Structural phase transition and potential superconductivity initiated by pressure-driven in 1T-CrSe2.

The exploration of the superconducting properties of antiferromagnetic parent compounds containing transition metals under pressure provides a unique idea for finding and designing superconducting materials with better performance. In this paper, the close relationship between the possible superconductivity and structure phase transition of the typical van der Waals layered material 1T-CrSe2 induced by pressure is studied by means of electrical transport and X-ray diffraction for the first time. We introduce the possibility of pressure-induced superconductivity at 20 GPa, with a critical Tc of approximately at 4 K. The superconductivity persists up to the highest measured pressure of 70 GPa, with a maximum Tc ~ 5 K at 24 GPa. We observed a structure phase transition from P-3m1 to C2/m space group in the range of 9.4-11.7 GPa. The results show that the structural phase transition leads to the metallization of 1T-CrSe2, and the further pressure effect makes the superconductivity appear in the new structure. The material undergoes a transition from a two-dimensional layered structure to a three-dimensional structure under pressure. This is the first time that possible superconductivity has been observed in 1T-CrSe2.

Out-of-plane Emission Dipole of Second Harmonic Generation in Odd- and Even-layered vdWs Janus Nb3SeI7.

Integration of atomically thin nonlinear optical (NLO) devices demands an out-of-plane (OP) emission dipole of second harmonic generation (SHG) to enhance the spontaneous emission for nanophotonics. However, the research on van der Waals (vdWs) materials with an OP emission dipole of SHG is still in its infancy. Here, by coupling back focal plane (BFP) imaging with numerical simulations and density functional theory (DFT) calculations, we demonstrate that vdWs Janus Nb3SeI7, ranging from bulk to the monolayer limit, exhibits a dominant OP emission dipole of SHG owing to the breaking of the OP symmetry. Explicitly, even-layered Nb3SeI7 with C6v symmetry is predicted to exhibit a pure OP emission dipole attributed to the only second-order susceptibility coefficient χzxx. Meanwhile, although odd-layered Nb3SeI7 with C3v symmetry has both OP and IP dipole components (χzxx and χyyy), the value of χzxx is 1 order of magnitude greater than that of χyyy, leading to an approximate OP emission dipole of SHG. Moreover, the crystal symmetry and OP emission dipole can be preserved under hydrostatic pressure, accompanied by the enhanced χzxx and the resulting 3-fold increase in SHG intensity. The reported stable OP dipole in 2D vdWs Nb3SeI7 can facilitate the rapid development of chip-integrated NLO devices.

Phase Transformation on Multilayer 2M-WS2 for Improved Surface-enhanced Raman Scattering.

In recent years, two-dimensional (2D) transition metal dichalcogenides (TMDCs) have been widely recognized as an ideal platform for surface-enhanced Raman scattering (SERS). Given their rich structural phases, phase transformation in 2D TMDCs is an efficient strategy to tailor their SERS performance. In this paper, we present the great SERS performance of multilayer 2M-WS2 and then investigate the effect of its phase transformation on SERS performance. It is observed that multilayer 2M-WS2 nanosheets undergo a thermally induced single-crystal phase transition from 2M-WS2 to 2H-WS2 upon thermal annealing or laser treatment. Distinguishing from the commercially available pure 2H-WS2 (P-2H-WS2), 2H-WS2 obtained by annealing and laser treatment still retain SERS properties comparable to those of 2M-WS2, among which the detection limits for CV molecules (10-8 M) are 3 orders of magnitude lower than that of P-2H-WS2 and the Raman intensity enhancements are ∼10-37 times higher. In contrast to the charge transfer (CT) mechanism governed by the Fermi level in metallic-phase 2M-WS2, 2H-WS2 obtained by phase transition exhibits accelerated CT facilitated by the bandgap reduction and reorganization resulting from the abundance of vacancies. This study introduces an interesting perspective and potential avenue for enhancing SERS through metal-to-semiconductor phase transitions in 2D TMDCs materials.

Stacking Faults Enabled Second Harmonic Generation in Centrosymmetric van der Waals RhI3.

