High brilliance uranium beams for the GSI FAIR

The 40 years old GSI-UNILAC (Universal Linear Accelerator) as well as the heavy ion synchrotron SIS18 will serve as a high current heavy ion injector for the new FAIR (Facility for Antiproton and Ion Research) synchrotron SIS100. In the context of an advanced machine investigation program in combination with the ongoing UNILAC upgrade program, a new uranium beam intensity record (11.5 emA, ${\mathrm{U}}^{29+}$) at very high beam brilliance was achieved recently in a machine experiment campaign. This is an important step paving the way to fulfill the FAIR heavy ion high intensity beam requirements. Results of high current uranium beam measurements applying a newly developed pulsed hydrogen g…

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…

Seaborgium's complex studies

Christoph E. Dullmann reflects on the excitement, and implications, of probing the reactivity of heavy element seaborgium.

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…

First ionization potential of the heaviest actinide lawrencium, element 103

The first ionization potential (IP1 ) of element 103, lawrencium (Lr), has been successfully determined for the first time by using a newly developed method based on a surface ionization process. The measured IP 1 value is 4.9630.08 0.07 eV. This value is the smallest among those of actinide elements and is in excellent agreement with the value of 4.963(15) eV predicted by state-of-the-art relativistic calculations also performed in this work. Our results strongly support that the Lr atom has an electronic configuration of [Rn]7s 2 5f 14 7p 1 1/2 , which is influenced by strong relativistic effects. The present work provides a reliable benchmark for theoretical calculations and also opens t…

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, isolation and characterization of radiochemically pure 163Ho samples for the ECHo-project

Abstract Several experiments on the study of the electron neutrino mass are based on high-statistics measurements of the energy spectrum following electron capture of the radionuclide 163Ho. They rely on the availability of large, radiochemically pure samples of 163Ho. Here, we describe the production, separation, characterization, and sample production within the Electron Capture in Holmium-163 (ECHo) project. 163Ho has been produced by thermal neutron activation of enriched, prepurified 162Er targets in the high flux reactor of the Institut Laue-Langevin, Grenoble, France, in irradiations lasting up to 54 days. Irradiated targets were chemically processed by means of extraction chromatogr…

First Ionization Potentials of Fm, Md, No, and Lr

We report the first ionization potentials (IP1) of the heavy actinides, fermium (Fm, atomic number Z = 100), mendelevium (Md, Z = 101), nobelium (No, Z = 102), and lawrencium (Lr, Z = 103), determined using a method based on a surface ionization process coupled to an online mass separation technique in an atom-at-a-time regime. The measured IP1 values agree well with those predicted by state-of-the-art relativistic calculations performed alongside the present measurements. Similar to the well-established behavior for the lanthanides, the IP1 values of the heavy actinides up to No increase with filling up the 5f orbital, while that of Lr is the lowest among the actinides. These results clear…

Anionic Fluoro Complex of Element 105, Db

We report on the characteristic anion-exchange behavior of the superheavy element dubnium (Db) with atomic number Z=105 in HF/HNO3 solution at the fluoride ion concentration [F−]=0.003 M. The resul...

Energy of the $^{229}$Th nuclear clock transition

The first nuclear excited state of $^{229}$Th offers the unique opportunity for laser-based optical control of a nucleus. Its exceptional properties allow for the development of a nuclear optical clock which offers a complementary technology and is expected to outperform current electronic-shell based atomic clocks. The development of a nuclear clock was so far impeded by an imprecise knowledge of the energy of the $^{229}$Th nuclear excited state. In this letter we report a direct excitation energy measurement of this elusive state and constrain this to 8.28$\pm$0.17 eV. The energy is determined by spectroscopy of the internal conversion electrons emitted in-flight during the decay of the …

Superheavy element flerovium (element 114) is a volatile metal.

