Synthesis and microstructure of metal oxide thin films containing metal nanoparticles by liquid phase deposition (LPD) method

Au nanoparticles dispersed SiO₂-TiO₂ composite films have been prepared by a novel wet process, Liquid Phase Deposition (LPD) method. The composite films were characterized by XRD, XPS, TEM, ICP, SEM and UV-VIS absorption spectroscopy. The results showed that the SiO₂-TiO₂ composite films containing Au^III and Au^I ionic species were co-deposited from a mixed solution of ammonium silicofluoride, ammonium hexafluorotitanate, boric acid and tetrachloroauric acid. The heat treatment induced the reduction of Au ions and formation of Au nanoparticles in the film. TEM observation revealed that the Au nanoparticles with 5-10 nm in diameter were found to be dispersed uniformly in the SiO₂-TiO₂ matrix. The optical absorption band due to the surface plasmon resonance of dispersed Au particles were observed at the wavelength of 550 nm and shifted toward longer wavelength with increasing heat treatment temperature. Received 28 November 2000     

Evidence for a solid phase of dodecahedral C 20

Evidence is presented for the formation of a solid phase based on the smallest fullerene, C₂₀, in thin diamond-like carbon films deposited by ultraviolet laser ablation from diamond onto nickel substrates at room temperature in the presence of 10^-4 torr of cyclohexane or benzene. Laser desorption mass spectrometry from the films shows the presence of C₂₀, C₂₁ and C₂₂ species, while micro-Raman spectroscopy and electron diffraction from selected particles together with first principle density-functional calculations, indicate a cubic solid with dodecahedral C₂₀ cages as building blocks. Unlike solid C₆₀ and fully protonated C₂₀, which are bound by van der Waals forces, the proposed structure is stabilized by linking of the C₂₀ dodecahedra with bridging carbon atoms at interstitial tetrahedral sites to form a face-centered-cubic lattice with 22 carbon atoms per unit cell. Received 10 October 2002 / Received in final form 24 December 2002 Published online 6 March 2003 RID="a" ID="a"e-mail: zafar.iqbal@njit.edu     

Electrical resistivity of the Ti\mathsf{_4}O\mathsf{_7} Magneli phase under high pressure

The electronic and positronic properties of the pentanary semiconductor alloys Ga_xIn_1-xP_ySb_zAs_1-y-z lattice matched to GaSb have been studied. The electron wave function is calculated semiempirically using the pseudopotential band model under the virtual crystal approximation. The positron wave function is evaluated under the point core approximation for the ionic potential. Electronic and positronic quantities namely, electronic structure and band gaps, positron band structure, effective mass and affinity, and electron-positron momentum densities have been predicted and their dependence on the phosphorus composition has been discussed. Received 30 August 2002 / Received in final form 12 February 2003 Published online 24 April 2003     

Size and concentration effects in the optical properties of alloyed ( Au x Ag 1 - x ) n and core-shell ( Ni x Ag 1 - x ) n embedded clusters

Optical properties of mixed clusters (Au_xAg _{1 - x} ) _n and (Ni_xAg _{1 - x} ) _n , produced by laser vaporization and embedded in an alumina matrix, are reported. The size effects are investigated for different concentrations (x = 0.25, 0.5 and 0.75) in the diameter range 2-4 nm. For alloyed clusters (Au_xAg _{1 - x} ) _n of a given size an almost linear evolution of the surface plasmon frequency ω _s with the concentration is observed (between those of pure gold and pure silver clusters). Moreover the blue-shift and the damping of the resonance with decreasing size is all the more important as the gold concentration in the particles increases. Such results are in agreement with theoretical calculations carried out in the frame of the time-dependent local-density-approximation (TDLDA) including an inner skin of ineffective screening and the porosity of the matrix. The optical response of (Ni_xAg _{1 - x} ) _n clusters exhibits a surface plasmon resonance in the same spectral range as the one observed for pure silver clusters, but considerably damped and broadened. For a given mean cluster size 3.0 nm, a blue-shift of the resonance is observed when increasing the nickel concentration (between x = 0.25 and x = 0.75). The results are in good qualitative agreement with classical predictions in the dipolar approximation, assuming a core-shell geometry. Received 21 November 2000     

