The electric quadrupole interaction of 111Cd in ZrZn2 and Zn in the samples prepared at 8 GPa

The perturbed angular correlation (PAC) measurements with the ¹¹¹In-¹¹¹Cd nuclear probe embedded into the lattice of the cubic (C15) Laves compound ZrZn₂ showed that ¹¹¹Cd nuclei experienced an axially symmetric electric quadrupole interaction with a frequency ν _Q  = 132.4 MHz at room temperature. The samples were synthesized and doped with the probe at a pressure 8 GPa. The temperature dependence of ν _Q was shown to be linear: ν _Q (T) = 147(1 − 0.033 T) MHz. Since the value of ν _Q is very close to that known for ¹¹¹Cd in the lattice of Zn, we have checked if it could be assigned to residual Zn metal in the sample. For the Zn sample melted and doped with ¹¹¹In at 8 GPa we have obtained ν _Q  = 117.3 MHz at 300 K and 127 MHz at 80 K – both values considerably lower than that for ¹¹¹In doped Zn samples prepared at an ambient pressure. These data, and the fact that ν _Q (T) in Zn is known to follow the T ^3/2 law, allow to attribute the ν _Q value quoted above to ¹¹¹Cd nuclei at the substitutional sites with tetrahedral symmetry in the Zn sublattice of ZrZn₂.     

Orientation of the oxygen-induced non-axially symmetric electric field gradient at181Ta in Ta

The interaction of dilute¹⁸¹Ta in Ta with interstitial oxygen has been investigated via the γ-γ TDPAC-technique applied to the 482 keV state in¹⁸¹Ta. The trapping of Oxygen leading to a quadrupole interaction frequency ν_Q=580(5) MHz with an asymmetry parameter of η-0.37 (1) has been observed after melting the radioactive parent isotope¹⁸¹Hf with Ta. The temperature dependence of the quadrupole interaction frequency between 17 K and 293 K was found to be very weak whereas η varied by about 10%. In a single crystal experiment the orientation of the three principal axes of the electric field gradient leading to ν_Q was determined. The V_zz-axis points in <110>, the V_yy-axis in <100> and the V_xx-axis in <110> direction. These results can be understood in the charge cloud model, suggested by Wrede et al. /1/ for a similar situation found in the HfNb system.     

Cavity formation at indium impurities in bcc metals

The defect formation in the bcc metals W and Mo above annealing stage III and the influence of rare gases on this process were investigated by means of the perturbed angular correlation technique using¹¹¹In as radioactive probe. In both metals a relatively high electric field gradient (EFG) could be observed at the indium site, characterized by the quadrupole interaction frequencies υ_Q=263 MHz, ν=0 and υ_Q=220 MHz, ν≈0.15 for W and Mo, respectively. The observations are assigned to the growth of threedimensional vacancy clusters at the probe atoms with the indium atoms situated in the inner surface of this cavities, thus experiencing the corresponding surface EFG.     

Study of highT c superconductivity in Y1Ba2Cu3O7−x by PAC

HighT _c superconductivity in the YBaCuO superconductor has been investigated through the quadrupole interaction of the probe nuclei⁹⁹Tc. The quadrupole interactions were measured by the TDPAC method from 77 to 296 K. The probe nuclei⁹⁹Tc were introduced into the YBaCuO superconducting specimen by diffusion. The derived electric quadrupole interaction parameters show that the probe nuclei are subject to a unique EFG interaction and occupy a substitutional lattice site in the YBaCuO superconductor. A strong EFG of 10¹⁹ V/cm² was observed. The temperature dependence of the EFG exhibits a linear decrease with temperature increase. Anomalies of both EFG and ν were found in the superconducting transition temperature region. The role of the oxygen vacancies in the Cu−O chains is discussed.     

Temperature dependence of the electric quadrupole interaction at scandium impurities in zirconium and hafnium

The PAC probe⁴⁴Sc was employed to study the magnitude and temperature dependence of the electric quadrupole interaction at the site of the transition metal Sc in the hexagonal host lattices Zr and Hf. In Zr ∼ 100% of the probe atoms were situated on regular lattice sites and a quadrupole interaction frequency of υ_Q=7.8(1)MHz was measured at room temperature. For Hf the fraction of the probe atoms on regular lattice sites was smaller and a damping of the interaction pattern (υ_Q=9.3(5)MHz at 293 K) could not be excluded. The temperature dependence of the electric field gradient in both host lattices was found to be weak.     

