Cd0.9Zn0.1Te (CZT) detector grade crystals were grown from zone refined Cd, Zn, and Te (7N) precursor materials, using the tellurium solvent method. These crystals were grown using a high temperature vertical furnace designed and installed in our laboratory. The furnace is capable of growing up to 8” diameter crystals, and custom pulling and ampoule rotation functions using custom electronics were furnished for this setup. CZT crystals were grown using excess Te as a solvent with growth temperatures lower than the melting temperatures of CZT (1092°C). Tellurium inclusions were characterized through IR transmittance maps for the grown CZT ingots. The crystals from the grown ingots were processed and characterized using I-V measurements for electrical resistivity, thermally stimulated current (TSC), and electron beam induced current (EBIC). Pulse height spectra (PHS) measurements were carried out using a 241 Am (59.6 keV) radiation source, and an energy resolution of ~4.2% FWHM was obtained. Our investigation demonstrates high quality detector grade CZT crystals growth using this low temperature solvent method.

Group II-VI narrow band gap compounds CdTe ZnCdTe and CdSeTe are known as the most suitable semiconductor materials for the room temperature gamma- and X-ray radiation detectors. In this work we investigated electronic properties of a quaternary compound ZnCdSeTe. Cl Cu Pr Er and oxygen doped host materials were synthesized from the grinded mixture of 6N purity ZnTe CdTe and CdSe by the help of CdCl2 flux. Precautions were applied to achieve an uniform doping and high quality of the crystal surfaces. Residue phases after the thermal treatments were removed by the help of a vacuum annealing. It was found that Zn increases a substitutional solubility of dopants in ZnCdSeTe and thus promotes optoelectronic properties of the ZnCdSeTe alloy. Cl substitutes Te whereas Cu and rare earth elements substitute Zn in ZnCdSeTe. Fabricated polycrystalline samples showed a high performance from NIR via VIS and UV to X-ray band. High stability good linearity and performance of samples was measured under X-ray excitation of Cu Kα 1.54056 Å at 40 kV.

The Czochralski pulling process is the most valuable and cost efficient method for producing large oriented single crystals of the group IV and III-V semiconductors. However, there have been only a small number of reported attempts to use the Czochralski process for growing the wide bandgap compound semiconductors, needed for the room temperature operated gamma-ray detectors. The main difficulty is in the low chemical stability and high vapor pressure of the group II, V and VI elements, leading to off-stoichiometric composition, and various related defects. Among the heavy metal halides, indium iodide and indium bromide present an interesting exception. InI has a high molecular disassociation energy and a low vapor pressure, allowing for Czochralski pulling. We will describe the procedures used and the results obtained by Czochralski growth and characterization of indium iodide and the related ternary compounds that appear to be quite encouraging.

We are developing highly transparent ceramic oxide scintillators for high energy (MeV) radiography screens. Lutetium oxide doped with europium (Lu2O3:Eu) is the material of choice due to its high light yield and stopping power. As an alternative to hot-pressing, we are utilizing vacuum sintering followed by hot isostatic pressing (HIP). Nano-scale starting powder was uniaxially pressed into compacts and then sintered under high vacuum, followed by HIP’ing. Vacuum sintering temperature proved to be a critical parameter in order to obtain highly transparent Lu2O3:Eu. Under-sintering resulted in open porosity disabling the driving force for densification during HIP’ing, while over-sintering lead to trapped pores in the Lu2O3:Eu grain interiors. Optimal vacuum sintering conditions allowed the pores to remain mobile during the subsequent HIP’ing step which provided enough pressure to close the pores completely resulting in fully-dense highly transparent ceramics. Currently, we have produced 3 mm thick by 4.5 cm diameter ceramics with excellent transparency, and anticipate scaling to larger sizes while maintaining comparable optical properties.

