Controlled contact to a C60 molecule

The tip of a low-temperature scanning tunneling microscope is approached towards a C60 molecule adsorbed at a pentagon-hexagon bond on Cu(100) to form a tip-molecule contact. The conductance rapidly increases to approximately 0.25 conductance quanta in the transition region from tunneling to contact. Ab-initio calculations within density functional theory and nonequilibrium Green's function techniques explain the experimental data in terms of the conductance of an essentially undeformed C60. The conductance in the transition region is affected by structural fluctuations which modulate the tip-molecule distance.     

Resonant electron heating and molecular phonon cooling in single C60 junctions

We study heating and heat dissipation of a single C(60) molecule in the junction of a scanning tunneling microscope by measuring the electron current required to thermally decompose the fullerene cage. The power for decomposition varies with electron energy and reflects the molecular resonance structure. When the scanning tunneling microscope tip contacts the fullerene the molecule can sustain much larger currents. Transport simulations explain these effects by molecular heating due to resonant electron-phonon coupling and molecular cooling by vibrational decay into the tip upon contact formation.     

Effects of electron-vibration coupling in transport through single molecules

Using scanning tunneling spectroscopy, we study the transport of electrons through C(60)?molecules on different metal surfaces. When electrons tunnel through a molecule, they may excite molecular vibrations. A fingerprint of these processes is a characteristic sub-structure in the differential conductance spectra of the molecular junction reflecting the onset of vibrational excitation. Although the intensity of these processes is generally weak, they become more important as the resonant character of the transport mechanism increases. The detection of single vibrational levels crucially depends on the energy level alignment and lifetimes of excited states. In the limit of large current densities, resonant electron-vibration coupling leads to an energy accumulation in the molecule, which eventually leads to its decomposition. With our experiments on C(60)?we are able to depict a molecular scale picture of how electrons interact with the vibrational degrees of freedom of single molecules in different transport regimes. This understanding helps in the development of stable molecular devices, which may also carry a switchable functionality.     

Bistability of single 1,5 cyclooctadiene molecules on Si(001)

The adsorption and current-induced bistability of single 1,5 cyclooctadiene molecules on Si(001) were studied in ultrahigh vacuum by low-temperature scanning tunneling microscopy (STM). After a dosage of ≈0.05 L at room temperature followed by cooling to the measuring temperature of 7 K, we find that the cyclic alkene molecule preferably adsorbs in the bridge structure with both C=C double bonds reacting with two adjacent Si dimers via [2+2] cycloaddition reaction. The time-dependent current measured upon tunneling through the adsorbed molecule at fixed STM tip height displays a switching between two current levels with the same mean residence time in each level. Higher bias and/or reduced tip height—and therefore higher current—increase the switching rate, suggesting that the reversible switching is due to inelastic electron tunneling. The observed bistability is interpreted as a dynamic interconversion between two degenerate conformations of the adsorbed molecule.     

Initial stage of the adsorption of fluorofullerene molecules on Si surface

Spatially resolved images of an individual C₆₀F₁₈ fluorofullerene molecule on Si(100) − 2 × 1 surface have been obtained using scanning tunneling microscopy. Scanning tunneling microscopy results and ab initio calculations show that the fluorofullerene molecules interact with the Si(100) − 2 × 1 surface with F atoms pointing down towards the surface. The adsorption energy of a C₆₀F₁₈ molecule on Si(100) − 2 × 1 surface is ∼12.1 eV, which is much higher than the adsorption energy of the same molecule on Si(111) − 7 × 7 surface (6.65 eV). C₆₀F₁₈ molecules are located in the troughs in-between the dimer rows occupying the four-dimer site on Si(100) − 2 × 1 surface.     

Selective adsorption of C60 on Ge/Si nanostructures

Selective adsorption of C60 on nanoscale Ge areas can be achieved, while neighboring Si(111) areas remain uncovered, if the whole surface is initially terminated by Bi. Fullerene chemisorption is found at Bi vacancies which form due to partial thermal desorption of the Bi surfactant. The growth rate and temperature dependence of the C60 adsorption were measured using scanning tunneling microscopy and are described consistently by a rate equation model. The selectivity of the C60 adsorption can be traced back to an easier vacancy formation in the Bi layer on top of the Ge areas compared to the Si areas. Furthermore, it is also possible to desorb C60 from Ge areas, allowing the use of C60 as a resist on the nanoscale.     

