Scintillation Mechanism Research Articles

Emulator-based Bayesian inference on non-proportional scintillation models by compton-edge probing

Scintillator detector response modeling has become an essential tool in various research fields such as particle and nuclear physics, astronomy or geophysics. Yet, due to the system complexity and the requirement for accurate electron response measurements, model inference and calibration remains a challenge. Here, we propose Compton edge probing to perform non-proportional scintillation model (NPSM) inference for inorganic scintillators. We use laboratory-based gamma-ray radiation measurements with a NaI(Tl) scintillator to perform Bayesian inference on a NPSM. Further, we apply machine learning to emulate the detector response obtained by Monte Carlo simulations. We show that the proposed methodology successfully constrains the NPSM and hereby quantifies the intrinsic resolution. Moreover, using the trained emulators, we can predict the spectral Compton edge dynamics as a function of the parameterized scintillation mechanisms. The presented framework offers a simple way to infer NPSMs for any inorganic scintillator without the need for additional electron response measurements.

Scintillation and radioluminescence mechanism in β-Ga2O3 semiconducting single crystals

In this paper, we present the results of experiments on samples of β-Ga2O3 single crystals under a project aimed at assessing and improving the scintillation performance of this material by studying scintillation and radioluminescence mechanism and its limitations. In addition to standard experiments, such as scintillation light yields and time profiles, radio-, and thermoluminescence, we developed and tested a new and promising two-beam experiment, in which a sample is excited by an X-ray beam and additionally stimulated by an IR laser diode.Fe and Mg doping compensate for the inherent n-type conductivity of β-Ga2O3 to obtain semi-insulating single crystals for large-area substrates and wafers. At the same time, residual Fe and Ir are ubiquitous uncontrolled impurities leached from the Ir crucibles used to grow large bulk crystals by the Czochralski method.For these experiments, we selected four samples cut from the Czochralski grown 2-cm diameter β-Ga2O3 single crystal boules; one with a reduced Fe content, two unintentionally Fe- and Ir-doped (UID) with lower and higher Fe content, and one doped with Mg.We find that steady-state radioluminescence spectra measured at temperatures between 10 and 350 K are dominated by the UV emission peaking at about 350–370 nm. Unfortunately, even for the best sample with a reduced Fe-content, the intensity of this emission drops precipitously with the temperature down to about 10 % at 300 K.From the two-beam experiments, we conclude that recombination via inadvertent Fe impurity involving three charge states (2+, 3+, and 4+) may reduce a steady-state UV emission of β-Ga2O3 under X-ray excitation by as much as 60–70 %, one-third to one-half of which is due to the recombination (specific for Fe-doped β-Ga2O3) involving the 4+ and 3+ charge states of Fe and the remaining 50–70 % being due to a more familiar route typical of other oxides, involving the 2+ and 3+ charge states of Fe. These losses are at higher temperatures enhanced by a thermally activated redistribution of self-trapped holes (STHs). In addition, the trapping of electrons by Fe and holes by Mg, Fe, and Ir may be responsible for scintillation light loss and reduction of the zero-time amplitude essential for the fast timing scintillation applications.Despite indirect evidence of competitive recombination in β-Ga2O3 involving a deep Ir3+/4+ donor level, we could not quantitatively assess losses of the UV steady state radioluminescence light due to the inadvertent Ir impurity.

Ultrafast and Radiation-Hard Lead Halide Perovskite Nanocomposite Scintillators.

