Metasurfaces enable diverse applications by controlling light's amplitude, phase, and polarization. Although deep learning-based inverse design has revolutionized metasurface design, current models are limited by fixed operating conditions and lack universality, often requiring retraining for new wavelengths, polarizations, or application scenarios. To address this, we introduce MetasurfaceViT (Metasurface Vision Transformer), a generic AI model for inverse design. Our solution leverages a large dataset of Jones matrices, significantly expanded via physics-informed data augmentation. By pretraining through masking wavelengths and polarization channels, MetasurfaceViT can reconstruct full-wavelength Jones matrices, which are then used by a fine-tuning model for inverse design. This versatility allows one-shot structure design for arbitrary wavelength, polarization, and application requirements. We demonstrate MetasurfaceViT's capabilities in designing multiplexed printings and holograms and broadband achromatic metalenses. Prediction accuracy exceeds 99% for physically realistic designs, showcasing a significant step toward a universal optical inverse design paradigm.
Zero-thermal-expansion (ZTE) materials are critical for stabilizing device performance under thermal fluctuations. Traditionally, achieving enhanced thermal stability has required three-dimensional (3D) ZTE, a stringent condition that severely limits material availability. Here, we show that low-dimensional ZTE can be realized in single crystals by orienting ubiquitous bond rotations along specific crystallographic axes in the framework structures, thus relaxing the strict requirements for 3D ZTE. This approach enables a two-dimensional ZTE response, as demonstrated in a trigonal YAl3(BO3)4 (YAB) crystal, which exhibits an ultralow thermal expansion coefficient of -0.02(7) MK-1 within the ab plane from 83 to 180 K. The practical impact of this low-dimensional ZTE is evidenced by the thermo-optical performance of YAB crystal: within the ZTE temperature range, the thermo-optical coefficient varies by only 0.03(2) × 10-8 K-2 in the ZTE plane, approximately two orders of magnitude lower than those of conventional optical materials. This study establishes a new design strategy for functional ZTE materials and highlights the application potential of dimensionally confined ZTE effects in precision optical and electronic devices.
Developing efficient electrocatalysts for selective CO2-to-C2+ conversion remains challenging due to the kinetic limitations of C-C coupling and catalyst stability issues. In this work, we report a nano-defect-stabilized approach where Pd nanoparticles are immobilized in electrochemically generated nanoscale pits on CuO nanosheets, forming a stable CuO-Pd interface. The optimized catalyst achieves 70.30% Faradaic efficiency for C2+ products at -1.5 V versus RHE, outperforming bare CuO by over two-fold, while maintaining stable performance over 17 h. In situ spectroscopic studies reveal that the Pd-enhanced interface promotes CO coverage and stabilizes C-C coupling intermediates (*COCO and *COCHO). Theoretical calculations validate that the Pd-Cu interaction facilitates CO adsorption and reduces the energy barrier for C-C coupling. This nano-defect-stabilized strategy, which utilizes in situ-formed nano-defects to stabilize active metal sites, provides a generalizable design strategy for developing robust bimetallic CO2 reduction electrocatalysts.
Photo-electrocatalytic CO2 reduction (PEC CO2RR) to high-value-added fuels and chemicals is of great significance for alleviating the energy crisis and global warming. Although this technology can synergistically utilize solar energy and external bias to achieve efficient charge separation and CO2 conversion, the development of high-performance photo-electrocatalytic materials still faces severe challenges. In this review, we are concerned with the progress of high-performance catalysts for PEC CO2RR to high value-added products. Firstly, we systematically expound the basic principles and pathways of PEC CO2RR. Secondly, the various catalytic materials for optimizing the PEC CO2RR performance are reviewed in detail, including traditional semiconductors, perovskites, metal-organic frameworks, covalent organic frameworks, carbon-based materials and molecular catalysts. Thirdly, the role of photovoltaic device design in enhancing the overall conversion efficiency and product selectivity was summarized. Finally, we briefly discuss the research prospects and challenges of high-performance photo-electrocatalytic materials in PEC CO2RR.
