Collinear laser spectroscopy on isotopic chains of refractory elements is under preparation at the SLOWRI facility in the radioactive isotope (RI) beam factory of RIKEN. Towards online measurement on RI beams, we have prepared an offline setup and performed test measurements using singly charged barium isotopes. Then we measured spectra of singly charged zirconium ions as a proof of principle for refractory elements.

An in-flight separator performs the important role of separating a single specific radioactive isotope (RI) beam from the thousands of RI beams produced by in-flight fission as well as projectile fragmentation. However, when looking at "separation" from a different viewpoint, more than 99% of simultaneously produced RI beams are just eliminated in the focal plane slits or elsewhere in the separator. In order to enhance the effective usability of the RIKEN in-flight separator BigRIPS, we have been developing an innovative method: parasitic laser ion source (PALIS), which implements parasitic low-energy RI beam production by saving eliminated RI beams during BigRIPS experiments. In this paper, we present the expected benefits and feasibility for the PALIS concept and the results of the first stopping examination for high-energy RI beams in the gas cell.

This paper describes the laser and optical system for the Parasitic radioactive isotope (RI) beam production by Laser Ion-Source (PALIS) in the RIKEN fragment separator facility. This system requires an optical path length of 70 m for transporting the laser beam from the laser light source to the place for resonance ionization. To accomplish this, we designed and implemented a simple optical system consisting of several mirrors equipped with compact stepping motor actuators, lenses, beam spot screens and network cameras. The system enables multi-step laser resonance ionization in the gas cell and gas jet via overlap with a diameter of a few millimeters, between the laser photons and atomic beam. Despite such a long transport distance, we achieved a transport efficiency for the UV laser beam of about 50%. We also confirmed that the position stability of the laser beam stays within a permissible range for dedicated resonance ionization experiments.

Spectroscopic properties of atomic species of plutonium were investigated by combining laser ablation and resonance absorption techniques for the analysis of a plutonium oxide sample. For 17 transitions of Pu atoms and ions, the absorbance, isotope shift, and hyperfine splitting were determined via Voigt profile fitting of the recorded absorption spectra. Three transitions were selected as candidates for analytical use. Using these transitions, we investigated the analytical performance that was attainable and determined a correlation coefficient R2 between the absorbance and plutonium concentration of 0.9999, a limit of detection of 30–130ppm, and a relative standard deviation of approximately 6% for an abundance of 240Pu of 2.4%. These results demonstrate that laser ablation absorption spectroscopy is applicable to the remote isotopic analysis of highly radioactive nuclear fuels and waste materials containing multiple actinide elements.

A study of the quasi-5-day wave (5DW) was performed using meteor radars at conjugate latitudes in the Northern and Southern hemispheres. These radars are located at Esrange, Sweden (68° N) and Juliusruh, Germany (55° N) in the Northern Hemisphere, and at Tierra del Fuego, Argentina (54° S) and Rothera Station, Antarctica (68° S) in the Southern Hemisphere. The analysis was performed using data collected during simultaneous measurements by the four radars from June 2010 to December 2012 at altitudes from 84 to 96 km. The 5DW was found to exhibit significant short-term, seasonal, and interannual variability at all sites. Typical events had planetary wave periods that ranged between 4 and 7 days, durations of only a few cycles, and infrequent strongly peaked variances and covariances. Winds exhibited rotary structures that varied strongly among sites and between events, and maximum amplitudes up to ~ 20 m s−1. Mean horizontal velocity covariances tended to be largely negative at all sites throughout the interval studied.