The use of scintillators for the detection of ionizing radiation is a critical aspect in many fields, including medicine, nuclear monitoring, and homeland security. Recently, lead halide perovskite nanocrystals (LHP-NCs) have emerged as promising scintillator materials. However, the difficulty of affordably upscaling synthesis to the multigram level and embedding NCs in optical-grade nanocomposites without compromising their optical properties still limits their widespread use. In addition, fundamental aspects of the scintillation mechanisms are not fully understood, leaving the scientific community without suitable fabrication protocols and rational guidelines for the full exploitation of their potential. In this work, we realize large polyacrylate nanocomposite scintillators based on CsPbBr3 NCs, which are synthesized via a novel room temperature, low waste turbo-emulsification approach, followed by their in situ transformation during the mass polymerization process. The interaction between NCs and polymer chains strengthens the scintillator structure, homogenizes the particle size distribution and passivates NC defects, resulting in nanocomposite prototypes with luminescence efficiency >90%, exceptional radiation hardness, 4800 ph/MeV scintillation yield even at low NC loading, and ultrafast response time, with over 30% of scintillation occurring in the first 80 ps, promising for fast-time applications in precision medicine and high-energy physics. Ultrafast radioluminescence and optical spectroscopy experiments using pulsed synchrotron light further disambiguate the origin of the scintillation kinetics as the result of charged-exciton and multiexciton recombination formed under ionizing excitation. This highlights the role of nonradiative Auger decay, whose potential impact on fast timing applications we anticipate via a kinetic model.

Simulation of Electron-Hole Pairs Created by γ-Rays Interaction in Scintillation Crystals Using Geant4 Toolkit

Understanding the electron-hole pair (e-h pair) production process in scintillators is essential for further studies of the scintillation mechanism. The number of e-h pairs can be derived from theoretical and empirical approaches. However, simulation approaches have been chosen to study all the related physical processes and spatial information in scintillation crystals. Due to the complexity of particle interaction and physical properties of solid-state, the simulation approach could be better than the analytical approach. This work aims to develop a Geant4-based simulation toolkit for studying scintillation mechanisms in single-crystalline scintillators since Geant4 can accurately calculate particle energy loss. Due to the lack of a solid-state physic model for insulators, the plasmon creation and phonon loss process for electrons are implemented in the Geant4 toolkit. The electrons, which are created by γ-rays interaction in crystals, can make further ionization to generate secondary electrons or create plasmons, or lose energy to phonons. Then the created plasmons decay into e-h pairs. These electrons and holes are tracked with information on energy and position. Therefore, the number of created e-h pairs and their spatial distribution can be extracted. In this work, we will present the result of the creation process of e-h pairs per MeV in scintillation crystals induced by γ-rays interaction. The number of e-h pairs created by γ ray in some popular inorganic crystals has been calculated. Assuming maximum conversion efficiency from the e-h pair to the luminescence light, we can calculate the maximum light yield of the intrinsic scintillator.

On the Quenching Mechanism of Ce, Tb Luminescence and Scintillation in Compositionally Disordered (Gd, Y, Yb)3Al2Ga3O12 Garnet Ceramics

Two series of (Gd, Y, Yb)3Al2Ga3O12 quintuple compounds with a garnet structure and solely doped with Ce and Tb were prepared in the form of ceramics by sintering in oxygen at 1600 °C for two hours and studied for the interaction of activator ions with ytterbium ions entering the matrix. It was shown that the photoluminescence and scintillation of Ce3+ ions are completely suppressed, predominantly by tunneling ionization through the charge transfer state (CTS) of the Ce4+-Yb2+ ions. The photoluminescence of Tb3+ ions is quenched in the presence of ytterbium, but not completely due to the poor resonance conditions of Tb3+ intraconfiguration transitions and the CTS of the single Yb3+ and the CTS of Ce4+-Yb2+ ions. The scintillation in the visible range of both Ce3+- and Tb3+-doped samples is intensely quenched as well, which indicates strong competition from Yb3+ ions to activators in interaction with the Gd substrate.

All‐Inorganic Glass Scintillators: Scintillation Mechanism, Materials, and Applications

AbstractGlass scintillators have several benefits compared to the currently used single or polycrystalline scintillators, including non‐hygroscopicity, mechanical ruggedness, ease of producing customizable shapes, and low‐cost synthesis. The combination of the inert glass matrix and the embedded highly scintillating center render them significant materials for medical imaging and therapy, non‐destructive probing, nuclear monitoring, and high‐energy physics. Recently, great progress has been made in exploring new kinds of glass scintillator materials, improving imaging resolution for radiation detection, and developing an enormous range of commercial products. However, the majority of efforts have been devoted to the variation of materials, while rationally designing this new family of scintillators toward expected properties and applications is still lacking. In this review, the focus is specifically on advances in glass scintillators, including the scintillation fundamentals, material designing rule, and current application status, as well as future challenges and future directions.

