Search

The formation of carbonyl complexes using atom-at-a-time quantities of short-lived transition metals from fusion and fission reactions was reported in 2012. Numerous studies focussing on this chemical system, which is also applicable for the superheavy elements followed. We report on a novel two-chamber approach for the synthesis of such complexes that allows spatial decoupling of thermalization and gas-phase carbonyl complex synthesis. Neutron induced fission on 235U and spontaneous fission of 248Cm were employed for the production of the fission products. These were stopped inside a gas volume behind the target and flushed with an inert-gas flow into a second chamber. This was flushed with carbon monoxide to allow the gas-phase synthesis of carbonyl complexes. Parameter studies of the transfer from the first into the second chamber as well as on the carbonyl complex formation and transport processes have been performed. High overall efficiencies of more than 50% were reached rendering this approach interesting for studies of superheavy elements. Our results show that carbonyl complex formation of thermalized fission products is a single-atom reaction, and not a hot-atom reaction.

A nuclear spectroscopy experiment was conducted to study α-decay chains stemming from isotopes of flerovium (element Z=114). An upgraded TASISpec decay station was placed behind the gas-filled separator TASCA at the GSI Helmholtzzentrum fur Schwerionenforschung in Darmstadt, Germany. The fusion-evaporation reactions ^{48}Ca+^{242}Pu and ^{48}Ca+^{244}Pu provided a total of 32 flerovium-candidate decay chains, of which two and eleven were firmly assigned to ^{286}Fl and ^{288}Fl, respectively. A prompt coincidence between a 9.60(1)-MeV α particle event and a 0.36(1)-MeV conversion electron marked the first observation of an excited state in an even-even isotope of the heaviest man-made elements, namely ^{282}Cn. Spectroscopy of ^{288}Fl decay chains fixed Q_{α}=10.06(1) MeV. In one case, a Q_{α}=9.46(1)-MeV decay from ^{284}Cn into ^{280}Ds was observed, with ^{280}Ds fissioning after only 518 μs. The impact of these findings, aggregated with existing data on decay chains of ^{286,288}Fl, on the size of an anticipated shell gap at proton number Z=114 is discussed in light of predictions from two beyond-mean-field calculations, which take into account triaxial deformation.

A search for production of the superheavy elements with atomic numbers 119 and 120 was performed in the 50Ti+249Bk and 50Ti+249Cf fusion-evaporation reactions, respectively, at the gas-filled recoil separator TASCA at GSI Darmstadt, Germany. Over four months of irradiation, the 249Bk target partially decayed into 249Cf, which allowed for a simultaneous search for both elements. Neither was detected at cross-section sensitivity levels of 65 and 200 fb for the 50Ti+249Bk and 50Ti+249Cf reactions, respectively, at a midtarget beam energy of Elab=281.5 MeV. The nonobservation of elements 119 and 120 is discussed within the concept of fusion-evaporation reactions including various theoretical predictions on the fission-barrier heights of superheavy nuclei in the region of the island of stability. peerReviewed

The electron-capture decay followed by a prompt fission process was searched for in the hitherto unknown most neutron-deficient Md isotope with mass number 244. Alpha decay with $\ensuremath{\alpha}$-particle energies of 8.73--8.86 MeV and with a half-life of ${0.30}_{\ensuremath{-}0.09}^{+0.19}\text{ }\text{ }\mathrm{s}$ was assigned to $^{244}\mathrm{Md}$. No fission event with a similar half-life potentially originating from spontaneous fissioning of the short-lived electron-capture decay daughter $^{244}\mathrm{Fm}$ was observed, which results in an upper limit of 0.14 for the electron-capture branching of $^{244}\mathrm{Md}$. Two groups of fission events with half-lives of ${0.9}_{\ensuremath{-}0.3}^{+0.6}\text{ }\text{ }\mathrm{ms}$ and ${5}_{\ensuremath{-}2}^{+3}\text{ }\text{ }\mathrm{ms}$ were observed. The ${0.9}_{\ensuremath{-}0.3}^{+0.6}\text{ }\text{ }\mathrm{ms}$ activity was assigned to originate from the decay of $^{245}\mathrm{Md}$. The origin of eight fission events resulting in a half-life of ${5}_{\ensuremath{-}2}^{+3}\text{ }\text{ }\mathrm{ms}$ could not be unambiguously identified within the present data while the possible explanation has to invoke previously unseen physics cases.

An upgraded TASISpec setup, with the addition of a veto DSSD and the new Compex detector-germanium array, has been employed with the gas-filled recoil separator TASCA at the GSI Helmholtzzentrum für Schwerionenforschung Darmstadt, to study flerovium (element 114) decay chains. The detector upgrades along with development of new analytical techniques have improved the sensitivity of the TASISpec setup for measuring α-photon coincidences. These improvements have been assessed with test reactions. The reaction 48Ca+206,207Pb was used for verification of experimental parameters such as transmission to implantation DSSD and target-segment to α-decay correlations. The reaction 48Ca+ nat Hf was used to produce several short-lived nuclei with multiple-α decay chains to investigate pile-up event deconvolution.

