Max Planck: closures will damage German science.
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Biomedical subjects
Publications and source records attributed to G J Wasserburg.
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On the basis of anomalous isotopic compositions of oxygen and magnesium, 14 oxide grains from two primitive meteorites (Bishunpur and Semarkona) have been identified as circumstellar condensates. One corundum grain has a high 18O/16O ratio and isotopic compositions of magnesium, calcium, and titanium that are compatible with a formation in ejecta of a type II supernova that was about 15 times the mass of the sun. The other grains have oxygen, magnesium, and titanium compositions that are consistent with a formation around asymptotic giant branch (AGB) stars with a range of mass and initial composition. The large range of aluminum/magnesium in circumstellar corundum and spinel is considered to reflect various stages of back-reaction between condensed corundum and gaseous magnesium in cooling stellar ejecta.
A suite of morphologically distinctive silicon carbide (SiC) grains from the Orgueil and Murchison carbonaceous chondrite meteorites contains Si and C of highly anomalous isotopic composition. All of the SiC grains in this suite are characterized by a distinctive platy morphology and roughly developed hexagonal crystal forms that allow them to be distinguished from other types of SiC found in the host meteorites. The delta 29Si and delta 30Si values of individual SiC crystals deviate from those of normal solar material by more than 100%, while the delta 13C values range from 150 to 5200%. Isotopically normal C and Si are not found in any of these SiC crystals. The SiC grains belonging to this morphological suite are isotopically distinct from fine-grained SiC aggregates and other morphological types of SiC in unequilibrated meteorites. The 29Si/28Si and 30Si/28Si ratios of these platy grains are well correlated and define a linear array that does not pass through the composition of normal, solar Si. This behavior contrasts sharply with the diverse and poorly correlated Si isotopic compositions shown by the total SiC population. We suggest that the distinctive morphological characteristics and comparatively simple Si isotope systematics identify the platy SiC crystals as a genetically related family, formed around a single, isotopically heterogeneous presolar star or an association of related stars. The enrichments in 13C and the Si isotope systematics of the platy SiC are broadly consistent with theoretical models of nucleosynthesis in low-mass, carbon stars on the asymptotic giant branch. The Si isotope array most plausibly reflects mixing between 28Si-rich material, inherited from a previous generation of stars, and material enriched in 29Si and 30Si, produced in intershell regions by neutron capture during He-burning. 13C is also produced in intershell regions by proton reactions on 12C seed nuclei and is carried with s-process nuclei to the stellar envelope by convection which penetrates down to the He shell. The absence of a correlation between the Si and C isotopic compositions of the SiC suggests either episodic condensation of SiC, extending over several thermal pulses, in the atmosphere of a single star, or derivation of the SiC from several stars characterized by different rates of 13C production. In the multiple star scenario, the linear correlation of the 29Si/28Si and 30Si/28Si ratios among the platy SiC indicates that these stars evolved from a common Si seed composition under similar conditions of neutron-capture nucleosynthesis. The 29Si/30Si ratio of the SiC, inferred by us to be produced by neutron capture in the stellar interior, is distinct from values calculated from models of nucleosynthesis in AGB stars.
An important but poorly understood factor that affects diffusion rates is the role of speciation during diffusion of a multi-species component. The diffusion of such a component is complicated by the different diffusion coefficient of each species and the interconversion reactions among the species. These complexities can be treated by a diffusion equation that incorporates the diffusive fluxes of all species contributing to the concentration of the component. The effects of speciation on the diffusion of the component can be investigated experimentally in some simple cases by measuring concentration profiles of all species developed during diffusion experiments or by studying some of their other consequences. Experimental data on water diffusion in rhyolitic glasses indicate that although dissolved water is present as two species, H2O molecules and OH groups, molecular H2O is the dominant diffusing species at very low to high water concentrations. This explains the apparently complex behavior of water diffusion. Experimental data on oxygen diffusion in some silicates using 18O tracers in the form of H2(18O) are consistent with the idea that 18O transport is dominated by diffusion of H2O molecules even at lower water contents (ppm or less). This explains why oxygen transport depends on the presence of water and generally depends on water fugacity linearly. For this mode of oxygen transport, there is a simple theoretical relationship between the effective total oxygen diffusion coefficient and the total water diffusion coefficient that is a function of only the water concentration of the silicate at low water content. This relationship appears to describe quantitatively the existing data over a wide range in water contents and diffusion coefficients in several phases.