Incorporation of the transition metal Hf into GaN

The perturbed angular correlation (PAC) technique was applied to study the incorporation of the transition metal Hf into GaN after implantation. To this end the PAC probe ¹⁸¹Hf(¹⁸¹Ta) was implanted into epitaxial Wurtzite GaN layers (1.3 μm on sapphire) with an energy of 160 keV and doses of 7× 10¹² at/cm². PAC spectra were recorded during an isochronal annealing programme, using rapid thermal annealing (RTA) and furnace annealing, in the 300–1000oC temperature range. After implantation the spectra show a damped oscillation corresponding to a quadrupole interaction frequency (QIF) of ν_Q= 340 MHz for 30% of the probe nuclei. Annealing up to 600oC reduces the damping of this frequency without an increase of the probe atom fraction f_s in these sites. Above 600oC f_s grows rapidly until after the 900oC RTA step more than 80% of the Hf probes experience a well defined QIF due to the incorporation of Hf on undisturbed sites of the hexagonal GaN wurtzite lattice. An interaction frequency of ν_Q= 340 MHz is derived. RTA and furnace annealing yield similar results for annealing up to 800oC, where the undisturbed fraction reaches about 60%. Then RTA at higher temperatures increases this fraction, while furnace annealing leads to a decrease down to 22% after annealing at 1000oC. To our knowledge this is the first time that a transition metal probe like Hf is incorporated to such a large extent into a semiconductor lattice. This revised version was published online in August 2006 with corrections to the Cover Date.     

High Pressure Mössbauer Studies on FCC Fe53Ni47 Alloy

Perturbed angular correlation measurements of the hyperfine interaction of ¹¹¹In in sapphire show, that after implantation and annealing at 1000°C, the fraction of undisturbed probe atoms exhibiting a unique quadrupole interaction with ν _Q = 219(1) MHz (η = 0) varies between 50% at 4 K, 5% at 100 K and 80% at 973 K in a reversible manner. A possible explanation for this surprising behaviour is the influence of so-called ‘after effects’ following the EC-decay of ¹¹¹In to ¹¹¹Cd. Immediately after the decay the ¹¹¹Cd is in an ionized state, then collects electrons from its surroundings and reaches the ground state. The different electronic configurations that arise during this relaxation process affect the amplitude (f _u) and the damping (δ _u) of the unique quadrupole interaction.     

Perturbed Angular Correlation Study of Naturally Occurring Zircon with very Small Impurity Concentrations

We used ¹⁸¹Ta-PAC spectroscopy to characterize the electric field gradient at Zr sites of zircon samples from the Harts Range in Australia. Zircons from this region contain very low levels of radioactive impurities. The PAC spectra between room temperature and 1100°C are axially symmetric and show little damping. The quadrupole frequency decreases linearly with increasing temperature, and the slope of the ν _Q vs. T graph increases above 900°C. This is attributed to a rearrangement of the Si–O coordination, which affects the Zr–O coordination. The spectra of all zircons show a distinct decrease of the anisotropy between 800 and 600°C. This behavior is also seen with samples that do not exhibit the change in slope in the ν _Q vs. T data. We believe that the decrease in the anisotropy is due to an aftereffect following the β-decay of ¹⁸¹Hf.     

Double resonance NMR-on study on oriented188Ir in iron

The quadrupole splitting of oriented¹⁸⁸Ir in iron was studied at 8.6 mK using a double resonance NMR-ON method. With r.f. power applied at the strongest resonance frequency, a second frequency was used to simultaneously investigate the second resonance component, where the splitting is caused by an electric quadrupole interaction. The electric hyperfine splitting frequency ν_Q=e ² qQ/h was measured to be 3.37(11) MHz. With the known electric field gradient of −0.283(6)×10¹⁷ V/cm² at Ir in iron, the spectroscopic quadrupole moment of¹⁸⁸Ir was deduced to be 0.492(26)b. The present results show that the double resonance method is a powerful tool in establishing the quadrupole splitting, if it leads to well-resolved NMR-ON resonance components.     

