C 78 IPR fullerenes: Computed B3LYP/6-31G*//HF/3-21G temperature-dependent relative concentrations

The five isolated-pentagon-rule (IPR) satisfying isomers of C₇₈, labeled 1-5, or according to symmetry as D₃, C_2v, C' _2v , D_3h, and D' _3h , are computed. The cage geometries are optimized at the ab initio HF level with the standard 3-21G basis set (HF/3-21G). The separation energetics is then computed using the B3LYP density-functional treatment in the standard 6-31G* basis set (B3LYP/6-31G*//HF/3-21G). Harmonic vibrational frequencies are calculated by the SAM1 semiempirical method. The computed energies, structural and vibrational data are employed in the construction of isomeric partition functions and evaluation of the relative Gibbs free energies. The results are converted into relative concentrations for a wide temperature interval. The C' _2v structure is the most populated throughout while the D_3h species is negligible at all temperatures. The agreement between theory and experiment is reasonable, though some aspects are still to be clarified. Received 28 November 2000     

Tautomery and H-bonding characteristics of 2-aminopurine: a combined experimental and theoretical study

An experimental and theoretical RHF, MP2 and DFT/6-31++G^** study is described of the matrix FT-IR spectra of monomer 2-aminopurine and H-bonded complexes of 2-aminopurine with water. 2-aminopurine occurs in Ar predominantly as the amino-N9H tautomer, but small amounts of the amino-N7H tautomer are also present. An approximate K_T value for this tautomeric equilibrium is found to be 0.016 (RHF) and 0.015 (DFT) using the infrared intensity measurement. Four H-bonded complexes of the abundant amino-N9H form with water are detected in the experimental FT-IR spectrum by their characteristic predicted absorptions, i.e. the three closed complexes N3 ^... H-O ^... H-N9, N1 ^... H-O ^... H-NH, N3 ^... H-O ^... H-NH and the open complex N7 ^... H-OH. From the experimental results, the proton affinity of the N7 atom in 2-aminopurine can be estimated. The dependence of the H-bond strength on the H-bond linearity is demonstrated by a correlation between the N ^... H distance and the N ^... H-O angle in closed N ^... H-O ^... H-N complexes. Received 10 December 2001 Published online 13 September 2002     

Charge radius change in the heavy tin isotopes until A = 132 from laser spectroscopy

Laser spectroscopy measurements have been carried out on the very neutron-rich tin isotopes with the COMPLIS experimental setup. Using the 5s ²5p ²³ P ₀ → 5s ²5p6s ³ P ₁ optical transition, hyperfine spectra of ^126-132Sn and ^{125m, 127m, 129m-131m}Sn where recorded for the first time. The variation of the mean-square charge radius ( δ〈r ²〉) between these nuclei and nuclear moments of the isomers and the odd isotopes were thus measured. An odd-even staggering which inverts at A = 130 is clearly observed. This indicates a small appearance of a plateau on the δ〈r ²〉 which has to be confirmed by measuring the isotope shift beyond A = 132. Received: 21 March 2002 / Accepted: 16 May 2002 / Published online: 31 October 2002 RID="a" ID="a"e-mail: leblanc@ipno.in2p3.fr     

Shape co-existence and structural evolution of the yrast band in 157Yb

The high-spin states of ¹⁵⁷Yb have been studied via the ¹⁴⁴Sm(¹⁶O, 3n) reaction at ¹⁶O energy of 90 MeV using techniques of in-beam γ-ray spectroscopy. Measurement of γ-γ-t coincidences was performed with 11 BGO(AC)HPGe detectors. Based on the measured results of γ-γ coincidences, γ-ray anisotropies and DCO ratios, the level scheme for ¹⁵⁷Yb was established. The shape co-existence and structural evolution of the νi _13/2 band with increasing angular momentum in ¹⁵⁷Yb have been discussed. The systematics of the νi _13/2 bands in the N = 87 odd-A isotones have been compared. Received: 7 January 2002 / Accepted: 10 April 2002     

Selective laser ionization of N≥82 indium isotopes: The new r-process nuclide 135In

