High Energy Radiation Detection Research Articles

Mapping and Characterization of Local Structures of CsPbBr3.

Inorganic perovskite CsPbBr3 is a promising material for optoelectronic applications and high-energy radiation detection due to its excellent photophysical properties, high carrier mobility, large carrier diffusion length, and higher stability than organic perovskite materials. Understanding phase transitions at the atomic level is crucial for optimizing its applications. Here, we employ experimental characterizations and molecular dynamics simulations to study the phase transitions in CsPbBr3 as a function of temperature. The simulation results are compared with the experimental results, which include X-ray diffraction (XRD). Our simulations provide new insights into the electronic structure and dynamic behavior of the Cs, Pb, and Br atoms as a function of temperature. We observe distinct phase transitions from monoclinic to cubic and analyze the associated changes in the local environment through atomic density contour maps. Our analysis of the atomic density distributions of the Pb, Br, and Cs atoms provides information about the crystal symmetry as a function of temperature. The tilt and rotation angles of [PbBr6] octahedra are increasing with the temperature increase and are found nonzero above 410 K when the structure is cubic, exhibiting the presence of dynamic tilting. Overall, our findings shed light on the thermal stability and structural dynamics of CsPbBr3, contribute to the fundamental understanding of its phase behavior, and provide a crucial pivot for guiding the design of next-generation optoelectronic and radiation detection devices.

Superdense Ce3+-activated lutetium silicate scintillating glass for radiation detection

The scintillating photonic glass has the great potential for medicine imaging, nuclear physics, high-energy physics, and national defense. However, the development of the candidate with the high density remains a significant challenge. Herein, the superdense scintillating glasses derived from the Ce3+-activated Lu2O3-SiO2 binary system were successfully fabricated by the strategy of contactless aerodynamic levitation heating under the N2 atmosphere. These glasses are colorless, optical homogeneous, and exhibit superdense density from 6.59 to 7.15 g/cm3, representing the highest density among the fast decay glass systems. The materials present excellent radiation-blocking ability, suitable emission wavelength, and fast response, indicating the promise for fast-event X-ray detection. The micro radiation probe was fabricated by connecting the scintillating glass and the optical fiber. The practical application in remote radiation detection is demonstrated and it exhibits excellent linear response and high signal-to-noise ratio. The results confirm that the fabricated superdense scintillating glass is promising for application in the field of high-energy radiation detection.

Stability of Cesium-Based Lead Halide Perovskites under UV Radiation.

Lead halide perovskites have been extensively studied for their potential applications, including photodetectors, solar cells, and high-energy radiation detection. These applications are possible because of their unique optoelectronic properties, such as tunable band gap, high optical absorption coefficient, and unique defect self-healing properties, which result in high defect tolerance. Despite these advantages, the long-term stability remains a critical issue that could hinder commercial applications of these materials. Reports on the stability of lead halide perovskites for optoelectronic applications have normally focused on methylammonium (MA)/formamidinium (FA), with very limited information for other systems, in particular, Cs-containing perovskites. In this paper, we report the stability of thick CsPbBr3-x Cl x polycrystalline thin films (∼8 μm) with several halide Br-Cl ratios after exposure to deep UV radiation. The chemical, crystal structure, optical, and electrical properties are analyzed, and the results are used to propose a degradation mechanism. The chemical analysis on the surface and bulk of the films indicates the formation of cesium oxide after UV exposure, with no significant change in the crystalline structure. The proposed mechanism explains the formation of cesium oxides during UV exposure. The I-V characteristics of diode structures also showed significant degradation after UV exposure, primarily at lower diode rectification ratios. The mechanism proposed in this paper can contribute to developing strategies to enhance the long-term stability of inorganic lead halide perovskites under UV exposure.

Cold-Sintered All-Inorganic Perovskite Bulk Composite Scintillators for Efficient X-ray Imaging.

