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.

The European physical journal / D 76(10), 190 (2022). doi:10.1140/epjd/s10053-022-00510-7, Published by Springer, Heidelberg

A recent experimental campaign performed at the LOHENGRIN spectrometer at ILL aimed at measuring the independent fission yield of 136Cs in the 239Pu(nth,f) reaction. This nuclide can have an important contribution to the total dose rate coming from spent light water reactor UOX and MOX fuels. Moreover, its impact is of first order on the uncertainty of the total dose rate calculated in specific areas of Nuclear Power Plants within accidental conditions. One of the most important sources of uncertainty is its independent fission yield. Therefore, a new measurement of its independent yield along with a rigorous uncertainty analysis was performed. Due to its low independent yield, a new measurement technique has been applied. Ions recoiling from neutron-irradiated 239Pu target were collected by implantation into an Al foil placed inside a vacuum chamber. This foil was then transferred to a low γ-ray background setup located at nearby laboratory (LPSC). The procedure was then repeated for different LOHENGRIN settings. Compared to the JEFF-3.1.1 library, a decrease of the fission yield of 136Cs with a reduced uncertainty is obtained.

Online gas-solid adsorption studies with single atom quantities of Hg, Tl, and Pb on SiO$_{2}$ and Au surfaces were carried out using short-lived radioisotopes with half-lives in the range of 4-49 s. This is a model study to measure adsorption enthalpies of superheavy elements Cn, Nh, and Fl. The short-lived isotopes were produced and separated by the gas-filled recoil separator TASCA at GSI. The products were stopped in He gas, and flushed into gas chromatography columns made of Si detectors whose surfaces were covered by SiO$_{2}$ or Au. The short-lived Tl and Pb were successfully measured by the Si detectors with the SiO$_{2}$ surface at room temperature. On the other hand, the Hg did not adsorb on the SiO$_{2}$ surface, but adsorbed on the Au surface. The results demonstrated that the adsorption properties of short-lived Hg, Tl, and Pb could be studied with this setup, and that this method is applicable to the experiment for Cn, Nh, and Fl., 半減期4$\sim$49秒の短寿命同位体を用いて、水銀(Hg), タリウム(Tl), 鉛(Pb)の単一原子レベルでのSiO$_{2}$及びAu表面への固体吸着挙動をオンライン気相実験により調べた。超重元素Cn, Nh, Flの吸着エンタルピー測定のためのモデル実験として実施した。短寿命同位体はドイツ重イオン研究所の反跳核分離装置TASCAを用いて生成・分離した。生成核はヘリウムガス中に捕集された後、SiO$_{2}$あるいはAuで表面を覆われたSi検出器で作製されたガスクロマトグラフィーカラムへと導入した。短寿命Tl及びPb同位体は室温においてSiO$_{2}$表面に吸着し、Si検出器で測定することに成功した。一方、HgはSiO$_{2}$表面には吸着せず、Au表面に吸着した。この結果より、本実験のセットアップを用いることで短寿命Hg, Tl, Pb同位体の吸着特性を調べることができると証明され、この手法がCn, Nh, Flの実験にも適用できることが確認された。

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.

Physics letters / B 820, 136601 (2021). doi:10.1016/j.physletb.2021.136601, Published by North-Holland Publ., Amsterdam

We present a measurement of the low-energy (0-60 keV) γ-ray spectrum produced in the α decay of ^{233}U using a dedicated cryogenic magnetic microcalorimeter. The energy resolution of ∼10 eV, together with exceptional gain linearity, allows us to determine the energy of the low-lying isomeric state in ^{229}Th using four complementary evaluation schemes. The most precise scheme determines the ^{229}Th isomer energy to be 8.10(17) eV, corresponding to 153.1(32) nm, superseding in precision previous values based on γ spectroscopy, and agreeing with a recent measurement based on internal conversion electrons. We also measure branching ratios of the relevant excited states to be b_{29}=9.3(6)% and b_{42}

Hyperfine interactions 241(1), 45 (2020). doi:10.1007/s10751-020-01712-4, Published by Springer Science + Business Media B.V, Dordrecht [u.a.]

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.

