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At least 127 records · Page 7

Simultaneous Isotopic Analysis of U, Pu, and Am in Spent Nuclear Fuel by Resonance Ionization Mass Spectrometry

Solid samples of spent nuclear fuel were analyzed for actinide isotopic composition by resonance ionization mass spectrometry. Isotopes of U, Pu, and Am were simultaneously quantified using a new method that removes and/or resolves the isobaric interferences at 238 U/ 238 Pu and 241 Pu/ 241 Am without sample preparation other than cutting and mounting small (~10 μm) samples. Trends in burnup and neutron capture product distributions were correlated with the sampling positions inside the reactor. Overall, the results show the skin effect, in which the core and near-edge regions of a fuel pellet exhibit strong differences in actinide concentrations and isotope distributions due to differences in the neutron energy spectra between the pellet rim and the core. While no elemental concentration measurements were made, the ability to measure the 238 Pu/ 239 Pu ratio in the presence of a 7400× excess of 238 U enabled an estimate of the enhancement in Pu concentration due to the skin effect at the rim of the pellet.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

The Prevalence of Anions at Plasmonic Nanojunctions: A Closer Look at P-Nitrothiophenol

We revisit the reductive coupling of p-nitrothiophenol (NTP) to form dimercaptoazobenzene (DMAB), herein monitored through gap-mode tip-enhanced Raman spectroscopy (TERS) and nano-imaging. We employ a plasmonic Au probe (100 nm diameter at its apex) illuminated with a 633 nm laser source (50 ?W/?m2 at the sample position) to image a NTP-coated faceted silver nanoparticle (~70 nm diameter). A detailed analysis of the recorded spectra reveals that anionic NTP species contribute to the recorded spectral images, in addition to the more thoroughly described DMAB product. Notably, the signatures of the anions are more pronounced than those of the DMAB product under our present experimental conditions. Our results thus demonstrate that anions and their spectral signatures must be considered in the analysis of plasmon-enhanced spectra and images.

Wang, Chih-Feng↗

Protein and RNA dynamical fingerprinting

Protein structural vibrations impact biology by steering the structure to functional intermediate states; enhancing tunneling events; and optimizing energy transfer. Strong water absorption and a broad continuous vibrational density of states have prevented optical identification of these vibrations. Recently spectroscopic signatures that change with functional state were measured using anisotropic terahertz microscopy. The technique however has complex sample positioning requirements and long measurement times, limiting access for the biomolecular community. Here we demonstrate that a simplified system increases spectroscopic structure to dynamically fingerprint biomacromolecules with a factor of 6 reduction in data acquisition time. Using this technique, polarization varying anisotropy terahertz microscopy, we show sensitivity to inhibitor binding and unique vibrational spectra for several proteins and an RNA G-quadruplex. The technique’s sensitivity to anisotropic absorbance and birefringence provides rapid assessment of macromolecular dynamics that impact biology.

59 BASIC BIOLOGICAL SCIENCES↗

Development of a portable high-T c spherical neutron polarimetry device at the Oak Ridge National Laboratory

Spherical neutron polarimetry is a powerful polarized neutron scattering technique used to determine complex magnetic structures which are only partly accessible by other methods. This technique measures the full neutron polarization change upon scattering from a sample by fully decoupling the incoming and outgoing neutron polarization with a zero-field chamber placed at the sample position. Recent advancements and testing are presented for a new spherical neutron polarimetry device utilizing high-T c superconducting YBCO films, PHiTPAD, at the High Flux Isotope Reactor at Oak Ridge National Laboratory. Furthermore, we introduce a conceptual design that utilizes wavelength-independent adiabatic transitions to adapt spherical neutron polarimetry for use with pulsed neutron sources, thereby expanding its potential applications in neutron scattering research.