Second harmonic generation (SHG) in van der Waals (vdW) materials has garnered significant attention due to its potential for integrated nonlinear optical and optoelectronic applications. Stacking faults in vdW materials are a typical kind of planar defect that introduces a degree of freedom to modulate the crystal symmetry and resultant SHG response. However, the physical origin and tunability of stacking-fault-governed SHG in vdW materials remain unclear. Here, taking the intrinsically centrosymmetric vdW RhI3 as an example, we theoretically reveal the origin of stacking-fault-governed SHG response, where the SHG response comes from the energetically favorable AC̅ stacking fault of which the electrical transitions along the high-symmetry paths Γ-M and Γ-K in the Brillion zone play the dominant role at 810 nm. Such a stacking-fault-governed SHG response is further confirmed via structural characterizations and SHG measurements. Furthermore, by applying hydrostatic pressure on RhI3, the correlation between structural evolution and SHG response is revealed with SHG enhancement up to 6.9 times, where the decreased electronic transition energies and higher momentum matrix elements due to the stronger interlayer interactions upon compression magnify the SHG susceptibility. This study develops a promising foundation for nonlinear nano-optics applications through the strategic design of stacking faults.

Nonlinear optical diode effect in a magnetic Weyl semimetal.

Diode effects are of great interest for both fundamental physics and modern technologies. Electrical diode effects (nonreciprocal transport) have been observed in Weyl systems. Optical diode effects arising from the Weyl fermions have been theoretically considered but not probed experimentally. Here, we report the observation of a nonlinear optical diode effect (NODE) in the magnetic Weyl semimetal CeAlSi, where the magnetization introduces a pronounced directionality in the nonlinear optical second-harmonic generation (SHG). We demonstrate a six-fold change of the measured SHG intensity between opposite propagation directions over a bandwidth exceeding 250 meV. Supported by density-functional theory, we establish the linearly dispersive bands emerging from Weyl nodes as the origin of this broadband effect. We further demonstrate current-induced magnetization switching and thus electrical control of the NODE. Our results advance ongoing research to identify novel nonlinear optical/transport phenomena in magnetic topological materials and further opens new pathways for the unidirectional manipulation of light.

Tunable anisotropic van der Waals films of 2M-WS2 for plasmon canalization.

In-plane anisotropic van der Waals materials have emerged as a natural platform for anisotropic polaritons. Extreme anisotropic polaritons with in-situ broadband tunability are of great significance for on-chip photonics, yet their application remains challenging. In this work, we experimentally characterize through Fourier transform infrared spectroscopy measurements a van der Waals plasmonic material, 2M-WS2, capable of supporting intrinsic room-temperature in-plane anisotropic plasmons in the far and mid-infrared regimes. In contrast to the recently revealed natural hyperbolic plasmons in other anisotropic materials, 2M-WS2 supports canalized plasmons with flat isofrequency contours in the frequency range of ~ 3000-5000 cm-1. Furthermore, the anisotropic plasmons and the corresponding isofrequency contours can be reversibly tuned via in-situ ion-intercalation. The tunable anisotropic and canalization plasmons may open up further application perspectives in the field of uniaxial plasmonics, such as serving as active components in directional sensing, radiation manipulation, and polarization-dependent optical modulators.

Ultralow Thermal Conductivity of a Chalcogenide System Pt3Bi4Q9 (Q = S, Se) Driven by the Hierarchy of Rigid [Pt6Q12]12- Clusters Embedded in Soft Bi-Q Sublattice.

