arXiv subjects

W. Schattke

Publications and source records attributed to W. Schattke.

13 recordsLinked to original sources

arXiv2019

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.

cond-mat.mes-hall↗

arXiv2015

Propagation of the photoelectron wave packet in an attosecond streaking experiment

Laser-assisted photoemission from a solid is considered within a numerically exactly solvable one-dimensional model of a crystal. The effect of the inelastic scattering and of the finite duration of the pump pulse on the photoelectron dynamics is elucidated. The phenomenological result that the photoexcited wave packet moves with the group velocity dE/dk and traverses on average the distance equal to the mean free path is found to hold for energies far from the spectral gaps of the final state band structure. On the contrary, close to a spectral gap the photoelectron is found to move during the excitation by the pump pulse with a velocity higher than the group velocity.

cond-mat.mtrl-sci↗

arXiv2007

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.

cond-mat.other↗

arXiv2006

Three-dimensional band structure of layered TiTe2: Photoemission final-state effects

Three-dimensional band structure of unoccupied and occupied states of the prototype layered material TiTe2 is determined focusing on the GammaA line of the Brillouin zone. Dispersions and lifetimes of the unoccupied states, acting as the final states in the photoemission process, are determined from a very-low-energy electron diffraction experiment supported by first-principles calculations based on a Bloch waves treatment of multiple scattering. The experimental unoccupied states of TiTe2 feature dramatic non-free-electron effects such as multiband composition and non-parabolic dispersions. The valence band layer-perpendicular dispersions are then determined from a photoemission experiment consistently interpreted on the basis of the experimental final states to achieve control over the 3-dimensional wavevector. The experimental results demonstrate the absence of the Te 4pz* Fermi surface pocket at the Gamma point and significant self-energy renormalization of the valence band dispersions. Photoemission calculations based on a novel Bloch waves formalism within the one-step theory reveal limitations of understanding photoemission from layered materials such as TiTe2 in terms of direct transitions.

cond-mat.str-el↗

arXiv2006

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.

cond-mat.mtrl-sci↗

arXiv2002

Unoccupied Band Structure of NbSe2 by Very-Low-Energy Electron Diffraction: Experiment and Theory

A combined experimental and theoretical study of very-low-energy electron diffraction at the (0001) surface of 2H-NbSe2 is presented. Electron transmission spectra have been measured for energies up to 50 eV above the Fermi level with k|| varying along the GammaK line of the Brillouin zone. Ab initio calculations of the spectra have been performed with the extended linear augmented plane wave k-p method. The experimental spectra are interpreted in terms of three-dimensional one-electron band structure. Special attention is paid to the quasi-particle lifetimes: by comparing the broadening of the spectral structures in the experimental and calculated spectra the energy dependence of the optical potential Vi is determined. A sharp increase of Vi at 20 eV is detected, which is associated with a plasmon peak in the Im(-1/epsilon) function. Furthermore, the electron energy loss spectrum and the reflectivity of NbSe2 are calculated ab initio and compared with optical experiments. The obtained information on the dispersions and lifetimes of the unoccupied states is important for photoemission studies of the 3D band structure of the valence band.

cond-mat.str-el↗

arXiv2000

Variational quantum Monte Carlo calculations for solid surfaces

Quantum Monte Carlo methods have proven to predict atomic and bulk properties of light and non-light elements with high accuracy. Here we report on the first variational quantum Monte Carlo (VMC) calculations for solid surfaces. Taking the boundary condition for the simulation from a finite layer geometry, the Hamiltonian, including a nonlocal pseudopotential, is cast in a layer resolved form and evaluated with a two-dimensional Ewald summation technique. The exact cancellation of all Jellium contributions to the Hamiltonian is ensured. The many-body trial wave function consists of a Slater determinant with parameterized localized orbitals and a Jastrow factor with a common two-body term plus a new confinement term representing further variational freedom to take into account the existence of the surface. We present results for the ideal (110) surface of Galliumarsenide for different system sizes. With the optimized trial wave function, we determine some properties related to a solid surface to illustrate that VMC techniques provide standard results under full inclusion of many-body effects at solid surfaces.

cond-mat.mtrl-sci↗

arXiv1999

How to determine Fermi vectors by angle resolved photoemission?

Angle resolved photoemission spectroscopy (ARPES) has been commonly applied to evaluate the shape of Fermi surfaces by employing simple criteria for the determination of the Fermi vector k_F parallel to the surface such as maximum photoemission intensity at the Fermi level or discontinuity in the momentum distribution function. Here we show that these criteria may lead to large uncertainties in particular for narrow band systems. We develop a reliable method for the determination of Fermi vectors employing high resolution ARPES at different temperatures. The relevance and accuracy of the method is discussed on data of the quasi two dimensional system TiTe_2.

cond-mat.mtrl-sci↗

arXiv1999

Valence band photoemission from the GaN(0001) surface

A detailed investigation by one-step photoemission calculations of the GaN(0001)-(1x1) surface in comparison with recent experiments is presented in order to clarify its structural properties and electronic structure. The discussion of normal and off-normal spectra reveals through the identified surface states clear fingerprints for the applicability of a surface model proposed by Smith et al. Especially the predicted metallic bonds are confirmed. In the context of direct transitions the calculated spectra allow to determine the valence band width and to argue in favor of one of two theoretical bulk band structures. Furthermore a commonly used experimental method to fix the valence band maximum is critically tested.

cond-mat↗

arXiv1997

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.

cond-mat.mtrl-sci↗

arXiv1997

Energetic and spatial bonding properties from angular distributions of ultraviolet photoelectrons: application to the GaAs(110) surface

Angle-resolved ultraviolet photoemission spectra are interpreted by combining the energetics and spatial properties of the contributing states. One-step calculations are in excellent agreement with new azimuthal experimental data for GaAs(110). Strong variations caused by the dispersion of the surface bands permit an accurate mapping of the electronic structure. The delocalization of the valence states is discussed analogous to photoelectron diffraction. The spatial origin of the electrons is determined, and found to be strongly energy dependent, with uv excitation probing the bonding region.

cond-mat.mtrl-sci↗

arXiv1996

Variational quantum Monte Carlo ground state of GaAs

Variational quantum Monte Carlo calculations are reported for the bulk GaAs semiconductor in order to present values for the ground-state energy, the lattice constant, the bulk modulus, and some derived properties. The statistical accuracy is significantly higher than the remaining differences to the experimental values, especially for the total-energy upper bound. The agreement with experiment is satisfactory. The results are also compared with those of density functional calculations. The accuracy of our results is comparable to the best of those calculations.

mtrl-th↗

arXiv1995

Impact Ionization in ZnS

The impact ionization rate and its orientation dependence in k space is calculated for ZnS. The numerical results indicate a strong correlation to the band structure. The use of a q-dependent screening function for the Coulomb interaction between conduction and valence electrons is found to be essential. A simple fit formula is presented for easy calculation of the energy dependent transition rate.

cond-mat↗