Solar overall water-splitting by a spin-hybrid all-organic semiconductor.

Direct solar-to-hydrogen conversion from pure water using all-organic heterogeneous catalysts remains elusive. The challenges are twofold: (i) full-band low-frequent photons in the solar spectrum cannot be harnessed into a unified S1 excited state for water-splitting based on the common Kasha-allowed S0 → S1 excitation; (ii) the H+ → H2 evolution suffers the high overpotential on pristine organic surfaces. Here, we report an organic molecular crystal nanobelt through the self-assembly of spin-one open-shell perylene diimide diradical anions (:PDI2-) and their tautomeric spin-zero closed-shell quinoid isomers (PDI2-). The self-assembled :PDI2-/PDI2- crystal nanobelt alters the spin-dependent excitation evolution, leading to spin-allowed S0S1 → 1(TT) → T1 + T1 singlet fission under visible-light (420 nm~700 nm) and a spin-forbidden S0 → T1 transition under near-infrared (700 nm~1100 nm) within spin-hybrid chromophores. With a triplet-triplet annihilation upconversion, a newly formed S1 excited state on the diradical-quinoid hybrid induces the H+ reduction through a favorable hydrophilic diradical-mediated electron transfer, which enables simultaneous H2 and O2 production from pure water with an average apparent quantum yield over 1.5% under the visible to near-infrared solar spectrum.

Acoustic Metagrating Holograms.

Metasurface holograms represent a common category of metasurface devices that utilize in-plane phase gradients to shape wavefronts, forming holographic images through the application of the generalized Snell's law (GSL). While conventional metasurfaces focus solely on phase gradients, metagratings, which incorporate higher-order wave diffraction, further expand the GSL's generality. Recent advances in certain acoustic metagratings demonstrate an updated GSL extension capable of reversing anomalous transmission and reflection, whose reversal is characterized by the parity of the number of wave propagation trips through the metagrating. However, the current extension of GSL remains limited to 1D metagratings, unable to access 2D holographic images in 3D spaces. Here, the GSL extension to 2D metagratings for manipulating waves within 3D spaces is investigated. Through this analysis, a series of acoustic metagrating holograms is experimentally demonstrated. These holographic images exhibit the unique ability to switch between transmission and reflection types independently. This study introduces an additional dimension to modern holography design and metasurface wavefront manipulation.

Observation of vortex-string chiral modes in metamaterials.

As hypothetical topological defects in the geometry of spacetime, vortex strings could have played many roles in cosmology, and their distinct features can provide observable clues about the early universe's evolution. A key feature of vortex strings is that they can interact with Weyl fermionic modes and support massless chiral-anomaly states along strings. To date, despite many attempts to detect vortex strings in astrophysics or to emulate them in artificially created systems, observation of these vortex-string chiral modes remains experimentally elusive. Here we report experimental observations of vortex-string chiral modes using a metamaterial system. This is implemented by inhomogeneous perturbation of Yang-monopole phononic metamaterials. The measured linear dispersion and modal profiles confirm the existence of topological modes bound to and propagating along the string with the chiral anomaly. Our work provides a platform for studying diverse cosmic topological defects in astrophysics and offers applications as topological fibres in communication techniques.

Three-dimensional flat Landau levels in an inhomogeneous acoustic crystal.

When electrons moving in two dimensions (2D) are subjected to a strong uniform magnetic field, they form flat bands called Landau levels (LLs). LLs can also arise from pseudomagnetic fields (PMFs) induced by lattice distortions. In three-dimensional (3D) systems, there has been no experimental demonstration of LLs  as a type of flat band thus far. Here, we report the experimental realization of a flat 3D LL in an acoustic crystal. Starting from a lattice whose bandstructure exhibits a nodal ring, we design an inhomogeneous distortion corresponding to a specific pseudomagnetic vector potential (PVP). This distortion causes the nodal ring states to break up into LLs, including a zeroth LL that is flat along all three directions. These findings suggest the possibility of using nodal ring materials to generate 3D flat bands, allowing access to strong interactions and other attractive physical regimes in 3D.

Spinful Topological Phases in Acoustic Crystals with Projective PT Symmetry.

