Ce Crystals Research Articles

A depth-of-interaction PET detector using a stair-shaped reflector arrangement and a single-ended scintillation light readout

Positron emission tomography (PET) detectors with the ability to encode depth-of-interaction (DOI) information allow us to simultaneously improve the spatial resolution and sensitivity of PET scanners. In this study, we propose a DOI PET detector based on a stair-pattern reflector arrangement inserted between pixelated crystals and a single-ended scintillation light readout. The main advantage of the proposed method is its simplicity; DOI information is decoded from a flood map and the data can be simply acquired by using a single-ended readout system. Another potential advantage is that the two-step DOI detectors can provide the largest peak position distance in a flood map because two-dimensional peak positions can be evenly distributed. We conducted a Monte Carlo simulation and obtained flood maps. Then, we conducted experimental studies using two-step DOI arrays of 5 × 5 Lu1.9Y0.1SiO5:Ce crystals with a cross-section of 1.7 × 1.7 mm2 and different detector configurations: an unpolished single-layer (US) array, a polished single-layer (PS) array and a polished stacked two-layer (PT) array. For each detector configuration, both air gaps and room-temperature vulcanization (RTV) silicone gaps were tested. Detectors US and PT showed good peak separation in each scintillator with an average peak-to-valley ratio (PVR) and distance-to-width ratio (DWR) of 2.09 and 1.53, respectively. Detector PSRTV showed lower PVR and DWR (1.65 and 1.34, respectively). The configuration of detector PTAir is preferable for the construction of time-of-flight-DOI detectors because timing resolution was degraded by only about 40 ps compared with that of a non-DOI detector. The performance of detectors USAir and PSRTV was lower than that of a non-DOI detector, and thus these designs are favorable when the manufacturing cost is more important than timing performance. The results demonstrate that the proposed DOI-encoding method is a promising candidate for PET scanners that require high resolution and sensitivity and operate with conventional acquisition systems.

Crystal growth and scintillation properties of undoped and Ce3+-doped GdI3 crystals

The growth and scintillation properties of undoped and Ce3+-doped GdI3 crystals were reported in this paper. These GdI3:χ%Ce (χ = 0, 1, 2) crystals were grown by the vertical Bridgman growth technique in evacuated quartz crucibles. X-ray excited optical luminescence spectra of GdI3:Ce exhibit a broad emission band (450 nm–650 nm) peaking at 520 nm corresponding to 5d1→4f1 transition of Ce3+ while the undoped GdI3 crystal consists of a broad band (400 nm-600 nm) and several sharp lines peaking at 462 nm, 482 nm, 492 nm, 549 nm, 579 nm owing to the impurities ions and defects. The excitation spectra of Ce3+ doped GdI3 consist of two broad bands between 300 nm and 500 nm corresponding to 4f1→5d1 absorption of Ce3+. The other absorption peaking at 262 nm in the spectrum of GdI3:2%Ce is assigned to band-to-band exciton transition. The excitation spectrum of undoped GdI3 contains a flat absorption band from 330 to 370 nm and a broad band between 390 and 450 nm peaking at 414 nm corresponding to the absorption of the unintentionally doped Ce3+, Dy3+, Ho3+ impurities and other defects. The emission spectrum of undoped GdI3 under 332 nm excitation has the identical line peaks with the spectrum measured under X-ray excitation. The emission spectra of GdI3:2%Ce and GdI3:1%Ce show a broad band in the range of 450–750 nm with the maximum at 550 nm corresponding to 5d1→4f1 transitions of Ce3+ ion. The GdI3, GdI3:1%Ce and GdI3:2%Ce show fast principle decay time constant 73 ns, 69 ns and 58 ns respectively, besides, the undoped also shows a slow decay constant 325 ns which doesn't appear in Ce3+-doped GdI3 crystal. The energy resolutions of GdI3:χ%Ce (χ = 1, 2) measured at 662 KeV are about 3%–5% and the undoped GdI3 is 13.3%.