47 OTHER INSTRUMENTATION↗

Development of an x-ray diffraction camera used in magnetic fields up to 10 T

A high-field x-ray diffraction (HF-XRD) camera was developed to observe structural changes of magnetic materials in magnetic fields up to 10 T. The instrument mainly consists of a Debye-Scherrer-type camera with a diameter of 80.1 mm, a 10-T cryocooled superconducting magnet with a 100-mm room-temperature bore, an x-ray source, a power supply, and a chiller for the x-ray source. An x-ray detector (image plate) in the HF-XRD camera can be taken out and inserted into the magnet without changing the sample position. The performance of the instrument was tested by measuring the HF-XRD for silicon and ferromagnetic MnBi powders. A change of x-ray diffraction pattern was observed due to the magnetic orientation of MnBi, showing that the instrument is useful for studying field-induced orientation processes and structural properties of field-controlled materials.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Combined resistive and laser heating technique for in situ radial X-ray diffraction in the diamond anvil cell at high pressure and temperature

To extend the range of high-temperature, high-pressure studies within the diamond anvil cell, a Liermann-type diamond anvil cell with radial diffraction geometry (rDAC) was redesigned and developed for synchrotron X-ray diffraction experiments at beamline 12.2.2 of the Advanced Light Source. The rDAC, equipped with graphite heating arrays, allows simultaneous resistive and laser heating while the material is subjected to high pressure. The goals are both to extend the temperature range of external (resistive) heating and to produce environments with lower temperature gradients in a simultaneously resistive- and laser-heated rDAC. Three different geomaterials were used as pilot samples to calibrate and optimize conditions for combined resistive and laser heating. For example, in Run1, FeO was loaded in a boron-mica gasket and compressed to 11 GPa then gradually resistively heated to 1007 K (1073 K at the diamond side). The laser heating was further applied to FeO to raise temperature to 2273 K. In Run2, Fe-Ni alloy was compressed to 18 GPa and resistively heated to 1785 K (1973 K at the diamond side). The combined resistive and laser heating was successfully performed again on (Mg{sub 0.9}Fe{sub 0.1})O in Run3. In this instance, the sample was loaded in a boron-kapton gasket, compressed to 29 GPa, resistive-heated up to 1007 K (1073 K at the diamond side), and further simultaneously laser-heated to achieve a temperature in excess of 2273 K at the sample position. Diffraction patterns obtained from the experiments were deconvoluted using the Rietveld method and quantified for lattice preferred orientation of each material under extreme conditions and during phase transformation.

36 MATERIALS SCIENCE↗

Undulator beamline of the Brockhouse sector at the Canadian Light Source

The Brockhouse project at the Canadian Light Source plans the construction of three beamlines, two wiggler beamlines, and one undulator beamline, that will be dedicated to x-ray diffraction and scattering. In this work, we will describe the undulator beamline main components and performance parameters, obtained from ray tracing using XOP-SHADOW codes. The undulator beamline will operate from 4.95 to 21 keV, using a 20 mm period hybrid undulator placed upstream of the wiggler in the same straight section. The beamline optics design was developed in cooperation with the Brazilian Synchrotron - LNLS. The beamline will have a double crystal monochromator with the options of Si(111) or Si(311) crystal pairs followed by two mirrors in the KB configuration to focus the beam at the sample position. The high brilliance of the undulator source will produce a very high flux of ∼10{sup 13} photons/s and high energy resolution into a small focus of 170 μm horizontal and 20-60 μm vertical, depending on the optical configuration and energy chosen. Two multi-axis goniometer experimental stations with area detectors and analyzers are foreseen to enable diffraction, resonant and inelastic scattering experiments, and SAXS/WAXS experiments with high resolution and time resolving capabilities.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Insight into hydrogenation of graphene: Effect of hydrogen plasma chemistry

Plasma hydrogenation of graphene has been proposed as a tool to modify the properties of graphene. However, hydrogen plasma is a complex system and controlled hydrogenation of graphene suffers from a lack of understanding of the plasma chemistry. Here, we correlate the modifications induced on monolayer graphene studied by Raman spectroscopy with the hydrogen ions energy distributions obtained by mass spectrometry. We measure the energy distribution of H{sup +}, H{sub 2}{sup +}, and H{sub 3}{sup +} ions for different plasma conditions showing that their energy strongly depends on the sample position, pressure, and plasma power and can reach values as high as 45 eV. Based on these measurements, we speculate that under specific plasma parameters, protons should possess enough energy to penetrate the graphene sheet. Therefore, a graphene membrane could become, under certain conditions, transparent to both protons and electrons.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

A compact and low-weight sputtering unit for in situ investigations of thin film growth at synchrotron radiation beamlines

