The shapes of Auger decay lines in photoelectron satellite spectra

The theory of the shapes of Auger decay lines of satellite two-hole-one particle states accompanying photoionization based on the Green's function method is developed. The lineshapes of Auger decay of satellite states [2 s 2 p ]( ^1,3 P )3 s ( ² P ), [2 s 2 p ]( ¹ P )4 s ( ² P ) and [3 s 3 p ]( ³ P )4 s ( ² P ) in valence p-photoelectron spectra of Ne and Ar atoms are calculated (hole states are indicated by square brackets throughout). It is shown that in some cases the Auger lineshapes reproduce the shape of the photoelectron satellite line, but in other cases Auger line may be narrower then the photoelectron line and may have opposite direction of asymmetry. The theoretical results are in agreement with experimental low-energy Auger spectra. Received: 25 May 1998 / Accepted: 2 October 1998     

Synthesis and microwave properties of TI2Ba2CaCu2O8 superconducting films grown by MOCVD

We report on the synthesis, structural and electrical characterization of high quality Tl₂Ba₂Ca₁Cu₂O₈ (Tl-2212) superconducting films. The samples have been grown ex-situ on mm² LaAlO₃ (100) substrates by a combined approach of metal-organic chemical vapor deposition (MOCVD) and thallium vapor diffusion. The morphological and compositional nature of the c-axis oriented films has been investigated by SEM and X-ray analyses. Typical values of K and MA/cm² at 77 K have been measured. Microwave measurements have been performed at f = 87 GHz inserting the film in a copper cavity and at f =1.5 GHz on patterned samples using a microstrip resonator technique. A penetration depth nm is evaluated by fitting the microwave data with phenomenological equations. The minimum value of the surface resistance measured at 4.2 K is 60 and 6 m at 1.5 GHz and 87 GHz respectively. The microwave data are described in the context of a modified two fluid model. An evaluation of the temperature dependence of the scattering rate has been performed through the simultaneous measurement of the surface resistance and the penetration depth. Received 16 December 1999 and Received in final form 17 March 2000     

Sextet levels in the phosphorus-like ion Cu

Delayed spectra of foil-excited fast Cu ions have been studied to find a number of 3s3p⁴, 3 s2 3 p2 3 d and 3s3p^33d levels in the P-like ion Cu¹⁴⁺ (spectrum Cu XV). Among these are 3 s 3 p3 3 d ⁶ D levels, which have never been observed before, although they are the lowest excited states that have the same parity as the ground configuration. The investigation combined theory and experiment. The calculations used the Cowan code with semi-empirically scaled parameters and extensive MCDF computations. Received: 14 April 1998 / Accepted: 18 April 1998     

Finestructure, hyperfine structure and isotope shift of 4f 6s7s in Er I

The isotope shift (IS) and hyperfine structure (hfs) of nine levels (31720 to 38921 cm^-1) assigned to the configuration 4 f ¹² 6 s 7 s in neutral erbium have been determined experimentally using Doppler-reduced saturation absorption spectroscopy in a gas discharge. We performed a fine structure analysis in the SL-coupling scheme of the single configuration 4 f ¹² 6 s 7 s, confirming and extending the classification of even parity Er I levels. We discriminated the different hfs contributions of the 4f¹² core and the (6 s +7 s) outer electrons of the shell in a non-relativistic JJ-coupling approach and in the relativistic effective tensor operator formalism in SL-coupling. The relativistic one-electron parameters of the hfs for ¹⁶⁷Er were fitted to the experimental data by a least squares fit procedure: [0pt] a ⁰¹ _4f =-147(3) MHz, [0pt] a ¹⁰ _6s + a ¹⁰ _7s =-1840(30) MHz, [0pt] b ⁰² _4f =6560(80) MHz. The level dependencies of the isotope shift were evaluated based on crossed second order (CSO) effects. We obtained the following results for the CSO parameters for the isotope pairs ^170-168Er: d _6s7s =-740(30) MHz, z _4f = 0(5) MHz, ( g _3,6s ( f , 6 s )+ g _{3, 7s} ( f , 7 s ))= -24(15) MHz and for ^170-166Er: d _6s7s =-1500(50) MHz, z _4f =0(10) MHz, ( g _3,6s ( f ,6 s )+ g _3,7s ( f +7 s ))=-50(29) MHz. The resulting parameters for the hfs are compared with those known for other configurations of the Er atom and ion. Received 16 May 1999 and Received in final form 31 January 2000     

Persistent spectral hole-burning in a -doped aluminosilicate glass from 8 to 295 K: Study of the burning and refilling kinetics, and of optical dephasing

