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A novel combination of advanced gas-chromatography and detection systems coupled to a buffer-gas cell was characterized on-line to allow gas-phase chemical studies of accelerator-produced short-lived α -decaying mercury, francium, and astatine isotopes. These were produced in 40Ar- and 48Ca-induced nuclear fusion–evaporation reactions, subsequently isolated in the recoil separators MARS at Texas A&M University, USA, and TASCA at GSI Darmstadt, Germany, before being thermalized in a buffer-gas-stopping cell. From the latter, the nuclear reaction products were extracted into gas-phase chromatographic systems, suitable for registering α -decaying short-lived radionuclides, such as isotopes of superheavy elements. Efficiencies of 21(3)% for 204-209Fr were reached for the extraction into the optimized miniCOMPACT gas-chromatography setup, indicating that this technique enables the identification of isotopes of volatile as well as non-volatile elements. These studies guide the path towards chemical investigations of superheavy elements beyond flerovium, which are out of reach with currently used setups.

Atoms 10(2), 51 (2022). doi:10.3390/atoms10020051, Published by MDPI, Basel

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

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.

Thorium ions exhibit unique nuclear properties with high relevance for testing symmetries of nature, and Paul traps feature an ideal experimental platform for performing high precision quantum logic spectroscopy. Loading of stable or long-lived isotopes is well-established and relies on ionization from an atomic beam. A different approach allows trapping short-lived isotopes available as alpha-decay daughters, which recoil from a thin sample of the precursor nuclide. A prominent example is the short-lived $^{229\text{m}}$Th, populated in a decay of long-lived $^{233}$U. Here, ions are provided by an external source and are decelerated to be available for trapping. Such setups offer the option to trap various isotopes and charge states of thorium. Investigating this complex procedure, we demonstrate the observation of single $^{232}$Th$^+$ ions trapped, embedded into and sympathetically cooled via Coulomb interactions by co-trapped $^{40}$Ca$^+$ ions. Furthermore, we discuss different options for a non-destructive identification of the sympathetically cooled thorium ions in the trap, and describe in detail our chosen experimental method, identifying mass and charge of thorium ions from the positions of calcium ions, as their fluorescence is imaged on a CCD camera. These findings are verified by means of a time-of-flight signal when extracting ions of different mass-to-charge ratio from the Paul trap and steering them into a detector.

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 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.

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.

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)