The dynamic behavior of an ablation plume in ambient gas has been investigated by laser-induced fluorescence imaging spectroscopy. The second harmonic beam from an Nd:YAG laser (0.5–6J/cm2) was focused on a sintered oxide pellet or a metal chip of gadolinium. The produced plume was subsequently intersected with a sheet-shaped UV beam from a dye laser so that time-resolved fluorescence images were acquired with an intensified CCD camera at various delay times. The obtained cross-sectional images of the plume indicate that the ablated ground state atoms and ions of gadolinium accumulate in a hemispherical contact layer between the plume and the ambient gas, and a cavity containing a smaller density of ablated species is formed near the center of the plume. At earlier expansion stage, another luminous component also expands in the cavity so that it coalesces into the hemispherical layer. The splitting and coalescence for atomic plume occur later than those for ionic plume. Furthermore, the hemispherical layer of neutral atoms appears later than that of ions; however, the locations of the layers are nearly identical. This coincidence of the appearance locations of the layers strongly suggests that the neutral atoms in the hemispherical layer are produced as a consequence of three-body recombination of ions through collisions with gas atoms. The obtained knowledge regarding plume expansion dynamics and detailed plume structure is useful for optimizing the experimental conditions for ablation-based spectroscopic analysis.

We have calculated the charge radii in the framework of the finite-range droplet model (FRDM) for 884 nuclei for which experimental charge radii are available. By comparing the results with the experimental radii, we found that the calculated radii were too big on average. This deviation can be minimized if we assume a nonstandard small value for the aden parameter in the FRDM calculation. However, even if we use this value, the calculated radii still deviate from the experimental ones in a systematic manner. Although we have calculated the shell corrections by using the microscopic wave function model and added them to the FRDM radii, the deviations have not been improved.

Neutron Resonance Densitometry (NRD) is proposed for the quantification of nuclear materials in particle-like debris of melted fuel from the reactors of the Fukushima Daiichi nuclear power plant. The method is based on a combination of neutron resonance transmission analysis (NRTA) and neutron resonance capture analysis (NRCA). It uses the neutron time-of-flight (TOF) technique with a pulsed white neutron source and a neutron flight path as short as 5 m. The spectrometer for NRCA is made of LaBr3(Ce) detectors. The achievable uncertainty due to only counting statistics is less than 1 % to determine Pu and U isotopes.

The impact of systematic effects on the areal density derived from a neutron resonance transmission analysis (NRTA) is investigated by measurements at the time-of-flight facility GELINA. The experiments were carried out at a 25m station using metallic natural Cu discs with different thicknesses. To derive the areal density from a fitting to the experimental transmission, the resonance shape analysis code REFIT was used. Large bias effects were observed using recommended resonance parameters. Therefore, neutron resonance parameters, in particular resonance energies and neutron widths, were derived from the transmission data obtained with a 0.25mm thick Cu metallic sample. These parameters were used to study the impact of the resonance strength and sample thickness on the accuracy of the areal density derived by NRTA.

The westward propagating zonal wavenumber 1 nonmigrating semidiurnal tide (SW1) enhanced at high latitudes during summer in the mesosphere and lower thermosphere (MLT) is believed to originate from the nonlinear interaction between the migrating semidiurnal tide (SW2) and the stationary planetary wave zonal wavenumber 1 (SPW1) in the opposite winter hemispheres. This paper presents correlations of the SW1 over the Antarctic and Arctic and the SPW1 in the opposite hemispheres. The SW1 is determined from horizontal wind measurements by the TIMED Doppler Interferometer (TIDI) and the SPW1 is from temperature measurements by the Sounding the Atmosphere using Broadband Emission Radiometry (SABER), both aboard the NASA׳s Thermosphere Ionosphere Mesosphere Energetics and Dynamics (TIMED) satellite. We focus on the SW1 over the Antarctic and the SPW1 in the northern hemisphere during an interval from mid-September to mid-November, and the SW1 over the Arctic and the SPW1 in the southern hemisphere during an interval from mid-March to mid-May. Large interannual variations of the SW1 and SPW1 are exhibited in both northern and southern hemispheres. For amplitudes of the SW1 at 90km and 82.5°S, positive correlations are exhibited with SPW1 amplitudes at ~55km in the equatorial region, and ~25km and 55°N. Although zonal SW1 amplitude at 95km and 86.5°N is positively correlated with SPW1 amplitudes at ~30°S above 35km, meridional SW1 amplitude is negatively correlated with SPW1 amplitudes equatorward of 30°S. We also present results of a correlation analysis for SW3 amplitudes during an interval from mid-January to mid-March over the Antarctic and from mid-July to mid-September over the Arctic with SPW1 amplitudes.