Recently, colorless polyimide (CPI) substrates with excellent optical properties, a suitable thermal stability, and a low dielectric constant have become a key factor in the development of wearable and portable flexible electronic devices. A series of branched CPI films has been successfully prepared here by using a self-made triamine (1,3,5-triple (2-trifluoromethyl-4-aminobenzyl) benzene [TFAPOB]). By adjusting the ratio of the cyclopentanone bis-spironorbornane tetracarboxylic dianhydride (CPODA) monomer and the 4,4-(hexafluoroisopropyl)-diphthalic anhydride (6FDA) monomer, an optimal film (CBPI-10) with the highest content of CPODA was obtained. This film could achieve the highest transmittance of 90% at 550 nm and the highest glass transition temperature of 311 degrees C. This result could be explained by the fact that CBPI-10 contained the least amount of trifluoromethyl side groups and the largest amount of alicyclic units, which resulted in the generation of the minimum free volume fraction (according to molecular dynamics simulations) and the disruption of the conjugation effect between the benzene rings. Additionally, it is worth mentioning that the highest dielectric constant of these films was only 2.17, which was significantly higher than those of traditional CPI polymers (2.61-2.72). Consequently, the present study has focused on developing a novel manufacturing scheme for branched CPIs, which is of guidance importance for the design of colorless polymers and the advancement of flexible display technology.
A molecular ligand separation method based on multivariate metal-organic frameworks (MOF) is developed to precisely regulate CuSn alloy for tuning the selectivity of HCOOH and CO in CO2 reduction. With this method, the agglomeration and heterogeneous nucleations of metals are effectively inhibited during the in situ electrochemical transformation of CuSn-MOFs into highly pure CuSn alloy. The low Sn content favors CO production, while the high Sn concentration facilitates HCOOH formation.
Although optical phenomena in crystalline materials are different, they are all generated from the polarization processes of microscopic structural units under a photoelectric field. Thus, the development of simple and effective models that can evaluate the polarization ability of optical materials is crucial for their structural screening and mechanism analysis. Herein, we applied the "flexibility (F) index", a model previously used to investigate the structural origin of second-order nonlinear optical responses in unitary and binary diamond-like materials. We demonstrated that this index has a negative correlation with their band gap and a positive correlation with their first- and second-order polarizabilities. Remarkably, the first-order polarizability showed a linear-function correlation with the F-index, while the second-order polarizability exhibited a cube-function correlation with the "projected-flexibility (Fp) index". These polarizability-order-dependent correlations validated the feasibility of the F-index in characterizing specific optical properties. The results of this study prove the universality of the F-index to describe optical polarization, which serves as a quick and efficient tool to evaluate the optical response in crystalline materials.
Ionizing radiation dosimetry is critical in medical and industrial applications, yet conventional dosimeters often lack visual readability and sufficient detection sensitivity. Current radiochromic photonic materials offer wavelength-based dose visualization but face complex fabrication. Here, we develop a novel X-ray-responsive photonic film by magnetically assembling the carbon-encapsulated Fe3O4 (Fe3O4@C) nanochains in a GelMA precursor encapsulated by BaF2 plates. The BaF2 scintillator converts X-rays to UV light, inducing GelMA cross-linking and volumetric contraction, which modulates structural color changes of photonic films. Finite element simulation analysis confirms that radiochromic behaviors stem from a reduction in interparticle spacing of Fe3O4@C nanoparticles (Fe3O4@C NPs) along the nanochains direction. The optimized film (B0.5/Fe4/1L/S-1) achieve a low detection threshold (6 Gy), high sensitivity (4.62 Gy), and linear dose-response (R2 = 0.981, 0-10 Gy). This study integrates scintillator energy conversion with photonic structural color changes, enabling real-time, naked-eye X-ray dosimetry with potential applications in low-dose monitoring.