Exchange coupling in ultrathin epitaxial yttrium iron garnet films

Magnetic exchange coupling has been observed for ultrathin films of yttrium iron garnet (Y₃Fe₅O₁₂ or YIG). Single-crystalline YIG films were prepared on yttrium aluminium garnet (Y₃Al₅O₁₂ or YAG) substrates by pulsed laser deposition. (111) and (110) oriented substrates were used. Film thicknesses were varied from 180 ? to 4600 ?. Epitaxial growth of YIG on YAG was obtained in spite of the lattice mismatch of 3%. Magnetic hysteresis loops recorded for ultrathin YIG films have a “bee-waist” shape and show a coupling between two different magnetic phases. The first phase is magnetically soft YIG. A composition study by secondary ion mass spectroscopy shows the second phase to be Y₃Fe_5-xAl_xO₁₂ due to the interdiffusion of Fe and Al at the film/substrate interface. This compound is known to be magnetically harder and to have weaker magnetization than YIG. The coupling of the two phases leads to a hysteresis loop displacement at low temperatures. This displacement varies differently with film thickness for two substrate orientations. Assuming an interfacial coupling, the maximal interaction energy is estimated to be about 0.17 erg/cm² at 5 K for (111) oriented sample. Received 3 June 2002 / Received in final form 7 October 2002 Published online 27 January 2003 RID="a" ID="a"Presently at LPM, Université H. Poincaré, BP 239, 54506 Vandœuvre-lès-Nancy e-mail: popova@lpm.u-nancy.fr     

Micromagnetic structure in multilayer films with moderate perpendicular anisotropy

Micromagnetic simulations have been performed in order to obtain deeper insight into the domain structures within multilayer films, as they are expected to differ from those of single films. These 2D calculations have been done in the case of multilayers exhibiting a moderate perpendicular anisotropy, with no indirect exchange coupling between the magnetic layers, where a “weak stripe" domain structure develops. First, these results are compared quantitatively to the very detailed experimental data available in the literature on the (Co/Au)_N system. More generally, the nucleation of a stripe pattern in multilayers is discussed as a function of the magnetic parameters and the number of magnetic layers in the stack. Compared to a single film, two main differences appear in the equilibrium domain period and the magnetization profiles. The physical origin of these effects is discussed. Received 12 January 2001 and Received in final form 15 May 2001     

Effects of the indium doping on structural and optical properties of CdSe thin films deposited by laser ablation technique

Thin films of n-type CdSe have been grown on a quartz substrate by laser ablating a target obtained by mixing CdSe and metallic In powders. The effects of different doping concentration of In have been investigated. X-ray diffraction spectra show that at low In density only the CdSe lattice is present in the deposited film, whereas CdIn₂Se₄ and InSe compounds are deposited at higher In concentration. Band gap narrowing and band tails are observed in the absorption spectra when the In concentration increases. Photoluminescence spectra show band-band recombinations from 10 K to room temperature. Received 27 September 2002 Published online 11 April 2003 RID="a" ID="a"e-mail: giuseppe.perna@ba.infn.it     

Maximally aligned states in 99Ag

Excited states of ⁹⁹Ag were populated via the ⁵⁰Cr + ⁵⁸Ni (261 MeV) reaction using the NORDBALL detector array equipped with charged-particle and neutron detector systems for reaction channel separation. On the basis of the measured γγ-coincidence relations and angular distribution ratios a significantly extended level scheme has been constructed up to E _x ∼ 7.8 MeV and I = 35/2. The experimental results were described within the framework of the shell model. Candidates for states fully aligned in the πg _9/2 ^-3ν(d _5/2, g _7/2)² valence configuration space were found at 4109 and 6265 keV. Received: 18 June 2002 / Accepted: 11 October 2002 / Published online: 4 February 2003 RID="a" ID="a"e-mail: sohler@atomki.hu Communicated by J. ?yst?     