Preferred orientations of encapsulated C60 molecules inside single wall carbon nanotubes

A systematical study of the orientational behavior of C60 molecules in single wall carbon nanotubes (SWCNTs) with different chirality and diameter has been performed by using a model of an infinite long nanotube filled with two C60 (denoted as C60-1 and C60-2) molecules. We studied the preferred orientation of the C60-1 molecule when the neighboring C60-2 molecule was fixed at the pentagon, double-bond, and hexagon orientations respectively. Our results showed that the C60-1 molecule prefers the pentagon (hexagon) orientation when the tube diameter is smaller (larger) than 1.31nm (1.36nm). For the tube diameter in between, the preferred molecular orientation of C60-1 changes from pentagon to hexagon with the increasing tube diameter when the neighboring C60-2 molecule is fixed at the pentagon or double-bond orientation. A novel vertex orientation for the C60-1 molecule has been found when the C60-2 molecule is fixed at the hexagon orientation.     

Tunneling measurement of a single quantum spin

Measurement of the tunneling current of spin-polarized electrons via a molecule with a localized spin provides information on the orientation of that spin. We show that a strong tunneling current due to the shot noise suppresses the spin dynamics, such as the spin precession in an external magnetic field, and the relaxation due to the environment (quantum Zeno effect). A weak tunneling current preserves the spin precession with the oscillatory component of the current of the same order as the noise. We propose an experiment to observe the Zeno effect in a tunneling system and describe how the tunneling current may be used to read a qubit represented by a single spin 1/2.     

The Unconventional Influence of a Nearby Molecule onto Transport of Single C_(60) Molecule Transistor

We study the transport property of single C_(60) molecular transistors with special focus on the situation that other molecules are in vicinity. The devices are prepared using electromigration and thermal deposition techniques. Pure single C_(60) molecule transistors show typical coulomb blockade behavior at low temperature. When we increase the coverage of molecules slightly by extending the deposition time, the transport spectrum of devices displays a switching behavior in the general coulomb blockade pattern. We attribute this unconventional phenomenon to the influence from a nearby C_(60) molecule. By analyzing this transport behavior quantitatively based on the parallel-double-quantum-dot model, the interaction from the nearby molecule is proved to be of capacity and tunneling coupling. Thermal stimulation is also applied to the device to investigate the effect of local charging environment variation on intermolecular interaction.     

Transformations of C-type defects on Si(100)-2 × 1 surface at room temperature – STM/STS study

We present a scanning tunneling microscopy study of the C-type defects on the Si(100)-2 × 1 surface and their transformations into other defect forms at room temperature. A model of the C defect as a dissociated water molecule was adopted for interpretation of the observed transformations. We explained the transformations by hopping the H or OH between bonding sites on Si dimers. Newly, the most stable defect form, corresponding to the H and hydroxyl group adsorbed on the same dimer, is reported. Real time observations provided an explanation for the defect C2-C2 described earlier. A reversible transition of this defect into another form, not revealed yet, is presented. Electronic structure of the observed defects is studied by means of scanning tunneling spectroscopy. Measured spectra show semiconducting character of the C defect. Spectra of the other defect forms are discussed.     

Emergence and visualization of an interface state during contact formation with a single molecule

Contact formation dynamics and electronic perturbations arising from the interaction of a metallic probe and a single molecule (1,3 cyclohexadiene) bound on the Si (100) surface are examined using a series of plane wave, density functional theory calculations. The approach of the probe induces a relaxation of the molecule that ultimately leads to the formation of an interface state due to a specific interaction between the probe apex atom and the C=C bond of the molecule. The calculated interface state is located 0.2 eV above the Fermi energy, in agreement with low temperature scanning tunneling spectroscopy local density of states data (0.35 eV), and is responsible for the contrast observed in low bias empty-state STM images.     

一种新的C_(60)二维畴拓扑结构

利用低温扫描隧道显微镜对吸附在硫醇膜表面的二维C6 0 岛进行研究 ,首次观察到化学键分辨的C6 0 分子结构 ,并发现一种新型的C6 0 二维取向畴界 .这种畴界仅仅由于两边C6 0 分子的取向不同而存在 ,附近没有结构缺陷 ,畴界附近C6 0 阵列的位置平移序和键取向序都得到了保持 .     