High-temperature persistent spectral hole-burning (PSHB), up to room temperature, has been observed in a Eu ³⁺ -doped aluminosilicate glass using a high peak-power nanosecond dye laser. Spontaneous refilling as well as thermal cycling measurements show that at least two mechanisms, a fast and a slow one, are involved in our sample. We suggest that the fast or “easy” component may correspond to a non-photochemical local rearrangement of the host or to photoreduction of the Eu ³⁺ ions and that the second one leading to very stable photoproducts may correspond to transfer of an electron over a sizable distance through a several-step process. The mechanisms we suggest agree with light-induced hole refilling measurements. Line broadening mechanisms are discussed and the temperature-dependent part of the homogeneous width and of the spectral shift is interpreted in terms of a two-phonon (Raman) process involving pseudo-local phonons. Received 28 July 1999     

Quantum theory of the magneto-optical effect induced by Ni ions in barium ferrites

To reveal the physical origin of the giant magneto-optical enhancement of Ni²⁺ ions in barium ferrite, quantitative calculations of the contributions of both the intra-ionic electric dipole transition between the 3d⁸ and 3d^{7 4p} configurations of the Ni²⁺ ions and the intra-ionic electric dipole transition induced by odd-parity crystal field terms are presented. It is deduced that the transition is important in the origin of the considered magneto-optical enhancement. The most important factor is the Ni-Fe superexchange interaction; since it is strong enough, the Faraday rotation produced by the Ni²⁺ ions is large though the energy difference between the 3d⁸ and 3 d7 4 p configurations is large. It is demonstrated that though the intra-ionic electric dipole transition does produce Faraday rotation peaks in the visible range, their magnitude is too small to explain the observed Faraday rotation. The effect of the spin-orbit interaction on the Faraday rotation is analysed. The spin-orbit interaction of the ground configuration plays a very important role in the occurrence of Faraday effects, but the Faraday rotation does not increase linearly with the strength of the spin-orbit coupling. On the contrary, the spin-orbit interaction of the excited configuration has almost no effect on the Faraday rotation. It is shown that the mixing of the different multiplets of the ground term induced by the crystal field has a great influence on the magneto-optical properties. Received 7 January 1998     

Charge ordering-disordering in the Th-doped CaMnO3

The structural transitions that appear in the manganites Ca_1-xTh_xMnO₃ versus temperature are studied in connection with their magnetic and transport properties, and compared to those of the Ca_1-xLn_xMnO₃ manganites. An orthorhombic to monoclinic transition is observed for low x values (;this structural distortion, also observed for Ln-doped oxides, is related to the magnetoresistance properties. For higher x values (), modulated commensurate and incommensurate phases are obtained at low temperature, with , b =2 a p and , which are related to Mn³⁺/Mn⁴⁺ charge ordering (CO) phenomena. T values, determined from electron diffraction, are in agreement with those determined from the M ( T ) curves. The low temperature electron microscopy shows that the CO in those oxides is more complex than in Ln-doped manganites. In particular, the destabilisation of CO and consequently of the antiferromagnetic interactions is evidenced as the thorium content increases which may explain the appearance of a spin-glass like behavior for higher x values not seen for Ca_1-xSm_xMnO₃ phases . Received 2 November 1998     

Photofragmentation of hydrated iron ions Fe(HO) () at 532, 355 and 266 nm

Photofragmentation of Fe(H₂O)n ⁺ clusters (n =1-9) is investigated at three different wavelengths, 532, 355 and 266 nm. Two fragmentation pathways are observed depending essentially on the photon energy, but also on the parent size n. The fragmentation products belong to two ion families, Fe(H₂O)m ⁺ and FeOH(H₂O)m ⁺ , which correspond to dehydration and intracluster dehydrogenation reactions respectively. The ion yields are studied as a function of the laser fluence in order to determine the number of photons implied in the photofragmentation process. This allows us to estimate that the D[(H₂O)_n-1Fe^+-(H₂O)] bond energy is ranging between 0.44 eV and 0.55 eV for .Photon absorption cross sections are also derived from the fluence experiments, and two different behaviors are observed: i) At 355 nm, far away from any transition, progressive solvation of the metal ion results in an increasing absorption cross section from n =2 to n =9. This can be attributed to a forbidden transition of bare , which becomes progressively allowed because of the interaction with more and more water ligands. ii) At 266 nm, close to several allowed transitions of bare , a distinct maximum is observed for the absorption of ion. It may be attributed to a change in the spin multiplicity when switching from and on one hand to Fe(H₂O) on the other. Received: 11 November 1997 / Revised: 18 February 1998 / Accepted: 22 April 1998     

A DMRG study of the -symmetric Heisenberg chain

The spin one-half Heisenberg chain with U q [ SU (2)] symmetry is studied via density-matrix renormalization. Ground-state energy and q-symmetric correlation functions are calculated for the non-Hermitian case with integer r. This gives bulk and surface exponents for (para)fermionic correlations in the related Ising and Potts models. The case of real q corresponding to a diffusion problem is treated analytically. Received: 18 February 1998 / Accepted: 17 March 1998     