Production yields and β-decay half-lives (T _1/2) of very neutron-rich indium isotopes were determined at CERN/ISOLDE using isobaric selectivity of a resonance-ionization laser ion-source. Beta-delayed neutron (βdn) multiscaling measurements have yielded improved T _1/2 for 206(6) ms ¹³²In, 165(3) ms ¹³³In and 141(5) ms ¹³⁴In. With 92(10) ms ¹³⁵In, a new r-process nuclide has been identified which acts as an important “waiting point” in the In isotopic chain for neutron densities in the range n _n≃ 10²⁴-10²⁶ n/cm³, where the r-matter flow has already passed the A≃ 130 abundance peak region. Received: 17 January 2002 / Accepted: 30 January 2002     

Observation of signature inversion in odd-odd 178Ir

High spin states in ¹⁷⁸Ir have been studied via the ¹⁵²Sm(³¹P, 5nγ)¹⁷⁸Ir reaction through excitation functions, X-γ and γ-γ-t coincidence measurements. According to the band structure characteristics and the measured intraband B(M1)/B(E2) ratios, two rotational bands are identified and assigned to be associated with the πh _9/2⊗νi _13/2 and πh _11/2⊗νi _13/2 configurations, respectively. Both bands show the signature inversion feature. Received: 23 March 2000 / Accepted: 31 July 2000     

A lower bound for the volume-averaged mean-square magnetostatic stray field

Based on a micromagnetics model, we develop a method through which quantitative information on the volume-averaged mean-square magnetostatic stray field 〈|H ^b _d|²〉 _v due to non-zero divergences of the magnetization M within the bulk of a ferromagnetic body can be obtained by analysis of magnetic-field-dependent small-angle neutron scattering data. In the limit of high applied magnetic field H _a, when the direction of M deviates only sligthly from H _a, we have estimated a lower bound for 〈|H ^b _d|²〉 _v as a function of the external field, and we have applied the method to bulk samples of nanocrystalline electrodeposited Ni and Co and coarse-grained polycrystalline cold-worked Ni. The root-mean-square magnetostatic stray field, which is inherent to a particular magnetic microstructure, shows a pronounced field dependence, with values ranging from about 5 to 50mT. Even at applied fields as large as 1.7T, the quantity μ〈|H ^b _d|²〉^1/2 _v of nanocrystalline Co is still 24mT, which suggests that contributions to the total magnetostatic field originating from the bulk are significant in nanocrystalline ferromagnets; therefore, 〈|H ^b _d|²〉 _v cannot be ignored in the interpretation of e.g. measurements of magnetization or spin-wave resonance. A comparison of 〈|H ^b _d|²〉 _v with the volume-averaged mean-square anisotropy field reveals that both quantities are of comparable magnitude. Received 25 April 2002 Published online 31 October 2002 RID="a" ID="a"e-mail: anmi@nano.uni.saarland.de     

Conformational analysis: Part 42. A modelling and LIS/NMR investigation of the conformations of some aromatic SO compounds

A refined Lanthanide‐Induced‐Shift Analysis (LISA), in which both the paramagnetic and the diamagnetic lanthanide induced chemical shifts are normalised separately, is used with molecular mechanics (MMFF94) and ab initio (RHF/6‐31G, RHF/6‐311G** and B3LYP/6‐311G**) calculations to investigate the conformations of methyl para‐tolyl sulphoxide 1 , sulphone 2 and sulphonate 3 and the conformational equilibria of methyl 2,4‐dimethylphenyl sulphoxide 4 and sulphone 5 . In 1 acceptable agreement factors (AFs) in the LISA analysis were only obtained when the SO/phenyl dihedral angle was increased from that (10–15°) of the computed geometries to 30–40°. The calculated geometries for 2 had the methyl group orthogonal to the phenyl ring and gave good AF in the LISA analysis. In both compounds, the AF were in the order MMFF94 ≤ B3LYP < RHF with the larger basis sets giving better agreement than the limiting 6‐31G* function. In 3 all the geometries again had the methoxy group orthogonal to the phenyl ring but, while the ab initio geometries still gave good AFs, the MMFF94 structure gave an AF which was only just acceptable. The unsymmetrical compounds 4 and 5 display conformational equilibria. In 4 two energy minima were found, both with the SMe group orthogonal to the phenyl ring, with the SO oxygen cis or trans to the 2‐methyl group. The energy difference (cis–trans) was calculated as 1.6 kcal/mol (MMFF94), 2.7 (6‐31G*), 1.9 (6‐311G**) but ?0.11 (DFT). The LISA analyses on the separate conformers gave poor agreement (ca. 3%) for the trans conformer but increasing the SO/Ph dihedral angle again gave an acceptable value (ca. 1.4%). Inclusion of even small amounts of the cis conformer in the LIS analysis gave poorer results. Thus, the LISA analysis confirms the MM and RHF prediction that the trans conformer is more stable and suggests that the conformer energy difference in solution is equal to or greater than the largest calculated value of 2.7 kcal/mol. In 5 all the calculations gave two mirror image conformations with the SMe orthogonal to the phenyl ring. The LISA analysis in this case is complicated by the fact that in the stable conformer the complexing oxygen atoms are not equivalent. This was resolved by considering both coordination sites in one Z‐matrix and varying the % coordination on each oxygen atom. This gave an acceptable AF of ca. 1.0% for all the geometries with ca. 2:1 coordination on the oxygen atoms trans and cis to the C2‐methyl. The difference in the geometries and conformer energies found by LISA for these molecules in solution compared to the theoretical values may be due to interactions with the chloroform solvent for these polar compounds. Copyright © 2010 John Wiley & Sons, Ltd.     