Knowledge of structure-property relationships in solids with intrinsic low thermal conductivity is crucial for fields such as thermoelectrics, thermal barrier coatings, and refractories. Herein, we propose a new "rigidness in softness" structural scheme for intrinsic low lattice thermal conductivity (κL), which embeds rigid clusters into the soft matrix to induce large lattice anharmonicity, and accordingly discover a new series of chalcogenides Pt3Bi4Q9 (Q = S, Se). Pt3Bi4S9-xSex (x = 3, 6) achieved an intrinsic ultralow κL down to 0.39 W/(m K) at 773 K, which is considerably low among the Bi chalcogenide thermoelectric materials. Pt3Bi4Q9 contains the rigid cubic [Pt6Q12]12- clusters embedded in the soft Bi-Q sublattice, involving multiple bonding interactions and vibration hierarchy. The hierarchical structure yields a large lattice anharmonicity with high Grüneisen parameters (γ) 1.97 of Pt3Bi4Q9, as verified by the effective scatter of low-lying optical phonons toward heat-carrying acoustic phonons. Consequently, the rigid-soft coupling significantly inhibits heat propagation, exhibiting low acoustic phonon frequencies (∼25 cm-1) and Debye temperatures (ΘD = 170.4 K) in Pt3Bi4Se9. Owing to the suppressed κL and considerable power factor (PF), the ZT value of Pt3Bi4S6Se3 can reach 0.56 at 773 K without heavy carrier doping, which is competitive among the pristine Bi chalcogenides. Theoretical calculations predicted a large potential for performance improvement via proper doping, indicating the great potential of this structure type for promising thermoelectric materials.

Protective effects of Prussian blue nanozyme against sepsis-induced acute lung injury by activating HO-1.

Sepsis is a life-threatening condition involving dysfunctional organ responses stemming from dysregulated host immune reactions to various infections. The lungs are most prone to failure during sepsis, resulting in acute lung injury (ALI). ALI is associated with oxidative stress and inflammation, and current therapeutic strategies are limited. To develop a more specific treatment, this study aimed to synthesise Prussian blue nanozyme (PBzyme), which can reduce oxidative stress and inflammation, to alleviate ALI. PBzyme with good biosafety was synthesised using a modified hydrothermal method. PBzyme was revealed to be an activator of haem oxygenase-1 (HO-1), improving survival rate and ameliorating lung injury in mice. Zinc protoporphyrin, an inhibitor of HO-1, inhibited the prophylactic therapeutic efficacy of PBzyme on ALI, and affected the nuclear factor-κB signaling pathway and activity of HO-1. This study demonstrates that PBzyme can alleviate oxidative stress and inflammation through HO-1 and has a prophylactic therapeutic effect on ALI. This provides a new strategy and direction for the clinical treatment of sepsis-induced ALI.

High intrinsic phase stability of ultrathin 2M WS2.

Metallic 2M or 1T'-phase transition metal dichalcogenides (TMDs) attract increasing interests owing to their fascinating physicochemical properties, such as superconductivity, optical nonlinearity, and enhanced electrochemical activity. However, these TMDs are metastable and tend to transform to the thermodynamically stable 2H phase. In this study, through systematic investigation and theoretical simulation of phase change of 2M WS2, we demonstrate that ultrathin 2M WS2 has significantly higher intrinsic thermal stabilities than the bulk counterparts. The 2M-to-2H phase transition temperature increases from 120 °C to 210 °C in the air as thickness of WS2 is reduced from bulk to bilayer. Monolayered 1T' WS2 can withstand temperatures up to 350 °C in the air before being oxidized, and up to 450 °C in argon atmosphere before transforming to 1H phase. The higher stability of thinner 2M WS2 is attributed to stiffened intralayer bonds, enhanced thermal conductivity and higher average barrier per layer during the layer(s)-by-layer(s) phase transition process. The observed high intrinsic phase stability can expand the practical applications of ultrathin 2M TMDs.

1D Insertion Chains Induced Small-Polaron Collapse in MoS2 2D Layers Toward Fast-Charging Sodium-Ion Batteries.

Molybdenum disulfide (MoS2 ) with high theoretical capacity is viewed as a promising anode for sodium-ion batteries but suffers from inferior rate capability owing to the polaron-induced slow charge transfer. Herein, a polaron collapse strategy induced by electron-rich insertions is proposed to effectively solve the above issue. Specifically, 1D [MoS] chains are inserted into MoS2 to break the symmetry states of 2D layers and induce small-polaron collapse to gain fast charge transfer so that the as-obtained thermodynamically stable Mo2 S3 shows metallic behavior with 107 times larger electrical conductivity than that of MoS2 . Theoretical calculations demonstrate that Mo2 S3 owns highly delocalized anions, which substantially reduce the interactions of Na-S to efficiently accelerate Na+ diffusion, endowing Mo2 S3 lower energy barrier (0.38 vs 0.65 eV of MoS2 ). The novel Mo2 S3 anode exhibits a high capacity of 510 mAh g-1 at 0.5 C and a superior high-rate stability of 217 mAh g-1 at 40 C over 15 000 cycles. Further in situ and ex situ characterizations reveal the in-depth reversible redox chemistry in Mo2 S3 . The proposed polaron collapse strategy for intrinsically facilitating charge transfer can be conducive to electrode design for fast-charging batteries.