A novel target preparation method based on Drop-on-Demand (DoD) inkjet printing has been developed. Conventional preparation methods like the electrochemical method “Molecular Plating” or the “Polymer-Assisted Deposition Method” are often limited, e.g., concerning the dimensions and geometries of depositions or by the requirement for electrically conducting substrates. Here, we report on the development of a new technique, which overcomes such limits by using a commercially available DoD dispenser. A variety of solutions with volumes down to 5 nL can be dispensed onto every manageable substrate. The dispensed volumes were determined with a radioactive tracer and the deposits of evaporated salt solutions were investigated on titanium and graphene foils. Additionally, the high precision of the printing system with which individual drops can be positioned was used to determine the spatial resolution of storage phosphor imaging plates with three tracers of different β -decay energies. The new technique is able to produce new kinds of targets with improved spatial geometries and thin layer deposits.

This work shows the ability of resonance ionization mass spectrometry (RIMS) to determine 99gTc at the ultratrace level. The characterization of the prepared samples by X-ray photoelectron spectroscopy (XPS) and optimization of the RIMS setup for this purpose, as well as the application of the RIMS method to a soil sample, are presented in this article. 97Tc was used as a tracer isotope to determine the amount of 99gTc in a soil sample with RIMS. With 8.8 × 1010 atoms of 97Tc as the tracer, the concentration of 99gTc was found to be 1.5 × 109 atoms per gram of dried sample material, demonstrating the sensitivity of the method. Furthermore, it could be shown that the 97Tc solution contained 98Tc as well. This is the first time that 97,98,99gTc have been simultaneously measured with RIMS.

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 fast-neutron-induced fission cross section of $^{242}\mathrm{Pu}$ was measured at the neutron time-of-flight facility $n$ELBE. A parallel-plate fission ionization chamber with novel, homogeneous, large-area $^{242}\mathrm{Pu}$ deposits on Si-wafer backings was used to determine this quantity relative to the IAEA neutron cross-section standard $^{235}\mathrm{U}(n,f)$ in the energy range of 0.5 to 10 MeV. The number of target nuclei was determined from the measured spontaneous fission rate of $^{242}\mathrm{Pu}$. This helps to reduce the influence of the fission fragment detection efficiency on the cross section. Neutron transport simulations performed with geant4, mcnp6, and fluka2011 are used to correct the cross-section data for neutron scattering. In the reported energy range the systematic uncertainty is below 2.7% and on average the statistical uncertainty is 4.9%. The determined results show an agreement within 0.67(16)% to recently published data and a good accordance to current evaluated data sets.

The measurement of neutron induced reactions on unstable isotopes is of interest in many fields, from nuclear energy to astrophysics or applications; in particular transuranic isotopes are essential for the development of innovative nuclear reactors and for the management of the radioactive waste. In such measurements, the quality of the associated radioactive target is crucial for the success of the experiment, but in many cases the geometry, amount of mass and encapsulation of the target are not optimal, leading to limited results. In this work we propose to produce high quality radioactive targets for capture as a stack of thin targets using the techniques usually employed for fission measurements. In particular, we have succeeded in making a 242Pu target of nearly 100 mg by combining seven thin (1 mg/cm2) fission-like targets with 45 mm in diameter achieving a total backing thickness of only of aluminum. The target has been shown to perform successfully in experiments at both a neutron time-of-flight facility (n_TOF at CERN) and a thermal neutron beam (BRR at KFKI), providing the most accurate data from thermal up to 500 keV to date., This measurement has received funding from the EC FP7 Programme under the projects NEUTANDALUS (Grant No. 334315) and CHANDA (Grant No. 605203), the Spanish Ministry of Economy and Competitiveness projects FPA2014-53290-C2-2-P and FPA2016-77689-C2-1-R and the V Plan Propio de Investigación from the University of Seville .

