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.Comment: 9 pages with 2 figures (eps) included, Latex 2.09, uses REVTEX style, submitted to Phys. Rev.

Measuring scattering distributions in scanning helium microscopy

A scanning helium microscope typically utilises a thermal energy helium atom beam, with an energy and wavelength (<100 meV, ~0.05 nm) particularly sensitive to surface structure. An angular detector stage for a scanning helium microscope is presented that facilitates the in-situ measurement of scattering distributions from a sample. We begin by demonstrating typical elastic and inelastic scattering from ordered surfaces. We then go on to show the role of topography in diffuse scattering from disordered surfaces, observing deviations from simple cosine scattering. In total, these studies demonstrate the wealth of information that is encoded into the scattering distributions obtained with the technique.Comment: 10 pages, 9 figure

Do schizophrenic patients who managed to get to university have a non-neurodevelopmental form of illness?

Background. Many people who develop schizophrenia have impairments in intellectual and social functioning that are detectable from early childhood. However, some patients do not exhibit such deficits, and this suggests that they may have suffered less neurodevelopmental damage. We hypothesized that the aetiology and form of schizophrenia may differ in such patients. We therefore studied a group of schizophrenic patients who were functioning well enough to enter university prior to illness onset. Methods. The casenotes of 46 university-educated patients and 48 non-university-educated patients were rated on several schedules including the OPCRIT checklist, and the two groups were compared using univariate statistical techniques. Principal components analysis was then performed using data from all patients, and the factor scores for each principal component were compared between groups. Results. Univariate analyses showed the university-educated patients had an excess of depressive symptoms, and a paucity of core schizophrenic symptoms. Four principal components emerged in the principal components analysis: mania, biological depression, schizophrenic symptoms, and a reactive depression. University-educated patients scored significantly higher on the reactive depression principal component, and lower on the schizophrenic symptoms principal component, than the non-university-educated patients. Conclusions. University-educated patients may have a non-developmental subtype of schizophrenia.link_to_subscribed_fulltex

Correlation effects in a quantum dot at high magnetic fields

We investigate the effects of electron correlations on the ground state energy and the chemical potential of a droplet confined by a parabolic potential at high magnetic fields. We demonstrate the importance of correlations in estimating the transition field at which the first edge reconstruction of the maximum density droplet occurs in the spin polarized regime.Comment: 11 pages (revtex) 3 postscript figures are included at the end of the tex file. To appear in Phys. Rev.

New reactive fluorophores in the 1,2,3-trianze series

A one-pot synthesis of new fluorescent 2,5-dihydro-1,2,3-triazines with reactive functional groups and a large Stokes shift of 200 nm is described

New reactive fluorophores in the 1,2,3-trianze series

A one-pot synthesis of new fluorescent 2,5-dihydro-1,2,3-triazines with reactive functional groups and a large Stokes shift of 200 nm is described

Quantum Monte Carlo calculations of the one-body density matrix and excitation energies of silicon

Quantum Monte Carlo (QMC) techniques are used to calculate the one-body density matrix and excitation energies for the valence electrons of bulk silicon. The one-body density matrix and energies are obtained from a Slater-Jastrow wave function with a determinant of local density approximation (LDA) orbitals. The QMC density matrix evaluated in a basis of LDA orbitals is strongly diagonally dominant. The natural orbitals obtained by diagonalizing the QMC density matrix resemble the LDA orbitals very closely. Replacing the determinant of LDA orbitals in the wave function by a determinant of natural orbitals makes no significant difference to the quality of the wave function's nodal surface, leaving the diffusion Monte Carlo energy unchanged. The Extended Koopmans' Theorem for correlated wave functions is used to calculate excitation energies for silicon, which are in reasonable agreement with the available experimental data. A diagonal approximation to the theorem, evaluated in the basis of LDA orbitals, works quite well for both the quasihole and quasielectron states. We have found that this approximation has an advantageous scaling with system size, allowing more efficient studies of larger systems.Comment: 13 pages, 4 figures. To appear in Phys. Rev.

Optimization of inhomogeneous electron correlation factors in periodic solids

A method is presented for the optimization of one-body and inhomogeneous two-body terms in correlated electronic wave functions of Jastrow-Slater type. The most general form of inhomogeneous correlation term which is compatible with crystal symmetry is used and the energy is minimized with respect to all parameters using a rapidly convergent iterative approach, based on Monte Carlo sampling of the energy and fitting energy fluctuations. The energy minimization is performed exactly within statistical sampling error for the energy derivatives and the resulting one- and two-body terms of the wave function are found to be well-determined. The largest calculations performed require the optimization of over 3000 parameters. The inhomogeneous two-electron correlation terms are calculated for diamond and rhombohedral graphite. The optimal terms in diamond are found to be approximately homogeneous and isotropic over all ranges of electron separation, but exhibit some inhomogeneity at short- and intermediate-range, whereas those in graphite are found to be homogeneous at short-range, but inhomogeneous and anisotropic at intermediate- and long-range electron separation.Comment: 23 pages, 15 figures, 1 table, REVTeX4, submitted to PR

Correlated sampling in quantum Monte Carlo: a route to forces

In order to find the equilibrium geometries of molecules and solids and to perform ab initio molecular dynamics, it is necessary to calculate the forces on the nuclei. We present a correlated sampling method to efficiently calculate numerical forces and potential energy surfaces in diffusion Monte Carlo. It employs a novel coordinate transformation, earlier used in variational Monte Carlo, to greatly reduce the statistical error. Results are presented for first-row diatomic molecules.Comment: 5 pages, 2 postscript figure

Photoinduced suppression of the ferroelectric instability in PbTe

The interactions between electrons and phonons drive a large array of technologically relevant material properties including ferroelectricity, thermoelectricity, and phase-change behaviour. In the case of many group IV-VI, V, and related materials, these interactions are strong and the materials exist near electronic and structural phase transitions. Their close proximity to phase instability produces a fragile balance among the various properties. The prototypical example is PbTe whose incipient ferroelectric behaviour has been associated with large phonon anharmonicity and thermoelectricity. Experimental measurements on PbTe reveal anomalous lattice dynamics, especially in the soft transverse optical phonon branch. This has been interpreted in terms of both giant anharmonicity and local symmetry breaking due to off-centering of the Pb ions. The observed anomalies have prompted renewed theoretical and computational interest, which has in turn revived focus on the extent that electron-phonon interactions drive lattice instabilities in PbTe and related materials. Here, we use Fourier-transform inelastic x-ray scattering (FT-IXS) to show that photo-injection of free carriers stabilizes the paraelectric state. With support from constrained density functional theory (CDFT) calculations, we find that photoexcitation weakens the long-range forces along the cubic direction tied to resonant bonding and incipient ferroelectricity. This demonstrates the importance of electronic states near the band edges in determining the equilibrium structure.Comment: 9 page, 3 figure