local density of states of the itinerant electrons at the surface, the Kondo resonance near the Fermi energy is analyzed. Probing bulk impurities in this well-defined scattering geometry allows separating the physics of the Kondo system and the measuring process. The line shape of the Kondo signature shows an oscillatory behavior as a function of depth of the impurity as well as a function of lateral distance. The oscillation period along the different directions reveals that the spectral function of the itinerant electrons is anisotropic.     

Role of surface States in scanning tunneling spectroscopy of (111) metal surfaces with Kondo adsorbates

A nearly free-electron model to describe scanning tunneling spectroscopy of (111) metal surfaces with Kondo impurities is presented. Surface states are found to play an important role giving a larger contribution to the conductance of Cu(111) and Au(111) than Ag(111) surfaces. The different line shapes observed when Co is adsorbed on the different substrates are mainly determined by the position of the surface band onset relative to the Fermi energy and the decay length of the surface state into the substrate. The lateral dependence of the line shape amplitude is found to be bulklike for R|| < or approximately 3-5 A and surfacelike at larger distances, in agreement with experimental data.     

Two-site Kondo effect in atomic chains

Linear CoCu(n)Co clusters on Cu(111) fabricated by atomic manipulation represent a two-site Kondo system with tunable interaction. Scanning tunneling spectroscopy reveals oscillations of the Kondo temperature T(K) with the number n of Cu atoms for n≥3. Density functional calculations show that the Ruderman-Kittel-Kasuya-Yosida interaction mediated by the Cu chains causes the oscillations. Calculations find ferromagnetic and antiferromagnetic interaction for n=1 and 2, respectively. Both interactions lead to a decrease of T(K) as experimentally observed.     

First-principles calculation of the single impurity surface Kondo resonance

We perform first-principles calculations of the surface and bulk wave functions of the Cu(111) surface and their hybridization energies to a Co adatom, including the potential scattering from the Co. By analyzing the calculated hybridization energies, we find the bulk states dominate the contribution to the Kondo temperature, in agreement with recent experiments. Furthermore, we also calculate the tunneling conductance of a scanning tunneling microscope and compare our results with recent experiments of Co impurities in the Cu(111) surface. Good quantitative agreement is found at short parallel impurity-tip distances (<6 A). Our results indicate the need for a new formulation of the problem at larger distances.     

Evolution of Kondo resonance from a single impurity molecule to the two-dimensional lattice

The successive spectral evolution of the Kondo resonance state was investigated from a single iron(II) phthalocyanine molecule to the two-dimensional lattice on Au(111) by interrogating the individual molecules with a scanning tunneling microscope. A sharp Kondo peak appears in the single-impurity regime, which broadens and splits as the lattice builds up. The origin of spectral evolution together with the electronic ground state of the lattice are discussed based on the competition of the Kondo effect and Rudermann-Kittel-Kasuya-Yosida coupling between the molecular spins.     

钴原子及其团簇在Rh(111)和Pd(111)表面的扫描隧道显微学研究

利用扫描隧道显微镜和扫描隧道谱(STM/STS)及单原子操纵,系统研究了单个钴原子(Co) 及其团簇在Rh (111)和Pd (111)两种表面的吸附和自旋电子输运性质. 发现单个Co原子在Rh (111)上有两种不同的稳定吸附位,分别对应于hcp和fcc空位, 他们的高度明显不同,在针尖的操纵下单个Co原子可以在两种吸附位之间相互转化. 在这两种吸附位的单个Co原子的STS谱的费米面附近都存在很显著的峰形结构, 经分析认为Rh (111)表面单个Co原子处于混价区,因此这一峰结构是d轨道共振 和近藤共振共同作用的结果.对于Rh (111)表面上的Co原子二聚体和三聚体, 其费米面附近没有观测到显著的峰,这可能是由于原子间磁交换相互作用 和原子间轨道杂化引起的体系态密度改变所共同导致.与Rh (111)表面不同, 在Pd (111)表面吸附的单个Co原子则表现出均一的高度.并且对于Pd (111)表面所有 单个Co原子及其二聚体和三聚体,在其STS谱的费米面附近均未探测到显著的电子结构, 表明Co原子吸附于Pd (111)表面具有与Rh (111)表面上不同的原子-衬底相互作用与自旋电子输运性质.     

