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1.
Qiu XH  Nazin GV  Ho W 《Science (New York, N.Y.)》2003,299(5606):542-546
Tunneling electrons from a scanning tunneling microscope (STM) were used to excite photon emission from individual porphyrin molecules adsorbed on an ultrathin alumina film grown on a NiAl(110) surface. Vibrational features were observed in the light-emission spectra that depended sensitively on the different molecular conformations and corresponding electronic states obtained by scanning tunneling spectroscopy. The high spatial resolution of the STM enabled the demonstration of variations in light-emission spectra from different parts of the molecule. These experiments realize the feasibility of fluorescence spectroscopy with the STM and enable the integration of optical spectroscopy with a nanoprobe for the investigation of single molecules.  相似文献   

2.
Wu SW  Ogawa N  Ho W 《Science (New York, N.Y.)》2006,312(5778):1362-1365
Spatial resolution at the atomic scale has been achieved in the coupling of light to single molecules adsorbed on a surface. Electron transfer to a single molecule induced by green to near-infrared light in the junction of a scanning tunneling microscope (STM) exhibited spatially varying probability that is confined within the molecule. The mechanism involves photo-induced resonant tunneling in which a photoexcited electron in the STM tip is transferred to the molecule. The coupling of photons to the tunneling process provides a pathway to explore molecular dynamics with the combined capabilities of lasers and the STM.  相似文献   

3.
Artificial nanostructures, each composed of a copper(II) phthalocyanine (CuPc) molecule bonded to two gold atomic chains with a controlled gap, were assembled on a NiAl(110) surface by manipulation of individual gold atoms and CuPc molecules with a scanning tunneling microscope. The electronic densities of states of these hybrid structures were measured by spatially resolved electronic spectroscopy and systematically tuned by varying the number of gold atoms in the chains one by one. The present approach provides structural images and electronic characterization of the metal-molecule-metal junction, thereby elucidating the nature of the contacts between the molecule and metal in this junction.  相似文献   

4.
The scanning tunneling microscope (STM) can be used to select a particular adsorbed molecule, probe its electronic structure, dissociate the molecule by using electrons from the STM tip, and then examine the dissociation products. These capabilities are demonstrated for decaborane(14) (B(10)H(14)) molecules adsorbed on a silicon(111)-(7 x 7) surface. In addition to basic studies, such selective dissociation processes can be used in a variety of applications to control surface chemistry on the molecular scale.  相似文献   

5.
Feng M  Zhao J  Petek H 《Science (New York, N.Y.)》2008,320(5874):359-362
The atomic electron orbitals that underlie molecular bonding originate from the central Coulomb potential of the atomic core. We used scanning tunneling microscopy and density functional theory to explore the relation between the nearly spherical shape and unoccupied electronic structure of buckminsterfullerene (C60) molecules adsorbed on copper surfaces. Besides the known pi* antibonding molecular orbitals of the carbon-atom framework, above 3.5 electron volts we found atomlike orbitals bound to the core of the hollow C60 cage. These "superatom" states hybridize like the s and p orbitals of hydrogen and alkali atoms into diatomic molecule-like dimers and free-electron bands of one-dimensional wires and two-dimensional quantum wells in C60 aggregates. We attribute the superatom states to the central potential binding an electron to its screening charge, a property expected for hollow-shell molecules derived from layered materials.  相似文献   

6.
Low-temperature scanning tunneling microscopy was used to selectively break the N-H bond of a methylaminocarbyne (CNHCH3) molecule on a Pt(111) surface at 4.7 kelvin, leaving the C-H bonds intact, to form an adsorbed methylisocyanide molecule (CNCH3). The methylisocyanide product was identified through comparison of its vibrational spectrum with that of directly adsorbed methylisocyanide as measured with inelastic electron tunneling spectroscopy. The CNHCH3 could be regenerated in situ by exposure to hydrogen at room temperature. The combination of tip-induced dehydrogenation with thermodynamically driven hydrogenation allows a completely reversible chemical cycle to be established at the single-molecule level in this system. By tailoring the pulse conditions, irreversible dissociation entailing cleavage of both the C-H and N-H bonds can also be demonstrated.  相似文献   

7.
Tunneling electrons from a low-temperature (5 kelvin) scanning tunneling microscope were used to control, through resonant electronic excitation, the molecular dynamics of an individual biphenyl molecule adsorbed on a silicon(100) surface. Different reversible molecular movements were selectively activated by tuning the electron energy and by selecting precise locations for the excitation inside the molecule. Both the spatial selectivity and energy dependence of the electronic control are supported by spectroscopic measurements with the scanning tunneling microscope. These experiments demonstrate the feasibility of controlling the molecular dynamics of a single molecule through the localization of the electronic excitation inside the molecule.  相似文献   

8.
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   

9.
The scanning tunneling microscope has been used to desorb hydrogen from hydrogen-terminated silicon (100) surfaces. As a result of control of the dose of incident electrons, a countable number of desorption sites can be created and the yield and cross section are thereby obtained. Two distinct desorption mechanisms are observed: (i) direct electronic excitation of the Si-H bond by field-emitted electrons and (ii) an atomic resolution mechanism that involves multiple-vibrational excitation by tunneling electrons at low applied voltages. This vibrational heating effect offers significant potential for controlling surface reactions involving adsorbed individual atoms and molecules.  相似文献   

