Determination of the activity and nuclear decay data of 157Tb.

Terbium-157 was radiochemically extracted from an irradiated tantalum target. Since the resulting material contained a significant impurity of 158Tb, 157Tb was isotopically purified using laser resonance ionization at the RISIKO mass separator in Mainz and then implanted on an aluminum (Al) foil. The implanted 157Tb was measured by two different calibrated gamma-ray spectrometers to determine photon emission rates. After dissolving the Al foil, a high purity 157Tb solution was obtained. The corresponding activity concentration was determined with a low relative uncertainty of 0.52% through a combination of liquid scintillation counting using the TDCR method and 4π(X,e)(LS)-(X,γ)(CeBr3) coincidence counting. By combining the results from all measurement techniques, emission intensities for K X-rays and gamma-rays were derived and found to be 16.05(31)% and 0.0064(2)%, respectively. The probability for K electron capture of the first forbidden non-unique transition to the ground state was determined to be 17.16(35)%. The probabilities for the electron-capture branch to the excited level and the ground state were found to be 0.084(4)% and 99.916(4)%, respectively. A Q+ value of 60.23(18) keV was estimated based on simplified BetaShape calculations, assuming an allowed transition.

Ion implantation of 226Ra for a primary 222Rn emanation standard.

Laser resonance ionization at the RISIKO 30 kV mass separator has been used to produce isotopically and isobarically pure and well quantified 222Rn emanation standards. Based upon laser-spectroscopic preparation studies, ion implantation into aluminum and tungsten targets has been carried out, providing overall implantation efficiencies of 40% up to 60%. The absolute implanted activity of 226Ra was determined by the technique of defined solid-angle α-particle spectrometry, where excellent energy resolution was observed. The 222Rn emanation coefficient of the produced targets was studied using α-particle and γ-ray spectrometry, and yielded results between 0.23 and 0.34, with relative uncertainty on the order of 1%. No dependence exceeding a 1% change of the emanation on humidity could be identified in the range of 15 %rH to 75 %rH, whereas there were hints of a slight correlation between the emanation and temperature. Additionally, and as expected, the emanation coefficient was found to be dependent on the target material as well as the implanted dose.

Terbium Medical Radioisotope Production: Laser Resonance Ionization Scheme Development.

Terbium (Tb) is a promising element for the theranostic approach in nuclear medicine. The new CERN-MEDICIS facility aims for production of its medical radioisotopes to support related R&D projects in biomedicine. The use of laser resonance ionization is essential to provide radioisotopic yields of highest quantity and quality, specifically regarding purity. This paper presents the results of preparation and characterization of a suitable two-step laser resonance ionization process for Tb. By resonance excitation via an auto-ionizing level, the high ionization efficiency of 53% was achieved. To simulate realistic production conditions for Tb radioisotopes, the influence of a surplus of Gd atoms, which is a typical target material for Tb generation, was considered, showing the necessity of radiochemical purification procedures before mass separation. Nevertheless, a 10-fold enhancement of the Tb ion beam using laser resonance ionization was observed even with Gd:Tb atomic ratio of 100:1.

Detection of the Lowest-Lying Odd-Parity Atomic Levels in Actinium.

Two lowest-energy odd-parity atomic levels of actinium, 7s^{2}7p^{2}P_{1/2}^{o}, 7s^{2}7p^{2}P_{3/2}^{o}, were observed via two-step resonant laser-ionization spectroscopy and their respective energies were measured to be 7477.36(4) and 12 276.59(2) cm^{-1}. The lifetimes of these states were determined as 668(11) and 255(7) ns, respectively. In addition, we observed the effect of the hyperfine structure on the line for the transition to ^{2}P_{3/2}^{o}. These properties were calculated using a hybrid approach that combines configuration interaction and coupled-cluster methods, in good agreement with the experiment. The data are of relevance for understanding the complex atomic spectra of actinides and for developing efficient laser cooling and ionization schemes for actinium, with possible applications for high-purity medical-isotope production and future fundamental physics experiments.

The electron affinity of astatine.

One of the most important properties influencing the chemical behavior of an element is the electron affinity (EA). Among the remaining elements with unknown EA is astatine, where one of its isotopes, 211At, is remarkably well suited for targeted radionuclide therapy of cancer. With the At- anion being involved in many aspects of current astatine labeling protocols, the knowledge of the electron affinity of this element is of prime importance. Here we report the measured value of the EA of astatine to be 2.41578(7) eV. This result is compared to state-of-the-art relativistic quantum mechanical calculations that incorporate both the Breit and the quantum electrodynamics (QED) corrections and the electron-electron correlation effects on the highest level that can be currently achieved for many-electron systems. The developed technique of laser-photodetachment spectroscopy of radioisotopes opens the path for future EA measurements of other radioelements such as polonium, and eventually super-heavy elements.

High-resolution laser resonance ionization spectroscopy of 143 - 147 Pm.

We present the results of high-resolution laser spectroscopy of the long-lived radioactive isotopes 143 - 147 Pm. The hyperfine structures and isotope shifts in two different atomic ground-state transitions at 452 nm and 468 nm were probed by in-source laser spectroscopy at the RISIKO mass separator in Mainz, using the PI-LIST ion source. From the hyperfine coupling constants the nuclear magnetic dipole and electric quadrupole moments for 143 - 147 Pm were derived, and the measured isotope shifts allowed the extraction of changes in nuclear mean square charge radii.

The consensus concept for thermostability engineering of proteins: further proof of concept.

Previously, we calculated a consensus amino acid sequence from 13 homologous fungal phytases. A synthetic gene was constructed and recombinantly expressed. Surprisingly, consensus phytase-1 was 15-26 degrees C more thermostable than all parent phytases used in its design [Lehmann et al. (2000)Protein Eng., 13, 49-57]. In the present study, inclusion of six further phytase sequences in the amino acid sequence alignment resulted in the replacement of 38 amino acid residues in either one or both of the new consensus phytases-10 and -11. Since consensus phytase-10, again, was 7.4 degrees C more thermostable than consensus phytase-1, the thermostability effects of most of the 38 amino acid substitutions were tested by site-directed mutagenesis. Both stabilizing and destabilizing mutations were identified, but all affected the stability of the enzyme by <3 degrees C. The combination of all stabilizing amino acid exchanges in a multiple mutant of consensus phytase-1 increased the unfolding temperature from 78.0 to 88.5 degrees C. Likewise, back-mutation of four destabilizing amino acids and introduction of an additional stabilizing amino acid in consensus phytase-10 further increased the unfolding temperature from 85.4 to 90.4 degrees C. The thermostabilization achieved is the result of a combination of slight improvements from multiple amino acid exchanges rather than being the effect of a single or of just a few dominating mutations that have been introduced by chance. The present findings support the general validity of the consensus concept for thermostability engineering of proteins.