Scintillation Yield Research Articles

Purcell-enhanced x-ray scintillation.

Scintillation materials convert high-energy radiation to optical light through a complex multistage process. The last stage of the process is spontaneous light emission, which usually governs and limits the scintillator emission rate and light yield. For decades, scintillator research focused on developing faster-emitting materials or external photonic coatings for improving light yields. Here, we experimentally demonstrate a fundamentally different approach: enhancing the scintillation rate and yield via the Purcell effect, utilizing optical environment engineering to boost spontaneous emission. This enhancement is universally applicable to any scintillating material and dopant when the material's nanoscale geometry is engineered. We design a thin multilayer nanophotonic scintillator, demonstrating Purcell-enhanced scintillation with 50% enhancement in emission rate and 80% enhancement in light yield. The emission is robust to fabrication disorder, further highlighting its potential for x-ray applications. Our results show prospects for bridging nanophotonics and scintillator science toward reduced radiation dosage and increased resolution for high-energy particle detection.

Exciton-harvesting enabled efficient charged particle detection in zero-dimensional halides

Materials for radiation detection are critically important and urgently demanded in diverse fields, starting from fundamental scientific research to medical diagnostics, homeland security, and environmental monitoring. Low-dimensional halides (LDHs) exhibiting efficient self-trapped exciton (STE) emission with high photoluminescence quantum yield (PLQY) have recently shown a great potential as scintillators. However, an overlooked issue of exciton-exciton interaction in LDHs under ionizing radiation hinders the broadening of its radiation detection applications. Here, we demonstrate an exceptional enhancement of exciton-harvesting efficiency in zero-dimensional (0D) Cs3Cu2I5:Tl halide single crystals by forming strongly localized Tl-bound excitons. Because of the suppression of non-radiative exciton-exciton interaction, an excellent α/β pulse-shape-discrimination (PSD) figure-of-merit (FoM) factor of 2.64, a superior rejection ratio of 10−9, and a high scintillation yield of 26 000 photons MeV−1 under 5.49 MeV α-ray are achieved in Cs3Cu2I5:Tl single crystals, outperforming the commercial ZnS:Ag/PVT composites for charged particle detection applications. Furthermore, a radiation detector prototype based on Cs3Cu2I5:Tl single crystal demonstrates the capability of identifying radioactive 220Rn gas for environmental radiation monitoring applications. We believe that the exciton-harvesting strategy proposed here can greatly boost the applications of LDHs materials.

Highly efficient In(I) doped Cs3Cu2I5 single crystals for light-emitting diodes and gamma spectroscopy applications

High-quality Cs3Cu2I5:In single crystals with a 7 mm diameter were grown by using the vertical Bridgman method. These crystals have a high optical transmittance (>75 %) and emit a bright red-orange light under both UV and X-ray irradiation. The Cs3Cu2I5:In crystals can exhibit a high photoluminescence quantum efficiency (PLQY) of 79.5 %, thus we explored the potential applications for light-emitting diodes (LED). The fabricated LED demonstrated CIE color coordinates of (0.553, 0.431) with a color rendering index (Ra) of 77, making it suitable for supplementary light in plant growth. Moreover, we evaluated their gamma-ray spectroscopy capability by using an avalanche photodiode (APD) detector. Under 137Cs gamma-ray irradiation, the gamma scintillation yield and energy resolution gradually degraded as the In concentration increased, which can be attributed to an enhanced afterglow after In doping.

On the Origin of the Light Yield Enhancement in Polymeric Composite Scintillators Loaded with Dense Nanoparticles.

Fast emitting polymeric scintillators are requested in advanced applications where high speed detectors with a large signal-to-noise ratio are needed. However, their low density implies a weak stopping power of high energy radiation and thus a limited light output and sensitivity. To enhance their performance, polymeric scintillators can be loaded with dense nanoparticles (NPs). We investigate the properties of a series of polymeric scintillators by means of photoluminescence and scintillation spectroscopy, comparing standard scintillators with a composite system loaded with dense hafnium dioxide (HfO2) NPs. The nanocomposite shows a scintillation yield enhancement of +100% with an unchanged time response. We provide for the first time an interpretation of this effect, pointing out the local effect of NPs in the generation of emissive states upon interaction with ionizing radiation. The obtained results indicate that coupling fast conjugated emitters with optically inert dense NPs could lead to surpassing the actual limits of pure polymeric scintillators.

