L. Limot

Visualizing the spin of individual cobalt-phthalocyanine molecules.

Low-temperature spin-polarized scanning tunneling microscopy is employed to study spin transport across single Cobalt-Phathalocyanine molecules adsorbed on well characterized magnetic nanoleads. A spin-polarized electronic resonance is identified over the center of the molecule and exploited to spatially resolve stationary spin states. These states reflect two molecular spin orientations and, as established by density functional calculations, originate from a ferromagnetic molecule-lead superexchange interaction mediated by the organic ligands.

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 Greens 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.

Atom transfer and single-adatom contacts

The point contact of a tunnel tip approaching towards Ag(111) and Cu(111) surfaces is investigated with a low temperature scanning tunneling microscope. A sharp jump to contact, random in nature, is observed in the conductance. After point contact, the tip-apex atom is transferred to the surface, indicating that a one-atom contact is formed during the approach. In sharp contrast, the conductance over single silver and copper adatoms exhibits a smooth and reproducible transition from tunneling to contact regime. Numerical simulations show that this is a consequence of the additional dipolar bonding between the adatom and the surface atoms.

Size-Dependent Surface States of Strained Cobalt Nanoislands on Cu(111)

Low-temperature scanning tunneling spectroscopy over Co nanoislands on Cu(111) showed that the surface states of the islands vary with their size. Occupied states exhibit a sizable downward energy shift as the island size decreases. The position of the occupied states also significantly changes across the islands. Atomic-scale simulations and ab initio calculations demonstrate that the driving force for the observed shift is related to size-dependent mesoscopic relaxations in the nanoislands.

Surface-state Stark shift in a scanning tunneling microscope.

We report a quantitative low-temperature scanning tunneling spectroscopy (STS) study on the Ag(111) surface state over an unprecedented range of currents (50 pA to 6 microA) through which we can tune the electric field in the tunnel junction of the microscope. We show that in STS a sizable Stark effect causes a shift of the surface-state binding energy E0. Data taken are reproduced by a one-dimensional potential model calculation, and are found to yield a Stark-free energy E0 in agreement with recent state-of-the-art photoemission spectroscopy measurements.

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.

Conductance of oriented C60 molecules.

C60 molecules adsorbed to Cu(100) are contacted with the tip of a cryogenic scanning tunneling microscope. Images with submolecular resolution reveal distinct orientations of the molecules. We find that the orientation significantly affects the conductance of the contact despite the high symmetry of C60.

Conductance-driven change of the Kondo effect in a single cobalt atom.

A low-temperature scanning tunneling microscope is employed to build a junction comprising a Co atom bridging a copper-coated tip and a Cu(100) surface. An Abrikosov-Suhl-Kondo resonance is evidenced in the differential conductance and its width is shown to vary exponentially with the ballistic conductance for all tips employed. Using a theoretical description based on the Anderson model, we show that the Kondo effect and the total conductance are related through the atomic relaxations affecting the environment of the Co atom.

Contact to single atoms and molecules with the tip of a scanning tunnelling microscope

Experiments using the tip of a scanning tunnelling microscope to contact atoms and molecules adsorbed on surfaces are reviewed. Conductance quantization upon forming or breaking a contact between the tip and surfaces as well as between the tip and specifically chosen atoms and molecular orbitals is addressed. Imaging the contact area prior to and after contact measurements allows one to monitor the status of the contacted object as well as that of the contacting electrodes. Spectroscopy with the tip in contact with individual atoms or molecules reveals the reproducibility of and control over such experiments today.

Assembly of ferrocene molecules on metal surfaces revisited

Metallocene (MCp2) wires have recently attracted considerable interest in relation to molecular spintronics due to predictions concerning their half-metallic nature. This exciting prospect is however hampered by the little and often-contradictory knowledge we have concerning the metallocene self-assembly and interaction with a metal. Here, we elucidate these aspects by focusing on the adsorption of ferrocene on Cu(111) and Cu(100). Combining low-temperature scanning tunneling microscopy and density functional theory calculations, we demonstrate that the two-dimensional molecular arrangement consists of vertical- and horizontal-lying molecules. The noncovalent T-shaped interactions between Cp rings of vertical and horizontal molecules are essential for the stability of the physisorbed molecular layer. These results provide a fresh insight into ferrocene adsorption on surfaces and may serve as an archetypal reference for future work with this important variety of organometallic molecules.