Dynamics of supercooled water in highly compacted clays studied by neutron scattering

The freezing behavior of water confined in compacted charged and uncharged clays (montmorillonite in Na-and Ca-forms, illite in Na-and Ca-forms, kaolinite and pyrophyllite) was investigated by neutron scattering. Firstly, the amount of frozen (immobile) water was measured as a function of temperature at the IN16 backscattering spectrometer, Institute Laue-Langevin (ILL). Water in uncharged, partly hydrophobic (kaolinite) and fully hydrophobic (pyrophyllite) clays exhibited a similar freezing and melting behavior to that of bulk water. In contrast, water in charged clays which are hydrophilic could be significantly supercooled. To observe the water dynamics in these clays, further experiments were performed using quasielastic neutron scattering. At temperatures of 250, 260 and 270 K the diffusive motion of water could still be observed, but with a strong reduction in the water mobility as compared with the values obtained above 273 K. The diffusion coefficients followed a non-Arrhenius temperature dependence well described by the Vogel-Fulcher-Tammann and the fractional power relations. The fits revealed that Na-and Ca-montmorillonite and Ca-illite have similar Vogel-Fulcher-Tammann temperatures (T-VFT, often referred to as the glass transition temperature) of similar to 120 K and similar temperatures at which the water undergoes the 'strong-fragile' transition, T-s similar to 210 K. On the other hand, Na-illite had significantly larger values of T-VFT similar to 180 K and T-s similar to 240 K. Surprisingly, Ca-illite has a similar freezing behavior of water to that of montmorillonites, even though it has a rather different structure. We attribute this to the stronger hydration of Ca ions as compared with the Na ions occurring in the illite clays.

Coupled W–Os–Pt isotope systematics in IVB iron meteorites: In situ neutron dosimetry for W isotope chronology

Tungsten isotope compositions of magmatic iron meteorites yield ages of differentiation that are within ±2 Ma of the formation of CAIs, with the exception of IVB irons that plot to systematically less radiogenic compositions yielding erroneously old ages. Secondary neutron capture due to galactic cosmic ray (GCR) irradiation is known to lower the ε182W of iron meteorites, adequate correction of which requires a measure of neutron dosage which has not been available, thus far. The W, Os and Pt isotope systematics of 12 of the 13 known IVB iron meteorites were determined by MC-ICP-MS (W, Os, Pt) and TIMS (Os). On the same dissolutions that yield precise ε182W, stable Os and Pt isotopes were determined as in situ neutron dosimeters for empirical correction of the ubiquitous cosmic-ray induced burn-out of 182W in iron meteorites. The W isotope data reveal a main cluster with ε182W of ∼−3.6, but a much larger range than observed in previous studies including irons (Weaver Mountains and Warburton Range) that show essentially no cosmogenic effect on their ε182W. The IVB data exhibits resolvable negative anomalies in ε189Os (−0.6ε) and complementary ε190Os anomalies (+0.4ε) in Tlacotepec due to neutron capture on 189Os which has approximately the same neutron capture cross section as 182W, and captures neutrons to produce 190Os. The least irradiated IVB iron, Warburton Range, has ε189Os and ε190Os identical to terrestrial values. Similarly, Pt isotopes, which are presented as ε192Pt, ε194Pt and ε196Pt range from +4.4ε to +53ε, +1.54ε to −0.32ε and +0.73ε to −0.20ε, respectively, also identify Tlacotepec and Dumont as the most GCR-damaged samples. In W–Os and W–Pt isotope space, the correlated isotope data back-project toward a 0-epsilon value of ε192Pt, ε189Os and ε190Os from which a pre-GCR irradiation ε182W of −3.42±0.09 (2σ) is derived. This pre-GCR irradiation ε182W is within uncertainty of the currently accepted CAI initial ε182W. The Pt and Os isotope correlations in the IVB irons are in good agreement with a nuclear model for spherical irons undergoing GCR spallation, although this model over-predicts the change of ε182W by ∼2×, indicating a need for better W neutron capture cross section determinations. A nucleosynthetic effect in ε184W in these irons of −0.14±0.08 is confirmed, consistent with the presence of Mo and Ru isotope anomalies in IVB irons. The lack of a non-GCR Os isotope anomaly in these irons requires more complex explanations for the production of W, Ru and Mo anomalies than nebular heterogeneity in the distribution of s-process to r-process nuclides.

Neutron capture on Pt isotopes in iron meteorites and the Hf–W chronology of core formation in planetesimals

The short-lived 182Hf–182W isotope system can provide powerful constraints on the timescales of planetary core formation, but its application to iron meteorites is hampered by neutron capture reactions on W isotopes resulting from exposure to galactic cosmic rays. Here we show that Pt isotopes in magmatic iron meteorites are also affected by capture of (epi)thermal neutrons and that the Pt isotope variations are correlated with variations in 182W/184W. This makes Pt isotopes a sensitive neutron dosimeter for correcting cosmic ray-induced W isotope shifts. The pre-exposure 182W/184W derived from the Pt–W isotope correlations of the IID, IVA and IVB iron meteorites are higher than most previous estimates and are more radiogenic than the initial 182W/184W of Ca–Al-rich inclusions (CAI). The Hf–W model ages for core formation range from +1.6±1.0 million years (Ma; for the IVA irons) to +2.7±1.3 Ma after CAI formation (for the IID irons), indicating that there was a time gap of at least ∼1 Ma between CAI formation and metal segregation in the parent bodies of some iron meteorites. From the Hf–W ages a time limit of <1.5–2 Ma after CAI formation can be inferred for the accretion of the IID, IVA and IVB iron meteorite parent bodies, consistent with earlier conclusions that the accretion of differentiated planetesimals predated that of most chondrite parent bodies.