DRiFT current mode, trigger settings and flexible detector specifications applied to scintillator arrays

MCNP radiation transport output is post-processed by DRiFT, a Detector Response Function Toolkit to simulate detailed nuclear instrumentation response. DRiFT can be used to assess the performance and potential limitations of scintillator, gas, and semiconductor detectors under a variety of simulated conditions not easily achievable in a laboratory setting. This work describes new updates in DRiFT for scintillator simulations which focus on the capability to simulate scintillators in current mode, an expansion of trigger options, and the ability to customize individual detector properties in a simulation. These improvements are designed to facilitate the ability to model large arrays of scintillator detectors with higher fidelity than was previously possible and are demonstrated in three examples. The first shows the difference between operating DRiFT in current and pulse mode. In the second example, which is intended to demonstrate deviations in individual detector performance, each detector has properties (PMT gain, optical transport, scintillation yield, etc.) that vary between detectors and are specified in DRiFT. A final example examines how DRiFT could be used to optimize digitizer settings in high rate measurements with split signals using the new common trigger option.

Understanding the xenon primary scintillation yield for cutting-edge rare event experiments

Xenon scintillation has been widely used in rare event detection experiments, such as in neutrinoless double beta decay, double electron captures and dark matter searches. Nonetheless, experimental values for primary scintillation yield in gaseous xenon (GXe) remain scarce and dispersed. The mean energy required to produce a scintillation photon, w sc, in GXe in the absence of recombination has been measured to be in the range of 34–111 eV. Lower w sc-values were reported for α-particles when compared to electrons produced by γ- or x-rays. Since w sc is expected to be similar for x-, γ-rays or electrons and almost equal to that obtained for α-particles, the above difference can not be understood. In addition, at present one may also pose the question of a dependence of w sc on photon energy. We carried out a systematic study on the absolute primary scintillation yield in GXe under reduced electric fields in the 70–300 V cm-1 bar-1 range and near atmospheric pressure, 1.2 bar, supported by a robust geometrical efficiency simulation model. We were able to clear-out the above standing problems: w sc was determined for x/γ-rays in the 5.9–60 keV energy range as well as for α-particles in the 1.5–2.5 MeV range, and no significant dependency neither on radiation type nor on energy has been observed. Our experimental w sc-values agree well with both up-to-date simulations and literature data obtained for α-particles. The discrepancy between our results and the experimental values found in the literature for x/γ-rays is discussed in this work and attributed to unaddressed large systematic errors in those previous studies. These findings can be extrapolated to other gases, and have impact on experiments such as double beta decay, double electron capture and directional dark matter searches while also on potential future detection systems such as DUNE-Gas. Only assuming the VUV emission band as is the case of most of the literature values, a mean w sc-value of 38.7 ± 0.6 (sta.)+7.7 -7.2 (sys.) eV was obtained. If the UV-VIS emission band is to be considered, the average energy to produce a photon was determined to be w 2nd = 43.5 ± 0.7 (sta.)+8.7 -8.1 (sys.) eV and w 3rd = 483 ± 7 (sta.+110 -105 (sys.) eV, in the VUV and UV-VIS bands, respectively.

Secondary scintillation yield from GEM electron avalanches in - and --isobutane for CYGNO — Directional Dark Matter search with an optical TPC

CYGNO is an international collaboration with the aim of operating a ▪ optical time projection chamber (TPC) for directional Dark Matter (DM) searches and solar neutrino spectroscopy, to be deployed at the Laboratori Nazionali del Gran Sasso (LNGS). A ▪/▪ (60/40) mixture is used, along with a triple Gas Electron Multiplier (GEM) cascade to amplify the ionisation signal. The scintillation produced in the electron avalanches is read out using a scientific complementary metal–oxide–semiconductor (sCMOS) camera. This solution has proven to provide very high sensitivity to interactions in the few ▪ energy range. The inclusion of a hydrogen-based gas will offer an even lighter target, resulting in a more efficient energy transfer in a DM particle collision, and consequently, a lower detection threshold. Additionally, longer track lengths of light nuclear recoils are easier to detect with a clearer direction. However, the addition of such gas will contribute to quenching the scintillation, jeopardizing the TPC performance. In this work, we demonstrate the feasibility of adding 1% to 5% isobutane to the ▪/▪ (60/40) mixture by measuring the respective absolute scintillation yield output. The overall scintillation produced in the charge avalanches is not drastically suppressed by quenching due to the isobutane addition. The presence of Penning transfer from excited He atoms to isobutane molecules increases the number of electrons in the avalanches, partially compensating for the loss of scintillation due to quenching. For the highest applied GEM voltage, the total number of photons produced in the avalanche per ▪ deposited in the absorption region presents a decrease of only a factor of about three, from 2.30(20)×104 to 8.2(4)×103▪, as the isobutane content increases from 0 to 5%. The quantification of the visible component of the scintillation shows that isobutane quenches both visible and ultraviolet (UV) photons emitted by ▪/▪.