Cost-effective bulk scintillators with high density, large-area, and long-term stability are desirable for high-energy radiation detections. Conventional bulk polycrystalline or single-crystal scintillators are generally synthesized by high-temperature approaches, and it is challenging to realize simultaneously high detectivity/responsivity, spatial resolution, and rapid time response. Here, we report the cold sintering of bulk scintillators (at 90 °C) based on an "emitter-in-matrix" principle, in which emissive CsPbBr3 nanocrystals are embedded in a durable and transparent Cs4PbBr6 matrix. These bulk scintillators exhibit high light yield (33,800 photons MeV-1), low detection limit (79 nGyair s-1), fast decay time (9.8 ns), and outstanding spatial resolution of 8.9 lp mm-1 to X-ray radiation and an energy resolution of 19.3% for γ-ray (59.6 keV) detection. The composite scintillator also shows exceptional stability against environmental degradation and cyclic X-ray radiation. Our results demonstrate a cost-effective strategy for developing perovskite-based bulk transparent scintillators with exceptional performance and high radioluminescence stability for high-energy radiation detection and imaging.

High-Performance and Stable Perovskite X-ray Detection and Imaging Based on a Ti Cathode.

High-energy radiation detectors with a good imaging resolution, fast response, and high sensitivity are desired to operate at a high electric field. However, strong ion migration triggered by electrochemical reactions at the interface between a high-potential electrode and an organic-inorganic hybrid perovskite limits the stability of radiation detectors under a high electric field. Herein, we demonstrate that such ion migration could be effectively suppressed in devices with a Ti cathode, even at a high electric field of 50 V mm-1, through time-of-flight secondary-ion mass spectrometry. X-ray photoelectron spectroscopy illustrates that Ti-N bonds formed at the interface of MAPbBr3 perovskite single crystals/Ti electrode effectively inhibit the electrochemical reaction in organic-inorganic hybrid perovskite devices and ultimately improve the operating stability under a high electric field. The device with a Ti electrode reaches a high sensitivity of 96 ± 1 mC Gyair-1 cm-2 and a low detection limit of 2.8 ± 0.3 nGy s-1 under hard X-ray energy.

Nanodevice simulations and electronic transport properties of a two-dimensional PbBr2 monolayer

Two-dimensional (2D) wide bandgap semiconductors are promising blocks for applications in photodetections, spintronics and high energy radiation detection. Here, we probe the mechanical, biaxial strain-relate, electronic transport, and optoelectronic properties of PbBr2 monolayer with wide bandgaps using first-principles calculations. The 2D Young's modulus of PbBr2 monolayer is determined to be 14.68 N m−1 and the shear modulus is calculated to be 5.83 N m−1 at 300 K, revealing that PbBr2 monolayer is mechanically more flexible than other 2D materials, such as hexagonal-BN and MoB2. Interestingly, a specific forbidden bandwidth can be obtained by implementing a suitable strain on PbBr2 monolayer, and such effect leads to indirect bandgap semiconductor properties. Furthermore, various PbBr2 monolayer nanodevices, including p-n junction diodes, p-i-n junction field-effect transistors (FETs), and phototransistors, are designed and explored to investigate their transport properties. A variety of excellent transport properties, including prominent unidirectional transport, remarkable electrical anisotropy, obvious field-effect property, strong photoelectric response, and prominent absorption characteristics in the ultraviolet region, have been observed in these nanodevices. Our results unveil the multifunctional nature and superior performance of PbBr2 monolayer and suggest a practical configuration for the experimental realization in next-generation semiconductor nanodevices.

Dimensionality Engineering of Organic-Inorganic Halide Perovskites for Next-Generation X-Ray Detector.

The next-generation X-ray detectors require novel semiconductors with low material/fabrication cost, excellent X-ray response characteristics, and robust operational stability. The family of organic-inorganic hybrid perovskites (OIHPs) materials comprises a range of crystal configuration (i.e., films, wafers, and single crystals) with tunable chemical composition, structures, and electronic properties, which can perfectly meet the multiple-stringent requirements of high-energy radiation detection, making them emerging as the cutting-edge candidate for next-generation X-ray detectors. From the perspective of molecular dimensionality, the physicochemical and optoelectronic characteristics of OIHPs exhibit dimensionality-dependent behavior, and thus the structural dimensionality is recognized as the key factor that determines the device performance of OIHPs-based X-ray detectors. Nevertheless, the correlation between dimensionality of OIHPs and performance of their X-ray detectors is still short of theoretical guidance, which become a bottleneck that impedes the development of efficient X-ray detectors. In the review, the advanced studies on the dimensionality engineering of OIHPs are critically assessed in X-ray detection application, discussing the current understanding on the "dimensionality-property" relationship of OIHPs and the state-of-the-art progresses on the dimensionality-engineered OIHPs-based X-ray detector, and highlight the open challenges and future outlook of this field.

