Metal halide perovskite CsPbBr3 crystals have emerged as promising candidates for ionizing radiation detection. However, larger sized single crystals possessing greater commercial viability usually exhibit interwafer inhomogeneity and instability in both electrical and radiation detection properties, which is attributed to the material inhomogeneity in CsPbBr3 crystals, especially because of structural imperfections. This study reports the spatial distribution patterns of twin defects in a 60 mm diameter CsPbBr3 ingot grown by the vertical Bridgman method, where the twin-plane normals point toward the central axis of the ingot. Further, the twin evolution is evaluated through controlled movement under a gradient temperature field, with the rapid thermal treatment (10 mm/h) replicating the unidirectional twin characteristic of the as-grown state. Ultimately, directional annealing with a speed of 2 mm/h is adopted to eliminate the twins in CsPbBr3, in which the internal stress accumulated from octahedral twisting during the phase transition has sufficient time to relax and dissipate, thereby suppressing twin formation. The resulting mobility increased approximately 140% (from 10.25 to 24.89 cm2 V-1 s-1), and the resistivity is comparable to that of as-grown CsPbBr3 crystals free from twins. This research provides a novel approach to defect engineering in perovskite single crystals.
Metal halide perovskite scintillators have emerged as promising candidates for X-ray imaging owing to their excellent scintillation performance and solution processability. However, simultaneously achieving high spatial and temporal resolution in scintillator films remains challenging. Increasing scintillator loading improves light yield but also induces particle aggregation and optical photon scattering, ultimately degrading spatial resolution. Here, the (C4H9NH3)2PbBr4@Poly(methyl methacrylate) (BA2PbBr4@PMMA) composite films with suppressed particle aggregation at high scintillator particle loading were achieved by in-situ regulating polymer confinement in the film preparation process, simultaneously enabling X-ray imaging with high spatial resolution and fast decay time. By establishing an adequate solvation environment, uniformly dispersed PMMA chains introduce homogeneous polymer confinement during crystallization, suppressing both solute aggregation and disorderly grain growth. The resulting uniformly dispersed fine-particle microstructure effectively suppresses optical photon scattering, thereby enhancing radioluminescence intensity, optical transmittance and the spatial resolution of the BA2PbBr4@PMMA scintillation film (from 6.0 to 17.5 lp mm-1). Furthermore, the composite films exhibit a fast decay time with an average value of 3.32ns, effectively eliminating ghosting effects in dynamic imaging. This work provides a general strategy for designing scintillator films with high light output and fast decay, and offers insights into microstructure engineering for optoelectronic devices.
The zero-dimensional (0D) copper halide perovskite Cs3Cu2I5 exhibits outstanding luminescence and scintillation properties, making it a highly promising scintillator for γ-ray detection. Solution growth is a favorable and inexpensive method for growing Cs3Cu2I5 single crystals; however, scalable growth of Cs3Cu2I5 crystals with low defect density suffers from the unavoidable formation of secondary phase CsCu2I3. In this work, centimeter-size, high quality Cs3Cu2I5 single crystals are synthesized via a constant-temperature solvent evaporation crystallization (CT-SEC) method, in which the formation of CsCu2I3 can be eliminated by precursor engineering. The phase evolution behavior is elucidated as the decrease in the I-/Cu+ concentration ratio during the growth of the Cs3Cu2I5 crystal. Through synergistic regulation of precursor antioxidative treatment and raw material stoichiometry, the long-term phase-stable growth of Cs3Cu2I5 single crystals is achieved. The obtained Cs3Cu2I5 crystals exhibit excellent energy resolutions of 5.38% for 137Cs and 13.30% for 241Am γ-ray irradiation.
