Heterogeneous dynamics at the glass transition in van der Waals liquids, in the bulk and in thin films

It has been shown over the last few years that the dynamics close to the glass transition is strongly heterogeneous, both by measuring the diffusion coefficient of tagged particles or by NMR studies. Recent experiments have also demonstrated that the glass transition temperature of thin polymer films can be shifted as compared to the same polymer in the bulk. We propose here first a thermodynamical model for van der Waals liquids, which accounts for experimental results regarding the bulk modulus of polymer melts and the evolution of the density with temperature. This model allows us to describe the density fluctuations in such van der Waals liquids. Then, by considering the thermally induced density fluctuations in the bulk, we propose that the 3D glass transition is controlled by the percolation of small domains of slow dynamics, which allows to explain the heterogeneous dynamics close to T _g. We show then that these domains percolate at a lower temperature in the quasi-2D case of thin suspended polymer films and we calculate the corresponding glass transition temperature reduction, in quantitative agreement with experimental results of Jones and co-workers. In the case of strongly adsorbed films, we show that the strong adsorption amounts to enhance the slow domains percolation. This effect leads to 1) a broadening of the glass transition and 2) an increase of T _g in quantitative agreement with experimental results. For both strongly and weakly adsorbed films, the shift in T _g is given by a power law, the exponent being the inverse of that of the correlation length of 3D percolation. Received 21 March 2000 and Received in final form 4 December 2000     

Formation of adhesive contacts: Spreading versus dewetting

A soft bead (radius R _b) is pressed with a force F against a hydrophobic glass plate through a water drop (“wet” JKR set-up). We observe with a fast camera the growth of the contact zone bridging the rubber bead to the glass. Depending on the approach velocity V, two regimes are observed : i) at large V a liquid film is squeezed at the interface and dewets by nucleation and growth of a dry contact; ii) at low velocities, the bead remains nearly spherical. As it comes into contact, the rubber bead spreads on the glass with a characteristic time (in the range of one millisecond) τ ≈ ηR _b ²/F, where η is the liquid viscosity. The laws of spreading are interpreted by a balance of global mechanical and viscous forces. Received: 22 December 2002 / Accepted: 24 March 2003 / Published online: 29 April 2003 RID="a" ID="a"e-mail: brochard@curie.fr     

String model description of polarisation and angular distributions in ¯pp → ¯ΛΛ at low energies

The observed polarisation of Λ hyperons from the inclusive pA → ΛX reaction at high energies has previously been well described within the Lund string model through polarised sˉs quark pair production in the string breaking hadronisation process. This model is here applied to the exclusive ˉpp → ˉΛΛ reaction at low energies and compared to available data sets down to an incident-beam momentum of 1.835 GeV/c. This required an extension of the diquark scattering model to involve three components: an isotropic part relevant close to the threshold, a spectator part and a forward-scattering part as in pA → ΛX at high energies. The observed angular distributions are then reproduced and, for momentum transfers above | t'| = 0.2 GeV², agreement with the measured polarisation is also obtained. Received: 2 April 2002 / Accepted: 24 July 2002 / Published online: 3 December 2002 RID="a" ID="a"Present address: Department of Neutron Research, Uppsala University, Box 525, S-75120 Uppsala, Sweden; e-mail: Stephan.Pomp@tsl.uu.se. RID="b" ID="b"Present address: ESRF, F-38043 Grenoble, France. Communicated by A. Sch?fer     

Status and prospects of synthesizing superheavy elements

The nuclear shell model predicts that the next doubly magic shell-closure beyond ²⁰⁸Pb is at a proton number between Z = 114 and 126 and at a neutron number N = 184. The outstanding aim of experimental investigations is the exploration of this region of spherical “Superheavy Elements”. This article describes the experiments that were performed at the GSI SHIP. They resulted in an unambiguous identification of elements 107 to 112. They were negative so far in searching for elements 113, 116 and 118 at SHIP; however, positive results were reported from experiments in Dubna on elements 114 and 116 and from experiments in Berkeley on element 118. The measured decay data are compared with theoretical predictions. Some aspects concerning the reaction mechanism and the use of radioactive beams are also presented. Received: 21 March 2002 / Accepted: 16 May 2002 / Published online: 31 October 2002 RID="a" ID="a"e-mail: S.Hofmann@gsi.de     