BACKGROUND:Relapsed/refractory acute lymphoblastic leukemia (R/R ALL) continues to be a major cause of mortality in children worldwide, with around 15% of ALL patients experiencing relapse and approximately 10% eventually dying from the disease. Early identification of R/R ALL in children has posed a longstanding clinical challenge. METHOD:Genetic analysis of survival outcomes in pediatric patients with ALL from the TARGET-ALL dataset revealed five risk score factors identified through the intersection of differential genes (relapse/non-relapse) from the GSE17703 and GSE6092 databases. A risk score equation was formulated using these factors and validated against prognostic data from 46 ALL cases at our institution. Patients from multiple datasets were stratified into high and low-score groups based on this equation. Protein-protein interaction networks (PPI) were then constructed using the intersecting differential genes from all three datasets to identify hub nodes and predict interacting transcription factors. Additionally, genes related to cell pyroptosis with varying expression across these datasets were screened, and a multifactorial ROC curve (incorporating risk score and differential expression of pyroptosis-related genes) was generated. Furthermore, relationships among variables in the predictive model were depicted using a nomogram, and model efficacy was assessed through decision curve analysis (DCA). RESULTS:By analyzing the TARGET-ALL, GSE17703, and GSE6092 databases, we developed a prognostic risk assessment model for pediatric ALL incorporating BAG2, EPHA4, FBXO9, SNX10, and WNK1. Validation of this model was conducted using data from 46 pediatric ALL cases obtained from our institution. Following the identification of 27 differentially expressed genes, we constructed a PPI and identified the top 10 hub genes (PTPRC, BTK, LCK, PRKCQ, CD3D, CD27, CD3G, BLNK, RASGRP1, VPREB1). Using this network, we predicted the top 5 transcription factors (HOXB4, MYC, SOX2, E2F1, NANOG). ROC and DCA were conducted on pyroptosis-related genes exhibiting differential expression and risk scores. Subsequently, a nomogram was generated, demonstrating the effectiveness of the risk score in predicting prognosis for pediatric ALL patients. CONCLUSIONS:We have developed a risk prediction model for pediatric R/R ALL utilizing the genes BAG2, EPHA4, FBXO9, SNX10, and WNK1. This model provides a scientific foundation for early identification of R/R ALL in children.
Microstructural evolution during fatigue is of significance for understanding the fatigue cracking of metallic alloys. Here, we visualized amorphization near the fatigue facets for an Mg-Gd-Y-Zn-Zr alloy with long-period stacking ordered (LPSO) phase upon very high cycle fatigue (VHCF). The small amorphous patches occurred in the relatively soft nano-Mg layers, compared to the hard LPSO phase, and the amorphous band propagated along with the basal plane near the LPSO/Mg interface. This should be intimately related to the local dislocation accumulation and cumulative damage upon the cycle loading-unloading.
To achieve optoelectronic devices with high resolution and efficiency, there is a pressing need for optical structural units that possess an ultrasmall footprint yet exhibit strong controllability in both the frequency and spatial domains. For dielectric nanoparticles, the overlap of electric and magnetic dipole moments can scatter light completely forward or backward, which is called Kerker theory. This effect can expand to any multipoles and any directions, re-named as generalized Kerker effect, and realize controllable light manipulation at full space and full spectrum using well-designed dielectric structures. However, the complex situations of multipole couplings make it difficult to achieve structural design. Here, generative artificial intelligence (AI) is utilized to facilitate multi-objective-oriented structural design, wherein we leverage the concept of "combined spectra" that consider both spectra and direction ratios as labels. The proposed generative adversarial network (GAN) is named as DDGAN (double-discriminator GAN) which discriminates both images and spectral labels. Using trained networks, we achieve the simultaneous design for scattering color and directivities, RGB color routers, as well as narrowband light routers. Notably, all generated structures possess a footprint less than 600x600 nm indicating their potential applications in optoelectronic devices with ultrahigh resolution.