Photoemission spectroscopy using synchrotron radiation was used to determine the energy level structure of Mn doped Li2B4O7crystals. Photoemission studies provided evidence of Mn in the bulk crystal at 47.2 eV. Valence band analysis provided the presence of surface states but no acceptor sites. Cathodoluminescence studies were also made on undoped and Mn doped Li2B4O7using various beam energies from 5 to 10 KeV at room temperature. Self trapped exciton emission states are evident in the undoped and Mn doped Li2B4O7 sample ranging in energies from 3.1 to 4.1 eV.

We have previously described a numerical model for carrier diffusion and nonlinear quenching in the track of an electron in a scintillator. Significant inequality of electron and hole mobilities predicts a characteristic “hump” in the light yield vs gamma energy, whereas low mobility of either or both carriers accentuates the universal roll-off due to nonlinear quenching at low gamma energy (high dE/dx). The material parameter basis of the two major trends in nonproportionality of scintillators can be related to the effective diffusion coefficient of excitations and the difference of electron and hole mobilities, respectively. Activator concentration, type of activator, and effect of transport anisotropy are associated with minor trends. The predicted trends are qualitatively consistent with empirical measures of nonproportionality including electron yield curves.

Using 0.5 ps pulses of 5.9 eV light to excite electron-hole concentrations varied up to 2x1020 e-h/cm3 corresponding to energy deposition within electron tracks, we measure dipole-dipole quenching rate constants K2 in SrI2 and CsI. We previously reported determination of K2 directly from the time dependence of quenched STE luminescence in CsI. The nonlinear quenching rate decreases rapidly within a few tens of picoseconds as the host excitation density drops below the Förster threshold. In the present work, we measure the dependence of integrated light yield on excitation density in the activated scintillators SrI2:Eu2+ and CsI:Tl+. The “z-scan” method of yield vs. irradiance is applicable to a wider range of materials, e.g. when the quenching population is not the main light-emitting population. Furthermore, because of using an integrating sphere and photomultiplier for light detection, the signal-to-noise is substantially better than the time-resolved method using a streak camera. As a result, both 2nd and 3rd orders of quenching (dipole-dipole and Auger) can be distinguished. Detailed comparison of SrI2 and CsI is of fundamental importance to help understand why SrI2 achieves substantially better proportionality than CsI in scintillator applications. The laser measurements, in contrast to scintillation, allow evaluating the rate constants of nonlinear quenching in a population which has small enough spatial gradient to suppress the effect of carrier diffusion.

We describe development of semiconductor scintillators (SCS) on the basis of AIIBVI compounds has bridged the gap in a series of “scintillator-photodiode” detectors used in modern multi-channel low-energy devices for visualization of hidden images (tomographs, introscopes). In accordance with the requirements of eventual applications, such SCS materials as ZnSe(Te) show the best matching of intrinsic radiation spectra to photosensitivity spectra of silicon photodiodes (PD) among the materials of similar kind. They are characterized by high radiation and thermal stability of their output parameters, as well as by high conversion efficiency. In this work, a thermodynamic model is described for interaction of isovalent dopants (IVD) with intrinsic point defects of AIIBVI semiconductor structures at different ratios of their charges, a decisive role of IVD is shown in formation of the luminescence centers, kinetics of solid-phase reactions and the role of a gas medium are considered under real preparation conditions of ZnSe(Te) scintillation crystals, and luminescence mechanisms in IVD-doped SCS are discussed.

The imperfect quality of CdZnTe (CZT) crystals for radiation detectors seriously diminishes their suitability for different applications. Dislocations and other dislocation-related defects, such as sub-grain boundaries and dislocation fields around Te inclusions, engender significant charge losses and, consequently, cause fluctuations in the detector’s output signals, thereby hindering their spectroscopic responses. In this paper, we discuss our results from characterizing CZT material by using a high-spatial-resolution X-ray response mapping system at BNL’s National Synchrotron Light Source. In this paper, we emphasize the roles of these dislocation-related defects and their contributions in degrading the detector’s performance. Specifically, we compare the effects of the sub-grain- and coherent twin-boundaries on the X-ray response maps.