Evidence for N1/3 dependence of the sticking cross-section of atoms on small and medium-size van der Waals clusters

This paper introduces a simple model describing the cluster growth in supersonic expansions. The predicted terminal mean cluster size is compared to the available data in the case of argon. The agreement between the model and the experimental results requires that the cross-section describing the sticking of an atom on a cluster of size N scales like with in the range 0.34-0.44, well below the predicted by the simplest geometrical scaling argument. We explain this unexpected result in two steps. First, using Monte Carlo simulations, we check that the potential between an atom and a cluster is accurately represented by the Gspann and Vollmar potential, even at finite temperature. Then, using Langevin's approximation, we show that the sticking cross-section scales like N ^1/3 for small to moderate N values and switches to the geometric scaling N ^2/3 for very large N values. The crossover between these two scalings occurs when for argon, but the mean exponent over the size range 1-10⁴ is 0.46. This N scaling of the sticking cross-section should play an important role whenever condensation is important as it modifies the kinetics of the early stages. Received 20 May 1999 and Revised in final form 22 July 1999     

Evolution of charge ordering in manganites

Charge ordering phenomena in the manganites Ca_1-xSm_xMnO₃ have been studied for , using electron diffraction and lattice imaging, completed by magnetic and transport measurements. Three domains can be distinguished, depending on the nature of the structural transitions with temperature. For , the structural transition from a pseudo-tetragonal to a monoclinic form, with decreasing temperature, coincides with the competition between ferromagnetism and antiferromagnetism that is characterized by the temperature T_peak on the M ( T ) curves; short-range charge ordering is observed for manganites. For the second domain, , a structural transition from an orthorhombic to a long-range charge ordered state is clearly observed with decreasing temperature. The corresponding temperature T_CO coincides with the temperature T_peak deduced from magnetic measurements. This long range charge ordering, which appears along a, is either commensurate or incommensurate depending on the x value, with a modulation vector, q being close to x. These modulated superstructures correspond to a stacking of single Mn³⁺ stripes with multiple Mn⁴⁺ stripes along a, either in a commensurate or in an incommensurate manner. The third domain , is characterized by a transition to a charge ordered state with commensurate superstructure at low temperature. The latter can be described as a “partially” charge ordered state in which single “Mn³⁺” stripes alternate with mixed “Mn³⁺/Mn⁴⁺” stripes. Received 17 June 1998     

Reaction and inelastic processes in the collision O () + O ()

A reduced dimensionality model is used to study the reaction OO O ₃ ( X1A1 ) + O( ³ P ) by means of time-dependent and time-independent quantum-mechanical methods. State-selected probabilities and rate constants are obtained for the reactive process as well as for the inelastic collision in which the vibrationally excited oxygen loses one or more quanta. It is found that the experimentally observed jump in depletion rates above a critical value of v could be partially explained by the vibrational relaxation rather than reaction. Reaction only becomes important for relatively high translational energies and therefore the calculated rates are too small at the temperatures of interest. It is concluded, however, that the reaction saddle point region in the potential energy surface plays a crucial role in the enhancement of vibrational relaxation. Received: 3 February 1998 / Revised: 27 March 1998 / Accepted: 15 May 1998     

Electron multiplicity in slow collisions of Ar ions with C

Electron capture by Ar⁸⁺ in collisions with C₆₀ fullerene has been investigated using coincident measurements of the number n of ejected electrons, the mass and charge of multicharged Cr+ ₆₀ recoil ions and their fragments Ci+ m and the final charge state of outgoing projectiles Ar(8-s)+ (). The number of captured electrons r is the sum of the numbers of stabilized and emitted electrons: r = n + s. The ratio n / s decreases by a factor three with s increasing from 1 to 7 showing that the multiply excited states populated by capture of a large number of electrons are rather stable against auto-ionisation. Each kinetic energy spectrum of Ar⁺ and Ar²⁺ projectiles is composed of two peaks which we attribute to collisions “inside” and “outside” the C₆₀ cage. The measured energy shift of the projectile keV is consistent with the corresponding energy loss keV in a carbon foil with an equivalent thickness. Inside collisions are characterized by a strong dissociation of recoil ions into light monocharged fragments and by a high multiplicity of ejected electrons. Received: 25 March 1998 / Received in final form and Accepted: 9 June 1998     

