Owen B. Drury

Transparent ceramic scintillators for gamma spectroscopy and radiography

Transparent ceramics combine the scintillation performance of single crystals with the ruggedness and processability of glass. We have developed a versatile, scaleable fabrication method, wherein nanoparticle feedstock is consolidated at temperatures well below melting to form inch-scale phase-pure transparent ceramics with optical scatter of α <0.1 cm-1. We have fabricated Cerium-doped Gadolinium Garnets with light yields of ~50,000 Ph/MeV and energy resolution of <5% at 662 keV. We have also developed methods to form sheets of the high-Z ceramic scintillator, Europium-doped Lutetium Oxide Bixbyite, producing ~75,000 Ph/MeV for radiographic imaging applications.

A multichannel superconducting soft x-ray spectrometer for high-resolution spectroscopy of dilute samples

We have built a high-resolution high-efficiency superconducting soft x-ray spectrometer for synchrotron-based fluorescence-detected absorption spectroscopy. The sensor is a 3×3 array of 200×200 μm2 superconducting Nb–Al–Al2O3–Al–Nb tunnel junctions with an energy resolution around 15 eV below 1 keV and a total count rate capability of ≈100 000 counts/s. This sensor array is cooled to ≈0.1 K by a two-stage adiabatic demagnetization refrigerator while held at the end of a 40-cm-long cold finger that can be inserted into an UHV sample chamber for x-ray fluorescence measurements. We present L-edge absorption spectra of dilute transition metals (≈few 100 ppm) and discuss spectrometer performance with respect to the analysis of metalloproteins.

Comparative gamma spectroscopy with SrI 2 (Eu), GYGAG(Ce) and Bi-loaded plastic scintillators

We are developing new scintillator materials that offer potential for high resolution gamma ray spectroscopy at low cost. Single crystal SrI<inf>2</inf>(Eu) offers ∼3% resolution at 662 keV, in sizes of ∼1 in³. We have developed ceramics processing technology allowing us to achieve cubic inch scale transparent ceramic scintillators offering gamma spectroscopy performance superior to NaI(Tl). Our bismuth-loaded plastic scintillator demonstrates energy resolution of ∼8% at 662 keV, for samples of ∼0.5 cm³.

SrI2 scintillator for gamma ray spectroscopy

We are working to perfect the growth of divalent Eu-doped strontium iodide single crystals and to optimize the design of SrI2(Eu)-based gamma ray spectrometers. SrI2(Eu) offers a light yield in excess of 100,000 photons/MeV and light yield proportionality surpassing that of Ce-doped lanthanum bromide. Thermal and x-ray diffraction analyses of SrI2 and EuI2 indicate an excellent match in melting and crystallographic parameters, and very modest thermal expansion anisotropy. We have demonstrated energy resolution with SrI2(4-6%Eu) of 2.6% at 662 keV and 7.6% at 60 keV with small crystals, while the resolution degrades somewhat for larger sizes. Our experiments suggest that digital techniques may be useful in improving the energy resolution in large crystals impaired by light-trapping, in which scintillation light is re-absorbed and re-emitted in large and/or highly Eu2+ -doped crystals. The light yield proportionality of SrI2(Eu) is found to be superior to that of other known scintillator materials, such as LaBr3(Ce) and NaI(Tl).

Development of Transparent Ceramic Ce-Doped Gadolinium Garnet Gamma Spectrometers

Transparent polycrystalline ceramic scintillators based on the garnet structure and incorporating gadolinium for high stopping power are being developed for use in gamma spectrometers. Optimization of energy resolution for gamma spectroscopy involves refining the material composition for high stopping and high light yield, developing ceramics fabrication methodology for material homogeneity, as well as selecting the size and geometry of the scintillator to match the photodetector characteristics and readout electronics. We have demonstrated energy resolution of 4% at 662 keV for 0.05 cm3 GYGAG(Ce) ceramics with photodiode readout, and 4.9% resolution at 662 keV for 18 cm 3 GYGAG(Ce) ceramics and PMT readout. Comparative gamma spectra acquired with GYGAG(Ce) and NaI(Tl) depict the higher resolution of GYGAG(Ce) for radioisotope identification applications. Light yield non-proportionality of garnets fabricated following different methods reveal that the fundamental shapes of the light yield dependence on energy are not intrinsic to the crystal structure, but may instead depend on trap state distributions. With exposure to 9 MeV Brehmsstrahlung radiation, we also find that GYGAG(Ce) ceramics exhibit excellent radiation hardness.

