Scott Olsen

An in situ rapid heat–quench cell for small-angle neutron scattering

A dual-temperature sample environment has been developed enabling the rapid heating and quenching of samples in situ for small-angle neutron scattering (SANS). The rapid heat and quench cell (RHQC) allows samples to be rapidly heated up to 600 K and then quenched to 150 K, or vice versa, in a single shot or cycle mode, with the sample in position for data collection. Measured cooling rates of up to 11 K s−1 and heating rates up to 19 K s−1 have been recorded during the testing stages. First results using the RHQC on a hydrogenated/deuterated paraffin blend quenched from the melt illustrate the value of the device in accessing the early stage phase separation kinetics with SANS.

A thermosyphon-driven hydrothermal flow-through cell for in situ and time-resolved neutron diffraction studies

A flow-through cell for hydrothermal phase transformation studies by in situ and time-resolved neutron diffraction has been designed and constructed. The cell has a large internal volume of 320 ml and can operate at temperatures up to 573 K under autogenous vapor pressures (ca 8.5 × 106 Pa). The fluid flow is driven by a thermosyphon, which is achieved by the proper design of temperature difference around the closed loop. The main body of the cell is made of stainless steel (316 type), but the sample compartment is constructed from non-scattering Ti–Zr alloy. The cell has been successfully commissioned on Australias new high-intensity powder diffractometer WOMBAT at the Australian Nuclear Science and Technology Organization, using two simple phase transformation reactions from KAlSi2O6 (leucite) to NaAlSi2O6·H2O (analcime) and then back from NaAlSi2O6·H2O to KAlSi2O6 as examples. The demonstration proved that the cell is an excellent tool for probing hydrothermal crystallization. By collecting diffraction data every 5 min, it was clearly seen that KAlSi2O6 was progressively transformed to NaAlSi2O6·H2O in a sodium chloride solution, and the produced NaAlSi2O6·H2O was progressively transformed back to KAlSi2O6 in a potassium carbonate solution.

QUOKKA, the pinhole small-angle neutron scattering instrument at the OPAL Research Reactor, Australia: design, performance, operation and scientific highlights

QUOKKA is a 40 m pinhole small-angle neutron scattering instrument in routine user operation at the OPAL research reactor at the Australian Nuclear Science and Technology Organisation. Operating with a neutron velocity selector enabling variable wavelength, QUOKKA has an adjustable collimation system providing source–sample distances of up to 20 m. Following the large-area sample position, a two-dimensional 1 m2 position-sensitive detector measures neutrons scattered from the sample over a secondary flight path of up to 20 m. Also offering incident beam polarization and analysis capability as well as lens focusing optics, QUOKKA has been designed as a general purpose SANS instrument to conduct research across a broad range of scientific disciplines, from structural biology to magnetism. As it has recently generated its first 100 publications through serving the needs of the domestic and international user communities, it is timely to detail a description of its as-built design, performance and operation as well as its scientific highlights. Scientific examples presented here reflect the Australian context, as do the industrial applications, many combined with innovative and unique sample environments.

A large volume cell for in situ neutron diffraction studies of hydrothermal crystallizations

A hydrothermal cell with 320 ml internal volume has been designed and constructed for in situ neutron diffraction studies of hydrothermal crystallizations. The cell design adopts a dumbbell configuration assembled with standard commercial stainless steel components and a zero-scattering Ti-Zr alloy sample compartment. The fluid movement and heat transfer are simply driven by natural convection due to the natural temperature gradient along the fluid path, so that the temperature at the sample compartment can be stably sustained by heating the fluid in the bottom fluid reservoir. The cell can operate at temperatures up to 300 °C and pressures up to 90 bars and is suitable for studying reactions requiring a large volume of hydrothermal fluid to damp out the negative effect from the change of fluid composition during the course of the reactions. The capability of the cell was demonstrated by a hydrothermal phase transformation investigation from leucite (KAlSi(2)O(6)) to analcime (NaAlSi(2)O(6)⋅H(2)O) at 210 °C on the high intensity powder diffractometer Wombat in ANSTO. The kinetics of the transformation has been resolved by collecting diffraction patterns every 10 min followed by Rietveld quantitative phase analysis. The classical Avrami/Arrhenius analysis gives an activation energy of 82.3±1.1 kJ  mol(-1). Estimations of the reaction rate under natural environments by extrapolations agree well with petrological observations.