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     

Photoexcitation of rare-gas neon and argon clusters doped with <Emphasis Type="Bold">H</Emphasis><Subscript><Emphasis Type="Bold">2</Emphasis></Subscript><Emphasis Type="Bold">O</Emphasis>

We have studied the fluorescence of electronically excited OH^*, H^* and H₂O^+* dissociation fragments after VUV excitation ( h ν≥11.6 eV) of rare-gas clusters (Rg = Ne, Ar) doped with H₂O molecules. In contrast to a free molecule, where Balmer H-series dominate the UV-visible spectra, only the OH ^* ( A ² Σ ⁺ ↦ X ² Π) emission band is observed in neon clusters. No emission of excited water ions has been observed. We find that while higher excitation energies (Ne vs. Ar) induce higher vibrational excitation of the OH^* ( A ) fragment, the rotational temperature is lower. This effect is attributed to the difference in the geometric position of the H₂O molecule on the surface or inside the Rg-cluster. The rotational relaxation in neon clusters is rapid while the vibrational relaxation is slow because of the coupling with the low energy matrix phonons. Received 7 March 2002 / Received in final form 27 May 2002 Published online 19 July 2002     

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     

Hole doping by Li substitution and antiferromagnetism in YBa Cu O studied by neutron powder diffraction measurements

The magnetic structure of tetragonal insulating YBa₂Cu_3-xLi_xO_y has been studied as a function of x and y. The Néel temperature and the mean ordered magnetic moment on the Cu2 sites were determined by neutron powder diffraction measurements. The decrease of these two parameters as compared to YBa₂Cu₃O₆ is much stronger for lithium than for zinc substitution. The difference is quantitatively explained by the presence of holes created in the CuO₂ planes. These holes arise from the substitution of plane Cu²⁺ by Li⁺. We suggest an explanation why such holes are not seen for the same substitution of plane Cu²⁺ by Li⁺ in orthorhombic superconducting YBa₂Cu_3-xLi_xO _{7 - δ} . Received 31 October 2001 and Received in final form 6 March 2002 Published online 25 June 2002     

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     

Broad-band dielectric spectroscopy of Ba 2NaNb 5O 15 single crystal

Barium sodium niobate (BNN) single crystals are studied by IR spectroscopy, time-domain THz transmission spectroscopy, HF coaxial wave-guide technique and LF dielectric spectroscopy to cover the frequency range 10²-10¹⁴ Hz in a wide temperature interval. The dielectric response parallel and perpendicular to the polar c-axis is discussed. The ferroelectric transition at T _c = 830 K is driven by a relaxational soft mode coupled with another central-mode type relaxation which both gradually disappear on cooling in the ferroelectric phase. Below T _i the parameters of the expected IR active amplitudon were estimated. The low-temperature permittivity increase on cooling for the field direction has been explained by an incipient proper ferroelectric-ferroelastic transition driven by an IR and Raman active B₂-symmetry soft mode. Received 24 August 2002 Published online 19 December 2002 RID="a" ID="a"e-mail: buixader@fzu.cz     

