Direct resolution of unoccupied states in solids via two photon photoemission

Non-linear effects in photoemission are shown to open a new access to the band structure of unoccupied states in solids, totally different from hitherto used photoemission spectroscopy. Despite its second-order nature, strong resonant transitions occur, obeying exact selection rules of energy, crystal symmetry, and momentum. Ab-initio calculations are used to demonstrate that such structures are present in low-energy laser spectroscopy experimental measurements on Si previously published. Similar resonances are expected in ultraviolet angle-resolved photoemission spectra, as shown in a model calculation on Al.Comment: 12 pages, including 4 figure

Electron scattering states at solid surfaces calculated with realistic potentials

Scattering states with LEED asymptotics are calculated for a general non-muffin tin potential, as e.g. for a pseudopotential with a suitable barrier and image potential part. The latter applies especially to the case of low lying conduction bands. The wave function is described with a reciprocal lattice representation parallel to the surface and a discretization of the real space perpendicular to the surface. The Schroedinger equation leads to a system of linear one-dimensional equations. The asymptotic boundary value problem is confined via the quantum transmitting boundary method to a finite interval. The solutions are obtained basing on a multigrid technique which yields a fast and reliable algorithm. The influence of the boundary conditions, the accuracy and the rate of convergence with several solvers are discussed. The resulting charge densities are investigated.Comment: 5 pages, 4 figures, copyright and acknowledgment added, typos etc. correcte

Nanomechanics of a Hydrogen Molecule Suspended between Two Equally Charged Tips

Geometric configuration and energy of a hydrogen molecule centered between two point-shaped tips of equal charge are calculated with the variational quantum Monte-Carlo (QMC) method without the restriction of the Born-Oppenheimer (BO) approximation. Ground state nuclear distribution, stability, and low vibrational excitation are investigated. Ground state results predict significant deviations from the BO treatment that is based on a potential energy surface (PES) obtained with the same QMC accuracy. The quantum mechanical distribution of molecular axis direction and bond length at a sub-nanometer level is fundamental for understanding nanomechanical dynamics with embedded hydrogen. Because of the tips' arrangement, cylindrical symmetry yields a uniform azimuthal distribution of the molecular axis vector relative to the tip-tip axis. With approaching tips towards each other, the QMC sampling shows an increasing loss of spherical symmetry with the molecular axis still uniformly distributed over the azimuthal angle but peaked at the tip-tip direction for negative tip charge while peaked at the equatorial plane for positive charge. This directional behavior can be switched between both stable configurations by changing the sign of the tip charge and by controlling the tip-tip distance. This suggests an application in the field of molecular machines.Comment: 20 pages, 10 figure

Dynamical polarization of graphene under strain

We study the dependence of the plasmon dispersion relation of graphene on applied uniaxial strain. Besides electron correlation at the RPA level, we also include local field effects specific for the honeycomb lattice. As a consequence of the two-band character of the electronic band structure, we find two distinct plasmon branches. We recover the square-root behavior of the low-energy branch, and find a nonmonotonic dependence of the strain-induced modification of its stiffness, as a function of the wavevector orientation with respect to applied strain.Comment: Phys. Rev. B, accepte

Band Mapping in One-Step Photoemission Theory: Multi-Bloch-Wave Structure of Final States and Interference Effects

A novel Bloch-waves based one-step theory of photoemission is developed within the augmented plane wave formalism. Implications of multi-Bloch-wave structure of photoelectron final states for band mapping are established. Interference between Bloch components of initial and final states leads to prominent spectral features with characteristic frequency dispersion experimentally observed in VSe_2 and TiTe_2. Interference effects together with a non-free-electron nature of final states strongly limit the applicability of the common direct transitions band mapping approach, making the tool of one-step analysis indispensable.Comment: 4 jpg figure

Lifetimes of Shockley electrons and holes at the Cu(111) surface

A theoretical many-body analysis is presented of the electron-electron inelastic lifetimes of Shockley electrons and holes at the (111) surface of Cu. For a description of the decay of Shockley states both below and above the Fermi level, single-particle wave functions have been obtained by solving the Schr\"odinger equation with the use of an approximate one-dimensional pseudopotential fitted to reproduce the correct bulk energy bands and surface-state dispersion. A comparison with previous calculations and experiment indicates that inelastic lifetimes are very sensitive to the actual shape of the surface-state single-particle orbitals beyond the $\bar\Gamma$ (${\bf k}_\parallel=0$) point, which controls the coupling between the Shockley electrons and holes.Comment: 4 pages, 3 figures, to appear in Phys. Rev.

Measuring correlated electron dynamics with time-resolved photoemission spectroscopy

Time-resolved photoemission experiments can reveal fascinating quantum dynamics of correlated electrons. However, the thermalization of the electronic system is typically so fast that very short probe pulses are necessary to resolve the time evolution of the quantum state, and this leads to poor energy resolution due to the energy-time uncertainty relation. Although the photoemission intensity can be calculated from the nonequilibrium electronic Green functions, the converse procedure is therefore difficult. We analyze a hypothetical time-resolved photoemission experiment on a correlated electronic system, described by the Falicov-Kimball model in dynamical mean-field theory, which relaxes between metallic and insulating phases. We find that the real-time Green function which describes the transient behavior during the buildup of the metallic state cannot be determined directly from the photoemission signal. On the other hand, the characteristic collapse-and-revival oscillations of an excited Mott insulator can be observed as oscillating weight in the center of the Mott gap in the time-dependent photoemission spectrum.Comment: 12 pages, 5 figure

Two-particle photoemission from strongly correlated systems: A dynamical-mean field approach

We study theoretically the simultaneous, photo-induced two-particle excitations of strongly correlated systems on the basis of the Hubbard model. Under certain conditions specified in this work, the corre- sponding transition probability is related to the two-particle spectral function which we calculate using three different methods: the dynamical-mean field theory combined with quantum Monte Carlo (DMFT- QMC) technique, the first order perturbation theory and the ladder approximations. The results are analyzed and compared for systems at the verge of the metal-insulator transitions. The dependencies on the electronic correlation strength and on doping are explored. In addition, the account for the orbital degeneracy allows an insight into the influence of interband correlations on the two particle excitations. A suitable experimental realization is discussed.Comment: 25 pp, 10 figs. to be published in PR