The electron shell structure of superheavy elements, i.e., elements with atomic number Z ≥ 104, is influenced by strong relativistic effects caused by the high Z. Early atomic calculations on element 112 (copernicium, Cn) and element 114 (flerovium, Fl) having closed and quasi-closed electron shell configurations of 6d(10)7s(2) and 6d(10)7s(2)7p1/2(2), respectively, predicted them to be noble-gas-like due to very strong relativistic effects on the 7s and 7p1/2 valence orbitals. Recent fully relativistic calculations studying Cn and Fl in different environments suggest them to be less reactive compared to their lighter homologues in the groups, but still exhibiting a metallic character. Expe…

Studying Chemical Properties of the Heaviest Elements: One Atom at a Time

The search for heavier elements has been an exciting endeavor for nuclear scientists for many decades. This was invigorated after the first predictions that nuclear shell effects might render superheavy elements to have lifetimes long enough for their experimental study, or even their occurrence in Nature. A fascinating aspect concerns the question of their chemical properties: will they conform to the well-established structure of the Periodic Table of the Elements, or will so-called relativistic effects—a result of the high velocities of electrons in the vicinity of highly-charged nuclei—lead to dramatic deviations? Chemical studies of the heaviest elements are complicated by small produc…

118 und (k)ein Ende in Sicht? Das Periodensystem feiert 150. Geburtstag

Opportunities for Fundamental Physics Research with Radioactive Molecules

Molecules containing short-lived, radioactive nuclei are uniquely positioned to enable a wide range of scientific discoveries in the areas of fundamental symmetries, astrophysics, nuclear structure, and chemistry. Recent advances in the ability to create, cool, and control complex molecules down to the quantum level, along with recent and upcoming advances in radioactive species production at several facilities around the world, create a compelling opportunity to coordinate and combine these efforts to bring precision measurement and control to molecules containing extreme nuclei. In this manuscript, we review the scientific case for studying radioactive molecules, discuss recent atomic, mo…

Optimization of a laser ion source for $^{163}$Ho isotope separation

To measure the mass of the electron neutrino, the “Electron Capture in Holmium-163” (ECHo) collaboration aims at calorimetrically measuring the spectrum following electron capture in 163Ho. The success of the ECHo experiment depends critically on the radiochemical purity of the 163Ho sample, which is ion-implanted into the calorimeters. For this, a 30 kV high transmission magnetic mass separator equipped with a resonance ionization laser ion source is used. To meet the ECHo requirements, the ion source unit was optimized with respect to its thermal characteristics and material composition by means of the finite element method thermal-electric calculations and chemical equilibrium simulation…

On the search for elements beyond Z =118. An outlook based on lessons from the heaviest known elements

Recently, IUPAC approved all elements up to Z = 118 as discovered. Search experiments for the heavier elements with Z = 119 and 120 have been performed in recent years, but have so far not led to their discovery. I will review some aspects associated with the study and identification of the heaviest known elements that are relevant for future search experiments for elements beyond Z = 118 and highlight pressing issues that should be addressed, both on the experimental as well as on the theory side, to allow for performing these future experiments under improved and better informed conditions.

Speeding up liquid-phase heavy element chemistry: Development of a vacuum to liquid transfer chamber (VLTC)

Abstract We present a new system, which is suitable for performing fast liquid phase chemistry experiments and gives access to shorter-lived isotopes of super heavy elements (SHE) than accessible with current techniques. With this novel vacuum to liquid transfer chamber (VLTC), which is mounted behind a physical preseparator, the desired isotopes are transported from the low-pressure side of the recoil separator directly into the liquid phase of a chemical experiment. Simulations on the kinematics of evaporation residues were performed using SRIM, validating the general plausibility of the VLTC concept. Subsequently, the feasibility was demonstrated with 250 , 252 Cf fission fragments, whic…

Atom-at-a-time laser resonance ionization spectroscopy of nobelium

Resonance ionization spectroscopy of nobelium (atomic number 102) reveals its ground-state transition and an upper limit for its ionization potential, paving the way to characterizing even heavier elements via optical spectroscopy. Characterizing the heaviest elements in the periodic table is a gruelling task because they are radioactive, exist only for split seconds at a time and need to be artificially produced in sufficient quantities by complicated procedures. The heaviest element that has been characterized by optical spectroscopy is fermium, which has an atomic number of 100. Mustapha Laatiaoui et al. extend the methods used for fermium to perform optical spectroscopy on nobelium (ato…

Simulation and optimization of the implantation of holmium atoms into metallic magnetic microcalorimeters for neutrino mass determination experiments

Abstract Several novel experiments designed to investigate the electron neutrino mass in the sub-eV region are based on the calorimetric measurement of the 163Ho electron capture spectrum. For this the 163Ho source, with a required activity of the order of 1 to 100 Bq , needs to be enclosed in the detector, having a volume smaller than 10 − 3 mm 3 . Ion implantation is presently considered to be the most reliable method to enclose this source in the detector homogeneously distributed in a well defined volume. We have investigated the distribution of implanted holmium ions in different target materials and for different implantation energies by means of Monte Carlo simulations based on the S…

