Size-fractionated plutonium isotopes in a coastal environment.

We have examined the distribution of individual Pu isotopes (239Pu, 240Pu, and 241Pu) in seawater from the Gulf of Maine (GOM). Samples were size-fractionated with a 1 kD cross-flow ultrafiltration (CFF) membrane. Subfractioned samples were radiochemically purified and Pu isotopes were analyzed using a three-stage thermal ionization mass spectrometer (TIMS). To our knowledge, this is the first time that both size class and Pu isotopic data have been obtained for seawater samples. Within measurement uncertainties a single 240Pu/239Pu atom ratio of 0.18 was found for all sample collection depths and sample size fractions. This signifies a current, single Pu source in GOM waters, namely global fallout, and suggests that no measurable isotopic fractionation occurred during CFF processing. The majority of Pu was found in the low molecular weight fraction (< 1 kD). Colloidal Pu varied from 8% of the total in surface waters to < 1% in the deepest (250 m) seawater sample. Evidence suggests that the vertical distribution of Pu in GOM is primarily controlled by conservative mixing processes. The high Pu fraction found in the low molecular size fraction implies that most of the Pu is in the non-particle-reactive oxidized fraction, and is consistent with the conservative Pu behavior. The activity levels are in agreement with other studies which show a slow decrease in Pu with time due to continued mixing and relatively slow particle removal.

The fall, recovery, orbit, and composition of the Tagish Lake meteorite: a new type of carbonaceous chondrite.

The preatmospheric mass of the Tagish Lake meteoroid was about 200,000 kilograms. Its calculated orbit indicates affinity to the Apollo asteroids with a semimajor axis in the middle of the asteroid belt, consistent with a linkage to low-albedo C, D, and P type asteroids. The mineralogy, oxygen isotope, and bulk chemical composition of recovered samples of the Tagish Lake meteorite are intermediate between CM and CI meteorites. These data suggest that the Tagish Lake meteorite may be one of the most primitive solar system materials yet studied.

Trace detection of krypton using laser-induced fluorescence.

Highly sensitive detection of neutral Kr atoms was accomplished by the use of laser-induced fluorescence. In one experiment, Kr at 40 parts per 10(12) in He was detected at a signal-to-noise ratio of 500 by time-resolved fluorescence measurements. The Kr metastable 1s(5) level was populated by cascade after two-photon excitation to the 2p(6) level by the frequency-tripled output of a pulsed single-longitudinalmode dye laser. After a delay, when scattered laser light and cascade resonance fluorescence became negligible, trace quantities of Kr were detected by the use of a pulsed-laser pumping scheme. In a related experiment, (78)Kr/(86)Kr isotope ratios ranging from 1 to 0.1 were measured with a resonant isotopic depletion technique first proposed by Makarov [Sov. J. Quantum Electron. 13, 722 (1983)]. The (86)Kr metastable population was selectively depleted by optical pumping to a higher-lying state that relaxed to the ground state by means of radiative cascade. After the (78)Kr/(86)Kr ratio of metastables had been enriched by a factor of 10, the (78)Kr population was probed by pulsed excitation. Premixed (78)Kr/(86)Kr ratios were measured to within an accuracy of 10%, even for unresolved, Doppler-broadened transitions.