Solution-processed polycrystalline perovskites are inevitably endowed with inherent discontinuity at device heterointerfaces, which creates numerous interface segments that demand deliberate engineering of metastable interfacial configurations. Nevertheless, critical challenge remains in synchronously manipulating interfacial microscale carrier management while maintaining their microstructural integrity under operational stresses. Herein we demonstrate a strategy to fabricate localized microscopic p-n heterointerfaces with high coherence and ionic bridging through encapsulating well-defined p-type CdTe quantum dots (QDs) on n-type perovskite grains. Surface embeddings of such QDs establish unidirectionally aligned built-in electric fields that facilitate directional carrier transport across micro-heterointerfaces while expanding depletion regions to minimize recombination loss. Moreover, CdTe-induced heteroepitaxial growth yields dislocation-less interfaces between CdTe and perovskite, simultaneously passivating accessible defects of iodine vacancies and undercoordinated Pb2+ at both the surface and grain boundaries, enabling high-crystallinity perovskite films with robust microstructures. Given these striking merits, a record-high efficiency of 26.73% (certified 26.02%) with a remarkable open-circuit voltage of 1.222 V is achieved, setting a new performance benchmark among regular perovskite solar cells, along with pronounced operational stability with negligible efficiency degradation after nearly 700 h. This work pioneers a transformative laser-mediated microscopic heterointerface engineering strategy that fundamentally reengineers microstructural carrier management and long-term durability in advanced optoelectronics.
Cadmium Zinc Telluride (CdZnTe) has become a key semiconductor material for room-temperature gamma-ray detectors. However, its performance and service life can be severely compromised by radiation damage in harsh radiation environments, particularly in space where protons constitute the predominant high-energy particles. In this work, we reveal an anomalous reduction in surface roughness of the CdZnTe crystals after proton irradiation, which is attributed to the predominance of smoothing mechanisms, such as the Herring-Mullins diffusion mechanism and radiation-induced viscous flow. Transmission electron microscopy (TEM) analysis elucidates the depth-dependent defect distribution in irradiated CdZnTe crystals. Frank loops and defect clusters dominate in the near-surface region, while stacking faults dominate in deeper regions, primarily due to the surface sink effect. Current-mode deep level transient spectroscopy (I-DLTS) analysis reveals a significant increase in defect concentration and the emergence of deep traps at higher fluences, leading to a sharp rise in the ratio of carrier detrapping time to capture time. These microstructural changes directly lead to the degradation of electrical and detection performances. Electron mobility decreases from 1087 cm2V-1s-1 before irradiation to 412 cm2V-1s-1 after irradiation. CdZnTe detector completely fails at the fluence of 5 & times; 1011 p/cm2. We systematically investigated the underlying mechanism of irradiation defect-induced performance degradation in CdZnTe crystals after proton irradiation, providing innovative design strategies and theoretical tools for accurately evaluating and enhancing the radiation tolerance and service reliability of CdZnTe detectors in space environments.
Zinc telluride (ZnTe) is a benchmark electro-optic crystal for terahertz time-domain spectroscopy and an infrared window material. However, the high refractive index of ZnTe causes approximately 20% efficiency loss due to Fresnel reflection, while conventional antireflection coatings suffer from poor adhesion. In this study, a versatile strategy combining the Langmuir-Blodgett method with reactive ion etching is proposed to fabricate centimeter-scale nanostructure arrays on a ZnTe crystal surface, enabling simultaneous performance enhancement in the near-infrared (NIR) and THz bands. Well-defined and 100% covered nanostructures with characteristic dimensions ranging from 100 to 450 nm were obtained by precisely modulating the mask dimensions and etching parameters. The effective refractive-index gradient formed by nanostructures with diameters of 300-450 nm suppresses Fresnel reflection across 800-2500 nm, yielding a transmittance enhancement of 18.5%. Furthermore, finite-difference time-domain simulations were employed, revealing the strong resonance modes surrounding 164 nm diameter units, which enhance the local power density of 800 nm probe light up to 5.6-fold. Consequently, the THz detection sensitivity was enhanced by 47.1% over a broadband range of 0.1-2.5 THz, highly consistent with the simulation results of 45%. This work develops a scalable method for fabricating large-area, controllable nanostructures on ZnTe to achieve dual-band enhancement, which alleviates the intrinsic efficiency limitations of systems based on high refractive-index crystals.