PEA2PbI4: fast two-dimensional lead iodide perovskite scintillator with green and red emission

Among the two-dimensional hybrid organic-inorganic perovskites, PEA2PbBr4 is one of the best scintillators combining high light yield and fast nanosecond decay time. However, it has limited sensitivity to X-ray and positron emission tomography because of insufficient mass density and effective atomic number. In this article, we show that exchanging the halide from bromide to iodide allows to shorten the absorption length as much as two times for X-ray energies. We present a detailed study on scintillation properties of self-grown samples of PEA2PbI4 crystal, which we compare with the previously reported results for PEA2PbBr4 crystal. The synthesis method of PEA2PbI4 crystal is based on dissolving the perovskite precursors in hydroiodic acid, which is then stirred and left for evaporation. Our measurements include the characterizations with optical, X-ray, and γ-ray sources. We observe two emission bands of PEA2PbI4 crystal centered at 532 (green) and 660 (red) nm, and we link them to the scintillation mechanisms involving exciton and surface defect states. We also report the scintillation light yields of 1,000 and 10,000 photons/MeV at room temperature and 10 K, respectively, and the coincidence timing resolution full width at half maximum of 138 ps, and the fast component in scintillation decay curve of 0.5 ns. This fast component is much faster than that of 13.4 ns of PEA2PbBr4 crystal, and with two times shorter absorption length, it secures better opportunities in timing applications in particular time-of-flight positron emission tomography and high energy physics.

Radiation resistance of praseodymium-doped aluminum lithium fluorophosphate scintillator glasses for laser fusion experiments

We report the gamma (γ)-ray radiation resistance of praseodymium (Pr3+)-doped aluminum lithium fluorophosphate scintillator glasses. For its assessment as a scintillator material for laser fusion experiments, a 20Al(PO3)3-80LiF-PrF3 (Pr3+-doped APLF) glass was irradiated with γ-rays from a cobalt-60 (60Co) source resulting in an absorbed dose of 5.2 kGy. Although γ-ray-irradiation results in increased absorption due to phosphorus-oxygen hole centers (POHCs) and PO3 2− electron centers (PO3 ECs), these radiation-induced defects do not modify the glass emission as both non-irradiated and γ-ray-irradiated glasses exhibit similar emission spectra and decay times under optical and X-ray excitation. The emission peaks observed also correspond to the different interconfigurational 4f5d → 4f2 and intraconfigurational 4f2 transitions of Pr3+ ions which are neither oxidized nor reduced by irradiation. Our results show that Pr3+-doped APLF glass still maintains its characteristic fast decay time and that γ-ray irradiation does not affect the glass scintillation mechanisms.

Pulse Shape Discrimination of low-energy nuclear and electron recoils for improved particle identification in NaI:Tl

The scintillation mechanism in NaI:Tl crystals produces different pulse shapes that are dependent on the incoming particle type. The time distribution of scintillation light from nuclear recoil events decays faster than for electron recoil events and this difference can be categorised using various Pulse Shape Discrimination (PSD) techniques. In this study, we measured nuclear and electron recoils in a NaI:Tl crystal, with electron equivalent energies between 2 and 40 keV. We report on a new PSD approach, based on an event-type likelihood; this outperforms the charge-weighted mean-time, which is the conventional metric for PSD in NaI:Tl. Furthermore, we show that a linear combination of the two methods improves the discrimination power at energies greater than 10 keV.

Role of the Dilution of the Gd Sublattice in Forming the Scintillation Properties of Quaternary (Gd,Lu)3Al2Ga3O12: Ce Ceramics

Technological factors and processes contributing to the scintillation mechanism have been considered in quaternary garnet ceramics doped with Ce(Gd,Lu)3Al2Ga3O12. The super-stoichiometric additive of gadolinium in the material composition or its co-doping with a low concentration of Mg were found to be effective tools to suppress phosphorescence in the quaternary garnet, confirming that it is not an intrinsic property of the material. The Monte-Carlo simulation of electronic excitation transfer demonstrates that the hopping migration along the gadolinium sublattice plays an essential role in forming the scintillation kinetic parameters. Breaking the integrity of the gadolinium sublattice by substitution with heavier lutetium ions increases the role of self-trapped states in the excitation of Ce3+ ions, which ensures both an increase in the fraction of short ~20 ns and very long ~600 ns components in the scintillation kinetics.