For the classification of topological phases of matter, an important consideration is whether a system is spinless or spinful, as these two classes have distinct symmetry algebra that gives rise to fundamentally different topological phases. However, only recently has it been realized theoretically that in the presence of gauge symmetry, the algebraic structure of symmetries can be projectively represented, which possibly enables the switch between spinless and spinful topological phases. Here, we report the experimental demonstration of this idea by realizing spinful topological phases in "spinless" acoustic crystals with projective space-time inversion symmetry. In particular, we realize a one-dimensional topologically gapped phase characterized by a 2Z winding number, which features double-degenerate bands in the entire Brillouin zone and two pairs of degenerate topological boundary modes. Our Letter thus overcomes a fundamental constraint on topological phases by spin classes.

Observation of Dirac Hierarchy in Three-Dimensional Acoustic Topological Insulators.

Dirac cones (DCs) play a pivotal role in various unique phenomena ranging from massless electrons in graphene to robust surface states in topological insulators (TIs). Recent studies have theoretically revealed a full Dirac hierarchy comprising an eightfold bulk DC, a fourfold surface DC, and a twofold hinge DC, associated with a hierarchy of topological phases including first-order to third-order three-dimensional (3D) topological insulators, using the same 3D base lattice. Here, we report the first experimental observation of the Dirac hierarchy in 3D acoustic TIs. Using acoustic measurements, we unambiguously reveal that lifting of multifold DCs in each hierarchy can induce two-dimensional topological surface states with a fourfold DC in a first-order 3D TI, one-dimensional topological hinge states with a twofold DC in a second-order 3D TI, and zero-dimensional topological corner states in a third-order 3D TI. Our Letter not only expands the fundamental research scope of Dirac physics, but also opens up a new route for multidimensional robust wave manipulation.

Intelligent fault diagnosis of hydraulic piston pump based on deep learning and Bayesian optimization.

Hydraulic axial piston pump is broadly-used in aerospace, ocean engineering and construction machinery since it is the vital component of fluid power systems. In the light of the undiscoverability of its fault and the potential serious losses, it is valuable and challenging to complete the fault identification of a hydraulic pump accurately and effectively. Owing to the limitations of shallow machine learning methods in the intelligent fault diagnosis, more attention has been paid to deep learning methods. Hyperparameter plays an important role in a deep learning model. Although some manual tuning methods may represent good results in some cases, it is hard to reproduce due to the differences of datasets and other factors. Hence, Bayesian optimization (BO) algorithm is adopted to automatically select the hyperparameters. Firstly, the time-frequency images of vibration signals by continuous wavelet transform are taken as input data. Secondly, by setting some hyperparameters, a preliminary convolutional neural network (CNN) model is established. Thirdly, by identifying the range of each hyperparameter, BO based on Gaussian process is employed to construct an adaptive CNN model named CNN-BO. The performance of CNN-BO is verified by comparing with traditional LeNet 5 and improved LeNet 5 with manual optimization. The results indicate that CNN-BO can accomplish the intelligent fault diagnosis of a hydraulic pump accurately.

Demonstration of negative refraction induced by synthetic gauge fields.

Negative refraction is a counterintuitive wave phenomenon that has inspired the development of metamaterials and metasurfaces with negative refractive indices and surface phase discontinuities, respectively. Recent theories have proposed an alternative mechanism for negative refraction: Synthetic gauge fields, induced by either dynamical modulation or motion, can shift a material's dispersion in momentum space, forcing a positive refractive index medium to exhibit negative refraction above a certain threshold. However, this phenomenon has not previously been observed. Here, we report on the experimental demonstration of gauge field­induced negative refraction in a twisted bilayer acoustic metamaterial. The synthetic gauge fields arise in a projected two-dimensional geometry and can be continuously tuned by varying the wave number along the third dimension. Gauge field­induced waveguiding with backward-propagating modes is also demonstrated in a trilayer configuration. These results introduce a mechanism for performing wave manipulation in artificially engineered materials.

Low-Frequency, Open, Sound-Insulation Barrier by Two Oppositely Oriented Helmholtz Resonators.

