Nuclear Hartree-Fock calculations on parallel computers

Hartree-Fock (HF) calculations have had remarkable success in describing large nuclei at high spin, temperature and deformation. To allow full range of possible deformations, the Skyrme HF equations can be discretized on a three-dimensional mesh. However, such calculations are currently limited by the computational resources provided by traditional supercomputers. To take advantage of recent developments in massively parallel computing technology, we have implemented the LLNL Skyrme-force static and rotational HF codes on Intel's DELTA and GAMMA systems at Caltech.

We decomposed the HF code by assigning a portion of the mesh to each node, with nearest neighbor meshes assigned to nodes connected by communication· channels. This kind of decomposition is well-suited for the DELTA and the GAMMA architecture because the only non-local operations are wave function orthogonalization and the boundary conditions of the Poisson equation for the Coulomb field.

Our first application of the HF code on parallel computers has been the study of identical superdeformed (SD) rotational bands in the Hg region. In the last ten years, many SD rotational bands have been found experimentally. One very surprising feature found in these SD rotational bands is that many pairs of bands in nuclei that differ by one or two mass units have nearly identical deexcitation gamma-ray energies. Our calculations of the five rotational bands in ^(192)Hg and ^(194)Pb show that the filling of specific orbitals can lead to bands with deexcitation gamma-ray energies differing by at most 2 keV in nuclei differing by two mass units and over a range of angular momenta comparable to that observed experimentally. Our calculations of SD rotational bands in the Dy region also show that twinning can be achieved by filling or emptying some specific orbitals.

The interpretation of future precise experiments on atomic parity nonconservation (PNC) in terms of parameters of the Standard Model could be hampered by uncertainties in the atomic and nuclear structure. As a further application of the massively parallel HF calculations, we calculated the proton and neutron densities of the Cesium isotopes from A = 125 to A = 139. Based on our good agreement with experimental charge radii, binding energies, and ground state spins, we conclude that the uncertainties in the ratios of weak charges are less than 10^(-3), comfortably smaller than the anticipated experimental error.

Coherent quantum control of atomic and molecular processes by using the technique of laser pulses

Several schemes for coherent quantum control of atomic and molecular processes have been proposed and investigated by using the techniques of adiabatic passage and ultrashort pulses, respectively. Some interesting results have been found.

Studying atomic-resolution by X-ray fluorescence holography

In this work, the results of numerical simulations of X-ray fluorescence holograms and the reconstructed atomic images for Fe single crystal are given. The influences of the recording angles ranges and the polarization effect on the reconstruction of the atomic images are discussed. The process for removing twin images by multiple energy fluorescence holography and expanding the energy range of the incident X-rays to improve the resolution of the reconstructed images is presented. (c) 2005 Elsevier B.V. All rights reserved.

Negative refractive index in a four-level atomic system

We propose a scheme for realizing negative refractive index in a four-level atomic system. It is shown that such a system can simultaneously exhibit negative permittivity and negative permeability in an optical frequency range. Furthermore, by analysing the dispersion property of the left-handed material, we find that the probe beam can be controlled from superluminal to subluminal or vice versa via choosing appropriate parameters.

Electronic structure and phonon thermodynamics of iron alloys

Inelastic neutron scattering (INS) and nuclear-resonant inelastic x-ray scattering (NRIXS) were used to measure phonon spectra of FeV as a B2- ordered compound and as a bcc solid solution. Contrary to the behavior of ordering alloys studied to date, the phonons in the B2-ordered phase are softer than in the solid solution. Ordering increases the vibrational entropy, which stabilizes the ordered phase to higher temperatures. Ab initio calculations show that the number of electronic states at the Fermi level increases upon ordering, enhancing the screening between ions, and reducing the interatomic force constants. The effect of screening is larger at the V atomic sites than at the Fe atomic sites.

The phonon spectra of Au-rich alloys of fcc Au-Fe were also measured. The main effect on the vibrational entropy of alloying comes from a stiffening of the Au partial phonon density of states (DOS) with Fe concentration that increases the miscibility gap temperature. The magnitude of the effect is non- linear and it is reduced at higher Fe concentrations. Force constants were calculated for several compositions and show a local stiffening of Au–Au bonds close to Fe atoms, but Au–Au bonds that are farther away do not show this effect. Phonon DOS curves calculated from the force constants reproduced the experimental trends. The Au–Fe bond is soft and favors ordering, but a charge transfer from the Fe to the Au atoms stiffens the Au–Au bonds enough to favor unmixing. The stiffening is attributed to two main effects comparable in magnitude: an increase in electron density in the free-electron-like states, and stronger sd-hybridization.

