Thermal nucleation of cavities in liquid helium at negative pressures

We have investigated the nucleation rate at which cavities are formed in 4He and 3He at negative pressures due to thermal fluctuations. To this end, we have used a density functional that reproduces the He liquid-gas interface along the coexistence line. The inclusion of thermal effects in the calculation of the barrier against nucleation results in a sizable decrease of the absolute value of the tensile strength above 1.5 K.

Multipole surface-plasmon modes on simple metals

The average multipole surface-plasmon energy for simple metals, as well as that of ordinary surface and bulk plasmons, is obtained using energy-weighted moments of the electronic response to sufficiently general external perturbations. A local approximation of exchange and correlation effects is used within a jellium model. Band-structure effects are incorporated through an effective electronic mass. Taking advantage of the transparency of the method, we analyze under what circumstances such modes might be observable. It is shown that due to an interplay between Coulomb and kinetic energies, the multipole modes become unobservable for increasing values of the transferred momentum (q) parallel to the surface. The value of q at which the multipole mode becomes unobservable is much smaller than the cutoff value for Landau damping. The effect of the electronic surface diffuseness is also analyzed. We compare our results with previous density-functional calculations and with recent experimental data for Na, K, and Cs.

Structure and far-infrared edge modes of quantum antidots at zero magnetic field

We have investigated edge modes of different multipolarity sustained by quantum antidots at zero magnetic field. The ground state of the antidot is described within a local-density-functional formalism. Two sum rules, which are exact within this formalism, have been derived and used to evaluate the energy of edge collective modes as a function of the surface density and the size of the antidot.

Magnetic-field dependence of hole levels in self-assembled InGaAs quantum dots

Recent magnetotransport experiments of holes in InGaAs quantum dots [D. Reuter, P. Kailuweit, A. D. Wieck, U. Zeitler, O. Wibbelhoff, C. Meier, A. Lorke, and J. C. Maan, Phys. Rev. Lett. 94, 026808 (2005)] are interpreted by employing a multiband k¿p Hamiltonian, which considers the interaction between heavy hole and light hole subbands explicitly. No need of invoking an incomplete energy shell filling is required within this model. The crucial role we ascribe to the heavy hole-light hole interaction is further supported by one-band local-spin-density functional calculations, which show that Coulomb interactions do not induce any incomplete hole shell filling and therefore cannot account for the experimental magnetic field dispersion.

Structure and Stability of 3He Droplets

We have studied the structure of 3He droplets at zero temperature using a density functional approach plus a configuration interaction calculation in an harmonic oscillator major shell. The most salient feature of open shell drops is that the valence atoms couple their spins to the maximum value compatible with Pauli's principle, building a large magnetic moment. We have determined that 29 atoms constitute the smallest self-bound droplet.

Pinning of quantized vortices in helium drops by dopant atoms and molecules

Using a density functional method, we investigate the properties of liquid 4He droplets doped with atoms (Ne and Xe) and molecules ( SF6 and hydrogen cyanide). We consider the case of droplets having a quantized vortex pinned to the dopant. A liquid-drop formula is proposed that accurately describes the total energy of the complex and allows one to extrapolate the density functional results to large N. For a given impurity, we find that the formation of a dopant+vortex+4HeN complex is energetically favored below a critical size Ncr. Our results support the possibility to observe quantized vortices in helium droplets by means of spectroscopic techniques.

Probing vortices in 4He nanodroplets

We present static and dynamical properties of linear vortices in 4He droplets obtained from density functional calculations. By comparing the adsorption properties of different atomic impurities embedded in pure droplets and in droplets where a quantized vortex has been created, we suggest that Ca atoms should be the dopant of choice to detect vortices by means of spectroscopic experiments.

Electronic structure and properties of Cu2O

The structural and electronic properties of Cu2O have been investigated using the periodic Hartree-Fock method and a posteriori density-functional corrections. The lattice parameter, bulk modulus, and elastic constants have been calculated. The electronic structure of and bonding in Cu2O are analyzed and compared with x-ray photoelectron spectroscopy spectra, showing a good agreement for the valence-band states. To check the quality of the calculated electron density, static structure factors and Compton profiles have been calculated, showing a good agreement with the available experimental data. The effective electron and hole masses have been evaluated for Cu2O at the center of the Brillouin zone. The calculated interaction energy between the two interpenetrated frameworks in the cuprite structure is estimated to be around -6.0 kcal/mol per Cu2O formula. The bonding between the two independent frameworks has been analyzed using a bimolecular model and the results indicate an important role of d10-d10 type interactions between copper atoms.

Ab initio cluster-model study of the on-top chemisorption of F and Cl on Si(111) and Ge(111) surfaces

The interaction of atomic F and Cl with Si4H9 and Ge4H9 cluster models has been studied by using ab initio pseudopotentials and basis sets of increasing complexity. The results show that the effect of d orbitals is important in order to reproduce the experimental findings. However, the use of polarization functions in the atoms which are directly involved in the chemisorption bond leads to results which are very close to those obtained using extended basis sets. The local nature of the chemisorption bond is also interpreted by means of a Mulliken population analysis. For F-Si4H9 and Cl-Si4H9 the present results are in good agreement with previous ab initio all-electron calculations, and for the chemisorption of Cl on Si(111) and Ge(111) surfaces, good agreement is found with respect to the available experimental results as well as with previous slab calculations based on the local-density-functional formalism.