We address the issue of decreasing band-gap with increasing atomic number, inherent in semiconducting materials, by introducing a concept we call dimensional reduction. The concept leads to semiconductor compounds containing high atomic number elements and simultaneously exhibiting a large band gap and high mass density suggesting that dimensional reduction can be successfully employed in developing new γ-ray detecting materials. As an example we discuss the compound Cs2Hg6S7 that exhibits a band-gap of 1.65eV and mobility-lifetime products comparable to those of optimized Cd0.9Zn0.1Te.

Synthetic CdZnTe or “CZT” crystals are highly suitable for γ-spectrometers operating at the room temperature. Secondary phases (SP) in CZT are known to inhibit detector performance, particularly when they are present in large numbers or dimensions. These SP may exist as voids or composites of non-cubic phase metallic Te layers with bodies of polycrystalline and amorphous CZT material and voids. Defects associated with crystal twining may also influence detector performance in CZT. Using transmission electron microscopy, we identify two types of defects that are on the nano scale. The first defect consists of 40 nm diameter metallic Pd/Te bodies on the grain boundaries of Te-rich composites. Although the nano-Pd/Te bodies around these composites may be unique to the growth source of this CZT material, noble metal impurities like these may contribute to SP formation in CZT. The second defect type consists of atom-scale grain boundary dislocations. Specifically, these involve inclined “finite-sized” planar defects or interfaces between layers of atoms that are associated with twins. Finite-sized twins may be responsible for the subtle but observable striations that can be seen with optical birefringence imaging and synchrotron X-ray topographic imaging.

Frisch collar detectors were fabricated from TlBr crystals with the dimensions of 2 mm × 2 mm × 4.4 mm. Spectroscopic performance of the TlBr Frisch collar detectors was evaluated at room temperature. An energy resolution of 2.9% FWHM at 662 keV was obtained from the detector without the depth correction. The detector exhibited stable spectral performance for 12 hours. Direct measurements of electron mobility-lifetime products were performed with the detectors. The TlBr crystals exhibited the electron mobility-lifetime products of ∼10−3 cm2/V at room temperature.

We report on the optical and charge transport properties of novel alkali metal chalcogenides, Cs2Hg6S7 and Cs2Cd3Te4, pertaining to their use in radiation detection. Optical absorption, photoconductivity, and gamma ray response measurements for undoped crystals were measured. The band gap energies of the Cs2Hg6S7 and Cs2Cd3Te4 compounds are 1.63 eV and 2.45 eV, respectively. The mobility-lifetime products for charge carriers are of the order of ~10-3 cm2/V for electrons and ~10-4 cm2/V for holes. Detectors fabricated from the ternary compound Cs2Hg6S7 shows well-resolved spectroscopic features at room temperature in response to ϒ -rays at 122 keV from a 57Co source, indicating its potential as a radiation detector.

This work is dedicated to the development of new type of UV phosphors based on single crystalline films (SCF) of aluminum garnet compounds grown by liquid phase epitaxy (LPE). The development of two types of UV emitting SCF scintillators is reported in this work: 1) Pr-doped SCF of Y-Lu-Al garnet having the intensive Pr3+ f-d luminescence in the 300-400 nm spectral ranges with a decay time of about 13-18 ns; 2) SCF of Y-Lu-Al-garnet doped with Sc3+ isoelectronic impurity emitting in the 290-400 nm range due to the formation of the ScY,Lu and ScAl centers with a luminescence decay time in the order of several hundred ns.

Residual impurities in manganese (Mn) are a big obstacle to obtaining high- performance CdMnTe (CMT) X-ray and gamma-ray detectors. Generally, the zone-refining method is an effective way to improve the material’s purity. In this work, we purified the MnTe compounds combining the zone-refining method with molten Te that has a very high solubility. We confirmed the improved purity of the material by glow-discharge mass spectrometry (GDMS). We also found that CMT crystals from a multiple refined MnTe source, grown by the vertical Bridgman method, yielded better performing detectors.