Effects of rare earth codoping on the optical and scintillation properties of Cs3Cu2I5:Tl single crystals

In this work, the effects of rare earth ion codoping on the optical and scintillation performance of Cs3Cu2I5:Tl single crystals were studied. Cs3Cu2I5:Tl single crystals codoped with different concentrations of Sc3+, Y3+, and La3+ ions were grown by the Bridgman method. It was found that rare earth ion codoping reduces the optical transmittance of the as-grown crystals, in particular the coloring caused by Sc3+codoping. The luminescence mechanism associated with self-trapped exciton (STE) and Tl-related emissions has not been affected by the introduction of rare earth ion. The gamma scintillation yield and energy resolution are degraded after rare earth ion codoping.

Fast Emitting Nanocomposites for High‐Resolution ToF‐PET Imaging Based on Multicomponent Scintillators

AbstractTime‐of‐Flight Positron Emission Tomography (ToF‐PET) is a medical imaging technique, based on the detection of two back‐to‐back γ‐photons generated from radiotracers injected into the body. Its limit is the ability of employed scintillation detectors to discriminate in time the arrival of γ‐pairs, that is, the coincidence time resolution (CTR). A CTR < 50 ps will enable fast imaging with ultralow radiotracer dose. Monolithic materials do not have simultaneously the required high light output and fast emission characteristics, thus the concept of scintillating heterostructure is proposed, where the device is made of a dense scintillator coupled to a fast‐emitting light material. Here a composite polymeric scintillator loaded with hafnium oxide nanoparticles is presented. This enhanced by +300% its scintillation yield, by surpassing commercial plastic scintillators. The nanocomposite is coupled to bismuth germanate oxide (BGO) realizing a multilayer metascintillator. The energy sharing between its components is observed, which activates the nanocomposite's fast emission enabling a net CTR improvement of 25% with respect to monolithic BGO. These results demonstrate that a controlled loading with dense nanomaterials is an excellent strategy to enhance the performance of polymeric scintillators for their use in advanced radiation detection and imaging technologies.

Effects of Zr4+ and Hf4+ co-doping on luminescence and scintillation properties of LuYAG:Pr3+ single crystals grown by micro-pulling-down technique

In this study, we aim to clarify the luminescence and scintillation performance of 0.2 at%Pr3+-doped LuYAG scintillators with either zirconium or hafnium co-doping obtained using the micro-pulling-down (μ-PD) method. Under radiation excitation, scintillation properties such as light yield, decay time, and afterglow level were measured and compared to non-co-doped LuYAG:Pr3+. The positive effect of Zr and Hf co-doping is to significantly shorten the scintillation time response. The negative effect is the decrease of scintillation yield and increase of afterglow. We propose that the positively charged defects induced by Zr/Hf co-doping are responsible for the spatial correlated traps around Pr centers causing the shortened scintillation decay via non-radiative recombination processes, and the deep traps as well for the prolonged afterglow.

Energy deposition in liquid scintillators composed of CsPbBr3 colloidal nanocrystal dispersions.

Liquid scintillation processes are commonly used for various applications involving radioactivity levels analysis, as well as experiments in the field of high energy physics, most commonly in the form of organic scintillating cocktails. In this paper, we explore the potential of halide perovskite nanocrystal colloidal dispersions as an alternative to those organic mixtures. After an optimization of the nanocrystals' mean size and surface chemistry, the scintillation yield of these composite mixtures is evaluated through Compton - Triple to Double Coincidence Ratio experiments and compared with commercial liquid scintillator. The obtained results shine a light on the energy deposition mechanisms in nanocrystals-based liquid scintillators.