The electron-capture decay followed by a prompt fission process was searched for in the hitherto unknown most neutron-deficient Md isotope with mass number 244. Alpha decay with α-particle energies of 8.73-8.86 MeV and with a half-life of 0.30_{-0.09}^{+0.19} s was assigned to ^{244}Md. No fission event with a similar half-life potentially originating from spontaneous fissioning of the short-lived electron-capture decay daughter ^{244}Fm was observed, which results in an upper limit of 0.14 for the electron-capture branching of ^{244}Md. Two groups of fission events with half-lives of 0.9_{-0.3}^{+0.6} ms and 5_{-2}^{+3} ms were observed. The 0.9_{-0.3}^{+0.6} ms activity was assigned to originate from the decay of ^{245}Md. The origin of eight fission events resulting in a half-life of 5_{-2}^{+3} ms could not be unambiguously identified within the present data while the possible explanation has to invoke previously unseen physics cases.

This review describes some key accomplishments of Günter Herrmann such as the establishment of the TRIGA Mark II research reactor at Mainz University, the identification of a large number of very neutron-rich fission products by fast, automated chemical separations, the study of their nuclear structure by spectroscopy with modern detection techniques, and the measurement of fission yields. After getting the nuclear chemistry group, the target laboratory, and the mass separator group established at the Gesellschaft für Schwerionenforschung (GSI) in Darmstadt, a number of large international collaborations were organized exploring the mechanism of deeply inelastic multi-nucleon transfer reactions in collisions of Xe and U ions with U targets, Ca and U ions with Cm targets, and the search for superheavy elements with chemical separations after these bombardments. After the Chernobyl accident, together with members of the Institute of Physics, a powerful laser technique, the resonance ionization mass spectometry (RIMS) was established for the ultra-trace detection of actinides and long-lived fission products in environmental samples. RIMS was also applied to determine with high precision the first ionization potentials of actinides all the way up to einsteinium. In the late 1980ies, high interest arose in results obtained in fusion-evaporation reactions between light projectiles and heavy actinide targets investigating the chemical properties of transactinide elements (Z≥104). Remarkable was the observation, that their chemical properties deviated from those of their lighter homologs in the Periodic Table because their valence electrons are increasingly influenced by relativistic effects. These chemical results could be reproduced with relativistic quantum-chemical calculations. The present review is selecting and describing examples for fast chemical separations that were successful at the TRIGA Mainz and heavy-ion reaction studies at GSI Darmstadt.

The isotopic distribution of nuclei produced in the 50Ti + 249Cf reaction has been studied at the gas-filled recoil separator TASCA at GSI Darmstadt, which separates ions according to differences in magnetic rigidity. The bombardment was performed at an energy around the Bass barrier and with the TASCA magnetic fields set for collecting fusion-evaporation reaction products. Fifty-three isotopes located “north-east” of 208Pb were identified as recoiling products formed in non-fusion channels of the reaction. These recoils were implanted with energies in two distinct ranges; besides one with higher energy, a significant low-energy contribution was identified. The latter observation was not expected to occur according to kinematics of the known types of reactions, namely quasi-elastic, multi-nucleon transfer, deep-inelastic collisions or quasifission. The present observations are discussed within the framework of two-body kinematics passing through the formation of a composite system.

The kinematics of multi-nucleon transfer reactions in 48Ca + 248Cm collisions at 262 MeV (center of target) was investigated by using a stacked-foil technique and radiochemical separations of trans-curium elements. Trans-curium isotopes were identified by α-particle spectroscopy. For Fm isotopes, by comparing the centroids of the measured post-neutron emission isotope distributions with the most probable primary mass number predicted by Volkov's generalized Q g g systematics, the missing mass (number of evaporated neutrons) is estimated. The latter is compared with that deduced from the measured centroid of the laboratory angular distribution peaked closely to the grazing angle and the centroid of the range distribution, being used to determine the average total kinetic energy loss (TKEL) and the average excitation energy. The latter agrees within the uncertainties with the missing mass so that a consistent picture of the reaction mechanism emerges. For products closer to the target Z, e.g., Cf and Bk, the distributions of kinetic energies are much broader than for Fm, reflecting the fact that in the former, values of TKEL reach from quasi-elastic scattering all the way to deep inelastic scattering. The measured laboratory angular distribution and the average laboratory kinetic energy of the Fm isotopes, being the prototypes for multi-nucleon transfer products, are benchmark values for the design of electromagnetic separators to be constructed for the separation and detection of unknown neutron-rich transactinides produced in this nuclear reaction type.

The heaviest currently known nuclei, which have up to 118 protons, have been produced in 48Ca induced reactions with actinide targets. Among them, the element tennessine (Ts), which has 117 protons, has been synthesized by fusing 48Ca with the radioactive target 249Bk, which has a half-life of 327 d. The experiment was performed at the gas-filled recoil separator TASCA. Two long and two short α decay chains were observed. The long chains were attributed to the decay of 294Ts. The possible origin of the short-decay chains is discussed in comparison with the known experimental data. They are found to fit with the decay chain patterns attributed to 293Ts. The present experimental results confirm the previous findings at the Dubna Gas-Filled Recoil Separator on the decay chains originating from the nuclei assigned to Ts.

Physics letters 760, 293-296(2016). doi:10.1016/j.physletb.2016.07.008, Published by North-Holland Publ., Amsterdam

Products of the fusion-evaporation reaction 48Ca + 243Am were studied with the TASISpec set-up at the gas-filled separator TASCA at the GSI Helmholtzzentrum für Schwerionenforschung, Darmstadt, Germany. Amongst the detected thirty correlated α-decay chains associated with the production of element Z=115, two recoil-α-fission and five recoil-α-α-fission events were observed. The latter five chains are similar to four such events reported from experiments performed at the Dubna gas-filled separator, and three such events reported from an experiment at the Berkeley gas-filled separator. The four chains observed at the Dubna gas-filled separator were assigned to start from the 2n-evaporation channel 289115 due to the fact that these recoil-α-α-fission events were observed only at low excitation energies. Contrary to this interpretation, we suggest that some of these recoil-α-α-fission decay chains, as well as some of the recoil-α-α-fission and recoil-α-fission decay chains reported from Berkeley and in this article, start from the 3n-evaporation channel 288115.