INS and NRIXS measurements were performed at elevated temperatures on B2-ordered FeTi and NRIXS measurements were performed at high pressures. The high-pressure behavior is quasi- harmonic. The softening of the phonon DOS curves with temperature is strongly nonharmonic. Calculations of the force constants and Born-von Karman fits to the experimental data show that the bonds between second nearest neighbors (2nn) are much stiffer than those between 1nn, but fits to the high temperature data show that the former softens at a faster rate with temperature. The Fe–Fe bond softens more than the Ti–Ti bond. The unusual stiffness of the 2nn bond is explained by the calculated charge distribution, which is highly aspherical and localized preferentially in the t2g orbitals. Ab initio molecular dynamics (AIMD) simulations show a charge transfer from the t2g orbitals to the eg orbitals at elevated temperatures. The asphericity decreases linearly with temperature and is more severe at the Fe sites.

Effects of Lorentz local field correction on propagation properties of few-cycle pulse in dense Λ-type atomic medium

By solving numerically the full Maxwell-Bloch equations without the slowly varying envelope approximation and the rotating-wave approximation, we investigate the effects of Lorentz local field correction (LFC) on the propagation properties of few-cycle laser pulse in a dense A-type three-level atomic medium. We find that: when the area of the input pulse is larger, split of pulse occurs and the number of the sub-pulses with LFC is larger than that without LFC; at the same distance, the time interval between the first sub-pulse and the second sub-pulse in the case without LFC is longer than that with LFC, the time of pulse appearing in the case without LFC is later than that in the case with LFC, and the two phenomena are more obvious with propagation distance increasing; time evolution rules of the populations of levels vertical bar 1 >, vertical bar 2 > and vertical bar 3 > in the two cases with and without LFC are much different. When the area of the input pulse is smaller, effects of LFC on time evolutions of the pulse and populations are remarkably smaller than those in the case of larger area pulse. (c) 2008 Elsevier B.V. All rights reserved.

Phase control of switching from positive to negative index material in a four-level atomic system

Electric and magnetic responses of the medium to the probe field are analysed in a four-level loop atomic system by taking into account the relative phase of the applied fields. An interesting phenomenon is found: under suitable conditions, a change of the refractive index from positive to negative can occur by modulating the relative phase of the applied fields. Then the medium can be switched from a positive index material to a negative index material in our scheme. In addition, a negative index material can be realized in different frequency regions by adjusting the relative phase. It may give us a convenient way to obtain the desired material with positive or negative index.

Sideband manipulation of population inversion in a three-level Λ atomic system

Sideband manipulation of population inversion in a three-level A atomic configuration is investigated theoretically. Compared with the case of a nearly monochromatic field, a population inversion between an excited state and a ground state has been found in a wide sideband intensity range by increasing the difference in frequency between three components. Furthermore, the population inversion can be controlled by the sum of the relative phases of the sideband components of the trichromatic pump field with respective to the phase of the central component. Changing the sum phase from 0 to pi, the population inversion between the excited state and the ground state can increase within nearly half of the sideband intensity range. At the same time, the sideband intensity range that corresponds to the system exhibiting inversion rho(00) > rho 11 also becomes wider evidently.

Trichromatic manipulation of Kerr nonlinearity in a three-level lambda atomic system

Trichromatic manipulation of Kerr nonlinearity in a three-level A atomic configuration is investigated theoretically. It is shown that for a weak monochromatic probe field, the enhanced Kerr nonlinearity can be achieved in multiple separate transparent windows due to interference effect of multiple two-photon Raman channels. Furthermore, the property of Kerr nonlinearity can be controlled by the sum of the relative phases of the sideband components of the trichromatic pump field compared to the central component.

Atom localization in a four-level alkaline earth atomic system

We propose an atom localization scheme for a four-level alkaline earth atom via a classical standing-wave field, and give the analytical expressions of the localization peak positions as well as the widths versus the parameters of the optical fields. We show that the probability of finding the atom at a particular position can be increased from 1/4 to 1/3 or 1/2 by adjusting the detuning of the probe field and the Rabi frequencies of the optical fields. Furthermore, the localization precision can be dramatically enhanced by increasing the intensity of the standing-wave field or decreasing the detuning of the probe field. The analytical results are quite accordant to the numerical solutions.

Crystal Coulomb energies: I. Organic donor-acceptor complexes--a review. II. Classical Ewald calculations of the Coulomb binding energy of four donor-acceptor crystals and Wurster's blue perchlorate. III. A rapid-convergence quantum-mechanical formalism for crystal electronic energies

Chapter I

Theories for organic donor-acceptor (DA) complexes in solution and in the solid state are reviewed, and compared with the available experimental data. As shown by McConnell et al. (Proc. Natl. Acad. Sci. U.S., 53, 46-50 (1965)), the DA crystals fall into two classes, the holoionic class with a fully or almost fully ionic ground state, and the nonionic class with little or no ionic character. If the total lattice binding energy 2ε₁ (per DA pair) gained in ionizing a DA lattice exceeds the cost 2ε_o of ionizing each DA pair, ε₁ + ε_o less than 0, then the lattice is holoionic. The charge-transfer (CT) band in crystals and in solution can be explained, following Mulliken, by a second-order mixing of states, or by any theory that makes the CT transition strongly allowed, and yet due to a small change in the ground state of the non-interacting components D and A (or D⁺ and A^-). The magnetic properties of the DA crystals are discussed.