CsPbBr3 is regarded as a promising alternative to state-of-the-art CdZnTe for room-temperature semiconductor detectors. However, currently, a high-resolution gamma-ray detector is only achieved with CsPbBr3 crystals and shows limited dimensions and efficiency due to the formation of undesirable secondary-phase precipitations. In this study, high-resistivity detector-grade CsPbBr3 crystals are grown using the vertical Bridgman method by tailoring the stoichiometric ratio of the raw materials. To avoid the formation of undesired secondary phases, a stoichiometric ratio with a 1.5% excess of CsBr is adopted, which minimizes the enrichment of PbBr2 at the solid-liquid interface during growth. As a result, the CsPbBr3 crystals exhibit a superior resistivity of 1.8 & times; 109 Omega cm and a hole mobility-lifetime product of 1.71 & times; 10-3 cm2 V-1. Finally, CsPbBr3 ingots with diameters of 60 mm and lengths exceeding 90 mm are obtained. The resulting CsPbBr3 planar detectors, with dimensions of 14 & times; 14 & times; 4 mm3, resolve the peaks of 137Cs@662 keV and 241Am@59.5 keV gamma-rays with energy resolutions of 9.16% and 12.69%, respectively. The proposedstrategy of tailoring the stoichiometric ratio in our work will pave the way for large detector-grade CsPbBr3 crystals in gamma-ray detection.
CsPbBr3 is a reliable and cost-effective semiconductor material with significant potential for radiation detection applications. However, a crucial challenge is maintaining both high performance and radiation stability, particularly under extreme irradiation conditions. Here, the intrinsic origin of the exceptional radiation hardness of CsPbBr3 single-crystal detectors is revealed by integrating performance changes with the evolution of point defects. It is shown that the detectors maintain exceptional radiation hardness under 60Co gamma-radiation (1.17 and 1.33 MeV) doses as high as 5 Mrad, with the crystal structure remaining stable, and no degradation, decomposition or phase segregation is observed. The combination of pulse height spectra response and deep level transient spectroscopy demonstrates that CsPbBr3 detectors exhibit a self-healing capability through efficient defect migration at room temperature. Low-dose irradiation (<= 500 krad) passivates intrinsic defects and reduces trap density, while high-dose irradiation (>= 1 Mrad) generates new defects and degrades energy resolution. The self-healing behavior is attributed to the defect repair mechanism of radiation-induced damage in CsPbBr3 through efficient defect migration. These findings position CsPbBr3 as a leading candidate for radiation-hardened applications and provide critical insights into self-healing semiconductor materials for extreme environments.
Organic semiconducting (OSC) X-ray detectors offer exciting opportunities for developing biocompatible, tissue-equivalent, flexible, and low-cost X-ray detection technologies. However, detection sensitivity is limited by the low X-ray attenuation efficiency of the organic active layer. Here, we present a novel strategy to enhance X-ray absorption by incorporating high atomic number ZnO nanoparticles (NPs) into 4-hydroxycyanobenzene (4HCB), an OSC material. A space-confined melt process was employed to fabricate well-oriented 4HCB/ZnO composite films. Strong pi-pi interactions between benzene rings in 4HCB promote layered growth, enabling uniform dispersion of ZnO NPs throughout the 4HCB film. Under 17.9 keV X-ray irradiation, the 4HCB/ZnO device exhibited a sensitivity of 477 mu C Gy(air)(-1) cm(-2), approximately 20 times higher than that of pure 4HCB film. This enhancement is primarily attributed to impact ionization induced by nanoparticles. Simulations confirmed that Mie scattering effect, resulting from the effective nanoparticle size, extends X-ray's radiation path length, leading to improved charge generation efficiency in the composite detectors. The composite film also exhibits high resistivity, fast mobility, a large on/off ratio, and a low detection limit, making the combination of inorganic NPs and OSC materials a promising strategy for achieving high-performance, low-cost X-ray detectors and imaging systems. (c) 2025 Published by Elsevier Ltd on behalf of The editorial office of Journal of Materials Science & Technology.