Laser crystals, serving as the laser gain medium, are key materials in all-solid-state lasers. Due to considerable thermal expansion and low thermal conductivity, the performance of conventional laser crystals strongly depends on thermal management systems to improve the laser quality and power, which inevitably restricts the development of laser technology. In this work, a new potential laser crystal of Mn2+-doped Zn4B6O13 (ZBO) with a low thermal expansion and high thermal conductivity was grown and characterized. The strong luminescence emission at 539 nm in ZBO:Mn2+ was observed, with a long lifetime of 16.20(7) ms, and the corresponding absorption bands in the range of 410-460 nm fall within the spectra of GaN- or InGaN-based laser diodes. In variable-temperature fluorescence spectra, promoted by relaxation on the parity-forbidden 4T1-to-6A1 transition from the increased phonon number, an abnormal negative thermal quenching was manifested below 140 K, with the lifetime consistently greater than 10 ms over the whole temperature range of 80-500 K. Meanwhile, ZBO:Mn2+ manifests very low thermal expansion (3.1 MK-1) and high thermal conductivity (27.44(6) W/(mK)) at room temperature (300 K). These excellent thermal properties, combined with good optical properties, make ZBO:Mn2+ an outstanding gain medium for green laser generation. Our study confirms that ZBO is a promising laser matrix crystal.
Single‐atom catalysts (SACs) have been emerging as attractive catalytic materials in electrocatalysis for sustainable energy storage and conversion. To realize the practical implementation of SACs, reliable support is highly imperative to stabilize atomically dispersed metals with strong metal–support interaction, tunable local electronic environment, and favorable electron/mass transport. Thanks to great designability and tunability of composition, structure, and morphology, porous organic polymers (POPs) have demonstrated grand promise as appropriate support platforms toward the design of SACs at the molecular level and the fabrication of SACs in a controlled manner. Herein, a comprehensive overview of recent advances toward the elucidation of general design principles, effective synthesis approaches, and fundamental catalytic mechanisms for boosting the development of high‐performance POPs‐based SACs in electrocatalytic transformations is provided. The authors first outline rationales for using POPs‐based supports to stabilize SACs and design principles for electrocatalysis, followed by discussing fabrication approaches of utilizing POPs and POPs‐derived nanocarbons to host single‐atom metals. Then, state‐of‐the‐art POPs‐based SACs and their applications in heterogeneous electrocatalysis (ORR, OER, HER, CO 2 RR, and NRR) are discussed, of which the focus is on revealing the structure–performance correlation and catalytic mechanisms. Finally, challenges and strategies associated with the rational design of high‐performance SACs are suggested.
Organic–inorganic hybrid MAPbCl 3 perovskite (MA + = CH 3 NH 3 + ) in UV photodetection is drawing interest due to its superior semiconductor properties and UV‐matchable optical bandgap. However, MAPbCl 3 ‐based photodetector targeting high‐performance polarized light detection has remained unexplored due to the isotropic structure of MAPbCl 3 . The photovoltaic effect in the heterojunction, which shows an angle dependence on light polarization, provides opportunities to break the restriction of intrinsic structure for realizing polarization‐sensitive photodetection. Herein, an effective strategy is reported to realize high‐performance polarization‐sensitive UV photodetection by constructing a heterojunction with two isotropic materials MAPbCl 3 and Silicon (Si). Emphatically, the photovoltage in MAPbCl 3 /Si heterojunction changes with the angle of polarized light with the maximum (minimum) value of 0.15 V (0.05 V), originating from the built‐in electric field. More interestingly, driven by the photovoltage, the device thus exhibits a large polarization ratio ( I max / I min ) of 2.9 at 377 nm under the self‐driven mode. Besides, the present device also delivers high‐performance photodetection in UV region owing to the superior photoresponse of MAPbCl 3 , including a high detectivity ( D* ) of 2.93 × 10 11 Jones, a superior responsibility of 8 mA W –1 , a substantial switching ratio of 900, and an ultrafast response speed of 40/98 µs at 0 V bias. This work opens a new avenue for high‐performance polarization‐sensitive photodetection by utilizing angle‐dependent photovoltage effect.