The complete reversal effect following angiotensin-converting enzyme inhibitors or angiotensin receptor blockers and beta-blockers after the primary diagnosis of dilated cardiomyopathy.

Background: Whether combination administration of angiotensin-converting enzyme inhibitors (ACEIs), angiotensin receptor blockers (ARBs), and beta-blockers (BBs) has a "reversal" effect on cardiac structure and function for first-diagnosed idiopathic dilated cardiomyopathy (FSIDCM) patients with unclear etiologies and inducements is unknown. Materials and Methods: We studied the effect of the protocol on FSIDCM patients. The effect was investigated in 26 FSIDCM patients. The criteria of "complete reversal" included left ventricular end-diastolic diameter (LVEDD) ≤50 mm for females or ≤55 mm for males and left ventricular ejection fraction (LVEF) ≥45%; the criteria of "partial reversal" was the decreased rate of LVEDD (ΔLVEDD) >10% or the increase rate of LVEF (ΔLVEF) >10%; the criteria of "no reversal" included LVEDD >50 mm for females or >55 mm for males and ΔLVEDD <10%, and LVEF <45% and ΔLVEF <10%. Results: Within the follow-up period, nine patients showed "complete reversal," eight "partial reversal," and nine "no reversal." Improvements in echocardiogram parameters were the most significant in "complete reversal" patients (P < 0.001), followed by "partial reversal" and "no reversal" patients (P < 0.05). The QRS (Q wave, R wave, S wave) duration and symptoms duration in "complete reversal" patients were the shortest, followed by "partial reversal" and "no reversal" patients. Conclusion: ACEIs or ARBs and BBs have a "complete reversal" effect on the left ventricular size and function of some FSIDCM patients. Patients with a narrow QRS and short symptom duration may have a good response.

An ISAR Image Component Recognition Method Based on Semantic Segmentation and Mask Matching.

The inverse synthetic aperture radar (ISAR) image is a kind of target feature data acquired by radar for moving targets, which can reflect the shape, structure, and motion information of the target, and has attracted a great deal of attention from the radar automatic target recognition (RATR) community. The identification of ISAR image components in radar satellite identification missions has not been carried out in related research, and the relevant segmentation methods of optical images applied to the research of semantic segmentation of ISAR images do not achieve ideal segmentation results. To address this problem, this paper proposes an ISAR image part recognition method based on semantic segmentation and mask matching. Furthermore, a reliable automatic ISAR image component labeling method is designed, and the satellite target component labeling ISAR image samples are obtained accurately and efficiently, and the satellite target component labeling ISAR image data set is obtained. On this basis, an ISAR image component recognition method based on semantic segmentation and mask matching is proposed in this paper. U-Net and Siamese Network are designed to complete the ISAR image binary semantic segmentation and binary mask matching, respectively. The component label of the ISAR image is predicted by the mask matching results. Experiments based on satellite component labeling ISAR image datasets confirm that the proposed method is feasible and effective, and it has greater comparative advantages compared to other classical semantic segmentation networks.

Manipulating Peierls Distortion in van der Waals NbOX2 Maximizes Second-Harmonic Generation.