Aqueous-Based Inorganic Colloidal Halide Perovskites Customizing Liquid Scintillators.

Compared to solid scintillators and organic liquid scintillators, aqueous-based liquid scintillators (AbLS) have more superiority in highly flexible scalability, yet are now limited by their low light yield (≈100 photons MeV-1 ). Here, aqueous-based inorganic colloidal halide perovskites with high photoluminescence quantum yield (PLQY) of three primary color luminescence up to 88.1% (red), 96% (green), and 81.8% (blue) are respectively synthesized, and a new generation of colloidal perovskite-mediated AbLS (PAbLS) with light yield increased in comparison with the commercial scintillator AbLS is fabricated. This paper exhibits that the excellent PLQY and colloidal dispersion of halide perovskites benefit from poly(ethylene glycol) modification and this modification ensures the vacancy inhibition and formation of defect-free surfaces in an aqueous solution. Moreover, their high luminescent emission can be maintained for 100 days at low temperatures, and such modification also promises the heat-to-cold customization of operating temperature even in ice below 0 °C. Finally, depending on the light yield of around 3058 and 8037 photons MeV-1 at room temperature and low temperature, PAbLS with shape/size scalability exhibit their robust radiation hardness (dose rate as high as 23 mGy s-1 ) and conceptual application potential in high-energy ray radiation detection from every angle of 360°.

Lead halide perovskites for radiation detectors: Perspectives

Halide perovskite, Bridgman grown single crystals have shown excellent performance for high energy radiation detectors. CsPbBr3 perovskite detectors with 1.4% energy resolution have been demonstrated. These detectors demonstrate a wide range of operations from −2 to 70 °C. Semiconductor hard radiation detectors have been used for applications in defense, medicine, and bioelectronics. In most of these applications, there is a need for the detectors to operate at room temperature and above. Previous hard radiation detector devices have used the material cadmium zinc telluride for room temperature operation [Luke et al., IEEE Trans. Nucl. Sci. 48, 282 (2001)]. There are now other semiconductors that show considerable promise. These include the halide perovskite compound semiconductors with a formula CsPbX3, where X = Cl, Br, I [Liu et al., Proc. SPIE 8852, 88520A (2013); Peters et al., J. Lumin. 243, 118661 (2022)]. These materials are also being developed for other device applications, including light-emitting diodes, lasers, solar cells, and photodetectors. It is claimed that these semiconductors are defect-tolerant, although the reason for this behavior is not well understood. Thermally stimulated current spectroscopy was used to detect electron traps in these materials to improve their performance. The halide compound cesium lead bromide has a bandgap of 2.25 eV, which makes it suitable for room temperature operation and above. They also have high permittivity. These halide perovskite semiconductors have shown room temperature detector device performance. Recently, we demonstrated hard radiation detectors using CsPbBr3 as the device platform. The detectors had 1.4% energy resolution for high-energy γ rays [He et al., Nat. Photonics 15, 36 (2021)]. The detectors demonstrate a wide temperature region from −2 to 70 °C for stable operations.

Thermal and chemical durability of metal halide perovskite CsPbBr3 single crystals

Halide perovskite CsPbBr3 single crystals have shown promising applications in high-energy radiation detection because of their high gamma-ray blocking capability, strong hole carrier transport capability, and manufacturing feasibility. However, the soft ionic properties of perovskite octahedral lattice facilitate the phase transformation of CsPbBr3 under a hydrothermal environment, which significantly limits their application. The current work systematically studied the phase stability of the CsPbBr3 single crystals under high temperatures and high humidity to accelerate their potential application in high-energy radiation detection. Thermal and water degradation behaviors of the CsPbBr3 single crystals under elevated temperature were investigated for the first time via in situ Raman spectroscopy and semi-dynamic leaching testing methods. Results indicated that the CsPbBr3 single crystals exhibited good thermal stability below 460 °C without obvious phase degradation and rapidly transformed to CsPb2Br5, followed by PbBr(OH) with the continuous water interaction. The water interaction and phase degradation mechanism of single crystals with the preferential release of Cs, surface reorganization, and formation of PbBr(OH) alteration layer with rod-like structure was revealed. The phase degradation of CsPbBr3 single crystals along surface defects from the growth process was further confirmed, which can be used to guide subsequent work on single-crystal stability regulation.