Band gaps and charge distribution in quasi-binary (GaSb) (InAs) crystals

Pseudopotential investigation of energy band gaps and charge distribution in quasi-binary (GaSb)_1-x(InAs)_x crystals has been reported. To the best of our knowledge, there had been no reported theoretical work on these materials. In agreement with experiment, the quasi-binary crystals of interest showed a significant narrowing of the optical band gap compared to the conventional Ga_xIn_1-xAs_ySb_1-y quaternary alloys (with x = 1 - y). Moreover, the absorption at the optical gaps indicated that (GaSb)_1-x(InAs)_x is a direct Γ to Γ band-gap semiconductor within a whole range of the x composition. The information derived from the present study predicts that the band gaps cross very important technological spectral regions and could be useful for thermophotovoltaic applications. Received 30 August 2002 Published online 1st April 2003 RID="a" ID="a"Present address: Physics Department, University of M'sila, 28000 M'sila, Algeria e-mail: N_Bouarissa@yahoo.fr     

Structural stability and structural imitation of (M = Mn,Mo, Nb,Ti, V,Al, Cr,Ni and Si)

The structural stability of La₂Co_17-xM_x (M = Mn, Mo, Nb, Ti, V, Al, Cr, Ni and Si) based on the interatomic potential has been studied. The calculated site preference of the third element M is found to be the 6c site, which is in agreement with the experiments. In the calculations, if the crystal cohesive energy of La₂Co₁₆Mn is taken as the highest one in the crystallization of La₂Co_17-xM_x, the lowest content x of the third element M (M = Mn, Mo, Nb, Ti and V) required to stabilize La₂Co_17-xM_x, is near that found in the experiments. The differences of the cell parameters between the calculated and the experimental values are less than 0.4%. The differences of the atomic parameters for Co (or M) between the calculated and the experimental values are about or even smaller than 1%, and that of La is about 3%. Because the energies of La(Co_1-xAl_x)₁₃ are lower than those of La₂(Co_1-xAl_x)₁₇, La₂(Co_1-xAl_x)₁₇ could not be formed in the experiments. In the calculations, with either a range of deformation of the structure or the reconstruction of the initial structure La₂Co₁₇ from LaCo₅, the same results including the cohesive energy curves and the crystallographic parameters can be retrieved after the action of the interatomic potentials. Received 1st November 2002 / Received in final form 17 February 2003 Published online 23 May 2003 RID="a" ID="a"e-mail: hchang@aphy.iphy.ac.cn     

First observation of the ν9/2[404] orbital in the A ∼ 100 mass region

A new band, populated by the spontaneous fission of ²⁴⁸Cm and studied by means of prompt γ-ray spectroscopy using the EUROGAM2 array, was observed in ⁹⁹Zr. The 1038.8 keV band head with a half-life T _1/2 = 54(10) ns is interpreted as a K-isomer, corresponding to the 9/2[404] neutron-hole excitation. It is the first observation of this orbital in the mass A ∼ 100 region. The quadrupole moment, Q ₀ = 3.9(3) eb deduced for the new band indicates a large deformation of β = 0.41, which is produced by a specific shape-coexistence mechanism, known in other regions and now found in the A ∼ 100 nuclei. Received: 11 September 2002 / Accepted: 31 October 2002 / Published online: 17 January 2003 RID="a" ID="a"e-mail: urban@fuw.edu.pl Communicated by D. Schwalm     

Competition in the carrier capture between InGaAs/AlGaAs quantum dots and deep point defects