In Section 1 we will discuss multi-nucleon transfer reactions with light heavy ions, which can be thought of as competing with complete fusion at higher impact parameters. Quasi-elastic and multi-nucleon transfer reactions with the heaviest projectiles will be discussed in Section 2 . In Section 3 we will cover recent developments focusing on theoretical predictions of cross sections of superheavy nuclei, cover some new possibilities and look into the existing experimental challenges.

Short-lived α-decaying nuclei "northeast" of 208Pb in the chart of nuclides were studied using the reaction 48Ca+243Am with the decay station TASISpec at TASCA, GSI Darmstadt. Decay energies and times from pile-up events were extracted with a tailor-made pulse-shape analysis routine and specific α-decay chains were identified in a correlation analysis. Decay chains starting with the even-even 220Ra and its odd-A neighbors, 219Fr, and 219,221Ra, with a focus on the 219Ra→215Rn decay, were studied by means of α-γ spectroscopy. A revised α-decay scheme of 219Ra is proposed, including a new decay branch from a previously not considered isomeric state at 17 keV excitation energy. Conclusions on nuclear structure are drawn from the experimental data, aided by Geant4 simulations and a discussion on theoretical calculations. (Less)

8 pags., 10 figs., 3 tabs., The Borromean drip-line nucleus Ne-17 has been suggested to possess a two-proton halo structure in its ground state. In the astrophysical rp-process, where the two-proton capture reaction O-15(2p,gamma) Ne-17 plays an important role, the calculated reaction rate differs by several orders of magnitude between different theoretical approaches. To add to the understanding of the Ne-17 structure we have studied nuclear and electromagnetic dissociation. A 500 MeV/u Ne-17 beam was directed toward lead, carbon, and polyethylene targets. Oxygen isotopes in the final state were measured in coincidence with one or two protons. Different reaction branches in the dissociation of Ne-17 were disentangled. The relative populations of s and d states in F-16 were determined for light and heavy targets. The differential cross section for electromagnetic dissociation (EMD) shows a continuous internal energy spectrum in the three-body system O-15 + 2p. The Ne-17 EMD data were compared to current theoretical models. None of them, however, yields satisfactory agreement with the experimental data presented here. These new data may facilitate future development of adequate models for description of the fragmentation process., This project is supported by NAVI, GSI-TU Darmstadt cooperation, HIC for FAIR, EMMI, and BMBF and from DFG through Grant No. SFB1245 and from BMBF via Project No. 05P15RDFN1, and from the Spanish Ministry by research grant FPA2015-64969-P. C.A.B. acknowledges support by the US DOE Grant No. DE-FG02-08ER41533 and the US NSF Grant No. 1415656.

Here we present a nuclear forensic study of uranium from German nuclear projects which used different geometries of metallic uranium fuel. Through measurement of the (230)Th/(234)U ratio, we could determine that the material had been produced in the period from 1940 to 1943. To determine the geographical origin of the uranium, the rare-earth-element content and the (87)Sr/(86)Sr ratio were measured. The results provide evidence that the uranium was mined in the Czech Republic. Trace amounts of (236)U and (239)Pu were detected at the level of their natural abundance, which indicates that the uranium fuel was not exposed to any major neutron fluence.

Wir berichten hier uber eine nuklearforensische Analyse verschiedener Uranmaterialien aus deutschen Nuklearprojekten der 1940er Jahre, bei denen Uranmetall in verschiedenen Geometrien verwendet wurde. Mithilfe des 230Th/234U-Isotopenverhaltnisses konnte fur das Metall ein Produktionszeitraum von 1940 bis 1943 bestimmt werden. Die geographische Herkunft des Urans wurde anhand des Spurengehalts an Seltenerdelementen und der Strontium-Isotopenverhaltnisse bestimmt. Die Ergebnisse zeigen, dass das bei den deutschen Nuklearprojekten verwendete Uran aus Minen in der Tschechischen Republik stammt. 236U und 239Pu wurden in Spuren nachgewiesen. Diese entsprechen in etwa der Haufigkeit dieser Isotope in Uranerzen, woraus sich ableiten lasst, dass die untersuchten Uranmetalle keinem signifikanten Neutronenfluss ausgesetzt waren.

A new technique for continuous dissolution of nuclear reaction products transported by a gas-jet system was developed for superheavy element (SHE) chemistry. In this technique, a hydrophobic membrane is utilized to separate an aqueous phase from the gas phase. With this technique, the dissolution efficiencies of short-lived radionuclides of 91m,93mMo and 176W were measured. Yields of more than 80 % were observed for short-lived radionuclides at aqueous-phase flow rates of 0.1–0.4 mL/s. The gas flow-rate had no influence on the dissolution efficiency within the studied flow range of 1.0–2.0 L/min. These results show that this technique is applicable for on-line chemical studies of SHEs in the liquid phase.

