NMRON studies of ferromagnetic hcp and fcc Co

The high resolution hyperfine spectroscopy, modulated adiabatic passage of oriented nuclei (MAPON), has been applied for the first time to high purity, elemental systems. Detailed comparisons between the electric quadrupole hyperfine interactions (EQI’s) and, in particular, their distributions, are obtained for⁶⁰CoCo where the hosts are a single crystal of hcp cobalt and a polycrystalline cobalt foil of predominantly fcc character. For hcp Co, with the electronic magnetization, M, parallel to the c-axis, the mode value P/h=3e²qQ/4I(2I−1)h=−48.5(5) kHz. This fractional distribution implies the sharpest electric field gradient (efg) measured in a metal to date, using MAPON spectroscopy, in excess of two times sharper than that of the most dilute impurity efg in a crystallographically cubic ferromagnetic host. The mode efg is V_zz=−27.3(32)×10¹⁹ Vm⁻². For the polycrystalline, predominantly fcc foil, prepared by quenching, the EQI mode value is P/h=−6.2(4) kHz with a FWHM of 12.0(7) kHz yielding a mode efg of V_zz=−3.5(5)×10¹⁹ Vm⁻².     

Studies of weak electric quadrupole interaction in57,60CoFe using modulated adiabatic passage on oriented nuclei

The electric quadrupole interactions at⁵⁷Co and⁶⁰Co in co-diffused^57,60CoFe single crystal have been measured using Modulated Adiabatic Passage on Oriented Nuclei (MAPON). The quadrupole splittings Δν_Q<100> are + 18(2) kHz for⁵⁷Co and +9(2) kHz for⁶⁰Co, corresponding to a principal electric field gradient (efg) tensorV _zz =2.0(5)×10¹⁹ Vm⁻² and 2.5(6)×10¹⁹ Vm⁻², respectively, in broad agreement with previous MAPON results for CoFe. The distributions of the efg’s are very similar for the two isotopes, verifying that previously reported differences in⁵⁸CoFe and⁶⁰CoFe could be attributed to different host preparations. The measurement of such weak efg’s which are not spectroscopically resolved, allows determination of new nuclear electric quadrupole moments, not accessible by other techniques. Applications to other systems are discussed.     

The low temperature quadrupole orientation of103Ru in ruthenium

The quadrupole frequencyv _Q =e ² qQ/h of¹⁰³Ru (Z=44,N=59) in a ruthenium single crystal has been measured using the technique of low temperature quadrupole orientation to bev _Q (¹⁰³RuRu)=−14.7(5) MHz. Temperatures below 2 mK were reached in this experiment using a PrNi₅ demagnetization stage attached to a³He−⁴He dilution refrigerator. Using the measured magnitude of the RuRu electric field gradient (EFG) at low temperatures |eq(RuRu)|=1.02(3)×10¹⁷ V.cm⁻² [1] and adopting the sign ofeq(RuRu) to be negative from systematics, this result yields a value for the ground-state electric quadrupole moment of¹⁰³Ru ofQ(¹⁰³Ru)=+0.59(2) b. This moment may be interpreted using the weak coupling model of de-Shalit [2]. A Korringa constant for¹⁰³RuRu ofC _K=39(6) Ks was measured in this experiment. Taking advantage of a small iridium contamination of the ruthenium single crystal, the quadrupole moment of the¹⁹²Ir ground state was determined to beQ(¹⁹²Ir)=+2.12(25) b. The sign of the IrRu electric field gradient was found to be negative as a result of this work.     

MAPON EFG Result for 54Mn in Cubic Cobalt

Modulated adiabatic passage on oriented nuclei (MAPON) spectroscopy has been used to measure the electric quadrupole interaction at dilute ⁵⁴Mn impurity probes in crystallographically cubic (fcc) cobalt. The measured value is P/h=+5.2(5) kHz and using Q=+0.33(3) b, leads to an electric field gradient of V _zz =+1.3(2)×10¹⁹ V m⁻². This result is consistent with established trends for Mn and Co probes in the 3d ferromagnetic hosts. This revised version was published online in September 2006 with corrections to the Cover Date.     

Transient NMRON of brute force oriented110mAgAg

A novel technique involving electrodeposition has been used to prepare an elemental silver specimen wherein radioactive^110mAg probe nuclei are confined to a surface layer of approximately 0.1 μm depth. This specimen was then brute force oriented in a field of 8T and the continuous wave (CW) nuclear magnetic resonance on oriented nuclei (NMRON) spectrum showed an integrated destruction of some 58%. Moreover the transient NMRON techniques of single and modulated adiabatic passage were successfully applied, resulting in a determination of the electric quadrupole interaction strength at the^110mAg site in polycrystalline silver of P/h=+0.74(5)kHz with a FWHM of ΔP/h=0.75(8)kHz. The resulting mode electric field gradient is V_zz=+1.87(23)×10¹⁸Vm⁻¹. Analysis of the single passage data provides an estimate for the nuclear spin lattice relaxation constant in silver at 8T of C_k=1.6(3)s.K.     