In this work, a low-frequency, open, sound-insulation barrier, composed of a single layer of periodic subwavelength units (with a thickness of λ/28), is demonstrated both numerically and experimentally. Each unit was constructed using two identical, oppositely oriented Helmholtz resonators, which were composed of a central square cavity surrounded by a coiled channel. In the design of the open barrier, the distance between two adjacent units was twice the width of the unit, showing high-performance ventilation, and low-frequency sound insulation. A minimum transmittance of 0.06 could be observed around 121.5 Hz, which arose from both sound reflections and absorptions, created by the coupling of symmetric and asymmetric eigenmodes of the unit, and the absorbed sound energy propagating into the central cavity was greatly reduced by the viscous loss in the channel. Additionally, by introducing a multilayer open barrier, a broadband sound insulation was obtained, and the fractional bandwidth could reach approximately 0.19 with four layers. Finally, the application of the multilayer open barrier in designing a ventilated room was further discussed, and the results presented an omnidirectional, broadband, sound-insulation effect. The proposed open, sound-insulation barrier with the advantages of ultrathin thickness; omnidirectional, low-frequency sound insulation; broad bandwidth; and high-performance ventilation has great potential in architectural acoustics and noise control.

Observation of Dislocation-Induced Topological Modes in a Three-Dimensional Acoustic Topological Insulator.

The interplay between real-space topological lattice defects and the reciprocal-space topology of energy bands can give rise to novel phenomena, such as one-dimensional topological modes bound to screw dislocations in three-dimensional topological insulators. We obtain direct experimental observations of dislocation-induced helical modes in an acoustic analog of a weak three-dimensional topological insulator. The spatial distribution of the helical modes is found through spin-resolved field mapping, and verified numerically by tight-binding and finite-element calculations. These one-dimensional helical channels can serve as robust waveguides in three-dimensional media. Our experiment paves the way to studying novel physical modes and functionalities enabled by topological lattice defects in three-dimensional classical topological materials.

Acoustic non-Hermitian skin effect from twisted winding topology.

The recently discovered non-Hermitian skin effect (NHSE) manifests the breakdown of current classification of topological phases in energy-nonconservative systems, and necessitates the introduction of non-Hermitian band topology. So far, all NHSE observations are based on one type of non-Hermitian band topology, in which the complex energy spectrum winds along a closed loop. As recently characterized along a synthetic dimension on a photonic platform, non-Hermitian band topology can exhibit almost arbitrary windings in momentum space, but their actual phenomena in real physical systems remain unclear. Here, we report the experimental realization of NHSE in a one-dimensional (1D) non-reciprocal acoustic crystal. With direct acoustic measurement, we demonstrate that a twisted winding, whose topology consists of two oppositely oriented loops in contact rather than a single loop, will dramatically change the NHSE, following previous predictions of unique features such as the bipolar localization and the Bloch point for a Bloch-wave-like extended state. This work reveals previously unnoticed features of NHSE, and provides the observation of physical phenomena originating from complex non-Hermitian winding topology.

Acoustic Bessel Vortex Beam by Quasi-Three-Dimensional Reflected Metasurfaces.

Vortex beams have a typical characteristic of orbital angular momentum, which provides a new degree of freedom for information processing in remote communication and a form of non-contact manipulation for trapping particles. In acoustics, vortex beams are generally observed on the surface of a metamaterial structure or in a waveguide with a hard boundary owing to the characteristic of easy diffusion in free space. The realization of an acoustic vortex beam with a long-distance propagation in free space still remains a challenge. To overcome this, we report a type of acoustic Bessel vortex (ABV) beam created by a quasi-three-dimensional reflected metasurface in free space based on phase modulation. By using the Bessel and vortex phase profiles, we can realize an ABV beam with the high performances of both Bessel and vortex beams, and its effective propagation distance is larger than 9.2λ in free space. Beyond that, we discuss the bandwidth and topological charge of the ABV beam in detail, and the fractional bandwidth can reach about 0.28. The proposed ABV beam has the advantages of a high-performance vortex, long-distance propagation, and broad bandwidth, which provide a new pathway for designing multifunctional vortex devices with promising applications.

Fundamental Flaw in the Current Construction of the TiO2 Electron Transport Layer of Perovskite Solar Cells and Its Elimination.

