Systematics of the odd-even effect in the resonance ionization of Os and Ti

Measurements of the odd-even effect in the mass spectrometric analysis of Ti and Os isotopes by resonance ionization mass spectrometry have been performed for ΔJ = + 1, 0 and -1 transitions. Under saturating conditions of the ionization and for ΔJ = + 1 transitions odd-even effects are reduced below the 0.5% level. Depending on the polarization state of the laser large odd isotope enrichments are observed for ΔJ = 0 and -1 transitions which can be reduced below the 0.5% level by depolarization of the laser field

Laser-induced isotopic selectivity in the resonance ionization of Os

Isotope selective effects in resonance ionization mass spectrometry (RIMS) pose a potentially serious limitation to the application of this technique to the precise and reproducible measurement of isotope ratios. In order to identify some of the underlying causes of isotope selectivity in RIMS and to establish procedures for minimizing these effects, we investigated laser-induced isotope selectivity in the resonance ionization of Os. A single-color, one-photon resonant ionization scheme was used for several different transitions to produce Os photoions from a thermal atomization source. Variations in Os isotope ratios were studied as a function of laser parameters such as wavelength, bandwidth, power and polarization state. Isotope selectivity is strongly dependent on laser power and wavelength, even when the bandwidth of the laser radiation is much larger than the optical isotope shift. Variations in the ^(190)Os/^(188)Os ratio of ≈20% for a detuning of 0.8 cm^(−1) were observed on a transition with a small oscillator strength. Large even—odd isotope selectivity with a 13% depletion of ^(189)Os was observed on a ΔJ = +1 transition at low laser intensity; the odd mass Os isotopes are systematically depleted. For ΔJ = −1 and 0 transitions the isotope selectivity was reduced by polarization scrambling and for strongly saturating conditions. A technique employing the wavelength dependence of even—even isotope selectivity as an internal wavelength standard was developed to permit accurate and reproducible wavelength adjustment of the laser radiation. This technique provides control over laser-induced isotope selectivity for single-color ionization and enabled us to obtain reproducible measurements of ^(192)Os/^(188)Os and ^(189)Os/^(190)Os ratios in the saturation regime for a ΔJ = +1 transition with a precision of better than 0.5%. The application of this wavelength-tuning procedure should significantly improve the quality of RIMS isotope ratio data for many elements

Systematics of isotope ratio measurements with resonant laser photoionization sources

Sources of laser-induced even-even and odd-even isotopic selectivity in the resonance ionization mass spectroscopy of Os and Ti have been investigated experimentally for various types of transitions. A set of conditions with regard to laser bandwidth and frequency tuning, polarization state and intensity was obtained for which isotopic selectivity is either absent or reduced below the 2 % level

Laser-induced isotopic effects in titanium resonance ionization

Titanium isotope ratios have been measured by resonance ionization mass spectrometry (RIMS) with special emphasis on the nature of laser-induced isotopic selectivity. A pronounced wavelength dependence of even mass isotope ratios is caused by large nuclear volume effects near the magic neutron number 28 in ^(50)Ti . Optical isotope shifts, ranging from 0.07 to 0.21 cm^(-l), between ^(50)Ti and ^(46)Ti were measured for several transitions. The ^(50)Ti/^(46)Ti and ^(48)Ti/^(46)Ti ratios, nevertheless, exhibited only mass-dependent fractionation, in which the lighter Ti isotopes were enriched by ~2.5%/amu, when the laser operating parameters were properly controlled. Odd-even mass isotopic selectivity in the resonant ionization process was also examined for several transitions as a function of the laser polarization state and intensity. Under saturating conditions for a ΔJ= +1 transition and a high degree of laser depolarization for a ΔJ = 0 transition, the odd-even isotopic enhancement was reduced below the 2% level. The Ti isotope data agree with our previous results for Os and indicate that, by a careful choice of resonance transitions and laser operating parameters, isotope ratios can be measured accurately and reliably with RIMS

An experimental study of Mg self-diffusion in spinel

Mg isotope heterogeneity, both between coexisting spinel and silicates and among spinels, is a prominent feature of Plagioclase-Olivine Inclusions (POIs) (1). The preservation of isotopic heterogeneity and relict spinel (Sp) in inclusions with igneous textures indicates that the thermal event which partially melted the precursor material either had too low a temperature or was too brief to allow Mg isotope homogenization between Sp and the melt. Since the temperature history required to homogenize Mg isotopes depends on the diffusion rate of Mg in Sp, we designed experiments using an isotope tracer method to determine this critical rate (2)

Ni-Pt-Ge-Rich Fremdlinge; indicators of a turbulent early solar nebula

One of the oddest aspects of CAis is the presence of Fremdlinge-complex aggregates of refractory metal alloys and volatile oxides and sulfides. In a series of recent studies of Fremdlinge we have provided evidence that (I) they are not isotopically anomalous and presumably formed in the solar nebula, (2) they were formed as solid objects before any of the major phases in CAis, (3) processes involved in their formation , prior to incorporation in CAis. included oxidation and reduction both at high and low temperatures, and (4) their phase assemblages and reaction textures place strict constraints on the maximum temperatures and cooling rates during CAl formation (Armstrong et al., 1984, 1985a, 1985b; Hutcheon et al., 1985)

Fremdlinge in Leoville and Allende CAI – Clues to Post-Formation Cooling and Alteration

Fremdlinge are perhaps the most exotic and least understood objects in CAI and their very existence places severe constraints regarding formation and cooling histories of the host CAI. Following the discovery and description of Willy, which appears to be an "Ur-Fremdling" or prototype for smaller Fremdlinge in CAI, we have begun a systematic study of CAI of different petrographic types to see if the Fremdlinge are consistent with a common mode of formation and differing degrees of reprocessing. Fifteen type B I, B2, and compact A CAI from Allende and Leoville were selected. The relative abundance of Fremdlinge varies dramatically among CAI, however some CAI of each type and from each meteorite contain abundant Fremdlinge. The range of phase assemblages and mineral chemistries of Fremdlinge from Allende and Leoville is very similar suggesting that the parent sources for Fremdlinge were quite similar. Chemically and texturally, Fremdlinge grade continuously from complex, heterogeneous Willy-like objects to altered, homogeneous metal nuggets. Some complex Fremdlinge like Willy were found in B1 CAI; none were observed in B2 CAI