Quadrupole moment measurement of the highly deformed πg 9/2⊗νh 11/2 band in 130Pr

The quadrupole moment for the πg _9/2⊗νh _11/2 band in the ^130>Pr nucleus has been measured using the Doppler-shift attenuation method. A centroid shift analysis was carried out and a value of Q₀=6.1±0.4 eb, corresponding to an axial prolate deformation of β₂=0.35(3), has been determined. This is the first direct experimental confirmation of the deformation-driving character of the πg _9/2 orbital in an odd-odd nucleus in the A≃135 superdeformed region. Received: 23 April 1998     

NMR study of the electric field gradient in the paramagnetic phase of M<Subscript>3</Subscript>V<Subscript>2</Subscript>O<Subscript>8</Subscript> (M = Co,Ni) compounds

The NMR spectra and the decay of a spin echo signal from ⁵¹V nuclei in Kagome-staircase Co₃V₂O₈ (CVO) and Ni₃V₂O₈ (NVO) single crystals are measured in the temperature range 30–300 K and a magnetic field H ₀ = 20 kOe. The orientation dependences of the ⁵¹V NMR line shape are used to determine the electric field gradient (EFG) parameters, namely, quadrupole frequency ν _Q and asymmetry parameter η. These parameters for NVO and CVO are ν _Q = 180(10) kHz, η = 0.5(1) and ν _Q = 130(10) kHz, η = 0.6(1), respectively. A comparison of the results of calculating EFG tensors with a point charge model and the NMR data indicates that the crystallographically equivalent vanadium atoms in the Ni₃V₂O₈ and Co₃V₂O₈ compounds differ in the EFG axis orientation. M₃V₂O₈ crystals are found to have vanadium positions (V1, V2) with different orientations of the z axis, which specifies the direction of the principal value of EFG (V _zz ): these orientations lie in the bc plane and make an angle of either +51(5)° (V1) or −51(5)° (V2) with axis c. In the temperature range 30–300 K, the EFG tensor components and the local symmetry of the charge surrounding of the vanadium positions in NVO and CVO oxides are found to change insignificantly.     

Study of the structure and electric quadrupole interaction in the intermetallic compound Hf2Fe

The electric quadrupole interactions at¹⁸¹Ta probe nuclei in a cubic Hf₂Fe lattice were studied by the TDPAC method. In addition, the crystalline structure study of the Hf₂Fe compound was performed. The results of the EQI measurement show the presence of two independent interactions, one at low frequency, characterized by ω _Q ⁽¹⁾ =33 Mrad/s and δ=30%, and the other at high frequency described by ω _Q ⁽²⁾ =207 ± 2 Mrad/s and δ=4%. Both interactions are found to be compatible with the crystalline structure established in this investigation. The large temperature dependence of the electric field gradient of the second interaction in the range from 78K to 1183K was determined. The change in the EFG follows the empiricalT ^3/2 -relation.     

Electric field gradients at the 111In site in the ferroelectric and paraelectric phases of LiTaO3

The temperature dependence of the electric-field gradient of ¹¹¹Cd in single crystalline LiTaO₃ was studied from room temperature to 1040 K in the ferroelectric and paraelectric phases. The data taken at room temperature show unambiguously the presence of two quadrupole interaction frequencies, ν_Q1=230 MHz and ν_Q2=242 MHz, with nonzero asymmetry parameters, while above the Curie temperature (T_C=878 K) the data are well described by a unique frequency. The electric field gradient shows a usual temperature dependence, increasing aproximately in a linear fashion until T_C and then decreasing faster. The initial increase is explained mostly by the lattice expansion, while above T_C it is necessary to consider Li and O displacements. This revised version was published online in August 2006 with corrections to the Cover Date.     

Temperature and pressure dependence of magnetic and electric hyperfine interactions in metallic Samarium

The magnetic and electric hyperfine interaction at¹¹¹Cd impurities in Samarium has been investigated by TDPAC measurements. The quadrupole frequency is _Q=20.0(2) MHz at 290 K and has a linear temperature dependence with the same slope (dln_Q/dT)_290K=–7.3(2) 10^–4 K^–1 in the rhombohedral and the hcp phase. The pressure dependence up to 7 kbar is (dln _Q/dT)=+8.7(1.4) 10^–3 kbar^–1. The magnetic hyperfine field of¹¹¹Cd in Sm is H_hf=242(6) kG at 4.2 K. Its temperature dependence confirms the existence of 2 different magnetic phases in Sm. The crystal field parameters B ₂ ⁰ and B ₄ ⁰ have been estimated from a comparison of H_hf(T) with molecular field models. The TDPAC spectra in the magnetic phases suggest that the impurities preferentially occupy the hexagonal Sm sites.     