A good knowledge of the radiative capture cross section of 242Pu is required for innovative nuclear reactor studies, especially for MoX fuel reactors. However, the experimental data available show discrepancies in the energy regions of interest: the thermal point and the keV region. Previous experimental results of the thermal cross section deviate from each other by 20% and these discrepancies are reflected also in the evaluated libraries, each of them giving more credit to different data sets. A recent measurement by Genreith et al. did not succeed to solve the existing discrepancy due to the large uncertainties and correction factors in the analysis. This work presents a new measurement of the thermal capture cross section of 242Pu carried out in the Budapest Research Reactor using the same thin targets of a previous measurement at n_TOF-EAR1, each containing 30mg of 99.995% pure 242Pu . The combined analysis of the full prompt γ -ray spectrum and the 243Pu decay has led to three compatible values for the thermal cross section. Their average value, 18.9(9)b, has an improved accuracy compared to recent measurements. Leaving aside the activation value of Genreith using an outdated intensity value for the 84 keV decay line of 243Pu , our average result is in very good agreement with the JEFF-3.2 evaluation and all the previous measurements, with the exception of the highest value 22.5(11)b reported by Marie et al., which has a strong influence in the ENDF evaluation., This measurement has received funding from the EC FP7 Programme under the projects NEUTANDALUS (Grant No. 334315) and the Transnational Access Activities Programme of CHANDA (Grant No. 605203), the Spanish Ministry of Economy and Competitiveness projects FPA2014-53290-C2-2-P and FPA2016-77689-C2-1-R and the V Plan Propio de Investigación Programme from the University of Sevilla. Support from the German Federal Ministry for Education and Research (BMBF), contract number 03NUK13A, is gratefully acknowledged

To study the chemical properties of the heaviest elements, a fast and efficient stopping and extraction of the highly energetic residues from heavy ion fusion reactions into the chemistry setup is essential. Currently used techniques like Recoil Transfer Chambers (RTC) relying on gas flow extraction provide high efficiencies for chemically non-reactive volatile species, but operate at extraction times t extr of about 0.5 s or more. Buffer Gas Cells (BGC) with electric and Radio-Frequency (RF) fields offer much faster extraction times. Here, we demonstrate the successful coupling of a BGC to a gas chromatography setup as is used for studies of chemical properties of superheavy elements. Using 223Ra and 225Ac recoil ion sources providing 219Rn and 221Fr ions for off-line tests, an extraction time t extr = 55(4) ms and an extraction efficiency of 35(3)% were achieved for the non-reactive 219Rn, while 221Fr was retained. The results show a BGC-based setup to be suitable for gas-phase experiments with short-lived volatile transactinide elements like Cn and Fl with half-lives substantially below 1 s.

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.

The aqueous chemistry of Np(V) in alkaline 0.01 to 5.5 M CaCl2 solutions at T = 23 ± 2 ℃ was thoroughly studied by long-term batch solubility experiments from both over- and undersaturation. Applying a comprehensive set of experimental and spectroscopic techniques including Vis/NIR and Np L3-edge EXAFS, the solubility controlling Np(V) solid phases and the predominant aqueous Np(V) species were identified. The results demonstrate that the solubility behavior of Np(V) in alkaline CaCl2 solutions differs completely from the one reported for alkaline NaCl and NaClO4 solutions: as solubility limiting solid phases, three so far not considered Ca-Np(V)-OH compounds were identified and their solubility and stability in CaCl2 solutions analyzed: CaNpO2(OH)2.6Cl0.4 · 2H2O(s) (I) (metastable), Ca0.5NpO2(OH)2 · 1.3H2O(s) (II) (long-term metastable) and Ca0.5NpO2(OH)2(s) (III) (stable). The considerably higher stability of these (qua)ternary phases which readily form in alkaline CaCl2 solutions from oversaturation (addition of NpO2 +) and undersaturation (addition of binary NpO2OH(am)) limit the Np(V) equilibrium concentrations to values that are up to 3 log-units lower compared to those for NpO2OH(am) in NaCl and NaClO4 systems. Based on systematic evaluation of the pH dependence (solubility curve slopes), Vis/NIR and EXAFS spectroscopic information, unhydrolysed NpO2 + and innersphere chloro complexes, NpO2Cl(aq) and Ca z [NpO2Cl]2z+ with z = 1 (EXAFS, Vis/NIR), were identified as prevailing Np(V) species in less alkaline solutions with pHm 2] ≤ 2.0 M and [CaCl2] > 2.0 M, respectively. The steep increase of the Np(V) solubility for pHm > 11 with slopes of approximately + 2.5 (for solid phase (I)) and + 3 (for solids (II) and (III)) as well as the Np L3-edge EXAFS results for the aqueous Np(V) species in 4.5 M CaCl2/pHm ≈ 12 confirm the presence of ternary Ca-Np(V)-OH complexes Ca x [NpO2(OH)2]2x–1 (x ≈ 1 is estimated within the thermodynamic evaluation in a subsequent paper (Fellhauer, D., Altmaier, M., Gaona, X., Lützenkirchen, J., Fanghänel, Th., Np(V) solubility, speciation and solid phase formation in alkaline CaCl2 solutions. Part II: Thermodynamics and implications for source term estimations of nuclear waste disposal (Radiochim. Acta, DOI 10.1515/ract-2015-2490), in the following referred to as “Part II” [1]) and Ca y [NpO2(OH)5]2y–4 with y ≈ 2.4 ± 1.5 (EXAFS result) as predominant Np(V) hydrolysis species in solution for [CaCl2] ≥ 0.25 and pHm > 10.5. The thermodynamic evaluation and implications of the new findings with respect to source term estimations for nuclear waste disposal scenarios are discussed in “Part II” [1]).