Organic semiconductor single crystals are considered promising materials for X-ray detection due to their tissue equivalence and low fabrication cost. However, due to the inherently weak intermolecular interactions of organic semiconductor single crystals, they generally exhibit relatively low carrier mobility, which limits the further improvement of their X-ray detection performance. Here, we obtain centimeter-sized anthracene-based 9,10diphenylanthracene (9,10-DPA) organic semiconductor single crystals via a side-chain engineering strategy to enhance the carrier mobility of anthracene. Compared with anthracene crystals, the it-it interaction between the phenyl side groups and the anthracene backbone of 9,10-DPA crystals achieves an electron mobility of 6.83 cm2 V- 1 s-1 and an alpha particle energy resolution of 33.06%. The enhanced carrier transport and collection properties endow the 9,10-DPA detectors with improved detection capabilities. Meanwhile, under low X-ray dose rates, hole trapping by defects induces the injection of additional free electrons, thus realizing photocurrent amplification with a maximum gain of 2000%. Therefore, the 9,10-DPA detector exhibits outstanding comprehensive Xray detection performance, with sensitivity as high as 1246 & micro;C Gyair - 1 cm- 2 and detection limit as low as 8.74 nGyair s- 1. Consequently, the detectors can realize high-resolution X-ray imaging with a spatial resolution of 4.8 lp mm-1 at a relatively lower dose rate (0.67 & micro;Gyair s-1). This work provides crucial support for the development of organic detectors in low-dose medical X-ray imaging.
Organic semiconductor single crystals (OSSCs) hold great promise for direct X-ray detection owing to their low cost and tissue equivalence. However, their performance is often limited by inefficient charge transport. Herein, we develop a cooling-rate-modulated polymorphic growth strategy to simultaneously regulate intermolecular torsion angles and molecular packing, yielding two large-sized polymorphs of 9,10-bis(4-methoxyphenyl)anthracene (BMOPA-α and BMOPA-β). Comparative studies on polymorphs reveal that the deviation angle between the charge transport pathway and the intermolecular interaction axis leads to significant differences in carrier mobility. The BMOPA-β crystal shows a much smaller deviation angle, enabling more efficient carrier transport, with the hole mobility reaching 8.59 cm2 V-1 s-1. As a result, the BMOPA-β single-crystal detector achieves a high sensitivity of 584.4 μC Gyair-1 cm-2, and an ultralow detection limit of 37.8 nGyair s-1, enabling high spatial-resolution (3.47 lp mm-1) X-ray imaging. This work highlights molecular packing structure control via polymorph engineering as an effective strategy for improving carrier transport characteristics in organic X-ray detectors.
Plasmon-induced photoacoustic streaming, considered as a potential application for micro-pumps in microfluidics, currently encounters ongoing debates concerning its fundamental mechanisms. In this study, we investigate the crucial role played by microbubbles in generation of jets in an ethanol aqueous solution. The power density threshold for bubble generation and its dependency on jet initiation are confirmed and the microbubble behavior is well regulated by manipulating the laser and liquid properties. Through simulations coupling fluidic and thermal fields, the significant role of Marangoni effect is validated in jet formation. Specifically, the temperature gradient of microbubbles is determined to be a pivotal factor in the generation of collimated jets. Additionally, factors influencing jetting, such as microbubble size and temperature gradients are studied, and noticeably, a stabilized jet lasting over 4 h is achieved based upon.
Heterointerfaces formed by the intimate connection of different materials with electromagnetic losses are expected to achieve stronger electromagnetic (EM) absorption. However, constructing composites with heterointerfaces still faces great challenges in facile preparation process, optimized impedance matching, high reflection loss (RL), and ultrathin matching thickness. In this work, we develop ZIF-8 functionalized MXene to produce hierarchical Ti3C2@C@ZnO composites with heterointerface to advance EM absorption enhancement. Modified with polydopamine (PDA), few-layer Ti3C2Tx MXene sheets enable adsorption of Zn2+ metal ions on Ti3C2Tx@PDA by electrostatic interaction for in-situ growth of ZIF-8. Ti3C2/C/ZnO heterointerface were obtained after heat treatment of Ti3C2Tx@PDA@ZIF-8 nanocomposites at various temperatures. The Ti3C2/C/ZnO-600 °C with 1.15 mm thickness have a RL of −50.241 dB and an effective absorption bandwidth of 3.50 GHz. In-depth studies on the electromagnetic loss mechanisms reveal that Ti3C2, carbon, and ZnO in nanocomposites generate multiple interfacial polarization losses beyond partial conductivity losses caused by Ti3C2 and ZnO. Oxygen vacancy defects in ZnO form dipole losses with carbon. This work not only provides a simple and effective concept for preparing MXene@MOFs heterogeneous composites as an ultrathin and strong electromagnetic wave absorber, but also offers a vital guideline to fabricate various metal oxides derived from the MXene and metal-organic frameworks (MOFs) precursors.