On the slow dynamics of density fluctuations near the colloidal glass transition

Slow dynamics of density fluctuations near the colloidal glass transition is discussed from a new viewpoint by numerically solving a nonlinear stochastic diffusion equation for the density fluctuations recently proposed by one of the present authors (MT). The effects of spatial heterogeneities on the dynamics of density fluctuations are then investigated in an equilibrium system. The spatial heterogeneities are generated by the nonlinear density fluctuations, while in a nonequilibrium system they are described by a nonlinear deterministic equation for the average number density. The dynamics of equilibrium density fluctuations is thus shown to be quite different from that of nonequilibrium ones, leading to a logarithmic decay followed by less distinct α- and β-relaxation processes. Received 9 March 2002 and Received in final form 19 September 2002     

Mirror decay of 75Sr

The β-decay of ⁷⁵Sr to its mirror nucleus ⁷⁵Rb was studied at the ISOLDE PSB facility at CERN by means of β-delayed γ and proton spectroscopy. The decay Q-value and β-delayed γ intensity were measured for the first time. These results, 10.60±0.22 MeV and 4.5^+1.9 _-0.7%, together with accurate measurements of the β-decay half-life and β-delayed proton branching ratio yielded the Gamow-Teller strength 0.35±0.05 for the mirror transition. Implications of the results on studies of deformation effects and on the path of the rapid proton capture process are discussed. Received: 26 September 2002 / Accepted: 30 October 2002 / Published online: 18 February 2003 RID="a" ID="a"e-mail: jussi.huikari@phys.jyu.lfi Communicated by D. Schwalm     

Single-particle quadrupole electromagnetic transitions in p-shell and sd-shell nuclei

Electron scattering Coulomb form factors for the single-particle quadrupole transitions in p-shell and sd-shell nuclei have been studied. Core polarization effects are included through a microscopic theory that includes excitations from the core orbits up to higher orbits with 2ω excitations. The modified surface delta interaction is adopted as a residual interaction. The results are discussed for the ( 1p _1/2 ^-1↦1p _3/2 ^-1) proton transition in ¹⁵N, ( 1d _5/2↦2s _1/2) neutron transition in ¹⁷O and ( 1d _3/2 ^-1↦2s _1/2 ^-1) proton transition in ³⁹K. The inclusion of core polarization effects modifies the form factors markedly and describes the experimental data very well in both the absolute strength and the momentum transfer dependence. Received: 18 April 2002 / Accepted: 1 July 2002 / Published online: 6 March 2003 RID="a" ID="a"e-mail: baguniv@uruklink.net Communicated by A. Molinari     

Specific heats of the charge density wave compounds o-TaS and (TaSe ) I

Specific heats of the charge-density-wave compounds o-TaS₃ and (TaSe₄)₂I have been measured over the wide temperature interval 10 K-300 K. Both systems exhibit strong non-Debye behavior. Very weak and broad anomalies are observed at the Peierls transition temperatures. For o-TaS₃, the change in the curvature of the specific heat occurs at temperature of 40 K where glass transition has been deduced from dielectric measurements, and an extended scaling analysis suggests that the glass transition is associated with a dynamical cross over in length scales. We briefly discuss the characteristics and physical origins of the anomalies at both the Peierls and glass transitions. Received 5 April 2002 / Received in final form 28 June 2002 Published online 17 September 2002     