通过单分子化学调控单个离子磁性--单分子"手术"开启分子磁性"开关"

报道了如何通过改变单个磁性离子的化学环境来调控其白旋性质．利用扫描隧道显微镜，对吸附于Au（111）表面的单个钴酞菁分子进行化学修饰，通过在针尖上施加一定的电压脉冲，将分子配合体外层的8个氢原子“剪裁”掉，使其与金衬底形成稳定的化学键合．在这个新的人造分子结构中，其中心钴离子的电子态在费米面上出现强烈的共振峰；通过理论的模拟和分析，发现出现这一共振峰的原因是，脱氢和与衬底的化学结合使中心钴离子自旋性质发生改变，从而导致了输运特性中近藤效应（Kondo effect）的出现．     

Conductance and Kondo effect in a controlled single-atom contact

The tip of a low-temperature scanning tunneling microscope is brought into contact with individual cobalt atoms adsorbed on Cu(100). A smooth transition from the tunneling regime to contact occurs at a conductance of G approximately G0. Spectroscopy in the contact regime, i.e., at currents in a muA range, was achieved and indicated a significant change of the Kondo temperature TK. Calculations indicate that the proximity of the tip shifts the cobalt d band and thus affects TK.     

Spin-resolved splitting of Kondo resonances in the presence of RKKY-type coupling

We have performed spin-resolved measurements on a Kondo impurity in the presence of RKKY-type exchange coupling. By placing manganese phthalocyanine (MnPc) molecules on Fe-supported Pb islands, a Kondo system is devised which is exchange coupled to a magnetic substrate via conduction electrons in Pb, inducing spin splitting of the Kondo resonance. The spin-polarized nature of the split Kondo resonance and a spin filter effect induced by spin-flip inelastic electron tunneling are revealed by spin-polarized scanning tunneling microscopy and spectroscopy.     

Link between adatom resonances and the Cu(111) Shockley surface state

Low-temperature scanning tunneling microscopy and spectroscopy at 7 K was used to assemble and characterize native adatom islands of successive size on the Cu(111) surface. Starting from the single adatom we observe the formation of a series of quantum states which merge into the well known two-dimensional Shockley surface state in the limit of large islands. Our experiments reveal a natural physical link between this fundamental surface property and the sp(z) hybrid resonance associated with the single Cu/Cu(111) adatom.     

Au(111)表面吸附单个八乙基钴卟啉分子的电子态和输运性质调控

通过低温超高真空扫描隧道显微镜及其谱学方法研究并展示了分子配体在调控表面吸附的单个八乙基钴卟啉(CoOEP)分子的电子态和输运性质中的重要作用. 通过单分子剪裁可以脱去该分子外围的甲基, 并在中心钴原子的微分电导谱中观察测到d轨道共振到近藤共振的演变. 实验结果结合第一性原理的理论计算研究表明, 在脱去甲基前后中心钴原子的化学环境和磁矩均未发生显著变化, 这一演变可以通过一个简化模型来阐释并被归结为脱去甲基后分子配体与衬底成键改变了体系隧穿参数所导致. 此外, 实验结果表明CoOEP分子配体的输运性质可受到分子间距离和范德华相互作用的显著调控. 在CoOEP低聚体中位于分子之间的乙基被抬高, 同时在其微分电导谱谱中0–0.8 V区域内新出现一个强的共振峰. 这一新的共振峰表现出等间距的多峰细节, 其峰间距与卟啉环和乙基之间的C–C键伸缩模式能量符合. 这一新共振峰的出现被归结为由于分子局部与衬底耦合减弱形成双结隧穿体系所导致的振子态隧穿峰.     

Surface-state localization at adatoms

Low-temperature scanning tunneling spectroscopy of magnetic and nonmagnetic metal atoms on Ag(111) and on Cu(111) surfaces reveals the existence of a common electronic resonance at an energy below the binding energies of the surface states. Using an extended Newns-Anderson model, we assign this resonance to an adsorbate-induced bound state, split off from the bottom of the surface-state band, and broadened by the interaction with bulk states. A line shape analysis of the bound state indicates that Ag and Cu adatoms on Ag(111) and Cu(111), respectively, decrease the surface-state lifetime, while a cobalt adatom causes no significant change.     