Design rules for time of flight Positron Emission Tomography (ToF-PET) heterostructure radiation detectors

Despite the clinical acceptance of ToF-PET, there is still a gap between the technology's performance and the end-user's needs. Core to bridging this gap is the ability to develop radiation detectors combining a short attenuation length and a sub-nanosecond time response. Currently, the detector of choice, Lu2SiO5:Ce3+ single crystal, is not selected for its ability to answer the performance needs, but as a trade-off between requirements and availability. To bypass the current performance limitations, in particular restricted time response, the concept of the heterostructured detector has been proposed. The concept aims at splitting the scintillation mechanisms across two materials, one acting primarily as an absorber and one as an ultra-fast emitter. If the concept has attracted the interest of the medical and material communities, little has been shown in terms of the benefits/limitations of the approach. Based on Monte Carlo simulations, we present a survey of heterostructure performance versus detector design. The data allow for a clear understanding of the design/performance relationship. This, in turn, enables the establishment of design rules toward the development and optimization of heterostructured detectors that could supersede the current detector technology in the medical imaging field but also across multiple sectors (e.g. high-energy physics, security).

Time and band-resolved scintillation in time projection chambers based on gaseous xenon

We present a systematic study of the time and band-resolved scintillation in xenon-based time projection chambers (TPCs), performed simultaneously for the primary (S1) and secondary (S2) components in a small, purity-controlled, setup. We explore a range of conditions of general academic interest, focusing on those of relevance to contemporary TPCs: pressure range 1–10 bar, pressure-reduced electric fields of 0–100 V/cm/bar in the drift region (S1) and up to the proportional scintillation regime in the multiplication region (S2), and wavelength bands 145–250/250–400/400–600 nm, for both alpha and beta particles. Attention is paid to the possibility of non-conventional scintillation mechanisms such as the 3rd continuum emission, recombination light from beta -electrons at high pressure (for S1), emission from high-lying excited states and neutral bremsstrahlung (for S2). Time constants and, specially, scintillation yields have been obtained as a function of electric field and pressure, the latter aided by Geant4 simulations.

Neutral Bremsstrahlung Emission in Xenon Unveiled

We present evidence of non-excimer-based secondary scintillation in gaseous xenon, obtained using both the NEXT-White TPC and a dedicated setup. Detailed comparison with first-principle calculations allows us to assign this scintillation mechanism to neutral bremsstrahlung (NBrS), a process that has been postulated to exist in xenon that has been largely overlooked. For photon emission below 1000 nm, the NBrS yield increases from about 10$^{-2}$ photon/e$^{-}$ cm$^{-1}$ bar$^{-1}$ at pressure-reduced electric field values of 50 V cm$^{-1}$ bar$^{-1}$ to above 3$\times$10$^{-1}$ photon/e$^{-}$ cm$^{-1}$ bar$^{-1}$ at 500 V cm$^{-1}$ bar$^{-1}$. Above 1.5 kV cm$^{-1}$ bar$^{-1}$, values that are typically employed for electroluminescence, it is estimated that NBrS is present with an intensity around 1 photon/e$^{-}$ cm$^{-1}$ bar$^{-1}$, which is about two orders of magnitude lower than conventional, excimer-based electroluminescence. Despite being fainter than its excimeric counterpart, our calculations reveal that NBrS causes luminous backgrounds that can interfere, in either gas or liquid phase, with the ability to distinguish and/or to precisely measure low primary-scintillation signals (S1). In particular, we show this to be the case in the "buffer" and "veto" regions, where keeping the electric field below the electroluminescence (EL) threshold will not suffice to extinguish secondary scintillation. The electric field in these regions should be chosen carefully to avoid intolerable levels of NBrS emission. Furthermore, we show that this new source of light emission opens up a viable path towards obtaining S2 signals for discrimination purposes in future single-phase liquid TPCs for neutrino and dark matter physics, with estimated yields up to 20-50 photons/e$^{-}$ cm$^{-1}$.