NMR study of the dissolution of laser-polarized xenon

NMR of laser-polarized xenon is used to probe the dissolution behaviour of the noble gas in different liquids. The dissolution and self-relaxation rates are extracted via a macroscopic model, and comparison of the decay rate of the xenon magnetization in deuterated and non-deuterated solvent pairs allows the determination of the pure dipole-dipole contribution to relaxation. A transient convective effect, tentatively assigned to the xenon concentration gradient, is observed and characterized by diffusion encoding MRI experiments. The flow of xenon penetrates inside the solvent near the walls of the NMR tube, the longitudinal images showing a “” shape, the transverse ones a “O” shape. This convection effect has implications for delivery conditions of laser-polarized xenon in continuous flow experiments and magnetic resonance imaging. Received 29 April 2002 / Received in final form 26 July 2002 Published online 22 October 2002 RID="a" ID="a"e-mail: hdesvaux@cea.fr RID="b" ID="b"URA CNRS/CEA 331     

Synthesis of superheavy nuclei in the reactions of 244Pu and 248Cm with 48Ca

This paper presents results of the experiments aimed at producing long-lived superheavy elements located near the spherical-shell closures with Z ⩾ 114 and N ⩾ 172 in the ²⁴⁴Pu + ⁴⁸Ca and ²⁴⁸Cm + ⁴⁸Ca reactions. The large measured α-particle energies of the newly observed nuclei, together with the long decay times and spontaneous fission terminating the chains, offer evidence of the decay of nuclei with high atomic numbers. The decay properties of the synthesized nuclei are consistent with the consecutive α-decays originating from the parent nuclides ^{288, 289}114 and ²⁹²116, produced in the 3n and 4n evaporation channels with cross-sections of about a picobarn. The present observations can be considered as experimental evidence of the existence of the “island of stability” of superheavy elements. Received: 21 March 2002 / Accepted: 16 May 2002 / Published online: 31 October 2002 RID="a" ID="a"e-mail: utyonkov@sungns.jinr.ru     

Coulomb breakup of 8B and the flux of 8B neutrinos from the Sun

A kinematically complete measurement was made of the Coulomb dissociation of ⁸B nuclei on a Pb target at 83 MeV/nucleon. The cross-section was measured at low relative energies in order to infer the astrophysical S-factor for the ⁷Be(p,γ)⁸B reaction. A first-order perturbation theory analysis of the reaction dynamics including E1, E2, and M1 transitions was employed to extract the E1 strength relevant to neutrino-producing reactions in the solar interior. By fitting the measured cross-section from E _rel = 130 keV to 400 keV, we find S ₁₇(0) = 17.8^+1.4 _-1.2 eV b. Semiclassical 1st-order perturbation theory and fully quantum-mechanical continuum-discretized coupled-channels analyses yield nearly identical results for the E1 strength relevant to solar-neutrino flux calculations, suggesting that theoretical reaction mechanism uncertainties need not limit the precision of Coulomb-breakup determinations of the ⁷Be(p,γ)⁸B S-factor. A recommended value of S ₁₇(0) based on a weighted average of this and other measurements is presented. This recommendation implies a revised value for the theoretical flux of ⁸B solar neutrinos, which is also given.-1 Received: 21 March 2002 / Accepted: 16 May 2002 / Published online: 31 October 2002 RID="a" ID="a"Present address: Kernfysisch Versneller Instituut, Zernikelaan 25, 9747 AA Groningen, The Netherlands; e-mail: davids@kvi.nl     

Radioactive decay of 217Pa

The radioactive decay of ²¹⁷Pa was investigated by means of α-γ-spectroscopy. Fine structure in the ground-state α-decay was established. Ambiguities in the fine structure of the α-decay of the previously known isomeric state could be clarified by α-γ-coincidence measurements. A previously unknown α-transition of E _α = (8306 ± 5) keV was detected and identified by means of delayed α-α- and α-γ-γ-coincidence measurements. A second isomeric state decaying by α-emission was not observed. The quality of the previously reported data of the α-decay fine structure of ²¹⁷Th was improved. Received: 29 April 2002 / Accepted: 17 June 2002 / Published online: 19 November 2002 RID="a" ID="a"e-mail: f.p.hessberger@gsi.de Communicated by J. ?yst?     