Chapter II

A computer program, EWALD, was written to calculate by the Ewald fast-convergence method the crystal Coulomb binding energy E_C due to classical monopole-monopole interactions for crystals of any symmetry. The precision of E_C values obtained is high: the uncertainties, estimated by the effect on E_C of changing the Ewald convergence parameter η, ranged from ± 0.00002 eV to ± 0.01 eV in the worst case. The charge distribution for organic ions was idealized as fractional point charges localized at the crystallographic atomic positions: these charges were chosen from available theoretical and experimental estimates. The uncertainty in E_C due to different charge distribution models is typically ± 0.1 eV (± 3%): thus, even the simple Hückel model can give decent results.

E_C for Wurster's Blue Perchl orate is -4.1 eV/molecule: the crystal is stable under the binding provided by direct Coulomb interactions. E_C for N-Methylphenazinium Tetracyanoquino- dimethanide is 0.1 eV: exchange Coulomb interactions, which cannot be estimated classically, must provide the necessary binding.

EWALD was also used to test the McConnell classification of DA crystals. For the holoionic (1:1)-(N,N,N',N'-Tetramethyl-para- phenylenediamine: 7,7,8,8-Tetracyanoquinodimethan) E_C = -4.0 eV while 2ε_o = 4.6₅ eV: clearly, exchange forces must provide the balance. For the holoionic (1:1)-(N,N,N',N'-Tetramethyl-para- phenylenediamine:para-Chloranil) E_C = -4.4 eV, while 2ε_o = 5.0 eV: again EC falls short of 2ε₁. As a Gedankenexperiment, two nonionic crystals were assumed to be ionized: for (1:1)-(Hexamethyl- benzene:para-Chloranil) E_C = -4.5 eV, 2ε_o = 6.6 eV; for (1:1)- (Napthalene:Tetracyanoethylene) E_C = -4.3 eV, 2ε_o = 6.5 eV. Thus, exchange energies in these nonionic crystals must not exceed 1 eV.

Chapter III

A rapid-convergence quantum-mechanical formalism is derived to calculate the electronic energy of an arbitrary molecular (or molecular-ion) crystal: this provides estimates of crystal binding energies which include the exchange Coulomb inter- actions. Previously obtained LCAO-MO wavefunctions for the isolated molecule(s) ("unit cell spin-orbitals") provide the starting-point. Bloch's theorem is used to construct "crystal spin-orbitals". Overlap between the unit cell orbitals localized in different unit cells is neglected, or is eliminated by Löwdin orthogonalization. Then simple formulas for the total kinetic energy Q^(XT)_λ, nuclear attraction [λ/λ]^XT, direct Coulomb [λλ/λ'λ']^XT and exchange Coulomb [λλ'/λ'λ]^XT integrals are obtained, and direct-space brute-force expansions in atomic wavefunctions are given. Fourier series are obtained for [λ/λ]^XT, [λλ/λ'λ']^XT, and [λλ/λ'λ]^XT with the help of the convolution theorem; the Fourier coefficients require the evaluation of Silverstone's two-center Fourier transform integrals. If the short-range interactions are calculated by brute-force integrations in direct space, and the long-range effects are summed in Fourier space, then rapid convergence is possible for [λ/λ]^XT, [λλ/λ'λ']^XT and [λλ'/λ'λ]^XT. This is achieved, as in the Ewald method, by modifying each atomic wavefunction by a "Gaussian convergence acceleration factor", and evaluating separately in direct and in Fourier space appropriate portions of [λ/λ]^XT, etc., where some of the portions contain the Gaussian factor.

Interaction between single molecules of Mac-1 and ICAM-1 in living cells: An atomic force microscopy study

The interaction between integrin macrophage differentiation antigen associated with complement three receptor function (Mac-1) and intercellular adhesion molecule-1 (ICAM-1), which is controlled tightly by the ligand-binding activity of Mac-1, is central to the regulation of neutrophil adhesion in host defense. Several "inside-out" signals and extracellular metal ions or antibodies have been found to activate Mac-1, resulting in an increased adhesiveness of Mac-1 to its ligands. However, the molecular basis for Mac-1 activation is not well understood yet. In this work, we have carried out a single-molecule study of Mac-1/ICAM-1 interaction force in living cells by atomic force microscopy (AFM). Our results showed that the binding probability and adhesion force of Mac-1 with ICAM-1 increased upon Mac-1 activation. Moreover, by comparing the dynamic force spectra of different Mac-1 mutants, we expected that Mac-1 activation is governed by the downward movement of its alpha 7 helix. (c) 2007 Elsevier Inc. All rights reserved.

Electromagnetically induced negative refractive index in a V-type four-level atomic system

We propose a scheme for realizing negative refractive index in a V-type four-level atomic system. It is shown that the negative refractive index can be achieved in a wide frequency band based on the effect of quantum coherence. It is also found that the frequency band of negative refractive index and the absorption property of left-handed material are manipulated by the pump and control fields. Furthermore, left-handed material with reduced absorption is possible by choosing appropriate parameters. (c) 2006 Elsevier B.V. All rights reserved.