In-Situ Analysis of Corrosion Products in Molten Salt: X-ray Absorption Reveals Both Ionic and Metallic Species
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Engineering topics
Publications and source records attributed to Marshall, Matthew S. J..
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Scintillation detectors exhibiting high spatial resolution and fast timing capabilities are of vital importance for synchrotron sources. These detectors may be exposed to a variety of X-ray energies (up to 140 keV) and used in high frame rate applications. Here, we describe the advances in the development of thin-film LuI3:Ce scintillators for higher energy X-ray imaging, with fast timing and high spatial resolution. When grown in a single crystalline form, these scintillators are bright, producing 115 000 photons/MeV. However, to achieve high spatial resolution, these scintillators are grown in thin-film form with a microcolumnar structure, controllable to column diameters of <1-30 mu m. Thus, a much thicker scintillator layer (10 mu m-3 mm or higher) may be grown, providing superior X-ray absorption while achieving high resolutions of 50 mu m or better, at the cost of reduced light yield. To study the timing characteristics of the scintillator, time-resolved X-ray excited optical luminescence (TR-XEOL) was performed on two different sets of three samples of LuI3 at the 1-BM beamline of the Advanced Photon Source at Argonne National Laboratory. Besides, we report timing measurements obtained using a photomultiplier tube (PMT) and oscilloscope at Radiation Monitoring Devices (RMD) Inc. Using the TR-XEOL, we determined the decay constants of LuI3 as a function of Ce doping, recording a fast decay component as low as 3.6 ns (39%), one of the fastest values recorded in inorganic scintillators. This fast decay opens up numerous novel applications, where ultrahigh frame rates are important using synchrotron X-rays. This article will discuss fabrication, characterization, and potential applications for this novel scintillator.
Combining high light output with the microcolumnar structure, the CsI:Tl films significantly reduce the need for painful tradeoff between thickness (hence, stopping power) and spatial resolution. But both films and monocrystals share two important deficiencies that hinder their use in many high-speed imaging and computed tomography applications: a persistent afterglow and hysteresis. These properties receive the primary attention of this investigation. In our earlier work, we reported that codoping with Sm 2+ brings about a significant reduction in the afterglow of CsI:Tl. Here, focusing on the microcolumnar films, we examine this afterglow-suppressive effect over a wide range of exposure times, from milliseconds to seconds, and at temperatures between 0 °C and 60 °C. Our measurements reveal well-defined dependences on both parameters. At room temperature (20 °C), defined as the normal operating condition, a 10-ms X-ray pulse leaves an afterglow from the standard (Sm-free) CsI:Tl of about 1% at 2 ms after the end of the pulse, changing little as a function of pulselength. Doping with Sm 2+ , however, reduces that afterglow by at least an order of magnitude, although somewhat less so after longer (100 and 1000 ms) pulses. When we change the temperature, however, we find markedly different behavior. Here, we find that a temperature increase of only 60°, without changing the pulselength, cuts the afterglow of standard CsI:Tl films by a factor of 20. However, films of codoped CsI:Tl,Sm, whose afterglow has already been suppressed by the presence of Sm 2+ , show much less change as a function of either temperature or pulse duration. It is the presence of Sm 2+ that makes the biggest difference. As for hysteresis, we again see an improvement, with the performance of the codoped CsI:Tl,Sm films bettering that of the standard (Sm-free) films. After an exposure of 300 mR, the change in light output falls to within 1% of the original after 1 min, whereas standard CsI:Tl films require 30 min to reach the same level.
The ability to map out electrostatic potentials in materials is critical for the development and the design of nanoscale electronic and spintronic devices in modern industry. Electron holography has been an important tool for revealing electric and magnetic field distributions in microelectronics and magnetic-based memory devices, however, its utility is hindered by several practical constraints, such as charging artifacts and limitations in sensitivity and in field of view. In this article, we report electron-beam-induced-current (EBIC) and secondary-electron voltage-contrast (SE-VC) with an aberration-corrected electron probe in a transmission electron microscope (TEM), as complementary techniques to electron holography, to measure electric fields and surface potentials, respectively. These two techniques were applied to ferroelectric thin films, multiferroic nanowires, and single crystals. Electrostatic potential maps obtained by off-axis electron holography were compared with EBIC and SE-VC to show that these techniques can be used as a complementary approach to validate quantitative results obtained from electron holography analysis.
Polar discontinuity at interfaces plays deterministic roles in charge transport, magnetism, and even superconductivity of functional oxides. To date, most polar discontinuity problems have been explored in hetero-interfaces between two dissimilar materials. Here, we show that charged domain walls (CDWs) in epitaxial thin films of ferroelectric PbZr 0.2 Ti 0.8 O 3 are strongly coupled to polar interfaces through the formation of ½<101>{h0l} type crystallographic shear planes (CSPs). Using atomic resolution imaging and spectroscopy we illustrate that the CSPs consist of both conservative and nonconservative segments when coupled to the CDWs, where necessary compensating charges for stabilizing the CDWs are associated with vacancies at the CSPs. Lasly, the CDW/CSP coupling yields an atomically narrow domain walls, consisting of a single atomic layer of oxygen. This study shows that the CDW/CSP coupling is a fascinating venue to develop emergent material properties.
Many microscopic investigations of materials may benefit from the recording of multiple successive images. This can include techniques common to several types of microscopy such as frame averaging to improve signal-to-noise ratios (SNR) or time series to study dynamic processes or more specific applications. In the scanning transmission electron microscope, this might include focal series for optical sectioning or aberration measurement, beam damage studies or camera-length series to study the effects of strain; whilst in the scanning tunnelling microscope, this might include bias voltage series to probe local electronic structure. Whatever the application, such investigations must begin with the careful alignment of these data stacks, an operation that is not always trivial. In addition, the presence of low-frequency scanning distortions can introduce intra-image shifts to the data. Here, we describe an improved automated method of performing non-rigid registration customised for the challenges unique to scanned microscope data specifically addressing the issues of low-SNR data, images containing a large proportion of crystalline material and/or local features of interest such as dislocations or edges. Careful attention has been paid to artefact testing of the non-rigid registration method used, and the importance of this registration for the quantitative interpretation of feature intensities and positions is evaluated.
Typical logic elements utilizing the field effect rely on the change in carrier concentration due to the field in the channel region of the device. Ferroelectric-field-effect devices provide a nonvolatile version of this effect due to the stable polarization order parameter in the ferroelectric. In this study, we describe an oxide/oxide ferroelectric heterostructure device based on (001)-oriented PbZr₀̣.₂Ti₀.₈O₃-LaNiO₃ where the dominant change in conductivity is a result of a significant mobility change in the interfacial channel region. The effect is confined to a few atomic layers at the interface and is reversible by switching the ferroelectric polarization. More interestingly, in one polarization state, the field effect induces a 1.7 eV shift of the interfacial bands to create a new conducting channel in the interfacial PbO layer of the ferroelectric.
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