EFG Studies at 111Cd in InBi Systems

TDPAC study of InBi_1−x Te _x with x=0.0, 0.01, 0.05, 0.1 and 0.2 as a function of temperature is done. Both pure and Te-doped samples show a semi-metallic character up to around room temperature. Above room temperature a steep transition to semiconducting state was observed, which is independent of the doping concentrations. Hence Te may be in the interstitial sites. Conductivity measurement of the above samples showed the same trend as observed in the EFG studies. Thus the importance of the conduction electron density is prominently seen in these systems. This revised version was published online in September 2006 with corrections to the Cover Date.     

Quadrupole Interaction of 99Ru in Pr,Nd and 100Rh in Tb Hosts

The electric field gradient at transition element impurities ⁹⁹Ru and ¹⁰⁰Rh in metallic rare earth hosts Pr, Nd and Tb has been investigated by time differential perturbed angular correlation (TDPAC) technique at room temperature. The electric field gradients, calculated from the measured quadrupole interaction frequencies at room temperature, are; RuPr: 6.06×10¹⁷ V/cm², RuNd: 5.83×10¹⁷ V/cm² and RhTb: 5.40×10¹⁷ V/cm². The electronic enhancement factors (α) for RuPr and RuNd are about 2.5 times the value observed in RuGd and RhTb (it is found to be more than 40 as in RhGd). The results cannot be explained in terms of the existing models based on charge transfer or volume mismatch of the impurity and the host. This revised version was published online in September 2006 with corrections to the Cover Date.     

Theg-factor of the 659 keV level in117In

We have measured theg-factor of the 659 keV, 3/2⁺, state in¹¹⁷In, using time differential perturbed angular correlation technique. The spin precession of this state was measured in an external field of 20·2 kG. The values of the Larmor precession frequencyω and theg-factor are obtained to be (60·1±0·3)10⁶ rads/sec and 0·625±0·007 respectively.     

Inorganic biochemistry with short-lived radioisotopes as nuclear probes

Metal ions are ubiquitous in the biosphere. In living organisms metalloproteins with specifically designed metal cores perform vital chemical processes. On the other hand, several heavy metals are detrimental to living organisms and nature has developed effective enzymatic detoxification systems which convert toxic metal ions to less toxic species. The nuclear spectroscopy technique Time Differential Perturbed Angular Correlation (TDPAC) of γ-rays uses radioactive isotopes as nuclear probes in these metal cores to obtain a better understanding of the structural and functional significance of these metal cores by monitoring the nuclear quadrupole interaction of the TDPAC probe. Since this technique is based on the nuclear decay, it is also applicable under physiological conditions, i.e., especially at picomolar concentrations. For these studies an indispensable prerequisite is the production of the TDPAC probes with highest possible specific activity and purity as is done by the on-line mass separator ISOLDE at CERN in Geneva. This revised version was published online in July 2006 with corrections to the Cover Date.     

LaFeO3纳米材料电四极超精细相互作用TDPAC测量

用时间微分扰动角关联方法测量了LaFeO3纳米中的电四极超精细相互作用. 扰动角关联探针核14057La 14058Ce由139La(n,γ)140La反应产生, 实验只观察到一个La晶位的四极相互作用. 在室温下， 20和40 nm 以及晶体LaFeO3的四极相互作用频率ω0分别为 687.4 , 698.3 和742.9 Mrad/s , 频率分布宽度系数σ分别为 0.014, 0.009和0.001, 电场梯度不对称系数η=0. 实验数据表明, 电场梯度主轴与晶轴方向一致; 样品具有菱方结构, 晶体到纳米发生菱方向正交结构转变, 纳米尺度越小, 越趋于正交结构; 由于邻近核的扰动, 随纳米颗粒增大, 四极相互作用频率分布宽度系数σ变小, 晶体时最小. The quadrupole interactions in the nano and crystalline LaFeO3 perovskites have been investigated by TDPAC. The TDPAC probing nuclei 14057La 14058Ce were produced through the nuclear reaction 139La(n.γ)140La at the CIAE heavy water experimental reactor. One electric quadrupole interaction was detected for each material, which is assigned to the La site. The quadrupole interaction frequencies of 687.4, 698.3 and 742.9 Mrad/s with a distribution coefficient of 0.014, 0.009 and 0.001 were observed at room temperature for the 20 and 40 nm nano LaFeO3 and crystalline LaFeO3, respectively. The fitting yielded the EFG asymmetry parameter η=0, which indicates that the principal axes of the EFG is aligned with the crystallographic axes. The experimental results show that the structure of crystalline LaFeO3 is rhombohedral, the changing of the structure towards the orthorhombic structure takes place from the crystalline LaFeO3 to the nano LaFeO3, and the smaller the nano grain size, the larger the change. The frequency distribution is caused by the perturbation of the neighboring atoms, and thus, the distribution coefficient increases with decreasing the nano grain size and the crystalline LaFeO3 arrives at its maximum.     

Hyperfine interaction study of electric field gradient in hafnium phosphide using181Ta probe

The hyperfine interaction of¹⁸¹Ta in HfP has been investigated by time differential perturbed angular correlation method which yielded interaction frequencyv _Q=630.20(15) MHz. The observed electric field gradient is calculated to be 1.66(25) × 10²⁰ V/m².     

The Electric Field Gradient of 111Ag in Macrocyclic Crown Thioethers

Time differential perturbed angular correlation experiments and ab-initio density functional theory calculation were used to determine the electric field gradients of the metal centres of the macrocyclic crown thioethers Ag(15S5)[BF₄], Ag(18S6-CH₂OH)[CF₃SO₃], Ag(18S6)⁺, Ag(19S6-OH)[Tosylat] and Ag(20S6-OH)[CF₃SO₃]. The density functional theory calculations have been performed with the Amsterdam Density Functional code ADF. A “fingerprint system” is introduced, which allows to assign electric field gradients to certain Ag coordinations in these crown thioether complexes.     

Nuclear probes in life sciences

The nuclear quadrupole interaction at metal sites in macromolecules monitored by time differential perturbed angular correlation provides information on the local environment of metal ions residing at these sites. This information is obtained in the ultra-trace regime and is, therefore, extremely valuable for research on reaction pathways of enzymatic heavy metal detoxification, for the development of radiopharmaceuticals, for investigations into protein architectures on surfaces, and for environmental research. This revised version was published online in August 2006 with corrections to the Cover Date.     

The Nuclear Quadrupole Interaction of 204mPb in Lead Oxides

The nuclear quadrupole interaction of ^204mPb in lead oxides has been measured by γ–γ time differential perturbed angular correlation. Ab-initio calculations of the electric field gradients and X-ray diffraction allowed the assignment of the detected nuclear quadrupole interactions to the different Pb sites in the PbO phases litharge and massicote as well as in Pb₃O₄. The TDPAC probe ^204mPb was produced with a ²⁰⁴Bi/^204mPb-generator at the home laboratory at the University of Leipzig. The use of a high performance liquid chromatography system increased significantly the yield, the specific activity of ^204mPb, and reduced the acidic concentration of the eluate.     

TDPAC Study of the Hydrogen Uptake Process in HfNi

The electronic properties of the HfNi-hydrogen system has been investigated, as a function of the hydrogen composition ratio (x), using combined Time Differential Perturbed Angular Correlation (TDPAC) technique and standard full-potential Linearized-Augmented-Plane-Wave method. The experimental TDPAC data confirm the presence of a two-step hydrogenation process in this system, with the octahedral holes filled first. The major part of the electric field gradient at the hafnium site is from p–p contribution, shifted down in energy by hydrogen s-states contribution.