Two-dimensional (2D) van der Waals (vdW) materials, featuring relaxed phase-matching conditions and highly tunable optical nonlinearity, endow them with potential applications in nanoscale nonlinear optical (NLO) devices. Despite significant progress, fundamental questions in 2D NLO materials remain, such as how structural distortion affects second-order NLO properties, which call for advanced regulation and in situ diagnostic tools. Here, by applying pressure to continuously tune the displacement of Nb atoms in 2D vdW NbOI2, we effectively modulate the polarization and achieve a 3-fold boost of the second-harmonic generation (SHG) at 2.5 GPa. By introducing a Peierls distortion parameter, λ, we establish a quantitative relationship between λ and SHG intensity. Importantly, we further demonstrate that the SHG enhancement can be achieved under ambient conditions by anionic substitution to tune the distortion in NbO(I1-xBrx)2 (x = 0-1) compounds, where the chemical tailoring simulates the pressure effects on the structural optimization. Consequently, NbO(I0.60Br0.40)2 with λ = 0.17 exhibits a giant SHG of over 2 orders of magnitude higher than that in monolayer WSe2, reaching the record-high value among reported 2D vdW NLO materials. This work unambiguously demonstrates the correlation between Peierls distortion and SHG property and, more broadly, opens new paths for the development of advanced NLO materials by manipulating the structure distortions.

Giant Reduction of Stabilized Pressure for the Superconducting Re0.8V0.2Se2 Phase.

Access to new superconducting phases in transition-metal dichalcogenides (TMDs) via pressure treatment has been the primary target in this field. As equally essential as the fabrication of new superconducting materials at high pressure, maneuvering new superconducting phases at moderate pressures is also one of the core goals in the synthesis community. Here, we successfully reduced the synthesized pressure of the superconducting phase in ReSe2 by combining V-doping and high-pressure techniques, with a reduction in pressure of 50% in contrast to ReSe2. Our electrical transport measurements displayed that metallization appeared at 10 GPa and subsequently superconductivity appeared at about 52.4 GPa with Tc ∼ 1.9 K. There was a giant reduction in the stable pressure of the superconducting phase derived from the d-electrons and interlayer interaction changes, as evidenced by the Hall effect and X-ray diffraction measurements. These findings serve as ideal starting points and guidance for designing superconducting TMDs at moderate pressures.

Customizable single-layer hydrogel robot with programmable NIR-triggered responsiveness.

Hydrogel robots are widely used in biomedical fields due to their excellent biocompatibility and response to external stimuli. However, traditional processing methods cannot rapidly fabricate complex structures, and smart response strategies often rely on double-layer structures fabricated from two materials with significantly different swelling properties. In this study, we present a single-layer hydrogel robot that can be fabricated in one step using a high-precision digital light processing (H-P DLP) 3D printing system. The robot has structural differences and the ability to maintain a repetitive response. Additionally, we fabricated several robot grippers to demonstrate their potential for customization and programming, as well as their potential applications in cargo delivery. Our work provides a new approach to achieve the formation and response of various irregular hydrogels, which is expected to advance the development of biomedical applications.

Femtosecond Laser-Driven Phase Engineering of WS2 for Nano-Periodic Phase Patterning and Sub-ppm Ammonia Gas Sensing.

Laser-driven phase transition of 2D transition metal dichalcogenides has attracted much attention due to its high flexibility and rapidity. However, there are some limitations during the laser irradiation process, especially the unsatisfied surface ablation, the inability of nanoscale phase patterning, and the unexploited physical properties of new phase. In this work, the well-controlled femtosecond (fs) laser-driven transformation from the metallic 2M-WS2 to the semiconducting 2H-WS2 is reported, which is confirmed to be a single-crystal to single-crystal transition without layer thinning or obvious ablation. Moreover, a highly ordered 2H/2M nano-periodic phase transition with a resolution of ≈435 nm is achieved, breaking through the existing size bottleneck of laser-driven phase transition, which is attributed to the selective deposition of plasmon energy induced by fs laser. It is also demonstrated that the achieved 2H-WS2 after laser irradiation contains rich sulfur vacancies, which exhibits highly competitive ammonia gas sensing performance, with a detection limit below 0.1 ppm and a fast response/recovery time of 43/67 s at room temperature. This study provides a new strategy for the preparation of the phase-selective transition homojunction and high-performance applications in electronics.

Topology Hierarchy of Transition Metal Dichalcogenides Built from Quantum Spin Hall Layers.