Water dehydration experiments on rhyolitic glasses have been carried out at 400-550 degrees C under a N2 atmosphere. Concentration profiles of both H2O molecules and OH groups were measured by Fourier transform infrared spectroscopy. As found in previous studies of water diffusion in rhyolitic melts, the measured total water concentration profiles do not match expectations based on a single constant diffusion coefficient for total water. The diffusion of total water is described by considering the diffusion of both H2O molecules and OH groups and the reaction between them. The concentration relationship between the two species has been obtained from direct infrared measurement on quenched experimental charges. The quench is inferred to be rapid enough to preserve concentrations of both species at experimental temperature based on experimental results designed to examine reaction kinetics. The measured species concentrations along diffusion profiles show that local equilibrium between H2O and OH is approximately reached at high temperatures and high water contents. However, at lower water content or lower temperature, local equilibrium is not reached. In treating the diffusion problem, this disequilibrium effect is partially compensated by using empirical relationships between H2O and OH concentrations based on measurements, instead of using an equilibrium relationship. It is thus possible to obtain diffusion coefficients for both species from their concentration profiles. The diffusion coefficient of OH is found to be negligible compared to that of H2O at 403-530 degrees C (DOH < 0.02 DH2O and could be much smaller); i.e., H2O is the dominant diffusing species even at total water concentration as low as 0.2 wt%. The variation of OH concentration along the diffusion profile is inferred to be due to the local interconversion between OH groups and H2O molecules; the reaction also provides the diffusing H2O species. DH20 values are found to vary by less than a factor of 2 over a total water concentration range of 0.2 to 1.7 wt%. This simple model, coupled with the assumption of local equilibrium between H2O and OH, yields a very good fit to the data from diffusion-couple experiments of LAPHAM et al. (1984) at 850 degrees C. When our data are combined with DH2O obtained from that fit, DH2O (in m2/s) is given by: ln DH2O = (-14.59 +/- 1.59) - (103000 +/- 5000) / RT; 673 K < or = T < or = 1123 K, where T is temperature in K and R is the gas constant in J K-1 mol-1. This equation also approximates well DH2O values calculated from previous measurements of concentration-dependent bulk water diffusion coefficients of KARSTEN et al. (1982). The diffusion of H2O is also compared to the diffusion of the noble gas elements. The activation energy for diffusion in rhyolitic glasses is well correlated with neutral species radii of He, Ne, H2O, and Ar. This supports the contention that the diffusing species for "water" is neutral molecular H2O. The role of speciation may also be important in understanding the diffusion of many other multi-species components, and the effect can be treated in a similar fashion as that during water diffusion.
The exact solutions for the isotopic compositions and the concentrations of the two-reservoir model for mantle-crust evolution are given for arbitrary rates of crustal growth and of back flow to the mantle. The critical parameters are the chemical fractionation factors for crustal growth and refluxing and the integrated fractional mass-removal rates from the crust and the mantle. For the case where refluxing is proportional to crustal growth, all the solutions reduce to simple analytic expressions. The expression for the mean age of the mass of the crust with refluxing is given. If refluxing is significant, the model shows that highly incompatible elements have short residence times in the mantle. With plausible concentration values, material balance implies that the continents were derived from only a small fraction of the mantle.
The initial isotopic compositions of Nd and Sr in basalts from the Central Siberian Plateau and other major continental flood basalts are reported. The continental flood basalts appear to be the product of partial melting of mantle sources that consist of relatively primitive undifferentiated material and are clearly distinct from midocean ridge basalts, which sample mantle reservoirs that have been modified by extraction of continental crust earlier in earth history. These observations provide fundamental constraints on models of mantle structure and dynamics. Isotopic effects of crustal contamination are clearly recognizable in some continental flood basalts, but these effects can be distinguished from isotopic patterns inherited from the mantle magma sources.
A simplified model of earth structure based on the Nd and Sr isotopic characteristics of oceanic and continental tholeiitic flood basalts is presented, taking into account the motion of crustal plates and a chemical balance for trace elements. The resulting structure that is inferred consists of a lower mantle that is still essentially undifferentiated, overlain by an upper mantle that is the residue of the original source from which the continents were derived.