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)

Precision optical spectroscopy of exotic ions reveals accurate information about nuclear properties such as charge radii and magnetic and quadrupole moments. Thorium ions exhibit unique nuclear properties with high relevance for testing symmetries of nature. We report loading and trapping of single $^{232}$Th$^+$ ions in a linear Paul trap, embedded into and sympathetically cooled by small crystals of trapped $^{40}$Ca$^+$ ions. Trapped Th ions are identified in a non-destructive manner from the voids in the laser-induced Ca fluorescence pattern emitted by the crystal, and alternatively, by means of a time-of-flight signal when extracting ions from the Paul trap and steering them into an external detector. We have loaded and handled a total of 231 individual Th ions. We reach a time-of-flight detection efficiency of $\gtrsim 95\, \%$, consistent with the quantum efficiency of the detector. The sympathetic cooling technique is expected to be applicable for other isotopes and various charge states of Th e.g., for future studies of $^{229m}$Th., Comment: 5 pages, 4 figures

Thin actinide layers deposited on various substrates are widely used as calibration sources in nuclear spectroscopy. Other applications include fundamental research in nuclear chemistry and –physics, e.g., the chemical and physical properties of super-heavy elements (SHE, Z > 103) or nuclear reaction studies with heavy ions. For the design of future nuclear reactors like fast-fission reactors and accelerator-driven systems for transmutation of nuclear waste, precise data for neutron absorption as well as neutron-induced fission cross section data for 242Pu with neutrons of different energies are of particular importance, requiring suitable Pu-targets. Another application includes studies of nuclear transitions in 229Th harvested as α-decay recoil product from a thin layer of its 233U precursor. For this, a thin and very smooth layer of 233U is used. We report here on the production of actinide layers mostly obtained by Molecular Plating (MP). MP is currently the only fabrication method in cases where the desired actinide material is available only in very limited amounts or possesses a high specific activity. Here, deposition is performed from organic solution applying a current density of 1-2 mA/cm2. Under these conditions target thicknesses of 500-1000 μg/cm2 are possible applying a single deposition step with deposition yields approaching 100 %. For yield determination α-particle spectroscopy, γ-spectroscopy and Neutron Activation Analysis is routinely used. Layer homogeneity is checked with Radiographic Imaging. As an alternative technique to MP the production of thin lanthanide and actinide layers by the so-called “Drop on Demand”-technique applied e.g., in ink-jet printing is currently under investigation.

To improve the properties and performance of thin layers produced by molecular plating as targets for nuclear experiments investigations with lanthanide elements (i.e., natural Nd and 147Sm-enriched Sm) were carried out. Plating parameters like roughness of the deposition substrate, plating solvent, electrolyte concentration, and applied current density were varied. The influence of each parameter on the properties of the layers was studied by characterizing the deposits. The characterizations showed that nuclear targets perform differently depending on their layer properties. The results obtained from the investigations were applied for the quantitative preparation of homogeneous large-area (i.e., 42 cm2) 242Pu targets to be used for transmutation-relevant experiments.