The top-performing perovskite solar cells (efficiency > 20%) generally rely on the use of a nanocrystal TiO2 electron transport layer (ETL). However, the efficacies and stability of the current stereotypically prepared TiO2 ETLs employing commercially available TiO2 nanocrystal paste are far from their maximum values. As revealed herein, the long-hidden reason for this discrepancy is that acidic protons (∼0.11 wt %) always remain in TiO2 ETLs after high-temperature sintering due to the decomposition of the organic proton solvent (mostly alcohol). These protons readily lead to the formation of Ti-H species upon light irradiation, which act to block the electron transfer at the perovskite/TiO2 interface. Affront this challenge, we introduced a simple deprotonation protocol by adding a small amount of strong proton acceptors (sodium ethoxide or NaOH) into the common TiO2 nanocrystal paste precursor and replicated the high-temperature sintering process, which wiped out nearly all protons in TiO2 ETLs during the sintering process. The use of deprotonated TiO2 ETLs not only promotes the PCE of both MAPbI3-based and FA0.85MA0.15PbI2.55Br0.45-based devices over 20% but also significantly improves the long-term photostability of the target devices upon 1000 h of continuous operation.

Vortex states in an acoustic Weyl crystal with a topological lattice defect.

Crystalline materials can host topological lattice defects that are robust against local deformations, and such defects can interact in interesting ways with the topological features of the underlying band structure. We design and implement a three dimensional acoustic Weyl metamaterial hosting robust modes bound to a one-dimensional topological lattice defect. The modes are related to topological features of the bulk bands, and carry nonzero orbital angular momentum locked to the direction of propagation. They span a range of axial wavenumbers defined by the projections of two bulk Weyl points to a one-dimensional subspace, in a manner analogous to the formation of Fermi arc surface states. We use acoustic experiments to probe their dispersion relation, orbital angular momentum locked waveguiding, and ability to emit acoustic vortices into free space. These results point to new possibilities for creating and exploiting topological modes in three-dimensional structures through the interplay between band topology in momentum space and topological lattice defects in real space.

Intelligent Diagnosis towards Hydraulic Axial Piston Pump Using a Novel Integrated CNN Model.

As a critical part of a hydraulic transmission system, a hydraulic axial piston pump plays an indispensable role in many significant industrial fields. Owing to the practical undesirable working environment and hidden faults, it is challenging to precisely and effectively detect and diagnose the varying fault in the engineering. Deep learning-based technology presents special strengths in processing mechanical big data. It can simultaneously complete the feature extraction and classification, and achieve the automatic information learning. The popular convolutional neural network (CNN) is exploited for its potent ability of image processing. In this paper, a novel combined intelligent method is developed for fault diagnosis towards a hydraulic axial piston pump. First, the conversion of signals to images is conducted via continuous wavelet transform; the effective feature is preliminarily extracted from the transformed time-frequency images. Second, a novel deep CNN model is constructed to achieve the fault classification. To disclose the potential learning in the disparate layers of the CNN model, the visualization of reduced features is performed by employing t-distributed stochastic neighbor embedding. The effectiveness and stability of the proposed model are validated through the experiments. With the proposed method, different fault types can be precisely identified and high classification accuracy is achieved in a hydraulic axial piston pump.

An Integrated Deep Learning Method towards Fault Diagnosis of Hydraulic Axial Piston Pump.

A hydraulic axial piston pump is the essential component of a hydraulic transmission system and plays a key role in modern industry. Considering varying working conditions and the implicity of frequent faults, it is difficult to accurately monitor the machinery faults in the actual operating process by using current fault diagnosis methods. Hence, it is urgent and significant to investigate effective and precise fault diagnosis approaches for pumps. Owing to the advantages of intelligent fault diagnosis methods in big data processing, methods based on deep learning have accomplished admirable performance for fault diagnosis of rotating machinery. The prevailing convolutional neural network (CNN) displays desirable automatic learning ability. Therefore, an integrated intelligent fault diagnosis method is proposed based on CNN and continuous wavelet transform (CWT), combining the feature extraction and classification. Firstly, CWT is used to convert the raw vibration signals into time-frequency representations and achieve the extraction of image features. Secondly, a new framework of deep CNN is established via designing the convolutional layers and sub-sampling layers. The learning process and results are visualized by t-distributed stochastic neighbor embedding (t-SNE). The results of the experiment present a higher classification accuracy compared with other models. It is demonstrated that the proposed approach is effective and stable for fault diagnosis of a hydraulic axial piston pump.

