ABSTRACT
The key to controlling reactions of molecules induced with the current of a scanning tunneling microscope (STM) tip is the ultrashort intermediate excited ionic state. The initial condition of the excited state is set by the energy and position of the injected current; thereafter, its dynamics determines the reaction outcome. We show that a STM can directly and controllably influence the excited-state dynamics. For the STM-induced desorption of toluene molecules from the Si(111)-7x7 surface, as the tip approaches the molecule, the probability of manipulation drops by two orders of magnitude. A two-channel quenching of the excited state is proposed, consisting of an invariant surface channel and a tip height-dependent channel. We conclude that picometer tip proximity regulates the lifetime of the excited state from 10 femtoseconds to less than 0.1 femtoseconds.
ABSTRACT
We have studied electron states present at the Pb(111) surface above Ar-filled nanocavities created by ion beam irradiation and annealing. Vertical confinement between the parallel crystal and nanocavity surfaces creates a series of quantum well state subbands. Differential conductance data measured by scanning tunneling spectroscopy contain a characteristic spectroscopic fine structure within the highest occupied subband, revealing additional quantization. Unexpectedly, reflection at the open boundary where the thin Pb film recovers its bulk thickness gives rise to the lateral confinement of electrons.
ABSTRACT
The tip of a scanning tunnelling microscope is an atomic-scale source of electrons and holes. As the injected charge spreads out, it can induce adsorbed molecules to react. By comparing large-scale 'before' and 'after' images of an adsorbate covered surface, the spatial extent of the nonlocal manipulation is revealed. Here, we measure the nonlocal manipulation of toluene molecules on the Si(111)-7 × 7 surface at room temperature. Both the range and probability of nonlocal manipulation have a voltage dependence. A region within 5-15 nm of the injection site shows a marked reduction in manipulation. We propose that this region marks the extent of the initial coherent (that is, ballistic) time-dependent evolution of the injected charge carrier. Using scanning tunnelling spectroscopy, we develop a model of this time-dependent expansion of the initially localized hole wavepacket within a particular surface state and deduce a quantum coherence (ballistic) lifetime of â¼10 fs.
ABSTRACT
We exploit the ability to precisely control the magnetic domain structure of perpendicularly magnetized Pt/Co/Pt trilayers to fabricate artificial domain wall arrays and study their transport properties. The scaling behavior of this model system confirms the intrinsic domain wall origin of the magnetoresistance, and systematic studies using domains patterned at various angles to the current flow are excellently described by an angular-dependent resistivity tensor containing perpendicular and parallel domain wall resistivities. We find that the latter are fully consistent with Levy-Zhang theory, which allows us to estimate the ratio of minority to majority spin carrier resistivities, rho downward arrow/rho upward arrow approximately 5.5, in good agreement with thin film band structure calculations.
ABSTRACT
The inelastic lifetimes of electrons in image-potential states at Cu(100) that are Stark shifted by the electrostatic tip-sample interaction in the scanning tunneling microscope are calculated using the many-body GW approximation. The results demonstrate that in typical tunneling conditions the image state lifetimes are significantly reduced from their field-free values. The Stark shift to higher energies increases the number of inelastic scattering channels that are available for decay, with field-induced changes in the image state wave function increasing the efficiency of the inelastic scattering through greater overlap with final state wave functions.
ABSTRACT
Quantum corrals are nanoscale structures formed by positioning individual atoms into geometrical arrangements that form closed structures using the STM. They can be used to control the spatial and spectral distribution of surface electrons. The theoretical modelling of these systems is described and illustrated, and the application of the corrals as quantum laboratories for controlling the interactions of surface-state electrons is described. A new three-dimensional scattering model is introduced that extends the description of the electron states within quantum corrals and which can form the basis of many-body calculations of the lifetimes of confined electrons.
ABSTRACT
Modification of the electronic structure of a single Mn adsorbate placed within a geometrical array of adatoms on Ag(111) is observed using local spectroscopy with the scanning tunneling microscope. The changes result from coupling between the adsorbate level and surface electronic states of the substrate. These surface states are scattered coherently within the adatom array, mediating the presence and shape of the array to the adsorbate within. The dimension and geometry of the adatom array thus provide a degree of control over the induced changes.
ABSTRACT
A long-standing discrepancy between experimental and theoretical values for the lifetimes of holes in the surface-state electron bands on noble metal surfaces is resolved; previous determinations of both are found to have been in error. The ability of the scanning tunneling microscope to verify surface quality before taking spectroscopic measurements is used to remove the effects of defect scattering on experimental lifetimes, found to have been a significant contribution to prior determinations. A theoretical treatment of inelastic electron-electron scattering is developed that explicitly includes intraband transitions within the surface state band. In our model, two-dimensional decay channels dominate the electron-electron interactions that contribute to the hole decay and are screened by the electron states of the underlying three-dimensional electron system.