Thermal neutron capture effects in radioactive and stable nuclide systems

Neutron capture effects in meteorites and lunar surface samples have been successfully used in the past to study exposure histories and shielding conditions. In recent years, however, it turned out that neutron capture effects produce a nuisance for some of the short-lived radionuclide systems. The most prominent example is the 182Hf-182W system in iron meteorites, for which neutron capture effects lower the 182W/184W ratio, thereby producing too old apparent ages. Here, we present a thorough study of neutron capture effects in iron meteorites, ordinary chondrites, and carbonaceous chondrites, whereas the focus is on iron meteorites. We study in detail the effects responsible for neutron production, neutron transport, and neutron slowing down and find that neutron capture in all studied meteorite types is not, as usually expected, exclusively via thermal neutrons. In contrast, most of the neutron capture in iron meteorites is in the epithermal energy range and there is a significant contribution from epithermal neutron capture even in stony meteorites. Using sophisticated particle spectra and evaluated cross section data files for neutron capture reactions we calculate the neutron capture effects for Sm, Gd, Cd, Pd, Pt, and Os isotopes, which all can serve as neutron-dose proxies, either in stony or in iron meteorites. In addition, we model neutron capture effects in W and Ag isotopes. For W isotopes, the GCR-induced shifts perfectly correlate with Os and Pt isotope shifts, which therefore can be used as neutron-dose proxies and permit a reliable correction. We also found that GCR-induced effects for the 107Pd-107Ag system can be significant and need to be corrected, a result that is in contrast to earlier studies.

Determination of the Weak Axial Vector Coupling λ=g_{A}/g_{V} from a Measurement of the β-Asymmetry Parameter A in Neutron Beta Decay

We report on a new measurement of the neutron beta-asymmetry parameter A with the instrument \perkeo. Main advancements are the high neutron polarization of P=99.7(1) from a novel arrangement of super mirror polarizers and reduced background from improvements in beam line and shielding. Leading corrections were thus reduced by a factor of 4, pushing them below the level of statistical error and resulting in a significant reduction of systematic uncertainty compared to our previous experiments. From the result A0=−0.11996(58), we derive the ratio of the axial-vector to the vector coupling constant λ=gA/gV=−1.2767(16)

A convolution model for energy transport in a therapeutic fast neutron beam

A three-dimensional model has been proposed that uses Monte Carlo and fast Fourier transform convolution techniques to calculate the dose distribution from a fast neutron beam. This method transports scattered neutrons and photons in the forward, lateral, and backward directions and protons, electrons, and positrons in the forward and lateral directions by convolving energy spread kernels with initial interaction available energy distributions. The primary neutron and photon spectrums have been derived from narrow beam attenuation measurements. The positions and strengths of the effective primary neutron, scattered neutron, and photon sources have been derived from dual ion chamber measurements. The size of the effective primary neutron source has been measured using a copper activation technique. Heterogeneous tissue calculations require a weighted sum of two convolutions for each component since the kernels must be invariant for FFT convolution. Comparisons between calculations and measurements were performed for several water and heterogeneous phantom geometries. ^

THE CALIBRATION AND IMPLEMENTATION OF CR-39 NUCLEAR TRACK DETECTOR MATERIAL AS A FAST NEUTRON MICRODOSIMETER

A detailed microdosimetric characterization of the M. D. Anderson 42 MeV (p,Be) fast neutron beam was performed using the techniques of microdosimetry and a 1/2 inch diameter Rossi proportional counter. These measurements were performed at 5, 15, and 30 cm depths on the central axis, 3 cm inside, and 3 cm outside the field edge for 10 $\times$ 10 and 20 $\times$ 20 cm field sizes. Spectra were also measured at 5 and 15 cm depth on central axis for a 6 $\times$ 6 cm field size. Continuous slowing down approximation calculations were performed to model the nuclear processes that occur in the fast neutron beam. Irradiation of the CR-39 was performed using a tandem electrostatic accelerator for protons of 10, 6, and 3 MeV and alpha particles of 15, 10, and 7 MeV incident energy on target at angles of incidence from 0 to 85 degrees. The critical angle as well as track etch rate and normal incidence diameter versus linear energy transfer (LET) were obtained from these measurements. The bulk etch rate was also calculated from these measurements. Dose response of the material was studied, and the angular distribution of charged particles created by the fast neutron beam was measured with CR-39. The efficiency of CR-39 was calculated versus that of the Rossi chamber, and an algorithm was devised for derivation of LET spectra from the major and minor axis dimensions of the observed tracks. The CR-39 was irradiated in the same positions as the Rossi chamber, and the derived spectra were compared directly. ^