A Depth-of-Interaction encoding method for SPECT monolithic scintillation detectors

The Depth of Interaction (DoI) discrimination of gamma-photons within scintillation crystals allows to improve imaging performance in PET scanners as well as in SPECT devices equipped with non-parallel collimators (e. g. pinhole ones). In previous works, the authors experimentally proved the efficiency of a DoI-encoding technique in case of a 20 mm-thick monolithic crystal PET module. For the thinner crystals commonly used in SPECT, DoI determination still remains a challenging goal. To this aim, in this work the authors have experimentally evaluated the DoI-encoding method on a 6 mm-thick monolithic LaBr3:Ce crystal. The results prove the efficiency and reliability of the proposed method. It indeed allows to discriminate the gamma photons interacting at the the top and the bottom of the crystal.

Localisation of gamma-ray interaction points in thick monolithic CeBr3 and LaBr3:Ce scintillators

Localisation of gamma-ray interaction points in monolithic scintillator crystals can simplify the design and improve the performance of a future Compton telescope for gamma-ray astronomy. In this paper we compare the position resolution of three monolithic scintillators: a 28×28×20mm3 (length×breadth × thickness) LaBr3:Ce crystal, a 25×25×20mm3 CeBr3 crystal and a 25×25×10mm3 CeBr3 crystal. Each crystal was encapsulated and coupled to an array of 4×4 silicon photomultipliers through an optical window. The measurements were conducted using 81keV and 356keV gamma-rays from a collimated 133Ba source. The 3D position reconstruction of interaction points was performed using artificial neural networks trained with experimental data. Although the position resolution was significantly better for the thinner crystal, the 20mm thick CeBr3 crystal showed an acceptable resolution of about 5.4mm FWHM for the x and y coordinates, and 7.8mm FWHM for the z-coordinate (crystal depth) at 356keV. These values were obtained from the full position scans of the crystal sides. The position resolution of the LaBr3:Ce crystal was found to be considerably worse, presumably due to the highly diffusive optical interface between the crystal and the optical window of the enclosure. The energy resolution (FWHM) measured for 662keV gamma-rays was 4.0% for LaBr3:Ce and 5.5% for CeBr3. The same crystals equipped with a PMT (Hamamatsu R6322-100) gave an energy resolution of 3.0% and 4.7%, respectively.

Nature of radiation resistance of LFS oxyorthosilicate crystals doped with Ce, Sc, Ca, and Y ions

Optical and luminescence characteristics of Lu2+2ySi1-yO5+y (LFS) scintillation crystals are studied before and after irradiation with doses to 45 Mrad from a 60Co source. LFS crystals were doped with Ce3+, Sc3+, Ca2+, and Y3+ ions with various concentrations. The dependence of the radiation resistance of LFS crystals on Ce ion concentration is detected. For the crystal of composition Ce:Sc:Ca:Y:LFS, it was found that its optical transmission (OT) and pulsed cathodoluminescence (PCL) spectra before irradiation do not differ from the spectra measured after irradiation with a dose of 45 Mrad within experimental error. The nature of the radiation resistance of rare-earth lutetium oxyorthosilicates (LFS) is discussed.

Aluminum and Gallium Substitution in Yttrium and Lutetium Aluminum–Gallium Garnets: Investigation by Single-Crystal NMR and TSL Methods

The work reports the results on 71Ga and 27Al NMR investigation of the gallium and aluminum ions distribution over tetrahedral and octahedral positions in the Y3Al5–x GaxO12:Ce single crystals and Lu3Al5–xGaxO12:Ce single-crystalline epitaxial films. The gallium content x varies between 0 and 5 in crystals and between 0.3 and 2 in films.. We find that in both the Y- and Lu-based solid solutions the larger gallium ions are preferably located at the tetrahedral position while the smaller aluminum ions prefer the octahedral position of the garnet host. Based on NMR data, the dependence of fractional occupation parameters of the tetrahedral site of Ga and Al ions on the Ga content is determined. In particular, in the Y3Al2Ga3O12:Ce crystal only 28% of Ga ions occupy octahedral sites, whereas 72% occupy tetrahedral ones. NMR investigations suggest that observed nonmonotonic dependences of electron trap depths monitored by thermally stimulated luminescence of Y3Al5–xGaxO12:Ce complex garnets on the Ga content a...