Temperature dependence of a single Kondo impurity

Recent advances in scanning tunneling microscopy have allowed the observation of the Kondo effect for individual magnetic atoms. One hallmark of the Kondo effect is a strong temperature-induced broadening of the Kondo resonance. In order to test this prediction for individual impurities, we have investigated the temperature dependent electronic structure of isolated Ti atoms on Ag(100). We find that the Kondo resonance is strongly broadened in the temperature range T = 6.8 K to T = 49.0 K. These results are in good agreement with theoretical predictions for Kondo impurities in the Fermi liquid regime, and confirm the role of electron-electron scattering as the main thermal broadening mechanism.     

Theory of the fano resonance in the STM tunneling density of states due to a single kondo impurity

The conduction electron density of states nearby single magnetic impurities, as measured recently by scanning tunneling microscopy (STM), is calculated, taking into account tunneling into conduction electron states only. The Kondo effect induces a narrow Fano resonance in the conduction electron density of states. The line shape varies with the distance between STM tip and impurity, in qualitative agreement with experiments, but is very sensitive to details of the band structure. For a Co impurity the experimentally observed width and shift of the Kondo resonance are in accordance with those obtained from a combination of band structure and strongly correlated calculations.     

Long-lived excited states at surfaces: Cs/Cu(111) and Cs/Cu(100) systems

One-electron and multielectron contributions to the decay of transient states in the Cs/Cu(111) and (100) systems are studied by a joined wave-packet propagation and many-body metal response approach. The long lifetime of these states is due to the Cu L and X band gaps which reduce the electron tunneling between Cs and Cu. In the (111) case, the decay is mainly by inelastic e-e interaction, whereas in the (100) case, electron tunneling is dominating. This accounts very well for the experimental findings [Bauer et al., Phys. Rev. B 55, 10 040 (1997) and Ogawa et al., Phys. Rev. Lett. 82, 1931 (1999)].     

Localization of the Cu111 surface state by single Cu adatoms

The Cu adatom-induced localization of the two-dimensional Shockley surface state at the Cu(111) surface was identified from experimental and simulated scanning tunneling microscopy spectra. The localization gives rise to a resonance located just below the surface state band edge. The adatom-induced surface state localization is discussed in terms of the existence theorem for bound states in any attractive two-dimensional potential. We also identify adatom-induced resonance states deriving from atomic orbitals in both experimental and simulated spectra.     

Triphenylene adsorption on Cu(111) and relevant graphene self-assembly

Investigations on adsorption behavior of triphenylene(TP) and subsequent graphene self-assembly on Cu(111) were carried out mainly by using scanning tunneling microscopy(STM).At monolayer coverage,TP molecules formed a longrange ordered adsorption structure on Cu(111) with an uniform orientation.Graphene self-assembly on the Cu(111) substrate with TP molecules as precursor was achieved by annealing the sample,and a large-scale graphene overlayer was successfully captured after the sample annealing up to 1000 K.Three different Moire patterns generated from relative rotational disorders between the graphene overlayer and the Cu(111) substrate were observed,one with 40 rotation between the graphene overlayer and the Cu(111) substrate with a periodicity of 2.93 nm,another with 70 rotation and 2.15 nm of the size of the Moire supercell,and the third with 100 rotation with a periodicity of 1.35 nm.     

Influence of copper crystal surface on the CVD growth of large area monolayer graphene

We study the influence of the surface structure of copper single crystals on the growth of large area monolayer graphene by chemical vapor deposition (CVD) in ultra-high vacuum (UHV). Using atomic-resolution scanning tunneling microscopy (STM), we find that graphene grows primarily in registry with the underlying copper lattice for both Cu(111) and Cu(100). The graphene has a hexagonal superstructure on Cu(111) with a significant electronic component,whereas it has a linear superstructure on Cu(100). Graphene on Cu(111) forms a microscopically uniform sheet, the quality of which is determined by the presence of grain boundaries where graphene grains with different orientations meet. Graphene grown on Cu(100) under similar conditions does not form a uniform sheet and instead displays exposed nanoscale edges. Our results indicate the importance of the copper crystal structure on the microstructure of graphene films produced by CVD.