Optimal design and characteristic analysis of CsPbBr3 nanocrystals hybridized with 2,5-diphenyloxazole molecules for UV and X-ray detection

Scintillation is a flash of light produced in a material by the passage of a high-energy particle or photon. Desirable properties of scintillators, such as high quantum yield, low afterglow, and radiation hardness, are determined by their physical and optoelectronic properties. Metal halide perovskite (CsPbX3, X = Cl, Br, I) nanocrystals (NCs) have gained increasing attention as materials for optical and X-ray scintillators across a wide range of incident photon energies owing to their outstanding luminescent properties. In this study, we demonstrate the dependence of scintillation yield (SY) on incident photon energy ranging from ultraviolet (UV) light to X-rays in colloidal CsPbBr3 NCs hybridized with organic molecules (2,5-diphenyloxazole: PPO). The measured SY varied with the changing concentration ratio of NCs and PPO molecules. Experimental and theoretical analyses suggested that the SY is associated with the competition between photoluminescence quenching (reabsorption) and photoelectric effect enhanced by X-ray photon induced charge transfer from the organic molecules to the NCs. The optimally engineered hybrid nanomaterial scintillator exhibits excellent X-ray imaging with sharp image contrast (i.e., super-resolved edge spread function (ESF)), under X-ray irradiation commonly used for diagnosis.

Highly Efficient and Flexible Scintillation Screen Based on Organic Mn(II) Halide Hybrids toward Planar and Nonplanar X‐Ray Imaging

AbstractThe urgency for cost‐effective, high‐resolution, flexible X‐ray imaging detectors is generating great demand for scintillators with low‐temperature processability, high scintillation yield, and negligible afterglow. X‐ray imaging materials are currently dominated by inorganic scintillators in the form of rigid films and bulk crystals, which have inherent limitations including high‐temperature, complex synthesis, and considerable challenges toward advanced nonplanar imaging. Here, high‐performance and flexible X‐ray scintillators based on novel zero‐dimensional (0D) (BTPP)2MnX4 (BTPP = benzyltriphenylphosphonium; X = Cl, Br) halides are reported. They emit bright green light originating from the 4T1‐6A1 transition of Mn2+ under X‐ray excitation. In particular, (BTPP)2MnBr4 single crystals exhibit excellent air‐ and radiation‐stability, a high scintillation yield of 53 000 photons MeV−1, a low detection limit of 89.9 nGyair s−1, and an ultralow afterglow comparable to commercial Bi4Ge3O12 (BGO) single crystals. Moreover, the (BTPP)2MnCl4@polydimethylsiloxane (PDMS) flexible scintillation screens achieve a high spatial resolution of 14.1 lp mm−1 and realize high‐quality imaging results of nonplanar objects. This study demonstrates that the flexible scintillation screens based on low‐dimensional Mn(II) hybrid halides have significant potential for low‐dose and high‐resolution X‐ray imaging applications.

Impact of temperature on light yield and pulse shape discrimination of polysiloxane-based organic scintillators formulated with commercial resins

This work investigates how increased temperature affects neutron/γ discrimination and light yield (LY) in several different polysiloxane-based scintillators doped with either 9,9-dimethyl-2-phenylflourene (PhF) or 2,5-diphenyloxazole (PPO) as a primary fluorophore and 9,9-dimethyl-2,7-di((E)-styryl) fluorene (SFS) as the secondary fluorophore. The polysiloxane matrices were prepared from the commercial resins Wacker Lumisil 579 or Shin-Etsu KER-6000. Control scintillators were prepared from poly(vinyltoluene) (PVT), the industry standard matrix, as a reference point for LY and pulse shape discrimination (PSD) measurements. Samples with PhF and PPO dopant concentrations of 1 wt% and 5 wt% in the polysiloxanes and 3 wt% and 5 wt% in the PVT samples were tested at 20 °C, 35 °C, and 50 °C. In the polysiloxane samples, the KER-6000 resin outperformed the Wacker 579 and PhF proved to be a better dopant than PPO in both LY and PSD capabilities. Polysiloxane scintillators showed slight decreases in LY and increases in neutron/γ discrimination at increased temperatures, while PVT scintillators showed a similar LY decrease with little to no improvement in neutron/γ discrimination at increased temperatures. Overall, polysiloxane scintillators may not require recalibration in applications where temperatures increase up to 50 °C.

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.

Tellurium-loaded organic scintillators

The R&D results of new tellurium-loaded liquid and plastic scintillators (TeLS and TePS) for the experiments on the search for neutrinoless double beta decay are presented. Linear alkylbenzene and polystyrene are used as a scintillation base for TeLS and TePS, respectively. Diphenyltellurium di-2-ethylhexanoate and a complex compound of diphenyltellurium oxide and di-(2-ethylhexyl)phosphoric acid are proposed as tellurium-containing additives. The transparency, light yield and long-term stability of the organic scintillators are discussed.