Holey Cobalt-Iron Nitride Nanosheet Arrays as High-Performance Bifunctional Electrocatalysts for Overall Water Splitting.

Designing efficient metal nitride electrocatalysts with advantageous nanostructures toward overall water splitting is of great significance for energy conversion. In this work, holey cobalt-iron nitride nanosheet arrays grown on Ni foam substrate (CoFeNx HNAs/NF) are prepared via a facile hydrothermal and subsequent thermal nitridation method. This unique HNA architecture can not only expose abundant active sites but also facilitate the charge/mass transfer. Resulting from these merits, the CoFeNx HNAs/NF exhibits high catalytic performance with overpotentials of 200 and 260 mV at 10 mA cm-2 for the hydrogen evolution reaction (HER) and 50 mA cm-2 for the oxygen evolution reaction (OER), respectively. Furthermore, when using CoFeNx-500 HNAs/NF as both anode and cathode, the alkaline electrolyzer could afford a current density of 10 mA cm-2 at 1.592 V, higher than many other metal nitride-based electrocatalysts. This work signifies a simple approach to prepare holey metal nitride nanosheet arrays, which can be applied in various fields of energy conversion and storage.

Research on the Single-Value Indicators for Centrifugal Pump Based on Vibration Signals.

Off-design operation conditions might not only seriously affect the internal flow status of a centrifugal pump, but also result in additional energy loss and potential mechanical damage. Therefore, early-stage monitoring and predication on off-design operation conditions for centrifugal pumps have become essential. Single-value indicators have favorable factors such as a smaller amount of calculation and easier identification. As a result, industries prefer the more straightforward approach: obtaining single-value indicators directly from the signals which could be easier compared with accepted standards. The possibility of applying the single-value indicators of vibration into operation condition monitoring for a centrifugal pump is studied theoretically and experimentally, which shows that the statistical features of vibration might be suitable for hydraulic instability detection for a centrifugal pump.

Observation of an acoustic octupole topological insulator.

Berry phase associated with energy bands in crystals can lead to quantised observables like quantised dipole polarizations in one-dimensional topological insulators. Recent theories have generalised the concept of quantised dipoles to multipoles, resulting in the discovery of multipole topological insulators which exhibit a hierarchy of multipole topology: a quantised octupole moment in a three-dimensional bulk induces quantised quadrupole moments on its two-dimensional surfaces, which in turn induce quantised dipole moments on one-dimensional hinges. Here, we report on the realisation of an octupole topological insulator in a three-dimensional acoustic metamaterial. We observe zero-dimensional topological corner states, one-dimensional gapped hinge states, two-dimensional gapped surface states, and three-dimensional gapped bulk states, representing the hierarchy of octupole, quadrupole and dipole moments. Conditions for forming a nontrivial octupole moment are demonstrated by comparisons with two different lattice configurations having trivial octupole moments. Our work establishes the multipole topology and its full hierarchy in three-dimensional geometries.

Observation of a topological nodal surface and its surface-state arcs in an artificial acoustic crystal.

Three-dimensional (3D) gapless topological phases can be classified by the dimensionality of the band degeneracies, including zero-dimensional (0D) nodal points, one-dimensional (1D) nodal lines, and two-dimensional (2D) nodal surfaces. Both nodal points and nodal lines have been realized recently in photonics and acoustics. However, a nodal surface has never been observed in any classical-wave system. Here, we report on the experimental observation of a twofold symmetry-enforced nodal surface in a 3D chiral acoustic crystal. In particular, the demonstrated nodal surface carries a topological charge of 2, constituting the first realization of a higher-dimensional topologically-charged band degeneracy. Using direct acoustic field measurements, we observe the projected nodal surface and its Fermi-arc-like surface states and demonstrate topologically-induced robustness of the surface states against disorders. This discovery of a higher-dimensional topologically-charged band degeneracy paves the way toward further explorations of the physics and applications of new topological semimetal phases.