For measurements of the neutron-induced fission cross section of 242Pu, large-area (42 cm2) 242Pu targets were prepared on Ti-coated Si wafers by means of constant current density molecular plating. Radiochemical separations were performed prior to the platings. Quantitative deposition yields (>95%) were determined for all targets by means of alpha-particle spectroscopy. Layer densities in the range of 100–150 μg/cm2 were obtained. The homogeneity of the targets was studied by radiographic imaging. A comparative study between the quality of the layers produced on the Ti-coated Si wafers and the quality of layers grown on normal Ti foils was carried out by applying scanning electron microscopy and energy dispersive X-ray spectroscopy. Ti-coated Si wafers resulted clearly superior to Ti foils in the production of homogeneous 242Pu layers with minimum defectivity.

Today’s most precise time and frequency measurements are performed with optical atomic clocks. However, it has been proposed that they could potentially be outperformed by a nuclear clock, which employs a nuclear transition instead of an atomic shell transition. There is only one known nuclear state that could serve as a nuclear clock using currently available technology, namely, the isomeric first excited state of 229Th (denoted 229mTh). Here we report the direct detection of this nuclear state, which is further confirmation of the existence of the isomer and lays the foundation for precise studies of its decay parameters. On the basis of this direct detection, the isomeric energy is constrained to between 6.3 and 18.3 electronvolts, and the half-life is found to be longer than 60 seconds for 229mTh2+. More precise determinations appear to be within reach, and would pave the way to the development of a nuclear frequency standard. Direct detection of the 229Th nuclear clock transition has been achieved, placing direct constraints on transition energy and half-life; these results are a step towards a nuclear clock, nuclear quantum optics and a nuclear laser. The accuracy of atomic clocks, which measure time based on atomic transitions, is central to the function of systems as diverse as GPS navigation and radio astronomy. In theory, a nuclear clock based on an optical excitation of a nuclear transition, could be even better than atomic clocks in terms of stability and compactness. However, the only nuclear state with an excitation energy sufficiently low for this application is the first excited state of thorium-229. But this is arguably most exotic transition in the whole nuclear landscape, and has proven to be extremely hard to detect. Only some indirect evidence could be obtained previously. Here, based on low-energy microchannel plate detection, Lars von der Wense and colleagues achieve direct detection of the thorium-229 nuclear-clock transition, placing new limits on the transition energy and measuring the state's half-life. As well as being a step towards a nuclear clock, these results also suggest that nuclear quantum optics and nuclear lasers based on this transition may be plausible possibilities.

After a successful production of isotopes of element 116 in the reaction 48Ca + 248Cm, the reaction 54Cr + 248Cm → 302120* was investigated at the velocity filter SHIP at GSI, Darmstadt, aiming to search for isotopes of element 120. One chain of events was observed, which is not created by chance with high probability. Parts of the chain agree with model predictions and measured data from a decay chain which could start at the isotope 299120. In a complementary study, model dependent shell-correction energies and related heights of fission barriers were deduced from measured Qα values. The results are compared with predictions of macroscopic-microscopic models. The consequences for calculations of crosssections are discussed.

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.

The reaction 54Cr$ + $248Cm was investigated at the velocity filter SHIP at GSI, Darmstadt, with the intention to study production and decay properties of isotopes of element 120. Three correlated signals were measured, which occurred within a period of 279ms. The heights of the signals correspond with the expectations for a decay sequence starting with an isotope of element 120. However, a complete decay chain cannot be established, since a signal from the implantation of the evaporation residue cannot be identified unambiguously. Measured properties of the event chain are discussed in detail. The result is compared with theoretical predictions. Previously measured decay properties of even element super-heavy nuclei were compiled in order to find arguments for an assignment from the systematics of experimental data. In the course of this review, a few tentatively assigned data could be corrected. New interpretations are given for results which could not be assigned definitely in previous studies. The discussion revealed that the cross-section for production of element 120 could be high enough so that a successful experiment seems possible with presently available techniques. However, a continuation of the experiment at SHIP for a necessary confirmation of the results obtained in a relatively short irradiation of five weeks is not possible at GSI presently. Therefore, we decided to publish the results of the measurement and of the review as they exist now. In the summary and outlook section we also present concepts for the continuation of research in the field of super-heavy nuclei.