The extraction and reduction behavior of Mo and W, lighter homologs of Sg, was studied in continuous on-line experiments at the JAEA tandem accelerator to develop a new chemistry assembly consisting of a membrane degasser (MDG), a flow electrolytic column (FEC), and the continuous liquid–liquid extraction apparatus (SISAK). Extraction yields of Mo and W from 0.1 M HCl/0.9 M LiCl into 4-isopropyltropolone (hinokitiol, HT) in toluene were investigated. In the reduction experiment, Mo(VI) was successfully reduced to a lower oxidation state while W(VI) showed no reduction under the given conditions.

Radioisotope mass spectrometry for the determination of long-lived nuclides can be several orders of magnitude more sensitive than the conventional radiometric methods. The principle of RIMS consists of the vaporization of the radionuclide to be determined and to perform a multiple resonant excitation and ionization of the atoms by laser light. This is followed by mass selective detection of the ions by a time-of-flight mass spectrometer. Several applications are presented.

Continuous liquid–liquid extraction of short-lived radionuclides has traditionally been performed with the SISAK system consisting of static mixers and H-centrifuges for phase separation. SISAK operates at flow rates of typically 1 mL/s. Thus, it produces large volumes of radioactive liquid waste that is difficult to dispose of. Therefore, it has been aimed to develop and use a further miniaturised extraction unit based on microtechnology and precision engineering to reduce the flow rate by at least two orders of magnitude. The accordingly developed MicroSISAK device is a micro membrane extractor in which a micromixer element with 2 × 16 feed channels of 30 µm width followed by a 60 µm high mixing chamber is used for intimately contacting the aqueous and organic phase. Subsequent phase separation is achieved via hydrophobic Teflon membranes with a pore size of 1 µm. The MicroSISAK device has been tested and optimized with radiotracers of the group-4 elements Zr and Hf in the system H2SO4/trioctyl amine (TOA) in toluene. At a temperature of 58°C and a flow rate of 0.2 mL/min of both phases, extraction yields of 87 ± 3% were achieved. The transport time from the micromixer to the first Teflon membrane was in this case 3.9 s. It can be shortened to 1.56 s at a flow rate of 0.5 mL/min. Under similar conditions, the extraction yield of 99m Tc milked from a 99Mo generator in the system HNO3/tetraphenyl arsonium chloride (TPAC) in chloroform was 83 ± 3%. In an on-line experiment at the TRIGA Mainz reactor, short-lived Tc isotopes produced in the fission of 235U with thermal neutrons were transported by a He/KCl gas-jet to the chemistry apparatus, deposited by impaction, dissolved in 0.01 mol/L HNO3/KBrO3, and extracted into 10−4 mol/L TPAC in chloroform in MicroSISAK. The separated phases were transported via capillaries to two separate flow-through cells positioned in front of two Ge detectors. The extraction yield determined as the ratio of the Tc γ-ray activities in both detectors was 76 ± 1%. With this experiment, it was demonstrated that MicroSISAK is in principle ready for an on-line experiment for the chemical characterization of the superheavy element bohrium, element 107. However, the detection of α-particle activities by liquid scintillation counting still needs to be worked out.

The heaviest elements are synthesized in heavy-ion induced hot fusion reactions with various actinide targets. Because the actinide material is often available only in very limited amounts, a deposition method with high yields (~90 %) is needed. We report on the production of 244Pu, 243Am, 248Cm, 249Bk, and 249Cf targets on thin Ti backings by molecular plating. Different chemical purification steps using ion chromatographic techniques were applied for the purification of 249Cf and 244Pu. The deposition procedure applied for the production of ~0.4–0.8 mg/cm2 thick targets is described. The deposition yield was determined either by α-particle or γ-ray spectroscopy. Furthermore, neutron activation analysis has been applied in the case of 244Pu, 243Am, and 248Cm. Information about the spatial distribution and homogeneity of the target layer was obtained by radiographic imaging.

Chemical studies of superheavy elements require fast and efficient techniques, due to short half-lives and low production rates of the investigated nuclides. Here, we advocate for using a tubular flow reactor for assessing the thermal stability of the Sg carbonyl complex – Sg(CO)6. The experimental setup was tested with Mo and W carbonyl complexes, as their properties are established and supported by theoretical predictions. The suggested approach proved to be effective in discriminating between the thermal stabilities of Mo(CO)6 and W(CO)6. Therefore, an experimental verification of the predicted Sg–CO bond dissociation energy seems to be feasible by applying this technique. By investigating the effect of 104,105Mo beta-decay on the formation of 104,105Tc carbonyl complex, we estimated the lower reaction time limit for the metal carbonyl synthesis in the gas phase to be more than 100 ms. We examined further the influence of the wall material of the recoil chamber, the carrier gas composition, the gas flow rate, and the pressure on the production yield of 104Mo(CO)6, so that the future stability tests with Sg(CO)6 can be optimized accordingly.