IoT-Enabled System for Detection, Monitoring, and Tracking of Nuclear Materials

A low-cost embedded system for high-energy radiation detection applications was developed for national security proposes, mainly to detect nuclear material and send the detection event to the cloud in real time with tracking capabilities. The proof of concept was built with state-of-the-art electronics such as an adequate Si-based photodetector, a trans-impedance amplifier, an ARM Cortex M4 microcontroller with sufficient ADC capture capabilities, an ESP8266 Internet of Things (IoT) module, an optimized Message Queuing Telemetry Transport (MQTT) protocol, a MySQL data base, and a Python handler program. The system is able to detect alfa particles and send the nuclear detection events to the CloudMQTT servers. Moreover, the detection message records the date and time of the ionization event for the tracking application, and due to a particular MQTT-optimized protocol the message is sent with low latency. Furthermore, the designed system was validated with a standard radiation instrumentation preamplifier 109A system from ORTEC company, and more than one node was demonstrated with an internet connection employing a 20,000 bits/s CloudMQTT plan. Therefore, the design can be escalated to produce a robust big data multisensor network.

Perovskite-Based X-ray Detectors.

X-ray detection has widespread applications in medical diagnosis, non-destructive industrial radiography and safety inspection, and especially, medical diagnosis realized by medical X-ray detectors is presenting an increasing demand. Perovskite materials are excellent candidates for high-energy radiation detection based on their promising material properties such as excellent carrier transport capability and high effective atomic number. In this review paper, we introduce X-ray detectors using all kinds of halide perovskite materials along with various crystal structures and discuss their device performance in detail. Single-crystal perovskite was first fabricated as an active material for X-ray detectors, having excellent performance under X-ray illumination due to its superior photoelectric properties of X-ray attenuation with μm thickness. The X-ray detector based on inorganic perovskite shows good environmental stability and high X-ray sensitivity. Owing to anisotropic carrier transport capability, two-dimensional layered perovskites with a preferred orientation parallel to the substrate can effectively suppress the dark current of the device despite poor light response to X-rays, resulting in lower sensitivity for the device. Double perovskite applied for X-ray detectors shows better attenuation of X-rays due to the introduction of high-atomic-numbered elements. Additionally, its stable crystal structure can effectively lower the dark current of X-ray detectors. Environmentally friendly lead-free perovskite exhibits potential application in X-ray detectors by virtue of its high attenuation of X-rays. In the last section, we specifically introduce the up-scaling process technology for fabricating large-area and thick perovskite films for X-ray detectors, which is critical for the commercialization and mass production of perovskite-based X-ray detectors.

Radioluminescent Cu-Au Metal Nanoclusters: Synthesis and Self-Assembly for Efficient X-ray Scintillation and Imaging.

Zero-dimensional (0D) scintillation materials have drawn tremendous attention due to their inherent advantages in the fabrication of flexible high-energy radiation scintillation screens by solution processes. Although considerable progress has been made in the development of 0D scintillators, such as the current leading lead-halide perovskite nanocrystals and quantum dots, challenges still persist, including potential issues with self-absorption, air stability, and eco-friendliness. Here, we present a strategy to overcome those limitations by synthesis and self-assembly of a new class of scintillators based on metal nanoclusters. We demonstrate the gram-scale synthesis of an atomically precise nanocluster with a Cu-Au alloy core exhibiting high phosphorescence quantum yield, aggregation-induced emission enhancement (AIEE) behavior, and intense radioluminescence. By controlling solvent interactions, the AIEE-active nanoclusters were self-assembled into submicron spherical superparticles in solution, which we exploited as a novel building block for flexible particle-deposited scintillation films with high-resolution X-ray imaging performance. This work reveals metal nanoclusters and their self-assembled superstructures as a promising class of scintillators for practical applications in high-energy radiation detection and imaging.