In this work, we report on a highly variable, compact, and light high-vacuum sputter deposition unit designed for in situ experiments using synchrotron radiation facilities. The chamber can be mounted at various synchrotron beamlines for scattering experiments in grazing incidence geometry. The sample position and the large exit window allow to perform x-ray experiments up to large q values. The sputtering unit is easy to mount on existing experimental setups and can be remote-controlled. In this paper, we describe in detail the design and the performance of the new sputtering chamber and present the installation of the apparatus at different 3rd generation light sources. Furthermore, we describe the different measurement options and present some selected results. The unit has been successfully commissioned and is now available for users at PETRA III at DESY.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

A method for the monitoring of metal recrystallization based on the in-situ measurement of the elastic energy release using neutron diffraction

A method is proposed for the monitoring of metal recrystallization using neutron diffraction that is based on the measurement of stored energy. Experiments were performed using deformed metal specimens heated in-situ while mounted at the sample position of the High Resolution Powder Diffractometer, HRPD (ISIS Facility), UK. Monitoring the breadth of the resulting Bragg lines during heating not only allows the time-dependence (or temperature-dependence) of the stored energy to be determined but also the recrystallized fraction. The analysis method presented here was developed using pure nickel (Ni270) specimens with different deformation levels from 0.29 to 0.94. In situ temperature ramping as well as isothermal annealing was undertaken. The method developed in this work allows accurate and quantitative monitoring of the recrystallization process. The results from neutron diffraction are satisfactorily compared to data obtained from calorimetry and hardness measurements.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Figure correction of a metallic ellipsoidal neutron focusing mirror

An increasing number of neutron focusing mirrors is being adopted in neutron scattering experiments in order to provide high fluxes at sample positions, reduce measurement time, and/or increase statistical reliability. To realize a small focusing spot and high beam intensity, mirrors with both high form accuracy and low surface roughness are required. To achieve this, we propose a new figure correction technique to fabricate a two-dimensional neutron focusing mirror made with electroless nickel-phosphorus (NiP) by effectively combining ultraprecision shaper cutting and fine polishing. An arc envelope shaper cutting method is introduced to generate high form accuracy, while a fine polishing method, in which the material is removed effectively without losing profile accuracy, is developed to reduce the surface roughness of the mirror. High form accuracy in the minor-axis and the major-axis is obtained through tool profile error compensation and corrective polishing, respectively, and low surface roughness is acquired under a low polishing load. As a result, an ellipsoidal neutron focusing mirror is successfully fabricated with high form accuracy of 0.5 μm peak-to-valley and low surface roughness of 0.2 nm root-mean-square.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Note: Small anaerobic chamber for optical spectroscopy

The study of oxygen-sensitive biological samples requires an effective control of the atmosphere in which they are housed. In this aim however, no commercial anaerobic chamber is adequate to solely enclose the sample and small enough to fit in a compact spectroscopic system with which analysis can be performed. Furthermore, spectroscopic analysis requires the probe beam to pass through the whole chamber, introducing a requirement for adequate windows. In response to these challenges, we present a 1 l anaerobic chamber that is suitable for broad-band spectroscopic analysis. This chamber has the advantage of (1) providing access, via a septum, to the sample and (2) allows the sample position to be adjusted while keeping the chamber fixed and hermetic during the experiment.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Temperature measurements during high flux ion beam irradiations

A systematic study of the ion beam heating effect was performed in a temperature range of –170 to 900 °C using a 10 MeV Au 3+ ion beam and a Yttria stabilized Zirconia (YSZ) sample at a flux of 5.5 × 10 12 cm –2 s –1 . Different geometric configurations of beam, sample, thermocouple positioning, and sample holder were compared to understand the heat/charge transport mechanisms responsible for the observed temperature increase. The beam heating exhibited a strong dependence on the background (initial) sample temperature with the largest temperature increases occurring at cryogenic temperatures and decreasing with increasing temperature. Comparison with numerical calculations suggests that the observed heating effect is, in reality, a predominantly electronic effect and the true temperature rise is small. Furthermore, a simple model was developed to explain this electronic effect in terms of an electrostatic potential that forms during ion irradiation. Such an artificial beam heating effect is potentially problematic in thermostated ion irradiation and ion beamanalysis apparatus, as the operation of temperature feedback systems can be significantly distorted by this effect.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Development of a multi-lane X-ray mirror providing variable beam sizes