High-resolution measurement of NMR-ON for191PtFe

NMR-ON measurements on¹⁹¹PtFe were repeated to look for a reported quadrupole splitting effect: a sample annealed at 850°C and measured at 15.1(6) mK gives a spectrum with a single gaussian peak with a line width of 0.39(4) MHz, the narrowest ever observed. The spectrum obtained with another sample annealed at 650°C and measured at 8.3(4) mK resembles one with a quadrupole splitting, but the ratio of the second sub-resonance to the first is inconsisten with the estimation from a model which takes account of a quadrupole splitting and fast relaxation limit. The present study shows the quadrupole splitting ofv _Q (¹⁹¹PtFe)≤0.86 MHz.     

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.     

Discrepancies in NMRON Knight Shifts of impurity nuclei in ferromagnets

Precision NMRON field shift studies have been carried out up to 8T on a⁵⁴MnNi single crystal along a hard [100] direction and on a¹²⁵SbFe single crystal along a hard [110] direction. For both systems, high field (B _app>-1T) and low field (0.3T<B _app<0.8T) data sets are obtained. The analysis reveals a significant discrepancy between the apparent Knight Shift dependent on whether the low field or high field data set is utilised. For both systems, consideration of the high field data sets yield a zero Knight Shift K(⁵⁴MnNi)=+0.0(0.2)% and K(¹²⁵SbFe)=+0.2(1.4)%, whereas the low field data sets yield K(⁵⁴MnNi)=+7.5(3.9)% and K(¹²⁵SbFe)=−5.4(3.3)% respectively. The field range dependence of K suggests that only Knight shifts measured in large fields (>-1T) are meaningful for establishing systematics. This casts some doubt on the greater bulk of the literature’s NMRON Knight shift studies, where predominantly low fields have been used to determine K.     

The sign of the electric field gradient at the nuclear site of Zn in Zn metal

By use of low temperature nuclear quadrupole orientation the quadrupole coupling constant of^69mZn in a Zn single crystal has been determined asv _Q=eQV _zz/h=–28(3) MHz.A positive sign forV _zzat the nuclear site of Zn in Zn is deduced. The half-life of^69mZn has been remeasured asT _1/2=13.756 (18)h.     

NMRON spin echo in a slowly varying magnetic field

Nuclear spin-spin relaxation of⁶⁰Co and⁵⁶Co in iron single crystals has been studied, using the three-pulse NMRON spin echo. A previously reported rapidT ₂ in⁶⁰CoFe is shown to have arisen from a modulation of the echo amplitude, caused by variations in the phase of the Larmor precession relative to the applied rf field. A lower limit ofT ₂∼0.2s is found in⁵⁶Co⁵⁶ Fe. Extension of this result to other CoFe samples is discussed.     

The sign of the quadrupole interaction of the 828 keV state of115In in Zn

Sign and magnitude of the electric quadrupole interaction of the 828 keV state of¹¹⁵In in a Zn single crystal was determined by aβ-γ TDPAC measurement. The result:v _Q =e·'Q _I V _zz /h=?193(13)MH_z confirms the universal correlation between the electronic and ionic contributions to the total electric field gradient proposed by R.S. Raghavan et al.     

Recent experiments with mapon spectroscopy

Electric quadrupole interactions of impurity nuclei in single crystals of⁵⁴MnNi,¹²⁵SbNi and¹²⁵SbFe have been studied as a function of crystal field direction and applied magnetic field using MAPON. Distributions are in all cases broad compared with the mode values of the EQI's. For⁵⁴MnNi the mode efg is isotropic to better than 5% between the easy <111> axis and a hard <100> axis. The efg is +0.88 (15)x 10¹⁹ Vm⁻². The mode efg for¹²⁵SbFe along its easy <100> axis is one half of that along a hard <112> axis, and one third of that measured along the easy <111> axis of¹²⁵SbNi. The much larger efg mode and distribution seen in¹²⁵SbNi, for four to eight times greater dilution than for¹²⁵SbFe, suggests intrinsic contributions due to valence screening effects in the more itinerant nickel host.     

The electric field gradient at188Os nuclei in Re metal

The electric quadrupole interaction of the first excited 2⁺ state of¹⁸⁸Os in hexagonal rhenium metal was investigated by means of the time-differential perturbed angular correlation technique. From the observed quadrupole frequencyV _Q=170(7) MHz, we deduce an electric field gradient value of |V_zz|=4.77(23)·10²¹V/m² for the system OsRe. The half-life of the 2⁺ state was measured to be 641(4)ps.     

