S. Raeder

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

Optical spectroscopy of a primordial isotope has traditionally formed the basis for understanding the atomic structure of an element. Such studies have been conducted for most elements and theoretical modelling can be performed to high precision, taking into account relativistic effects that scale approximately as the square of the atomic number. However, for the transfermium elements (those with atomic numbers greater than 100), the atomic structure is experimentally unknown. These radioactive elements are produced in nuclear fusion reactions at rates of only a few atoms per second at most and must be studied immediately following their production, which has so far precluded their optical spectroscopy. Here we report laser resonance ionization spectroscopy of nobelium (No; atomic number 102) in single-atom-at-a-time quantities, in which we identify the ground-state transition 1S0 1P1. By combining this result with data from an observed Rydberg series, we obtain an upper limit for the ionization potential of nobelium. These accurate results from direct laser excitations of outer-shell electrons cannot be achieved using state-of-the-art relativistic many-body calculations that include quantum electrodynamic effects, owing to large uncertainties in the modelled transition energies of the complex systems under consideration. Our work opens the door to high-precision measurements of various atomic and nuclear properties of elements heavier than nobelium, and motivates future theoretical work.

An All-Solid-State High Repetiton Rate Titanium:Sapphire Laser System For Resonance Ionization Laser Ion Sources

On‐line production facilities for radioactive isotopes nowadays heavily rely on resonance ionization laser ion sources due to their demonstrated unsurpassed efficiency and elemental selectivity. Powerful high repetition rate tunable pulsed dye or Ti:sapphire lasers can be used for this purpose. To counteract limitations of short pulse pump lasers, as needed for dye laser pumping, i.e. copper vapor lasers, which include high maintenance and nevertheless often only imperfect reliability, an all‐solid‐state Nd:YAG pumped Ti:sapphire laser system has been constructed. This could complement or even replace dye laser systems, eliminating their disadvantages but on the other hand introduce shortcomings on the side of the available wavelength range. Pros and cons of these developments will be discussed.

Towards high-resolution laser ionization spectroscopy of the heaviest elements in supersonic gas jet expansion

Resonant laser ionization and spectroscopy are widely used techniques at radioactive ion beam facilities to produce pure beams of exotic nuclei and measure the shape, size, spin and electromagnetic multipole moments of these nuclei. However, in such measurements it is difficult to combine a high efficiency with a high spectral resolution. Here we demonstrate the on-line application of atomic laser ionization spectroscopy in a supersonic gas jet, a technique suited for high-precision studies of the ground- and isomeric-state properties of nuclei located at the extremes of stability. The technique is characterized in a measurement on actinium isotopes around the N=126 neutron shell closure. A significant improvement in the spectral resolution by more than one order of magnitude is achieved in these experiments without loss in efficiency.

Detection of plutonium isotopes at lowest quantities using in-source resonance ionization mass spectrometry

The in-source resonance ionization mass spectrometry technique was applied for quantification of ultratrace amounts of plutonium isotopes as a proof of principle study. In addition to an overall detection limit of 104 to 105 atoms, this method enables the unambiguous identification and individual quantification of the plutonium isotopes 238Pu and 241Pu which are of relevance for dating of radiogenic samples. Due to the element-selective ionization process, these isotopes can be measured even under a high surplus of isobaric contaminations from 238U or 241Am, which considerably simplifies chemical preparation. The technique was developed, tested, and characterized on a variety of synthetic and calibration samples and is presently applied to analyze environmental samples.

Ion production from solid state laser ion sources.

Laser ion sources based on resonant excitation and ionization of atoms are well-established tools for selective and efficient production of radioactive ion beams. Recent developments are focused on the use of the state-of-the-art all solid-state laser systems. To date, 35 elements of the periodic table are available from laser ion sources based on tunable Ti:sapphire lasers. Recent progress in this field regarding the establishment of suitable optical excitation schemes for Ti:sapphire lasers are reported.

Laser Resonance Ionization Spectroscopy of the Lanthanides Tb, Dy and Ho as Homologues to Actinides and Super Heavy Elements

Spectroscopic investigations of the rare earth elements Tb, Dy and Ho have been carried out using laser resonance ionization mass spectroscopy. A variety of new intermediate energy levels and autoionizing states were observed in these elements. Efficient and selective excitation and ionization schemes for the elements have been developed for Ti:Sapphire lasers using the spectroscopic data. Resonant ionization schemes for Np were also been studied as the preparation work for related investigations on actinide elements and for the spectroscopy on the heaviest elements, where spectroscopic data so far are scarce or not existing at all.

Precision Measurement of the First Ionization Potential of Nobelium

One of the most important atomic properties governing an elements chemical behavior is the energy required to remove its least-bound electron, referred to as the first ionization potential. For the heaviest elements, this fundamental quantity is strongly influenced by relativistic effects which lead to unique chemical properties. Laser spectroscopy on an atom-at-a-time scale was developed and applied to probe the optical spectrum of neutral nobelium near the ionization threshold. The first ionization potential of nobelium is determined here with a very high precision from the convergence of measured Rydberg series to be 6.626 21±0.000 05  eV. This work provides a stringent benchmark for state-of-the-art many-body atomic modeling that considers relativistic and quantum electrodynamic effects and paves the way for high-precision measurements of atomic properties of elements only available from heavy-ion accelerator facilities.

Production of negative osmium ions by laser desorption and ionization

The interest to produce negative osmium ions is manifold in the realm of high-accuracy ion trap experiments: high-resolution nearly Doppler-free laser spectroscopy, antihydrogen formation in its ground state, and contributions to neutrino mass spectrometry. Production of these ions is generally accomplished by sputtering an Os sample with Cs(+) ions at tens of keV. Though this is a well-established method commonly used at accelerators, these kind of sources are quite demanding and tricky to operate. Therefore, the development of a more straightforward and cost effective production scheme will be of benefit for ion trap and other experiments. Such a scheme makes use of desorption and ionization with pulsed lasers and identification of the ions by time-of-flight mass spectrometry. First investigations of negative osmium ion production using a pulsed laser for desorption and ionization and a commercial matrix-assisted laser desorption/ionization time-of-flight system for identification has demonstrated the suitability of this technique. More than 10(3) negative osmium ions per shot were registered after bombarding pure osmium powder with a 5 ns pulse width Nd:yttrium aluminum garnet laser. The limitation in the ion number was imposed by the detection limit of the microchannel plate detector.