Rapid Synthesis of Radioactive Transition-Metal Carbonyl Complexes at Ambient Conditions

Carbonyl complexes of radioactive transition metals can be easily synthesized with high yields by stopping nuclear fission or fusion products in a gas volume containing CO. Here, we focus on Mo, W, and Os complexes. The reaction takes place at pressures of around 1 bar at room temperature, i.e., at conditions that are easy to accommodate. The formed complexes are highly volatile. They can thus be transported within a gas stream without major losses to setups for their further investigation or direct use. The rapid synthesis holds promise for radiochemical purposes and will be useful for studying, e.g., chemical properties of superheavy elements.

Attempts to chemically investigate element 112

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)…

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…

Production and study of chemical properties of superheavy elements

Abstract Some highlight examples on the study of production and chemical properties of heaviest elements carried out mostly at GSI Darmstadt are presented. They focus on the production of some of the heaviest known elements (114Fl, 115Mc, and 117Mc), studies of non-fusion reactions, and on chemical studies of 114Fl. This is the heaviest element, for which chemical studies have been performed to date.

Highly efficient isotope separation and ion implantation of  163Ho for the ECHo project

Abstract The effective electron neutrino mass measurement in the framework of the ECHo experiment requires radiochemically pure 163 Ho, which is ion implanted into detector absorbers. To meet the project specifications in efficiency and purity, the entire process chain of ionization, isotope separation , and implantation of 163Ho was optimized. A new two-step resonant laser ionization scheme was established at the 30 kV magnetic mass separator RISIKO. For ionization and separation, an average efficiency of 69 ( 5 )  stat(4)sys% was achieved using intra-cavity frequency doubled Ti:sapphire lasers. The implantation of undesired 166 m Ho, which is present in trace amounts in the initial  163Ho…

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)%…

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…

Development of a fast characterization setup for radionuclide generators demonstrated by a 227Ac-based generator

Abstract The development of a setup for a fast online characterization of radionuclide generators is reported. A generator utilizing the mother nuclide 227Ac sorbed on a cation exchange resin is continuously eluted by using a peristaltic pump. To allow continuous and pulse-free elution of a large volume over extended time periods a 3D-printed interface designed to remove pressure-oscillations induced by the pump was placed between pump and generator column to ensure undisturbed generator elution. The eluate of the generator is passed through a 3D printed flow cell placed inside a borehole Na(Tl)-scintillation detector for high counting efficiency. Alternatively, a HPGe detector suitable for…

118 and Counting … The Periodic Table on its 150th Anniversary.

"Is there still room for more elements in the modern periodic table with its currently 118 elements? Will we need another extra series in the periodic table besides the classical s-, p-, and d-block, and the lanthanides/actinides? Will the periodic table in this region still feature periodicity? …" Read more in the Guest Editorial by C. E. Dullmann.

In-situ formation, thermal decomposition, and adsorption studies of transition metal carbonyl complexes with short-lived radioisotopes

Abstract We report on the in-situ synthesis of metal carbonyl complexes with short-lived isotopes of transition metals. Complexes of molybdenum, technetium, ruthenium and rhodium were synthesized by thermalisation of products of neutron-induced fission of 249Cf in a carbon monoxide-nitrogen mixture. Complexes of tungsten, rhenium, osmium, and iridium were synthesized by thermalizing short-lived isotopes produced in 24Mg-induced fusion evaporation reactions in a carbon monoxide containing atmosphere. The chemical reactions took place at ambient temperature and pressure conditions. The complexes were rapidly transported in a gas stream to collection setups or gas phase chromatography devices.…

Impact of buffer gas quenching on the $^1S_0$ $\to$ $^1P_1$ ground-state atomic transition in nobelium

International audience; Using the sensitive Radiation Detected Resonance Ionization Spectroscopy (RADRIS) techniquean optical transition in neutral nobelium (No, Z = 102) was identified. A remnant signal when delaying the ionizing laser indicated the influence of a strong buffer gas induced de-excitation of the optically populated level. A subsequent investigation of the chemical homologue, ytterbium (Yb, Z = 70), enabled a detailed study of the atomic levels involved in this process, leading to the development of a rate equation model. This paves the way for characterizing resonance ionization spectroscopy (RIS) schemes used in the studyof nobelium and beyond, where atomic properties are c…