Dissipative many-electron dynamics of ionizing systems

In this paper, we perform many-electron dynamics using the time-dependent configuration-interaction method in its reduced density matrix formulation (ρ-TDCI). Dissipation is treated implicitly using the Lindblad formalism. To include the effect of ionization on the state-resolved dynamics, we extend a recently introduced heuristic model for ionizing states to the ρ-TDCI method, which leads to a reduced density matrix evolution that is not norm-preserving. We apply the new method to the laser-driven excitation of H(2) in a strongly dissipative environment, for which the state-resolve lifetimes are tuned to a few femtoseconds, typical for dynamics of adsorbate at metallic surfaces. Further testing is made on the laser-induced intramolecular charge transfer in a quinone derivative as a model for a molecular switch. A modified scheme to treat ionizing states is proposed to reduce the computational burden associated with the density matrix propagation, and it is thoroughly tested and compared to the results obtained with the former model. The new approach scales favorably (～N(2)) with the number of configurations N used to represent the reduced density matrix in the ρ-TDCI method, as compared to a N(3) scaling for the model in its original form.     

Impurity analysis of gentamicin bulk samples by improved liquid chromatography-ion trap mass spectrometry

Several gentamicin bulk samples from different origins were investigated using an LC/MS method.LC equipped with ion trap MS with positive ionization was performed on a Capcell Pak C18(AQ) column with the mobile phase containing 50 mM trifluoroacetic(TFA) and methanol.Impurities present in batches of gentamicin bulk samples were elucidated and compared according to their fragmentation behavior.In total seventeen impurities present in samples,five impurities were not elucidated and two compounds were identifi...     

Fluorescence A 4.3 μm en fonction de la pression dans un laser CO2 supraatmospherique

We have observed the 4.3 μm fluorescence signal produced by a superatmospheric double-discharge CO₂ laser, up to a pressure of 5 atm. The evolution of the signal amplitude with pressure reveals an unusual behaviour which we associate to the hot bands. Moreover, we have deduced the V-V relaxation times of CO₂ in mixtures CO₂:N₂:He of (10:5:85) and CO₂:He of (9:91).     

Using preconditioned adaptive step size Runge-Kutta methods for solving the time-dependent Schrödinger equation

If the Hamiltonian is time dependent it is common to solve the time-dependent Schr?dinger equation by dividing the propagation interval into slices and using an (e.g., split operator, Chebyshev, Lanczos) approximate matrix exponential within each slice. We show that a preconditioned adaptive step size Runge-Kutta method can be much more efficient. For a chirped laser pulse designed to favor the dissociation of HF the preconditioned adaptive step size Runge-Kutta method is about an order of magnitude more efficient than the time sliced method.     

Increased Felkin-Anh selectivity using AlMe(3) in the addition of vinyllithiums to alpha-chiral aldehydes: do "ate" complexes play any role?

[reaction: see text] AlMe(3) dramatically increases the diastereoselectivity of addition of vinyllithiums to alpha-chiral aldehydes but decreases that of methyllithium. Our results are explained in terms of an addition of the free vinyllithium on the Me(3)Al-aldehyde complex.     

Pseudogap and spin fluctuations in the normal state of the electron-doped cuprates

We present reliable many-body calculations for the t-t(')-t(')-U Hubbard model that explain in detail the results of recent angle-resolved photoemission experiments on electron-doped high-temperature superconductors. The origin of the pseudogap is traced to two-dimensional antiferromagnetic spin fluctuations whose calculated temperature-dependent correlation length also agrees with recent neutron scattering measurements. We make specific predictions for photoemission, for neutron scattering, and for the phase diagram.     

Strong-coupling perturbation theory of the Hubbard model

The strong-coupling perturbation theory of the Hubbard model is presented and carried out to order (t/U)⁵ for the one-particle Green function in arbitrary dimension. The spectral weight is expressed as a Jacobi continued fraction and compared with new Monte-Carlo data of the one-dimensional, half-filled Hubbard model. Different regimes (insulator, conductor and short-range antiferromagnet) are identified in the temperature-hopping integral (T,t) plane. This work completes a first paper on the subject (Phys. Rev. Lett. 80, 5389 (1998)) by providing details on diagrammatic rules and higher-order results. In addition, the non half-filled case, infinite resummations of diagrams and the double occupancy are discussed. Various tests of the method are also presented. Received 25 October 1999     

Calculating vibrational energies and wave functions of vinylidene using a contracted basis with a locally reorthogonalized coupled two-term Lanczos eigensolver

We use a contracted basis+Lanczos eigensolver approach to compute vinylidene-like vibrational states of the acetylene-vinylidene system. To overcome problems caused by loss of orthogonality of the Lanczos vectors we reorthogonalize Lanczos vector and use a coupled two-term approach. The calculations are done in CC-HH diatom-diatom Jacobi coordinates which make it easy to compute states one irreducible representation at a time. The most costly parts of the calculation are parallelized and scale well. We estimate that the vinylidene energies we compute are converged to approximately 1 cm(-1).     

Improving the numerical convergence of viscous-plastic sea ice models with the Jacobian-free Newton–Krylov method

We have implemented the Jacobian-free Newton–Krylov (JFNK) method to solve the sea ice momentum equation with a viscous-plastic (VP) formulation. The JFNK method has many advantages: the system matrix (the Jacobian) does not need to be formed and stored, the method is parallelizable and the convergence can be nearly quadratic in the vicinity of the solution. The convergence rate of our JFNK implementation is characterized by two phases: an initial phase with slow convergence and a fast phase for which the residual norm decreases significantly from one Newton iteration to the next. Because of this fast phase, the computational gain of the JFNK method over the standard solver used in existing VP models increases with the required drop in the residual norm (termination criterion). The JFNK method is between 3 and 6.6 times faster (depending on the spatial resolution and termination criterion) than the standard solver using a preconditioned generalized minimum residual method. Resolutions tested in this study are 80, 40, 20 and 10 km. For a large required drop in the residual norm, both JFNK and standard solvers sometimes do not converge. The failure rate for both solvers increases as the grid is refined but stays relatively small (less than 2.3% of failures). With increasing spatial resolution, the velocity gradients (sea ice deformations) get more and more important. Nonlinear solvers such as the JFNK method tend to have difficulties when there are such sharp structures in the solution. This lack of robustness of both solvers is however a debatable problem as it mostly occurs for large required drops in the residual norm. Furthermore, when it occurs, it usually affects only a few grid cells, i.e., the residual is small for all the velocity components except in very localized regions. Globalization approaches for the JFNK solver, such as the line search method, have not yet proven to be successful. Further investigation is needed.