Simulation of π0-γ Separation Study for Proposed CMS Forward Electromagnetic Calorimeter

The Forward Electromagnetic Calorimeter of the CMS detector is going to be upgraded in the high luminosity running as the energy of the present Electromagnetic Calorimeter (PbWO4) will degrade in the high luminosity (luminosity 1034cm-2s-1) running due to extensive radiation (hadron flux 1013neutrons cm,-2). Shashlik Electromagnetic Calorimeter which consists of alternate layers of 1.5 mm LYSO(Ce) crystal plates and 2.5 mm Tungsten absorbers, was a proposal for high luminosity running. One of the performance points for any electromagnetic calorimeter is the ability to separate π0 s from true photons, since final states with photons are a clean and one of the most important final states in proton-proton collisions at the LHC. The objective of this project is to study the possibility of π0 and γ separation in the Shashlik detector using Multivariate Analysis (MVA) technique.

Optimized Magneto-optical Isolator Designs Inspired by Seedlayer-Free Terbium Iron Garnets with Opposite Chirality

Simulations demonstrate that undoped yttrium iron garnet (YIG) seedlayers cause reduced Faraday rotation in silicon-on-insulator waveguides with Ce-doped YIG claddings. Undoped seedlayers are required for the crystallization of the magneto-optical Ce:YIG claddings, but they diminish the interaction of the Ce:YIG with the guided modes. Therefore, new magneto-optical garnets, terbium iron garnet (TIG) and bismuth-doped TIG (Bi:TIG), are introduced that can be integrated directly on Si and quartz substrates without seedlayers. The Faraday rotations of TIG and Bi:TIG films at 1550 nm were measured to be +500°/cm and −500°/cm, respectively. Simulations show that these new garnets have the potential to significantly mitigate the negative impact of the seedlayers under Ce:YIG claddings. The successful growth of TIG and Bi:TIG on low-index fused quartz inspired novel garnet-core waveguide isolator designs, simulated using finite difference time domain methods. These designs use alternating segments of positive an...

Position sensitivity in large spectroscopic LaBr3:Ce crystals for Doppler broadening correction

The position sensitivity of a large LaBr3:Ce crystal was investigated with the aim of correcting for the Doppler broadening in nuclear physics experiments. The crystal was cylindrical, 3in×3in (7.62cm x 7.62cm) and with diffusive surfaces as typically used in nuclear physics basic research to measure medium or high energy gamma rays (0.5MeV<Eγ<20MeV). The crystal was coupled to Position Sensitive Photomultipliers (PSPMT). The signals from the 256 segments of the four PSPMTs were acquired grouping them into 16 elements. An event by event analysis was performed and a positon resolution of the order of 2cm was found. It was verified that this allows an important reduction of the Doppler broadening induced by relativistic beams in Nuclear Physics experiments.

Non-proportionality study of CaMoO4 and GAGG:Ce scintillation crystals using Compton coincidence technique

In this study, the CCT technique and nuclear instrument module (NIM) setup for the measurements of coincidence electron energy spectra of calcium molybdate (CaMoO4) and cerium doped gadolinium aluminium gallium garnet (Gd3Al2Ga3O12:Ce or GAGG:Ce) scintillation crystals were carried out. The 137Cs irradiated gamma rays with an energy (Eγ) of 662keV was used as a radioactive source. The coincidence electron energy spectra were recorded at seven scattering angles of 30°–120°. It was found that seven corresponding electron energies were in the range of 100.5–435.4keV. The results show that, for all electron energies, the electron energy peaks of CaMoO4 crystal yielded higher number of counts than those of GAGG:Ce crystal. The electron energy resolution, the light yield and non-proportionality were also determined. It was found that the energy resolutions are inverse proportional to the square root of electron energy for both crystals. Furthermore, the results show that the light yield of GAGG:Ce crystal is much higher than that of CaMoO4 crystal. It was also found that both CaMoO4 and GAGG:Ce crystals demonstrated good proportional property in the electron energy range of 260–435.4keV.