Shell-correction energies of super-heavy nuclei are approximated by using $ Q_{\alpha}$ values of measured decay chains. Five decay chains were analyzed, which start at the isotopes 285Fl, 294118, 291Lv, 292Lv and 293Lv. The data are compared with predictions of macroscopic-microscopic models. Fission barriers are estimated that can be used to eliminate uncertainties in partial fission half-lives and in calculations of evaporation-residue cross-sections. In that calculations, fission probability of the compound nucleus is a major factor contributing to the total cross-section. The data also provide constraints on the cross-sections of capture and quasi-fission in the entrance channel of the fusion reaction. Arguments are presented that fusion reactions for synthesis of isotopes of elements 118 and 120 may have higher cross-sections than assumed so far.

TRAKULA ( Tra nsmutationsrelevante k ernphysikalische U ntersuchungen l anglebiger A ktinide, i.e., nuclear physical investigations of long-lived actinides with relevance to transmutation) is a joint research project of the German Federal Ministry of Science and Education (BMBF) on nuclear physics investigations with modern scientific, technological and numerical methods. Experiments concerning the transmutation of radioactive waste are a central topic of the project. For this, large-area samples (≥40 cm 2 ) of 235,238 U and 239,242 Pu compounds are required for the calibration of fission chambers and for fission yield measurements. Another topic within the project requires large-area targets for precise measurements of the half-life, t 1/2 , of very long-lived α-particle emitters like 144 Nd ( t 1/2 ≈2×10 15 y). Here, we report on electrodeposition tests with Gd and Nd (used as chemical homologs of the actinides), which were performed to find optimal deposition conditions for small-area targets that should be applicable to future large-area targets. The layers were produced by molecular plating. A new stirring technique, ultrasonic stirring, was adopted and found to be suitable for producing large-area targets. Moreover, two different current densities (namely 0.7 and 1.4 mA/cm 2 ) were studied and found appropriate for target preparation. Characterization of the layers with different analytical techniques played a major role in these studies to gain a deeper understanding of the deposition process itself: neutron activation analysis and γ-spectroscopy were used for yield measurements, radiographic imaging for homogeneity studies, scanning electron microscopy for morphology studies, and atomic force microscopy for roughness studies. According to the obtained results, a new electrochemical cell for the production of large-area targets was designed.

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.

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.

The superheavy element with atomic number Z=117 was produced as an evaporation residue in the 48Ca+249Bk fusion reaction at the gas-filled recoil separator TASCA at GSI Darmstadt, Germany. The radioactive decay of evaporation residues and their α-decay products was studied using a detection setup that allowed measuring decays of single atomic nuclei with half-lives between sub-μs and a few days. Two decay chains comprising seven α decays and a spontaneous fission each were identified and are assigned to the isotope 294-117 and its decay products. A hitherto unknown α-decay branch in 270Db (Z=105) was observed, which populated the new isotope 266Lr (Z=103). The identification of the long-lived (T1/2=1.0+1.9−0.4 h) α-emitter 270Db marks an important step towards the observation of even more long-lived nuclei of superheavy elements located on an “island of stability.” (Less)

The fission process still remains a main factor that determines the stability of the atomic nucleus of heaviest elements. Fission half-lives vary over a wide range, 10^−19 to 10^24 s. Present experimental techniques for the synthesis of the superheavy elements that usually measure α-decay chains are sensitive only in a limited range of half-lives, often 10^5 to 10^3 s. In the past years, measurement techniques for very short-lived and very long-lived nuclei were significantly improved at the gas-filled recoil separator TASCA at GSI Darmstadt. Recently, several experimental studies of fission-related phenomena have successfully been performed. In this paper, results on 254−256Rf and 266Lr are presented and corresponding factors for retarding the fission process are discussed. (Less)