Site occupancy and molecular complex formation of 19F ions in fullerenes C60 and C70 studied by TDPAD

TDPAD spectroscopy measurements have been performed on two fullerene samples, C₆₀ and C₇₀, with recoil implanted ¹⁹F ions as probe nuclei. Quadrupole coupling frequencies of ν_Q= 54(1) MHz for C₆₀ and ν_Q= 57(1) MHz for C₇₀ were observed. These frequencies are associated with a C–F molecular complex formation. The C₇₀ sample was also examined for possible effects due to variation of temperature. No significant changes were observed. An additional frequency of ν_Q= 13(1) MHz registered for both samples has to be attributed to the formation of H–F complexes. Finally, both samples were analysed for proton dose dependent effects, due to the (p,p'γ) implantation process but no effects have shown up. Specifically, computational studies based on quantum chemical methods were performed to assist in the interpretation of the experimental results, using the code MOPAC. This revised version was published online in August 2006 with corrections to the Cover Date.     

Initial operation at liquid-helium temperature of the M =2270 kg Al 5056 gravitational-wave antenna of the Rome group

Summary We report on the cooling at liquid-helium temperature of our 2270 kg 5056 Al bar at CERN. The liquid-helium container had been filled up to 1500 liters ensuring to keep the antenna cold for more than one month. The antenna is equipped with a resonant capacitive transducer operating at constant electrical charge with a FET low-noise amplifier. The transducer is tuned to the antenna within less than I Hz and the two normal-mode frequencies are ν₋=908.160 Hz and ν₊=924.234 Hz with an applied electrical field in the transducer of 10⁶ V/m. The corresponding overall merit factors areQ ₋=5.20·10⁶ andQ ₊=7.25·10⁶. The transducer has been tested up to an electrical field of 6·10⁶ V/m: in this condition we have βQ≈10⁴. The antenna has been in operation for several weeks giving, for the Brownian noise, values in agreement with the calculated values. We report also on the results of tests performed on a DC SQUID, whose input was connected to a commercial capacitor via a transformer with turn ratio of 1000. Supported in part by Japan Society for the Promotion of Science.     

ECTDL study of N 2 - and O 2 -pressure broadening of a series of ammonia lines in the 1.5 μm (ν 1 +ν 3 ) combination band

Nitrogen and oxygen pressure broadening parameters for seven ^r P(J”,0) transitions of the ν₁+ν₃ overtone band of the main isotope of ammonia with J” varied from 2 to 9 have been measured at room temperature using an external cavity tunable diode laser spectrometer. Air-broadening parameters have also been calculated from the N₂ and O₂ measurements. The results are compared to previous measurements in the ν₁, ν₂, ν₃, ν₄ and ν₁+ν₃ bands and to the parameters for the ν₃ band that are reported in the HITRAN database. PACS 33.70.Jg; 33.70.-W; 33.20.Ea; 42.62.Fi; 42.68.Ca     

Studies of molecular dynamics of thiazides by<Superscript>35</Superscript>Cl NQR spectroscopy and DFT calculation