Prospects of charge signal analyses in liquid xenon TPCs with proportional scintillation in the liquid phase

As liquid xenon TPCs increase in target mass while pursuing the direct detection of WIMP dark matter, the technical challenges arising due to their size call for new solutions and open the discussion on alternative detector concepts. Proportional scintillation in liquid xenon allows for a single-phase design evading problems related to the liquid-gas interface and the precise gas gap required in a dual-phase TPC.Aside from a different scintillation mechanism, the successful detection- and analysis scheme of state-of-the-art experiments is maintained in this approach.We study the impact on charge signal analysis in a single-phase detector of DARWIN dimensions, where the fast timing of the proportional scintillation signal allows for the precise identification of the single electrons in the ionisation signal.Such a discrete electron-counting approach can lead to a better signal resolution for low energies when compared to the classical dual-phase continuous method.The absence of the liquid-gas interface can further benefit the S2-only energy resolution significantly. This can reduce the uncertainties from the scintillation and signal-detection process to a level significantly below the irreducible fluctuation in the primary ionisation. Exploiting the precise electron arrival time information can further allow for a powerful single vs. multiple site interaction discrimination with 93% rejection efficiency and 98% signal acceptance. This outperforms the design goal of the DARWIN observatory by a reduction factor of 4.2 in non-rejected multiple site neutron events.

Temperature dependent scintillation properties and mechanisms of (PEA)2PbBr4 single crystals.

In this work the scintillation properties of PEA2PbBr4 are studied as function of temperature, accessing the potential use of these materials for low temperature applications. The scintillation properties and mechanism have been studied using a combination of temperature dependent photoluminescence emission and excitation, X-ray excited emission and decay measurements. At room temperature the X-ray excited emission is dominated by the 442 nm emission with a lifetime of 35.2 ns. Under UV-Vis photon excitation an additional emission peak is observed at 412 nm. At 10 K, both X-ray and UV-Vis photon excited emission spectra show a narrow emission peak at 412 nm and a broad emission band centred around 525 nm with a lifetime of 1.53 ns (24%) and 154 ns (76%) respectively. The exact nature of the observed emission peaks is not known. For this reason two potential mechanisms explaining the difference between UV-Vis photon and X-ray excitation and their temperature dependent emissions are explored. The total spectral intensity decreases to 72% of the intensity at room temperature at 10 K. It is suggested that the observed negative thermal quenching behaviour results from a combination of more self absorption and a higher degree of self trapped exciton formation under X-ray excitation. Based on the observed fast decay component at 10 K and light yield of 9400 photons per MeV at room temperature, showing only a 28% decrease at 10 K, could make this material potentially interesting for low temperature and fast timing applications.

An all-inorganic Li-doped Cs3Cu2I5 single crystal for dual gamma ray and neutron detection applications

Study on the growth and scintillation mechanism of Li+-doped Cs3Cu2I5 crystal with an excellent FOM value for dual gamma-ray and neutron detection applications.

Improvement of Performance Characteristics for LiI:Ag Single‐Crystal Scintillators by Defect Structure Tailoring Using Sr Codopant

Lithium iodides are very efficient single‐crystal scintillators for thermal neutron detection. Doping with silver, as activator ions, has shown to improve its limitation of discriminating gamma background by introducing pulse shape discrimination ability. To improve the scintillation performance, single crystals of LiI:Ag, codoped with different concentration of Sr ions, are grown and characterized in details. A systematic investigation of radioluminescence, thermoluminescence, and scintillation properties along with the decay kinetics provides better understanding about the role of defect structure in scintillation mechanism. The extra charge, provided by Sr2+ ions, is found to alter the defect structure with relative reduction of the contribution from the deeper trap centers in comparison with the shallow traps. Consequently, it leads to a significant improvement of light yield quenching under higher excitation density of charged particle irradiation. The 0.1% Sr codoped crystals provide a better discrimination ability of neutron and gamma radiations for simultaneous detection.