Phase transition and random-field induced domain wall response of SrTi O 3

The dielectric permittivity ε^′ - i of SrTi ¹⁸O ₃ (STO18) is studied under a dc electric field E as a function of the temperature, T. In ε^′ vs. T, a double-peak is found when 0 < E < 30 KV/m. While the peak at high-T is attributed to the smeared ferroelectric phase transition, the low-T one is induced by domain wall motion. The transverse Ising model including an external homogeneous and quenched random-fields is successfully used to describe both the smeared phase transition and the domain wall response in the low-T domain state. The calculations are in good agreement with the experimental results. Received 4 January 2002 / Received in final form 25 March 2002 Published online 19 July 2002     

Measurement of 2+ 1 level lifetimes in 162Yb and 162Er by fast electronic scintillation timing

Lifetime measurements for the 2⁺ ₁ levels of ¹⁶²Er and ¹⁶²Yb were obtained in β⁺/ɛ decay at the Yale Moving Tape Collector by fast electronic scintillation timing of β⁺γ coincidences. Received: 2 September 2002 / Accepted: 1 October 2002 / Published online: 4 February 2003 RID="a" ID="a"e-mail: mark.caprio@yale.edu Communicated by J. ?yst?     

Three-body decays of light nuclei: 6Be, 8Li, 9Be, 12O, 16Ne, and 17Ne

The theoretical approach to the two-proton radioactivity and three-body decays developed in (L.V. Grigorenko, R.C. Johnson, I.G. Mukha, I.J. Thompson, M.V. Zhukov, Phys. Rev. Lett. 85, 22 (2000) and to be published in Phys. Rev. C) is applied to the range of light nuclear systems. We study nuclear structures, widths, and momentum correlations for the decay fragments. Strong contradictions with experiment, as well as effects of special interest, are found in ¹²O and ¹⁶Ne nuclei. Received: 21 March 2002 / Accepted: 16 May 2002 / Published online: 31 October 2002 RID="a" ID="a"e-mail: l.grigorenko@surrey.ac.uk     

Signature inversion in πi13/2⊗νi13/2 structure in 178Ir

High-spin states in ¹⁷⁸Ir were investigated by means of in-beam γ-ray spectroscopy techniques using the multidetector array GASP. Excited states of ¹⁷⁸Ir were populated through the ¹⁵⁹Tb(²⁴Mg, 5n) fusion-evaporation reaction at E(²⁴ Mg) = 131-141 MeV. Several rotational bands were observed. Among them, the πi _13/2⊗νi _13/2 structure has been identified up to spin 36 ?. This band exhibits an anomalous signature splitting and a signature inversion around spin 25 ?. Received: 13 December 2000 / Accepted: 11 April 2001     

High resolution laser spectroscopy of NaAr: Improved interaction potential for the ground state

The absorption spectrum of NaAr has been investigated with high resolution using a supersonic beam of molecules and a tunable dye laser. About 3 300 absorption lines due to the transition A ² Π ← X and B ² Σ ← X have been observed. In addition, we observed the spectral distribution of the fluorescence for a particular absorption line. From all experimental data the X ² Σ ⁺ interaction potential has been deduced in a fully quantum-mechanical method of approach. The potential is given in terms of an analytical Hartree-Fock-Dispersion function. For the equilibrium parameters of the X state we get R _e = 5.01(1) ? and D _e = 41.6(2) cm ^-1 . Received 28 August 2002 / Received in final form 15 October 2002 Published online 17 December 2002 RID="a" ID="a"Now at Knick Elektronische Messger?te, Beuckestr. 22, 14163 Berlin, Germany. RID="b" ID="b"e-mail: dz@kalium.physik.tu-berlin.de     

The neutron and proton two-particle nucleus 134Sb: New low-spin states observed in the decay of 134Sn and an estimate of the energy of the 7- isomer

Excited states in the ¹³⁴Sb nucleus, populated in the β^--decay of ¹³⁴Sn, have been studied at the mass separator OSIRIS. The ¹³⁴Sn activity was produced via fast neutron-induced fission of ²³⁸U target. A main result was the discovery of a very low-lying first-excited state of ¹³⁴Sb, at 13keV, which has led to a strong revision of the level scheme. The new results are compared with different theoretical calculations and with the known data for the analogous neutron and proton two-particle nucleus in the ²⁰⁸Pb region. On the basis of this comparison, the energy of the ( πg _7/2νf _7/2)_7- isomer is estimated to be about 250keV, some 100keV lower than previously reported. Received: 21 March 2002 / Accepted: 16 May 2002 / Published online: 31 October 2002 RID="a" ID="a"e-mail: anovak@fuw.edu.pl