Molecular dynamics of three derivatives of 1,2,4-benzothiadiazine-1,1-dioxide, hydrochlorothiazide (HCTZ), althiazide (ATZ) and chlorothiazide (CTZ), was studied by³⁵Cl nuclear quadrupole resonance (NQR) spectroscopy. The temperature dependence of the resonance frequency was analyzed within the 6 known standard models. The activation energies estimated from the temperature dependence of the³⁵Cl NQR frequency assuming the Bayer model were 1.07, 2.35 and 2.76 kJ/mol for HCTZ, ATZ and CTZ respectively, which confirms that HCTZ is less rigid than CTZ and ATZ is much more rigid than HCTZ, and suggests that the mechanism of relaxation is based on small amplitude librations. The characteristic temperatures estimated from the Bayer model, with that for CTZ (332.5 K) being much higher than for HCTZ (132.1 K), mean that the intermolecular interactions in CTZ are much stronger than in HCTZ, as suggested by the melting point of CTZ being higher than that for HCTZ. For ATZ the characteristic temperature (288 K) takes an intermediate value, which suggests that the intermolecular interactions in this compound are stronger than in HCTZ and weaker than in CTZ. A significant narrowing of the resonance³⁵Cl NQR line observed for all these compounds at room temperature, relative to that at the liquid nitrogen temperature, suggests an averaging of dipolar interactions as a result of fast rotation of nonquadrupole nuclei in the vicinity of the quadrupole nuclei, when 2πν_Qτ_c ≫ 1 (a rotation of the −NH₂ group in the direct neighborhood of the chlorine nuclei) or a change in the gradient orientation with its value preserved (which is equivalent to rotation of the quadrupole nucleus Cl). The influence of the rotations of the −NH₂ and −CH₂SCH₂CH=CH₂ groups (ATZ) or −CHCl₂ group (TCTZ) on the³⁵Cl NQR frequency was modelled by the B3LYP/6-31G^* method. The frequencies of the libration vibrations calculated from the temperature dependence of the NQR resonance frequency were compared with experimental ones and those implied by the density functional theory, infrared and Raman spectra. For HCTZ the anomalies in the temperature dependence of the³⁵Cl NQR frequency, the lack of hysteresis and small but notable changes in the slope and the jump in the frequency observed at 253 K which does not exceed 0.05 MHz suggest a second-order phase transition at 253 K.     

The mapon technique and recent developments

Typical linewidths observed in NMRON on dilute impurities in ferromagnetic metals are of order 1 MHz, making difficult the observation of structure in the resonance with splitting Δv much less than this value. The technique of Modulated Adiabatic Passage on Oriented Nuclei (MAPON) was recently developed as a means of measuring the weak electric quadrupole splitting Δv_Q of the nuclear hyperfine interaction due to an electric field gradient V_zz. MAPON has successfully been applied to measure Δv_Q as low as 4 kHz, i.e. less than 0.5% of the inhomogeneously broadened NMRON CWFM resonance line. The isotopes⁵⁶Co,⁵⁷Co,⁵⁸Co and⁶⁰Co have been studied in iron single crystal hosts, yielding Δv_Q consistent with known and estimated quadrupole moments. In addition the results to date give striking confirmation of analyses based on the single impurity relaxation model. Following a brief summary of the theoretical development of MAPON a review of experimental data is given for the CoFe<100> system. The variation of Δv_Q with direction of magnetization, measured in⁵⁸CoFe and⁶⁰CoFe single crystal samples, is also described. Further MAPON measurements are described for a⁵⁶CoFe polycrystalline sample, for which the most probable value and width of the distribution of V_zz can be described simply in terms of the single crystal principal axis results. The application of the MAPON technique to the measurement of nuclear electric quadrupole moments in implanted and diffused samples is discussed.     

Diode-laser absorption measurements of CO2, H2O, N2O, and NH3 near 2.0 μm

2 , H₂O, N₂O, and NH₃ concentrations in various flowfields using absorption spectroscopy and extractive sampling techniques. An external-cavity diode laser with a tuning range of 1.953–2.057 μm was used to record absorption lineshapes from measured transitions in the CO₂ 4ν₂ ⁰+ν₃, ν₁+2ν₂ ⁰+ν₃, and 2ν₁+ν₃ bands, H₂O ν₂+ν₃and ν₁+ν₂ bands, N₂O 2ν₁+4ν₂ ⁰, ν₂ ¹+2ν₃, 3ν₁+2ν₂ ⁰, and 4ν₁ bands, and NH₃ν₁+ν₄ and ν₃+ν₄ bands. Measured CO₂, H₂O, and N₂O survey spectra were compared to calculations to verify the HITRAN96 database and used to determine optimum transitions for species detection. Individual lineshape measurements were used to determine fundamental spectroscopic parameters including the line strength, line-center frequency, and self-broadening coefficient of the probed transition. The results represent the first measurements of CO₂, H₂O, N₂O, and NH₃ absorption near 2.0 μm using room-temperature near-IR diode lasers. Received: 12 March 1998/Revised version: 7 May 1998