arXiv subjects

Uzi Landman

Publications and source records attributed to Uzi Landman.

85 records · Page 5Linked to original sources

arXiv2000

Multiply charged metal cluster anions

Formation, stability patterns, and decay channels of silver dianionic and gold trianionic clusters are investigated with Penning-trap experiments and a shell-correction method including shape deformations. The theoretical predictions pertaining to the appearance sizes and electronic shell effects are in remarkable agreement with the experiments. Decay of the multiply anionic clusters occurs predominantly by electron tunneling through a Coulomb barrier, rather than via fission, leading to appearance sizes unrelated to those of multiply cationic clusters.

cond-mat.mtrl-sci↗

arXiv2000

Spontaneous symmetry breaking in single and molecular quantum dots

Classes of spontaneous symmetry breaking at zero and low magnetic fields in single quantum dots (QD's) and quantum dot molecules (QDM's) are discussed in relation to the ratio R_W between the interelectron Coulomb repulsion and the harmonic confinement, using spin-and-Space unrestricted Hartree-Fock calculations. These include: Wigner crystallization for R_W > 1, and formation of non-crystallized electron puddles localized on the individual dots in QDM's, as well as spin-density waves in single QD's, for R_W < 1. Erratum: Subsequent to the the publication of our Letter, we have performed further systematic spin-and-space unrestricted Hartree-Fock calculations. While the behavior and magnitudes of the addition energies shown in our Letter are maintained, as well as our finding pertaining to the prevalent violation of Hund's first rule, our improved calculations yield in certain instances different spin polarizations.

cond-mat.mes-hall↗

arXiv2000

Collective and independent-particle motion in two-electron artificial atoms

Investigations of the exactly solvable excitation spectra of two-electron quantum dots with a parabolic confinement, for different values of the parameter R_W expressing the relative magnitudes of the interelectron repulsion and the zero-point kinetic energy of the confined electrons, reveal for large R_W a remarkably well-developed ro-vibrational spectrum associated with formation of a linear trimeric rigid molecule composed of the two electrons and the infinitely heavy confining dot. This spectrum transforms to one characteristic of a "floppy" molecule for smaller values of R_W. The conditional probability distribution calculated for the exact two-electron wave functions allows for the identification of the ro-vibrational excitations as rotations and stretching/bending vibrations, and provides direct evidence pertaining to the formation of such molecules.

cond-mat.mes-hall↗

arXiv2000

Formation and control of electron molecules in artificial atoms: Impurity and magnetic-field effects

Interelectron interactions and correlations in quantum dots can lead to spontaneous symmetry breaking of the self-consistent mean field resulting in formation of Wigner molecules. With the use of spin-and-space unrestricted Hartree-Fock (sS-UHF) calculations, such symmetry breaking is discussed for field-free conditions, as well as under the influence of an external magnetic field. Using as paradigms impurity-doped (as well as the limiting case of clean) two-electron quantum dots (which are analogs to helium-like atoms), it is shown that the interplay between the interelectron repulsion and the electronic zero-point kinetic energy leads, for a broad range of impurity parameters, to formation of a singlet ground-state electron molecule, reminiscent of the molecular picture of doubly-excited helium. Comparative analysis of the conditional probability distributions for the sS-UHF and the exact solutions for the ground state of two interacting electrons in a clean parabolic quantum dot reveals that both of them describe formation of an electron molecule with similar characteristics. The self-consistent field associated with the triplet excited state of the two-electron quantum dot (clean as well as impurity-doped) exhibits symmetry breaking of the Jahn-Teller type, similar to that underlying formation of nonspherical open-shell nuclei and metal clusters. Furthermore, impurity and/or magnetic-field effects can be used to achieve controlled manipulation of the formation and pinning of the discrete orientations of the Wigner molecules. Impurity effects are futher illustrated for the case of a quantum dot with more than two electrons.

cond-mat.mes-hall↗

arXiv2000

Decay channels and appearance sizes of doubly anionic gold and silver clusters

Second electron affinities of Au_N and Ag_N clusters and the dissociation energies for fission of the Au_N^{2-} and Ag_N^{2-} dianions are calculated using the finite-temperature shell-correction method and allowing for triaxial deformations. Dianionic clusters with N > 2 are found to be energetically stable against fission, leaving electron autodetachment as the dominant decay process. The second electron affinities exhibit pronounced shell effects in excellent agreement with measured abundance spectra for Au_N^{2-} (N < 30), with appearance sizes N=12 for gold dianionic clusters and N=24 for silver dianionic clusters.

physics.atm-clus↗

arXiv1999

Photoelectron spectra of aluminum cluster anions: Temperature effects and ab initio simulations

