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1.
We studied the dynamics of a single cobalt (Co) atom during lateral manipulation on a copper (111) surface in a low-temperature scanning tunneling microscope. The Co binding site locations were revealed in a detailed image that resulted from lateral Co atom motion within the trapping potential of the scanning tip. Random telegraph noise, corresponding to the Co atom switching between hexagonal close-packed (hcp) and face-centered cubic (fcc) sites, was seen when the tip was used to try to position the Co atom over the higher energy hcp site. Varying the probe tip height modified the normal copper (111) potential landscape and allowed the residence time of the Co atom in these sites to be varied. At low tunneling voltages (less than approximately 5 millielectron volts), the transfer rate between sites was independent of tunneling voltage, current, and temperature. At higher voltages, the transfer rate exhibited a strong dependence on tunneling voltage, indicative of vibrational heating by inelastic electron scattering.  相似文献   

2.
We report a method for controllably attaching an arbitrary number of charge dopant atoms directly to a single, isolated molecule. Charge-donating K atoms adsorbed on a silver surface were reversibly attached to a C60 molecule by moving it over K atoms with a scanning tunneling microscope tip. Spectroscopic measurements reveal that each attached K atom donates a constant amount of charge (approximately 0.6 electron charge) to the C60 host, thereby enabling its molecular electronic structure to be precisely and reversibly tuned.  相似文献   

3.
The dynamics of cesium atom motion above the copper(111) surface following electronic excitation with light was studied with femtosecond (10(-15) seconds) time resolution. Unusual changes in the surface electronic structure within 160 femtoseconds after excitation, observed by time-resolved two-photon photoemission spectroscopy, are attributed to atomic motion in a copper-cesium bond-breaking process. Describing the change in energy of the cesium antibonding state with a simple classical model provides information on the mechanical forces acting on cesium atoms that are "turned on" by photoexcitation. Within 160 femtoseconds, the copper-cesium bond extends by 0.35 angstrom from its equilibrium value.  相似文献   

4.
Copper K-edge x-ray absorption data indicate that an axial oxygen-centered lattice instability accompanying the 93 K superconducting transition in YBa(2)Cu(3)O(7) is of a pseudo-(anti)ferroelectric type, in that it appears to involve the softening of a double potential well into a structure in which the difference between the two copper-oxygen distances and the barrier height have both decreased. This softer structure is present only at temperatures within a fluctuation region around the transition. A similar process involving the analogous axial oxygen atom also accompanies the superconducting transition in T1Ba(2)Ca(3)Cu(4)O(11), where the superconducting transition temperature T(c) is ~120 K. The mean square relative displacement of this oxygen atom in YBa(2)Cu(3)O(7) is also specifically affected by a reduction in the oxygen content and by the substitution of cobalt for copper, providing further evidence for the sensitivity of the displacement to additional factors that also influence the superconductivity. On the basis of the implied coupling of this ionic motion to the superconductivity, a scenario for high-temperature superconductivity is presented in which both phonon and electronic (charge transfer) channels are synergistically involved.  相似文献   

5.
The controlled manipulation of silicon at the nanometer scale will facilitate the fabrication of new types of electronic devices. The scanning tunneling microscope (STM) can be used to manipulate strongly bound silicon atoms or clusters at room temperature. Specifically, by using a combination of electrostatic and chemical forces, surface atoms can be removed and deposited on the STM tip. The tip can then move to a predetermined surface site, and the atom or cluster can be redeposited. The magnitude of such forces and the amount of material removed can be controlled by applying voltage pulses at different tip-surface separations.  相似文献   

6.
The atomic force microscope images surfaces by sensing the forces between a sharp tip and a sample. If the tip-sample interaction is dominated by short-range forces due to the formation of covalent bonds, the image of an individual atom should reflect the angular symmetry of the interaction. Here, we report on a distinct substructure in the images of individual adatoms on silicon (111)-(7x7), two crescents with a spherical envelope. The crescents are interpreted as images of two atomic orbitals of the front atom of the tip. Key for the observation of these subatomic features is a force-detection scheme with superior noise performance and enhanced sensitivity to short-range forces.  相似文献   