Elaboration and TL&OSL response study of 1% Sb-doped Al2O3 dosimeter for high-energy radiation detection and dosimetry

Elaboration and TL&OSL response study of 1% Sb-doped Al2O3 dosimeter for high-energy radiation detection and dosimetry

The Highly Accurate Interatomic Potential of CsPbBr3 Perovskite with Temperature Dependence on the Structure and Thermal Properties

CsPbBr3 perovskite has excellent optoelectronic properties and many important application prospects in solar cells, photodetectors, high-energy radiation detectors and other fields. For this kind of perovskite structure, to theoretically predict its macroscopic properties through molecular dynamic (MD) simulations, a highly accurate interatomic potential is first necessary. In this article, a new classical interatomic potential for CsPbBr3 was developed within the framework of the bond-valence (BV) theory. The optimized parameters of the BV model were calculated through first-principle and intelligent optimization algorithms. Calculated lattice parameters and elastic constants for the isobaric-isothermal ensemble (NPT) by our model are in accordance with the experimental data within a reasonable error and have a higher accuracy than the traditional Born-Mayer (BM) model. In our potential model, the temperature dependence of CsPbBr3 structural properties, such as radial distribution functions and interatomic bond lengths, was calculated. Moreover, the temperature-driven phase transition was found, and the phase transition temperature was close to the experimental value. The thermal conductivities of different crystal phases were further calculated, which agreed with the experimental data. All these comparative studies proved that the proposed atomic bond potential is highly accurate, and thus, by using this interatomic potential, the structural stability and mechanical and thermal properties of pure inorganic halide and mixed halide perovskites can be effectively predicted.

Recent Development of Halide Perovskite Materials and Devices for Ionizing Radiation Detection.

Ionizing radiation such as X-rays and γ-rays has been extensively studied and used in various fields such as medical imaging, radiographic nondestructive testing, nuclear defense, homeland security, and scientific research. Therefore, the detection of such high-energy radiation with high-sensitivity and low-cost-based materials and devices is highly important and desirable. Halide perovskites have emerged as promising candidates for radiation detection due to the large light absorption coefficient, large resistivity, low leakage current, high mobility, and simplicity in synthesis and processing as compared with commercial silicon (Si) and amorphous selenium (a-Se). In this review, we provide an extensive overview of current progress in terms of materials development and corresponding device architectures for radiation detection. We discuss the properties of a plethora of reported compounds involving organic-inorganic hybrid, all-inorganic, all-organic perovskite and antiperovskite structures, as well as the continuous breakthroughs in device architectures, performance, and environmental stability. We focus on the critical advancements of the field in the past few years and we provide valuable insight for the development of next-generation materials and devices for radiation detection and imaging applications.

Cerium and europium doping of Ruddlesden-Popper aluminate phases and their radioluminescence properties

Although many scintillator detectors with the fast and efficient detection of high-energy radiation are commercially produced, new materials are still of great interest. Oxide matrices doped with ions possessing fast and intense 5d–4f radiative transition are one of the researched groups of materials. So called Ruddlesden–Popper phases are structures combining halite-like and perovskite-like structures. The aluminates subgroup (AII n+1-yAIII y) n+1 Al n O3n+1 has been only rarely studied for scintillation use. These phases are stable oxides with a relatively high density and, moreover, they melt congruently, which enables growth from a melt. In this study, we tested Ce3+- and Eu2+-doped (Sr,Ca)1(Gd,Y) n Al n O3n+1 (n = 1; 2) analogues. The samples were prepared by the chelating sol-gel method combined with the annealing in reducing atmosphere to reduce both ions to the intended valence. After the samples were characterized by X-ray diffraction, radioluminescence was used for the basic study of luminescence behaviour of Ce3+ and Eu2+ ions. While Ce3+-doped samples exhibited the 5d-4f radiative transition, Eu-doped samples manifested only luminescence spectra characteristic for Eu3+ ions.

