Actinide and lanthanide thin-layer developments using a drop-on-demand printing system

Actinide and lanthanide thin layers with specific requirements regarding thickness, homogeneity, chemical purity, mechanical stability, and backing properties are applied in a multitude of physics and chemistry experiments. A novel target preparation method, the so-called “Drop-on-Demand” (DoD) technique, based on a commercial nanoliter (nL) dispenser is applied since a few years in the Nuclear Chemistry unit at Johannes Gutenberg University Mainz. The wetting behaviour of the nL droplets on the substrate’s surface is a key parameter determining the spatial distribution of the deposited material after evaporation. By switching from aqueous to organic solvents as well as by substrate surface…

Direct detection of the 229Th nuclear clock transition

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 const…

Development and characterization of a Drop-on-Demand inkjet printing system for nuclear target fabrication

Abstract 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 eva…

The recoil transfer chamber—An interface to connect the physical preseparator TASCA with chemistry and counting setups

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 o…

Trapping and sympathetic cooling of single thorium ions for spectroscopy

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 ex…

Recoil-α-fission and recoil-α–α-fission events observed in the reaction 48Ca + 243Am

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 ch…

Alpha spectrometric characterization of thin $^{233}$U sources for $^{229\text{(m)}}$Th production

Four different techniques were applied for the production of $^{233}$U alpha recoil ion sources, providing $^{229}$Th ions. They were compared with respect to a minimum energy spread of the $^{229}$Th recoil ions, using the emitted alpha particles as an indicator. The techniques of Molecular Plating, Drop-on-Demand inkjet printing, chelation from dilute nitric acid solution on chemically functionalized silicon surfaces, and self-adsorption on passivated titanium surfaces were used. All fabricated sources were characterized by using alpha spectrometry, radiographic imaging, and scanning electron microscopy. A direct validation for the estimated recoil ion rate was obtained by collecting $^{2…

Production and Decay of Element 114: High Cross Sections and the New NucleusHs277

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…

Systematic evidence for quasifission in Be9−, C12−, and O16 -induced reactions forming No258,260

Low-lying states in Ra219 and Rn215 : Sampling microsecond α -decaying nuclei

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 …

Application of Resonance Ionization Mass Spectrometry for Ultratrace Analysis of Technetium

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 …

Zeptosecond contact times for element Z=120 synthesis

The synthesis of new superheavy elements beyond oganesson (Z=118) requires fusion reactions with projectile nuclei with proton numbers larger than that of $^{48}$Ca (Z=20), which has been successfully employed for the synthesis of elements with Z=112-118. In such reactions, fusion is drastically hindered by fast non-equilibrated dynamical processes. Attempts to produce nuclei with Z=120 using the $^{64}$Ni+$^{238}$U, $^{58}$Fe+$^{244}$Pu, $^{54}$Cr+$^{248}$Cm, and $^{50}$Ti+$^{249}$Cf reactions have been made, which all result in larger Coulomb forces than for $^{48}$Ca-induced reactions, but no discovery has been confirmed to date. In this work, mass and angle distributions of fission frag…

Fission in the landscape of heaviest elements: Some recent examples

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 ar…

Rapid extraction of short-lived isotopes from a buffer gas cell for use in gas-phase chemistry experiments. Part I: Off-line studies with  219Rn and  221Fr

Abstract 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 eleme…

Ca48+Bk249Fusion Reaction Leading to ElementZ=117: Long-Livedα-DecayingDb270and Discovery ofLr266

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-liv…

Measurement of the first ionization potential of lawrencium (element 103)

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 vi…

First superheavy element experiments at the GSI recoil separator TASCA: The production and decay of element 114 in thePu244(Ca48,3-4n) reaction

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 as…

Quantitative molecular plating of large-area 242Pu targets with improved layer properties

Abstract 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…

On the use of stacks of fission-like targets for neutron capture experiments

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 me…

Radiochemical study of the kinematics of multi-nucleon transfer reactions in 48Ca + 248Cm collisions 10% above the Coulomb barrier

Abstract 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…

Measurement of the Th229 Isomer Energy with a Magnetic Microcalorimeter

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)%…

Toward large-area targets for “TRAKULA”

Abstract 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-a…

Gas phase synthesis of 4d transition metal carbonyl complexes with thermalized fission fragments in single-atom reactions

Abstract 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 fl…

Study of non-fusion products in the Ti50+Cf249 reaction

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 ex…

Spectroscopy along Flerovium Decay Chains: Discovery ofDs280and an Excited State inCn282

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 eleme…

TASCAを用いたCn, Nh, Fl化学実験のためのHg, Tl, PbのSiO2及びAu表面に対するオンライン化学吸着研究

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 no…

Fast-neutron-induced fission cross section of Pu242 measured at the neutron time-of-flight facility nELBE

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 ar…

Sensitive search for near-symmetric and super-asymmetric fusion-fission of the superheavy element Flerovium (Z=114)

Physics letters / B 820, 136601 (2021). doi:10.1016/j.physletb.2021.136601