Free carrier absorption in self-activated PbWO4 and Ce-doped Y3(Al0.25Ga0.75)3O12 and Gd3Al2Ga3O12 garnet scintillators

Nonequilibrium carrier dynamics in the scintillators prospective for fast timing in high energy physics and medical imaging applications was studied. The time-resolved free carrier absorption investigation was carried out to study the dynamics of nonequilibrium carriers in wide-band-gap scintillation materials: self-activated led tungstate (PbWO4, PWO) ant two garnet crystals, GAGG:Ce and YAGG:Ce. It was shown that free electrons appear in the conduction band of PWO and YAGG:Ce crystals within a sub-picosecond time scale, while the free holes in GAGG:Ce appear due to delocalization from Gd3+ ground states to the valence band within a few picoseconds after short-pulse excitation. The influence of Gd ions on the nonequilibrium carrier dynamics is discussed on the base of comparison the results of the free carrier absorption in GAGG:Ce containing gadolinium and in YAGG without Gd in the host lattice.

Characterization of LaBr3:Ce and CeBr3 calorimeter modules for 3D imaging in gamma-ray astronomy

For the purpose of future space instrumentation for γ-ray astronomy, we developed a small prototype of a Compton telescope and studied novel detector modules aimed for Compton imaging. We assembled and tested 2 modules, one with a cerium-doped lanthanum(III) bromide (LaBr3:Ce) crystal and the other with cerium(III) bromide (CeBr3). Both crystals measure 5×5cm2 in area and are 1cm thick. They are coupled to and read out by 64-channel multi-anode PMTs. Our goals are to obtain the best possible energy resolution and position resolution in 3D on the first impact of an incident γ-ray within the detector. Both information are vital for successful reconstruction of a Compton image with the telescope prototype. We developed a test bench to experimentally study both modules and have utilized a customized readout electronics and data acquisition system. Furthermore, we have written a detailed Geant4 simulation of the experiment, and utilize simulated data to train an Artificial Neural Network (ANN) algorithm to create a simplified 3D impact position reconstruction method. We give experimental test results obtained by both modules and present detailed parametrization and results from the Geant4 simulation and from the ANN. We compare and discuss the performance of the modules and conclude by giving a brief overview of the future prospects for using such modules in γ-ray astronomy.

A 32 mm × 32 mm × 22 mm monolithic LYSO:Ce detector with dual-sided digital photon counter readout for ultrahigh-performance TOF-PET and TOF-PET/MRI

New applications for positron emission tomography (PET) and combined PET/magnetic resonance imaging (MRI) are currently emerging, for example in the fields of neurological, breast, and pediatric imaging. Such applications require improved image quality, reduced dose, shorter scanning times, and more precise quantification. This can be achieved by means of dedicated scanners based on ultrahigh-performance detectors, which should provide excellent spatial resolution, precise depth-of-interaction (DOI) estimation, outstanding time-of-flight (TOF) capability, and high detection efficiency. Here, we introduce such an ultrahigh-performance TOF/DOI PET detector, based on a 32 mm × 32 mm × 22 mm monolithic LYSO:Ce crystal. The 32 mm × 32 mm front and back faces of the crystal are coupled to a digital photon counter (DPC) array, in so-called dual-sided readout (DSR) configuration. The fully digital detector offers a spatial resolution of ~1.1 mm full width at half maximum (FWHM)/~1.2 mm mean absolute error, together with a DOI resolution of ~2.4 mm FWHM, an energy resolution of 10.2% FWHM, and a coincidence resolving time of 147 ps FWHM. The time resolution closely approaches the best results (135 ps FWHM) obtained to date with small crystals made from the same material coupled to the same DPC arrays, illustrating the excellent correction for optical and electronic transit time spreads that can be achieved in monolithic scintillators using maximum-likelihood techniques for estimating the time of interaction. The performance barely degrades for events with missing data (up to 6 out of 32 DPC dies missing), permitting the use of almost all events registered under realistic acquisition conditions. Moreover, the calibration procedures and computational methods used for position and time estimation follow recently made improvements that make them fast and practical, opening up realistic perspectives for using DSR monolithic scintillator detectors in TOF-PET and TOF-PET/MRI systems.