The evolution of the physical properties of 2D material from monolayer limit to the bulk reveals unique consequences from dimension confinement and provides a distinct tuning knob for applications. Monolayer 1T'-phase transition metal dichalcogenides (1T'-TMDs) with ubiquitous quantum spin Hall (QSH) states are ideal 2D building blocks of various 3D topological phases. However, the stacking geometry has been previously limited to the bulk 1T'-WTe2 type. Here, the novel 2M-TMDs consisting of translationally stacked 1T'-monolayers are introduced as promising material platforms with tunable inverted bandgaps and interlayer coupling. By performing advanced polarization-dependent angle-resolved photoemission spectroscopy as well as first-principles calculations on the electronic structure of 2M-TMDs, a topology hierarchy is revealed: 2M-WSe2 , MoS2, and MoSe2 are weak topological insulators (WTIs), whereas 2M-WS2 is a strong topological insulator (STI). Further demonstration of topological phase transitions by tunning interlayer distance indicates that band inversion amplitude and interlayer coupling jointly determine different topological states in 2M-TMDs. It is proposed that 2M-TMDs are parent compounds of various exotic phases including topological superconductors and promise great application potentials in quantum electronics due to their flexibility in patterning with 2D materials.

Polarization-Independent Second Harmonic Generation in 2D Van Der Waals Kagome Nb3 SeI7 Crystals.

Second harmonic generation (SHG) of 2D crystals has been of great interest due to its advantages of phase-matching and easy integration into nanophotonic devices. However, the polarization-dependence character of the SHG signal makes it highly troublesome but necessary to match the laser polarization orientation relative to the crystal, thus achieving the maximum polarized SHG intensity. Here, it is demonstrated a polarization-independent SHG, for the first time, in the van der Waals Nb3 SeI7 crystals with a breathing Kagome lattice. The Nb3 triangular clusters and Janus-structure of each Nb3 SeI7 layer are confirmed by the STEM. Nb3 SeI7 flake shows a strong SHG response due to its noncentrosymmetric crystal structure. More interestingly, the SHG signals of Nb3 SeI7 are independent of the polarization of the excitation light owing to the in-plane isotropic arrangement of nonlinear active units. This work provides the first layered nonlinear optical crystal with the polarization-independent SHG effect, providing new possibilities for nonlinear optics.

Ultrathin Mo2S3 Nanowire Network for High-Sensitivity Breathable Piezoresistive Electronic Skins.

Flexible piezosensing electronic skins (e-skins) have attracted considerable interest owing to their applications in real-time human-health monitoring, human-machine interactions, and soft bionic robot perception. However, the fabrication of piezosensing e-skins with high sensitivity, biological affinity, and good permeability at the same time is challenging. Herein, we designed and synthesized Mo2S3 nanowires by inserting ∞1[Mo2+S] chains between MoS2 interlayers. The resulting Mo2S3 nanowires feature high conductivity (4.9 × 104 S m-1) and a high aspect ratio (∼200). An ultrathin (∼500 nm) Mo2S3 nanowire network was fabricated using a simple liquid/liquid interface self-assembly method, showing high piezoresistive sensitivity (5.65 kPa-1), a considerably low pressure detection limit (0.08 Pa), and gratifying air permeability. Moreover, this nanowire network can be directly attached to human skin for real-time human pulse detection, finger movement monitoring, and sign language recognition, exhibiting excellent potential for health monitoring and human-machine interactions.

Alternating Direction Method of Multipliers for Convolutive Non-Negative Matrix Factorization.

Non-negative matrix factorization (NMF) has become a popular method for learning interpretable patterns from data. As one of the variants of standard NMF, convolutive NMF (CNMF) incorporates an extra time dimension to each basis, known as convolutive bases, which is well suited for representing sequential patterns. Previously proposed algorithms for solving CNMF use multiplicative updates which can be derived by either heuristic or majorization-minimization (MM) methods. However, these algorithms suffer from problems, such as low convergence rates, difficulty to reach exact zeroes during iterations and prone to poor local optima. Inspired by the success of alternating direction method of multipliers (ADMMs) on solving NMF, we explore variable splitting (i.e., the core idea of ADMM) for CNMF in this article. New closed-form algorithms of CNMF are derived with the commonly used ß -divergences as optimization objectives. Experimental results have demonstrated the efficacy of the proposed algorithms on their faster convergence, better optima, and sparser results than state-of-the-art baselines.