Recent experiments with transient NMRON

High resolution magnetic and electric hyperfine interaction distributions are determined for single crystal⁵⁴MnNi with diffused impurity concentrations of 0.14 and 0.40 at%, and for a 0.1 µm layer of⁶⁰CoFe co-plated onto single crystal Fe. High quality gamma detected nuclear spin echoes recorded for the⁶⁰CoFe specimen demonstrate that a reduced influence of the RF skin effect far outweighs any magnetic hyperfine field interaction broadening associated with the co-plating process.     

Electric field gradients created by near neighbour impurity atoms in a cubic silver host

The electric quadrupole interactions produced by near neighbour impurity atoms of Cu, Au, Zn, In, Sn and Bi on¹¹¹Cd probe nuclei in a cubic Ag lattice were studied by the TDPAC method. The effects of the type of impurity and its concentration have been investigated. The results show the presence of a high-frequency interactionv _Q ^h superimposed to a smeared out low frequencyv _Q ^l . The high frequency interaction, in the range 20 to 600 MHz, is attributed to impurity atoms located in nearest neighbour sites, while the low frequency interaction, in the range 2 to 12 MHz, is generated by impurities distributed at various different atomic distances from the probe nuclei. Bothv _Q ^h andv _Q ^l increase with impurity concentration leaving the ratiov _Q ^h /v _Q ^l almost constant. The results show that the high frequencyv _Q ^h is linearly dependent on the solute valence, and a logarithmic function of the impurity concentration, in the range 0.5 to 4.5 at. %. Large size effects have been observed in CuAg and BiAg alloys. Instead for ZnAg and SnAg, thev _Q ^h andv _Q ^l variation is attributed basically to charge effects.Work supported in part by Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq) and Financiadora de Estudos e Projetos (FINEP).     

The effect of temperature and concentration on the electric field gradient in binary indium alloys

The concentration and temperature dependence of the quadrupole hyperfine interaction of¹¹¹Cd in InTl (hcp),InPb (fct),InTl (fct) andInCd (fct and fcc) alloys were studied using the perturbed angular correlation technique. The change in the observed quadrupole interaction frequency with concentration can be described by a linear dependence on the axial ratioc/a in all cases. In the alloys with identical crystal structures the strength of thec/a dependence is independent of the solute, in contrast to the strength of the concentration dependence. In all cases where no phase transition occurs, the change in the electric field gradient with temperature follows the empirical relationV _zz (T)=V _zz(0) · (1–B·T ^3/2), where the coefficientB depends on the lattice structure, on the solute-solvent combination and on the concentration. The phase transitions ofInCd alloys at 293 K could clearly be seen as discontinuities in the temperature curves. A similar series of discontinuities observed around 116 K suggests the existence of a cubic low temperature phase.     

Quadrupole interaction studies of Hg in Sb

Time differential perturbed angular correlation and nuclear orientation studies of the electric quadrupole interaction for Hg in Sb have been performed. The effective field gradients |V _zz ^eff (HgSb)|=1.43(18)×10¹⁷V cm^–2 at room temperature andV _zz ^eff (HgSb)=+1.8(2) × 10¹⁷V cm^–2 below 0.05 K have been derived. These two values are no indication for an anomalous temperature dependence of the effective field gradient for Hg in Sb. The value of the electric field gradient fits well into the systematics for Hg in other hosts. It is shown that the electronic enhancements of the field gradients are correlated to the valence of the impurities and are rather insensitive to the host properties.On leave of absence from: University of Lisboa, Portugal     

Pulsed NMRON oscillatory free induction decay signals in the angular distribution of gamma radiation from plated60CoFe

Results for an inhomogeneously broadened⁶⁰CoFe NMRON sample have been obtained for gamma detected single pulse (nutation) and two pulse (free induction decay) experiments in the region of intermediate-to-lowR(=₁/). Here ₁ is the angular frequency measure of the strength of the ferromagnetically enhanced RF field at the nucleus and is the HWHM of the inhomogeneously broadened line. Comparisons of the oscillatory FID signals obtained are made with the theoretical predictions of the following paper [6].     

DPAC study of radiation damage in178W recoil implanted silicon

The annealing behaviour of radiation damage in¹⁷⁸W recoil implanted n-type Si is studied from 295 to 641 K by the differential perturbed angular correlation method (DPAC), using¹⁷⁸Hf as probe nuclei for the first time. Preliminary results suggest that oxygen-vacancy (O-V) pairs are observed, which give rise to a quadrupole interaction characterized by |V _zz|=5.41×10¹⁸ V/cm² (v _Q=2550 MHz). The probe nuclei also experience an electric field gradient (EFG) due to distant defects.     

LMR quadrupole interaction measurement on69mGe and71mGe in Zn

A new experimental set-up to perform in-beam LMR (Level Mixing Resonance) measurements is briefly outlined. The first results are reported here. The quadrupole interaction of^69mGeZn is measured and in good agreement with earlier measurements:v _Q=80.6(4) MHz; for^71mGeZn, the valuev _Q=33.1(30)MHz is found. In addition, the relaxation behaviour and radiation damage of Ge recoil implanted in Zn is studied.