We synthesize a series of polyvinylcarbazole (PVK) monoliths containing varying loadings of triphenyl bismuth as a high-Z dopant and varying fluors, either organic or organometallic, in order to study their use as scintillators capable of gamma ray spectroscopy. A trend of increasing bismuth loading resulting in a better resolved photopeak is observed. For PVK parts with no fluor or a standard organic fluor, diphenylanthracene (DPA), increasing bismuth loading results in decreasing light yield while with samples 1 or 3 % by weight of the triplet harvesting organometallic fluor bis(4,6-difluoropyridinato-N,C2)picolinatoiridium (FIrpic) show increasing light yield with increasing bismuth loading. Our best performing PVK/ BiPh3/FIrpic scintillator with 40 wt % BiPh3 and 3 wt % FIrpic has an emission maximum of 500 nm, a light yield of ∼30,000 photons/MeV, and energy resolution better than 7% FWHM at 662 keV. Replacing the Ir complex with an equal weight of DPA produces a sample with a light yield of ∼6,000 photons/MeV, with an emission maximum at 420 nm and energy resolution of 9% at 662 keV. Transmission electron microscopy studies show that the BiPh3 forms small clusters of approximately 5 nm diameter.

Solid-state neutron detectors from heterostructures that incorporate Gd intrinsically or as a dopant may significantly benefit from the high thermal neutron capture cross section of gadolinium. Semiconducting devices with Gd atoms can act as a neutron capture medium and simultaneously detect the electronic signal that characterizes the interaction. Neutron capture in natural isotopic abundance gadolinium predominantly occurs via the formation of 158mGd, which decays to the ground state through the emission of high-energy gamma rays and an internal conversion electron. Detection of the internal conversion electron and/or the subsequent Auger electron emission provides a distinct and identifiable signature that neutron capture has occurred. Ensuring that the medium responds to these emissions is imperative to maximizing the efficiency and separating out other interactions from the radiation environment. A GEANT4 model, which includes incorporation of the nuclear structure of Gd, has been constructed to simulate the expected device behavior. This model allows the energy deposited from the decay of the meta-stable state to be localized and transported, providing for analysis of various device parameters. Device fabrication has been completed for Gd doped HfO2 on n-type silicon, Gd2O3 on p-type silicon and Gd2O3 on SiC for validation of the code. A preliminary evaluation of neutron detection capabilities of these devices using a GEANT4 modeling approach is presented.

We investigated defects in CdZnTe crystals produced from various conditions and their impact on fabricated devices. In this study, we employed transmission and scanning transmission electron microscope (TEM and STEM), because defects at the nano-scale are not observed readily under an optical or infrared microscope, or by most other techniques. Our approach revealed several types of defects in the crystals, such as low-angle boundaries, dislocations and precipitates, which likely are major causes in degrading the electrical properties of CdZnTe devices, and eventually limiting their performance.

In this present work we report the growth of Cd0.9Zn0.1Te doped with In by a modified THM technique. It has been demonstrated that by controlling the microscopically flat growth interface, the size distribution and concentration of Te inclusions can be drastically reduced in the as-grown ingots. This results in as-grown detector-grade CZT by the THM technique. The three-dimensional size distribution and concentrations of Te inclusions/precipitations were studied. The size distributions of the Te precipitations/inclusions were observed to be below the 10-μm range with the total concentration less than 105 cm-3. The relatively low value of Te inclusions/precipitations results in excellent charge transport properties of our as-grown samples. The (μτ)e values for different as-grown samples varied between 6-20 x10-3 cm2/V. The as-grown samples also showed fairly good detector response with resolution of ∼1.5%, 2.7% and about 3.8% at 662 keV for quasi-hemispherical geometry for detector volumes of 0.18 cm3, 1 cm3 and 4.2 cm3, respectively.