Progress of ultra trace determination of technetium using laser resonance ionization mass spectrometry.

Laser resonance ionization mass spectrometry (RIMS) represents one of the most sensitive and selective techniques for ultra trace determination of long-lived radioisotopes. The isotope (99g)Tc constitutes a specific candidate of high relevance concerning its environmental behavior as well as fundamental research applications. Based on the recent precision determination of the ionization potential of technetium by laser resonance ionization, refined resonant optical excitation pathways have been derived for analytical determination of ultra trace amounts of (99g)Tc by laser mass spectrometric approaches. The state of the art and the specifications of RIMS-based ultra trace determination for (99g)Tc, leading to a level of detection of ε ≈ 3 × 10(-4) atoms (3 µBq), are reported.

Resonance ionization mass spectrometry of ion beam sputtered neutrals for element- and isotope-selective analysis of plutonium in micro-particles.

Micro-particles containing actinides are of interest for risk assessments of contaminated areas, nuclear forensic analyses, and IAEA as well as Euratom safeguards programs. For their analysis, secondary ion mass spectrometry (SIMS) has been established as the state-of-the-art standard technique. In the case of actinide mixtures within the particles, however, SIMS suffers from isobaric interferences (e.g., (238)U/(238)Pu, (241)Am/(241)Pu). This can be eliminated by applying resonance ionization mass spectrometry which is based on stepwise resonant excitation and ionization of atoms with laser light, followed by mass spectrometric detection of the produced ions, combining high elemental selectivity with the analysis of isotopic compositions. This paper describes the instrumental modifications for coupling a commercial time-of-flight (TOF)-SIMS apparatus with three-step resonant post-ionization of the sputtered neutrals using a high-repetition-rate (kHz) Nd:YAG laser pumped tunable titanium:sapphire laser system. Spatially resolved ion images obtained from actinide-containing particles in TOF-SIMS mode demonstrate the capability for isotopic and spatial resolution. Results from three-step resonant post-ionization of bulk Gd and Pu samples successfully demonstrate the high elemental selectivity of this process.

Ultratrace analysis and isotope ratio measurements of long-lived radioisotopes by resonance ionization mass spectrometry (RIMS).

Resonance Ionization Mass Spectrometry (RIMS) is a sensitive and selective method for ultratrace analysis of long-lived radioisotopes and isotope ratio measurements. It provides extremely high isobaric suppression and good overall efficiency. The experimental limits of detection are as low as 10(6) atoms per sample and isotopic selectivities of 5x10(12) have been obtained. The widespread potential of RIMS, using different experimental arrangements, is demonstrated for the determination of the radiotoxic isotopes Pu-238 to Pu-244 and Sr-89/Sr-90 in various environmental samples as well as for Ca-41 in nuclear reactor components and biomedical samples.

First observation of atomic levels for the element fermium (Z=100).

The atomic level structure of the element fermium was investigated for the first time using a sample of 2.7x10(10) atoms of the isotope 255Fm with a half-life of 20.1 h. The atoms were evaporated from a filament and stored in the argon buffer gas of an optical cell. Atomic levels were sought by the method of resonance ionization spectroscopy using an excimer-dye-laser combination. Two atomic levels were found at wave numbers (25 099.8+/-0.2) and (25 111.8+/-0.2) cm(-1). Partial transition rates to the 5f(12)7s(2) (3)H(e)(6) ground state have been determined from their saturation characteristics. Multiconfiguration Dirac-Fock calculations suggest that the leading orders of these levels could be the 5f(12)7s7p (5)I(o)(6) and 5f(12)7s7p (5)G(o)(5) terms.