The unique role of the heaviest elements in chemical and physical sciences is discussed. With the actinide series (Z = 90-103) and the superactinide series (Z = 122-155), the heaviest elements have significantly shaped the architecture of the Periodic Table of the elements. Relativistic effects in the electron shells of the heaviest elements change the chemical properties in a given group in a non-linear fashion. Relativistically stabilized sub-shell closures give rise to a new category of elements in the Periodic Table: volatile metals. The prototype for this property is element 114 which, due to the relativistic stabilization of its 7s2 7p2 1/2 electron configuration, is volatile in its elementary state, but, in contrast to a noble gas, exhibits a marked metalmetal interaction with a gold surface at room temperature. Nuclear shell effects dominate the physical properties of the transuranium elements. These give rise to superdeformed shape isomers (fission isomers) in the actinides (U-Bk). Superheavy elements (Z ≥ 104) owe their existence solely to nuclear shell effects at N = 152, 162, and 184. At this time, a building lot is the location of the next spherical proton shell closure as there is evidence that the center of the “island of stability” is not at Z = 114. This needs urgently further theoretical and experimental efforts. The cross sections for the syntheses of elements 119 and 120 will give us important information on the “upper end of the Periodic Table of the elements”.

The sorption of Np(V) onto hybrid clay-based materials (HCMs) prepared from montmorillonite in the Maillard reaction was studied at environmentally relevant concentrations. Above pH 7, the sorption of Np(V) on HCM is weaker than that on the pure montmorillonite, with a reversed trend observed at lower pH values. With increasing pH, increasing amounts of melanoidins are released into the aqueous phase, thus the complexation of Np(V) in the aqueous phase was studied as well. The complexation in the aqueous phase is obviously increasing the mobility of Np(V). The sorption of Np(V) on the HCM is compared to the prediction by the linear additive model.

The average charge states of Pb-188 and No-252,No-254 ions in dilute helium gas were measured at the gas-filled recoil separator TASCA. Hydrogen gas was also used as a filling gas for measurements of the average charge state of No-254. Helium and hydrogen gases at pressures from 0.2 mbar to 2.0 mbar were used. A strong dependence of the average charge state on the pressure of the filling gases was observed for both, helium and hydrogen. The influence of this dependence, classically attributed to the so-called "density effect", on the performance of TASCA was investigated. The average charge states of No-254 ions were also measured in mixtures of helium and hydrogen gases at low gas pressures around 1.0 mbar. From the experimental results simple expressions for the prediction of average charge states of heavy ions moving in rarefied helium gas, hydrogen gas, and in their mixture were derived. (C) 2012 Elsevier B.V. All rights reserved.

Two short-lived isotopes ^{221}U and ^{222}U were produced as evaporation residues in the fusion reaction ^{50}Ti+^{176}Yb at the gas-filled recoil separator TASCA. An α decay with an energy of E_{α}=9.31(5) MeV and half-life T_{1/2}=4.7(7) μs was attributed to ^{222}U. The new isotope ^{221}U was identified in α-decay chains starting with E_{α}=9.71(5) MeV and T_{1/2}=0.66(14) μs leading to known daughters. Synthesis and detection of these unstable heavy nuclei and their descendants were achieved thanks to a fast data readout system. The evolution of the N=126 shell closure and its influence on the stability of uranium isotopes are discussed within the framework of α-decay reduced width.

Standard wafer solar cells are made of near-semiconductor quality silicon. This high quality material makes up a significant part of the total costs of a solar module. Therefore, new concepts with less expensive so called solar grade silicon directly based on physiochemically upgraded metallurgical grade silicon are investigated. Metallurgical grade silicon contains large amounts of impurities, mainly transition metals like Fe, Cr, Mn, and Co, which degrade the minority carrier lifetime and thus the solar cell efficiency. A major reduction of the transition metal content occurs during the unidirectional crystallization due to the low segregation coefficient between the solid and liquid phase. A further reduction of the impurity level has to be done by gettering procedures applied to the silicon wafers. The efficiency of such cleaning procedures of metallurgical grade silicon is studied by instrumental neutron activation analysis (INAA). Small sized silicon wafers of app roximately 200. mg with and without gettering step were analyzed. To accelerate the detection of transition metals in a crystallized silicon ingot, experiments of scanning whole vertical silicon columns with a diameter of approximately 1. cm by gamma spectroscopy were carried out. It was demonstrated that impurity profiles can be obtained in a comparably short time. Relatively constant transition metal ratios were found throughout an entire silicon ingot. This led to the conclusion that the determination of several metal profiles might be possible by the detection of only one "leading element". As the determination of Mn in silicon can be done quite fast compared to elements like Fe, Cr, and Co, it could be used as a rough marker for the overall metal concentration level. Thus, a fast way to determine impurities in photovoltaic silicon material is demonstrated.

Performing experiments with transactinide elements demands highly sensitive detection methods due to the extremely low production rates (one-atom-at-a-time conditions). Preseparation with a physical recoil separator is a powerful method to significantly reduce the background in experiments with sufficiently long-lived isotopes (t1/2≥0.5 s). In the last years, the new gas-filled TransActinide Separator and Chemistry Apparatus (TASCA) was installed and successfully commissioned at GSI. Here, we report on the design and performance of a Recoil Transfer Chamber (RTC) for TASCA—an interface to connect various chemistry and counting setups with the separator. Nuclear reaction products recoiling out of the target are separated according to their magnetic rigidity within TASCA, and the wanted products are guided to the focal plane of TASCA. In the focal plane, they pass a thin Mylar window that separates the ∼1 mbar atmosphere in TASCA from the RTC kept at ∼1 bar. The ions are stopped in the RTC and transported by a continuous gas flow from the RTC to the ancillary setup. In this paper, we report on measurements of the transportation yields under various conditions and on the first chemistry experiments at TASCA—an electrochemistry experiment with osmium and an ion exchange experiment with the transactinide element rutherfordium.