The crawling process of snakes is known to have fascinating tribological phenomena, whereas investigations on their frictional properties depending on patterned cuticles are insufficient. In this study, we have designed and fabricated biomimetic microstructures inspired by the geometric microunits of Achalinus spinalis cuticle using polyurethane acrylate (PUA) material and performed its tribological analysis. The micro-morphology of this Achalinus-inspired textured polymer surface (AITPS) is characterized by the closely and evenly quasi-rectangular microgrooves, periodically arranged along certain orientations. We have compared the frictional performance of our fabricated AITPS with other competitive microstructure, using a smooth steel ball and commercial clay as an interacting surface. After performing massive friction tests with steel ball and clay, AITPS still maintains good resistance reduction performed compared to the patterned surface with straight microgrooves, which is most likely due to the reduction of actual contact areas at the frictional interface.
Resonances are ubiquitous in modern photonics, with the more familiar Fano and Fabry–Pérot resonators as key components of sophisticated optical devices with unique properties. However, the fundamental drawback of these devices is the difficulty in altering the resonance‐related features of the underlying optical structures postfabrication. This study investigates an active electrochromic tungsten oxide (WO 3 )‐based reconfigurable photonic structure with reversible switching between the Fano and Fabry–Pérot (F–P) resonances. This remarkable resonance switching occurs as a result of a change in the WO 3 film optical indices ( n , k ) via Li + intercalation/deintercalation, which can be inferred from the spectral response or dynamic reflected colors. When the bottom Ag layer's thickness is decreased from 130 to 10 nm, a semitransparent structure with unique optical properties emerges. The F–P resonant structure reflects and transmits different colors before Li + intercalation, while the Fano resonant structure reflects and transmits the same color after Li + intercalation. Along with these unique optical properties, a trans‐reflective filter and beam splitter filter are also developed based on the reversible electrochromism of a fixed optical configuration.
Plasmonic semiconductors with both features of metals and semiconductors are expected materials for solar light harvesting. Here, plasmonic semiconductor heterostructures were constructed by coupling pyroelectric black phosphorus (BP) and plasmonic tungsten oxides (WO) as photocatalyst for CO2 reduction. Intriguingly, under visible and near-infrared (NIR) light irradiation, the plasmonic BP/WO heterostructures with optimal composition exhibit high-selective 26.1 mu mol g(-1)h(-1) CO generation (98 %), which is 7-and 17-fold higher than those of plasmonic WO and pyroelectric BP, respectively. The interface bonds (P-O-W) were detected by FTIR spectra and demonstrated by density functional theory (DFT) calculations as dominant channels for electron transfer from BP to WO. Plasmonic thermal effect of WO can increase the local temperature to 86 C under visible and NIR light irradiation, triggering pyroelectric effect of BP and generating pyroelectric carriers, which enhance the electron transfer from BP to WO. Therefore, continuous electron injection from pyroelectric BP to WO enhances surface plasmon resonance for high-selective CO2 reduction. This work provides clear proofs to demonstrate that constructing pyroelectric effect on plasmonic heterostructures is one useful strategy to promote NIR-harvesting for artificial photosynthesis.
Two-dimensional perovskites of interlayer-multiple-cations (IMCs), which possess an intrinsic light absorption anisotropy, have the potential to become the candidate in polarization-sensitive photodetection.
Optical sensing technology has been widely used because of its advantages of high precision, low delay and imaging. With the rapid development of information technology such as big data and Internet of things, the demand for miniaturization and portability of optical detection and inspection platform is becoming more and more urgent. In order to overcome the dependence on large-scale special equipment and improve the applicability of on-site rapid detection and light-load platform application scenarios, in recent years on-chip integrated optical sensing technology has attracted great attention. With the integration of optical source, optical sensing and photoelectric detection units, as well as the development of on-chip light dispersion technology, the on-chip integration of optical sensing signal extraction and photoelectric signal conversion can be effectively realized, which contributes to the realization of the miniaturization and multi-functional integration. The relevant technical principles and technology development status were introduced, the pros and cons of the existing techniques were discussed, and the future development direction and application prospects were summarized.