Investigations into the alpha-decay of <Superscript>195</Superscript>At

The low-energy nuclear structure and decay properties of the neutron-deficient isotopes ¹⁹⁵At and ¹⁹¹Bi have been studied. ¹⁹⁵At was produced in the reaction ¹⁴²Nd(⁵⁶Fe,p2n)¹⁹⁵At and ¹⁹¹Bi as the daughter activity of ¹⁹⁵At. The activities were implanted in a position-sensitive silicon detector after being separated from the primary beam by a gas-filled recoil separator. The 1/2⁺ intruder state was determined to be the ground state in ¹⁹⁵At with an alpha-decay energy of E _α = 6953(3) keV and a half-life T _1/2 = 328(20) ms. Another state with an alpha-decay energy E _α = 7075(4) keV and a half-life T _1/2 = 147(5) ms was found to decay to a 148.7(5) keV excited state in ¹⁹¹Bi for which a spin and parity of 7/2^- were deduced. Consequently, the same 7/2^- character was assigned to the initial state at 32(7) keV in ¹⁹⁵At on the basis of unhindered alpha-decay. The 9/2^- state, being the ground state in heavier odd-mass astatine isotopes, was not observed. Received: 16 September 2002 / Accepted: 19 December 2002 / Published online: 25 March 2003 RID="a" ID="a"e-mail: heikki.kettunen@phys.jyu.fi RID="b" ID="b"Present address: Laboratory of Radiochemistry, P.O. Box 55, FIN-00014, University of Helsinki, Finland. RID="c" ID="c"Present address: Radiation and Nuclear Safety Authority, P.O. Box 14, FIN-00881 Helsinki, Finland. Communicated by W. Henning     

Core polarization effects on C4 form factors of sd-shell nuclei

Coulomb form factors of C4 transitions in even-even N = Z sd-shell nuclei ( ²⁰Ne, ²⁴Mg, ²⁸Si and ³²S) are discussed taking into account higher-energy configurations outside the sd-shell model space which are called core polarization effects. Higher configurations are taken into account through a microscopic theory, which allows particle-hole excitations from the 1s and 1p shells core orbits and also from the 2s1d-shell orbits to the higher allowed orbits with excitations up to 4 ω. The effect of core polarization is found essential in both the transition strengths and momentum transfer dependence of form factors, and gives a remarkably good agreement with the measured data with no adjustable parameters. The calculations are based on the Wildenthal interaction for the sd-shell model space and on the modified surface delta interaction (MSDI) for the core polarization effects. Received: 24 January 2002 / Accepted: 29 July 2002 / Published online: 6 March 2003 RID="a" ID="a"e-mail: baguniv@uruklink.net Communicated by P. Schuck     

Isomeric states in proton-unbound 187, 189Bi isotopes

Prompt and delayed gamma-ray spectroscopy of very neutron-deficient bismuth isotopes ^{187, 189}Bi has been performed using the Recoil Decay Tagging (RTD) method. The isomeric i _13/2 states have been identified and their lifetimes have been measured. The systematics of these long-lived M2 isomers has been extended to the proton-unbound isotopes. The general behaviour of single-proton states is discussed within the systematics and interpreted within the shell-model framework. Received: 2 May 2002 / Accepted: 3 June 2002 / Published online: 19 November 2002 RID="a" ID="a"e-mail: wkorten@cea.fr RID="b" ID="b"Present address: GANIL, Caen, France. RID="c" ID="c"Present address: Radiation and Nuclear Safety Authority, P.O. Box 14, FIN-00881 Helsinki. Communicated by D. Schwalm     