Design and implementation of a differential scanning calorimeter for the simultaneous measurement of small angle neutron scattering

For almost 30 years, at synchrotron facilities, it has been possible to perform small-angle x-ray scattering experiments whilst simultaneously measuring differential scanning calorimetry (DSC). However, a range of challenges exist to enable the collection of simultaneous small-angle neutron scattering (SANS) and DSC data associated not only with intrinsic flux limitations but also scattering geometry and thermal control. The development of a DSC (temperature range ca. −150 °C to 500 °C) suitable for SANS is detailed here and its successful use is illustrated with combined measurements on a binary blend of normal alkanes in which one component has been deuterium labelled.

A 100-position robotic sample changer for powder diffraction with low-background vacuum chamber

At the new Australian OPAL research reactor, experiments carried out at room temperature use a substantial fraction of beam time on the high-resolution powder diffractometer, Echidna. With an average data collection time of 2 h and a complicated safety interlock system to protect users, the need for a fully automated and remotely controlled system was quickly realized. This report presents a solution based on a commercial four-axis robot capable of loading samples from two 50-position sample trays, in any order, into an automatically evacuated chamber. This chamber significantly reduced background signal arising from air scattering, with the effect being especially pronounced at low and high 2θ angles. In the case of textured or inhomogeneous samples, the system may be re-configured so that the robot rotates the sample in the beam or translates it vertically through the beam.

Single-pass flow-through reaction cell for high- temperature and high-pressure in situ neutron diffraction studies of hydrothermal crystallization processes

A large-volume single-pass flow-through cell for in situ neutron diffraction investigation of hydrothermal crystallization processes is reported. The cell is much more versatile than previous designs owing to the ability to control independently and precisely temperature (up to 673 K), pressure (up to 46 MPa), flow rate (0.01-10 ml min-1) and reaction-fluid volume ([greater-than or equal to]65 ml). Such versatility is realized by an innovative design consisting of a room-temperature and ambient-pressure external fluid supply module, a high-pressure reaction module which includes a high-temperature sample compartment enclosed in a vacuum furnace, and a room-temperature and high-pressure backpressure regulation module for pressure control. The cell provides a new avenue for studying various parameters of hydrothermal crystallizations independently, in situ and in real time at extreme hydrothermal conditions (e.g. supercritical). The cell was successfully commissioned on the high-intensity powder diffractometer beamline, Wombat, at the Australian Nuclear Science and Technology Organisation by investigating the effect of pressure on the hydrothermal pseudomorphic conversion from SrSO4 (celestine) to SrCO3 (strontianite) at a constant temperature of 473 K and flow rate of 5 ml min-1. The results show that the increase of pressure exerts a nonlinear effect on the conversion rate, which first increases with increasing pressure from 14 to 20 MPa, and then decreases when pressure further increases to 24 MPa.

NOVEL CRYOGENIC ENGINEERING SOLUTIONS FOR THE NEW AUSTRALIAN RESEARCH REACTOR OPAL

In August 2006 the new 20MW low enriched uranium research reactor OPAL went critical. The reactor has 3 main functions, radio pharmaceutical production, silicon irradiation and as a neutron source. Commissioning on 7 neutron scattering instruments began in December 2006. Three of these instruments (Small Angle Neutron Scattering, Reflectometer and Time-of-flight Spectrometer) utilize cold neutrons.The OPAL Cold Neutron Source, located inside the reactor, is a 20L liquid deuterium moderated source operating at 20K, 330kPa with a nominal refrigeration capacity of 5 kW and a peak flux at 4.2meV (equivalent to a wavelength of 0.4nm). The Thermosiphon and Moderator Chamber are cooled by helium gas delivered at 19.8K using the Brayton cycle. The helium is compressed by two 250kW compressors (one with a variable frequency drive to lower power consumption).A 5 Tesla BSCCO (2223) horizontal field HTS magnet will be delivered in the 2nd half of 2007 for use on all the cold neutron instruments. The magnet is cooled ...