To determine experimental conditions suitable for isotope analysis, we studied the plume dynamics of uranium. A uranium oxide sample was ablated by 2nd harmonic radiation from a Nd:YAG laser at a fluence of 0.5 J/cm2. The temporal evolution of the ablation plume was investigated in 800 Pa helium environment. It was found that the observation at 3–5 μs after the ablation at the height of about 2.5 mm are most suited for obtaining higher sensitivity. Using the established conditions, we obtained the limit of detection of the isotope ratio (235U/238U) to be 0.01 %. In addition, the limit of detection of elemental abundance of uranium in uranium glass was also evaluated.

Neutron resonance densitometry (NRD) has been proposed to quantify nuclear materials in melted fuel (MF) that will be removed from the Fukushima Daiichi nuclear power plant. The problem is complex due to the expected presence of strong neutron absorbing impurities such as 10B and high radiation field that is mainly caused by 137Cs. To identify the impurities under the high radiation field, NRD is based on a combination of neutron resonance transmission analysis (NRTA) and neutron resonance capture analysis (NRCA). We investigated with Geant4 the performance of a gamma-ray detector for NRCA in NRD. The gamma-ray detector has a well shape, consisting of cylindrical and tube type LaBr3 scintillators. We show how it measures 478 keV gamma rays derived from 10B(n, αγ) reaction in MF under a high 137Cs-radiation environment. It was found that the gamma-ray detector was able to well suppress the Compton edge of 662-keV gamma rays of 137Cs and had a high peak-to-Compton continuum ratio, by using the tube type scintillator as a back-catcher detector. Then, we demonstrate that with this ability, detection of 478-keV gamma rays from 10B is accomplished in realistic measuring time.

To determine experimental conditions suitable for isotope analysis, we studied the plume dynamics of uranium. A uranium oxide sample was ablated by 2nd harmonic radiation from a Nd:YAG laser at a fluence of 0.5 J/cm2. The temporal evolution of the ablation plume was investigated in vacuum and helium environments. In vacuum, the flow velocity perpendicular to the sample surface was determined to be 2.7 km/s for neutral atoms and 4.0 km/s for singly charged atoms. These velocities are about 20 % lower than those of cerium measured under similar conditions. From the evolution of the plume in helium, we found that an observation time of 3–5 μs and an observation height of about 2.5 mm are most suited for obtaining higher sensitivity. Observation times less than 3 μs were unsuitable for precise isotope analysis since the spectral modifications arising from the Doppler splitting effect are different between the two uranium isotopes. Using the established conditions, we evaluated the calibration curve linearity, limit of detection, and precision for three samples having different abundances of 235U.

A new laser ion source configuration based on resonant photoionization in a gas cell has been developed at RIBF RIKEN. This system is intended for the future PArasitic RI-beam production by Laser Ion-Source (PALIS) project which will be installed at RIKEN's fragment separator, BigRIPS. A novel implementation of differential pumping, in combination with a sextupole ion beam guide (SPIG), has been developed. A few small scroll pumps create a pressure difference from 1000 hPa–10−3 Pa within a geometry drastically miniaturized compared to conventional systems. This system can utilize a large exit hole for fast evacuation times, minimizing the decay loss for short-lived nuclei during extraction from a buffer gas cell, while sufficient gas cell pressure is maintained for stopping high energy RI-beams. In spite of the motion in a dense pressure gradient, the photo-ionized ions inside the gas cell are ejected with an assisting force gas jet and successfully transported to a high-vacuum region via SPIG followed by a quadrupole mass separator. Observed behaviors agree with the results of gas flow and Monte Carlo simulations.