The presence of an extrinsic photoluminescence (PL) band peaked at 1.356 eV at low temperature is observed, on a large number of self-assembled InAs and In_0.5Ga_0.5As quantum dot (QD) structures, when exciting just below the GaAs absorption edge. A detailed optical characterization allows us to attribute the 1.356 eV PL band to the radiative transition between the conduction band and the doubly ionized Cu _Ga acceptor in GaAs. A striking common feature is observed in all investigated samples, namely a resonant quenching of the QD-PL when exciting on the excited level of this deep defect. Moreover, the photoluminescence excitation (PLE) spectrum of the 1.356 eV emission turns out to be almost specular to the QD PLE. This correlation between the PL efficiency of the QDs and the Cu centers evidences a competition in the carrier capture arising from a resonant coupling between the excited level of the defect and the electronic states of the wetting layer on which the QDs nucleate. The estimated Cu concentration is compatible with a contamination during the epitaxial growth. Received 13 November 2001 / Received in final form 28 May 2002 Published online 19 July 2002     

Quantum topological excitations: from the sawtooth lattice to the Heisenberg chain

From the recently determined structure of the delafossite YCuO_2.5, we argue that the Cu-O network has nearly independent Δ chains but with different interactions between the s = 1/2 spins. Motivated by this observation, we study the Δ chain for different ratios of the base-base and base-vertex interactions, J _bb/J _bv. By exact diagonalization and extrapolation, we show that the elementary excitation spectrum is the same for total spins S _tot = 0 and 1, but not for S _tot = 2, and has a gap only in the interval 0.4874(1) ⩽ J _bb/J _bv ⩽ 1.53(1). The gap, known to be dispersionless for J _bb = J _bv, is found to acquire increasing k-dependence as J _bb/J _bv moves away from unity. Received 29 October 2002 / Received in final form 14 January 2003 Published online 6 March 2003 RID="a" ID="a"e-mail: sblundell@cea.fr RID="b" ID="b"e-mail: nunezreg@lps.u-psud.fr     

Surface Plasmon Resonance and Field Enhancement of Au/Ag Alloyed Hollow Nanoshells

We investigate the nanostructure, surface plasmon resonance （SPR） absorption and nonlinear enhancement of Au/Ag alloyed hollow nanoshells prepared by the replacement reaction of Ag nanoparticles in a HAuCI4 aqueous solution. As the volume of HAuCl4 increases from OmL to 0.S mL, the SPR band of the Au/Ag alloyed nanoshells is tuned from 430nm to 780nm, and the third-order nonlinear optical susceptibility is enhanced nearly by an order of magnitude, which indicates a large enhancement of local field in the Au/Ag alloyed hollow nanoshells with hole defects.     

Magnetic properties of the cyclic spincluster Fe6:bicine

The magnetic properties of the cyclic compound [Fe₆(bicine)₆] LiClO₄ ^. 2MeOH are reported. The cluster Fe₆(bicine)₆ forms an antiferromagnetically coupled ring structure of Fe ^III ions. The magnetic susceptibility is measured between 2 and 300 K and yields the exchange coupling of J/k _B = - 27.5±0.5 K. The field dependence of the magnetic moment is studied at 3 and 6 K in magnetic fields up to 5 T. The zero-field splitting of the first excited spin states with S = 2 and 3 are determined by ESR at 94 GHz. The intra-molecular interactions of the Fe ^III ions are analyzed and the on-site anisotropy of the Fe ^III due to the ligand-configuration is determined to d /k _B = - 0.633±0.008K. Received 28 October 2002 / Received in final form 22 February 2003 Published online 20 June 2003 RID="a" ID="a"e-mail: bernd@piobelix.physik.uni-karlsruhe.de     

Vortex matter in lead nanowires

Theoretical and experimental magnetizations of lead nanowire arrays well below the superconducting transition temperature T_c are described. The magnetic response of the array was investigated with a SQUID magnetometer. Hysteretic behaviour and phase transitions have been observed in sweeping up and down the external magnetic field at different temperatures. The Meissner and Abrikosov states were also experimentally observed in this apparently type-I superconductor. This fact brings to the fore the non-trivial behaviour of the critical boundary κ _c ( = 1/ in bulk materials) between type-I and type-II phase transitions at mesoscopic scales. The time-independent Ginzburg-Landau equations particularized to cylindrically symmetric configurations enable one to explain and reproduce the experimental magnetization curves within 10% of error. Received 16 January 2003 / Received in final form 27 March 2003 Published online 23 May 2003 RID="a" ID="a"e-mail: stenuit@fynu.ucl.ac.be     

