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Superconductivity caused by the pairing of plutonium 5f Eelectrons in PuCoGa5.

On the basis of electronic structure calculations we identify the superconductivity in the novel, high-temperature superconductor PuCoGa5 to be caused by the pairing of Pu 5f electrons. Assuming delocalized Pu 5f states, we compute theoretical crystallographic constants very near to the experimental ones, and the calculated specific heat coefficient compares reasonably to the measured coefficient. The theoretical Fermi surface is quasi-two-dimensional and the material appears to be close to a magnetic phase instability.

Journal Article↗

Failure of Russell-Saunders coupling in the 5f states of plutonium.

Using high energy-electron energy loss spectroscopy, transmission electron microscopy, and synchrotron-radiation-based x-ray absorption spectroscopy, we provide the first experimental evidence that Russell-Saunders (LS) coupling fails for the 5f states of Pu. These results support the assumption that only the use of jj or intermediate coupling is appropriate for the 5f states of Pu. High energy-electron energy loss spectroscopy experiments were performed by use of a transmission electron microscope and are coupled with image and diffraction data; therefore, the measurements are completely phase specific.

Journal Article↗

Experimental electronic heat capacities of alpha- and delta-plutonium: heavy-fermion physics in an element.

We have measured the heat capacities of delta-Pu0.95Al0.05 and alpha-Pu over the temperature range 2-303 K. The availability of data below 10 K plus an estimate of the phonon contribution to the heat capacity based on recent neutron-scattering experiments on the same sample enable us to make a reliable deduc-tion of the electronic contribution to the heat capacity of delta-Pu0.95Al0.05; we find gamma=64+/-3 mJ K(-2) mol(-1) as T-->0. This is larger than that of any element and large enough for delta-Pu0.95Al0.05 to be classed as a heavy-fermion system. By contrast, gamma=17+/-1 mJ K(-2) mol(-1) in alpha-Pu. Two distinct anomalies are seen in the electronic contribution to the heat capacity of delta-Pu0.95Al0.05, one or both of which may be associated with the formation of the alpha(')-martensitic phase. We suggest that the large gamma value of delta-Pu0.95Al0.05 may be caused by proximity to a quantum-critical point.

Journal Article↗

Unusual phonon softening in delta-phase plutonium.

The phonon density of states and adiabatic sound velocities were measured on fcc-stabilized 242Pu0.95Al0.05. The phonon frequencies and sound velocities decrease considerably (soften) with increasing temperature despite negligible thermal expansion. The frequency softening of the transverse branch along the [111] direction is anomalously large ( approximately 30%) and is very sensitive to alloy composition. The large magnitude of the phonon softening is not observed in any other fcc metals and may arise from an unusual temperature dependence of the electronic structure in this narrow 5f-band metal.

Journal Article↗

Effects of plutonium on soil microorganisms.

As a first phase in an investigation of the role of the soil microflora in Pu complex formation and solubilization in soil, the effects of Pu concentration, form, and specific activity on microbial types, colony-forming units, and CO(2) evolution rate were determined in soils amended with C and N sources to optimize microbial activity. The effects of Pu differed with organism type and incubation time. After 30 days of incubation, aerobic sporeforming and anaerobic bacteria were significantly affected by soil Pu levels as low as 1 mug/g when Pu was added as the hydrolyzable Pu(NO(3))(4) (solubility, <0.1% in soil). Other classes of organisms, except the fungi, were significantly affected at soil Pu levels of 10 mug/g. Fungi were affected only at soil Pu levels of 180 mug/g. Soil CO(2) evolution rate and total accumulated CO(2) were affected by Pu only at the 180 mug/g level. Because of the possible role of resistant organisms in complex formation, the mechanisms of effects of Pu on the soil fungi were further evaluated. The effect of Pu on soil fungal colony-forming units was a function of Pu solubility in soil and Pu specific activity. When Pu was added in a soluble, complexed form [Pu(2)(diethylenetriaminepentaacetate)(3)], effects occurred at Pu levels of 1 mug/g and persisted for at least 95 days. Toxicity was due primarily to radiation effects rather than to chemical effects, suggesting that, at least in the case of the fungi, formation of Pu complexes would result primarily from ligands associated with normal (in contrast to chemically-induced) biochemical pathways.

Journal Article↗

Liver cancers in Mayak workers.

Liver cancer mortality risks were evaluated in 11,000 workers who started working at the "Mayak" Production Association in 1948-1958 and who were exposed to both internally deposited plutonium and external gamma radiation. Comparisons with Russian liver cancer incidence rates indicate excess risk, especially among those with detectable plutonium body burdens and among female workers in the plutonium plant. Comparisons within the Mayak worker cohort which evaluate the role of plutonium body burden with adjustment for cumulative external dose indicate excess risk among workers with burdens estimated to exceed 7.4 kBq (relative risk = 17; 95% CI = 8. 0-36) and among workers in the plutonium plant who did not have routine plutonium monitoring data based on urine measurements (relative risk = 2.8; 95% CI = 1.3-6.2). In addition, analyses treating the estimated plutonium body burden as a continuous variable indicate increasing risk with increasing burden (P < 0.001). Relative risks tended to be higher for females than for males, probably because of the lower baseline risk and the higher levels of plutonium measured in females. Because of limitations in current plutonium dosimetry, no attempt was made to quantify liver cancer risks from plutonium in terms of organ dose, and risk from external dose could not be reliably evaluated.