Single C59N molecule as a molecular rectifier

We report a new kind of experimental realization of a molecular rectifier, which is based on a single azafullerene C59N molecule in a double-barrier tunnel junction via the single electron tunneling effect. An obvious rectifying effect is observed. The positive onset voltage is about 0.5-0.7 V, while the negative onset voltage is about 1.6-1.8 V. Theoretical analyses show that the half-occupied molecular orbital of the C59N molecule and the asymmetric shift of the molecular Fermi level when the molecule is charged are responsible for the molecular rectification.     

Adsorption and thermal decomposition of C60 on Co/Si(111)-7 × 7

We present a study on the adsorption and thermal decomposition of C₆₀ on Co covered Si(111)-7 × 7 using scanning tunneling microscopy and X-ray photoelectron spectroscopy. Co-induced magic clusters grown on Si(111)-7 × 7 are identified as a possible adsorption site where 51 ± 3% of C₆₀ molecules adsorb at room temperature. On Co/Si(111)-7 × 7, C₆₀ molecules start to decompose at 450 °C, and are completely dissociated to form SiC by 720 °C. This temperature is significantly lower than 910 °C at which C₆₀ completely dissociates on clean Si(111)-7 × 7. This is a possible low temperature method for growing crystalline SiC films using C₆₀ as a precursor molecule.     

Engineering negative differential conductance with the Cu(111) surface state

Low-temperature scanning tunneling microscopy and spectroscopy are employed to investigate electron tunneling from a C60-terminated tip into a Cu(111) surface. Tunneling between a C60 orbital and the Shockley surface states of copper is shown to produce negative differential conductance (NDC) contrary to conventional expectations. NDC can be tuned through barrier thickness or C60 orientation up to complete extinction. The orientation dependence of NDC is a result of a symmetry matching between the molecular tip and the surface states.     

C59N单分子整流器

通过将单个C59N分子置于双势垒隧道结中，从而利用单电子隧穿效应和C59N分子的特殊能级结构，我们成功地实现了一种新型的单分子整流器件．实验中这个整流器件的正向导通电压约为0．5-0．7V，反向击穿电压约为1．6—1．8V．理论分析表明，中性C59N分子的半占据费米能级以及在不同充电情况下费米能级的不对称移动是形成整流效应的主要原因．其构成原理也决定了该器件具有稳定、易重复的特点．     

Excitation of molecular vibrational modes with inelastic scanning tunneling microscopy processes: examination through action spectra of cis-2-butene on Pd(110)

Inelastically tunneled electrons from a scanning tunneling microscope (STM) were used to induce vibrationally mediated motion of a single cis-2-butene molecule among four equivalent orientations on Pd(110) at 4.8 K. The action spectrum obtained from the motion clearly detects more vibrational modes than inelastic electron tunneling spectroscopy with a STM. We demonstrate the usefulness of the action spectroscopy as a novel single molecule vibrational spectroscopic method. We also discuss its selection rules in terms of resonance tunneling.     

Long-distance electron tunneling in proteins: A new challenge for time-resolved spectroscopy

Long-distance electron tunneling is a fundamental process which is involved in energy generation in cells. The tunneling occurs between the metal centers in the respiratory enzymes, typically over distances up to 20 or 30 such distances, the tunneling time—i.e., the time during which an electron passes through the body of the protein molecule from one metal center to another—is of the order of 10 fs. Here the process of electron tunneling in proteins is reviewed, and a possibility of experimental observation of real-time electron tunneling in a single protein molecule is discussed.     

Tunneling Dynamics Between Any Two Multi-atomic-molecular Bose-Einstein Condensates

Tunneling dynamics of multi-atomic molecules between any two multi-atomic molecular Bose-Einstein condensates with Feshbach resonance is investigated. It is indicated that the tunneling in the two Bose-Einstein condensates depends not only on the inter-molecular nonlinear interactions and the initial number of molecule in these condensates, but also on the tunneling coupling between them. It is discovered that besides oscillating tunneling current between the multi-atomic molecular condensates, the nonlinear multi-atomic molecular tunneling dynamics sustains a self-locked population imbalance: a macroscopic quantum self-trapping effect. The influence of de-coherence caused by non-condensate molecule on the tunneling dynamics is studied. It is shown that de-coherence suppresses the multi-atomic molecular tunneling.