The synthesis of element 116 in fusion-evaporation reactions of a 48Ca beam with radioactive 248Cm targets was studied at the velocity filter SHIP of GSI in Darmstadt. At excitation energies of the compound nuclei of 40.9MeV, four decay chains were measured, which were assigned to the isotope 292116, and one chain, which was assigned to 293116. Measured cross-sections of (3.4−1.6+2.7) pb and (0.9−0.7+2.1), respectively, and decay data of the chains agree with data measured previously at the Flerov Laboratory of Nuclear Reactions in Dubna. As a new result, one α-decay chain was measured, which terminates after four α decays by spontaneous fission. The α energies of the second-to-fourth decay are considerably higher than those measured for the α decays of 289114, 285Cn, and 281Ds and the spontaneous fission half-life is significantly longer than that of 277Hs measured in previous experiments. A possible assignment is discussed in the frame of excited quasiparticle states of nuclei populated in the decay chain from 293116. Also other possible assignments were considered and are discussed. At an excitation energy of 45.0MeV no events were observed resulting in a one-event cross-section limit of 1.6 pb. The technical aspects related with the use of radioactive target material at SHIP are described in detail. The experience gained in this experiment will serve as a basis for future experiments aiming to study still heavier elements at the velocity filter SHIP.

Experiments with the new recoil separator, Transactinide Separator and Chemistry Apparatus (TASCA), at the GSI were performed by using beams of Ca-48 to irradiate targets of Pb206-208, which led to the production of No252-254 isotopes. These studies allowed for evaluation of the performance of TASCA when coupled to a new detector and electronics system. By following these studies, the isotopes of element 114 ((288-291)114) were produced in irradiations of Pu-244 targets with Ca-48 beams at compound nucleus excitation energies around 41.7 and 37.5 MeV, demonstrating TASCA's ability to perform experiments with picobarn-level cross sections. A total of 15 decay chains were observed and were assigned to the decay of 288-291114. A new a-decay branch in (281)Ds was observed, leading to the new nucleus (277)Hs. (Less)

The fusion-evaporation reaction Pu-244(Ca-48, 3-4n)(288,289)114 was studied at the new gas-filled recoil separator TASCA. Thirteen correlated decay chains were observed and assigned to the production and decay of (288, 289)114. At a compound nucleus excitation energy of E* = 39.8-43.9 MeV, the 4n evaporation channel cross section was 9.8(-3.1)(+3.9) pb. At E* = 36.1-39.5 MeV, that of the 3n evaporation channel was 8.0-(+7.4)(4.5) pb. In one of the 3n evaporation channel decay chains, a previously unobserved alpha branch in (281)Ds was observed ( probability to be of random origin from background: 0.1%). This alpha decay populated the new nucleus (277)Hs, which decayed by spontaneous fission after a lifetime of 4.5 ms.

The deformed doubly magic nucleus (270)Hs has so far only been observed as the four-neutron (4n) evaporation residue of the reaction Mg-26+Cm-248, where a maximum cross section of 3 pb was measured. Theoretical studies on the formation of (270)Hs in the 4n evaporation channel of fusion reactions with different entrance channel asymmetry in the framework of a two-parameter Smoluchowski equation predict that the reactions Ca-48+Ra-226 and S-36+U-238 result in higher cross sections due to lower reaction Q values, in contrast to simple arguments based on the reaction asymmetry, which predict opposite trends. Calculations using HIVAP predict cross sections for the reaction S-36+U-238 that are similar to those of the Mg-26+Cm-248 reaction. Here, we report on the first measurement of evaporation residues formed in the complete nuclear fusion reaction S-36+U-238 and the observation of (270)Hs, which is produced in the 4n evaporation channel, with a measured cross section of 0.8(-0.7)(+2.6) pb at 51-MeV excitation energy. The one-event cross-section limits (68% confidence level) for the 3n, 4n, and 5n evaporation channels at 39-MeV excitation energy are 2.9 pb, while the cross-section limits of the 3n and 5n channel at 51 MeV are 1.5 pb. This is significantly lower than the 5n cross section of the Mg-26+Cm-248 reaction at similar excitation energy.