Soft modes and phonon interactions in studied by neutron scattering

The low frequency lattice dynamics and its relationship to the second order paraelectric-to-ferroelectric transition in Sn₂P₂S₆ is studied. The dispersion branches of the acoustic and lowest lying optical phonons in the a^*-c^* plane have been obtained in the ferroelectric phase, for x-polarized phonons. Close to the phase transition a considerable softening is found for the lowest optical mode (P_x), comparable to the behaviour observed in previous Raman investigations. As found previously in Sn₂P₂Se₆, a strong coupling between the TO(P_x) and TA(u_xz) phonons is observed, although, apparently, not strong enough to lead to an incommensurate phase. The soft TO(P_x) mode at the zone center is observed. The temperature dependence of its frequency and damping shows that the transition is not entirely displacive. At low temperatures an unusual apparent negative LO-TO splitting is observed which is shown to arise from the coupling of the x-polarized soft mode to the nearby z-polarized optical phonon. For comparison, the soft TO(P_x) dispersion in the a^*-b^* plane is measured in both the paraelectric and ferroelectric phases. Consistent frequency changes and LO-TO splitting are observed, revealing a significant interaction between the TA(u_yx) and LA(u_xx) acoustics branches and the TO and LO soft optic branches, respectively. In contrast, the nearby y-polarized optic branch shows almost no temperature dependence. Finally, the influence of piezoelectric effects on the limiting acoustic slopes in the ferroelectric phase is discussed. Received: 11 May 1998 / Revised and Accepted: 15 June 1998     

Magnetic properties of the S = 1/2 one-dimensional antiferromagnet MgVO

The magnetic susceptibility and the electron spin resonance in the X-band of the transition metal oxide compound MgVO₃ are reported. We show that this compound, made of weakly coupled infinite chains of VO₅ pyramids, behaves as a S =1/2 one-dimensional Heisenberg antiferromagnet. From the ESR and magnetic experiments we deduce the Néel temperature K, the in-chain coupling constant K and the g-factor values g x = g z =1.972(2), g y =1.946(1) for V⁴⁺ ions in MgVO₃. Received 14 July 1999     

Doublet and quartet states of Li 2 −

Electronic states of the molecular lithium anion are investigated by configuration-interaction calculations. Comparison with the analogously computed potential energy curves for the lowest singlet and triplet states of the neutral Li₂ shows that in addition to the well-known stable ground state X there also exist metastable excited states of Li ₂ ^- . Within the quartet sector, two candidates for such long-lived states are identified and their spectroscopic properties studied. Received 23 March 1999     

Ga-NMR study of the low-energy excitations in

We report the results of ⁶⁹Ga- and ⁷¹Ga-NMR measurements on NdGa₂ at temperatures between 0.1 and and in applied magnetic fields between zero and 74 kOe. NdGa₂ orders antiferromagnetically below and undergoes several metamagnetic transitions in external magnetic fields. In zero applied magnetic field and below the temperature dependence of the spin-lattice relaxation rate T1 ^-1 ( T ) shows a large linear-in-T term, about two orders of magnitude higher than for the reference compound LaGa₂. This strong enhancement confirms the presence of low-energy excitations in the antiferromagnetic phase of NdGa₂ as was previously indicated by specific heat data. Above , T1 ^-1 ( T ) is dominated by an exponential term, which we associate with excitations between the lowest energy levels of the f-electron system. The separation of these energy levels is determined by exchange, crystal-field and Zeeman interactions. Received 3 September 1998 and Received in final form 3 November 1998     

Phase transitions in Sr 0.61 Ba 0.39 Nb 2 O 6 :Ce 3+ : II. Linear birefringence studies of spontaneous and precursor polarization

The linear birefringence (LB) of Sr _0.61-x Ba _0.39 Nb ₂ O ₆ :Ce ³⁺ x (SBN61:Ce) has been measured as a function of temperature within the range of . Large tails have been observed above the ferroelectric phase transition temperatures T _c = 350, 328, 320 and 291 K for the concentrations x = 0, 0.0066, 0.0113 and 0.0207, respectively. Within an Ornstein-Zernike analysis the critical exponents , and are determined. It suggests that pure SBN61 belongs to the 3D Ising universality class. Doping with Ce ³⁺ ions, which seem to act as random fields, enhances the relaxor properties. The critical exponents and of SBN61:Ce shift against those of the three-dimensional random-field Ising model. Received 1 October 1999     

Ground-state landscape of J Ising spin glasses

Large numbers of ground states of two-dimensional Ising spin glasses with periodic boundary conditions in both directions are calculated for sizes up to 40². A combination of a genetic algorithm and Cluster-Exact Approximation is used. For each quenched realization of the bonds up to 40 independent ground states are obtained. For the infinite system a ground-state energy of e =-1.4015(3) is extrapolated. The ground-state landscape is investigated using a finite-size scaling analysis of the distribution of overlaps. The mean-field picture assuming a complex landscape describes the situation better than the droplet-scaling model, where for the infinite system mainly two ground states exist. Strong evidence is found that the ground states are not organized in an ultrametric fashion in contrast to previous results for three-dimensional spin glasses. Received 12 October 1998