(Student Award, 2nd Place) Optical and Mechanical Properties of Europium-Doped Sicn Thin Films Prepared By Integrated Ecr-PECVD and Magnetron Sputtering

Silicon carbonitride (SiCN) is a wide bandgap semiconductor material that has drawn significant interest over the past few decades due to its excellent optical, electrical, and mechanical properties[1]. Rare earth doping in wide bandgap semiconductors has several prospective applications in the field of photoelectric devices, solid-state lasers, flat panel displays, and high-energy radiation detectors [2]. Among the various rare earth materials, europium (Eu) is particularly interesting due to its optically active divalent and trivalent states capable of emitting in different visible spectral ranges [3].In this work, Eu-doped SiCN thin films were prepared by electron cyclotron resonance plasma-enhanced chemical vapor deposition (ECR-PECVD) with integrated magnetron sputtering [4] on p-type 3” Si (100) substrates. Silane (diluted in 90% argon), nitrogen (diluted in 90% argon) and ethane (C2H6) were used as precursor gases, and a 99.9% pure Eu sputtering target was used as a sputtering source. To understand the effect of C incorporation in the Eu-doped SiCN matrix, we have prepared a set of samples without C. The as-deposited samples were annealed over a wide range of temperatures from 600 to 1100° C in an internet N2 environment. Rutherford backscattering spectrometry (RBS) was performed to determine the atomic concentration of the constituents. Variable angle spectroscopic ellipsometry (VASE) analysis was performed to investigate the optical properties of the films. The room temperature photoluminescence (PL) experiments were carried out with a laser diode excitation source, operating at a wavelength of 375nm. Finally, we performed nanoindentation measurements to understand the deformation behavior of SiCN films as a function of the incorporation of C. The indentation hardness and Young’s modulus of the films were investigated for different Eu and C concentrations.

Effect of Solution and Dry Processing Techniques on the Optical and Transport Properties of Inorganic CsPbBr3 Perovskite Films

Cesium-based inorganic CsPbBr3 perovskite material possesses remarkable optoelectronic properties, such as high light absorption coefficient, high carrier mobility, and long diffusion length, and hence has promising applications in solar cells, photo-detectors, and high-energy radiation detectors, among others. Because of its simplicity, low cost, and high efficiency, spin-coating deposition for the CsPbBr3 perovskite layer for such diverse applications has been widely used. However, the spin-coating technique has technological constraints when it comes to uniformly deposit large-area films. Thermal evaporation, on the other hand, is inexpensive and produces a uniform and repeatable thin film. In this study, the stability, energy band alignment, surface morphologies, and light absorption of a CsPbBr3 perovskite layer produced by spin coating and thermal evaporation are investigated and discussed.

Photoluminescence and X-ray induced scintillation in Gd3+-modified fluorophosphate glasses doped with Ce3+

In this work, we report the fabrication of Gd3+-modified fluorophosphate glasses doped with Ce3+ with the new compositions 50NaPO3–20BaF2-(10-x)CaF2-20GdF3-xCeCl3, x = 0.3; 1; 3 and 5 mol% and their promising features as scintillators. The glasses present high molar density values (ρ ≅ 4 g cm−3), comparable to that of crystal scintillators, and distinguished optical properties. By UV–visible absorption, photoluminescence emission and excitation, excited state decay curves and radioluminescence measurements, the photophysical properties of the glasses were fully characterized. In addition, x-ray photoelectron spectroscopy (XPS) was employed to confirm the valence state of Ce ions. The results of emission spectra measured in the visible range upon UV excitation together with the excited state lifetime values of Ce3+ (5d → 4f transition) and Gd3+ (8S7/2→6Ij transition) clearly evidence energy transfer (ET) from the latter to the former ion. Though not quantified, the ET favors the fast decaying (τ = 24 ns) efficient emission of Ce3+ which makes the materials promising for fast response high energy radiation detectors. The response to X-ray excitation associated with the relatively high molar density of the glasses, indicate the promising application of these glasses for medical diagnosis where, in particular, a fast and intense response under high-energy radiation excitation is crucial.