Development of a Cerium-Doped Lanthanum Bromide Gamma-Ray Spectrometer for Planetary Missions and Feasibility Studies for Determination of Elemental Abundances of Radioactive Elements (Th, K and U)

We present the development of a cerium-doped lanthanum bromide (LaBr 3 : Ce) gamma-ray spectrometer (GRS) with the primary objective of determining the abundance and distribution of Th, U, K, and other major elements, including Fe on the entire planetary surface by measuring gamma-ray signals produced by radioactive decay, neutron inelastic scattering and neutron capture reactions in the energy region 0.03- 8 MeV. The energy resolution of the LaBr3 : Ce GRS developed in-house using front-end and processing electronics at 511 and 1274 keV is estimated to be 4.1% and 2.5% respectively. The intrinsic activity count rate for our 3 n * 3 n LaBr 3 : Ce GRS is ~61 counts s -1 (i.e. ~0.18 counts s -1 cm -3 ) for the 40K energy window (1400-1520 keV) and ~3.4 counts s -1 for the 232 Th (2550-2700 keV) energy window. Although this large intrinsic activity of the LaBr 3 : Ce crystal inhibits estimation of the concentrations of Th and K, our attempts using a NaI(Tl) GRS (with electronics developed in-house) were more successful. The Th concentration of US-110 was estimated to be ~11.4 ppm and is within 14% of the 13.2 ppm value determined using a HPGe GRS. The K concentration of US-110 was estimated to be 0.87% and is within ~10% of the 0.78% value determined independently using a HPGe GRS.

Towards monolithic scintillator based TOF-PET systems: practical methods for detector calibration and operation

Gamma-ray detectors based on thick monolithic scintillator crystals can achieve spatial resolutions <2 mm full-width-at-half-maximum (FWHM) and coincidence resolving times (CRTs) better than 200 ps FWHM. Moreover, they provide high sensitivity and depth-of-interaction (DOI) information. While these are excellent characteristics for clinical time-of-flight (TOF) positron emission tomography (PET), the application of monolithic scintillators has so far been hampered by the lengthy and complex procedures needed for position- and time-of-interaction estimation. Here, the algorithms previously developed in our group are revised to make the calibration and operation of a large number of monolithic scintillator detectors in a TOF-PET system practical. In particular, the k-nearest neighbor (k-NN) classification method for x,y-position estimation is accelerated with an algorithm that quickly preselects only the most useful reference events, reducing the computation time for position estimation by a factor of ~200 compared to the previously published k-NN 1D method. Also, the procedures for estimating the DOI and time of interaction are revised to enable full detector calibration by means of fan-beam or flood irradiations only. Moreover, a new technique is presented to allow the use of events in which some of the photosensor pixel values and/or timestamps are missing (e.g. due to dead time), so as to further increase system sensitivity. The accelerated methods were tested on a monolithic scintillator detector specifically developed for clinical PET applications, consisting of a 32 mm × 32 mm × 22 mm LYSO : Ce crystal coupled to a digital photon counter (DPC) array. This resulted in a spatial resolution of 1.7 mm FWHM, an average DOI resolution of 3.7 mm FWHM, and a CRT of 214 ps. Moreover, the possibility of using events missing the information of up to 16 out of 64 photosensor pixels is shown. This results in only a small deterioration of the detector performance.

Reduced γ–γ time walk to below 50 ps using the multiplexed-start and multiplexed-stop fast-timing technique with LaBr3(Ce) detectors

The electronic γ–γ fast-timing technique using arrays consisting of many LaBr3(Ce) detectors is a powerful method to determine lifetimes of nuclear excited states with a lower limit of about 5ps. This method requires the determination of the energy-dependent time walk of the zero time which is represented by the centroid of a prompt γ–γ time distribution. The full-energy peak versus full-energy peak prompt response difference which represents the linearly combined mean γ–γ time walk of a fast-timing array consisting of 8 LaBr3(Ce) detectors was measured using a standard 152Eu γ-ray source for the energy region of 40–1408keV. The data were acquired using a “multiplexed-start and multiplexed-stop” analogue electronics circuitry and analysed by employing the generalized centroid difference method. Concerning the cylindrical 1.5in.×1.5in. LaBr3(Ce) crystals which are coupled to the Hamamatsu R9779 photomultiplier tubes, the best fast-timing array time resolution of 202(3)ps is obtained for the two prompt γ lines of 60Co by using the leading-edge timing principle. When using the zero-crossover timing principle the time resolution is degraded by up to 30%, dependent on the energy and the shaping delay time of the constant fraction discriminator model Ortec 935. The smallest γ–γ time walk to below 50ps is obtained by using a shaping delay time of about 17ns and an optimum “time-walk adjustment” needed for detector output pulses with amplitudes smaller than 400mV.