Plasmonic superlattices enable the precise manipulation of electromagnetic fields at the nanoscale. However, the optical properties of static lattices are dictated by their geometry and cannot be reconfigured. Here, we present a surface-interface engineered plasmonic superlattice with confined polyelectrolyte-functionalized metal-organic framework (MOF) hybrid layers to tune plasmon resonance for ultrafast chemical sensing. The surface lattice resonance frequency in the visible spectrum was achieved using electron-beam lithography with a humidity-responsive polyelectrolyte brush grafted onto the thiol-initiator-modified gold nanoparticle surface through atom transfer radical polymerization. An MOF thin film was assembled on the polyelectrolyte-functionalized gold nanoparticle lattice via a layer-by-layer immersion. Surface lattice resonance was observed without additional matched dielectric environment around the NPs, and the resonance frequency was tuned by adjusting the thickness and refractive index of the polyelectrolyte layer. Furthermore, high chemical sensitivity and ultrafast response were achieved due to the coherence between the MOFs and polymer layers.
Terahertz (THz)-based sensing technology shows promise for the rapid and efficient detection of unlabeled biomolecules and pathogens, attributed to their significant absorption in the THz range. However, its application has been limited by low sensitivity and specificity. Addressing this, we creatively constructed an advanced detection technique named immuno-THz technology, integrating monoclonal antibody (mAb)-based specific molecular recognition with THz sensing. Detection of a variety of pathogenic microorganisms was highly sensitive and specific in our proof-of-concept assay, achieving a limit of detection of 74.57 colony-forming units/ml for Escherichia coli O157:H7, 0.05495 μg/ml for HAdV-B55 Hexon protein, and 0.00479 μg/ml for Staphylococcal enterotoxin B in phosphate-buffered saline solution. The immuno-THz technique substantially enhances detection sensitivity, marking a 100-fold improvement over traditional THz spectroscopy methods, particularly in detecting E. coli O157:H7. The advanced sensitivity and specificity of the immuno-THz technique will offer an improved approach for the detection of pathogenic microorganisms, be applied in a wide range of applications, and impact on food safety and public health and national defense security.
The CsPbBr3 crystal grown by the solution method is regarded as an attractive and cost-effective material for radiation detection. However, approaching large-size, high-quality CsPbBr3 single crystals is restricted by mass nucleation and an unstable growth interface. Here, the confined geometry assisted solution method is employed to obtain high-quality CsPbBr3 single crystals with dimensions up to 17 x 17 x 2 mm(3). High yield growth of CsPbBr3 seed crystals is achieved by adopting 2-bromopropionic acid (2-BPA) in the precursor, which expands the metastable zone twice and reduces nucleation. The crystal growth environment, simulated with a specific laminar flow model, reveals the uniform concentration distribution is realized by suitable forced convection velocity, thereby substantially enhancing the stability of the crystal growth interface. The resulting CsPbBr3 single crystal exhibits low trap density states of 2.27 x 109 cm(-3), leading to a high hole mobility of 377.63 cm2 V-1 s(-1). Finally, a high sensitivity of 1.6 x 105 mu C Gyair( -1) cm(-2) is realized under 50 kVp X-rays at 500 V cm(-1). These results promote the application of large-sized CsPbBr3 single crystals in X-ray radiation detection as well as the reference and guidance for the growth of other perovskite single crystals.
The strong-field terahertz (THz) driven by ultrafast high-intensity laser has been attracting increasingly attention in THz probe and imaging. As the leading potential nonlinear optical material for strong-field terahertz (THz) generation and detection, the ZnTe tends to be damaged by focused laser irradiation. In this work, the laser ablation and morphology modification of ZnTe single crystal under a 800 nm, 100 fs Ti:Sapphire laser are investigated. The inconstant laser induced damage threshold (LIDT) of the ZnTe is precisely measured, in which a reference safety energy 38 mJ/cm2 is obtained. According to the Keldysh theory, the photoionization rate in irradiated area is calculated as high as 1034 cm-3s-1, which introduces an intense plasma and in turn dominates the weak LIDT of ZnTe. In addition, the fs-laser shots induce the oxidation on the damaged surface preventing the further ablation of the crystal. A surface eruption model is proposed to elaborate the fs-laser induced damage evolution and the formation of cracks and eruption holes on ZnTe. Finally, the XPS deep etching demonstrates relative shallower ablation affected zone occurred on the surface since the interaction process happens in an ultrashort timescale. Thus, the THz response behaviors of ZnTe aged by fs-laser is able to be recovered by removing the damage layer simply. Our work provides insight into the laser damage behavior of the ZnTe single crystal and lays a foundation for further fs-laser micro-processing and laser-damage resistance improvement.
