Chris A. Tulk

Transmission Bragg edge spectroscopy measurements at ORNL Spallation Neutron Source

Results of neutron transmission Bragg edge spectroscopic experiments performed at the SNAP beamline of the Spallation Neutron Source are presented. A high resolution neutron counting detector with a neutron sensitive microchannel plate and Timepix ASIC readout is capable of energy resolved two dimensional mapping of neutron transmission with spatial accuracy of ~55 μm, limited by the readout pixel size, and energy resolution limited by the duration of the initial neutron pulse. A two dimensional map of the Fe 110 Bragg edge position was obtained for a bent steel screw sample. Although the neutron pulse duration corresponded to ~30 mA energy resolution for 15.3 m flight path, the accuracy of the Bragg edge position in our measurements was improved by analytical fitting to a few mA level. A two dimensional strain map was calculated from measured Bragg edge values with an accuracy of ~few hundreds μistrain for 300s of data acquisition time.

Design challenges and performance of nested neutron mirrors for microfocusing on SNAP

Kirkpatrick–Baez (KB) neutron supermirrors can efficiently focus polyxadchromatic neutron beams to micrometre dimensions. The ultimate size is determined mainly by the perfection of the mirrors and by the size of the beam needed to have sufficient experimental signal. Nested or Montel KB mirrors can collect ∼2.6 times more beam than standard sequential KB optics, but require good figure perfection at the edge of one mirror. This paper describes the characterization of the figure errors over the important reflective portions of the two mirrors needed for a Montel focusing pair. The measurements are placed in context with theoretical predictions and are used to predict mirror focusing performance. Strategies to improve on the focusing of this class of optics are suggested and early results from these mirrors installed on the Spallation Neutrons at Pressure (SNAP) Beamline 3 at the Spallation Neutron Source (SNS) at Oak Ridge are presented.

The structure of CO2 hydrate between 0.7 and 1.0 GPa

A deuterated sample of CO2 structure I (sI) clathrate hydrate (CO2·8.3 D2O) has been formed and neutron diffraction experiments up to 1.0 GPa at 240 K were performed. The sI CO2 hydrate transformed at 0.7 GPa into the high pressure phase that had been observed previously by Hirai et al. [J. Phys. Chem. 133, 124511 (2010)] and Bollengier et al. [Geochim. Cosmochim. Acta 119, 322 (2013)], but which had not been structurally identified. The current neutron diffraction data were successfully fitted to a filled ice structure with CO2 molecules filling the water channels. This CO2+water system has also been investigated using classical molecular dynamics and density functional ab initio methods to provide additional characterization of the high pressure structure. Both models indicate the water network adapts a MH-III like filled ice structure with considerable disorder of the orientations of the CO2 molecule. Furthermore, the disorder appears to be a direct result of the level of proton disorder in the water network. In contrast to the conclusions of Bollengier et al., our neutron diffraction data show that the filled ice phase can be recovered to ambient pressure (0.1u2009MPa) at 96 K, and recrystallization to sI hydrate occurs upon subsequent heating to 150u2009K, possibly by first forming low density amorphous ice. Unlike other clathrate hydrate systems, which transform from the sI or sII structure to the hexagonal structure (sH) then to the filled ice structure, CO2 hydrate transforms directly from the sI form to the filled ice structure.

Characterization of Crystallographic Structures Using Bragg-Edge Neutron Imaging at the Spallation Neutron Source

Over the past decade, wavelength-dependent neutron radiography, also known as Bragg-edge imaging, has been employed as a non-destructive bulk characterization method due to its sensitivity to coherent elastic neutron scattering that is associated with crystalline structures. Several analysis approaches have been developed to quantitatively determine crystalline orientation, lattice strain, and phase distribution. In this study, we report a systematic investigation of the crystal structures of metallic materials (such as selected textureless powder samples and additively manufactured (AM) Inconel 718 samples), using Bragg-edge imaging at the Oak Ridge National Laboratory (ORNL) Spallation Neutron Source (SNS). Firstly, we have implemented a phenomenological Gaussian-based fitting in a Python-based computer called iBeatles. Secondly, we have developed a model-based approach to analyze Bragg-edge transmission spectra, which allows quantitative determination of the crystallographic attributes. Moreover, neutron diffraction measurements were carried out to validate the Bragg-edge analytical methods. These results demonstrate that the microstructural complexity (in this case, texture) plays a key role in determining the crystallographic parameters (lattice constant or interplanar spacing), which implies that the Bragg-edge image analysis methods must be carefully selected based on the material structures.