7.
Junctions between metals and molecules play an important role in molecular electronics. Advances in this field are hampered by the lack of understanding of the electronic structure of organic-metal interfaces. In his Perspective, Kummel highlights the report by Nazin et al. (3), who have used scanning tunneling microscopy (STM) to assemble a metal-molecule-metal junction. Subsequently, they employed the STM tip to probe the atomic structure and local electronic properties of the metal-molecule interface in unprecedented detail. They find evidence for strong coupling between the molecular and metal states. Such coupling affects the conductivity of metal-molecule-metal junctions.  相似文献   

8.
采用第一性原理的密度泛函理论计算了O原子在Rh(100)表面的吸附,得到了电子特性及各种结构参数,并给出了不同覆盖度下O原子在Rh(100)表面上3个位置吸附后的能量,结果表明,O原子在Rh(100)表面可以发生稳定的吸附,最高吸附能为2.53eV。同时,通过对O原子的态密度进行分析,得到如下结论:O原子在Rh(100)面上的吸附主要是由于O的2p轨道与基底金属的4d轨道相互作用的结果。  相似文献   

9.
Boland JJ 《Science (New York, N.Y.)》1993,262(5140):1703-1706
Chlorine atoms strongly chemisorbed at dangling bond sites on the Si(100)-(2 x 1) surface are observed by scanning tunneling microscopy (STM) to hop between adjacent sites. The origin of this behavior is suggested to be an interaction between the field of the probe tip and the dipole moment of the silicon-chlorine bond. Chlorine atom migration is shown to be facilitated by the presence of a metastable chlorine bridge-bonded minimum. The STM probe was used to excite single chlorine atoms into this bridging configuration, resulting in a local population inversion. Selective application of voltage pulses between the probe tip and the surface rearranged the local bonding and induced transformations between different types of chlorine sites. In this manner, adsorbed species can be dissected and their composition and structure directly probed.  相似文献   

10.
Reaction path methods provide a powerful tool for bridging the gap between electronic structure and chemical dynamics. Classical mechanical reaction paths may usually be understood in terms of the force field in the vicinity of a minimum energy path (MEP). When there is a significant component of hydrogenic motion along the MEP and a barrier much higher than the average energy of reactants, quantal tunneling paths must be considered, and these tend to be located on the corner-cutting side of the MEP. As the curvature of the MEP in mass-scaled coordinates is increased, the quantal reaction paths may deviate considerably from the classical ones, and the force field must be mapped out over a wider region, called the reaction swath. The required force fields may be represented by global or semiglobal analytic functions, or the dynamics may be computed "directly" from the electronic structure results without the intermediacy of potential energy functions. Applications to atom and diatom reactions in the gas phase and at gas-solid interfaces and to reactions of polyatomic molecules in the gas phase, in clusters, and in aqueous solution are discussed as examples.  相似文献   

11.
Ye J  Kimble HJ  Katori H 《Science (New York, N.Y.)》2008,320(5884):1734-1738
Precision metrology and quantum measurement often demand that matter be prepared in well-defined quantum states for both internal and external degrees of freedom. Laser-cooled neutral atoms localized in a deeply confining optical potential satisfy this requirement. With an appropriate choice of wavelength and polarization for the optical trap, two electronic states of an atom can experience the same trapping potential, permitting coherent control of electronic transitions independent of the atomic center-of-mass motion. Here, we review a number of recent experiments that use this approach to investigate precision quantum metrology for optical atomic clocks and coherent control of optical interactions of single atoms and photons within the context of cavity quantum electrodynamics. We also provide a brief survey of promising prospects for future work.  相似文献   

12.
Al13- is a cluster known for the pronounced stability that arises from coincident closures of its geometric and electronic shells. We present experimental evidence for a very stable cluster corresponding to Al13I-. Ab initio calculations show that the cluster features a structurally unperturbed Al13- core and a region of high charge density on the aluminum vertex opposite from the iodine atom. This ionically bound magic cluster can be understood by considering that Al13 has an electronic structure reminiscent of a halogen atom. Comparisons to polyhalides provide a sound explanation for our chemical observations.  相似文献   

13.
The energetics and the electronic, magnetic, and geometric structure of the metallocarbohedrene Ti(8)C(12) have been calculated self-consistently in the density functional formulation. The structure of Ti(8)C(12) is a distorted dodecahedron with a binding energy of 6.1 electron volts per atom. The unusual stability is derived from covalent-like bonding between carbon atoms and between titanium and carbon atoms with no appreciable interaction between titanium atoms. The density of states at the Fermi energy is high and is derived from a strong hybridization between titanium 3d and carbon sp electrons. Titanium sites carry a small magnetic moment of 0.35 Bohr magneton per atom and the cluster is only weakly magnetic.  相似文献   