Fast neutron measurements with 7Li and 6Li enriched CLYC scintillators

The recently developed Cs2LiYCl6:Ce (CLYC) crystals are interesting scintillation detectors not only for their gamma energy resolution (<5% at 662keV) but also for their capability to identify and measure the energy of both gamma rays and fast/thermal neutrons. The thermal neutrons were detected by the 6Li(n,α)t reaction while for the fast neutrons the 35Cl(n,p)35S and 35Cl(n,α)32P neutron-capture reactions were exploited. The energy of the outgoing proton or α particle scales linearly with the incident neutron energy. The kinetic energy of the fast neutrons can be measured using both the Time Of Flight (TOF) technique and using the CLYC energy signal. In this work, the response to monochromatic fast neutrons (1.9–3.8MeV) of two CLYC 1″×1″ crystals was measured using both the TOF and the energy signal. The observables were combined to identify fast neutrons, to subtract the thermal neutron background and to identify different fast neutron-capture reactions on 35Cl, in other words to understand if the detected particle is an α or a proton. We performed a dedicated measurement at the CN accelerator facility of the INFN Legnaro National Laboratories (Italy), where the fast neutrons were produced by impinging a proton beam (4.5, 5.0 and 5.5MeV) on a 7LiF target. We tested a CLYC detector 6Li-enriched at about 95%, which is ideal for thermal neutron measurements, in parallel with another CLYC detector 7Li-enriched at more than 99%, which is suitable for fast neutron measurements.

Radiation Tolerance of LuAG:Ce and YAG:Ce Crystals Under High Levels of Gamma- and Proton-Irradiation

The extremely harsh conditions, in which the detectors will have to operate during the High Luminosity phase of the Large Hadron Collider at CERN, set stringent requirements on the properties of the scintillators which can be used. Among different scintillating materials under study, inorganic crystals such as LuAG:Ce and YAG:Ce represent good candidates for such application. A detailed investigation of the radiation hardness of LuAG:Ce and YAG:Ce crystal samples ( $1 \times 1 \times 1 ~\hbox{cm}^3$ cubes) produced by Crytur is presented in this study. Given their potential in many calorimeter designs, YAG:Ce samples with high aspect ratio ( $1 \times 1 \times 14 ~\hbox{cm}^3$ ) have also been tested. Optical and scintillating properties of the samples were studied before and after irradiation with different sources and at different intensities. Irradiation with gamma-rays to the doses of 1 and 100 kGy and with 24 GeV protons up to an integrated fluence of ${10^{14}}~\hbox{cm}^{ - 2}$ were performed at CERN. The scintillating properties of the crystals, as emission and excitation spectra and light yield remained unchanged after irradiation and only small levels of induced absorption were observed. The results obtained in this test confirm the potential of LuAG:Ce and YAG:Ce crystals as good candidates for calorimetry applications in future high energy physics experiments.

Light response of YAP:Ce and LaBr3:Ce scintillators to 4–30 MeV protons for applications to Telescope Proton Recoil neutron spectrometers

The light response of two thin inorganic scintillators based on YAP:Ce and LaBr3:Ce crystals has been measured with protons in the 4–8MeV energy range at the Uppsala tandem accelerator and in the 8–26MeV energy range at the Legnaro tandem accelerator. The crystals have been calibrated in situ with 137Cs and 60Co γ-ray sources. The relative light yields of protons with respect to gammas have been measured and are here reported to be (96±2)% and (80±2)% for YAP:Ce and LaBr3:Ce, respectively. The results open up to the development of a Telescope Proton Recoil spectrometer based on either of the two crystals as alternative to a silicon based spectrometer for applications to high neutron fluxes.

Role of flux on synthesis of poly single crystals of Ce3+ doped yttrium aluminum garnet

Yttrium aluminum garnet powders of good morphology are composed of tiny single crystals of regular faces. However, the growth mechanism of those ploy single crystals remains unknown. This paper provides morphology images of particles uncrushed, and it is found that those tiny crystals grow from large clusters in a pomegranate‐like manner. The morphology change occurs after phase transition, and is driven by flux, which provides a semi‐liquid environment around the crystals. This paper is beneficial for understanding growth mechanism of poly tiny single crystals of yttrium aluminum garnet powders.