Electronic structure and properties of Cu2O

The structural and electronic properties of Cu2O have been investigated using the periodic Hartree-Fock method and a posteriori density-functional corrections. The lattice parameter, bulk modulus, and elastic constants have been calculated. The electronic structure of and bonding in Cu2O are analyzed and compared with x-ray photoelectron spectroscopy spectra, showing a good agreement for the valence-band states. To check the quality of the calculated electron density, static structure factors and Compton profiles have been calculated, showing a good agreement with the available experimental data. The effective electron and hole masses have been evaluated for Cu2O at the center of the Brillouin zone. The calculated interaction energy between the two interpenetrated frameworks in the cuprite structure is estimated to be around -6.0 kcal/mol per Cu2O formula. The bonding between the two independent frameworks has been analyzed using a bimolecular model and the results indicate an important role of d10-d10 type interactions between copper atoms.

Electric dipole polarizability in 208Pb: insights from the droplet model

We study the electric dipole polarizability α D in 208 Pb based on the predictions of a large and representative set of relativistic and nonrelativistic nuclear mean-field models. We adopt the droplet model as a guide to better understand the correlations between α D and other isovector observables. Insights from the droplet model suggest that the product of α D and the nuclear symmetry energy at saturation density J is much better correlated with the neutron skin thickness r np of 208 Pb than the polarizability alone. Correlations of α D J with r np and with the symmetry energy slope parameter L suggest that α D J is a strong isovector indicator. Hence, we explore the possibility of constraining the isovector sector of the nuclear energy density functional by comparing our theoretical predictions against measurements of both α D and the parity-violating asymmetry in 208 Pb. We find that the recent experimental determination of α D in 208 Pb in combination with the range for the symmetry energy at saturation density J = [31 ± (2) est] MeV suggests r np (208 Pb) = 0 . 165 ± (0 . 009) expt ± (0 . 013) theor ± (0.021) est fm and L = 43 ± (6) expt ± (8) theor ± (12) est MeV

Importance of the embedding environment on the strain within small rings in siliceous materials

The effect of the local environment on the energetic strain within small (SiO)N rings (with N=2,3) in silica materials is investigated via periodic model systems employing density functional calculations. Through comparison of the energies of various nonterminated systems containing small rings in strained and relatively unstrained environments, with alpha quartz, we demonstrate how small ring strain is affected by the nature of the embedding environment. We compare our findings with numerous previously reported calculations, often predicting significantly different small-ring strain energies, leading to a critical assessment of methods of calculating accurate localized ring energies. The results have relevance for estimates of the strain-induced response (e.g., chemical, photo, and radio) of small silica rings, and the propensity for them to form in bulk glasses, thin films, and nanoclusters.

Estudo da adsorção de hidrogênio e sulfeto na superfície de paládio: aspectos experimentais (eletroquímica) e teóricos (ab initio e Teoria do Funcional da Densidade)

The adsorption of H and S2- species on Pd (100) has been studied with ab initio, density-functional calculations and electrochemical methods. A cluster of five Pd atoms with a frozen geometry described the surface. The computational calculations were performed through the GAUSSIAN94 program, and the basis functions adapted to a pseudo-potential obtained by using the Generator Coordinate Method adapted to the this program. Using the cyclic voltammetry technique through a Model 283 Potentiostat/Galvanostat E.G.&G-PAR obtained the electrochemical results. The calculated chemisorption geometry has a Pd-H distance of 1.55Å, and the potential energy surface was calculated using the Becke3P86//(GCM/DFT/SBK) methodology. The adsorption of S2- ions on Pd surface obtained both through comparison between the experimental and theoretical results, at MP2 level, suggest a S2- absorption into the metallic cluster. The produced Pd-(S2-) system was show to be very stable under the employed experimental conditions. The paper has shows the powerful aid of computational methods to interpret adsorption experimental data.

Reduced ceria nanofilms from structure prediction

Experimentally, Ce2O3 films are used to study cerium oxide in its fully or partially reduced state, as present in many applications. We have explored the space of low energy Ce2O3 nanofilms using structure prediction and density functional calculations, yielding more than 30 distinct nanofilm structures. First, our results help to rationalize the roles of thermodynamics and kinetics in the preparation of reduced ceria nanofilms with different bulk crystalline structures (e.g. A-type or bixbyite) depending on the support used. Second, we predict a novel, as yet experimentally unresolved, nanofilm which has a structure that does not correspond to any previously reported bulk A2B3 phase and which has an energetic stability between that of A-type and bixbyite. To assist identification and fabrication of this new Ce2O3 nanofilm we calculate some observable properties and propose supports for its epitaxial growth.

Optical spectroscopy of organic material based on C60

The structure and optical properties of thin films based on C60 materials are studied. Reproducible vacuum method of thin fullerene films production with Cd impurity on Si, glass and mica surfaces is developed. Surface morphology of the films are investigated by AFM and SEM methods. The ab initio quantum - chemical calculations of the geometry, total energy and excited energy states of complex fullerene- cadmium telluride supramolecules are performed. Photoluminescence spectra of composite thin films based on C60 before and after X-ray irradiation were measured. The intensity of additional peaks is defined as the charge composition due to the type of substrate. These results are interpreted as an appearance of the dipole-allowed transitions in the fullerene excited singlet states spectrum cause of an interference with cadmium telluride. X-ray irradiated films were investigated, and additional peaks in photoluminescence spectra were detected. These peaks appear as a result of molecular complexes formation from C60CdTe mixture and dimerization of the films. Density functional B3LYP quantum-chemical calculations for C60CdTe, molecular complexes, (C60)2 and C120O dimers were performed to elucidate some experimental results.