Body Burden↗

Risks of fatal cancer from inhalation of 239,240plutonium by humans: a combined four-method approach with uncertainty evaluation.

The risk per unit dose to the four primary cancer sites for plutonium inhalation exposure (lung, liver, bone, bone marrow) is estimated by combining the risk estimates that are derived from four independent approaches. Each approach represents a fundamentally different source of data from which plutonium risk estimates can be derived. These are: (1) epidemiologic studies of workers exposed to plutonium; (2) epidemiologic studies of persons exposed to low-LET radiation combined with a factor for the relative biological effectiveness (RBE) of plutonium alpha particles appropriate for each cancer site of concern; (3) epidemiologic studies of persons exposed to alpha-emitting radionuclides other than plutonium; and (4) controlled studies of animals exposed to plutonium and other alpha-emitting radionuclides extrapolated to humans. This procedure yielded the following organ-specific estimates of the distribution of mortality risk per unit dose from exposure to plutonium expressed as the median estimate with the 5th to 95th percentiles of the distribution in parentheses: lung 0.13 Gy(-1) (0.022-0.53 Gy(-1)); liver 0.057 Gy(-1) (0.011-0.47 Gy(-1)); bone 0.0013 Gy(-1) (0.000060-0.025 Gy(-1)); bone marrow (leukemia), 0.013 Gy(-1) (0.00061-0.05 Gy(-1)). Because the different tissues do not receive the same dose following an inhalation exposure, the mortality risk per unit intake of activity via inhalation of a 1-microm AMAD plutonium aerosol also was determined. To do this, inhalation dose coefficients based on the most recent ICRP models and accounting for input parameter uncertainties were combined with the risk coefficients described above. The following estimates of the distribution of mortality risk per unit intake were determined for a 1-microm AMAD plutonium aerosol with a geometric standard deviation of 2.5: lung 5.3 x 10(-7) Bq(-1) (0.65-35 x 10(-7) Bq(-1)), liver 1.2 x 10(-7) Bq(-1) (0.091-20 x 10(-7) Bq(-1)), bone 0.11 x 10(-7) Bq(-1) (0.0030-4.3 x 10(-7) Bq(-1)), bone marrow (leukemia) 0.049 x 10(-7) Bq(-1) (0.0017-0.59 x 10(-7) Bq(-1)). The cancer mortality risk for all sites was estimated to be 10 x 10(-7) Bq(-1) (2.1-55 x 10(-7) Bq(-1))--a result that agrees very well with other recent estimates. The large uncertainties in the risks per unit intake of activity reflect the combined uncertainty in the dose and risk coefficients.

Administration, Inhalation↗

The uptake and redistribution of 241pu within the gonads.

Male and female hamsters and a female rabbit were injected with 241Pu citrate. The hamsters were killed serially at 15 min, 2 hours, 1 day and 10 days after injection, and the rabbit 1 week after injection. The gonads were examined for 241Pu by tissue-section autoradiography. Soon after injection the plutonium was concentrated by the contents of atretic Graafian follicles and by thecal rings in the ovary, but was found to be dispersed throughout the testes. It is suggested that the disperse distribution in the testes which is only seen soon after injection may be an artefact of tissue processing. One day after injection, plutonium was accumulated by macrophages in both the follicles of the ovary and in the interstitial tissue of the testes. Macrophages containing plutonium later migrated away from the aretic ovarian follicles towards the ovarian medulla. This pattern of distribution and redistribution in the ovary is regarded as likely to lower the effective dose from a-emitting plutonium isotopes to the viable oocytes. No migration of macrophages was seen in the testes. Histochemical staining methods revealed the presence of acid protoglycans, including chondroitin sulphate, and glycoproteins at the sites of plutonium concentration in the ovary. These molecules are regarded as likely receptor sites for plutonium. In the testes no acidic carbohydrates were found, and it is suggested that the initial binding site for plutonium may be a compound lipid. This was deduced from the apparent inability of the interstitial tissue of the testes to bind plutonium in situ.

Animals↗

Bone cancers in Mayak workers.

Bone cancer mortality risks were evaluated in 11,000 workers who started working at the "Mayak" Production Association in 1948-1958 and who were exposed to both internally deposited plutonium and external gamma radiation. Comparisons with Russian and U.S. general population rates indicate excess mortality, especially among females, plutonium plant workers, and workers with external doses exceeding 1 Sv. Comparisons within the Mayak worker cohort, which evaluate the role of plutonium body burden with adjustment for cumulative external dose, indicate excess mortality among workers with burdens estimated to exceed 7.4 kBq (relative risk = 7.9; 95% CI = 1.6-32) and among workers in the plutonium plant who did not have routine plutonium monitoring data based on urine measurements (relative risk = 4.1; 95% CI = 1.2-14). In addition, analyses treating the estimated plutonium body burden as a continuous variable indicate increasing risk with increasing burden (P < 0.001). Because of limitations in current plutonium dosimetry, no attempt was made to quantify bone cancer risks from plutonium in terms of organ dose, and risk from external dose could not be reliably evaluated.

Adult↗