A new experimental method for the determination of the one phonon density of states in GaAs

The one phonon density of states in GaAs is obtained from the measured disorder-activated-first-order Raman-scattering in Ga_1?xAl_xAs_x alloys. The agreement with several theoretical determinations is excellent. We discuss the requirements that, both the isoelectronic substitution and the experimental conditions must fullfil in order to apply this method to other III–V compounds.     

Disorder activated Raman scattering in Ga1−xAlxAs alloys

We report Raman scattering experiments in mixed crystals Ga_1?xAl_xAs in the spectral range 20 – 400 cm^?1. We performed the measurements for several incident and scattered light polarizations. Besides the D.A.L.A. already observed¹ we find a new band at lower energy. We interpret this structure as due to disorder activated transverse acoustical phonons and label it D.A.T.A. Several weaker bands corresponding to disorder activated optical processes are also seen. Our results are compared with recent calculations of Talwar et al².     

Production and distribution function of fast ions in laser produced plasma

Fast ions theoretical distribution functions deduced from ponderomotive force mechanism are computed and compared to those obtained in laser plasma experiments. Within the limit of validity of the calculations, experimental and theoretical results are in good agreement.     

General properties of the hartree-fock problem demonstrated on the frontier orbital model

The general Hartree-Fock energy in the frontier orbital model in the terms of independent variables is given. The existence conditions for extrema of this expression are derived and their relation with various types of solutions of the HF problem as RHF, UHF and complex wavefunctions is shown. The connection between overall properties of the energy surface and the local properties i.e. the stability and instability conditions of various kinds is demonstrated. The conditions for the occurrence of strange HF solutions are expressed in terms of quantities characterizing the correlation effects. This shows explicitly that the lack of respecting the electronic correlation is the reason for the occurrence of the strange HF solutions for the molecular configurations which exhibit a certain amount of diradical character.The summary of the results has been presented at the 6th Jerusalem Symposium on Quantum Chemistry and Biochemistry and at the I. Congress of Quantum Chemistry, Menton, July 1973.On leave of absence from Institute Rudjer Bokovi, Zagreb, Yugoslavia.     

Search for exotic mesons produced by baryon exchange in the reaction π+p → Λ + x++ at 12 GeV/c

A search for exotic mesons has been carried out at the CERN Omega spectrometer. The baryon-exchange reaction π⁺p → Λ + x⁺⁺ was studied at 12 GeV/c incident beam momentum. No evidence was found for the existence of doubly-charged strange mesons. The upper limit (95% confidence level) for this reaction is 60 nb for exotic mesons with squared masses from 1 to 7 (GeV/c²)² and 150 nb for 7 to 13 (GeV/c²)². These limits are of the same order of magnitude as the exotic cross-sections expected from two-component duality arguments.     

Insights into CO/styrene copolymerization by using Pd(II) catalysts containing modular pyridine-imidazoline ligands

Continuing our studies into the effect that N-N' ligands have on CO/styrene copolymerization, we prepared new C(1)-symmetrical pyridine-imidazoline ligands with 4',5'-cis stereochemistry in the imidazoline ring (5) and 4',5'-trans stereochemistry (6-10) and compared them with our previously reported ligands (1-4). Their coordination to neutral methylpalladium(II) (5 a-10 a) and cationic complexes (5 b-10 b), investigated in solution by NMR spectroscopy, indicates that both the electronic and steric properties of the imidazolines determine the stereochemistry of the palladium complexes. The crystal structures of two neutral palladium precursors [Pd(Me)(2-n)Cl(n)(N-N')] (n=1 for 8 a; n=2 for 9 a') show that the Pd-N coordination distances and the geometrical distortions in the imidazoline ring depend on the electronic nature of the substituents in the imidazoline fragment. Density functional calculations performed on selected neutral and cationic palladium complexes compare well with NMR and X-ray data. The calculations also account for the formation of only one or two stereoisomers of the cationic complexes. The performance of the cationic complexes as catalyst precursors in CO/4-tert-butylstyrene copolymerization under mild pressures and temperatures was analyzed in terms of the productivity and degree of stereoregularity of the polyketones obtained. Insertion of CO into the Pd-Me bond, which was monitored by multinuclear NMR spectroscopy, shows that the N ligand influences the stereochemistry of the acyl species formed.     

Virtual experimentation through 3D full-loop simulation of a circulating fluidized bed

Eulerian granular multiphase model with a drag coefficient correction based on the energy-minimization multi-scale （EMMS） model was used to simulate a semi-industry scale circulating fluidized bed （CFB）. Three-dimensional （3D）, time-dependent simulation of a full-loop CFB revealed that the axial profiles of cross-sectionally averaged solid volume fraction, and the radial profiles of solid axial velocity and solid volume fraction were in reasonable agreement with experimental data. Based on this agreement, database derived from experiments not yet accomplished was replenished with such simulations, and fluid regime diagrams and pressure balance around the CFB loop were derived accordingly. This work presents an integrated viewpoint on CFB and unfolds a fresh paradigm for CFB modeling, which can be expected to help resolve certain issues long in dispute but bard for experiments.     

Theoretical exploration of ultrafast spectroscopy of small clusters

We present the ultrafast multistate nuclear dynamics involving adiabatic and nonadiabatic excited states of non-stoichiometric halide deficient clusters (Na_nF_n-1) characterized by strong ionic bonding and one-excess electron for which the “frozen ionic bonds” approximation has been justified allowing to consider the optical response of the single excess electron in the effective field of the other electrons. We combined the Wigner-Moyal representation of the vibronic density matrix with the ab initio multi state molecular dynamics in the ground and excited electronic states including the nonadiabatic couplings calculated “on the fly” at low computational demand. This method allows the simulation of femtosecond pump-probe and pump-dump signals based on an analytical formulation, which utilizes temperature dependent ground state initial conditions, an ensemble of trajectories carried out on the electronic excited state as well as on the ground state after the passage through the conical intersection in the case of nonadiabatic dynamics and for probing either in the cationic state or in the ground state. The choice of the systems we presented has been made in order to determine the timescales of the fast geometric relaxation leaving the bonding frame intact as during the dynamics in the first excited state of Na₄F₃, and of the bond breaking processes leading to conical intersection between the first excited state and the ground state as in Na₃F₂. The former is the smallest finite system prototype for an surface F-center of bulk color centers. The latter allows to study the photo isomerization in full complexity taking into account all degrees of freedom. In the case of Na₄F₃ after the fast geometric relaxation in the excited state leading to deformed cuboidal structure without breaking of bonds, different types of internal vibrational redistribution (IVR) processes have been identified in pump-dump signals by tuning the dump laser. In contrast, from the analysis of the pump-probe signals of Na₃F₂ cluster, the timescales for the metallic and the ionic bond breaking, as well as for the passage through conical intersection have been determined. Finally the conditions under which these processes can be experimentally observed have been identified. Received 22 December 2000