A carbonyl compound that tips the scales Life is short for the heaviest elements. They emerge from high-energy nuclear collisions with scant time for detection before they break up into lighter atoms. Even et al. report that even a few seconds is long enough for carbon to bond to the 106th element, seaborgium (see the Perspective by Loveland). The authors used a custom apparatus to direct the freshly made atoms out of the hot collision environment and through a stream of carbon monoxide and helium. They compared the detected products with theoretical modeling results and conclude that hexacarbonyl Sg(CO) 6 was the most likely structural formula. Science , this issue p. 1491 ; see also p. 1451

International audience; We describe the status of the new measurement of the neutron electric dipole moment (nEDM) to be performed at the strong source of ultra-cold neutrons at the Paul Scherrer Institut. The experimental technique is based on Ramsey's method of separated oscillatory fields, applied to UCN stored in vacuum in a chamber at room temperature. Our approach is performed in three phases: in phase one, new components have been developed and tested at the Institut Laue-Langevin. Phase two is being performed at PSI, where the apparatus was moved in 2009. Here, together with the optimization of the magnetic environment, the prospective UCN density of not, vert, similar 100 cm-3 should enable an improvement of the currently best limit by a factor of five within two years of data taking. In the third phase, a new spectrometer will then gain another order of magnitude in sensitivity. The improvements will be mainly due to (1) much higher UCN intensity, (2) improved magnetometry and magnetic field control, and (3) a double chamber configuration with opposite electric field directions.

The study of the interactions among metals, minerals, and humic substances is essential in understanding the migration of inorganic pollutants in the geosphere. A considerable amount of organic matter in the environment is associated with clay minerals. To understand the role of organic matter in the environment and its association with clay minerals, a hybrid clay-based material (HCM), montmorillonite (STx-1)-melanoidin, was prepared from L-tyrosine and L-glutamic acid by the Maillard reaction. The HCM was characterized by elemental analysis, nuclear magnetic resonance, x-ray photoelectron spectroscopy (XPS), scanning transmission x-ray microscopy (STXM), and thermal analysis. The presence of organic materials on the surface was confirmed by XPS and STXM. The STXM results showed the presence of organic spots on the surface of the STx-1 and the characterization of the functional groups present in those spots. Thermal analysis confirmed the existence of organic materials in the montmorillonite interlayer, indicating the formation of a composite of melanoidin and montmorillonite. The melanoidin appeared to be located partially between the layers of montmorillonite and partially at the surface, forming a structure that resembles the way a cork sits on the top of a champagne bottle.

It is of great interest to study chemical properties of the transactinide elements with atomic numbers (Z) ≥ 104. One of the most important subjects is to establish the position of the elements at the extreme end of the periodic table. To this end we perform studies of chemical properties of these transactinides and compare them with those of their lighter homologues and with the ones expected from extrapolations in the periodic table. So far, chromatographic studies of the transactinides have provided experimental proof of placing rutherfordium (Rf, Z = 104) through hassium (Hs, Z = 108) into groups 4 to 8, respectively. 1-10 Quite recently, copernicium (Cn, Z = 112) has been shown to be a member of group 12. 11 To gain a better understanding, it is even more interesting to study chemical properties of the transactinide elements in greater detail and to compare those with the ones of their lighter homologues. Theoretical calculations predict that the ground state electronic structure of the heaviest elements varies due to strong relativistic effects. Accordingly, chemical properties of these elements may deviate from those expected from linear extrapolations based on lighter homologues. 12-14 Systematically, detailed chemical investigations are, therefore, required to characterize properties of the transactinide elements influenced by relativistic effects.

International audience; The effort towards a new measurement of the neutron electric dipole moment (nEDM) at the Paul Scherrer Institut's (PSI) new high intensity source of ultracold neutrons (UCN) is described. The experimental technique relies on Ramsey's method of separated oscillatory fields, using UCN in vacuum with the apparatus at ambient temperature. In the first phase, R&D towards the upgrade of the RAL/Sussex/ILL apparatus is being performed at the Institut Laue-Langevin (ILL). In the second phase the apparatus, moved from ILL to PSI, will allow an improvement in experimental sensitivity by a factor of 5. In the third phase, a new spectrometer should gain another order of magnitude in sensitivity. The improvements will be mainly due to (1) much higher UCN intensity, (2) improved magnetometry and magnetic field control, and (3) a double chamber configuration with opposite electric field directions.

The unbound isotopes 10Li, 12Li and 13Li have been observed after nucleon-knockout reactions at relativistic energies with 11Li and 14Be beams impinging on a liquid hydrogen target. The channels , and were analysed in the ALADIN-LAND setup at GSI. The 10Li data confirm earlier findings, while the 12Li and 13Li nuclei were observed for the first time. The relative-energy spectrum shows that the ground state of 12Li can be described as a virtual s-state with a scattering length of -13.7(1.6) fm. A broad energy spectrum was found for the channel. Based on the assumption that the relative-energy spectrum is dominated by a correlated background presumably stemming from initial correlations in the 14Be ground-state, evidence for a 13Li resonance at 1.47(31) MeV above the threshold with a width around 2 MeV has been found.