Water–montmorillonite systems: Neutron scattering and tracer throughdiffusion studies

Designs for deep geological respositories of nuclear waste include bentonite as a hydraulic and chemisorption buffer material to protect the biosphere from leakage of radionuclides. Bentonite is chosen because it is a cheap, naturally occurring material with the required properties. It consists essentially of montmorillonite, a swelling clay mineral. Upon contact with groundwater such clays can seal the repository by incorporating water in the interlayers of their crystalline structure. The intercalated water exhibits significantly different properties to bulk water in the surrounding interparticle pores, such as lower diffusion coefficients (González Sánchez et. al. 2008). This doctoral thesis presents water distribution and diffusion behavior on various time and space scales in montmorillonite. Experimental results are presented for Na- and Cs-montmorillonite samples with a range of bulk dry densities (0.8 to 1.7 g/cm3). The experimental methods employed were neutron scattering (backscattering, diffraction, time-of-flight), adsorption measurements (water, nitrogen) and tracer-through diffusion. For the tracer experiments the samples were fully saturated via the liquid phase under volume-constrained conditions. In contrast, for the neutron scattering experiments, the samples were hydrated via the vapor phase and subsequently compacted, leaving a significant fraction of interparticle pores unfilled with water. Owing to these differences in saturation, the water contents of the samples for neutron scattering were characterized by gravimetry whereas those for the tracer experiments were obtained from the bulk dry density. The amount of surface water in interlayer pores could be successfully discriminated from the amount of bulk-like water in interparticle pores in Na- and Csmontmorillonite using neutron spectroscopy. For the first time in the literature, the distribution of water between these two pore environments was deciphered as a function of gravimetric water content. The amount was compared to a geometrical estimation of the amount of interlayer and interparticle water determined by neutron diffraction and adsorption measurements. The relative abundances of the 1 to 4 molecular water layers in the interlayer were determined from the area ratios of the (001)-diffraction peaks. Depending on the characterization method, different fractions of surface water and interlayer water were obtained. Only surface and interlayer water exists in amontmorillonite with water contents up to 0.18 g/g according to spectroscopic measurements and up to 0.32 g/g according to geometrical estimations, respectively. At higher water contents, bulk-like and interparticle water also exists. The amounts increase monotonically, but not linearly, from zero to 0.33 g/g for bulk-like water and to 0.43 g/g for interparticle water. It was found that water most likely redistributes between the surface and interlayer sites during the spectroscopic measurements and therefore the reported fraction is relevant only below about -10 ºC (Anderson, 1967). The redistribution effect can explain the discrepancy in fractions between the methods. In a novel approach the fractions of water in different pore environments were treated as a fixed parameter to derive local diffusion coefficients for water from quasielastic neutron scattering data, in particular for samples with high water contents. Local diffusion coefficients were obtained for the 1 to 4 molecular water layers in the interlayer of 0.5·10–9, 0.9·10–9, 1.5·10–9 and 1.4·10–9 m²/s, respectively, taking account of the different water fractions (molecular water layer, bulk-like water). The diffusive transport of 22Na and HTO through Na-montmorillonite was measured on the laboratory experimental scale (i.e. cm, days) by tracer through-diffusion experiments. We confirmed that diffusion of HTO is independent of the ionic strength of the external solution in contact with the clay sample but dependent on the bulk dry density. In contrast, the diffusion of 22Na was found to depend on both the ionic strength of the pore solution and on the bulk dry density. The ratio of the pore and surface diffusion could be experimentally determined for 22Na from the dependence of the diffusion coefficient on the ionic strength. Activation energies were derived from the temperaturedependent diffusion coefficients via the Arrhenius relation. In samples with high bulk dry density the activation energies are slightly higher than those of bulk water whereas in low density samples they are lower. The activation energies as a function of ionic strengths of the pore solutions are similar for 22Na and HTO. The facts that (i) the slope of the logarithmic effective diffusion coefficients as a function of the logarithmic ionic strength is less than unity for low bulk dry densities and (ii) two water populations can be observed for high gravimetric water contents (low bulk dry densities) support the interlayer and interparticle porosity model proposed by Glaus et al. (2007), Bourg et al. (2006, 2007) and Gimmi and Kosakowski (2011).

The neutron background of the XENON100 dark matter experiment

TheXENON100 experiment, installed underground at the LaboratoriNazionali del Gran Sasso, aims to directly detect dark matter in the form of weakly interacting massive particles (WIMPs) via their elastic scattering off xenon nuclei. This paper presents a study on the nuclear recoil background of the experiment, taking into account neutron backgrounds from (alpha, n) reactions and spontaneous fission due to natural radioactivity in the detector and shield materials, as well as muon-induced neutrons. Based on MonteCarlo simulations and using measured radioactive contaminations of all detector components, we predict the nuclear recoil backgrounds for the WIMP search results published by theXENON100 experiment in 2011 and 2012, 0.11(-0.04)(+0.08) events and 0.17(-0.07)(+0.12) events, respectively, and conclude that they do not limit the sensitivity of the experiment.