10.
In monolayer graphene, substitutional doping during growth can be used to alter its electronic properties. We used scanning tunneling microscopy, Raman spectroscopy, x-ray spectroscopy, and first principles calculations to characterize individual nitrogen dopants in monolayer graphene grown on a copper substrate. Individual nitrogen atoms were incorporated as graphitic dopants, and a fraction of the extra electron on each nitrogen atom was delocalized into the graphene lattice. The electronic structure of nitrogen-doped graphene was strongly modified only within a few lattice spacings of the site of the nitrogen dopant. These findings show that chemical doping is a promising route to achieving high-quality graphene films with a large carrier concentration.  相似文献   

11.
The transmission electron energy-loss spectrum shows characteristic "edges" corresponding to the excitation of inner-shell electrons of atoms in a thin sample. Analysis of these edges provides detailed chemical, structural, and electronic data from the radiated volume. By combining electron spectroscopy and electron microscopy, this microanalytical technique can be performed in conjunction with highresolution imaging of the sample. It is shown that this approach has advantages of sensitivity, spatial resolution, and convenience over other comparable techniques.  相似文献   

12.
Magnetotunneling spectroscopy is used as a noninvasive and nondestructive probe to produce two-dimensional spatial images of the probability density of an electron confined in a self-assembled semiconductor quantum dot. The technique exploits the effect of the classical Lorentz force on the motion of a tunneling electron and can be regarded as the momentum (k) space analog of scanning tunneling microscopy imaging. The images reveal the elliptical symmetry of the ground state and the characteristic lobes of the higher energy states.  相似文献   

13.
Real-space observations of long-range electronic perturbations caused by defects have been made with scanning tunneling microscopy. The defects are isolated adsorbed molecules on the surface of graphite. These defects perturb the charge density, giving periodic oscillations similar to Friedel oscillations. The oscillations have a wavelength radical3 times that of the graphite lattice, and the symmetry of the oscillations reflects the nature of the defect.  相似文献   

14.
Much current experimental research on transport in molecular junctions focuses on finite voltages, where substantial polarization-induced nonlinearities may result in technologically relevant device-type responses. Because molecules have strong polarization responses to changing charge state or external field, molecules isolated between electrodes can show strongly nonlinear current-voltage responses. For small applied voltages (up to approximately 0.3 volt), weak interaction between transporting electrons and molecular vibrations provides the basis for inelastic electron tunneling spectroscopy. At higher voltages and for certain time scale regimes, strong coupling effects occur, including Coulomb blockade, negative differential resistance, dynamical switching and switching noise, current hysteresis, heating, and chemical reactions. We discuss a general picture for such phenomena that arise from charging, strong correlation, and polarization (electronic and vibrational) effects in the molecule and at the interface.  相似文献   

15.
Femtosecond laser irradiation is used to excite adsorbed CO molecules on a Cu110 surface; the ensuing motion of individual molecules across the surface is characterized on a site-to-site basis by in situ scanning tunneling microscopy. Adsorbate motion both along and perpendicular to the rows of the Cu110 surface occurs readily, in marked contrast to the behavior seen for equilibrium diffusion processes. The experimental findings for the probability and direction of the molecular motion can be understood as a manifestation of strong coupling between the adsorbates' lateral degrees of freedom and the substrate electronic excitation produced by the femtosecond laser radiation.  相似文献   

16.
A combination of chemical vapor deposition and scanning tunneling microscopy techniques have been used to produce nanometer-scale, iron-containing deposits with high aspect ratios from an iron pentacarbonyl precursor both on a substrate and on the tunneling tip itself. The structure and composition of the resulting nanodeposits were determined by transmission electron microscopy and high spatial resolution Auger electron spectroscopy. Either polycrystalline, relatively pure, body-centered-cubic iron or disordered carbon-rich material can be deposited, depending on the bias conditions of the tip sample junction and the precursor pressure. Two mechanisms of decomposition are inferred from the growth phenomenology.  相似文献   

17.
Wu XL  Zhang Z  Wang YL  Lieber CM 《Science (New York, N.Y.)》1990,248(4960):1211-1214
The structural and electronic effects of lead substitution in the high-temperature superconducting materials Pb(x)Bi(2-x)Sr(2)CaCu(2)O(8) have been characterized by scanning tunneling microscopy (STM) and scanning tunneling spectroscopy (STS). Large-area STM images of the Bi(Pb)-O layers show that lead substitution distorts and disorders the one-dimensional superlattice found in these materials. Atomic-resolution images indicate that extra oxygen atoms are present in the Bi(Pb)-O layers. STS data show that the electronic structure of the Bi(Pb)-O layers is insensitive to lead substitution within +/-0.5 electron volt of the Fermi level; however, a systematic decrease in the density of states is observed at approximately 1 electron volt above the Fermi level. Because the superconducting transition temperatures are independent of x(Pb) (x 相似文献   

18.
By means of scanning tunneling microscopy, it is observed that molecules of the form n-alkylcyanobiphenyl, where n = 8 to 12, form two-dimensional crystalline domains when adsorbed onto graphite. The layer spacings measured by tunneling microscopy are 20% larger than those measured previously on bulk material by x-ray diffraction. The structure of the adsorbed molecules is quite different from that of the bulk.  相似文献   

19.
We have measured the quantum yield for exciting the motion of a single Co atom in CoCu(n) linear molecules constructed on a Cu(111) surface. The Co atom switched between two lattice positions during electron excitation from the tip of a scanning tunneling microscope. The tip location with highest probability for inducing motion was consistent with the position of an active state identified through electronic structure calculations. Atom motion within the molecule decreased with increased molecular length and reflected the corresponding variation in electronic structure.  相似文献   

20.
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   

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