Lanthanide and actinide targets are prepared at the University of Mainz by molecular plating, an electrochemical deposition from an organic solvent, for heavy-ion reaction studies at GSI. To acquire information about deposition yield, target thickness, and target homogeneity, the following analysis methods are applied. With neutron activation analysis (NAA) the deposition yield and the average thickness of the deposited material is determined. We report on the analytical procedure of NAA performed subsequent to the molecular plating process. Scanning electron microscope (SEM) is used to determine the morphology of the target surfaces. In combination with energy dispersive X-ray spectrometer (EDS), we also could obtain qualitative information about the chemical form of the deposited material. So far, gadolinium, samarium, holmium, and uranium targets have been investigated with SEM/EDS. With radiographic imaging (RI), targets of uranium prepared by molecular plating and by vacuum vaporization are investigated. This method is suitable to obtain information about the spatial distribution, the homogeneity, and the thickness of the target layer deposition.

The Transactinide Separator and Chemistry Apparatus (TASCA) is a recoil separator with maximized transmission designed for performing advanced chemical studies as well as nuclear reaction and structure investigations of the transactinide elements ( Z >103) on a one-atom-at-a-time basis. TASCA will provide a very clean transactinide fraction with negligible contamination of lighter elements from nuclear side reactions in the target. For TASCA a new target chamber was designed and built at GSI including the rotating target wheel assembly ARTESIA for beam intensities up to 2 μA (particle). For the production of longer-lived isotopes of neutron-rich heavier actinide and transactinide elements, hot fusion reactions with actinide targets are required. Here, possible target materials range from thorium up to curium or even heavier elements. For the deposition of lanthanide and actinide elements on thin aluminum and titanium backings by means of Molecular Plating (MP), a new deposition cell has been constructed that allows precise temperature control of the organic solvent and stirring of the solution. The electrode geometry ensures homogeneity of the electric field inside the cell. With the new set-up, holmium and gadolinium layers (500 μg/cm 2 ) on 2–5 μm thin titanium backings have been produced with deposition yields of the order of 90%. Systematic investigations are under way to further optimize the deposition conditions for other lanthanide and actinide elements including uranium and plutonium on different backing materials.

The production rates of ultracold neutrons (UCN) with a solid deuterium converter have been measured at the pulsed reactor TRIGA Mainz. Exposed to a thermal neutron fluence of $\ensuremath \sim 1\cdot 10^{13}$ n·cm^-2·pulse^-1, the number of detected very cold and ultracold neutrons ranges up to 200 000 at 7mol of solid deuterium (sD2) in combination with a pre-moderator (mesitylene). About 50% of the measured neutrons can be assigned to UCN with energies E of $\ensuremath V_{\rm F}({\rm sD}_2)\leq E \leq V_{\rm F}{\rm (guide)}$ where V F(sD 2) = 105 neV and V F(guide) = 190 neV are the Fermi potentials of the sD2 converter and our stainless steel neutron guides, respectively. Thermal cycling of solid deuterium, which was frozen out from the gas phase, considerably improved the UCN yield, in particular at higher amounts of sD2.

The speciation of plutonium (Pu) in contact with humic substances (HS) and kaolinite has been performed in aquifer systems. Mainly the redox behavior, complexation, and sorption of plutonium are discussed here. The redox behavior of Pu(VI) in contact with HS was studied and it was found that Pu(VI) is reduced to Pu(III) and Pu(IV) within a couple of weeks. The complexation constants (log β LC ) of Pu(III) and Pu(IV) with HS have been determined by means of the ultrafiltration method. Furthermore, the sorption of Pu(III) and Pu(IV) onto kaolinite has been investigated as a function of pH by batch experiments under aerobic and anaerobic conditions.

The neutron-rich isotopes 129–133Sn were studied in a Coulomb excitation experiment at about 500 AMeV using the FRS-LAND setup at GSI. From the exclusive measurement of all projectile-like particles following the excitation and decay of the projectile in a high-Z target, the energy differential cross section can be extracted. At these beam energies dipole transitions are dominating, and within the semi-classical approach the Coulomb excitation cross sections can be transformed into photoabsorption cross sections. In contrast to stable Sn nuclei, a substantial fraction of dipole strength is observed at energies below the giant dipole resonance (GDR). For 130Sn and 132Sn this strength is located in a peak-like structure around 10 MeV excitation energy and exhibits a few percent of the Thomas-Reiche Kuhn (TRK) sum-rule strength. Several calculations predict the appearance of dipole strength at low excitation energies in neutron-rich nuclei. This low-lying strength is often referred to as pygmy dipole resonance (PDR) and, in a macroscopic picture, is discussed in terms of a collective oscillation of excess neutrons versus the core nucleons. Moreover, a sharp rise is observed at the neutron separation threshold around 5 MeV for the odd isotopes. A possible contribution of 'threshold strength', which can be described within the direct-breakup model is discussed. The results for the neutron-rich Sn isotopes are confronted with results on stable nuclei investigated in experiments using real photons.