Grazing incidence mirrors are used on most X-ray synchrotron beamlines to focus, collimate or suppress harmonics. Increasingly beamline users are demanding variable beam shapes and sizes at the sample position. We have now developed a new concept to rapidly vary the beam size and shape of a focused X-ray beam. The surface of an elliptically figured mirror is divided into a number of laterally separated lanes, each of which is given an additional longitudinal height profile calculated to shape the X-ray beam to a top-hat profile in the focal plane. We have now fabricated two prototype mirrors and present the results of metrology tests and measurements made with one of the mirrors focusing the X-rays on a synchrotron beamline. We envisage that such mirrors could be widely applied to rapid beam-size switching on many synchrotron beamlines.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Partially coherent wavefront propagation simulations: Mirror and monochromator crystal quality assessment

We have applied fully-and partially-coherent synchrotron radiation wavefront propagation simulations, implemented in the “Synchrotron Radiation Workshop” (SRW) computer code, to analyse the effects of imperfect mirrors and monochromator at the Coherent Hard X-ray beamline. This beamline is designed for X-ray Photon Correlation Spectroscopy, a technique that heavily relies on the partial coherence of the X-ray beam and benefits from a careful preservation of the X-ray wavefront. We present simulations and a comparison with the measured beam profile at the sample position, which show the impact of imperfect optics on the wavefront.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Physical optics simulations with PHASE for SwissFEL beamlines

PHASE is a software tool for physical optics simulation based on the stationary phase approximation method. The code is under continuous development since about 20 years and has been used for instance for fundamental studies and ray tracing of various beamlines at the Swiss Light Source. Along with the planning for SwissFEL a new hard X-ray free electron laser under construction, new features have been added to permit practical performance predictions including diffraction effects which emerge with the fully coherent source. We present the application of the package on the example of the ARAMIS 1 beamline at SwissFEL. The X-ray pulse calculated with GENESIS and given as an electrical field distribution has been propagated through the beamline to the sample position. We demonstrate the new features of PHASE like the treatment of measured figure errors, apertures and coatings of the mirrors and the application of Fourier optics propagators for free space propagation.

43 PARTICLE ACCELERATORS↗

Increasing minority carrier lifetime in as-grown multicrystalline silicon by low temperature internal gettering

We report a systematic study into the effects of long low temperature (≤500 °C) annealing on the lifetime and interstitial iron distributions in as-grown multicrystalline silicon (mc-Si) from different ingot height positions. Samples are characterised in terms of dislocation density, and lifetime and interstitial iron concentration measurements are made at every stage using a temporary room temperature iodine-ethanol surface passivation scheme. Our measurement procedure allows these properties to be monitored during processing in a pseudo in situ way. Sufficient annealing at 300 °C and 400 °C increases lifetime in all cases studied, and annealing at 500 °C was only found to improve relatively poor wafers from the top and bottom of the block. We demonstrate that lifetime in poor as-grown wafers can be improved substantially by a low cost process in the absence of any bulk passivation which might result from a dielectric surface film. Substantial improvements are found in bottom wafers, for which annealing at 400 °C for 35 h increases lifetime from 5.5 μs to 38.7 μs. The lifetime of top wafers is improved from 12.1 μs to 23.8 μs under the same conditions. A correlation between interstitial iron concentration reduction and lifetime improvement is found in these cases. Surprisingly, although the interstitial iron concentration exceeds the expected solubility values, low temperature annealing seems to result in an initial increase in interstitial iron concentration, and any subsequent decay is a complex process driven not only by diffusion of interstitial iron.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Wavelength-selective ultraviolet (Mg,Zn)O photodiodes: Tuning of parallel composition gradients with oxygen pressure

We report on ultraviolet photodiodes with integrated optical filter based on the wurtzite (Mg,Zn)O thin films. Tuning of the bandgap of filter and active layers was realized by employing a continuous composition spread approach relying on the ablation of a single segmented target in pulsed-laser deposition. Filter and active layers of the device were deposited on opposite sides of a sapphire substrate with nearly parallel compositional gradients. Ensure that for each sample position the bandgap of the filter layer blocking the high energy radiation is higher than that of the active layer. Different oxygen pressures during the two depositions runs. The absorption edge is tuned over 360 meV and the spectral bandwidth of photodiodes is typically 100 meV and as low as 50 meV.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