The success of CsPbBr3 in a host of optoelectrical fields is chiefly attributed to its remarkable carrier transport properties, which have been described as unique compared with other semiconductors. Therefore, the dynamics of carriers continue to captivate the interest of researchers. In this study, by utilizing the optical-pump terahertz-probe (OPTP) techniques under a 400 nm laser excitation with varying pump fluences, the existence of polaron was directly confirmed from the THz photoconductivity spectra. Meanwhile, a two-step exciton-polaron transform model was introduced to elucidate the dynamics of polaron formation in the CsPbBr3 single crystal, with an exciton dissociation time of 3 ps. Moreover, the exciton-polaron transform was found to be reversible, which exerted a significant impact on the bimolecular recombination process, thereby prolonging the carrier lifetime. Eventually, based on the Drude-Lorentz model in conjunction with Feynman's theory, the polaron mobility was calculated as 197 cm(2)V-1s(-1) for CsPbBr3. These findings not only clarify the role of excitons in polaron dynamics but also provide essential guidance for optimizing CsPbBr3-based optoelectrical devices.
Efficient discrimination between fast neutrons and gamma rays is crucial yet challenging for radiation detection. Here, the successful growth of large‐size, high‐quality 2D organic–inorganic hybrid perovskite single crystals, (GABA) 2 PbBr 4 , via an in situ seed‐assisted cooling method is reported. This material integrates hydrogen‐rich GABA cations with heavy‐atom lead halide layers, offering strong excitonic emission, efficient γ‐ray absorption, and fast neutron sensitivity. X‐ray diffraction reveals highly oriented crystals along the (004) plane with a narrow full width at half maximum (FWHM) of 12.81″. Optical characterizations indicate a wide bandgap (≈3.0 eV), sharp excitonic emission, and prominent self‐trapped exciton behavior, supported by transient and temperature‐dependent photoluminescence. The crystals exhibit an energy resolution of 9.0% at 662 keV and a high light yield of 10 695 ph MeV −1 . Notably, superior neutron/gamma pulse shape discrimination (PSD) is achieved with a maximum figure‐of‐merit (FOM) of 1.74, enabling clear signal separation. Additionally, flexible composite scintillation films based on (GABA) 2 PbBr 4 demonstrate high‐resolution X‐ray imaging up to 10 LP mm −1 . These results highlight the potential of (GABA) 2 PbBr 4 as a multifunctional scintillator for advanced radiation detection and imaging applications.
Monolayer MoS2 has garnered significant interest because of its exceptional optoelectronic and tribological properties and potential application as a lubrication layer in micro- and nanoelectromechanical systems. Although the nanotribological performance of chemical vapor deposition (CVD)-grown MoS2 and the characteristics associated with CVD growth have been extensively studied, challenges remain in designing specific regions on the monolayer MoS2 surface with reduced friction. Here, we develop nuclei with an onion-shell structure on CVD-grown monolayer MoS2 to achieve remarkable friction and adhesion reduction. These nuclei, dispersed on high-quality and crystalline MoS2, consist of an oxi-sulfide core surrounded by a multilayer MoS2 shell. Lateral force microscopy results indicate that onion-shell nuclei create an ensemble effect that decreases friction and adhesion by up to 45% and 20%, respectively, compared with those of MoS2 because of the multilayer structure and in-plane tensile strain, both of which minimize out-of-plane deformation. Derjaguin-M & uuml;ller-Toporov (DMT) model calculations and step-down load-friction correlations illustrate that the work of adhesion, shear strength, and coefficient of friction on the nucleus decrease by more than 22%, 19%, and 34%, respectively, compared with those on MoS2. The onion-shell nucleus presents a novel lubrication strategy to mitigate friction and adhesion in CVD-grown two-dimensional (2D) materials, with potential applications in lubricating nanoscale friction pairs.