Lawrencium, with atomic number 103, has an isotope with a half-life of 27 seconds; even so, its first ionization potential has now been measured on an atom-at-a-time scale and agrees well with state-of-the-art theoretical calculations that include relativistic effects. The most dramatic modern revision of Mendeleev's periodic table of elements came in 1944 when Glenn T. Seaborg placed a new series of elements, the actinides (atomic numbers 89–103), below the lanthanides. In this issue of Nature, Yuichiro Nagame and colleagues report the first measurement of one of the basic atomic properties of element 103 (lawrencium), namely its first ionization potential. Lawrencium is only accessible via atom-at-a-time synthesis in heavy-ion accelerators, so experimental investigations of its properties are rare. Nagame and colleagues were able to reduce the number of atoms required to measure the ionization potential from billions to thousands, and these results — in agreement with the latest theoretical calculations — show that the last valence electron in lawrencium is the most weakly bound one in all actinides and any other element beyond group 1 of the periodic table. This signature — in a region of the periodic table where the sheer size of the atoms means that relativistic effects play a crucial role — confirms the end of the actinide series at element 103. The chemical properties of an element are primarily governed by the configuration of electrons in the valence shell. Relativistic effects influence the electronic structure of heavy elements in the sixth row of the periodic table, and these effects increase dramatically in the seventh row—including the actinides—even affecting ground-state configurations1,2. Atomic s and p1/2 orbitals are stabilized by relativistic effects, whereas p3/2, d and f orbitals are destabilized, so that ground-state configurations of heavy elements may differ from those of lighter elements in the same group. The first ionization potential (IP1) is a measure of the energy required to remove one valence electron from a neutral atom, and is an atomic property that reflects the outermost electronic configuration. Precise and accurate experimental determination of IP1 gives information on the binding energy of valence electrons, and also, therefore, on the degree of relativistic stabilization. However, such measurements are hampered by the difficulty in obtaining the heaviest elements on scales of more than one atom at a time3,4,5. Here we report that the experimentally obtained IP1 of the heaviest actinide, lawrencium (Lr, atomic number 103), is electronvolts. The IP1 of Lr was measured with 256Lr (half-life 27 seconds) using an efficient surface ion-source and a radioisotope detection system coupled to a mass separator. The measured IP1 is in excellent agreement with the value of 4.963(15) electronvolts predicted here by state-of-the-art relativistic calculations. The present work provides a reliable benchmark for theoretical calculations and also opens the way for IP1 measurements of superheavy elements (that is, transactinides) on an atom-at-a-time scale.

J. Marganiec et al.; 9 pags.; 11 figs.; 2 tabs., © 2015, SIF, Springer-Verlag Berlin Heidelberg. Two-proton decay of the unbound Tz = -2 nucleus 16Ne , produced in one-neutron knockout from a 500 MeV/u 17Ne beam, has been studied at GSI. The ground state, at a resonance energy 1.388(15) MeV, (Γ = 0.082(15) MeV) above the 14O +p+p threshold, and two narrow resonances at Er = 3.220(46) MeV and 7.57(6) MeV have been investigated. A comparison of the energy difference between the first excited 2+ state and the 0+ ground state in 16Ne with its mirror nucleus 16C reveals a small Thomas-Ehrman shift (TES) of +70(46) keV. A trend of the TES for the T = 2 quintet is obtained by completing the known data with a prediction for 16F obtained from an IMME analysis. The decay mechanisms of the observed three resonances were revealed from an analysis of the energy and angular correlations of the 14O +p+p decay products. The ground state decay can be considered as a genuine three-body (democratic) mode and the excited states decay sequentially via states in the intermediate nucleus 15F , the 3.22 MeV state predominantly via the 15F ground-state resonance, while the 7.57 MeV state decays via the 5/2+ resonance in 15F at 2.8 MeV above the 14O +p+p threshold. Further, from an analysis of angular correlations, the spin-parity of the 7.57 MeV state has been determined as IП = 2+ and assigned as the third 2+ state in 16Ne based on a comparison with 16C., This work is partly supported by the Helmholtz International Center for FAIR within the framework of the LOEWE program launched by the State of Hesse, by the German Federal Ministry for Education and Research (BMBF), EU(EURONS), ExtreMe Matter Institute EMMI, GSI-TU Darmstadt cooperation, Nuclear Astrophysics Virtual Institutes NAVI. Financial support from the Swedish Research Council, the Spanish grants FPA-2010-17142, MICCIN FPA2009-14604-C02-01, FPA2012- 39404-C02-01and MINECO FPA 2012-32443 are also acknowledged. One of us (BJ) is a Helmholtz International Fellow

Summary Two experiments aiming at the chemical investigation of element 112 produced in the heavy ion induced nuclear fusion reaction of 48Ca with 238U were performed at the Gesellschaft für Schwerionenforschung (GSI), Darmstadt, Germany. Both experiments were designed to determine the adsorption enthalpy of element 112 on a gold surface using a thermochromatography setup. The temperature range covered in the thermochromatography experiments allowed the adsorption of Hg at about 35 °C and of Rn at about -180 °C. Reports from the Flerov Laboratory for Nuclear Reactions (FLNR), Dubna, Russia claim production of a 5-min spontaneous fission (SF) activity assigned to 283112 for the 238U(48Ca,3n) 283112 reaction. Hence, Experiment I was designed to detect spontaneously fissioning (SF) isotopes of element 112 with half-lives (t 1/2) longer than about 20 s. 11 high-energy events were detected. 7 events exhibit a deposition pattern resembling a chromatographic peak in the vicinity of Rn deposition. However, the energy of the events observed in Experiment I was lower than expected for a SF-decay of 283112. Therefore, these events could not be unambiguously attributed to the decay of 283112. In contradiction with earlier publications newer reports from FLNR Dubna claim that 283112 decays by α-particle emission (E α = 9.5 MeV) with t 1/2 = 4 s followed by a SF-decay of 279Ds (t 1/2 = 0.2 s). Therefore, Experiment II was designed to be sensitive to both claimed decay properties of 283112. However, during this experiment neither short α-SF correlations nor SF coincidences were detected. The conclusion is that 283112 was not unambiguously detected, neither in Experiment I nor in Experiment II.