Gd-admixed (Lu,Gd)AlO3 single crystals: breakthrough in heavy perovskite scintillators

We report a breakthrough concept for a bulk single crystal as a heavy aluminum perovskite scintillator, where due to bandgap engineering by a balanced Gd admixture in a Lu cation sublattice, the scintillation performance dramatically increases. In an optimized composition of (Lu, Gd)AlO3:Ce (LuGdAP:Ce), the light yield approaches 21,000 phot/MeV, which is close to that of classical but much less dense YAP:Ce and 50% higher than the best LuYAP:Ce reported in the literature. Moreover, contrary to LuYAP:Ce, the LuGdAP host maintains a high effective atomic number close to that of LuAP:Ce (Zeff = 64.9), which is comparable to commercial LSO:Ce. An enormous decrease in afterglow on the millisecond time scale and acceleration in the rise time of the scintillation response further increase the application potential of the LuGdAP host. The related acceleration of the transfer stage in the scintillation mechanism due to diminishing electron trap depths is proven by thermally stimulated luminescence (TSL). Furthermore, we quantitatively characterize and model the energy transfer processes that are responsible for the change in the photoluminescence and scintillation decay kinetics of Ce3+ in the LuGdAP matrix. Such an innovative (Lu, Gd)AP:Ce scintillator will become competitive for use in applications that require heavy, fast, and high light yield bulk scintillators.

Analysis and comparison of the Core-to-Valence Luminescence mechanism in a large CLYC crystal under neutron and γ-ray irradiation through optical filtering selection of the scintillation light

7Li enriched Cs2LiYCl6:Ce3+ (CLYC) is a promising inorganic scintillator for real-time γ-ray and fast neutron spectrometry. The neutron/γ-ray discrimination is usually accomplished exploiting the different quenching effects of high Linear Energy Transfer (LET) particles on different scintillation mechanisms, usually by means of the time analysis of the pulse shape. In principle, the emission wavelength information could be used to address the same task. However, a systematic study of the correlations between the CLYC decay time, its radio-luminescence spectrum and the LET of the impinging particle has not yet been performed. We therefore investigated the CLYC scintillation process under neutron and γ-ray irradiation, correlating the time response to the scintillation wavelength spectrum using a 1–inch right cylinder>99% 7Li enriched CLYC. We found that the relative intensity of the Core to Valence Luminescence (CVL) is almost constant with photons in the energy range 20–660 keV, i.e. 0.5–5 keV/μm LET, and is only partially quenched by neutrons. Instead, the direct electron-hole capture scintillation mechanism is completely cut under neutron irradiation. The luminescence in between the deep-Ultraviolet and the Near Ultraviolet region (250–350 nm) might be attributed to both the CVL and the host luminescence, also in thick highly Ce3+-doped crystals.

Co-Adjuvant Nanoparticles for Radiotherapy Treatments of Oncological Diseases

Nanomedicine is emerging as promising approach for the implementation of oncological methods. In this review, we describe the most recent methods exploiting heavy nanoparticles and hybrid nanomaterials aiming at improving the traditional X-rays-based treatments. High-Z nanoparticles are proposed as radiosensitizers due to their ability to stop the ionizing radiation and to increase the locally delivered therapeutic dose. Other nanoparticles working as catalysts can generate reactive oxygen species upon X-rays exposure. Thanks to their high toxicity and reactivity, these species promote DNA cancer cells damage and apoptosis. Hybrid nanoparticles, composed by scintillators coupled to organic molecules, are suitable in X-rays activated photodynamic therapy. This work highlights the roles played by the diverse nanoparticles, upon ionizing radiation irradiation, according to their physico-chemical properties, surface functionalization, and targeting strategies. The description of nanoparticle qualities demanded by the oncological nanomedicine is presented in relation to the processes occurring in biological medium when X-ray radiation interacts with heavy nanoparticles, including the scintillation mechanisms, the stopping power amplification, and the disputed modeling of the effective deposit of energy within nanomaterials. The comprehension of these issues in nanomedicine drives the strategies of nanoparticles engineering and paves the way for the development of advanced medical therapies.