Electronic localization in an extreme 1-D conductor: the organic salt (TTDM-TTF) [Au(mnt) ]

This article reports the investigation of a new low-dimensional organic salt, (TTDM-TTF)₂ [Au(mnt)₂], by single crystal X-ray diffraction, static magnetic susceptibility, EPR, thermopower, electrical resistivity measurements under pressure up to 25 kbar and band structure calculations. The crystal structure consists in a dimerized head to tail stacking of TTDM-TTF molecules separated by layers of orthogonal Au(mnt)₂ anions. The absence of overlap between neighboring chains coming from this particular crystal structure leads to an extreme one-dimensionality (1-D) for which the carriers of the half-filled conduction band become strongly localized in a Mott-Hubbard insulating state. This material is the first 1-D conductor in which the Mott-Hubbard insulating character cannot be suppressed under pressure. Received 15 April 2002 / Received in final form 17 June 2002 Published online 17 September 2002     

Cyclotron resonance of polarons in ternary mixed crystals

Rayleigh-Schr?dinger perturbation theory and an improved Wigner-Brillouin perturbation theory has been used to study the cyclotron resonance of the polarons in ternary mixed crystals in the zero-temperature limit. The interaction between an electron and two branches of longitudinal optical phonon modes is taken into account in the framework of the random-element-isodisplacement model. The numerical results for several ternary mixed crystals show that the polaronic cyclotron energy and mass split successively twice related to the higher and lower branches of longitudinal optical phonon modes of ternary mixed crystals. A non-linear dependence of the polaronic cyclotron energy and mass on the composition x is found. Received 19 March 2002 / Received in final form 21 March 2003 Published online 20 June 2003 RID="a" ID="a"e-mail: xxliang@imu.edu.cn     

Giant entropy change at the co-occurrence of structural and magnetic transitions in the Ni Mn Ga Heusler alloy

We have studied the isothermal entropy change around a first-order structural transformation and in correspondence to the second-order Curie transition in the ferromagnetic Heusler alloy Ni_2.15Mn_0.85Ga. The results have been compared with those obtained for the composition Ni_2.19Mn_0.81Ga, in which the martensitic structural transformation and the magnetic transition occur simultaneously. With a magnetic field span from 0 to 1.6 T, the magnetic entropy change reaches the value of 20 J/kg K when transitions are co-occurring, while 5 J/kg K is found when the only structural transition occurs. Received 27 September 2002 / Received in final form 17 February 2003 Published online 11 April 2003 RID="a" ID="a"e-mail: solzi@fis.unipr.it     

Dynamic fracture model for acoustic emission

We consider the spin-glass phase of the Sherrington-Kirkpatrick model in the presence of a magnetic field. The series expansion of the Parisi function q(x) is computed at high orders in powers of τ = T _c - T and H. We find that none of the Parisi-Toulouse scaling hypotheses on the q(x) behavior strictly holds, although some of them are violated only at high orders. The series is resummed yielding results in the whole spin-glass phase which are compared with those from a numerical evaluation of the q(x). At the high order considered, the transition turns out to be third order on the Almeida-Thouless line, a result which is confirmed rigorously computing the expansion of the solution near the line at finite τ. The transition becomes smoother for infinitesimally small field while it is third order at strictly zero field. Received 3 March 2003 Published online 4 June 2003 RID="a" ID="a"e-mail: andrea.crisanti@phys.uniroma1.it RID="b" ID="b"e-mail: tommaso.rizzo@phys.uniroma1.it RID="c" ID="c"e-mail: temtam@helios.elte.hu