Correlated electron transport in molecular electronics

Theoretical and experimental values to date for the resistances of single molecules commonly disagree by orders of magnitude. By reformulating the transport problem using boundary conditions suitable for correlated many-electron systems, we approach electron transport across molecules from a new standpoint. Application of our correlated formalism to benzene-dithiol gives current-voltage characteristics close to experimental observations. The method can solve the open system quantum many-body problem accurately, treats spin exactly, and is valid beyond the linear response regime.

C-60 as a Faraday cage

Endohedral fullerenes have been proposed for a number of technological uses, for example, as a nanoscale switch, memory bit and as qubits for quantum computation. For these technology applications, it is important to know the ease with which the endohedral atom can be manipulated using an applied electric field. We find that the Buckminsterfullerene (C-60) acts effectively as a small Faraday cage, with only 25% of the field penetrating the interior of the molecule. Thus influencing the atom is difficult, but as a qubit the endohedral atom should be well shielded from environmental electrical noise. We also predict how the field penetration should increase with the fullerene radius. (C) 2004 American Institute of Physics.

Accurate and efficient non-adiabatic quantum molecular dynamics approach for laser-matter interactions

A non-adiabatic quantum molecular dynamics approach for treating the interaction of matter with intense, short-duration laser pulses is developed. This approach, which is parallelized to run on massively-parallel supercomputers, is shown to be both accurate and efficient. Illustrative results are presented for harmonic generation occurring in diatomic molecules using linearly polarized laser pulses.

Ionization dynamics of laser-driven H-2(+)

We set out aspects of a numerical algorithm used in solving the full-dimensionality time-dependent Schrodinger equation describing the electronic motion of the hydrogen molecular ion driven by an intense, linearly polarized laser pulse aligned along the molecular axis. This algorithm has been implemented within the fixed inter-nuclear separation approximation in a parallel computer code, a brief summary of which is given. Ionization rates are calculated and compared with results from other methods, notably the time-independent Floquet method. Our results compare very favourably with the precise predictions of the Floquet method, although there is some disagreement with other wavepacket calculations. Visualizations of the electron dynamics are also presented in which electron rescattering is observed.

Molecular effects in the ionization of N-2, O-2, and F-2 by intense laser fields

In this paper we study the response in time of N2, O2, and F2 to laser pulses having a wavelength of 390 nm. We find single-ionization suppression in O2 and its absence in F2, in accordance with experimental results at lambda= 800 nm. Within our framework of time-dependent density functional theory we are able to explain deviations from the predictions of intense-field many-body S-matrix theory (IMST). We confirm the connection of ionization suppression with destructive interference of outgoing electron waves from the ionized electron orbital. However, the prediction of ionization suppression, justified within the IMST approach through the symmetry of the highest occupied molecular orbital (HOMO), is not reliable since it turns out that—e.g., in the case of F2—the electronic response to the laser pulse is rather complicated and does not lead to dominant depletion of the HOMO. Therefore, the symmetry of the HOMO is not sufficient to predict ionization suppression. However, at least for F2, the symmetry of the dominantly ionized orbital is consistent with the nonsuppression of ionization.

Correlation Effects in the Compton Profile of Silicon

Ab initio nonlocal pseudopotential variational quantum Monte Carlo techniques are used to compute the correlation effects on the valence momentum density and Compton profile of silicon. Our results for this case are in excellent agreement with the Lam-Platzman correction computed within the local density approximation. Within the approximations used, we rule out valence electron correlations as the dominant source of discrepancies between calculated and measured Compton profiles of silicon.

Quantized conductance of multiwalled carbon nanotubes

We report calculations of the transport properties of multiwalled carbon nanotubes based on a scattering-theoretic approach that takes into account scattering within each tube, between tubes, and at the metal contacts. We find that only the outer tube contributes to the conductance, as has been implied by experiments. Referring to experiments performed with liquid-metal contacts, we also explain why the measured conductance is close to an integer number of conductance quanta, when the tubes are immersed in the liquid metal for several hundreds of nanometers and is not an integer when they are immersed for only a few nanometers. Finally, we propose that the observed conductance of only one quantum

The basis for the formation of stable metal clusters on an electrode surface

Metal nanoclusters can be produced cheaply and precisely in an electrochemical environment. Experimentally this method works in some systems, but not in others, and the unusual stability of the clusters has remained a mystery. We have simulated the deposition of the clusters using classical molecular dynamics and studied their stability by grand-canonical Monte Carlo simulations. We find that electrochemically stable clusters occur only in those cases where the two metals involved form stable alloys.

Generation of palladium clusters on Au(111) electrodes: Experiments and simulations

The properties of palladium clusters, generated with the electrochemical scanning tunneling microscope, have been investigated both by experiments and by computer simulations. The clusters are found to be larger and more stable if the tip is moved further towards the electrode surface in the generation process. The simulations suggest that the larger clusters consist of a palladium - gold mixture, which is more stable than pure palladium. Dissolution of the clusters occurs from the edges rather than layer by layer

Macroscopic evidence of soliton formation in multiterawatt laser-plasma interaction

A novel physical phenomenon has been observed following the interaction of an intense (10(19) W/cm(2)) laser pulse with an underdense plasma. Long-lived, macroscopic bubblelike structures have been detected through the deflection that the associated electric charge separation causes in a proton probe beam. These structures are interpreted as the remnants of a cloud of relativistic solitons generated in the plasma by the ultraintense laser pulse. This interpretation is supported by an analytical study of the soliton cloud evolution, by particle-in-cell simulations, and by a reconstruction of the proton-beam deflection.

Multi-MeV proton source investigations in ultraintense laser- foil interactions

A study of the properties of multi-MeV proton emission from thin foils following ultraintense laser irradiation has been carried out. It has been shown that the protons are emitted, in a quasilaminar fashion, from a region of transverse size of the order of 100-200 mum. The imaging properties of the proton source are equivalent to those of a much smaller source located several hundred mum in front of the foil. This finding has been obtained by analyzing proton radiographs of periodically structured test objects, and is corroborated by observations of proton emission from laser-heated thick targets.