14.
We have measured the angular dependence of chemical bonding forces between a carbon monoxide molecule that is adsorbed to a copper surface and the terminal atom of the metallic tip of a combined scanning tunneling microscope and atomic force microscope. We provide tomographic maps of force and current as a function of distance that revealed the emergence of strongly directional chemical bonds as tip and sample approach. The force maps show pronounced single, dual, or triple minima depending on the orientation of the tip atom, whereas tunneling current maps showed a single minimum for all three tip conditions. We introduce an angular dependent model for the bonding energy that maps the observed experimental data for all observed orientations and distances.  相似文献   

15.
Nilius N  Wallis TM  Ho W 《Science (New York, N.Y.)》2002,297(5588):1853-1856
The ability of a scanning tunneling microscope to manipulate single atoms is used to build well-defined gold chains on NiAl(110). The electronic properties of the one-dimensional chains are dominated by an unoccupied electron band, gradually developing from a single atomic orbital present in a gold atom. Spatially resolved conductance measurements along a 20-atom chain provide the dispersion relation, effective mass, and density of states of the free electron-like band. These experiments demonstrate a strategy for probing the interrelation between geometric structure, elemental composition, and electronic properties in metallic nanostructures.  相似文献   

16.
Rhenium heptafluoride, ReF(7), is one of only two stable binary compounds MX(7) with a heptacoordinated metal atom M and halide atom X. Its low-temperature crystal structure, as determined by high-resolution powder neutron diffraction, reveals the molecular structure, which has been the subject of speculation and debate for many years. Here it is shown within experimental error that at 1.5 kelvin the lowest energy configuration of ReF(7) has symmetry Cs (m) and is a distorted pentagonal bipyramid. The deviation of the two axial Re-F bonds from collinear and the puckering of the ring of equatorial fluorine atoms are similar to what has been postulated as one of the conformations of the pseudorotational motion observed at higher temperatures.  相似文献   

17.
Lee HJ  Ho W 《Science (New York, N.Y.)》1999,286(5445):1719-1722
A scanning tunneling microscope (STM) was used to manipulate the bonding of a carbon monoxide (CO) molecule and to analyze the structure and vibrational properties of individual products. Individual iron (Fe) atoms were evaporated and coadsorbed with CO molecules on a silver (110) surface at 13 kelvin. A CO molecule was transferred from the surface to the STM tip and bonded with an Fe atom to form Fe(CO). A second CO molecule was similarly transferred and bonded with Fe(CO) to form Fe(CO)(2). Controlled bond formation and characterization at the single-bond level probe chemistry at the spatial limit.  相似文献   

18.
The motion of individual cesium atoms trapped inside an optical resonator is revealed with the atom-cavity microscope (ACM). A single atom moving within the resonator generates large variations in the transmission of a weak probe laser, which are recorded in real time. An inversion algorithm then allows individual atom trajectories to be reconstructed from the record of cavity transmission and reveals single atoms bound in orbit by the mechanical forces associated with single photons. In these initial experiments, the ACM yields 2-micrometer spatial resolution in a 10-microsecond time interval. Over the duration of the observation, the sensitivity is near the standard quantum limit for sensing the motion of a cesium atom.  相似文献   

19.
The tip-surface region of a scanning tunneling microscope (STM) emits light when the energy of the tunneling electrons is sufficient to excite luminescent processes. These processes provide access to dynamic aspects of the local electronic structure that are not directly amenable to conventional STM experiments. From monolayer films of carbon-60 fullerenes on gold(110) surfaces, intense emission is observed when the STM tip is placed above an individual molecule. The diameter of this emission spot associated with carbon-60 is approximately 4 angstroms. These results demonstrate the highest spatial resolution of light emission to date with a scanning probe technique.  相似文献   

20.
The electrical resistance of wires consisting of either a single xenon atom or two xenon atoms in series was measured and calculated on the basis of an atom-jellium model. Both the measurement and the calculation yielded a resistance of 10(5) ohms for the single-xenon atom system and 10(7) ohms for the two-xenon atom system. These resistances greatly exceeded the 12,900-ohm resistance of an ideal one-dimensional conduction channel because conduction through the xenon atoms occurs through the tail of the xenon 6s resonance, which lies far above the Fermi level. This conduction process in an atom-sized system can now be understood in terms of the electronic states of individual atoms.  相似文献   

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