Transparent Ceramic Scintillator Fabrication, Properties and Applications

Transparent ceramics offer an alternative to single crystals for scintillator applications such as gamma ray spectroscopy and radiography. We have developed a versatile, scaleable fabrication method, using Flame Spray Pyrolysis (FSP) to produce feedstock which is readily converted into phase-pure transparent ceramics. We measure integral light yields in excess of 80,000 Ph/MeV with Cerium-doped Garnets, and excellent optical quality. Avalanche photodiode readout of Garnets provides resolution near 6%. For radiography applications, Lutetium Oxide offers a high performance metric and is formable by ceramics processing. Scatter in transparent ceramics due to secondary phases is the principal limitation to optical quality, and afterglow issues that affect the scintillation performance are presently being addressed.

Sensitivity and S/N-ratio of superconducting high-resolution X-ray spectrometers

Superconducting tunnel junction (STJ) X-ray spectrometers have been developed for synchrotron-based high-resolution soft X-ray spectroscopy. We are quantifying the improvements in sensitivity and signal-to-noise ratio that STJ spectrometers can offer for the analysis of dilute specimens over conventional semiconductor and grating spectrometers. We present analytical equations to quantify the improvements in terms of spectrometer resolution, detection efficiency and count rate capabilities as a function of line separation and spectral background. We discuss the implications of this analysis for L-edge spectroscopy of first-row transition metals.

Molybdenum X-ray absorption edges from 200 to 20,000eV: the benefits of soft X-ray spectroscopy for chemical speciation.

We have surveyed the chemical utility of the near-edge structure of molybdenum X-ray absorption edges from the hard X-ray K-edge at 20,000eV down to the soft X-ray M(4,5)-edges at approximately 230eV. We compared, for each edge, the spectra of two tetrahedral anions, MoO(4)(2-) and MoS(4)(2-). We used three criteria for assessing near-edge structure of each edge: (i) the ratio of the observed chemical shift between MoO(4)(2-) and MoS(4)(2-) and the linewidth, (ii) the chemical information from analysis of the near-edge structure and (iii) the ease of measurement using fluorescence detection. Not surprisingly, the K-edge was by far the easiest to measure, but it contained the least information. The L(2,3)-edges, although harder to measure, had benefits with regard to selection rules and chemical speciation in that they had both a greater chemical shift as well as detailed lineshapes which could be theoretically analyzed in terms of Mo ligand field, symmetry, and covalency. The soft X-ray M(2,3)-edges were perhaps the least useful, in that they were difficult to measure using fluorescence detection and had very similar information content to the corresponding L(2,3)-edges. Interestingly, the soft X-ray, low energy ( approximately 230eV) M(4,5)-edges had greatest potential chemical sensitivity and using our high-resolution superconducting tunnel junction (STJ) fluorescence detector they appear to be straightforward to measure. The spectra were amenable to analysis using both the TT-multiplet approach and FEFF. The results using FEFF indicate that the sharp near-edge peaks arise from 3d-->5p transitions, while the broad edge structure has predominately 3d-->4f character. A proper understanding of the dependence of these soft X-ray spectra on ligand field and site geometry is necessary before a complete assessment of the utility of the Mo M(4,5)-edges can be made. This work includes crystallographic characterization of sodium tetrathiomolybdate.

Fabrication of Mo/Cu multilayer and bilayer transition edge sensors

We are developing cryogenic high-resolution X-ray, Gamma-ray and neutron spectrometers based on superconducting Mo/Cu transition edge sensors. Here we discuss the sensor design for different applications, present the photolithographic fabrication techniques, and outline future detector development to increase the spectrometer sensitivity.

Design of a multichannel ultra-high-resolution superconducting gamma-ray spectrometer

Superconducting Gamma-ray microcalorimeters operated at temperatures around ~0.1 K offer an order of magnitude improvement in energy resolution over conventional high-purity Germanium spectrometers. The calorimeters consist of a ~1 mm3 superconducting or insulating absorber and a sensitive thermistor, which are weakly coupled to a cold bath. Gamma-ray capture increases the absorber temperature in proportion to the Gamma-ray energy, this is measured by the thermistor, and both subsequently cool back down to the base temperature through the weak link. We are developing ultra-high-resolution Gamma-ray spectrometers based on Sn absorbers and superconducting Mo/Cu multilayer thermistors for nuclear non-proliferation applications. They have achieved an energy resolution between 60 and 90 eV for Gamma-rays up to 100 keV. We also build two-stage adiabatic demagnetization refrigerators for user-friendly detector operation at 0.1 K. We present recent results on the performance of single pixel Gamma-ray spectrometers, and discuss the design of a large detector array for increased sensitivity.