Photoelectron (PES) spectra from aluminum cluster anions (from 12 to 15 atoms) at various temperature regimes, were studied using ab-initio molecular dynamics simulations and experimentally. The calculated PES spectra, obtained via shifting of the simulated electronic densities of states by the self-consistently determined values of the asymptotic exchange-correlation potential, agree well with the measured ones, allowing reliable structural assignments and theoretical estimation of the clusters' temperatures.

physics.atm-clus↗

arXiv1999

Gold nanowires and their chemical modifications

Equilibrium structure, local densities of states, and electronic transport in a gold nanowire made of a four-atom chain supported by two gold electrodes, which has been imaged recently by high-resolution electron microscopy, and chemical modification of the wire via the adsorption of a methylthiol molecule, are investigated with ab-initio local density functional simulations. In the bare wire at the imaged geometry the middle two atoms dimerize, and the structure is strongly modified by the adsorption of the molecule with an accompanying increase of the ballistic conductance through the wire.

cond-mat.mtrl-sci↗

arXiv1999

Dissociation, fragmentation and fission of simple metal clusters

This pedagogical review presents the Shell Correction Method (SCM) and variants thereof, appropriate for describing shape deformations and electronic shell effects, energetics and decay pathways of metal-cluster fragmentation processes (e.g., monomer/dimer dissociation and fission). The experimental trends are compared to the theoretical SCM interpretations, and in addition theoretical results for fission from first-principles molecular-dynamics simulations are discussed. Some latest insights concerning the importance of electronic-entropy and finite-temperature effects are given special attention.

physics.atm-clus↗

arXiv1999

Comment on "Density functional theory study of some structural and energetic properties of small lithium clusters" [J. Chem. Phys. 105, 9933 (1996)]

The Ionization Potentials of small Li_N clusters are calculated with a Shell Correction Method. They are used to illustrate that, within the jellium approximation, deformed cluster shapes provide an adequate description of the observed systematic size dependence of the properties of simple metal clusters. Such deformation effects were overlooked in the analysis of Gardet et al.

physics.atm-clus↗

arXiv1999

Electronic entropy, shell structure, and size-evolutionary patterns of metal clusters

We show that electronic-entropy effects in the size-evolutionary patterns of relatively small (as small as 20 atoms), simple-metal clusters become prominent already at moderate temperatures. Detailed agreement between our finite-temperature-shell-correction-method calculations and experimental results is obtained for certain temperatures. This agreement includes a size-dependent smearing out of fine-structure features, accompanied by a measurable reduction of the heights of the steps marking major-shell and subshell closings, thus allowing for a quantitative analysis of cluster temperatures.

physics.atm-clus↗

arXiv1999

On mesoscopic forces and quantized conductance in model metallic nanowires

Energetics and conductance in jellium modelled nanowires are investigated using the local-density-functional-based shell correction method. In analogy with studies of other finite-size fermion systems, e.g., simple-metal clusters or He-3 clusters, we find that the energetics of the wire as a function of its radius (transverse reduced dimension) leads to formation of self-selecting magic wire configurations (MWC's, i.e., discrete sequence of wire radii with enhanced stability), originating from quantization of the electronic spectrum, namely formation of subbands which are the analogs of electronic shells in clusters. These variations in the energy result in oscillations in the force required to affect a transition from one MWC of the nanowire to another, and are correlated directly with step-wise variations of the quantized conductance of the nanowire in units of 2*e^2/h.

cond-mat.mes-hall↗

arXiv1998

Energetics, forces, and quantized conductance in jellium modeled metallic nanowires

Energetics and quantized conductance in jellium modeled nanowires are investigated using the local density functional based shell correction method, extending our previous study of uniform in shape wires [C. Yannouleas and U. Landman, J. Phys. Chem. B 101, 5780 (1997)] to wires containing a variable shaped constricted region. The energetics of the wire (sodium) as a function of the length of the volume conserving, adiabatically shaped constriction leads to formation of self selecting magic wire configurations. The variations in the energy result in oscillations in the force required to elongate the wire and are directly correlated with the stepwise variations of the conductance of the nanowire in units of 2e^2/h. The oscillatory patterns in the energetics and forces, and the correlated stepwise variation in the conductance are shown, numerically and through a semiclassical analysis, to be dominated by the quantized spectrum of the transverse states at the narrowmost part of the constriction in the wire.

cond-mat.mes-hall↗

arXiv1998

Molecular dynamics in shape space and femtosecond vibrational spectroscopy of metal clusters

We introduce a method of molecular dynamics in shape space aimed at metal clusters. The ionic degrees of freedom are described via a dynamically deformable jellium with inertia parameters derived from an incompressible, irrotational flow. The shell correction method is used to calculate the electronic potential energy surface underlying the dynamics. Our finite temperature simulations of Ag_14 and its ions, following the negative to neutral to positive scheme, demonstrate the potential of pump and probe ultrashort laser pulses as a spectroscopy of cluster shape vibrations.

cond-mat↗