Rotational alignment of the h11/2 band in 157Dy

High-spin states of ¹⁵⁷Dy were investigated using in-beam γ-ray spectroscopy techniques with a ¹⁵⁰Nd(¹²C, 5n) reaction. Three rotational bands with the h _9/2, i _13/2 and h _11/2 configurations were observed up to (43/2^-), 53/2⁺ and 45/2^-, respectively. Interband M1 transitions in the h _11/2 (high-Ω) band were also measured up to the highest-spin state. The high-spin states were well reproduced by calculations using the tilted-axis-cranking model (TAC). The B(M1)/B(E2) ratio, Routhian and the tilted angle of the angular-momentum vector are found to be in good agreement with the result of the TAC calculation. Received: 22 August 2002 / Accepted: 26 September 2002 / Published online: 19 November 2002 RID="a" ID="a"e-mail: hayakawa@jball4.tokai.jaeri.go.jp Communicated by W. Henning     

Investigation of α-nucleus interaction in the 27Al (α,α)27Al scattering and 27Al (α, d )29Si reaction

Full finite-range macroscopic calculations in the distorted-wave Born approximation have been performed using the molecular and Michel α-nucleus potentials to analyze the angular distributions of cross-sections of the ²⁷Al(α, d)²⁹Si reaction, at 26.5 and 27.2 MeV incident energies, leading to seven transitions up to the excitation energy E _X = 4.08 MeV of the final nucleus. The parameters of the two types of the α-nucleus potentials are determined from the elastic-scattering data. Both the molecular and Michel potentials, without any adjustment to the parameters needed to fit the elastic-scattering data, are able in most cases to reproduce, simultaneously, the absolute cross-sections particularly at large angles, where the previous calculations failed to reproduce by orders of magnitude, and the gross pattern of angular distributions of the reaction. The deuteron-cluster spectroscopic factors for most of the seven transitions, deduced using the two α-²⁷Al potentials, differ from those obtained in earlier works. The spectroscopic factor for the ground-state transition, deduced in the present work for the 25.8 MeV data, agrees well with the shell model prediction. Received: 15 July 2002 / Accepted: 8 August 2002 / Published online: 10 December 2002 RID="a" ID="a"e-mail: akbasak2001@Yahoo.com Communicated by G. Orlandini     

Studies with one- and two-proton drip line nuclei

In recent experiments at GANIL, we studied nuclei at the one- and two-proton drip line. The production rates allowed to search for direct 2p emission in the drip line nuclei ⁴²Cr, ⁴⁵Fe, and ⁴⁹Ni. No evidence for this decay mode was found in ⁴²Cr and ⁴⁹Ni, whereas the situation stays unclear for ⁴⁵Fe due to the limited statistics. In the medium-mass region ( A = 50-70), the half-life was measured for all proton-rich nuclei in the range T _z = 0 to T _z = - 1 between Z = 27 and Z = 36. First half-lives were determined for ⁶⁰Ga, ⁶²Ge, ⁶⁴As and ⁶⁶Se. Finally, β-decay studies of the 0⁺ → 0⁺ decay of ⁶²Ga have been performed at IGISOL in Jyv?skyl?. Non-analog transitions have been observed and are compared to theoretical predictions. Received: 21 March 2002 / Accepted: 16 May 2002 / Published online: 31 October 2002 RID="a" ID="a"e-mail: blank@cenbg.in2p3.fr     

Heavy-element chemistry --Status and perspectives

In the past ten years, nuclear chemists have made considerable progress in developing fast on-line separation techniques, which allowed to chemically characterize the first four transactinide elements Rf (rutherfordium, Z = 104), Db (dubnium, Z = 105), Sg (seaborgium, Z = 106), and recently also Bh (bohrium, Z = 107). In all cases the isolated nuclides were unambiguously identified by observing genetically linked decay chains. Nuclides with production cross-sections of less than 100 pb and half-lives as short as a few seconds have been chemically isolated. Thus, chemists have discovered or significantly contributed to the characterization of the nuclear-decay properties of a number of transactinide nuclei. New techniques with greatly improved overall efficiencies should allow chemists to extend their studies to even heavier elements such as Hs (hassium, Z = 108) and to the recently discovered superheavy elements with Z = 112 and 114, which can be produced only with picobarn cross-sections. Received: 21 March 2002 / Accepted: 16 May 2002 / Published online: 31 October 2002 RID="a" ID="a"e-mail: andreas.tuerler@psi.ch