Secondary scintillation properties of multi-layer THGEMs operated in low-pressure CF4 and Ar/5%Xe

We present a measurement of the secondary scintillation yield produced by two-layer Thick Gas Electron Multipliers (M-THGEMs) in pure Tetrafluoromethane (CF4) gas and in Ar mixed with 5% Xe in low-pressures down to 20 Torr. The detector was irradiated with 5.49 MeV alpha particles from a low-rate 241-Am source. The secondary scintillation light generated during the gas avalanche process was read out by a Hamamatsu photomultiplier tube (model R8520-406), sensitive to a broad wavelength range (160–650 nm). The avalanche charge was collected on the bottom electrode of M-THGEM and correlated to the scintillation light on an event-by-event basis. We observed that, for both gas types, the value of the photon to electron production ratio (0.4 ph/el in CF4 and 0.1 ph/el in Ar/5%Xe) increases with the thickness of the M-THGEM electrodes and varies significantly with the pressure, being higher at lower values. The decrease in electroluminescence yield at higher pressures is much more pronounced in the Ar/Xe mixture. In addition, because of a larger gas avalanche volume, the electroluminescence light yield is larger in thicker M-THGEM structures. Presented results are particularly useful for designing the next generation of Optical-readout Time Projection Chambers (O-TPCs) operated at low-pressure CF4; applications include experimental nuclear physics with rare isotope beams, dark matter detection with directional sensitivity and observation of the Migdal effect in a low-pressure Optical TPC.

One-dimensional scintillator film with benign grain boundaries for high-resolution and fast x-ray imaging.

Fast and high-resolution x-ray imaging demands scintillator films with negligible afterglow, high scintillation yield, and minimized cross-talk. However, grain boundaries (GBs) are abundant in polycrystalline scintillator film, and, for current inorganic scintillators, detrimental dangling bonds at GBs inevitably extend radioluminescence lifetime and increase nonradiative recombination loss, deteriorating afterglow and scintillation yield. Here, we demonstrate that scintillators with one-dimensional (1D) crystal structure, Cs5Cu3Cl6I2 explored here, possess benign GBs without dangling bonds, yielding nearly identical afterglow and scintillation yield for single crystals and polycrystalline films. Because of its 1D crystal structure, Cs5Cu3Cl6I2 films with desired columnar morphology are easily obtained via close space sublimation, exhibit negligible afterglow (0.1% at 10 ms) and high scintillation yield (1.2 times of CsI:Tl). We have also demonstrated fast x-ray imaging with 27 line pairs mm-1 resolution and frame rate up to 33 fps, surpassing most existing scintillators. We believe that the 1D scintillators can greatly boost x-ray imaging performance.

Perovskite Scintillators for Improved X‐ray Detection and Imaging

AbstractHalide perovskites (HPs) recently have emerged as one class of competitive scintillators for X‐ray detection and imaging owing to its high quantum efficiency, short decay time, superior X‐ray absorption capacity, low cost, and ease of crystal growth. The tunable structure and versatile chemical compositions of halide perovskites provide distinguishable advantages over traditional inorganic scintillators for optimizing scintillation performance. Since the first observation of the scintillation phenomenon in HPs, substantial efforts have been devoted to expanding the inventory of HP scintillators and regulating material properties. Understanding the relationship between the structure and scintillation properties of HP scintillators is essential for developing materials with improved X‐ray detection and imaging capacities. This review summarizes strategies for improving the light yield of HP scintillators and provides a roadmap for improving the X‐ray imaging performance. Additionally, methods for controlling the light propagation direction in HP scintillators are highlighted for improving X‐ray imaging resolution. Finally, we highlight the current challenge in HP scintillators and provide a perspective on the future development of this emerging scintillator.

Perovskite Scintillators for Improved X-ray Detection and Imaging.

Halide perovskites (HPs) recently have emerged as one class of competitive scintillators for X-ray detection and imaging owing to its high quantum efficiency, short decay time, superior X-ray absorption capacity, low cost, and ease of crystal growth. The tunable structure and versatile chemical compositions of halide perovskites provide distinguishable advantages over traditional inorganic scintillators for optimizing scintillation performance. Since the first observation of the scintillation phenomenon in HPs, substantial efforts have been devoted to expanding the inventory of HP scintillators and regulating material properties. Understanding the relationship between the structure and scintillation properties of HP scintillators is essential for developing materials with improved X-ray detection and imaging capacities. This review summarizes strategies for improving the light yield of HP scintillators and provides a roadmap for improving the X-ray imaging performance. Additionally, methods for controlling the light propagation direction in HP scintillators are highlighted for improving X-ray imaging resolution. Finally, we highlight the current challenge in HP scintillators and provide a perspective on the future development of this emerging scintillator.